CARBON
·
2022
·
IF 11.307
Meizhe Yu,Xiuzhi Guo,Haojie Lu,Peili Li,Ruobing Huang,Chunning Xu,Xuedong Gong,Yuhong Xiao,Xiaodong Xing
Developing efficient and safe approach to counteract the bacterial infections has become an urgent clinical challenge. In this work, we report folic acid derived carbon dots (FA-CDs) prepared by a one-step pyrolysis method. The FA-CDs can respond to the environmental stimuli of bacterial infections and acquire antimicrobial capacity “on demand” as a simple and effective antimicrobial nanosystem. The assays on antibacterial properties and mechanism show that FA-CDs are able to induce the gradual increase of intracellular reactive oxygen species (ROS) levels in bacteria under the simulated acidic environment and display pH-responsive biocidal activity. In a neutral condition, FA-CDs have no antibacterial activity, which will be conducive to mitigating the rise of bacterial drug resistance. The responsive antibacterial behavior can be attributed to that FA-CDs exhibit distinctive oxidase-like and peroxidase-like activity under acidic stimuli and inhibit the superoxide dismutase activity in bacteria cells, causing the accumulation of intracellular ROS. Meanwhile, FA-CDs can selectively kill Gram-positive bacterium S. aureus and remove mature biofilms. Besides, the in vitro and in vivo experiments demonstrate that FA-CDs possess excellent biocompatibility, and show remarkable therapeutic effect on the S. aureus -infected back wound models of mouse, which are crucial for clinical applications. Thus, this study highlights the potential application of FA-CDs as an ultra-succinct smart antimicrobial nanosystem for coping with infections caused by S. au reus in the clinical setting, and will bring about a new perspective on developing antimicrobial CDs.
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APPLIED SURFACE SCIENCE
·
2022
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IF 7.392
Lina Wang,Yun Zhao,Lijuan Cao,Yong Li,Gaoyi Han,Canliang Ma,Zongping Shao
Exfoliated graphite (EG) as important matrix material for potassium-ion batteries (PIBs) suffers from its inherent low surface activity, which results in poor interactions with active matter (e.g. metal sulfides) and undesired initial capacity decay of the EG-based electrodes. To address these issues, in this study, an attempt for EG’ surface engineering has been carried out through a stepwise gas-phase strategy. A S-doped carbon nanofiber/nanotube (CNF/CNT) hybrid was in-situ introduced on the surface of EG to form a novel micro-/nano- multiscale matrix structure. CoS nanoparticles are encapsulated in the inner of CNFs and CNTs. The special core–shell configuration not only prevents the aggregation of CoS during the sulfidation process, but also confines the active nanoparticles to avoid pulverization and maintains stable integrated electrode structure. Moreover, the couple effect between the active site-rich nature of CNFs and the high conductivity of CNTs as well as the formation of 3D porous network contribute to substantially elevated reversible capacity (411 mAh g −1 ), excellent initial cycling stability and rate capability (184 mAh g −1 at 2.0 A g −1 ). The effective surface modification strategy dominated by rational hybridization of CNFs and CNTs provides a new avenue for the development of high-performance electrode materials in PIB applications.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Jiangfu Zheng,Changzheng Fan,Xiaoming Li,Qi Yang,Dongbo Wang,Abing Duan,Jinglin Ding,Shengxiang Rong,Zhuo Chen,Jun Luo,Baowei Zhang
A novel hexagonal AgBr/Zn-Al MMO S-scheme photocatalyst was prepared by adopting a simplified hydrothermal and co-precipitation method. The prepared photocatalytic system exhibited excellent photocatalytic performance in degradation of tetracycline hydrochloride (TC). In particular, the ABMO0.2/Vis system generated the best TC removal rate (95%) within 60 min of visible light irradiation. Moreover, no significant decrease of the photocatalytic performance had been observed after four cycles, while the leaching of silver ions was effectively controlled. The excellent photocatalytic performance can be attributed to the synergistic effect occurring between the unique morphological structure and the S-scheme heterojunction charge transfer mechanism, since that that synergistic effect enhanced light absorption capacity and separation efficiency of the photogenerated carriers and the redox ability. In addition, liquid chromatography-mass spectrometry (LC-MS) analysis clarified the mineralization behavior and detailed decomposition pathways of TC. This work opens a new pathway for the design of efficient S-scheme heterojunctions and provides new insights into the photocatalytic degradation mechanism of antibiotics.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2022
