Publications by authors named "Sisi Wang"

120 Publications

Predicting COVID-19 epidemiological trend by applying population mobility data in two-stage modeling.

Zhejiang Da Xue Xue Bao Yi Xue Ban 2021 Feb;50(1):68-73

Collaborative Innovation Center for Diagnosis and Treatment of Infectious Diseases,Zhejiang University,Hangzhou 310003,China.

:To predict the epidemiological trend of coronavirus disease 2019 (COVID-19) by mathematical modeling based on the population mobility and the epidemic prevention and control measures. : As of February 8,2020,the information of 151 confirmed cases in Yueqing,Zhejiang province were obtained,including patients' infection process,population mobility between Yueqing and Wuhan,etc. To simulate and predict the development trend of COVID-19 in Yueqing, the study established two-stage mathematical models,integrating the population mobility data with the date of symptom appearance of confirmed cases and the transmission dynamics of imported and local cases. : It was found that in the early stage of the pandemic,the number of daily imported cases from Wuhan (using the date of symptom appearance) was positively associated with the number of population travelling from Wuhan to Yueqing on the same day and 6 and 9 days before that. The study predicted that the final outbreak size in Yueqing would be 170 according to the number of imported cases estimated by consulting the population number travelling from Wuhan to Yueqing and the susceptible-exposed-infectious-recovered (SEIR) model; while the number would be 165 if using the reported daily number of imported cases. These estimates were close to the 170,the actual monitoring number of cases in Yueqing as of April 27,2020. : The two-stage modeling approach used in this study can accurately predict COVID-19 epidemiological trend.
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http://dx.doi.org/10.3724/zdxbyxb-2021-0043DOI Listing
February 2021

Impact of socioeconomic status,population mobility and control measures on COVID-10 development in major cities of China.

Zhejiang Da Xue Xue Bao Yi Xue Ban 2021 Feb;50(1):52-60

Yale School of Public Health,Yale University,New Haven 06520,Connecticut,USA.

:To evaluate the impact of socioeconomic status,population mobility,prevention and control measures on the early-stage coronavirus disease 2019 (COVID-19) development in major cities of China. : The rate of daily new confirmed COVID-19 cases in the 51 cities with the largest number of cumulative confirmed cases as of February 19,2020 (except those in Hubei province) were collected and analyzed using the time series cluster analysis. It was then assessed according to three aspects,that is, socioeconomic status,population mobility,and control measures for the pandemic. : According to the analysis on the 51 cities,4 development patterns of COVID-19 were obtained,including a high-incidence pattern (in Xinyu),a late high-incidence pattern (in Ganzi),a moderate incidence pattern (in Wenzhou and other 12 cities),and a low and stable incidence pattern (in Hangzhou and other 35 cities). Cities with different types and within the same type both had different scores on the three aspects. : There were relatively large difference on the COVID-19 development among different cities in China,possibly affected by socioeconomic status,population mobility and prevention and control measures that were taken. Therefore,a timely public health emergency response and travel restriction measures inside the city can interfere the development of the pandemic. Population flow from high risk area can largely affect the number of cumulative confirmed cases.
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http://dx.doi.org/10.3724/zdxbyxb-2021-0028DOI Listing
February 2021

Impact of Wuhan lockdown on the spread of COVID-19 in China: a study based on the data of population mobility.

Zhejiang Da Xue Xue Bao Yi Xue Ban 2021 Feb;50(1):61-67

Department of Surgical Oncology,Sir Run Run Shaw Hospital,Zhejiang University School of Medicine,Hangzhou 310016,China.

This study aimed to quantitatively assess the effectiveness of the Wuhan lockdown measure on controlling the spread of coronavirus diesase 2019 (COVID-19). : Firstly,estimate the daily new infection rate in Wuhan before January 23,2020 when the city went into lockdown by consulting the data of Wuhan population mobility and the number of cases imported from Wuhan in 217 cities of Mainland China. Then estimate what the daily new infection rate would have been in Wuhan from January 24 to January 30th if the lockdown measure had been delayed for 7 days,assuming that the daily new infection in Wuhan after January 23 increased in a high,moderate and low trend respectively (using exponential, linear and logarithm growth models). Based on that,calculate the number of infection cases imported from Wuhan during this period. Finally,predict the possible impact of 7-day delayed lockdown in Wuhan on the epidemic situation in China using the susceptible-exposed-infectious-removed (SEIR) model. : The daily new infection rate in Wuhan was estimated to be 0.021%,0.026%,0.029%,0.033% and 0.070% respectively from January 19 to January 23. And there were at least 20 066 infection cases in Wuhan by January 23,2020. If Wuhan lockdown measure had been delayed for 7 days,the daily new infection rate on January 30 would have been 0.335% in the exponential growth model,0.129% in the linear growth model,and 0.070% in the logarithm growth model. Correspondingly,there would have been 32 075,24 819 and 20 334 infection cases travelling from Wuhan to other areas of Mainland China,and the number of cumulative confirmed cases as of March 19 in Mainland China would have been 3.3-3.9 times of the officially reported number. Conclusions: Timely taking city-level lockdown measure in Wuhan in the early stage of COVID-19 outbreak is essential in containing the spread of the disease in China.
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http://dx.doi.org/10.3724/zdxbyxb-2021-0021DOI Listing
February 2021

Understanding celiac disease monitoring patterns and outcomes after diagnosis: A multinational, retrospective chart review study.

World J Gastroenterol 2021 May;27(20):2603-2614

Takeda Pharmaceuticals International Co., Cambridge, MA 02139, United States.

Background: Long-term outcomes and monitoring patterns in real-world practice are largely unknown among patients with celiac disease.

Aim: To understand patterns of follow-up and management of patients with celiac disease, and to characterize symptoms and villous atrophy after diagnosis.

Methods: A retrospective chart review study was performed using medical chart data of patients diagnosed with celiac disease. Three gastroenterology referral centers, with substantial expertise in celiac disease, participated in the United Kingdom, United States, and Norway. Demographic and clinical data were collected from medical charts. Descriptive analyses were conducted on patients with biopsy-confirmed celiac disease, diagnosed between 2008 and 2012, with at least one follow-up visit before December 31, 2017. Patient demographic and clinical characteristics, biopsy/serology tests and results, symptoms, and comorbidities were captured at diagnosis and for each clinic visit occurring within the study period (, before the study end date of December 31, 2017).

