Publications by authors named "Jingquan Liu"

170 Publications

Self-adaptive cardiac optogenetics device based on negative stretching-resistive strain sensor.

Sci Adv 2021 Nov 24;7(48):eabj4273. Epub 2021 Nov 24.

National Key Laboratory of Science and Technology on Micro/Nano Fabrication, Shanghai Jiao Tong University, Shanghai 200240, China.

[Figure: see text].
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http://dx.doi.org/10.1126/sciadv.abj4273DOI Listing
November 2021

Specific sensing of resorcin based on the hierarchical porous nanoprobes constructed by cuttlefish-derived biomaterials through differential pulse voltammetry.

Anal Chim Acta 2021 Dec 21;1188:339203. Epub 2021 Oct 21.

College of Materials Science and Engineering, Institute for Graphene Applied Technology Innovation, Qingdao University, Qingdao, 266071, China. Electronic address:

The specific detection of resorcin from its isomers is a current research hotspot. Thus in our work, a ternary hierarchical porous nanoprobe has been constructed based on the combination of cuttlefish ink and bimetallic [email protected] nanoclusters for the specific sensing of resorcin. Briefly, through electrostatic interaction, [email protected] core-shell nanoclusters are immobilized on the surface of polydopamine extracted from cuttlefish, which is turned into nitrogen-doped porous carbon functionalized by bimetallic [email protected] by topological transformation subsequently. Afterward, an electrochemical sensor is fabricated based on the nanoprobes for specifically determining resorcin in solution by differential pulse voltammetry, and the linear detection ranges of the sensor are 1-100 μM and 1.2-4 mM while the detection limit reaches 0.06 μM. Meanwhile, the sensing mechanism of resorcin by the pre-fabricated sensor is detailedly studied by density functional theory to obtain a clear electrochemical process. Besides, the selectivity, stability, plus reproducibility of the pre-fabricated sensor have been also tested, and the determinations for resorcin in real environmental water samples have also been performed with good recoveries, revealing the auspicious application potential in the environmental monitoring.
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http://dx.doi.org/10.1016/j.aca.2021.339203DOI Listing
December 2021

Dense Packed Drivable Optrode Array for Precise Optical Stimulation and Neural Recording in Multiple-Brain Regions.

ACS Sens 2021 Nov 15;6(11):4126-4135. Epub 2021 Nov 15.

National Key Laboratory of Science and Technology on Micro/Nano Fabrication, Shanghai Jiao Tong University, Shanghai 200240, China.

The input-output function of neural networks is complicated due to the huge number of neurons and synapses, and some high-density implantable electrophysiology recording tools with a plane structure have been developed for neural circuit studies in recent years. However, traditional plane probes are limited by the record-only function and inability to monitor multiple-brain regions simultaneously, and the complete cognition of neural networks still has a long way away. Herein, we develop a three-dimensional (3D) high-density drivable optrode array for multiple-brain recording and precise optical stimulation simultaneously. The optrode array contains four-layer probes with 1024 microelectrodes and two thinned optical fibers assembled into a 3D-printed drivable module. The recording performance of microelectrodes is optimized by electrochemical modification, and precise implantation depth control of drivable optrodes is verified in agar. Moreover, in vivo experiments indicate neural activities from CA1 and dentate gyrus regions are monitored, and a tracking of the neuron firing for 2 weeks is achieved. The suppression of neuron firing by blue light has been realized through high-density optrodes during optogenetics experiments. With the feature of large-scale recording, optoelectronic integration, and 3D assembly, the high-density drivable optrode array possesses an important value in the research of brain diseases and neural networks.
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http://dx.doi.org/10.1021/acssensors.1c01650DOI Listing
November 2021

Scalable Fabrication of TiCT MXene/RGO/Carbon Hybrid Aerogel for Organics Absorption and Energy Conversion.

ACS Appl Mater Interfaces 2021 Nov 25;13(43):51333-51342. Epub 2021 Oct 25.

Institute for Frontier Materials, Deakin University, Geelong, Victoria 3216, Australia.

High aspect ratio two-dimensional TiCT MXene flakes with extraordinary mechanical, electrical, and thermal properties are ideal candidates for assembling elastic and conductive aerogels. However, the scalable fabrication of large MXene-based aerogels remains a challenge because the traditional preparation method relies on supercritical drying techniques such as freeze drying, resulting in poor scalability and high cost. Herein, the use of porous melamine foam as a robust template for MXene/reduced graphene oxide aerogel circumvents the volume shrinkage during its natural drying process. Through this approach, we were able to produce large size (up to 600 cm) MXene-based aerogel with controllable shape. In addition, the aerogels possess an interconnected cellular structure and display resilience up to 70% of compressive strain. Some key features also include high solvent absorption capacity (∼50-90 g g), good photothermal conversion ability (an average evaporation rate of 1.48 kg m h for steam generation), and an excellent electrothermal conversion rate (1.8 kg m h at 1 V). More importantly, this passive drying process provides a scalable, convenient, and cost-effective approach to produce high-performance MXene-based aerogels, demonstrating the feasibility of commercial production of MXene-based aerogels toward practical applications.
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http://dx.doi.org/10.1021/acsami.1c13808DOI Listing
November 2021

In Situ Synthesis of CoCeS Bimetallic Sulfide Nanoparticles on a Bi-Pyrene Terminated Molecular Wire Modified Graphene Surface for Supercapacitors.

Chemistry 2021 Oct 14. Epub 2021 Oct 14.

College of Materials Science and Engineering Institute for Graphene Applied Technology Innovation Collaborative Innovation Centre for Marine Biomass Fibers Materials and Textiles of Shandong Province, Qingdao University, Qingdao, 266071, China.

