Publications by authors named "Ying Luo"

605 Publications

Optimized culture methods for isolating small extracellular vesicles derived from human induced pluripotent stem cells.

J Extracell Vesicles 2021 Apr 10;10(6):e12065. Epub 2021 Apr 10.

Tianjin Key Laboratory of Artificial Cell Tianjin Institute of Hepatobiliary Disease Nankai University Affiliated Third Center Hospital Tianjin China.

Extracellular vesicles that are derived from stem cells play an important role in the treatment of disease. To obtain high-quality small extracellular vesicles (sEVs), we optimized the culture conditions of human induced pluripotent stem cells (hiPSCs), the supernatant collection time, and sEVs extraction methods. Firstly, hiPSCs were cultured in extracellular vesicles-production medium (EVs-PM) containing different concentrations (0%, 0.25%, 0.5%, 2%, 5%, and 20%) of extracellular vesicle-depleted knockout serum replacement (ED-KSR), and the culture supernatants were collected continuously for 5 days. Then, the sEVs were isolated, followed by an evaluation of their characteristics. The survival rates of the hiPSCs lines that were cultured in EVs-PM containing 0.5% to 20% ED-KSR were not significantly different (> 0.05). The survival rates of the hiPSCs in 0.5% ED-KSR after the culture supernatants were continuously collected for day 1, day 3, and day 5 were not statistically significant (> 0.05). After 5 days of continuous collection of the supernatant, the hiPSCs expressed some pluripotent markers, while SSEA4 and TRA-1-60 expression changed gradually. The sEVs that were extracted by the two methods were all 50-200 nm, double-layered and oval or round cellular vesicles and expressed the marker proteins CD63, TSG101, and HSP70. The characteristics of sEVs extracted on day 1, day 3, and day 5 were almost identical on morphology, size and the relative quantity of annexin V-positive subpopulations. The PKH67 staining showed that the sEVs could be endocytosed by HepG2 cells and aggregated in the cytoplasm. The proliferation experiments showed that the sEVs can promote cell proliferation. In Conclusion, the 0.5% ED-KSR is the optimal concentration, and that the hiPSCs culture supernatant can be continuously collected for 5 days while maintaining high cell viability and some pluripotent characteristics. Both of the methods extraction can be used to obtain biologically active sEVs.
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http://dx.doi.org/10.1002/jev2.12065DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8035677PMC
April 2021

Resveratrol as a plant type antioxidant modifier for polysulfone membranes to improve hemodialysis-induced oxidative stress.

Mater Sci Eng C Mater Biol Appl 2021 Apr 10;123:111953. Epub 2021 Feb 10.

State Key Laboratory of Separation Membranes and Membrane Processes, School of Materials Science and Engineering, Tiangong University, Tianjin 300387, People's Republic of China.

Resveratrol (RES) is a plant extract with excellent antioxidant, biocompatibility, anti-inflammatory and inhibition of platelet aggregation. RES-modified polysulfone (PSF) hemodialysis membranes have been fabricated using an immersion phase transformation method. The antioxidant properties of the blend membranes were evaluated in terms of their 2,2-diphenyl-1-picrylhydrazyl (DPPH) and 2,2'-azinobis-(3-ethylbenzothiazoline-6-sulfonate) (ABTS), reactive oxygen species (ROS) free radicals scavenging, total antioxidant capacity (T-AOC) of serum and lipid peroxidation inhibition. The observed results of decreasing DPPH and ABTS levels, scavenging ROS, significant inhibition of lipid peroxidation and improving the T-AOC of serum all contribute to the recovery of oxidative balance and the use of RES as an antioxidant modifier. The antioxidant stability of PSF/RES blend membranes was also studied. Moreover, the results of blood compatibility experiments showed that the addition of RES improved the blood compatibility of PSF membrane, inhibited the adhesion of red blood cells and platelets; inhibited complement activation; and reduced the blood cells deformation rate. The dialysis simulation experiment indicated that PSF/RES membrane (M-3) can clear 90.33% urea, 89.50% creatinine, 74.60% lysozyme and retention 90.47% BSA. All these results showed the new PSF/RES blend membranes have potential to be used in the field of hemodialysis to improve oxidative stress status in patients.
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http://dx.doi.org/10.1016/j.msec.2021.111953DOI Listing
April 2021

Risk factors on admission associated with hospital length of stay in patients with COVID-19: a retrospective cohort study.

Sci Rep 2021 03 31;11(1):7310. Epub 2021 Mar 31.

Department of Pharmacy, The First Affiliated Hospital of USTC, Division of Life Sciences and Medicine, University of Science and Technology of China, Hefei, Anhui, 230001, People's Republic of China.

Treating patients with COVID-19 is expensive, thus it is essential to identify factors on admission associated with hospital length of stay (LOS) and provide a risk assessment for clinical treatment. To address this, we conduct a retrospective study, which involved patients with laboratory-confirmed COVID-19 infection in Hefei, China and being discharged between January 20 2020 and March 16 2020. Demographic information, clinical treatment, and laboratory data for the participants were extracted from medical records. A prolonged LOS was defined as equal to or greater than the median length of hospitable stay. The median LOS for the 75 patients was 17 days (IQR 13-22). We used univariable and multivariable logistic regressions to explore the risk factors associated with a prolonged hospital LOS. Adjusted odds ratios (aORs) and 95% confidence intervals (CIs) were estimated. The median age of the 75 patients was 47 years. Approximately 75% of the patients had mild or general disease. The univariate logistic regression model showed that female sex and having a fever on admission were significantly associated with longer duration of hospitalization. The multivariate logistic regression model enhances these associations. Odds of a prolonged LOS were associated with male sex (aOR 0.19, 95% CI 0.05-0.63, p = 0.01), having fever on admission (aOR 8.27, 95% CI 1.47-72.16, p = 0.028) and pre-existing chronic kidney or liver disease (aOR 13.73 95% CI 1.95-145.4, p = 0.015) as well as each 1-unit increase in creatinine level (aOR 0.94, 95% CI 0.9-0.98, p = 0.007). We also found that a prolonged LOS was associated with increased creatinine levels in patients with chronic kidney or liver disease (p < 0.001). In conclusion, female sex, fever, chronic kidney or liver disease before admission and increasing creatinine levels were associated with prolonged LOS in patients with COVID-19.
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http://dx.doi.org/10.1038/s41598-021-86853-4DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8012638PMC
March 2021

Clinical translation and challenges of biodegradable magnesium-based interference screws in ACL reconstruction.

