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Energy & Environmental Materials 2024年第4期7卷 143-152页

作者： Yuan Liu Qing Lin Xiaocui Chen Xufeng Meng Baoxiu Hou Haiyan Liu Shuaihua Zhang Ningzhao Shang Zheng Wang Chaoyue Zhang Jianjun Song Xiaoxian Zhao Department of chemistry College of Science Hebei Agricultural University College of chemistry and chemical engineering Qingdao University College of Physics Qingdao University

The Fe-based anode of sodium-ion batteries attracts much attention due to the abundant source,low-cost,and high specific ***,the low electron and ion transfer rate,poor structural stability,and shuttle effect of NaS2intermediate restrain its further ***,the Fe3O4/Fe/FeS tri-heterojunction node spawned N-carbon nanotube scaffold structure（FHNCS） was designed using the modified MIL-88B（Fe） as a template followed by catalytic growth and sulfidation process.

关键词： anode core-shell heterojunction hollow structure sodium ion batteries

Self-derivation and reconstruction of silver nanoparticle reinforced cobalt-nickel bimetallic hydroxides through interface engineering for overall water splitting

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Journal of Energy chemistry 2024年第3期90卷 590-599,I0013页

作者： Yan Li Jie Han Weiwei Bao Junjun Zhang Taotao Ai Mameng Yang Chunming Yang Pengfei Zhang National and Local Joint engineering Laboratory for Slag Comprehensive Utilization and Environmental Technology School of Materials Science and EngineeringShaanxi University of TechnologyHanzhong 723000ShaanxiChina State Key Laboratory of High-efficiency Utilization of Coal and Green chemical engineering College of Chemistry&Chemical EngineeringNingxia UniversityYinchuan 750021NingxiaChina College of chemistry&chemical engineering Yan’an UniversityYan’an 716000ShaanxiChina School of chemistry and chemical engineering Shanghai Jiao Tong UniversityShanghai 200240China

Designing efficient and long-lasting non-metal electrocatalysts is an urgent task for addressing the issue of kinetic hysteresis in electrochemical oxidation *** bimetallic hydroxides,catalyzing the oxygen evolution reaction(OER),have significant research potential because hydroxide reconstruction to generate an active phase is a remarkable ***,the complete reconstruction of ultrathin CoNi(OH)_(2) nanosheets was achieved by embedding Ag nanoparticles into the hydroxide to induce a spontaneous redox reaction(SRR),forming heterojunction Ag@CoNi(OH)_(2) for bifunctional *** calculations and in situ Raman and ex situ characterizations revealed that the inductive effect of the Ag cation redistributed the charge to promote phase transformation to highly activate Ag-modified *** Co-Ni dual sites in Co/NiOOH serve as novel active sites for optimizing the intermediates,thereby weakening the barrier formed by OOH^*.Ag@CoNi(OH)_(2) required a potential of 1.55 V to drive water splitting at a current density of 10 mA cm^(-2),with nearly 98.6% Faraday *** ion induction and triggering of electron regulation in the OER via the synergistic action of the heterogeneous interface and surface reconstruction,this strategic design can overcome the limited capacity of bimetallic hydroxides and bridge the gap between the basic theory and industrialization of water decomposition.

关键词： Surface reconstruction Bimetallic hydroxides Ag nanoparticle Operando Raman Overall water splitting

Performance optimization of chalcogenide catalytic materials in lithium-sulfur batteries:Structural and electronic engineering

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Chinese chemical Letters 2024年第7期35卷 147-166页

作者： Jianmei Han Peng Wang Hua Zhang Ning Song Xuguang An Baojuan Xi Shenglin Xiong College of chemistry and chemical engineering Taishan UniversityTai'an 271021China Key Laboratory of Colloid and Interface chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShandong UniversityJi'nan 250100China School of Mechanical engineering Chengdu UniversityChengdu 610106China