The excellent electrical conductivity of graphene is due to its highly-conjugated structures. Manipulation of the electronic and mechanical properties of graphene can be achieved by controlling the destruction of its in-sheet conjugation system. Herein, we report the preparation of CoCeS [email protected]@RGO through π-π stacking interactions at the molecular level. In this study, sodium alginate was reacted with Co and Ce , and the composite was loaded onto a graphene surface. The graphene sheets were prepared using a bi-pyrene terminated molecular wire (BPMW) to avoid re-stacking of the grapheme sheets, thereby forming nanoscale spaces between sheets. The angle between the BPMW coplanar pyrene group and the phenyl group was 33.2°, and the graphene layer is supported in an oblique direction. Finally, a three-dimensional porous composite was obtained after annealing and vulcanization. The obtained CoCeS [email protected]@RGO exhibited excellent electrical conductivity and remarkable cycle stability. When the current density was 1 A g , its specific capacitance was as high as 1004 F g . BPMW modifies graphene through the synergistic effect of π-π stacking interaction and special structure to obtain excellent electrochemical performance. Moreover, a solid-state asymmetric supercapacitor device was fabricated based on the synthesized CoCeS [email protected]@RGO hybrid, which exhibited a power density of 979 W kg at an energy density of 23.96 Wh kg .
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http://dx.doi.org/10.1002/chem.202103145DOI Listing
October 2021

Assembly of gold nanorods with L-cysteine reduced graphene oxide for highly efficient NIR-triggered photothermal therapy.

Spectrochim Acta A Mol Biomol Spectrosc 2022 Feb 29;266:120458. Epub 2021 Sep 29.

School of Mechanical and Electrical Engineering, Qingdao University, Qingdao 266071, China. Electronic address:

Near-infrared (NIR) photothermal therapy is an effective partner to the chemotherapy of tumors with the merits of high therapeutic ability and slight side effect on normal tissues. Herein, we synthesized gold nanorods and assembled them with L-cysteine reduced graphene oxide ([email protected]) for efficient photothermal therapy. The high therapeutic efficacy of [email protected] can be due to the high photothermal effect of gold nanorods and reduced graphene oxide, and the synergistic effect of them. The nontoxicity of L-cysteine also guarantees the comfortable biocompatibility of reduced graphene oxide, which is essential for the photothermal absorber used in human tissue. The results demonstrate that assembly of gold nanorods with reduced graphene oxide ([email protected]) is a promising photothermal agent with high efficient NIR-triggered photothermal therapy efficiency, excellent stability, superior biocompatibility.
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http://dx.doi.org/10.1016/j.saa.2021.120458DOI Listing
February 2022

Origami and layered-shaped ZnNiFe-LDH synthesized on Cu(OH) nanorods array to enhance the energy storage capability.

J Colloid Interface Sci 2022 Feb 16;607(Pt 2):1269-1279. Epub 2021 Sep 16.

College of Materials Science and Engineering, Institute for Graphene Applied Technology Innovation, Collaborative Innovation Centre for Marine Biomass Fibers, Materials and Textiles of Shandong Province, Qingdao University, Qingdao 266071, China. Electronic address:

The combination of layered nanorod arrays with unique core-shell structure and transition metal layered double hydroxide (LDH) is considered as a feasible solution to improve the electrochemical performances of capacitor electrode. In this study, layered [email protected](OH)/CF core-shell nanorod arrays, which consist of ultrathin ZnNiFe-LDHs nanosheet shells and ordered Cu(OH) nanorod inner cores, are successfully designed and fabricated by a typical hydrothermal way and a simple in situ oxidation reaction. The electrode prepared using [email protected](OH)/CF nanomaterial reveals an remarkable area capacitance of 6100 mF cm at 3 mA cm current density, which is excellently superior than those of [email protected](OH)/CF, [email protected](OH)/CF, Cu(OH)/CF and CF. Additionally, the capacitance retention remains as high as 83.4% after 5000 cycles and a very small Rs (0.567 Ω) can be observed. In addition, an asymmetric supercapacitor device is successfully fabricated employing [email protected](OH)/CF. Meanwhile, the [email protected](OH)/CF//AC device can achieve an energy density of 44 Wh kg and a corresponding power density of 720 W kg and possess the capability to light up a multi-function monitor for 33 min just using two ASC equipments connected in series. Therefore, the prepared [email protected](OH)/CF composite materials with unique structure has great application potential in energy storage devices.
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http://dx.doi.org/10.1016/j.jcis.2021.09.062DOI Listing
February 2022

lncRNA-SNHG14 Plays a Role in Acute Lung Injury Induced by Lipopolysaccharide through Regulating Autophagy via miR-223-3p/Foxo3a.

Mediators Inflamm 2021 8;2021:7890288. Epub 2021 Sep 8.

Department of Intensive Care Unit, Zhejiang Provincial People's Hospital (People's Hospital of Hangzhou Medicine College), Hangzhou 310014, China.

lncRNAs play important roles in lipopolysaccharide- (LPS-) induced acute lung injury. But the mechanism still needs further research. In the present study, we investigate the functional role of the lncRNA-SNHG14/miR-223-3p/Foxo3a pathway in LPS-induced ALI and tried to confirm its regulatory effect on autophagy. Transcriptomic profile changes were identified by RNA-seq in LPS-treated alveolar type II epithelial cells. The expression changes of lncRNA-SNHG14/miR-223-3p/Foxo3a were confirmed using qRT-PCR and west blot. The binding relationship of lncRNA-SNHG14/miR-223-3p/and miR-223-3p/Foxo3a was verified using dual-luciferase reporter, RNA immunoprecipitation, and RNA pull-down assays. Using gain-of-function or loss-of-function approaches, the effect of lncRNA-SNHG14/miR-223-3p/Foxo3a was investigated in LPS-induced acute lung injury mice model and in . Increasing of lncRNA-SNHG14 and Foxo3a with reducing miR-223-3p was found in LPS-treated A549 cells and lung tissue collected from the LPS-induced ALI model. lncRNA-SNHG14 inhibited miR-223-3p but promoted Foxo3a expression as a ceRNA. Artificially changes of lncRNA-SNHG14/miR-223-3p/Foxo3a pathway promoted or protected cell injury from LPS and in . Autophagy activity could be influenced by lncRNA-SNHG14/miR-223-3p/Foxo3a pathway in cells with or without LPS treatment. In conclusion, aberrant expression changes of lncRNA-SNHG14 participated alveolar type II epithelial cell injury and acute lung injury induced by LPS through regulating autophagy. One underlying mechanism is that lncRNA-SNHG14 regulated autophagy by controlling miR-223-3p/Foxo3a as a ceRNA. It suggested that lncRNA-SNHG14 may serve as a potential therapeutic target for patients with sepsis-induced ALI.
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http://dx.doi.org/10.1155/2021/7890288DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8443345PMC
September 2021