Results: A total of 300 patients were included in this study [72% female; mean age at diagnosis: 38.9 years, standard deviation (SD) 17.2]. Patients were followed-up for a mean of 29.9 mo (SD 22.1) and there were, on average, three follow-up visits patient during the study period. Over two-thirds (68.4%) of patients were recorded as having ongoing gastrointestinal symptoms and 11.0% had ongoing symptoms and enteropathy during follow-up. Approximately 80% of patients were referred to a dietician at least once during the follow-up period. Half (50.0%) of the patients underwent at least one follow-up duodenal biopsy and 36.6% had continued villous atrophy. Patterns of monitoring varied between sites. Biopsies were conducted more frequently in Norway and patients in the United States had a longer follow-up duration.

Conclusion: This real-world study demonstrates variable follow-up of patients with celiac disease despite most patients continuing to have abnormal histology and symptoms after diagnosis.
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http://dx.doi.org/10.3748/wjg.v27.i20.2603DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8160626PMC
May 2021

Electroacupuncture inhibits the interaction between peripheral TRPV1 and P2X3 in rats with different pathological pain.

Physiol Res 2021 Jun 1. Epub 2021 Jun 1.

Department of Neurobiology and Acupuncture Research, the Third Clinical Medical College, Zhejiang Chinese Medical University, Key Laboratory of Acupuncture and Neurology of Zhejiang Province, Hangzhou, China.

Chronic pain is regarded to be one of the common and refractory diseases to cure in the clinic. One hundred Hz electroacupuncture (EA) is commonly used for inflammatory pain and 2 Hz for neuropathic pain possibly by modulating the transient receptor potential vanilloid subtype 1 (TRPV1) or the purinergic P2X3 related pathways. To clarify the mechanism of EA under various conditions of pathological pain, rats received a subcutaneous administration of complete Freund's adjuvant (CFA) for inflammatory pain and spared nerve injury (SNI) for neuropathic pain. The EA was performed at the bilateral ST36 and BL60 1 d after CFA or SNI being successfully established for 3 consecutive days. The mechanical hyperalgesia test was measured at baseline, 1 d after model establishment, 1 d and 3 d after EA. The co-expression changes, co-immunoprecipitation of TRPV1 and P2X3, and spontaneous pain behaviors (SPB) test were performed 3 d after EA stimulation. One hundred Hz EA or 2Hz EA stimulation could effectively down-regulate the hyperalgesia of CFA or SNI rats. The increased co-expression ratio between TRPV1 and P2X3 at the dorsal root ganglion (DRG) in two types of pain could be reduced by 100Hz or 2Hz EA intervention. While 100Hz or 2Hz EA was not able to eliminate the direct physical interaction between TRPV1 and P2X3. Moreover, EA could significantly inhibit the SPB induced by the co-activation of peripheral TRPV1 and P2X3. All results indicated that EA could significantly reduce the hyperalgesia and the SPB, which was partly related to inhibiting the co-expression and indirect interaction between peripheral TRPV1 and P2X3.
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June 2021

Phosphoproteomic Profiling of Rat's Dorsal Root Ganglia Reveals mTOR as a Potential Target in Bone Cancer Pain and Electro-Acupuncture's Analgesia.

Front Pharmacol 2021 29;12:593043. Epub 2021 Apr 29.

Key Laboratory of Acupuncture and Neurology of Zhejiang Province, Department of Neurobiology and Acupuncture Research, The Third Clinical Medical College, Zhejiang Chinese Medical University, Hangzhou, China.

Bone cancer pain (BCP) is a clinical refractory mixed pain involving neuropathic and inflammatory pain, with the underlying mechanisms remaining largely unknown. Electro-acupuncture (EA) can partly alleviate BCP according to previous research. We aim to explore the proteins and major pathways involved in BCP and EA treatment through phosphoproteomic profiling. BCP rat model was built by tibial inoculation of MRMT-1 mammary gland carcinoma cells. Mechanical hyperalgesia determined by paw withdrawal thresholds (PWTs) and bone destruction manifested on the radiographs confirmed the success of modeling, which were attenuated by EA treatment. The differentially expressed phosphorylated proteins (DEPs) co-regulated by BCP modeling and EA treatment in rat dorsal root ganglions (DRGs) were analyzed through PEX100 Protein microarray. Kyoto Encyclopedia of Genes and Genomes (KEGG) analysis revealed that DEPs were significantly enriched in mammalian target of rapamycin (mTOR) signaling pathway. The phosphorylations of mTOR at Ser2448 and Thr2446 were increased in BCP and downregulated by EA. In addition, the phosphorylation of S6K and Akt, markers of the mTOR complex, were also increased in BCP and downregulated by EA. Inhibition of mTOR signaling alleviated the PWTs of BCP rats, while the mTOR agonist impaired the analgesic effect of EA. Thus, our study provided a landscape of protein phosphorylation changes in DRGs of EA-treated BCP rats and revealed that mTOR signaling can be potentially targeted to alleviate BCP by EA treatment.
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http://dx.doi.org/10.3389/fphar.2021.593043DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8117331PMC
April 2021

Metabolic risk factors, genetic predisposition, and risk of severe liver disease in Chinese: a prospective study of 0.5 million people.

Am J Clin Nutr 2021 May 8. Epub 2021 May 8.

Department of Epidemiology & Biostatistics, School of Public Health, Peking University, Beijing, China.

Background: Metabolic risk factors have been shown to be associated with severe liver disease (SLD) in Chinese populations. However, there is limited evidence on the combined impact of these factors, or the genetic variants associated with SLD.

Objectives: We examined the associations of combined metabolic risk factors with risks of SLD, both overall and by genetic predisposition to SLD.

Methods: The study population involved 486,828 participants of the prospective China Kadoorie Biobank aged 30-79 years from 10 diverse areas in China without a history of cancer or liver disease at baseline. Cox regression was used to estimate adjusted HRs for SLD associated with combined metabolic risk factors (central adiposity, physical inactivity, and diabetes) by stratum of genetic risk [assessed separately by a PNPLA3 variant (rs738409) and a BMI genetic risk score].

Results: During ∼10 years of follow-up, 3279 incident cases of SLD were recorded. The overall mean BMI was 23.8 kg/m2 (SD, 3.4 kg/m2), and 5.9% participants had diabetes. Compared with those with 3 metabolic factors, participants with 2, 1, and 0 metabolic factors had 31% (HR, 0.69; 95% CI: 0.65-0.73), 43% (HR, 0.57; 95% CI: 0.53-0.60), and 52% (HR, 0.48; 95% CI: 0.42-0.56) lower risks of SLD, respectively. For both BMI and nonalcoholic fatty liver disease variants, participants with fewer metabolic factors had a lower risk of SLD, lower levels of gamma-glutamyl transferase, and lower fatty liver index scores, in participants with low and high genetic risks (P value for interaction > 0.05).