Lithium-sulfur batteries(LSBs)boasting remarkable energy density have garnered significant attention within academic and industrial ***,the progression of LSBs remains constrained by the languid redox kinetics intrinsic to sulfur and the pronounced shuttle effect induced by lithium polysulfides(Li PSs),which seriously affecting the energy density,cycling life and rate *** conceptualization and implementation of catalytic materials stand acknowledged as a propitious stratagem for orchestrating kinetic modulation,particularly in excavating the conversion of LiPSs and has evolved into a focal point for *** them,chalcogenide catalytic materials(CCMs)have shown satisfactory catalytic effects ascribe to the unique physicochemical properties,and have been extensively developed in recent *** the lack of systematic summary regarding the development of CCMs and corresponding performance optimization strategies,herein,we initiate a comprehensive review regarding the recent progress of CCMs for effective collaborative immobilization and accelerated transformation kinetics of Li *** that,the modulation strategies to improve the catalytic activity of CCMs are summarized,including structural engineering(morphology engineering,surface/interface engineering,crystal engineering)and electronic engineering(doping and vacancy,etc.).Finally,the application prospect of CCMs in LSBs is clarified,and some enlightenment is provided for the reasonable design of CCMs serving practical LSBs.

关键词： Lithium-sulfur batteries Chalcogenide Catalytic materials Lithium polysulfides Structural engineering Electronic engineering

Study of the Relationship Between New Ionic Interaction Parameters and Salt Solubility in Electrolyte Solutions Based on Molecular Dynamics Simulation

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Journal of Ocean University of China 2024年第2期23卷 467-476页

作者： SUN Wenting HU Yangdong ZHENG Jiahuan SUN Qichao Chen Xia DING Jiakun ZHANG Weitao WU Lianying College of chemistry and chemical engineering Ocean University of ChinaQingdao 266100China Institute of chemical engineering Guangdong Academy of Science Guangzhou 510665China

Studying the relationship between ionic interactions and salt solubility in seawater has implications for seawater desalination and mineral *** this paper,a new method of expressing ion-to-ion interaction is proposed by using molecular dynamics simulation,and the relationship between ion-to-ion interaction and salt solubility in a simulated seawater water-salt system is *** analyzing the variation of distance and contact time between ions in an electrolyte solution,from both spatial and temporal perspectives,new parameters were proposed to describe the interaction between ions:interaction distance(ID),and interaction time ratio(ITR).The best correlation between characteristic time ratio and solubility was found for a molar ratio of salt-to-water of 10:100 with a correlation coefficient of *** the same salt,a positive correlation was found between CTR and the molar ratio of salt and *** type 1-1,type 2-1,type 1-2,and type 2-2 salts,the correlation coefficients between CTR and solubility were 0.93,0.96,0.92,and 0.98 for a salt-to-water molar ratio of 10:100,*** solubility of multiple salts was predicted by simulations and compared with experimental values,yielding an average relative deviation of 12.4%.The new ion-interaction parameters offer significant advantages in describing strongly correlated and strongly hydrated electrolyte solutions.

关键词： molecular dynamics simulation interaction distance interaction time rate electrolyte aqueous solutions solubility

Nature-inspired design of droplet-synthesized polymeric nanoelectrode for photoelectrochemical microRNA sensing within single cells

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Science Bulletin 2024年第2期69卷 159-162页

作者： Si-Yuan Yu Yi-Li Liu Zheng Li Dechen Jiang Jing-Juan Xu Hong-Yuan Chen Wei-Wei Zhao State Key Laboratory of Analytical chemistry for Life Science School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Nanoelectrodes have been shown to be powerful tools for nanoscopic research on single entities,deepening the understanding of heterogeneity and stochastics for single molecules,nanoparticles and cells[1–3].However,despite their importance,current nanoelectrode preparations are highly restrained to flame/electrochemical etching,metal sputtering,electrochemical deposition,etc.[3],resulting in a limited range of materials(mainly gold,platinum and carbon)for potential-resolved detection of redox-active species(Table S1 online).The enrichment of preparation methods to introduce novel materials and mechanisms should prove significant for the development of nanoelectrodes.