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IF 4.598
Mingzhu Cui,Zhiqiang Xie,Meiling Wang,Xianming Zhang
Development of a high-performance electrode materials for the simultaneous sensing of ascorbic acid (AA), dopamine (DA) and uric acid (UA) is critical in clinical diagnostics. Novel polymer hydrogel-derived porous carbon has been investigated in sensing due to their high conductivity, hierarchical porous structure and environmental benignity. However, the high cost and cumbersome synthesis of the crosslinker for polymer hydrogel precursors make carbon production by pyrolysis greatly compromised. To address this challenge, here, a facile approach to N, O, S co-doped three-dimensional porous carbon frameworks (N, O, S-HCF) derived from methyl orange (MO) crosslinked polypyrrole hydrogel is developed. Experimental and spectroscopy demonstrate that the derived 3D porous structure and heteroatom doping effect create multidimensional electron transfer pathways and electrocatalytic activity centers. Specifically, the sensor exhibits potent and persistent electrochemical behavior with well-separated oxidation peaks and enhanced oxidation peak currents towards ascorbic acid (AA), dopamine (DA) and uric acid (UA). As a result, the N, O, S-HCF contributes to the effective determination of the three analytes in their mixture and the calibration curves show linear range of 2.5 × 10 −6 –1.0 × 10 −2 M, 1.8 × 10 −7 –8.7 × 10 −5 M, and 2.5 × 10 −7 –1.0 × 10 −4 M with detection limits of 1.0 × 10 −6 , 1.2 × 10 −7 , and 1.8 × 10 −7 M for AA, DA and UA, respectively. This study provides a simple strategy to build heteroatom doped porous carbon for the simultaneous monitoring of multiple electroactive species.
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ACS Applied Materials & Interfaces
·
2022
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IF 10.383
Mengna Li,Weiwang Qiu,Qian Wang,Na Li,Lu Liu,Xueli Wang,Jianyong Yu,Xiaoran Li,Faxue Li,Dequn Wu
Bacterial biofilms on wounds can lead to ongoing inflammation and delayed reepithelialization, which brings a heavy burden to the medical systems. Nitric oxide based treatment has attracted attention because it is a promising strategy to eliminate biofilms and heal infected wounds. Herein, a series of tryptophan-based poly(ester urea)s with good biodegradation and biocompatibility were developed for the preparation of composite mats by electrospinning. Furthermore, the mats were grafted with a nitric oxide donor (nitrosoglutathione, GSNO) to provide one type of NO loading cargo. The mats were found to have a prolonged NO release profile for 408 h with a maximum release of 1.0 μmol/L, which had a significant effect on killing bacteria and destructing biofilms. The designed mats were demonstrated to promote the growth of cells, regulate inflammatory factors, and significantly improve collagen deposition in the wound, eventually accelerating wound-size reduction. Thus, the studies presented herein provide insights into the production of NO-releasing wound dressings and support the application of full-thickness wound healing.
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PubMed
高影响因子
Solar RRL
·
2022
·Vol. 6
·期 8
·2200150
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IF 9.173
Chengfeng Ma,Chunxu Xiang,Xinge Liu,Bingyan Li,Xinyu Li,Shuaiqi Han,Qi Dai,Weibo Yan,Hao Xin