Conclusions: In relatively lean Chinese adults, individuals with fewer metabolic risk factors had a lower relative risk of SLD and a more favorable profile of liver biomarkers across all strata of genetic risk.
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http://dx.doi.org/10.1093/ajcn/nqab099DOI Listing
May 2021

Spatial and Temporal Characteristics of Environmental Air Quality and Its Relationship with Seasonal Climatic Conditions in Eastern China during 2015-2018.

Int J Environ Res Public Health 2021 04 24;18(9). Epub 2021 Apr 24.

College of Geography and Environmental Sciences, Zhejiang Normal University, Jinhua 321004, China.

Exploring the relationship between environmental air quality (EAQ) and climatic conditions on a large scale can help better understand the main distribution characteristics and the mechanisms of EAQ in China, which is significant for the implementation of policies of joint prevention and control of regional air pollution. In this study, we used the concentrations of six conventional air pollutants, i.e., carbon monoxide (CO), sulfur dioxide (SO), nitrogen dioxide (NO), fine particulate matter (PM), coarse particulate matter (PM), and ozone (O), derived from about 1300 monitoring sites in eastern China (EC) from January 2015 to December 2018. Exploiting the grading concentration limit (GB3095-2012) of various pollutants in China, we also calculated the monthly average air quality index (AQI) in EC. The results show that, generally, the EAQ has improved in all seasons in EC from 2015 to 2018. In particular, the concentrations of conventional air pollutants, such as CO, SO, and NO, have been decreasing year by year. However, the concentrations of particulate matter, such as PM and PM, have changed little, and the O concentration increased from 2015 to 2018. Empirical mode decomposition (EOF) was used to analyze the major patterns of AQI in EC. The first mode (EOF1) was characterized by a uniform structure in AQI over EC. These phenomena are due to the precipitation variability associated with the East Asian summer monsoon (EASM), referred to as the "summer-winter" pattern. The second EOF mode (EOF2) showed that the AQI over EC is a north-south dipole pattern, which is bound by the Qinling Mountains and Huaihe River (about 35° N). The EOF2 is mainly caused by seasonal variations of the mixed concentration of PM and O. Associated with EOF2, the Mongolia-Siberian High influences the AQI variation over northern EC by dominating the low-level winds (10 m and 850 hPa) in autumn and winter, and precipitation affects the AQI variation over southern EC in spring and summer.
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http://dx.doi.org/10.3390/ijerph18094524DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8123133PMC
April 2021

Systemic Inflammation Response Index (SIRI) Independently Predicts Survival in Advanced Lung Adenocarcinoma Patients Treated with First-Generation EGFR-TKIs.

Cancer Manag Res 2021 15;13:1315-1322. Epub 2021 Feb 15.

Department of Oncology, The Second Xiangya Hospital, Central South University, Changsha, 410011, Hunan, People's Republic of China.

Background: Systemic inflammation response index (SIRI) has been reported to be an effective blood-based biomarker for predicting prognosis in various kinds of cancer patients. However, the prognostic role of SIRI in advanced lung adenocarcinoma patient remains unclear.

Methods: The aim of the present study is to evaluate the prognostic role of SIRI in EGFR-mutant advanced lung adenocarcinoma patients treated with first-generation EGFR-TKIs. A total of 245 patients who received gefitinib, erlotinib, or icotinib at the Second Xiangya Hospital were retrospectively evaluated. SIRI was defined as neutrophil count×monocyte/lymphocyte count. The optimal cut-off value was determined according to receiver operation characteristic curve analysis. Characteristics of patients were compared via chi-square test or Fisher's exact test. Survivals were estimated by the Kaplan-Meier method and compared by the Log rank test. Multivariate analysis was estimated using the Cox proportional hazards model.

Results: It is showed that high SIRI was associated with male patient, smoker, worse ECOG PS, 19-DEL mutation. Kaplan-Meier survival analysis showed that ECOG PS, brain metastasis, SIRI were significantly correlated with progression-free survival (PFS), and gender, ECOG PS, brain metastasis, NLR and SIRI were significantly correlated with overall survival (OS). Multivariate analysis showed that SIRI and ECOG PS independently predict PFS and OS.

Conclusion: Our findings indicate that SIRI is an effective and convenient marker for predicting prognosis in advanced EGFR-mutant lung adenocarcinoma patients treated with first-generation TKI.
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http://dx.doi.org/10.2147/CMAR.S287897DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7900776PMC
February 2021

Highly stretchable and self-foaming polyurethane composite skeleton with thermally tunable microwave absorption properties.

Nanotechnology 2021 Feb 25. Epub 2021 Feb 25.

College of Engineering, Zhejiang Normal University, Jinhua, CHINA.

Stretchable and lightweight polymer composite material possessing tunable microwave absorption properties under thermal radiations remains a significant challenge. Here, we proposed a facile strategy to fabricate stretchable, magnetic composite skeletons by incorporating the tadpole-like [email protected] nanoparticles into self-foaming polyurethane (PU) matrix and the electromagnetic responsive of [email protected]/PU composite foams with different CNTs contents under heating-cooling cycle in a temperature range of 253~333K were carefully investigated. Enhanced complex permittivity and shifting peak frequency were observed at elevated temperatures. For instance, the [email protected]/PU sample with 15wt% loading content at 333K exhibits excellent microwave absorption (MA) properties including a minimum reflection loss (RLm) of 66.9 dB and ultrabroad effective frequency bandwidth (RL  20 dB) of 9.98 GHz at the thickness of 1.58~3.37 mm. Meanwhile, great recoverability in terms of RL-f profile was achieved in the process of thermal cooling back to 253 K. Such adjustable MA property was attributed to the well-matched impedance and dramatic attenuation ability, benefiting from the temperature-dependant electrical conductivity, abundant interfacial polarization and interior microcellular structures. Besides, the rising temperature increased the sample elongation and electrical conductivity with a slight sacrifice of maximum tensile strength. This stretchable PU skeleton with a unique assembly of CNTs and Fe3O4 nanoparticles are expected to be promising candidates as smart absorbers for application in the harsh environments.
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http://dx.doi.org/10.1088/1361-6528/abe9e7DOI Listing
February 2021

Analysis of Molecular Mechanism of YiqiChutan Formula Regulating DLL4-Notch Signaling to Inhibit Angiogenesis in Lung Cancer.

Biomed Res Int 2021 12;2021:8875503. Epub 2021 Feb 12.

Department of Medical Technologic, The First Affiliated Hospital to Guangzhou University of Chinese Medicine, Guangzhou 510405, China.