Bioact Mater 2021 Oct 12;6(10):3231-3243. Epub 2021 Mar 12.

School of Biomedical Engineering, Sun Yat-sen University, Guangzhou, 510006, China.

As one of the most promising fixators developed for anterior cruciate ligament (ACL) reconstruction, biodegradable magnesium (Mg)-based interference screws have gained increasing attention attributed to their appropriate modulus and favorable biological properties during degradation after surgical insertion. However, its fast degradation and insufficient mechanical strength have also been recognized as one of the major causes to limit their further application clinically. This review focused on the following four parts. Firstly, the advantages of Mg or its alloys over their counterparts as orthopaedic implants in the fixation of tendon grafts in ACL reconstruction were discussed. Subsequently, the underlying mechanisms behind the contributions of Mg ions to the tendon-bone healing were introduced. Thirdly, the technical challenges of Mg-based interference screws towards clinical trials were discussed, which was followed by the introduction of currently used modification methods for gaining improved corrosion resistance and mechanical properties. Finally, novel strategies including development of Mg/Titanium (Ti) hybrid fixators and Mg-based screws with innovative structure for achieving clinically customized therapies were proposed. Collectively, the advancements in the basic and translational research on the Mg-based interference screws may lay the foundation for exploring a new era in the treatment of the tendon-bone insertion (TBI) and related disorders.
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http://dx.doi.org/10.1016/j.bioactmat.2021.02.032DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7966853PMC
October 2021

Qinzhuliangxue mixture alleviates psoriasis-like skin lesions via inhibiting the IL6/STAT3 axis.

J Ethnopharmacol 2021 Mar 20;274:114041. Epub 2021 Mar 20.

Department of Dermatology, Shaanxi Hospital of Traditional Chinese Medicine, Xi'an 710003, China. Electronic address:

Ethnopharmacological Relevance: Psoriasis is a chronic inflammatory skin disease mediated by immunity. Our pre-clinical studies have proved that QZLX mixture can improve patients' clinical symptoms with psoriasis without noticeable adverse reactions. In a psoriasis-like mouse model induced by imiquimod, QZLX mixture has been shown to alleviate epidermal inflammation and inhibit the hyperproliferation of keratinocytes. However, its related molecular mechanism remains to be elucidated.

Aim Of The Study: To assess the mechanism of QZLX mixture against psoriasis.

Materials And Methods: This study combines network pharmacology and experiments to study the mechanism of QZLX against psoriasis. First, construct the active compound-target network and PPI network. Secondly, determine possible drug targets through Molecular docking and KEGG. Thirdly, high-performance liquid chromatography (HPLC) was used for the quality control of QZLX. Finally, use a mouse model of psoriasis to further confirm the role of QZLX.

Results: (1) Network pharmacology analysis shows that QZLX alleviates psoriasis's epidermal inflammation, and neovascularization may be achieved by inhibiting the IL6/STAT3 signaling pathway. (2) QZLX improves the pathological characteristics of IMQ-induced skin damage in psoriasis-like mice. (3) QZLX inhibits the IL6/STAT3 signaling pathway and reduces the expression of IL-17, IL-23, and TNF-α related to inflammation in peripheral blood, as well as the expression of S100A7 in the lesion area. QZLX is better than MTX in inhibiting neovascularization by down-regulating the expression of HIF-1 and CD31 in the lesion area. Finally, inhibition of Ki67 alleviates the excessive proliferation of keratinocytes.

Conclusion: In sum, this study clarifies the mechanism of QZLX against psoriasis and provides evidence to support its clinical use.
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http://dx.doi.org/10.1016/j.jep.2021.114041DOI Listing
March 2021

Prediction of Sepsis in COVID-19 Using Laboratory Indicators.

Front Cell Infect Microbiol 2020 2;10:586054. Epub 2021 Mar 2.

Department of Laboratory Medicine, Tongji Hospital, Tongji Medical College, Huazhong University of Science and Technology, Wuhan, China.

Background: The outbreak of coronavirus disease 2019 (COVID-19) has become a global public health concern. Many inpatients with COVID-19 have shown clinical symptoms related to sepsis, which will aggravate the deterioration of patients' condition. We aim to diagnose Viral Sepsis Caused by SARS-CoV-2 by analyzing laboratory test data of patients with COVID-19 and establish an early predictive model for sepsis risk among patients with COVID-19.

Methods: This study retrospectively investigated laboratory test data of 2,453 patients with COVID-19 from electronic health records. Extreme gradient boosting (XGBoost) was employed to build four models with different feature subsets of a total of 69 collected indicators. Meanwhile, the explainable Shapley Additive ePlanation (SHAP) method was adopted to interpret predictive results and to analyze the feature importance of risk factors.

Findings: The model for classifying COVID-19 viral sepsis with seven coagulation function indicators achieved the area under the receiver operating characteristic curve (AUC) 0.9213 (95% CI, 89.94-94.31%), sensitivity 97.17% (95% CI, 94.97-98.46%), and specificity 82.05% (95% CI, 77.24-86.06%). The model for identifying COVID-19 coagulation disorders with eight features provided an average of 3.68 (±) 4.60 days in advance for early warning prediction with 0.9298 AUC (95% CI, 86.91-99.04%), 82.22% sensitivity (95% CI, 67.41-91.49%), and 84.00% specificity (95% CI, 63.08-94.75%).

Interpretation: We found that an abnormality of the coagulation function was related to the occurrence of sepsis and the other routine laboratory test represented by inflammatory factors had a moderate predictive value on coagulopathy, which indicated that early warning of sepsis in COVID-19 patients could be achieved by our established model to improve the patient's prognosis and to reduce mortality.
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http://dx.doi.org/10.3389/fcimb.2020.586054DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7966961PMC
April 2021

Exosome-guided bone targeted delivery of Antagomir-188 as an anabolic therapy for bone loss.

Bioact Mater 2021 Sep 23;6(9):2905-2913. Epub 2021 Feb 23.

Department of Trauma Orthopedics, Changhai Hospital, Naval Medical University, Shanghai, 200433, China.