Trapping and Detection of Single Viruses in an Optofluidic Chip.

ACS Sens 2021 09 10;6(9):3445-3450. Epub 2021 Sep 10.

School of Electrical and Electronic Engineering, Nanyang Technological University, 639798 Singapore.

Accurate single virus detection is critical for disease diagnosis and early prevention, especially in view of current pandemics. Numerous detection methods have been proposed with the single virus sensitivity, including the optical approaches and immunoassays. However, few of them hitherto have the capability of both trapping and detection of single viruses in the microchannel. Here, we report an optofluidic potential well array to trap nanoparticles stably in the flow stream. The nanoparticle is bound with single viruses and fluorescence quantum dots through an immunolabeling protocol. Single viruses can be swiftly captured in the microchannel by optical forces and imaged by a camera. The number of viruses in solution and on each particle can be quantified via image processing. Our method can trap and detect single viruses in the 1 mL serum or water in 2 h, paving an avenue for the advanced, fast, and accurate clinical diagnosis, as well as the study of virus infectivity, mutation, drug inhibition, etc.
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http://dx.doi.org/10.1021/acssensors.1c01350DOI Listing
September 2021

DMPP reduces nitrogen fertilizer application rate, improves fruit quality, and reduces environmental cost of intensive apple production in China.

Sci Total Environ 2022 Jan 24;802:149813. Epub 2021 Aug 24.

State Key Laboratory of Crop Biology, College of Horticulture Science and Engineering, Shandong Agricultural University, Tai'an, Shandong 271018, China. Electronic address:

In China, excessive application of nitrogen (N) fertilizer is common in intensive apple production. To resolve issues of benefit reduction and environmental pollution caused by excessive N, a two-year trial was conducted in an apple orchard with a split-plot design, in which the main factor was the N level (500, 400, 300, and 200 kg N ha year, expressed as TN, TN80%, TN60%, and TN40%, respectively) and the deputy factor was whether or not to add 3,4-dimethylpyrazole phosphate (DMPP, expressed as +D). The effects of N reduction combined with DMPP on soil N transformation, fruit quality, economic benefits, and environmental effects were investigated. The results showed that DMPP reduced the production of nitrate and its vertical migration by inhibiting the abundance of AOB amoA and decreased NO emission by reducing nirKC1 levels. Moreover, N reduction combined with DMPP improved N use efficiency (26.67-49.35%) and reduced N loss rate (15.25-38.76%). Compared with TN, TN60% + D increased the content of anthocyanin and soluble sugar by 21.15% and 13.09%, respectively, and decreased environmental costs caused by NH volatilization and NO emission by 33.84%, while maintaining yield and N utilization rate at relatively high levels. Considering the agronomic, economic and environmental benefits, on the basis of traditional N application rate, 40% N reduction combined with DMPP (TN60% + D) could ensure target yield, corresponding quality and economic benefits, maintain soil N fertility, and reduce the risk of N losses to the environment. The present research could provide references for green, efficient, and sustainable development of apple production.
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http://dx.doi.org/10.1016/j.scitotenv.2021.149813DOI Listing
January 2022

Endothelial GABBR2 Regulates Post-ischemic Angiogenesis by Inhibiting the Glycolysis Pathway.

Front Cardiovasc Med 2021 4;8:696578. Epub 2021 Aug 4.

Department of Intensive Care Unit, Zhejiang Provincial People's Hospital, Hangzhou, China.

Angiogenesis post-ischemia plays an essential role in preventing ischemic damage to tissue by improving the blood recovery. Determining the regulatory mechanism of ischemic angiogenesis, therefore, could provide effective therapeutics for ischemic injury. The RNA sequencing (RNA-seq) database was used to predict the association of gamma-aminobutyric acid type B receptor subunit 2 (GABBR2) with endothelial-specific expression. The role of GABBR2 in angiogenesis was verified by downregulating GABBR2 in human umbilical vein endothelial cells (HUVECs) with lentiviral vectors. Besides, the effect of GABBR2 on the blood recovery of an ischemic hindlimb was demonstrated by establishing a hindlimb ischemia model in normal and GABBR2 adenoviral vector-infected mice. Then, the mobilization of endothelial progenitor cells (EPCs) in peripheral blood post-ischemia was determined by flow cytometry. Finally, the XF analyzer and Western blot were used to determine the effect of GABBR2 on endothelial metabolism. The RNA-seq results indicated a strong association between GABBR2 and endothelial revascularization, and the upregulation of GABBR2 was detected in both hypoxia-treated HUVECs and ischemic mouse hindlimb. Hypoxia treatment for 6 h increased the proliferation, migration, and tube formation of HUVECs, which were inhibited by GABBR2 knockdown. Additionally, GABBR2 downregulation significantly decreased the blood flow recovery of mouse ischemic hindlimb. The expressions of the EPC markers CD34 and CD133 significantly decreased in the peripheral blood in hindlimb post-ischemia. Mechanically, glycolysis-dominated metabolism of HUVECs was compromised by GABBR2 knockdown. Evidences of the decreased expressions of HKII, PFKFB3, and PKM1 also supported the compromised glycolysis induced by GABBR2 downregulation. Our study demonstrated that GABBR2 regulated angiogenesis post-ischemia by inhibiting the glycolysis pathway.
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http://dx.doi.org/10.3389/fcvm.2021.696578DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8371460PMC
August 2021

Fabrication and Characterization of Iridium Oxide pH Microelectrodes Based on Sputter Deposition Method.

