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A review on the rational design and fabrication of nanosized highentropy materials

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Nano Research 2023年第5期16卷 7874-7905页

作者： Yuanbo Zhou Xiaowei Shen Tao Qian chenglin yan Jianmei Lu Collaborative Innovation Center of Suzhou Nano Science and Technology College of Chemistry Chemical Engineering and Materials Science Soochow University199 Ren’ai RoadSuzhou 215123China Key Laboratory of Core Technology of High Specific Energy Battery and Key Materials for Petroleum and Chemical Industry College of EnergySoochow UniversitySuzhou 215006China School of Chemistry and Chemical Engineering Nantong UniversityNantong 226019China School of Electrical Engineering Nantong UniversityNantong 226019China Light Industry Institute of Electrochemical Power Sources Suzhou 215600China

High-entropy materials are mainly composed of high-entropy alloys(HEAs)and their *** them,HEAs account for a big *** a new kind of alloy,they are now arousing great interests because of their high mechanical strength,extraordinary fracture toughness,corrosion resistance compared with traditional *** characteristics allow the use of HEAs in various fields,including mechanical manufacturing,heat-resistant,radiation-resistant,corrosion-resistant,wear-resistant coatings,energy storage,heterocatalysis,*** order to promote the extensive application of HEAs,it is of significance to realize their rational design and *** this paper,a systematic review focusing on the rational design and fabrication of nanosized HEAs is *** design principles of how to match different elements in HEAs and the premise for the formation of single-phase solid solution HEAs are first *** methods for the prediction of formation conditions and properties of HEAs are also in ***,a detailed description and comparison of the synthesis methods of HEAs and their derivate,as well as their growing mechanism under various synthetic environments is *** commonly used characterization methods for the detection of HEAs,along with the typical cases of the application of HEAs in industrial materials,energy storage materials and catalytic materials are also ***,the challenges and perspectives in the design and synthesis of HEAs would be *** hope this review will give guidance for the future development of HEAs materials.

关键词： high-entropy alloys high-entropy alloy(HEA)derivate rational design synthesis strategies characterization application

Deciphering engineering principle of three-phase interface for advanced gas-involved electrochemical reactions

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Journal of Energy Chemistry 2023年第5期80卷 302-323,I0008页

作者： yanzheng He Sisi Liu Mengfan Wang Qiyang Cheng Tao Qian chenglin yan Collaborative Innovation Center of Suzhou Nano Science and Technology College of EnergySoochow UniversitySuzhou 215006JiangsuChina School of Chemistry and Chemical Engineering Nantong UniversityNantong 226019JiangsuChina Light Industry Institute of Electrochemical Power Sources Suzhou 215600JiangsuChina

As an alternative to conventional energy conversion and storage reactions,gas-involved electrochemical reactions,including the carbon dioxide reduction reaction(CO_(2)RR),nitrogen reduction reaction(NRR)and hydrogen evolution reaction(HER),have become an emerging research direction and have gained increasing attention due to their advantages of environmental friendliness and *** studies have been designed to accelerate sluggish kinetics but with limited *** of them promote the reaction by modulating the intrinsic properties of the catalyst,ignoring the synergistic effect of the reaction as a *** to the introduction of gas,traditional liquid-solid two-phase reactions are no longer applicable to future *** gas-involved electrochemical reactions mostly occur at the junctions of gaseous reactants,liquid electrolytes and solid catalysts,the focus of future research on reaction kinetics should gradually shift to three-phase reaction *** this review,we briefly introduce the formation and constraints of the three-phase interface and propose three criteria to judge its merit,namely,the active site,mass diffusion and electron mass ***,a series of modulation methods and relevant works are discussed in detail from the three improvement directions of‘exposing more active sites,promoting mass diffusion and accelerating electron transfer’.Definitively,we provide farsighted insights into the understanding and research of three-phase interfaces in the future and point out the possible development direction of future regulatory methods,hoping that this review can broaden the future applications of the three-phase interface,including but not limited to gas-involved electrochemical reactions.

关键词： Three-phase reaction Surface reactions Mass diffusion Electron transfer Gas-involved electrochemical reactions

Insight into the reaction mechanism of sulfur chains adjustable polymer cathode for high-loading lithium-organosulfur batteries

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Journal of Energy Chemistry 2021年第5期30卷 238-244页

作者： Jinqiu Zhou Xi Zhou Yawen Sun Xiaowei Shen Tao Qian chenglin yan Soochow Institute for Energy and Materials Innovations College of EnergyKey Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu ProvinceSoochow UniversitySuzhou 215006JiangsuChina Institute of Chemical Industry of Forestry Products Chinese Academy of ForestryNanjing 210042JiangsuChina

Small molecules with adjustable sulfur atoms in the confined structure were acted as precursor for the synthesis of polymer cathodes for lithium-organosulfur *** them,poly(diallyl tetrasulfide)(PDATtS)delivered a high capacity of 700 mAh g^(-1),stable capacity retention of 85%after 300 cycles,high areal capacity~4 m Ah cm^(-2) for electrode with up to 10.3 mg cm^(-2) *** insight into the reaction mechanism of PDATtS electrode that radicals arisen from the homolytic cleavage of S-S bond in PDATtS reacted with Li+to generate thiolates(RSLi)and insoluble lithium sulfides(Li_(2)S)or lithium disulfide(Li_(2)S_(2))was clearly verified by in-situ UV/Vis spectroscopy,nuclear magnetic resonance(NMR)studies and density-functional theory(DFT)***,based on the unique reaction mechanism,problems of rapid capacity fading due to the formation of soluble polysulfide intermediates and their serious shuttle effect in conventional lithium-sulfur(Li-S)batteries was totally avoided,realizing the dendrite-free lithium sulfur *** study sets new trends for avenues of further research to advance Li-S battery technologies.