The differentiation shift from osteogenesis to adipogenesis of bone marrow mesenchymal stem cells (BMSCs) characterizes many pathological bone loss conditions. Stromal cell-derived factor-1 (SDF1) is highly enriched in the bone marrow for C-X-C motif chemokine receptor 4 (CXCR4)-positive hematopoietic stem cell (HSC) homing and tumor bone metastasis. In this study, we displayed CXCR4 on the surface of exosomes derived from genetically engineered NIH-3T3 cells. CXCR4 exosomes selectively accumulated in the bone marrow. Then, we fused CXCR4 exosomes with liposomes carrying antagomir-188 to produce hybrid nanoparticles (NPs). The hybrid NPs specifically gathered in the bone marrow and released antagomir-188, which promoted osteogenesis and inhibited adipogenesis of BMSCs and thereby reversed age-related trabecular bone loss and decreased cortical bone porosity in mice. Taken together, this study presents a novel way to obtain bone-targeted exosomes via surface display of CXCR4 and a promising anabolic therapeutic approach for age-related bone loss.
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http://dx.doi.org/10.1016/j.bioactmat.2021.02.014DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7917458PMC
September 2021

HIF1α epigenetically repressed macrophages via CRISPR/Cas9-EZH2 system for enhanced cancer immunotherapy.

Bioact Mater 2021 Sep 20;6(9):2870-2880. Epub 2021 Feb 20.

Department of Hematology, Tangdu Hospital, Fourth Military Medical University, Xi'an, 710038, People's Republic of China.

Immune suppressive microenvironment in tumor emerges as the main obstacle for cancer immunotherapy. In this study, we identified that HIF1 was activated in the tumor associated macrophages and acted as an important factor for the immune suppressive microenvironment. Epigenetically silencing of via histone H3 methylation in the promoter region was achieved by CRISPR/dCas9-EZH2 system, in which histone H3 methylase EZH2 was recruited to the promoter region specifically. The silenced macrophage, namely HERM ( Epigenetically Repressed Macrophage) manifested as inheritable tumor suppressing phenotype. In the subcutaneous B16-F10 melanoma syngeneic model, intratumoral injection of HERMs reprogrammed the immune suppressive microenvironment to the active one, reducing tumor burden and prolonging overall survival. Additionally, HERMs therapy remarkably inhibited tumor angiogenesis. Together, our study has not only identified a promising cellular and molecular target for reverting immune suppressive microenvironment, but also provided a potent strategy for reprogramming tumor microenvironment via epigenetically reprogrammed macrophages.
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http://dx.doi.org/10.1016/j.bioactmat.2021.02.008DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7905236PMC
September 2021

In vitro fertilization outcomes in women with polycystic ovary syndrome: A meta-analysis.

Eur J Obstet Gynecol Reprod Biol 2021 Apr 24;259:146-152. Epub 2021 Feb 24.

Prenatal Diagnosis Center, Department of Clinical Laboratory, Changning Maternity and Infant Health Hospital, East China Normal University, Shanghai, 200051, China.

Objective: During the past three decades, applying IVF for infertility treatment PCOS women has increased significantly, and the landscape of treatment strategies has changed dramatically. However, early review of IVF on PCOS have insufficiently accounted for efficacy and safety of the technic. With abundant studies in recent years, there is a need to reconcile these new data.

Material And Methods: To compare reproductive and obstetric outcomes of IVF between women with and without PCOS, a meta-analysis of 95 studies involving more than 21289 PCOS patients and 43036 controls was performed.

Results: Despite longer stimulation duration (WMD = 0.34 day, 95 % CI: 0.09, 0.59) and lower dose of Gn required (WMD = -361.3 IU, 95 % CI: -442.3, -280.4), more oocytes (WMD = 3.67, 95 % CI: 3.14-4.21) and matured oocytes (WMD = 2.16, 95 % CI: 1.52-2.80) per cycle were obtained from PCOS women. There were no statistically significant differences for cleavage, high-grade embryo and implantation rate. Although similar pregnancy and live birth rates per cycle were achieved in PCOS and non-PCOS women after IVF, women with PCOS still suffered from significantly increased risks of miscarriage (OR = 1.44, 95 % CI: 1.20-1.72), biochemical pregnancy loss (OR = 1.89, 95 % CI: 1.48-2.41), and OHSS (OR = 3.58, 95 % CI: 2.86-4.48), in addition to lower fertilization rate (OR = 0.79, 95 % CI: 0.71-0.88). Adverse obstetric outcomes including ectopics pregnancy and multiple pregnancies are comparable between two groups. The overall cycle cancellation rate was significantly higher among PCOS women with OR of 2.55 (95 % CI: 1.67-3.89), and concern over OHSS or hyper-response constitute the main cause. Similar results were also observed after stratified analysis.

Conclusions: Our results support the effectiveness of IVF for infertility treatment among PCOS patients. However, options to minimize adverse outcomes regarding to lower fertilization, miscarriage, biochemical pregnancy loss and OHSS are required. Further studies elucidating detailed mechanism underlying these adverse outcomes could be of great importance to improve the experience of IVF treatment.
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http://dx.doi.org/10.1016/j.ejogrb.2021.02.023DOI Listing
April 2021

Metabolic engineering of microorganisms for the production of multifunctional non-protein amino acids: γ-aminobutyric acid and δ-aminolevulinic acid.

Microb Biotechnol 2021 Mar 6. Epub 2021 Mar 6.

State Key Laboratory of Agrobiotechnology and Key Laboratory of Soil Microbiology, Ministry of Agriculture, College of Biological Sciences, China Agricultural University, No.2 Yuanmingyuan West Road, Haidian District, Beijing, 100193, China.

Gamma-aminobutyric acid (GABA) and delta-aminolevulinic acid (ALA), playing important roles in agriculture, medicine and other fields, are multifunctional non-protein amino acids with similar and comparable properties and biosynthesis pathways. Recently, microbial synthesis has become an inevitable trend to produce GABA and ALA due to its green and sustainable characteristics. In addition, the development of metabolic engineering and synthetic biology has continuously accelerated and increased the GABA and ALA yield in microorganisms. Here, focusing on the current trends in metabolic engineering strategies for microbial synthesis of GABA and ALA, we analysed and compared the efficiency of various metabolic strategies in detail. Moreover, we provide the insights to meet challenges of realizing industrially competitive strains and highlight the future perspectives of GABA and ALA production.
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http://dx.doi.org/10.1111/1751-7915.13783DOI Listing
March 2021

Effects of Replacing Ensiled-Alfalfa with Fresh-Alfalfa on Dynamic Fermentation Characteristics, Chemical Compositions, and Protein Fractions in Fermented Total Mixed Ration with Different Additives.