Sensors (Basel) 2021 Jul 23;21(15). Epub 2021 Jul 23.

National Key Laboratory of Science and Technology on Micro/Nano Fabrication Laboratory, Collaborative Innovation Center of IFSA, Department of Micro/Nano-Electronics, Shanghai Jiao Tong University, Shanghai 200240, China.

pH value plays an important role in many fields such as chemistry and biology; therefore, rapid and accurate pH measurement is very important. Because of its advantages in preparation, wide test range, rapid response, and good biocompatibility, iridium oxide material has received more and more attention. In this paper, we present a method for preparing iridium oxide pH microelectrodes based on the sputter deposition method. The sputtering parameters of iridium oxide are also studied and optimized. Open-circuit potential tests show that microelectrodes exhibit near-Nernstian pH response with good linearity (about 60 mV/pH), fast response, high stability (a slight periodic fluctuation of potential change <2.5 mV in 24 h), and good reversibility in the pH range of 1.00-13.00.
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http://dx.doi.org/10.3390/s21154996DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8348779PMC
July 2021

Direct Observation of Amide Bond Formation in a Plasmonic Nanocavity Triggered by Single Nanoparticle Collisions.

J Am Chem Soc 2021 07 24;143(26):9781-9790. Epub 2021 Jun 24.

School of Life and Environmental Sciences, Deakin University, Geelong, VIC 3216, Australia.

The real-time observation of chemical bond formation at the single-molecule level is one of the great challenges in the fields of organic and biomolecular chemistry. Valuable information can be gleaned that is not accessible using ensemble-average measurements. Although remarkably sophisticated techniques for monitoring chemical reactions have been developed, the ability to detect the specific formation of a chemical bond at the single-molecule level has remained an elusive goal. Amide bonds are routinely formed from the aminolysis of -hydroxysuccinimide (NHS) esters by primary amines, and the protocol is widely used for the synthesis, cross-linking, and labeling of peptides and proteins. Herein, a plasmonic nanocavity was applied to study aminolysis reaction for amide bond formation, which was initiated by single nanoparticle collision events between suitably functionalized free-moving gold nanoparticles and a gold nanoelectrode in an aqueous buffer. By means of simultaneous surface enhanced Raman spectroscopy (SERS) and single-entity electrochemistry (EC) measurements, we have probed the dynamic evolution of amide bond formation in the aminolysis reaction with 10 s of millisecond time resolution. Hence, we demonstrate that single-entity EC-SERS is a valuable and sensitive technique by which chemical reactions can be studied at the single-molecule level.
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http://dx.doi.org/10.1021/jacs.1c02426DOI Listing
July 2021

A systemic ultrasound positioning protocol for nasointestinal tube in critically ill patients.

Crit Care 2021 06 19;25(1):213. Epub 2021 Jun 19.

Department of Medical Education and Simulation Center, Zhejiang Provincial People's Hospital, Affiliated People's Hospital, Hangzhou Medical College, Hangzhou, 310014, Zhejiang, China.

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http://dx.doi.org/10.1186/s13054-021-03641-2DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8214456PMC
June 2021

Fabrication of Cobaltous Sulfide Nanoparticle-Modified 3D MXene/Carbon Foam Hybrid Aerogels for All-Solid-State Supercapacitors.

ACS Appl Mater Interfaces 2021 Jun 9;13(24):28222-28230. Epub 2021 Jun 9.

College of Material Science and Engineering, Institute for Graphene Applied Technology Innovation, Collaborative Innovation Centre for Marine Biomass Fibers, Materials and Textiles of Shandong Province, Qingdao University, Qingdao 266071, Shandong, China.

MXene is a neoteric type of bidimensional (2D) transition metal carbide/nitride with broad application prospects, in particular with electrochemical energy storage. The electrochemical performance of MXene is unsatisfactory because it is easy to stack resulting in the difficulty of electrolyte penetration and ion transport. In this study, the cobaltous sulfide-modified 3D MXene/N-doped carbon foam ([email protected]/CF) hybrid aerogel is projected and manufactured via simple in situ growth and thermal annealing strategies. The capacitance of the as-fabricated 300-CMC-31:1 electrode material reaches 250 F g (1 A g), which is obviously higher than those of MXene, [email protected], 400-CMC-31:1, 300-CMC-10:1, 300-CMC-50:1, CF, and MXene/CF electrode materials. Moreover, it can hold 97.5% of the original capacitance after 10,000 cycles and the internal resistance () is only 0.50 Ω. A green bulb can be lit by two all-solid asymmetric supercapacitors installed in series. The prepared [email protected]/CF hybrid aerogel exhibits promising potential for practical application in energy storage areas.
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http://dx.doi.org/10.1021/acsami.1c05904DOI Listing
June 2021

A Comparison of Blood Pathogen Detection Among Droplet Digital PCR, Metagenomic Next-Generation Sequencing, and Blood Culture in Critically Ill Patients With Suspected Bloodstream Infections.

Front Microbiol 2021 17;12:641202. Epub 2021 May 17.

Intensive Care Unit, Zhejiang Provincial People's Hospital, People's Hospital of Hangzhou Medical College, Hangzhou, China.