In order to explore the specific mechanism of YiqiChutan formula (YQCTF) in inhibiting the angiogenesis of lung cancer and its relationship with delta-like ligand 4- (DLL4-) Notch signaling, 30 healthy BALB/c-nu/nu rats were selected and divided into three groups: A549 group (implanted with lung adenocarcinoma cell line A549), NCI-H460 group (implanted with human lung large-cell carcinoma cell line NCI-H460), and NCI-H446 group (implanted with human lung small cell carcinoma cell line NCI-H446) for constructing lung cancer transplanted tumor models. After modeling, the group treated with normal saline was taken as control group, 200 mg/kg of YQCTF was adopted for intervention, and the tumor volume and growth inhibition rate were compared with the vascular targeted inhibitor Sorafenib. HE staining, CD31 fluorescent antibody staining, and microelectron microscopy were adopted to observe the neovascular endothelial cells of the transplanted tumor. The expression of VEGF, HIF-1, DLL4, and Notch-1 in the transplanted tumors in each group was detected by Western blot and RT-PCR at the protein level or mRNA level. Compared with the control group, the YQCTF-treated group had obvious inhibitory effect on lung cancer transplanted tumor and lung cancer angiogenesis. In the YQCTF-treated group, the density of angiogenesis decreased significantly and the vascular lumen structure also decreased, and the expression levels of VEGF, HIF-1, DLL4, and Notch-1 in the YQCTF-treated group were all lower than those in the control group. YQCTF could inhibit the growth of lung cancer transplanted tumor through antiangiogenesis, and it could also reduce the amount of angiogenesis in lung cancer transplanted tumor. In addition, the generation of lumen structure was also hindered, which was realized through the VEGF signaling pathway and DLL4-Notch signaling pathway.
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http://dx.doi.org/10.1155/2021/8875503DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7895574PMC
May 2021

Insights in the Recalcitrance of Theasinensin A to Human Gut Microbial Degradation.

J Agric Food Chem 2021 Mar 23;69(8):2477-2484. Epub 2021 Feb 23.

Laboratory of Food Chemistry, Wageningen University, P.O. Box 17, Wageningen 6700 AA , The Netherlands.

Due to low bioavailability of dietary phenolic compounds in small intestine, their metabolism by gut microbiota is gaining increasing attention. The microbial metabolism of theasinensin A (TSA), a bioactive catechin dimer found in black tea, has not been studied yet. Here, TSA was extracted and purified for fermentation by human fecal microbiota, and epigallocatechin gallate (EGCG) and procyanidin B2 (PCB2) were used for comparison. Despite the similarity in their flavan-3-ol skeletons, metabolic fate of TSA was distinctively different. After degalloylation, its core biphenyl-2,2',3,3',4,4'-hexaol structure remained intact during fermentation. Conversely, EGCG and PCB2 were promptly degraded into a series of hydroxylated phenylcarboxylic acids. Computational analyses comparing TSA and PCB2 revealed that TSA's stronger interflavanic bond and more compact stereo-configuration might underlie its lower fermentability. These insights in the recalcitrance of theasinensins to degradation by human gut microbiota are of key importance for a comprehensive understanding of its health benefits.
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http://dx.doi.org/10.1021/acs.jafc.1c00727DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8028050PMC
March 2021

Adaptive federated filter for multi-sensor nonlinear system with cross-correlated noises.

PLoS One 2021 19;16(2):e0246680. Epub 2021 Feb 19.

School of Navigation, Guangdong Ocean University, Zhanjiang, China.

This paper presents an adaptive approach to the federated filter for multi-sensor nonlinear systems with cross-correlations between process noise and local measurement noise. The adaptive Gaussian filter is used as the local filter of the federated filter for the first time, which overcomes the performance degradation caused by the cross-correlated noises. Two kinds of adaptive federated filters are proposed, one uses a de-correlation framework as local filter, and the subfilter of the other one is defined as a Gaussian filter with correlated noises at the same-epoch, and much effort is made to verify the theoretical equivalence of the two algorithms in the nonlinear fusion system. Simulation results show that the proposed algorithms are superior to the traditional federated filter and Gaussian filter with same-paced correlated noises, and the equivalence between the proposed algorithms and high degree cubature federated filter is also demonstrated.
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http://journals.plos.org/plosone/article?id=10.1371/journal.pone.0246680PLOS
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7895398PMC
February 2021

Thermal switches between delayed fluorescence and persistent phosphorescence based on a keto-BODIPY electron acceptor.

Org Biomol Chem 2021 Mar;19(9):2030-2037

State Key Laboratory of Coordination Chemistry, Collaborative Innovation Center of Advanced Microstructures, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210046, P. R. China.

A new type of twisted donor-acceptor molecular material 3a and 3b containing carbazole as an electron donor and keto-BODIPY bearing keto-isoindolinyl and pyridyl subunits as an acceptor has been prepared and characterized. Chemical modifications at the meso-position of keto-BODIPY with a nitrogen atom and a cyano group enhance the electron withdrawing ability and cause the emission color change from blue to yellow and red. Steady-state absorption and emission spectra of the two compounds show a strong intramolecular charge transfer (ICT) character. Time-resolved emission spectra and transient decay curves of 3a and 3b show efficient delayed fluorescence with a lifetime of 12.64 μs for 3a and 16.59 μs for 3b at room temperature, whereas persistent phosphorescence with a lifetime of 576.65 ms for 3a and 273.76 ms for 3b was obviously detected at 77 K. These photophysical behaviors have been fully revealed via X-ray diffraction analysis and theoretical calculations, and thus attributed to the hybridized local and charge-transfer (HLCT) states and increased spin-orbital coupling (SOC) strength by mixed n → π* and π → π* transitions involving heteroatom lone pairs and the π-conjugated skeleton, respectively.
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http://dx.doi.org/10.1039/d0ob02390fDOI Listing
March 2021

Highly regioselective palladium-catalyzed domino reaction for post-functionalization of BODIPY.

Chem Commun (Camb) 2021 Feb;57(14):1758-1761

State Key Laboratory of Coordination Chemistry, Collaborative Innovation Center of Advanced Microstructures, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210046, P. R. China.

A series of benzo[a]-fused BODIPYs and the corresponding isomeric naphthyl-BODIPYs have been synthesized through a facile one-pot palladium-catalyzed domino reaction of BODIPY precursors (2-bromo-BODIPYs) with diarylethynes, via "cis, cis" and "trans, cis" addition transition states with alkynes, respectively. This reaction exhibits unprecedentedly complete cyclization regioselectivity to the a-position of the BODIPY over the b-one, and the resulting products can be effectively regulated by the substituent choice on the diarylethynes.
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http://dx.doi.org/10.1039/d0cc08163aDOI Listing
February 2021

Luminescent Quantum Dots Stabilized by N-Heterocyclic Carbene Polymer Ligands.

J Am Chem Soc 2021 02 15;143(4):1873-1884. Epub 2021 Jan 15.

Department of Chemistry and Biochemistry, Florida State University, 95 Chieftan Way, Tallahassee, Florida 32306, United States.