Animals (Basel) 2021 Feb 22;11(2). Epub 2021 Feb 22.

College of Grassland Science and Technology, China Agricultural University, Beijing 100193, China.

Alfalfa () is one of the high protein ingredients of fermented total mixed ration (FTMR). Additionally, FTMR is widely used to satisfy the nutrition requirements of animals. This study was conducted to confirm the fermentation characteristics, chemical compositions and protein fractions changes when replacing ensiled-alfalfa with fresh-alfalfa in FTMR with additives. Three additives were separately applied to fresh-alfalfa total mixed ration (TMR) and ensiled-alfalfa TMR, including molasses (MOL), (LP) and MOL plus LP (MOL+LP). The same volume of distilled water was sprayed onto the prepared TMR as performed for the control (CK). Each treatment included 18 repetitions and opened 3 repetitions at each fermenting day (1, 3, 7, 15, 30 and 60 d). The results showed that fresh-alfalfa FTMR (F-FTMR) exhibited slight changes in the fermentation characteristics during the first 7 d and showed similar trends in terms of the pH and organic acids content to ensiled-alfalfa FTMR (E-FTMR). The lactic acid contents of F-FTMR were significantly lower than those of E-FTMR at 60 d fermentation and the ammonia nitrogen contents were lower than E-FTMR during the entire fermenting period. The crude protein of the F-FTMR was enhanced after 60 d of fermenting. F-FTMR supplemented with MOL+LP exhibited a lower nonprotein nitrogen content, variable to slow protein and indigestible protein contents, and higher fast degradable protein and true protein degraded intermediately contents at 60 d fermenting, indicating that it effectively inhibited protein degradation.
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http://dx.doi.org/10.3390/ani11020572DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7926667PMC
February 2021

Optimal Fractional-Order Active Disturbance Rejection Controller Design for PMSM Speed Servo System.

Entropy (Basel) 2021 Feb 24;23(3). Epub 2021 Feb 24.

School of Engineering, University of California, 5200 N.Lake Road, Merced, CA 95343, USA.

In this paper, a fractional-order active disturbance rejection controller (FOADRC), combining a fractional-order proportional derivative (FOPD) controller and an extended state observer (ESO), is proposed for a permanent magnet synchronous motor (PMSM) speed servo system. The global stable region in the parameter (, )-space corresponding to the observer bandwidth ωo can be obtained by D-decomposition method. To achieve a satisfied tracking and anti-load disturbance performance, an optimal ADRC tuning strategy is proposed. This tuning strategy is applicable to both FOADRC and integer-order active disturbance rejection controller (IOADRC). The tuning method not only meets user-specified frequency-domain indicators but also achieves a time-domain performance index. Simulation and experimental results demonstrate that the proposed FOADRC achieves better speed tracking, and more robustness to external disturbance performances than traditional IOADRC and typical Proportional-Integral- Derivative (PID) controller. For example, the JITAE for speed tracking of the designed FOADRC are less than 52.59% and 55.36% of the JITAE of IOADRC and PID controller, respectively. Besides, the JITAE for anti-load disturbance of the designed FOADRC are less than 17.11% and 52.50% of the JITAE of IOADRC and PID controller, respectively.
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http://dx.doi.org/10.3390/e23030262DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7995987PMC
February 2021

Correction: Yan, L., et al. Combined Taurine, Epigallocatechin Gallate and Genistein Therapy Reduces HSC-T6 Cell Proliferation and Modulates the Expression of Fibrogenic Factors. 2013, , 20543-20554.

Int J Mol Sci 2021 Feb 26;22(5). Epub 2021 Feb 26.

Medical Scientific Research Center, Guangxi Medical University, Nanning 530021, China.

The authors regret that, during the preparation of our published manuscript "Combined taurine, epigallocatechin gallate and genistein therapy reduces HSC-T6 cell proliferation and modulates the expression of fibrogenic factors" [...].
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http://dx.doi.org/10.3390/ijms22052343DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7956543PMC
February 2021

Meta-analysis on current status, efficacy, and safety of laparoscopic and robotic ventral mesh rectopexy for rectal prolapse treatment: can robotic surgery become the gold standard?

Int J Colorectal Dis 2021 Mar 1. Epub 2021 Mar 1.

Institute of Hepatobiliary Disease, Tianjin Third Center Hospital, No.83, Jintang Road, Hedong District, Tianjin, 300170, China.

Purpose: Robotic-assisted surgery and robotic-assisted ventral mesh rectopexy are gaining attention in the treatment of rectal prolapse and increased positive findings are proposed. The objective of this meta-analysis was to investigate whether robotic-assisted ventral mesh rectopexy is comparable with the conventional laparoscopic approach surgery.

Methods: Five major databases (PubMed, Sciencedirect, Web of Science, Embase, and Cochrane Library) were searched for eligible studies. Observational studies of the effect and safety of robotic-assisted and laparoscopic approaches on ventral mesh rectopexy were included. Odd ratios (OR) and weight mean difference (WMD) were used for dichotomous data and continuous data analysis. Clinical outcomes, functional outcomes, and cost-effectiveness data were extracted for meta-analysis.

Results: Compared to the laparoscopic approach, a significant shorter length of hospital stay (LOS), lesser intraoperative blood loss, and lower post-operative complication rate of RVMR group were observed. However, operation time of RVMR was significant increased. The expense of RVMR was higher than LVMR; mean Wexner scores and fecal incontinence were lower in RVMR group while there were no statistical differences.

Conclusion: The result of the current analysis revealed that the robotic-assisted ventral mesh rectopexy is effective and feasible in the treatment of rectal prolapse. However, long-term follow-up and results are needed for the promotion of this approach. There is a long way for robotic-assisted surgery to become a gold standard in rectal surgery.
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http://dx.doi.org/10.1007/s00384-021-03885-yDOI Listing
March 2021

Size controlled fabrication of enzyme encapsulated amorphous calcium phosphate nanoparticle and its intracellular biosensing application.

Colloids Surf B Biointerfaces 2021 May 18;201:111638. Epub 2021 Feb 18.