Metagenomic next-generation sequencing (mNGS) and droplet digital PCR (ddPCR) have recently demonstrated a great potential for pathogen detection. However, few studies have been undertaken to compare these two nucleic acid detection methods for identifying pathogens in patients with bloodstream infections (BSIs). This prospective study was thus conducted to compare these two methods for diagnostic applications in a clinical setting for critically ill patients with suspected BSIs. Upon suspicion of BSIs, whole blood samples were simultaneously drawn for ddPCR covering 20 common isolated pathogens and four antimicrobial resistance (AMR) genes, mNGS, and blood culture. Then, a head-to-head comparison was performed between ddPCR and mNGS. A total of 60 episodes of suspected BSIs were investigated in 45 critically ill patients, and ddPCR was positive in 50 (83.3%), mNGS in 41 (68.3%, not including viruses), and blood culture in 10 (16.7%) episodes. Of the 10 positive blood cultures, nine were concordantly identified by both mNGS and ddPCR methods. The head-to-head comparison showed that ddPCR was more rapid (~4 h vs. ~2 days) and sensitive (88 vs. 53 detectable pathogens) than mNGS within the detection range of ddPCR, while mNGS detected a broader range of pathogens (126 vs. 88 detectable pathogens, including viruses) than ddPCR. In addition, a total of 17 AMR genes, including 14 and 3 genes, were exclusively identified by ddPCR. Based on their respective limitations and strengths, the ddPCR method is more useful for rapid detection of common isolated pathogens as well as AMR genes in critically ill patients with suspected BSI, whereas mNGS testing is more appropriate for the diagnosis of BSI where classic microbiological or molecular diagnostic approaches fail to identify causative pathogens.
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http://dx.doi.org/10.3389/fmicb.2021.641202DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8165239PMC
May 2021

A molecularly imprinted nanoreactor with spatially confined effect fabricated with nano-caged cascaded enzymatic system for specific detection of monosaccharides.

Biosens Bioelectron 2021 Sep 20;188:113355. Epub 2021 May 20.

College of Materials Science and Engineering; Institute for Graphene Applied Technology Innovation, College of Life Sciences, Qingdao University, 266071, China. Electronic address:

Glucose oxidase (GOx), traditionally regarded as an oxidoreductase with high β-D-glucose specificity, has been widely applied as sensing probe for β-D-glucose detection. However, it is found that the specificity of GOx is not absolute and GOx cannot decern β-D-glucose among its isomers such as xylose, mannose and galactose. The existence of the other monosaccharides in sensing system could compromise the sensitivity for β-D-glucose, therefore, it is of great urgency to achieve the highly specific catalytic performance of GOx. Herein, porous metal-organic frameworks (MOF) are prepared as the host matrix for immobilization of both GOx and bovine hemoglobin (BHb), obtained a cascaded catalytic system ([email protected]@BHb) with both enhanced GOx activity and peroxidase-like activity owing to the spatially confined effect. Then, using β-D-glucose as both template molecules and substances, hydroxyl radicals are produced continuously and applied for initiating the polymerization of molecular imprinting polymers (MIPs) on the surface of [email protected]@BHb. Impressively, the obtaining molecularly imprinted GOx (noted as [email protected]@BHb-MIPs) achieves the highly sensitive and specific detection of β-D-glucose in the concentration range of 0.5-20 μM with the LOD = 0.4 μM (S/N = 3) by colorimetry. Similarly, [email protected]@BHb-MIPs are subsequently obtained using mannose, xylose and galactose as template molecules, respectively, and also show satisfied specific catalytic activity towards corresponding templates, indicating the effectiveness of the proposed strategy to achieve highly specific catalytic performance of GOx.
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http://dx.doi.org/10.1016/j.bios.2021.113355DOI Listing
September 2021

Multiomics Analysis Reveals New Insights into the Apple Fruit Quality Decline under High Nitrogen Conditions.

J Agric Food Chem 2021 May 4;69(19):5559-5572. Epub 2021 May 4.

State Key Laboratory of Crop Biology, College of Horticulture Science and Engineering, Shandong Agricultural University, Tai'an 271018, Shandong, China.

Excessive application of nitrogen (N) fertilizer is common in Chinese apple production. High N reduced the contents of soluble sugar and total flavonoids by 16.05 and 19.01%, respectively, resulting in poor fruit quality. Moreover, high N increased the total N and decreased the total C and C/N ratio of apple fruits. On the basis of the transcriptomic, proteomic, and metabolomic analyses, the global network was revealed. High N inhibited the accumulation of carbohydrates (sucrose, glucose, and trehalose) and flavonoids (rhamnetin-3--rutinoside, rutin, and trihydroxyisoflavone-7--galactoside) in fruits, and more C skeletons were used to synthesize amino acids and their derivatives (especially low C/N ratio, e.g., arginine) to be transferred to N metabolism. This study revealed new insights into the decline in soluble sugar and flavonoids caused by high N, and hub genes (MD07G1172700, MD05G1222800, MD16G1227200, MD01G1174400, and MD02G1207200) and hub proteins (PFK, gapN, and HK) were obtained.
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http://dx.doi.org/10.1021/acs.jafc.1c01548DOI Listing
May 2021

Ultrafast generation of highly crystalline graphene quantum dots from graphite paper via laser writing.

J Colloid Interface Sci 2021 Jul 15;594:460-465. Epub 2021 Mar 15.