We have tested the ability of N-heterocyclic carbene (NHC)-modified ligands to coordinate and stabilize luminescent CdSe-ZnS core-shell quantum dot (QD) dispersions in hydrophilic media. In particular, we probed the effects of ligand structure and coordination number on the coating affinity to the nanocrystals. We find that such NHC-based ligands rapidly coordinate onto the QDs (requiring ∼5-10 min of reaction time), which reflects the soft Lewis base nature of the NHC groups, with its two electrons sharing capacity. Removal of the hydrophobic cap and promotion of carbene-driven coordination on the nanocrystals have been verified by H NMR spectroscopy, while C NMR was used to identify the formation of carbene-Zn complexes. The newly coated QD dispersions exhibit great long-term colloidal stability over a wide range of conditions. Additionally, we find that coordination onto the QD surfaces affects the optical and spectroscopic properties of the nanocrystals. These include a size-dependent red-shift of the absorption and fluorescence spectra and a pronounced increase in the measured fluorescence intensity when the samples are stored under white light exposure compared to those stored in the dark.
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http://dx.doi.org/10.1021/jacs.0c10592DOI Listing
February 2021

Systemic Inflammation Response Index Is a Predictor of Poor Survival in Locally Advanced Nasopharyngeal Carcinoma: A Propensity Score Matching Study.

Front Oncol 2020 10;10:575417. Epub 2020 Dec 10.

Department of Oncology, The Second Xiangya Hospital, Central South University, Changsha, China.

Introduction: Nasopharyngeal carcinoma (NPC) is a common malignancy in China and known prognostic factors are limited. In this study, neutrophil-to-lymphocyte ratio (NLR), platelet-to-lymphocyte ratio (PLR), systemic immune inflammation index (SII), and systemic inflammation response index (SIRI) were evaluated as prognostic factors in locally advanced NPC patients.

Materials And Methods: NPC patients who received curative radiation or chemoradiation between January 2012 and December 2015 at the Second Xiangya Hospital were retrospectively reviewed, and a total of 516 patients were shortlisted. After propensity score matching (PSM), 417 patients were eventually enrolled. Laboratory and clinical data were collected from the patients' records. Receiver operating characteristic curve analysis was used to determine the optimal cut-off value. Survival curves were analyzed using the Kaplan-Meier method. The Cox proportional hazard model was used to identify prognostic variables.

Results: After PSM, all basic characteristics between patients in the high SIRI group and low SIRI group were balanced except for sex (=0.001) and clinical stage (=0.036). Univariate analysis showed that NLR (=0.001), PLR (=0.008), SII (=0.001), and SIRI <0.001) were prognostic factors for progression-free survival (PFS) and overall survival (OS). However, further multivariate Cox regression analysis showed that only SIRI was an independent predictor of PFS and OS (hazard ratio (HR):2.83; 95% confidence interval (CI): 1.561-5.131; =0.001, HR: 5.19; 95% CI: 2.588-10.406; <0.001), respectively.

Conclusion: Our findings indicate that SIRI might be a promising predictive indicator of locally advanced NPC patients.
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http://dx.doi.org/10.3389/fonc.2020.575417DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7759154PMC
December 2020

Higher blood cadmium level is associated with greater cognitive decline in rural Chinese adults aged 65 or older.

Sci Total Environ 2021 Feb 26;756:144072. Epub 2020 Nov 26.

Department of Biostatistics, Indiana University School of Medicine, Indianapolis, IN 46202-2872, USA.

Cadmium (Cd) exposure has been reported to have neurotoxic effects in animal studies and associated with increased Alzheimer's Disease mortality and lower cognitive function in cross-sectional and case-control studies. However, no results from longitudinal studies on Cd and cognitive decline are available. In this prospective cohort study, we recruited 1867 participants aged 65 years or older from rural areas in China, blood Cd and cognitive function were measured at baseline (2010-2012), and 1554 participants completed cognitive function tests during a 3-year follow-up (2013-2015). Cognitive function was evaluated using nine standardized cognitive tests: The Community Screening Instrument for Dementia, the CERAD Word List Learning, Word list recall, IU Story Recall, Animal Fluency Test, Boston Naming Test, Stick Design, Delayed Stick Design and the IU Token Test. Analysis of covariance models and logistic regression models were used to determine the association between Cd and standardized cognitive decline adjusting for covariates. The median blood Cd concentration of this study population was 2.12 μg/L, and the interquartile range was 1.42-4.64 μg/L. Significant association of higher Cd levels with lower cognitive scores were observed in five individual cognitive tests (Delayed Stick Design Test, Boston Naming Test, CERAD Word List Learning Test, Word List Recall Test and IU Story Recall Test) and the composite cognitive score adjusting for multi-covariates at baseline. Higher Cd levels were significantly associated with greater 3-year cognitive decline in Delayed Stick Design Test, Boston Naming Test, IU Token Test, Word List Recall Test and Composite cognitive score. For these cognitive tests, participants in the top two Cd quartile groups had significantly greater decline than those in the lowest Cd quartile group, while the two lowest Cd quartile groups were not significantly different. Our findings suggest that higher Cd exposure is associated with greater cognitive decline in older Chinese adults.
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http://dx.doi.org/10.1016/j.scitotenv.2020.144072DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7775354PMC
February 2021

The Transferability and Design of Commercial Printer Settings in PLA/PBAT Fused Filament Fabrication.

Polymers (Basel) 2020 Nov 2;12(11). Epub 2020 Nov 2.

Centre for Polymer and Material Technologies (CPMT), Department of Materials, Textiles and Chemical Engineering, Ghent University, Technologiepark 130, 9052 Zwijnaarde, Belgium.

In many fused filament fabrication (FFF) processes, commercial printers are used, but rarely are printer settings transferred from one commercial printer to the other to give similar final tensile part performance. Here, we report such translation going from the Felix 3.0 to Prusa i3 MK3 printer by adjusting the flow rate and overlap of strands, utilizing an in-house developed blend of polylactic acid (PLA) and poly(butylene adipate-co-terephthalate) (PBAT). We perform a sensitivity analysis for the Prusa printer, covering variations in nozzle temperature, nozzle diameter, layer thickness, and printing speed (, , LT, and ), aiming at minimizing anisotropy and improving interlayer bonding. Higher mass, larger width, and thickness are obtained with larger , lower , higher LT, and higher . A higher results in less tensile strain at break, but it remains at a high strain value for samples printed with equal to 0.5 mm. has no significant effect on the tensile modulus and tensile and impact strength of the samples. If LT is fixed, an increased is beneficial for the tensile strength, ductility, and impact strength of the printed sample due to better bonding from a wider raster structure, while an increased LT leads to deterioration of mechanical properties. If the ratio /LT is greater than 2, a good tensile performance is obtained. An improved leads to a sufficient flow of material, contributing to the performance of the printed device. The considerations brought forward result in a deeper understanding of the FFF process and offer guidance about parameter selection. The optimal //LT/ combination is 0.5 mm/120 mm s/0.15 mm/230 °C.
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http://dx.doi.org/10.3390/polym12112573DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7694024PMC
November 2020

The mRNA expression levels of GABA receptor α1 and α2 subunits in patients with major depressive disorder during onset and remission.