College of Pharmacy, School of Medicine, Hangzhou Normal University, China. Electronic address:

Inorganic-enzyme composites have been widely used for applications in catalysis and analytical science. Amorphous calcium phosphate, as a biocompatible material, can form open hydrated structure to encapsulate and protect enzymes. So far, there have been few progress on size-adjustable amorphous calcium phosphate nanoparticles since the diameter controllability is limited by its natural aggregation characteristics. By co-precipitation and nano-channel extrusion, we developed enzyme-loaded amorphous calcium phosphate nanoparticles with adjustable diameters. These enzyme-loaded particles showed high thermal and chemical stability as well as biocompatibility. The nano-sized enzyme-loaded particles can further expand their application fields and be used as intracellular enzyme probes. Delivering glucose oxidase enzyme by amorphous calcium phosphate nanoparticles enables fluorescent monitoring of glucose levels in living cells, which can be used to study the metabolism rates of cancer cells and normal cells. The nano-channel extrusion method can also be used as a template to encapsulate different kinds of enzymes to expand catalysis and biosensing applications.
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http://dx.doi.org/10.1016/j.colsurfb.2021.111638DOI Listing
May 2021

Point-of-Care Monitoring of Colitis Using Intestinal Alkaline Phosphatase in Inflammatory Bowel Disease.

ACS Sens 2021 03 26;6(3):698-702. Epub 2021 Feb 26.

Department of Chemistry, Georgia State University 788 Petit Science Center, Atlanta, Georgia 30302, United States.

Intestinal Alkaline Phosphatase (IAP) was investigated as a potential biomarker to monitor colitis in a mouse model of Inflammatory Bowel Disease (IBD). We developed a Point-Of-Care (POC) assay to detect IAP with a glucose meter in 15 min. We synthesized a paracetamol-bearing compound specifically cleaved by IAP to release paracetamol, which can be detected with a personal glucometer. Interleukin 10 deficient (IL 10-/-) mouse model samples were used to compare the IAP level in mice with mild or severe colitis. The results showed that fecal IAP level was significantly lower in each mouse sample with severe colitis than with mild colitis. Mice treated with anti-Tumor Necrosis Factor-alpha (anti-TNF-α) to decrease inflammation exhibited a much higher level of IAP than those without treatment (IAP levels from anti-TNF-α treated vs nontreated = 2.80 U vs 0.11 U, < 0.0001). Taken together, IAP can be considered as a potential biomarker to monitor colitis, and a rapid, user-friendly POC glucometer-based assay can be potentially used to monitor colitis levels and inflammation flareups in IBD.
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http://dx.doi.org/10.1021/acssensors.0c02177DOI Listing
March 2021

The Distinct Function of p21 With p16 in Modulating Aging Phenotypes of Werner Syndrome by Affecting Tissue Homeostasis.

Front Genet 2021 5;12:597566. Epub 2021 Feb 5.

Laboratory of Molecular Genetics of Aging & Tumor, Medical School, Kunming University of Science and Technology, Kunming, China.

Human Werner syndrome (WS) is an autosomal recessive progeria disease. A mouse model of WS manifests the disease through telomere dysfunction-induced aging phenotypes, which might result from cell cycle control and cellular senescence. Both p21 (p21, encoded by the gene) and p16 (p16, encoded by the gene) are cell cycle inhibitors and are involved in regulating two key pathways of cellular senescence. To test the effect of p21 and p16 deficiencies in WS, we crossed WS mice (DKO) with or mice to construct triple knockout (p21-TKO or p16-TKO) mice. By studying the survival curve, bone density, regenerative tissue (testis), and stem cell capacity (intestine), we surprisingly found that p21-TKO mice displayed accelerated premature aging compared with DKO mice, while p16-TKO mice showed attenuation of the aging phenotypes. The incidence of apoptosis and cellular senescence were upregulated in p21-TKO mice tissue and downregulated in p16-TKO mice. Surprisingly, cellular proliferation in p21-TKO mice tissue was also upregulated, and the p21-TKO mice did not show telomere shortening compared with age-matched DKO mice, although p16-TKO mice displayed obvious enhancement of telomere lengthening. Consistent with these phenotypes, the SIRT1-PGC1 pathway was upregulated in p16-TKO but downregulated in p21-TKO compared with DKO mouse embryo fibroblasts (MEFs). However, the DNA damage response pathway was highly activated in p21-TKO, but rescued in p16-TKO, compared with DKO MEFs. These data suggest that p21 protected the stem cell reservoir by regulating cellular proliferation and turnover at a proper rate and that p21 loss in WS activated fairly severe DNA damage responses (DDR), which might cause an abnormal increase in tissue homeostasis. On the other hand, p16 promoted cellular senescence by inhibiting cellular proliferation, and p16 deficiency released this barrier signal without causing severe DDR.
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http://dx.doi.org/10.3389/fgene.2021.597566DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7901894PMC
February 2021

Cost-effectiveness of paclitaxel, doxorubicin, cyclophosphamide and trastuzumab versus docetaxel, cisplatin and trastuzumab in new adjuvant therapy of breast cancer in china.

Cost Eff Resour Alloc 2021 Feb 23;19(1):11. Epub 2021 Feb 23.

Department of Pharmacy, Hangzhou First People's Hospital, School of Medicine, Zhejiang University, Hangzhou, 310006, China.

Background: Breast cancer is the most common cancer among women in China. Amplification of the Human epidermal growth factor receptor type 2 (HER2) gene is present and overexpressed in 18-20% of breast cancers and historically has been associated with inferior disease-related outcomes. There has been increasing interest in de-escalation of therapy for low-risk disease. This study analyzes the cost-effectiveness of Doxorubicin/ Cyclophosphamide/ Paclitaxel/ Trastuzumab (AC-TH) and Docetaxel/Carboplatin/Trastuzumab(TCH) from payer perspective over a 5 year time horizon.

Methods: A half-cycle corrected Markov model was built to simulate the process of breast cancer events and death occurred in both AC-TH and TCH armed patients. Cost data came from studies based on a Chinese hospital. One-way sensitivity analyses as well as second-order Monte Carlo and probabilistic sensitivity analyses were performed.The transition probabilities and utilities were extracted from published literature, and deterministic sensitivity analyses were conducted.

Results: We identified 41 breast cancer patients at Hangzhou First People's Hospital, among whom 15 (60%) had a partial response for AC-TH treatment and 13 (81.25%) had a partial response for TCH treatment.No cardiac toxicity was observed. Hematologic grade 3 or 4 toxicities were observed in 1 of 28 patients.Nonhematologic grade 3 or 4 toxicities with a reverse pattern were observed in 6 of 29 patients. The mean QALY gain per patient compared with TCH was 0.25 with AC-TH, while the incremental costs were $US13,142. The incremental cost-effectiveness ratio (ICER) of AC-TH versus TCH was $US 52,565 per QALY gained.