College of Materials Science and Engineering, Linyi University, Linyi 276000, Shandong, China; College of Materials Science and Engineering, Institute for Graphene Applied Technology Innovation, Collaborative Innovation Centre for Marine Biomass Fibers, Materials and Textiles of Shandong Province, Qingdao University, Qingdao 266071, China. Electronic address:

Graphene quantum dots (GQDs) are attractive fluorescent nanoparticles that have wide applicability, are inexpensive, nontoxic, photostable, water-dispersible, biocompatible and environmental-friendly. Various strategies for the synthesis of GQDs have been reported. However, simple and efficient methods of producing GQDs with control over the size of the GQDs, and hence their optical properties, are sorely needed. Herein, an ultra-fast and efficient laser writing technique is presented as a means to produce GQDs with homogeneous size from graphene produced by the instantaneous photothermal gasification and recrystallization mechanism. Controlling the laser scan speed and output power, the yield of GQDs can reach to be about 31.458 mg/s, which shows promising potential for large-scale production. The entire process eliminates the need for chemical solvents or any other reagents. Notably, the prepared laser writing produced GQDs (LWP-GQDs) exhibit blue fluorescence under UV irradiation of 365 nm and the Commission Internationale de L'Eclairage (CIE) chromaticity coordinates is measured at (0.1721, 0.123). Overall, this method exhibits superior advantages over the complex procedures and low yields required by other existing methods, and thus has great potential for the commercial applications.
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http://dx.doi.org/10.1016/j.jcis.2021.03.044DOI Listing
July 2021

[email protected] layered double hydroxide core-shell nanocomposites on nickel foam as superior electrode for all-solid-state asymmetric supercapacitors.

J Colloid Interface Sci 2021 Jun 7;592:455-467. Epub 2021 Feb 7.

College of Materials Science and Engineering, Institute for Graphene Applied Technology Innovation, Qingdao University, Qingdao 266071, China; College of Materials Science and Engineering, Linyi University, Linyi, 276000 Shandong, China. Electronic address:

In this work, [email protected] layered double hydroxide (LDH) core-shell structured nanocomposites on Ni foam (NF) are synthesized by facile hydrothermal and calcination methods. MgCoO/NF is synthesized first via a hydrothermal reaction and annealing treatment, and then utilized to prepare [email protected]/NF core-shell structured nanocomposites via the second hydrothermal process. It is found that the [email protected]/NF nanocomposite prepared from 6 h hydrothermal reaction ([email protected]) exhibits an excellent specific capacitance of 3757.2 F g (at 1 A g). Moreover, a high capacitance retention (86.9% after 6000 cycles) and a low internal resistance (Rs) (0.565 Ω) can be achieved. Furthermore, an all-solid-state asymmetric supercapacitor (ASC) is assembled using [email protected]/NF-2 as positive electrode and activated carbon (AC) as negative electrode. The as-fabricated [email protected]/NF-2//AC ASC shows a high energy density of 62.33 Wh kg at 750 W kg. Meanwhile, the [email protected]/NF-2//AC ASC device possesses an outstanding cycling stability of 93.7% retention of the initial capacitance after 6000 cycles and three ASC devices connected in series can light up a LED bulb for 15 min. Our results manifest that these core-shell structure [email protected] nanocomposites could envision huge potential application in energy storage devices.
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http://dx.doi.org/10.1016/j.jcis.2021.02.011DOI Listing
June 2021

Flexible Noncontact Sensing for Human-Machine Interaction.

Adv Mater 2021 Apr 8;33(16):e2100218. Epub 2021 Mar 8.

National Key Laboratory of Science and Technology on Micro/Nano Fabrication, Department of Micro/Nano Electronics, Shanghai Jiao Tong University, Shanghai, 200240, China.

From typical electrical appliances to thriving intelligent robots, the exchange of information between humans and machines has mainly relied on the contact sensor medium. However, this kind of contact interaction can cause severe problems, such as inevitable mechanical wear and cross-infection of bacteria or viruses between the users, especially during the COVID-19 pandemic. Therefore, revolutionary noncontact human-machine interaction (HMI) is highly desired in remote online detection and noncontact control systems. In this study, a flexible high-sensitivity humidity sensor and array are presented, fabricated by anchoring multilayer graphene (MG) into electrospun polyamide (PA) 66. The sensor works in noncontact mode for asthma detection, via monitoring the respiration rate in real time, and remote alarm systems and provides touchless interfaces in medicine delivery for bedridden patients. The physical structure of the large specific surface area and the chemical structure of the abundant water-absorbing functional groups of the PA66 nanofiber networks contribute to the high performance synergistically. This work can lead to a new era of noncontact HMI without the risk of contagiousness and provide a general and effective strategy for the development of smart electronics that require noncontact interaction.
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http://dx.doi.org/10.1002/adma.202100218DOI Listing
April 2021

Superelastic TiCT MXene-Based Hybrid Aerogels for Compression-Resilient Devices.

ACS Nano 2021 Mar 26;15(3):5000-5010. Epub 2021 Feb 26.

Institute for Frontier Materials, Deakin University, Geelong, VIC 3216, Australia.

Superelastic aerogels with excellent electrical conductivity, reversible compressibility, and high durability hold great potential for varied emerging applications, ranging from wearable electronics to multifunctional scaffolds. In the present work, superelastic MXene/reduced graphene oxide (rGO) aerogels are fabricated by mixing MXene and GO flakes, followed by a multistep reduction of GO, freeze-casting, and finally an annealing process. By optimizing both the composition and reducing conditions, the resultant aerogel shows a reversible compressive strain of 95%, surpassing all current reported values. The conducting MXene/rGO network provides fast electron transfer and stable structural integrity under compression/release cycles. When assembled into compressible supercapacitors, 97.2% of the capacitance was retained after 1000 compression/release cycles. Moreover, the high conductivity and porous structure also enabled the fabrication of a piezoresistive sensor with high sensitivity (0.28 kPa), wide detection range (up to 66.98 kPa), and ultralow detection limit (∼60 Pa). It is envisaged that the superelasticity of MXene/rGO aerogels offers a versatile platform for utilizing MXene-based materials in a wide array of applications including wearable electronics, electromagnetic interference shielding, and flexible energy storage devices.
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http://dx.doi.org/10.1021/acsnano.0c09959DOI Listing
March 2021

Resonance-trapped bound states in the continuum in metallic THz metasurfaces.