关键词： electrode deepening restrained

Quantitative lithium substitution of carboxyl hydrogens in polyacrylic acid binder enables robust SiO electrodes with durable lithium storage stability

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Journal of Energy chemistry 2024年第10期97卷 352-360页

作者： Weihua Wang Wenyi Li Siyi Jing Huiping Yang Huiqun Wang Ling Huang Yuxiang Mao Xikun Pang Yudai Huang Li Zhang State Key Laboratory of Physical chemistry of Solid Surfaces Department of Chemical and Biochemical Engineering College of Chemistry and Chemical EngineeringCollaborative Innovation Centre of Chemistry for Energy Materials (iChEM) Xiamen University State Key Laboratory of chemistry and Utilization of Carbon-Based Energy Resources College of Chemistry Xinjiang University

The design of advanced binders plays a critical role in stabilizing the cycling performance of large-volume-effect silicon monoxide（SiO） *** the classic polyacrylic acid（PAA） binder,the self-association of-COOH groups in PAA leads to the formation of intramolecular and intermolecular hydrogen bonds,greatly weakening the bonding force of the binder to SiO ***,strengthening the binder-material interaction from the perspective of binder molecular regulation poses a significant ***,a modified PAA-Lix（0.25 ≤x≤1） binder with prominent mechanical properties and adhesion strength is specifically synthesized for SiO anodes by quantitatively substituting the carboxylic hydrogen with *** appropriate lithium substitution（x=0.25） not only effectively increases the number of hydrogen bonds between the PAA binder and SiO surface owing to charge repulsion effect between ions,but also guarantees moderate entanglement between PAA-Lixmolecular chains through the ion-dipole *** such,the PAA-Li0.25/SiO electrode exhibits exceptional mechanical properties and the lowest volume change,as well as the optimum cycling(1237.3 mA h g-1after 100cycles at 0.1 C) and rate performance(1000.6 mA h g-1at 1 C),significantly outperforming the electrode using pristine PAA *** work paves the way for quantitative regulation of binders at the molecular level.

关键词： Adhesion strength Charge repulsion effect Polyacrylic acid binder Quantitative lithium substitution SiO anode

Bifunctional two-carbon reagent made from acetylene via 1,2-difunctionalization and its applications

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Science China chemistry 2024年第3期67卷 936-944页

作者： Bo Yang Kangkui Li Yongdong Wang Shifa Zhu Key Laboratory of Functional Molecular engineering of Guangdong Province School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China School of chemistry and chemical engineering Zhejiang Sci-Tech UniversityHangzhou 310018China Singfar Laboratories Guangzhou 510670China

There are very limited approaches to directly gluing two molecules for the production of internal alkenes using the vastly abundant acetylene via 1,2-difunctionalization. Conversion of gaseous acetylene to internal alkenes via 1,2-difunctionalization in a desired manner is not as easy as it might be expected due to the potential competition reactions between acetylene and alkene produced and the difficulty in handling this harmful reagent and controlling the regio-and stereoselectivity. In this work, we designed an efficient catalytic system for the incorporation of acetylene gas into tremendous(E)-β-bromo vinylsulfones, which are bench-stable, easy to operate, and can function as bifunctional acetylene and show a rich reactivity profile in Sonogashira coupling, Heck coupling, substituted reaction, and various desulfonylation transformations, providing numerous internal alkenes.

关键词： acetylene 1 2-difunctionalization photocatalysis vinylsulfone

Steric hindrance shielding viologen against alkali attack in realizing ultrastable aqueous flow batteries

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Journal of Energy chemistry 2024年第10期97卷 529-534页

作者： Liwen Wang Kai Wan Xianzhi Yuan Zhipeng Xiang Zhiyong Fu Zhenxing Liang Guangdong Provincial Key Laboratory of Fuel Cell Technology School of Chemistry and Chemical Engineering South China University of Technology State Key Laboratory of Pulp and Paper engineering South China University of Technology Guangdong Provincial Laboratory of chemistry and Fine chemical engineering Jieyang Center