Conclusions: This study concluded that TCH neoadjuvant chemotherapy was feasible and active in HER2-overexpressing breast cancer patients in terms of the pathological complete response, complete response, and partial response rates and manageable toxicities.
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http://dx.doi.org/10.1186/s12962-021-00264-wDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7901219PMC
February 2021

Quantitative assessment of SARS-CoV-2 RNAemia and outcome in patients with coronavirus disease 2019.

J Med Virol 2021 05 1;93(5):3165-3175. Epub 2021 Mar 1.

Prenatal Diagnosis Center, Department of Clinical Laboratory, Changning Maternity and Infant Health Hospital, East China Normal University, Shanghai, China.

The disease spectrum of coronavirus disease 2019 (COVID-19) varies from asymptomatic infection to critical illness and death. Identification of prognostic markers is vital for predicting progression and clinical practice. Severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) RNA, known as RNAemia, has been detected in the blood. However, the potential clinical value of SARS-CoV-2 RNAemia remains unknown. We, therefore, conducted a meta-analysis using a random-effects model to estimate the pooled prevalence of SARS-CoV-2 RNAemia as well as summary strength of RNAemia in association with disease severity and unfavorable clinical outcomes. A total of 21 studies involving 2181 patients were included. SARS-CoV-2 RNAemia in COVID-19 patients varied from 9.4% to 74.1%, with a pooled estimate of 34% (95% confidene interval [CI]: 26%-43%). Overall, SARS-CoV-2 RNAemia was associated with COVID-19 severity with odds ratio (OR) of 5.43 (95% CI: 3.46-8.53). In addition, SARS-CoV-2 RNAemia was a significant risk factor for unfavorable clinical outcomes (OR = 6.54, 95% CI: 3.82-11.21). The summary OR was 4.28 (95% CI: 2.20-8.33) for intensive care unit (ICU) admission, 11.07 (95% CI: 5.60-21.88) for mortality. Furthermore, RNAemia was also a significant risk factor for invasive mechanical ventilation and multiple organ failure. SARS-CoV-2 RNAemia is associated with disease severity, ICU admission, death in COVID-19, and may serve as a clinical predictor. More prospective trials in evaluating the potential of SARS-CoV-2 RNAemia as a prognostic indicator are necessary.
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http://dx.doi.org/10.1002/jmv.26876DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8014647PMC
May 2021

Learning From Architectural Redundancy: Enhanced Deep Supervision in Deep Multipath Encoder-Decoder Networks.

IEEE Trans Neural Netw Learn Syst 2021 Feb 15;PP. Epub 2021 Feb 15.

Deep encoder-decoders are the model of choice for pixel-level estimation due to their redundant deep architectures. Yet they still suffer from the vanishing supervision information issue that affects convergence because of their overly deep architectures. In this work, we propose and theoretically derive an enhanced deep supervision (EDS) method which improves on conventional deep supervision (DS) by incorporating variance minimization into the optimization. A new structure variance loss is introduced to build a bridge between deep encoder-decoders and variance minimization, and provides a new way to minimize the variance by forcing different intermediate decoding outputs (paths) to reach an agreement. We also design a focal weighting strategy to effectively combine multiple losses in a scale-balanced way, so that the supervision information is sufficiently enforced throughout the encoder-decoders. To evaluate the proposed method on the pixel-level estimation task, a novel multipath residual encoder is proposed and extensive experiments are conducted on four challenging density estimation and crowd counting benchmarks. The experimental results demonstrate the superiority of our EDS over other paradigms, and improved estimation performance is reported using our deeply supervised encoder-decoder.
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http://dx.doi.org/10.1109/TNNLS.2021.3056384DOI Listing
February 2021

Sequential cocatalyst decoration on BaTaON towards highly-active Z-scheme water splitting.

Nat Commun 2021 Feb 12;12(1):1005. Epub 2021 Feb 12.

Research Initiative for Supra-Materials, Interdisciplinary Cluster for Cutting Edge Research, Shinshu University, Nagano-shi, Nagano, Japan.

Oxynitride photocatalysts hold promise for renewable solar hydrogen production via water splitting owing to their intense visible light absorption. Cocatalyst loading is essential for activation of such oxynitride photocatalysts. However, cocatalyst nanoparticles form aggregates and exhibit weak interaction with photocatalysts, which prevents eliciting their intrinsic photocatalytic performance. Here, we demonstrate efficient utilization of photoexcited electrons in a single-crystalline particulate BaTaON photocatalyst prepared with the assistance of RbCl flux for H evolution reactions via sequential decoration of Pt cocatalyst by impregnation-reduction followed by site-selective photodeposition. The Pt-loaded BaTaON photocatalyst evolves H over 100 times more efficiently than before, with an apparent quantum yield of 6.8% at the wavelength of 420 nm, from a methanol aqueous solution, and a solar-to-hydrogen energy conversion efficiency of 0.24% in Z-scheme water splitting. Enabling uniform dispersion and intimate contact of cocatalyst nanoparticles on single-crystalline narrow-bandgap particulate photocatalysts is a key to efficient solar-to-chemical energy conversion.
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http://dx.doi.org/10.1038/s41467-021-21284-3DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7881033PMC
February 2021

Chinese Herbal Medicine for Psoriasis: Evidence From 11 High-Quality Randomized Controlled Trials.

Front Pharmacol 2020 22;11:599433. Epub 2021 Jan 22.

Department of Dermatology, Yueyang Hospital of Integrated Traditional Chinese and Western Medicine, Shanghai University of Traditional Chinese Medicine, Shanghai, China.