Opt Lett 2021 Jan;46(2):162-165

The realization of bound states in the continuum (BICs) in optical systems has been relying mainly on symmetry breaking. In contrast, another mechanism, known as resonance-trapped (or Friedrich-Wintgen) scenario, has been reported in the limited scope of dielectric resonant inclusions or at off- points. In this Letter, we demonstrate that the coupling coefficient between two coplanar metallic split-ring resonators can be tuned to satisfy the Friedrich-Wintgen BIC condition with normal terahertz (THz) incidence when metals are modeled as perfect electric conductors. Temporal coupled-mode theory is applied to validate the results. Experimentally, a BIC-induced cloaking effect has been observed, owing to the intrinsic dissipation loss of the constitutive materials. Our findings suggest an alternative strategy to construct BICs in metallic metasurfaces apart from conventional symmetry-breaking methods.
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http://dx.doi.org/10.1364/OL.410791DOI Listing
January 2021

Flower-like nanosheets directly grown on Co foil as efficient bifunctional catalysts for overall water splitting.

J Colloid Interface Sci 2021 Apr 12;587:650-660. Epub 2020 Nov 12.

College of Materials Science and Engineering, Institute for Graphene Applied Technology Innovation, Qingdao University, Qingdao 266071, China; College of Materials Science and Engineering, Linyi University, Linyi 276000, Shandong, China. Electronic address:

Hydrogen generation through electrochemical water decomposition is a promising method to address the global energy crisis. Herein, we report the synthesis of a series of flower-like MoS/CoS composites on Co foil (MoS/[email protected]) as high-performance electrochemical water-splitting catalysts in an alkaline environment. The flower-like array structure of MoS/[email protected] not only increases the electrochemically active surface area of ​​the catalyst, but also facilitates the release of bubbles generated, resulting in enhanced catalytic activity. For the hydrogen evolution reaction, the MoS/[email protected] electrode exhibits good stability and excellent catalytic activity in 1.0 M KOH (η = 105 mV), 1.0 M PBS (η = 92 mV) and 0.5 M HSO (η = 68 mV) solutions. For the oxygen evolution reaction, the electrode displays excellent stability and catalytic activity in 1.0 M KOH solution (η = 215 mV). When used for overall water splitting in 1.0 M KOH solution, MoS/[email protected] achieves a current density of 10 mA cm at a low potential of 1.58 V and maintains it stably for 40 h. This study presents a simple method for preparing transition metal-based bimetallic composite catalysts for efficient hydrogen production.
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http://dx.doi.org/10.1016/j.jcis.2020.11.025DOI Listing
April 2021

Solvent Effect on Supramolecular Self-Assembly of Chlorophylls a on Chemically Reduced Graphene Oxide.

Langmuir 2020 11 21;36(45):13575-13582. Epub 2020 Oct 21.

School of Life and Environmental Science, Deakin University, Geelong, Victoria 3216, Australia.

Solvent plays an important role in the surface interaction of molecules. In this study, we use "chlorophyll a", an archetypical molecule, to investigate its supramolecular self-assembly with chemically reduced graphene oxide in three different types of solvents: polar protic, polar aprotic, and non-polar. It was observed that only a polar protic solvent that can donate protons facilitates the hydrogen bonding between chlorophyll a and chemically reduced graphene oxide nanosheets in a hybrid system. The formation of hydrogen bonds further initiates the other non-covalent interactions such as π-π stacking and hydrophobic interaction, which altogether play a key driving force for supramolecular self-assembly of chlorophylls on chemically reduced graphene oxides. The experimental results are strongly supported by density functional theory calculations, which show robust electron coupling between chlorophylls and chemically reduced graphene oxide.
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http://dx.doi.org/10.1021/acs.langmuir.0c02370DOI Listing
November 2020

Energy Band Attraction Effect in Non-Hermitian Systems.

Phys Rev Lett 2020 Sep;125(13):137703

State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China.

The energy band attraction (EBA) caused by the nonorthogonal eigenvectors is a unique phenomenon in the non-Hermitian (NH) system. However, restricted by the required tight-binding approximation and meticulously engineered complex potentials, such an effect has never been experimentally demonstrated before. Here by a suitable design of all-dielectric Mie resonators in a parallel-plate transmission line, we for the first time verify the photonic analog of the EBA effects both theoretically and experimentally. The evolution of the EBA effect in a two-level NH system from gapped bands to gapless bands to flat bands is observed by precisely tuning the loss of the Mie resonators. The transmission spectra can be theoretically connected to the eigenvalues and eigenvectors of the NH Hamiltonian. Furthermore we extend our methods to a graphenelike two-dimensional NH system. Our works show a metamaterial approach toward NH topological photonics and foster a deeper understanding of band theory in open systems.
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http://dx.doi.org/10.1103/PhysRevLett.125.137703DOI Listing
September 2020

In Situ Fabrication of a Uniform Co-MOF Shell Coordinated with CoNiO to Enhance the Energy Storage Capability of NiCo-LDH via Vapor-Phase Growth.

ACS Appl Mater Interfaces 2020 Oct 8;12(42):47526-47538. Epub 2020 Oct 8.

College of Material Science and Engineering, Qingdao University, Qingdao 266071, Shandong, China.