Int J Neurosci 2021 Mar 4:1-7. Epub 2021 Mar 4.

Department of Psychiatry, The First Affiliated Hospital of Jinan University, Guangzhou, Guangdong, China.

Objective: We aimed to investigate the expression levels of GABA and GABA receptor α1 and α2 subunits in patients with major depressive disorder (MDD) during onset and remission.

Materials And Methods: 48 patients with MDD during onset and 45 patients with MDD during remission who were treated in our university were selected. Moreover, the control group included 46 healthy volunteers recruited in the community. The depression and anxiety symptoms were assessed by Hamilton Depression (HAMD) Scale and Hamilton Anxiety (HAMA) Scale. ELISA was used to determine the serum GABA levels. The mRNA expression of GABA receptor α1 and α2 subunits in peripheral blood were detected by RT-PCR.

Results: The expression levels of serum GABA and of GABA receptor α1 and α2 subunits in MDD depression attack group were notably decreased in comparison with those in MDD remission group and control group ((4.10 ± 0.73) v.s. (5.91 ± 1.25) and (5.83 ± 1.17) umol/L,  = 5.61,  < 0.001; (0.53 ± 0.32) v.s. (0.91 ± 0.18) and (0.93 ± 0.21),  = 8.37,  < 0.001; (1.45 ± 0.86) v.s. (2.33 ± 1.49) and (2.28 ± 1.50),  = 8.23,  < 0.001). However, there were no marked difference in the levels of these three indices between the MDD remission group and the control group ( > 0.05). Serum GABA levels were negatively correlated with HAMA total score (r = -0.34,  = 0.02), HAMD total score (r = -0.46,  = 0.01) and depression core symptom score (r = -0.32,  = 0.03).

Conclusions: During the onset of MDD, there may be GABA neuronal dysfunction and abnormal expression of GABA receptor subunits, and those changes showed a state change, which gradually returned to normal during remission.
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http://dx.doi.org/10.1080/00207454.2020.1829618DOI Listing
March 2021

Severe metabolic disorders coexisting with Werner syndrome: a case report.

Endocr J 2021 Mar 20;68(3):261-267. Epub 2020 Oct 20.

Department of Endocrinology, The Second Hospital of Jilin University, Changchun, Jilin, China.

Werner syndrome, also called adult progeria, is a heritable autosomal recessive human disorder characterized by the premature onset of numerous age-related diseases including juvenile cataracts, dyslipidemia, diabetes mellitus (DM), osteoporosis, atherosclerosis, and cancer. Werner syndrome is a segmental progeroid syndrome whose presentation resembles accelerated aging. The most common causes of death for WS patients are atherosclerosis and cancer. A 40-year-old female presented with short stature, bird-like facies, canities with alopecia, scleroderma-like skin changes, and non-healing foot ulcers. The patient reported a history of delayed puberty, abortion, hypertriglyceridemia, and juvenile cataracts. A clinical diagnosis of WS was made and subsequently confirmed. We discovered two WRN gene mutations in the patient, Variant 1 was the most common WRN mutation, nonsense mutation (c.1105C>T:p.R369Ter) in exon 9, which caused a premature termination codon (PTC) at position 369. Variant 2 was a frameshift mutation (c.1134delA:p.E379KfsTer5) in exon 9, which caused a PTC at position 383 and has no published reports describing. Patients with WS can show a wide variety of clinical and biological manifestations in endocrine-metabolic systems (DM, thyroid dysfunction, and hyperlipidemia). Doctors must be cognizant of early manifestations of WS and treatment options.
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http://dx.doi.org/10.1507/endocrj.EJ20-0448DOI Listing
March 2021

Stimulus-induced Alpha Suppression Tracks the Difficulty of Attentional Selection, Not Visual Working Memory Storage.

J Cogn Neurosci 2021 Mar 15;33(3):536-562. Epub 2020 Oct 15.

Vanderbilt University.

Human alpha-band activity (8-12 Hz) has been proposed to index a variety of mechanisms during visual processing. Here, we distinguished between an account in which alpha suppression indexes selective attention versus an account in which it indexes subsequent working memory storage. We manipulated two aspects of the visual stimuli that perceptual attention is believed to mitigate before working memory storage: the potential interference from distractors and the size of the focus of attention. We found that the magnitude of alpha-band suppression tracked both of these aspects of the visual arrays. Thus, alpha-band activity after stimulus onset is clearly related to how the visual system deploys perceptual attention and appears to be distinct from mechanisms that store target representations in working memory.
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http://dx.doi.org/10.1162/jocn_a_01637DOI Listing
March 2021

Prospective phenotyping of long-term survivors of generalized arterial calcification of infancy (GACI).

Genet Med 2021 02 2;23(2):396-407. Epub 2020 Oct 2.

Medical Genetics Branch, National Human Genome Research Institute, National Institutes of Health, Bethesda, MD, USA.

Purpose: Generalized arterial calcification of infancy (GACI), characterized by vascular calcifications that are often fatal shortly after birth, is usually caused by deficiency of ENPP1. A small fraction of GACI cases result from deficiency of ABCC6, a membrane transporter. The natural history of GACI survivors has not been established in a prospective fashion.

Methods: We performed deep phenotyping of 20 GACI survivors.

Results: Sixteen of 20 subjects presented with arterial calcifications, but only 5 had residual involvement at the time of evaluation. Individuals with ENPP1 deficiency either had hypophosphatemic rickets or were predicted to develop it by 14 years of age; 14/16 had elevated intact FGF23 levels (iFGF23). Blood phosphate levels correlated inversely with iFGF23. For ENPP1-deficient individuals, the lifetime risk of cervical spine fusion was 25%, that of hearing loss was 75%, and the main morbidity in adults was related to enthesis calcification. Four ENPP1-deficient individuals manifested classic skin or retinal findings of PXE. We estimated the minimal incidence of ENPP1 deficiency at ~1 in 200,000 pregnancies.

Conclusion: GACI appears to be more common than previously thought, with an expanding spectrum of overlapping phenotypes. The relationships among decreased ENPP1, increased iFGF23, and rickets could inform future therapies.
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http://dx.doi.org/10.1038/s41436-020-00983-0DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7867608PMC
February 2021

Graphene oxide inhibits cell migration and invasion by destroying actin cytoskeleton in cervical cancer cells.