Chinese herbal medicine (CHM) provides a theoretical basis for the treatment of psoriasis with considerable benefits and a low toxicity. The purpose of this quantitative study was to show high-quality evidence of the efficacy and safety of CHM for the treatment of psoriasis to promote its clinical application. Several databases were systematically searched including PubMed, Embase, Cochrane Central Register of Controlled Trials, China Network Knowledge Infrastructure, Chinese Scientific Journals Database, and Wan Fang Database. High-quality randomized controlled trials that compared CHM with non-CHM interventions were included. The RevMan5.3 software was used to calculate risk ratios (RR) at 95% confidence intervals (CI) and conduct the meta-analysis. Altogether, 1,215 patients participated in this study, including 711 in the experimental group and 504 in the control group. The psoriasis area severity index (PASI) score of the CHM group was significantly lower than that of the placebo group (MD, -4.02; 95% CI, -6.71 to -1.34; = 0.003). To achieve PASI-60 and PASI-75, the arrival rate of the CHM group was higher than that of the placebo group (PASI-60: RR, 3.52; 95% CI, 1.17 to 10.61; = 0.03; PASI-75: RR, 9.87; 95% CI, 3.11 to 31.31; = 0.0001). Furthermore, the efficacy rate was higher in patients receiving CHM than in those receiving placebo (RR, 1.72; 95% CI, 1.01 to 2.93; = 0.04). The results suggested a greater impact of CHM in improving the dermatology life quality index (DLQI) of patients (MD, -2.12; 95% CI, -3.75 to -0.49; = 0.01). Regarding pruritus severity, there was no significant difference between the two groups (MD, -1.90; 95% CI, -3.79 to -0.01; = 0.05). The meta-analysis revealed that the recurrence rate (RR, 0.74; 95% CI, 0.32 to 1.71; = 0.48) and proportion of adverse events (RR, 1.36; 95% CI, 0.95 to 1.93; = 0.09) associated with using CHM were similar to those associated with using a placebo. CHM appears safe and effective in the treatment of psoriasis and has a great positive impact on the DQLI of patients; however, CHM could not completely eliminate skin lesions, improve pruritus severity, and reduce the recurrence rate.
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http://dx.doi.org/10.3389/fphar.2020.599433DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7862748PMC
January 2021

Optimal robust fractional order PID controller synthesis for first order plus time delay systems.

ISA Trans 2021 Jan 8. Epub 2021 Jan 8.

School of Engineering, University of California, 5200 N.Lake Road, Merced, CA, 95343 USA.

In this paper, a practical and systematic tuning procedure combining both frequency-domain (FD) and time-domain (TD) specifications is proposed to obtain an optimal robust fractional order (FO) PID (FOPID) controller for the first order plus time delay (FOPTD) processes. The FD specifications (i.e. phase margin (PM), gain crossover frequency (ω) and flat phase constrain (FPC)) guarantee the systemic stability and robustness to plant gain variations. Meanwhile, the TD specification (i.e. the smallest J) achieves optimal dynamic performance. Furthermore, the entire feasible regions of two frequency-domain specifications ω and PM have been obtained with a synthesis scheme and visualized in three-dimensional plots which can be used as prior knowledge before the controller design. The comparisons of feasible region with FOPI and integer order PID (IOPID) controllers clearly present the superiority of proposed FOPID controller. Simulation illustration for delay dominant systems, lag dominant systems and high order system with one zero, using the proposed optimal robust FOPID controller is presented to demonstrate the significant performance improvement over FOPI controller, three-parameter FOPID controller, Ziegler-Nichols FOPID controller, fractional filter-FOPID controller and SIMC-PI controller.
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http://dx.doi.org/10.1016/j.isatra.2020.12.043DOI Listing
January 2021

A Simplified Fractional Order PID Controller's Optimal Tuning: A Case Study on a PMSM Speed Servo.

Entropy (Basel) 2021 Jan 20;23(2). Epub 2021 Jan 20.

School of Automation Science and Engineering, South China University of Technology, 381 Wushan Road, Guangzhou 510641, China.

A simplified fractional order PID (FOPID) controller is proposed by the suitable definition of the parameter relation with the optimized changeable coefficient. The number of the pending controller parameters is reduced, but all the proportional, integral, and derivative components are kept. The estimation model of the optimal relation coefficient between the controller parameters is established, according to which the optimal FOPID controller parameters can be calculated analytically. A case study is provided, focusing on the practical application of the simplified FOPID controller to a permanent magnet synchronous motor (PMSM) speed servo. The dynamic performance of the simplified FOPID control system is tested by motor speed control simulation and experiments. Comparisons are performed between the control systems using the proposed method and those using some other existing methods. According to the simulation and experimental results, the simplified FOPID control system achieves the optimal dynamic performance. Therefore, the validity of the proposed controller structure and tuning method is demonstrated.
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http://dx.doi.org/10.3390/e23020130DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7908999PMC
January 2021

A non-linear dose-response relation of female body mass index and in vitro fertilization outcomes.

J Assist Reprod Genet 2021 Jan 26. Epub 2021 Jan 26.

Prenatal Diagnosis Center, Department of Clinical Laboratory, Changning Maternity and Infant Health Hospital, East China Normal University, #786 Yuyuan Road, Shanghai, 200051, China.

Purpose: Obesity, measured by body mass index (BMI), is implicated in adverse pregnancy outcomes for women seeking in vitro fertilization (IVF) care. However, the shape of the dose-response relationship between BMI and IVF outcomes remains unclear.

Methods: We therefore conducted a dose-response meta-analysis using a random effects model to estimate summary relative risk (RR) for clinical pregnancy (CPR), live birth (LBR), and miscarriage risk (MR) after IVF.

Results: A total of 18 cohort-based studies involving 975,889 cycles were included. For each 5-unit increase in BMI, the summary RR was 0.95 (95% CI: 0.94-0.97) for CPR, 0.93 (95% CI: 0.92-0.95) for LBR, and 1.09 (95% CI: 1.05-1.12) for MR. There was evidence of a non-linear association between BMI and CPR (P < 10) with CPR decreasing sharply among obese women (BMI > 30). Non-linear dose-response meta-analysis showed a relatively flat curve over a broad range of BMI from 16 to 30 for LBR (P = 0.0009). In addition, we observed a J-shaped association between BMI and MR (P = 0.006) with the lowest miscarriage risk observed with a BMI of 22-25.

Conclusions: In conclusion, obesity contributed to increased risk of adverse IVF outcomes in a non-linear dose-response manner. More prospective trials in evaluating the effect of body weight control are necessary.
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http://dx.doi.org/10.1007/s10815-021-02082-8DOI Listing
January 2021

Correction to: Indole hydrazide compound ZJQ-24 inhibits angiogenesis and induces apoptosis cell death through abrogation of AKT/mTOR pathway in hepatocellular carcinoma.

Cell Death Dis 2021 Jan 25;12(1):124. Epub 2021 Jan 25.