Viologens known as a kind of promising negolyte materials for aqueous organic redox flow batteries,face a critical stability challenge due to the SN2 nucleophilic attack by hydroxide ions（OH-） during the battery *** this work,a N-cyclic quaternary ammonium-grafted viologen molecule,viz.1,1'-bis（4,4'-dime thylpiperidiniumyl）-4,4'-bipyridinium tetrachloride(（DBPPy）Cl4),is developed by the molecular engineering *** obtained（DBPPy）Cl4molecule shows a decent solubility of 1.84 M and a redox potential of-0.52 V ***/AgCl,Experimental and theoretical results reveal that the grafted N-cyclic quaternary ammonium groups act as the steric hindrance to prevent nucleophilic attack by OH-,increasing the alkali resistance of the electroactive *** symmetrical battery with 0.50 M（DBPPy）Cl4shows negligible decay during the 13-day cycling *** demonstration,the flow battery utilizing 1.0 M（DBPPy）Cl4as the negolyte and 1-（1-oxyl-2,2',6,6'-tetramethylpiperidin-4-yl）-1'-(3-（trimethylammonio）propyl)-4,4'-bipyridinium trichloride as the posolyte exhibits a high capacity retention rate of 99.99% per cycle at 60 mA cm-2.

关键词： Alkali resistance Aqueous organic flow batteries Stability Steric hindrance Viologen

Study on trifluoromethanesulfonic acid-promoted synthesis of daidzein: Process optimization and reaction mechanism

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Chinese Journal of chemical engineering 2024年第7期71卷 132-139页

作者： Hai Cao Haibin Yang Yanxiong Fang Yuandi Zeng Xiaolan Cai Jingjing Ma School of chemical engineering and Light Industry Guangdong University of TechnologyGuangzhou 510006China Jieyang Branch of chemistry and chemical engineering Guangdong Laboratory(Rongjiang Laboratory) Jieyang 515200China

Daidzein has been widely used in pharmaceuticals,nutraceuticals,cosmetics,feed additives,*** preparation process and related reaction mechanism need to be further investigated.A cost-effective process for synthesizing daidzein was developed in this *** this article,a two-step synthesis of daidzein(Friedel–Crafts acylation and[5+1]cyclization)was developed via the employment of trifluoromethanesulfonic acid(TfOH)as an effective promoting *** effect of reaction conditions such as solvent,the amount of TfOH,reaction temperature,and reactant ratio on the conversion rate and the yield of the reaction,respectively,was systematically investigated,and daidzein was obtained in 74.0%isolated yield under optimal *** to the facilitating effect of TfOH,the Friedel–Crafts acylation was completed within 10 min at 90℃ and the[5+1]cyclization was completed within 180 min at 25℃.In addition,a possible reaction mechanism for this process was *** results of the study may provide useful guidance for industrial production of daidzein on a large scale.

关键词： Synthesis Optimal design chemical processes Reaction mechanism

Metal-organic framework hybrid materials of ZIF-8/RGO for immobilization of D-amino acid dehydrogenase

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Nano Research 2024年第1期17卷 290-296页

作者： Hangbin Lei Qian Zhang Xiaoyan Xiang Liang Jiang Shiyan Wang Lingxuan Duan Shizhen Wang Department of chemical and Biochemical engineering College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Xiamen Key Laboratory of Synthetic Biotechnology Xiamen UniversityXiamen 361005China

Immobilization of D-amino acid dehydrogenase(DAADH)by the assembly of peptide linker was studied for the biosynthesis of *** material of zeolitic imidazolate framework-8(ZIF-8)combined with reduced graphene oxide(RGO)was applied for the immobilization of DAADH from Ureibacillus *** recovery rate of DAADH/ZIF-8/RGO was 165.6%.DAADH/ZIF-8/RGO remained 53.4%of its initial activity at 50°C for 10 h while the free enzyme was ***/ZIF-8/RGO maintained 70.5%activity in hyperalkaline solution with pH *** parameters indicated that DAADH/ZIF-8/RGO had greater affinity of phenylpyruvate as V_(max)/K_(m)of DAADH/ZIF-8/RGO was 1.27-fold than free *** seven recycles,the activity of DAADH/ZIF-8/RGO remained 64.3%.Furthermore,one-step separation and in situ immobilization of DAADH by ZIF-8/RGO/Ni was carried out with 1.5-fold activity *** peptide linker and metal-organic framework(MOF)immobilization,thermostability and activity of the immobilized DAADH were significantly improved.

关键词： D-Amino acid dehydrogenase immobilization metal-organic frameworks zeolitic imidazolate framework-8(ZIF-8) reduced graphene oxide