Aging (Albany NY) 2020 Sep 14;12(17):17625-17633. Epub 2020 Sep 14.

Department of Pathology, Hebei North University, Zhangjiakou, Hebei Province, China.

Objective: To investigate the antitumor effects of Graphene oxide (GO) on tumor invasion and metastasis in human cervical cancer Hela cells.

Results: GO significantly inhibited cell viability and the number of clones, promoted cell apoptosis, as well as suppressed cell migration and invasion, and destroyed the structure of actin cytoskeleton of Hela cells in a dose-dependent manner in. Moreover, the expression of metastasis-related proteins, including MMP2 and Cdc42, were significantly suppressed by the treatment of GO. And the expression of MMP3 was remarkably increased by Smad inhibitor and the protein levels of MMP3 and ICAM were elevated by the JNK inhibitor in GO-treated Hela cells.

Conclusion: GO exhibited inhibitory effects on cell migration and invasion possibly by destroying actin cytoskeleton in Hela cells, which is a potential component of the Smad and JNK signalling pathways.

Methods: GO was prepared and chracterized by UV visible light absorption spectroscopy and atomic force microscopy. Hela cells were treated with Go at different dose levels. Then, in vitro cytotoxicity of GO was evaluated by the MTT assay, colony-forming assay and cell apoptosis assay. The inhibitory effects of GO on tumor cell migration and invasion as well as actin cytoskeleton were explored using Hela cells.
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http://dx.doi.org/10.18632/aging.103821DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7521503PMC
September 2020

A visualized clinical model predicting good quality blastocyst development in the first IVF/ICSI cycle.

Reprod Biomed Online 2020 Nov 23;41(5):807-817. Epub 2020 Jul 23.

Shenzhen Key Laboratory of Reproductive Immunology for Peri-Implantation, Shenzhen Zhongshan Institute for Reproduction and Genetics, Fertility Center, Shenzhen Zhongshan Urology Hospital, Shenzhen Guangdong 518045, People's Republic of China. Electronic address:

Research Question: Is it possible to establish a visualized clinical model predicting good quality blastocyst (GQB) formation for patients in their first IVF/intracytoplasmic sperm injection (ICSI) cycle?

Design: A total of 4783 patients in their first IVF/ICSI cycle between January 2015 and December 2019 were retrospectively included and randomly divided into the training set (n = 3826) and the testing set (n = 957) in an 8:2 ratio. The least absolute shrinkage and selection operator (LASSO) regression was adopted to select the most critical predictors for GQB formation to construct a visualized nomogram model based on the data of patients in the training set. Receiver operating characteristic and calibration curves were used to evaluate the predictive accuracy and discriminative ability. The performance of the model was also validated on independent data from patients treated in the testing set.

Results: Maternal age, maternal serum anti-Müllerian hormone (MsAMH) concentration and the number of oocytes retrieved were highlighted as critical predictors of GQB development and were incorporated into the nomogram model. Based on the area under the curve (AUC) values, the predictive ability for ≥1, ≥3 and ≥5 GQB were 0.831, 0.734 and 0.748, respectively. The calibration curve also showed high concordance between the observed and predicted results. The AUC for predicting ≥1, ≥3 and ≥5 GQB in the testing set were 0.805, 0.695 and 0.707, respectively, which were similar to those for the training set.

Conclusions: The visualized nomogram model provides great predictive value for GQB development in patients in their first IVF/ICSI cycle and can be used to improve clinical counselling.
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http://dx.doi.org/10.1016/j.rbmo.2020.07.018DOI Listing
November 2020

Long Noncoding RNA Contributes to the Tumorigenesis of Colorectal Cancer Through Regulating Expression by Sponging .

Cancer Biother Radiopharm 2020 Jul 17. Epub 2020 Jul 17.

Health Management Center, Qingdao Municipal Hospital, Qingdao, China.

Colorectal cancer (CRC), a malignant tumor, has become a highly relevant social problem. Nuclear paraspeckle assembly transcript 1 () was reported as an oncogenic long noncoding RNA in diverse tumors, including CRC. Nevertheless, the mechanism of in CRC remains unknown. The expression levels of and solute carrier family 38 member 1 () in CRC tissues and cells were detected by real-time quantitative polymerase chain reaction. The protein levels of p62, microtubule-associated protein light (LC3-I), LC3-II, and were examined by Western blot assay. Cell proliferation, apoptosis, and invasion were measured by 3-(4, 5-dimethyl-2-thiazolyl)-2, 5-diphenyl-2-H-tetrazolium bromide (MTT), and flow cytometry and transwell assays, respectively. The interaction between and or was predicted by StarBase or TargetScan, and verified by the dual-luciferase reporter assay. The effect of on tumor growth was determined in CRC mice model. The expression of and was upregulated in CRC tissues and cells. knockdown or downregulation restrained cell proliferation and invasion, and accelerated cell apoptosis and autophagy of CRC cells. acted as a sponge of to regulate expression. Furthermore, deficiency suppressed tumor growth These studies disclosed that knockdown inhibited CRC progression by / axis, providing an underlying target for CRC treatment.
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http://dx.doi.org/10.1089/cbr.2020.3608DOI Listing
July 2020

TLR13, TLR22, TRAF6, and TAK1 in the soiny mullet (Liza haematocheila): Molecular characterization and expression profiling analysis.

Dev Comp Immunol 2020 11 4;112:103774. Epub 2020 Jul 4.

Key Laboratory of Exploration and Utilization of Aquatic Genetic Resources, Ministry of Education, Shanghai Ocean University, Shanghai, 201306, China. Electronic address:

Toll-like receptors (TLRs) and their associated signaling pathways play pivotal roles in the immune response to invading pathogens. Here, TLR13, TLR22, tumor necrosis factor receptor-associated factor 6 (TRAF6), and transforming growth factor-β-activated kinase1 (TAK1) were characterized in the soiny mullet (Liza haematocheila), representative mugilid species that is widely cultured in Asia. The four mullet genes, which shared characteristic features with their counterparts in other teleosts, were ubiquitously expressed in all of the examined tissues, albeit with different expression patterns. Following Streptococcus dysgalactiae infection, the four genes were upregulated to different degrees in various mullet tissues. These results indicated that the four genes were involved in the mullet immune response to bacterial infection. To the best of our knowledge, this is the first characterization of these four genes in mullet. Our results provide a basis for future studies of TLR signaling pathways in mullet, as well as for similar studies in other mugilids.
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http://dx.doi.org/10.1016/j.dci.2020.103774DOI Listing
November 2020

Electroacupuncture Regulates Pain Transition by Inhibiting the mGluR5-PKCε Signaling Pathway in the Dorsal Root Ganglia.