Laboratory of Molecular Genetics of Aging and Tumor, Medical School, Kunming University of Science and Technology, Kunming, 650500, PR China.

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http://dx.doi.org/10.1038/s41419-021-03388-2DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7835225PMC
January 2021

Rapid, user-friendly, and inexpensive detection of azidothymidine.

Anal Bioanal Chem 2021 Mar 23;413(7):1999-2006. Epub 2021 Jan 23.

788 Petit Science Center, Department of Chemistry, Center for Diagnostics and Therapeutics, Georgia State University, 161 Jesse Hill Jr. Drive, Atlanta, GA, 30302, USA.

Strict adherence to highly active antiretroviral therapy (HAART) is very important to improve the quality of life for HIV-positive patients to reduce new infections and determine treatment success. Azidothymidine (AZT) is an antiretroviral drug commonly used in HAART treatment. In this research, an "add, mix, and measure" assay was developed to detect AZT within minutes. Three different probes designed to release fluorophores when samples containing AZT are added were synthesized and characterized. The limit of detection to AZT in simulated urine samples was determined to be 4 μM in 5 min for one of the probes. This simple and rapid point-of-care test could potentially be used by clinicians and health care workers to monitor the presence of AZT in low resource settings.
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http://dx.doi.org/10.1007/s00216-021-03168-zDOI Listing
March 2021

The role of macrophage in regulating tumour microenvironment and the strategies for reprogramming tumour-associated macrophages in antitumour therapy.

Eur J Cell Biol 2021 Mar 13;100(2):151153. Epub 2021 Jan 13.

Faculty of Life Science and Technology, Kunming University of Science and Technology, Kunming, 650500, PR China; Guizhou Provincial Key Laboratory & Drug Development on Common Disease, School of Basic Medicine, Guizhou Medical University, Guiyang, Guizhou, China. Electronic address:

Tumour-associated macrophages (TAMs) that present abundantly in the tumour microenvironment (TME) exhibit a protumour property, such as promoting genetic instability, tumour metastasis and immunosuppression. Macrophage-targeted therapeutic approaches hence have been applied and shown their significances in the process of tumour immune treatment, including blocking TAM recruitment, depleting or transforming TAMs that already exist in the tumour site. Here, we summarized the functional regulation of TAMs in the respects of hypoxia environment, metabolism in the tumour microenvironment and the transcription factors involved. We reviewed the strategies for transforming TAMs, including immune stimuli targeting TAMs, inhibitors against TAMs, pathogen or irradiation stimulation on TAMs, and the application of natural compounds in TAMs. Furthermore, we also discussed the macrophage-targeted therapies in the clinical studies. Taken together, this review tries to shed light on the TAM regulation and the main strategies of TAM reprogramming for an enhanced immune surveillance.
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http://dx.doi.org/10.1016/j.ejcb.2021.151153DOI Listing
March 2021

LINC00538 promotes the progression of colon cancer through inhibiting NKD2 expression.

J BUON 2020 Nov-Dec;25(6):2657-2664

School of Basic Medicine, Youjiang Medical University for Nationalities, Baise, China.

Purpose: The purpose of this study was to explore the possible role and mechanism of LINC00538 in the pathogenesis of colon cancer.

Methods: The expression levels of LINC00538 in 70 pairs of colon cancer tissue samples and adjacent ones were examined by qRT-PCR, and survival analysis of patients was performed according to the result. Meanwhile, colon cancer cell lines were screened. In addition, LINC00538 siRNA was transfected into colon cancer cells using liposome method, and then cell proliferation and cell cycle were examined by CCK8 and EDU assays, while cell apoptosis was detected by flow cytometry. Finally, the mechanism of LINC00538 in colon cancer was further explored by RNA-binding protein immunoprecipitation and chromatin immunoprecipitation.

Results: The expression of LINC00538 in colon cancer tissues was remarkably higher than that in normal ones, and the overall survival of patients with colon cancer was negatively correlated with the expression of LINC00538. After transfection of LINC00538 siRNA, the proliferation rate of colon cancer cell lines including HCT116 and RKO cells was weakened, the S phase of the cell cycle was shortened, while the cell apoptosis was elevated. In addition, further mechanism studies demonstrated that LINC00538 can bind to EZH2 and inhibit the expression of NKD2, thereby regulating the proliferation and apoptosis of colon cancer cells.

Conclusions: This study demonstrated for the first time that LINC00538 was highly expressed in colon cancer and was associated with poor prognosis of patients. Knockdown of LINC00538 in colon cancer cell lines was able to inhibit the cell proliferation and cell cycle, while it promoted the apoptosis. It's mechanism of participating in the development of colon cancer may be through the down-regulation of NKD2 and the regulation of EZH2.
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January 2021

Hydride Affinities for Main-Group Hydride Reductants: Assessment of Density Functionals and Trends in Reactivities.

J Phys Chem A 2021 Jan 15;125(3):835-842. Epub 2021 Jan 15.

Graduate School of Engineering, Nagasaki University, Bunkyo 1-14, Nagasaki-shi, Nagasaki 852-8521, Japan.

In the present study, we have examined hydride affinities relevant to a range of group 13 and group 14 reductants. We use the high-level W1X-G0, G4(MP2)-XK, and DSD-PBEP86 methods to obtain the RHA42 set of accurate reductant hydride affinities. Assessment of DFT methods with the RHA42 set shows that all functionals that we have examined are fairly accurate. Overall, we find ωB97X-V to be the most accurate. The MN12-SX screened-exchange functional and the nonhybrid B97-D3BJ method also perform well, and they may provide a lower-cost means for obtaining hydride affinities. The trend in the hydride affinities suggests an increased reducing power when one moves down the periodic table, e.g., with TlH being a stronger reductant than BH. We also find that group 13 hydrides are stronger reductants than the group 13 analogues. In general, substitution of a hydrogen, e.g., BH → BHMe, and the formation of dimer, e.g., BH → BH, also lead to stronger reductants. A notable observation is the small hydride affinities for silyl cations, which are indicative of the potential of silanes as strong reducing agents. In particular, poly(methylhydrosiloxane) (PMHS) cations are associated with especially small hydride affinities owing to the presence of intramolecular oxygen atoms that can stabilize the cation center. We have further found the germanium analogues of the silanes to be more reactive, and they may further widen the scope of main-group hydride reducing agents.
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http://dx.doi.org/10.1021/acs.jpca.0c10543DOI Listing
January 2021