NiCo-layered double hydroxide (LDH) has attracted increasing attention in recent years for application in supercapacitors (SCs) owing to its high redox activity and intercalating capability. However, the pristine NiCo-LDH is unable to reach theoretical specific capacitance and satisfying rate capability due to the limited electroactive species and a low ion diffusion rate. Here, we demonstrate novel vertically aligned nanosheet arrays of cobalt metal-organic framework (Co-MOF)@CoNiO core-shell composites constructed by the in situ grown Co-MOF shell with a uniform and controlled thickness on the CoNiO core via a vapor-phase approach. Owing to the intimate contact and synergistic effect between the Co-MOF shell and the CoNiO core, the as-synthesized [email protected] displays a high specific capacitance of about 571 F g, which is significantly higher than the pristine NiCo-LDH electrode (380 F g). Moreover, the capacitive properties of [email protected] can be further boosted to 757.2 F g after cyclic voltammetry oxidation. The easy preparation and high electrochemical performance of the [email protected] composite make it a potential material for SC application. These findings may inspire the exploration and construction of other MOF shell coating metal oxide from various nanostructured LDHs for varied applications. In addition, the as-assembled [email protected]/carbon cloth (CC)//activated carbon (AC) device can achieve a high capacitance of 87.67 F g. Meanwhile, the asymmetric supercapacitor (ASC) device exhibits a high energy density of 27.4 Wh kg at a power density of 750 W kg.
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http://dx.doi.org/10.1021/acsami.0c12759DOI Listing
October 2020

Three-dimensional self-floating foam composite impregnated with porous carbon and polyaniline for solar steam generation.

J Colloid Interface Sci 2021 Jan 31;581(Pt B):504-513. Epub 2020 Jul 31.

College of Materials Science and Engineering, Institute for Graphene Applied Technology Innovation, Collaborative Innovation Center for Marine Biomass Fibers Materials and Textiles of Shandong Province, Qingdao University, Qingdao 266071, China; College of Materials Science and Engineering, Linyi University, Linyi, Shandong, China. Electronic address:

A promising approach to resolving insufficient freshwater resources is utilizing solar energy for steam generation. Although various types of photothermal conversion materials have been developed, there are still some obstacles, such as complicated system structure fabrication and low energy utilization, that severely hinder their practical application. Herein, we designed and produced a self-floating porous carbon/polyaniline foam (PCPF) evaporator via impregnating melamine foam with porous carbon generated following the bottom-up pyrolytic method and polyaniline, followed by thermal treatment, for efficient solar steam generation. The PCPF obtained with a porous carbon (PC) to polyaniline (PAN) mass ratio of 3:5 (PCPF-3) exhibited a rich pore structure, good hydrophilicity, low thermal conductivity (0.0413 W m K), and excellent light absorption (96.1%). Our results show that, without additional thermal insulators, the evaporation rate of PCPF-3 reached 1.496 kg m h, and the photothermal conversion efficiency reached 87.3% under one sun irradiation. Furthermore, it also exhibited good durability and desalination performance. This type of environmentally friendly, low-cost, and stable photothermal conversion material could be used in water treatment and seawater desalination.
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http://dx.doi.org/10.1016/j.jcis.2020.07.136DOI Listing
January 2021

Nickel cobalt manganese ternary carbonate hydroxide nanoflakes branched on cobalt carbonate hydroxide nanowire arrays as novel electrode material for supercapacitors with outstanding performance.

J Colloid Interface Sci 2021 Jan 28;581(Pt A):11-20. Epub 2020 Jul 28.

College of Material Science and Engineering, Institute for Graphene Applied Technology Innovation, Qingdao University, Qingdao 266071, Shandong, China; College of Material Science and Engineering, Linyi University, Linyi 276000 Shandong, China. Electronic address:

In this work, for the first time we are reporting the development of a kind of high rate and long cycle life electrode composed of nickel cobalt manganese ternary carbonate hydroxide (NiCoMn-CH) ultrathin nanoflakes coated on Co-CH nanowire arrays (NWAs), which are directly generated on a nickel foam (NF) support. The hierarchical heterostructures are synthesized via a scalable two step solvothermal strategy without any adscititious surfactant and binder. The smart combination of Co-CH and NiCoMn-CH nanostructures in the nanowire arrays shows significant synergistic effect on the enhancement of the electrochemical performance of the as-fabricated supercapacitors. The as-obtained electrode exhibits excellent conductivity and high specific surface area, resulting in an unprecedented high specific capacitance (up to 3224F g at 1 A g in a three-electrode system) and an ultralong cycling stability (92.4% retention after 6000 successive charge-discharge cycles 5 A g). Meanwhile, an asymmetric supercapacitor device assembled of the [email protected] hierarchical nanostructures as positive electrode and activated carbon (AC) as negative electrode delivers good energy density of 20.31 W h kg at the power density of 748.46 W kg in the operation window 0-1.5 V. This methodology could be generalized to the design of other novel structured nanomaterials for energy storage devices and other applications.
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http://dx.doi.org/10.1016/j.jcis.2020.07.124DOI Listing
January 2021

Favorable Amorphous-Crystalline Iron Oxyhydroxide Phase Boundaries for Boosted Alkaline Water Oxidation.

ChemSusChem 2020 Sep 19;13(18):4911-4915. Epub 2020 Aug 19.

College of Materials Science and Engineering, Qingdao University, Qingdao, 266071, Shandong, P. R. China.

Interface engineering has proven an effective strategy for designing high-performance water-oxidation catalysts. Interface construction combining the respective advantages of amorphous and crystalline phases, especially embedding amorphous phases in crystalline lattices, has been the focus of intensive research. This study concerns the construction of an amorphous-crystalline FeOOH phase boundary (a-c-FeOOH) by structural evolution of iron oxyhydroxide-isolated Fe(OH) precursors from one-step hydrothermal synthesis. a-c-FeOOH demonstrates superb electrocatalytic activity for the oxygen evolution reaction (OER) with overpotential of 330 mV to drive a current density of 300 mA cm in 1.0 m KOH, which is among the best OER catalysts and much better than the pristine amorphous or crystalline FeOOH alone. Density functional theory calculations reveal that the high-density a-c phase boundaries play a critical role in determining high OER activity.
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http://dx.doi.org/10.1002/cssc.202001229DOI Listing
September 2020
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