关键词： Lithium-sulfur battery Organosulfur polymer Adjustable sulfur chains Cathode material

Altering the rate-determining step over cobalt single clusters leading to highly efficient ammonia synthesis

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National Science Review 2021年第5期8卷 110-118页

作者： Sisi Liu Mengfan Wang Haoqing Ji Xiaowei Shen chenglin yan Tao Qian College of Energy Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu ProvinceSoochow University

Activation of high-energy triple-bonds of N2is the most significant bottleneck of ammonia synthesis under ambient conditions. Here, by importing cobalt single clusters as strong electron-donating promoter into the catalyst, the rate-determining step of ammonia synthesis is altered to the subsequent proton addition so that the barrier of N2dissociation can be successfully overcome. As revealed by density functional theory calculations, the N2dissociation becomes exothermic over the cobalt single cluster upon the strong electron backdonation from metal to the N2antibonding orbitals. The energy barrier of the positively shifted rate-determining step is also greatly reduced. At the same time, advanced sampling molecular dynamics simulations indicate a barrier-less process of the N2approaching the active sites that greatly facilitates the mass transfer. With suitable thermodynamic and dynamic property, a high ammonia yield rate of 76.2 μg h–1mgcat–*** superior Faradaic efficiency of 52.9% were simultaneously achieved.

关键词： nitrogen reduction reaction rate-determining step cobalt single cluster mass transfer molecular dynamics simulations

Single lithium-ion channel polymer binder for stabilizing sulfur cathodes

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National Science Review 2020年第2期7卷 315-323页

作者： Chaoqun Niu Jie Liu Tao Qian Xiaowei Shen Jinqiu Zhou chenglin yan College of Energy Collaborative Innovation Center of Suzhou Nano Science and Technology Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu ProvinceSoochow University

Lithium–sulfur batteries have great potential for high-performance energy-storage devices, yet the severe diffusion of soluble polysulfide to electrolyte greatly limits their practical applications. To address the above issues, herein we design and synthesize a novel polymer binder with single lithium-ion channels allowing fast lithium-ion transport while blocking the shuttle of unnecessary polysulfide anions. In situ UV–vis spectroscopy measurements reveal that the prepared polymer binder has effective immobilization to polysulfide intermediates. As expected, the resultant sulfur cathode achieves an excellent specific capacity of 1310 mAh g-1at 0.2 C, high Coulombic efficiency of 99.5% at 0.5 C after 100 cycles and stable cycling performance for 300 cycles at 1 C(1 C = 1675 mA g-1). This study reports a new avenue to assemble a polymer binder with a single lithium-ion channel for solving the serious problem of energy attenuation of lithium–sulfur batteries.

关键词： polymer binders single lithium-ion channels polysulfide intermediates lithium–sulfur batteries

Ordered lithium ion channels of covalent organic frameworks with lithiophilic groups enable uniform and efficient Li plating/stripping

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Journal of Energy Chemistry 2021年第10期30卷 135-140,I0004页

作者： Xuyan Ni Jie Liu Haoqing Ji Libao Chen Tao Qian chenglin yan College of Energy Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu ProvinceSoochow UniversitySuzhou 215006JiangsuChina State Key Laboratory for Powder Metallurgy Central South UniversityChangsha 410083HunanChina Light Industry Institute of Electrochemical Power Sources Suzhou 215006JiangsuChina

Covalent organic frameworks(COFs)are a kind of materials composed of organic blocks linked through robust covalent bonds[1,2].In these materials,the organic blocks are integrated into symmetric structures that extend infinitely under the guidance of topological diagram,founded by periodic skeletons and nanopores[3-5].On account of the extensive building blocks,variety of topology design diagram and the variety of linkages,various COFs with different functionalities can be designed and synthesized for versatile applications.