J Pain Res 2020 19;13:1471-1483. Epub 2020 Jun 19.

Department of Neurobiology and Acupuncture Research, The Third Clinical Medical College, Zhejiang Chinese Medical University, Key Laboratory of Acupuncture and Neurology of Zhejiang Province, Hangzhou 310053, People's Republic of China.

Background: Acute pain can transition to chronic pain, presenting a major clinical challenge. Electroacupuncture (EA) can partly prevent the transition from acute to chronic pain. However, little is known about the mechanisms underlying the effect of EA. This study investigated the effect of EA on pain transition and the activation of metabotropic glutamate receptor 5 (mGluR5)-protein kinase C epsilon (PKCε) signaling pathway in the dorsal root ganglia (DRG).

Methods: The hyperalgesic priming model was established by the sequential intraplantar injection of carrageenan (1%, 100 μL) and prostaglandin E2 (PGE2) into the left hind paw of rats. EA treatment (2/100 Hz, 30 min, once/day) was applied at bilateral Zusanli (ST36) and Kunlun (BL60) acupoints in rats. Von Frey filaments were used to investigate the mechanical withdrawal threshold (MWT) at different time points. The protein expression levels of mGluR5 and PKCε in the ipsilateral L4-L6 DRGs of rats were detected by Western blot. Some pharmacological experiments were performed to evaluate the relationship between mGluR5, PKCε and the MWT. It was also used to test the effects of EA on the expression levels of mGluR5 and PKCε and changes in the MWT.

Results: Sequential injection of carrageenan and PGE2 significantly decreased the MWT of rats and up-regulated the expression level of mGluR5 and PKCε in the ipsilateral L4-L6 DRGs. EA can reverse the hyperalgesic priming induced by sequential injection of carrageenan/PGE and down-regulate the protein expression of mGluR5 and PKCε. Glutamate injection instead of PGE2 can mimic the hyperalgesic priming model. Pharmacological blocking of mGluR5 with specific antagonist MTEP can prevent the hyperalgesic priming and inhibit the activation of PKCε in DRGs. Furthermore, EA also produced analgesic effect on the hyperalgesic priming rats induced by carrageenan/mGluR5 injection and inhibited the high expression of PKCε. Sham EA produced none analgesic and regulatory effect.

Conclusion: EA can regulate pain transition and it may relate with its inhibitory effect on the activation of mGluR5-PKCε signaling pathway in the DRGs.
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http://dx.doi.org/10.2147/JPR.S251948DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7311359PMC
June 2020

Enhanced Stabilization and Easy Phase Transfer of CsPbBr Perovskite Quantum Dots Promoted by High-Affinity Polyzwitterionic Ligands.

J Am Chem Soc 2020 07 13;142(29):12669-12680. Epub 2020 Jul 13.

Florida State University, Department of Chemistry and Biochemistry, 95 Chieftan Way, Tallahassee, Florida 32306, United States.

The successful growth of colloidal lead halide perovskite quantum dots (PQDs) has generated tremendous interest in the community, due to the unique properties and the promise PQDs offer for use in applications involving light-emitting devices and solar cell technology. However, tangible progress in probing their fundamental properties and/or their integration into optoelectronic devices has been hampered by issues of colloidal and photophysical instability. Here, we introduce a promising surface coating strategy relying on a polyzwitterion polymer, where high-affinity binding onto the QDs is driven by multicoordinating electrostatic interactions with the ion-rich surfaces of CsPbBr PQDs. The polymer ligands were synthesized by installing a stoichiometric mixture of amine-modified sulfobetaine anchors and solubilizing motifs on poly(isobutylene--maleic anhydride), PIMA, via nucleophilic addition reaction. We find that this coating approach imparts enhanced colloidal and photophysical stability to the nanocrystals over a broad range of solvent conditions and in powder form. This approach also allows easy phase transfer of the PQDs from nonpolar media to an array of solutions with varying polarities and properties. Additionally, the stabilization strategy preserves the photophysical and structural characteristics of the nanocrystals over a period extending to 1.5 years under certain conditions.
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http://dx.doi.org/10.1021/jacs.0c03682DOI Listing
July 2020

Regulation of an Ambient-Light-Induced Photocyclization Pathway (Norrish-Yang Versus 6π) by Substituent Choice.

Chemistry 2020 Sep 4;26(54):12418-12430. Epub 2020 Sep 4.

State Key Laboratory of Coordination Chemistry, Collaborative Innovation Center of Advanced Microstructures, School of Chemistry and Chemical Engineering Nanjing University, Nanjing, 210046, P. R. China.

Photocyclization, irrespective of whether multiple steps (e.g., Norrish-Yang cyclization) or a single concerted step (e.g., 6π photocyclization) are involved, is an intramolecular photochemical process resulting in the formation of one new single bond to afford a ring system. In particular, visible-light-induced photocyclization offers a green and sustainable route to organic cyclic compounds that are difficult to access by thermal reactions. Herein, we describe the ambient light-induced intramolecular photocyclization of a series of donor/acceptor chromophores 1 d-3 d containing two types of photoresponsive motifs, namely an electron-deficient BF -chelated ketone fused with an electron-rich thiophene, and probe the solution-phase and solid-state photochromic performance of these compounds. The results reveal that simple variation of R substituents on the diaryl moiety allows one to control the intramolecular photocyclization mechanism with high photochemical selectivity, e.g., under ambient light, methyl-substituted 1 d and 2 d undergo reversible 6π photocyclization, whereas ethyl-substituted 3 d exclusively undergoes irreversible Norrish-Yang photocyclization. Single-crystal X-ray analysis of Norrish-Yang cyclization products reveals the formation of four pairs of conformational enantiomers differing in the dihedral angle between benzothiophene and the BF core, namely (±)N-3 [email protected]°, (±)N-3 [email protected]°, (±)N-3 [email protected]°, and (±)N-3 [email protected]°. The UV/Vis absorption spectra of 1 d-3 d cover a broad visible-light region (380-572 nm), while DFT and TD-DFT calculations reveal that absorption in this region is dominated by the charge-transfer (CT) transition from the thiophene-centered HOMO to the LUMO of the electron-deficient π-conjugated BF -chelated unit and the n→π* and π→π* transitions within the latter unit. The spatial separation of the HOMO and LUMO of these dyes promotes triplet-state generation and self-photosensitizes intramolecular photocyclization in the visible-light region. Three-dimensional time-resolved and steady-state emission spectra of 3 d show that the Norrish-Yang photocyclization takes place within milliseconds with excellent conversion efficiency (96 %).
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http://dx.doi.org/10.1002/chem.202000990DOI Listing
September 2020