Solution-processed chalcopyrite copper indium gallium sulfoselenide (Cu(In,Ga)(S,Se) 2 , CIGSSe) thin-film solar cells have achieved efficiency beyond 18% and have great potential as an alternative to vacuum-based ones. However, most of the efficient solution-based CIGSSe solar cells are fabricated by spin-coating in an inert atmosphere, which limits the transfer from lab protocol to industrial large-scale production. Herein, a scalable doctor-blading technique is applied to fabricate CuIn(S,Se) 2 (CISSe) absorbers from N,N-dimethylformamide molecular precursor solution in ambient air. With the optimization of the precursor concentration to reduce the residue solvent and change the thermal annealing process from one-step to two-step to separate solvent evaporation and complex decomposition to suppress fluidity, high-quality absorber films with densely packed large grains have been fabricated and a champion CISSe solar cell with a power conversion efficiency of 12.54% has been achieved. Importantly, unlike the spin-coating technique which may cause composition change due to the different solubilities of the precursors, the doctor-bladed film has a composition very close to the precursor solution, which is very important for precise control of the absorber composition for industrial production.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Kunyu Chen,Zhanguo Cui,Zhiqiang Zhang,Heliang Pang,Jing Yang,Xiaojiang Huang,Jinsuo Lu
The present study developed a prolonged oxidizable sulfur(IV)/ferrate(VI) system for the generation of hydroxyl radical ( OH) and sulfate radical (SO 4 − ) within 120 min, and proposed a reaction mechanism. In the presence of H + in solution, the S(IV)/Fe(IV) system provided excellent oxidation performance of refractory organics O,O-dimethyl-S-methylcarbamoyl methyl phosphorothioate (dimethoate, a widely used organophosphorus pesticide) within 120 min. The degradation efficiency of dimethoate in the bisulfite/Fe(VI) system (e.g., 90.06% dimethoate) was higher than that in the sulfite/Fe(VI) system (e.g., 51.03% dimethoate), while Fe(VI) alone degraded 27.81% of dimethoate. In the S(IV)/Fe(VI) system, the active species consisted of Fe(VI) (including the highly-reactive iron-based intermediate species, i.e. Fe(V) and Fe(IV)), OH and SO 4 − , with OH being identified as the main active species, contributing more than half of the total. The degradation mechanism of dimethoate in the S(IV)/Fe(VI) system mainly included the cleavage of the S-P bond, C-S bond and the oxidation of the P = S bond. Two plausible degradation pathways were proposed based on the detected transformation products. Dimethoate could be efficiently degraded when the [bisulfite]/[Fe(VI)] molar ratio was 4:1 with a low Fe(VI) dosage (218 µM), the changes in HA and HCO 3 − concentrations affected the transformation of dimethoate, the presence of Cl − , SO 4 2− and NO 3 − had a negligible effect, and the S(IV)/Fe(VI) system performed well in real waters. The S(IV)/Fe(VI) system has excellent oxidation performance for the removal of organic pollutants in water, with a final pH (pH = 6.6) close to neutral and ultimate products of SO 4 2− and Fe(OH) 3 , which has great potential for engineering applications.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Yabin Li,Jingyao Qi,Jimin Shen,Binyuan Wang,Jing Kang,Pengwei Yan,Yizhen Cheng,Li Li,Linlu Shen,Zhonglin Chen
Extensive studies revealed that Cl - could inhibit the removal of targeted pollutants under low Cl - conditions in the peroxymonosulfate (PMS) system. However, the enhanced effect of Cl - has always been overlooked under high Cl - conditions. Here, we find that high concentration of Cl - played a critical role in bisphenol S (BPS) degradation by activating PMS using 16%-CoFe 2 O 4 @PAL (16% [email protected] ). The removal of BPS was sharply enhanced after introducing 0.5 and 1.0 M Cl - , and the corresponding k obs increased to 0.922 min −1 and 1.103 min −1 , which was 6-fold and 7-fold higher than the control (0.144 min −1 ), respectively. HOCl was demonstrated as the dominant species for removing BPS in 16% [email protected] /PMS system under high Cl - circumstances. The typical chlorinated BPS intermediates were identified, which showed higher eco-toxicity than BPS. The chlorinated byproducts along with their toxicity could be effectively eliminated after 30 min. The possible formation mechanism of chlorinated products was further revealed by theoretical calculations. Toxicity assessment experiments showed that BPS significantly affected hormone levels of zebrafish and showed toxicity on the testis and liver of zebrafish, which could be reduced using 16% [email protected] /PMS system. This study attracts attention to the overlooked HOCl in PMS-based processes under high salinity conditions.