关键词： Lithium metal anodes Lithiophilic covalent organic frameworks Dendrite-free In-situ characterization

Loading Fe3O4 nanoparticles on paper-derived carbon scaffold toward advanced lithium-sulfur batteries

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Journal of Energy Chemistry 2021年第1期30卷 1-11,I0001页

作者： Jianmei Han Qiang Fu Baojuan Xi Xuyan Ni chenglin yan Jinkui Feng Shenglin Xiong Key Laboratory of Colloid and Interface Chemistry Ministry of EducationSchool of Chemistry and Chemical Engineeringand State Key Laboratory of Crystal MaterialsShandong UniversityJinan 250100ShandongChina Soochow Institute for Energy and Materials InnovationS College of EnergySoochow UniversitySuzhou 215006JiangsuChina Key Laboratory for Liquid-solid Structural Evolution&Processing of Materials(Ministry of Education) Shandong UniversityJinan 250061ShandongChina College of Chemistry and Chemical Engineering Taishan UniversityTai’an 271021ShandongChina

Lithium-sulfur batteries(LSBs) are regarded as a competitive next-generation energy storage ***, their practical performance is seriously restricted due to the undesired polysulfides ***, a multifunctional interlayer composed of paper-derived carbon(PC) scaffold, Fe3O4 nanoparticles,graphene, and graphite sheets is designed for applications in LSBs. The porous PC skeleton formed by the interweaving long-fibers not only facilitates fast transfer of Li ions and electrons but also provides a physical barrier for the polysulfide shuttling. The secondary Fe3O4@graphene component can reduce the polarization, boost the attachment of polysulfides, and promote the charging-discharging kinetics. The outer graphitic sheets layers benefit the interfacial electrochemistry and the utilization of S-containing *** efficient obstruction of polysulfides diffusion is further witnessed via in situ ultraviolet-visible characterization and first-principles simulations. When 73% sulfur/commercial acetylene black is used as the cathode, the cell exhibits excellent capacity retention with high capacities at 0.5 C for 1000 cycles and even up to 10 C for 500 cycles, an ultrahigh rate capability up to 10 C(478 m Ah g-1), and a high arealsulfur loading of 8.05 mg cm-2. The strategy paves the way for developing multifunctional composites for LSBs with superior performance.

关键词： Paper-derived carbon nanosheets Fe3O4 Lithium-sulfur batteries Multifunctional interlayer Polysulfides

Advanced In Situ Characterization Techniques for Direct Observation of Gas-Involved Electrochemical Reactions

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Energy & Environmental Materials 2023年第6期6卷 73-112页

作者： yanzheng He Sisi Liu Mengfan Wang Qiyang Cheng Haoqing Ji Tao Qian chenglin yan Key Laboratory of Core Technology of High Specific Energy Battery and Key Materials for Petroleum and Chemical Industry College of EnergySoochow UniversitySuzhou 215006China School of Chemistry and Chemical Engineering Nantong UniversityNantong 226019China Light Industry Institute of Electrochemical Power Sources Suzhou 215600China

Gas-involved electrochemical reactions provide feasible solutions to the worldwide energy crisis and environmental *** has been recognized that various elements of the reaction system,including catalysts,intermediates,and products,will undergo real-time variations during the reaction process,which are of significant meaning to the in-depth understanding of reaction mechanisms,material structure,and active *** judicious tools for real-time monitoring of the changes in these complex elements,in situ techniques have been exposed to the spotlight in recent *** review aims to highlight significant progress of various advanced in situ characterization techniques,such as in situ X-ray based technologies,in situ spectrum technologies,and in situ scanning probe technologies,that enhance our understanding of heterogeneous electrocatalytic carbon dioxide reduction reaction,nitrogen reduction reaction,and hydrogen evolution *** provide a summary of recent advances in the development and applications of these in situ characterization techniques,from the working principle and detection modes to detailed applications in different reactions,along with key questions that need to be ***,in view of the unique application and limitation of different in situ characterization techniques,we conclude by putting forward some insights and perspectives on the development direction and emerging combinations in the future.

关键词： carbon dioxide reduction reaction gas-involved electrochemical reactions hydrogen evolution reaction in situ characterizations nitrogen reduction reaction

Low-temperature Li-S batteries enabled by all amorphous con version process of organosulfur cathode

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Journal of Energy Chemistry 2022年第1期31卷 496-502,I0013页

作者： Zhenkang Wang Xiaowei Shen Sijie Li Yuxuan Wu Tingzhou yang Jie Liu Tao Qian chenglin yan College of Energy Key Laboratory of Advanced Carb on Materials and Wearable Energy Technologies of Jiangsu ProvinceSoochow UniversitySuzhou 215006JiangsuChina College of Chemistry and Chemical Engineering.Nantong University Seyuan 9Nantong 226000JiangsuChina

The high degree of crystallinity of discharging in termediates of Li-S batteries(Li_(2)S_(2)/Li_(2)S)causes a severe capacity attenuation at low ***,a sulfur-rich polymer is fabricated,which enables all the discharging in termediates to exist in an amorphous state without long-range order,promoti ng the substantial conversion of discharging intermediates and enhancing Li-S batteries'performance at low temperatures *** cathode material exhibits excellent performance both at room and low *** under an extremely low temperature(-40℃),the discharge capacity can remain 67% of that at room ***,in-situ UV/Vis spectroscopy and density functional theory calculations reveal that this organosulfur cathode undergoes a new mechanism during ***_(2)S_(6) and Li_(2)S_(3) are the primary discharging intermediates that are quite different from conventional Li-S *** results provide a new directi on for a broader range of applications of Li-S batteries.

关键词： Low temperature Organosulfur polymers Li-S battery Crystallinity