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ORGANIC PROCESS RESEARCH & DEVELOPMENT
·
2022
·
IF 3.858
Xiangxiang Wang,Youyu Xie,Zhicai Wang,Ke Zhang,Hualei Wang,Dongzhi Wei
We developed a continuous flow system using ω-transaminase covalently immobilized on an epoxy resin modified with ethylenediamine (EDA) to synthesize (S)-1-Boc-3-aminopiperidine, which is a key intermediate for several novel inhibitors. A second functional group (−NH3+) was introduced to rapidly adsorb ω-transaminase, which was further rigidified by multipoint covalent attachment to the modified resin with high binding efficiency (>95%) and activity recovery (75%). The resulting immobilized ω-transaminase was stable with 90% residual activity after 15 reuse cycles. We synthesized (S)-1-Boc-3-aminopiperidine using this continuous flow system, and 95% conversion was obtained within 10 min of residence. The system was continuously operated for 24 h and achieved a space–time yield of 930.73 g·L–1·day–1, indicating outstanding reaction efficiency. This efficient continuous bioprocess has potential for large-scale production of (S)-1-Boc-3-aminopiperidine.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Qishan Fu,Muzi Yang,Zhongfei Liu,Hao Yang,Fengquan She,Xiaoqi Zhang,Fangyan Xie,Yuwen Hu,Jian Chen
Two-dimensional (2D) transition metal carbides (MXene) have shown great advantages as electrode materials in the new generation of energy storage, especially in supercapacitors . However, the inherent low specific capacitance and restacking layers of nanosheets that occur during electrode preparation further reduce the electrochemical performance of the materials. Based on this, we design a N, S co-doping electrode with a three-dimensional (3D) structure, which not only improves the specific capacitance through fundamentally modifying the electronic structure of the electrode materials, but also effectively improves the rate performance of the electrode by preventing the restacking of 2D materials . The N, S co-doping 3D architecture Ti 3 C 2 T x electrode (TC/NS-3D) exhibits an excellent capacitance value of 440 F g −1 at 5 mV s −1 and 64% capacitance retention rate at a high scan rate of 1000 mV s −1 in 3 mol L −1 H 2 SO 4 electrolyte. The TC/NS-3D electrode also shows excellent capacitance retention of 97.2% after the 10,000 cycles stability test. The density functional theory (DFT) analysis reveals the enhanced performance is attributed to accelerated intermediates transport kinetics promoted by 3D structure engineering and N, S co-doping for Ti 3 C 2 T x . This study is promising in designing heteroatomic doping 3D structure MXene-based materials for electrochemical energy storage systems.
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ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Jie Li,Youcai Lu,Shiyu Ma,Zhongjun Li,Qingchao Liu
Li–O 2 battery has attracted wide attention because it can satisfy the need for a new energy storage system with high energy density. However, poor oxygen reduction (ORR)/oxygen evolution (OER) kinetics involving Li 2 O 2 formation/decomposition is a major obstacle to its development. By designing suitable cathode with desired structure and surface electronic states, the formation/morphology of Li 2 O 2 and the reaction kinetics of charge process can be efficiently optimized simultaneously. In this work, a novel sulfur (S) and chlorine (Cl) co-doped porous carbon (CSC) were synthesized by one-step pyrolysis strategy, and the amount of heterogeneous atoms could be flexibly controlled by different calcination temperatures . Experimental combined with theoretical calculations show that the content of C Cl bond plays an important role in the adsorption of intermediate LiO 2 , thus regulating the morphology of Li 2 O 2 and ultimately affecting the release of battery energy. The C S bond mainly acts on the dynamics of the ORR and OER processes, which has an important influence on improving the round-trip efficiency of the battery. Benefiting from the synergistic effect of heteroatoms , the electrochemical performances of the Li–O 2 battery, including round-trip efficiency, discharge capacity and cycling stability are greatly improved.
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CHINESE JOURNAL OF CATALYSIS
·
2022
·
IF 12.92
Hui Yang,Jin feng Zhang,Kai Dai
Achieving a strong redox ability and high visible-light absorption ability in a single semiconductor material is difficult. Designing a heterojunction between two semiconductor materials is a feasible method. The new step (S-scheme) heterojunction can effectively promote the separation and transfer of photogenerated electron-hole pairs and retain strong redox ability. We designed and prepared a CdSe 0.8 S 0.2 -diethylenetriamine (DETA)/SnNb 2 O 6 heterostructure material via the solvothermal method. When CdSe 0.8 S 0.2 -DETA and SnNb2O6 form an S-scheme heterojunction, 30%CdSe 0.8 S 0.2 -DETA/SnNb2O6 exhibits the highest CO production rate (17.31 μmol·g –1 ·h –1 ), which is factors of 2.8 and 4.8 higher than that of traditional solvothermal SnNb 2 O 6 (6.2 μmol·g –1 ·h –1 ) and CdSe 0.8 S 0.2 -DETA (3.6 μmol·g –1 ·h –1 ), respectively. X-ray photoelectron spectroscopy characterization data provided evidence that the transfer pathway of space charge in the CO 2 reduction process was in accordance with the S-scheme. This research provides a simple strategy through which one can optimize the band structure to promote the separation of photogenerated carriers and achieve a high efficiency of CO 2 reduction.
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