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Surface engineering of 1D nanocatalysts for value-added selective electrooxidation of organic chemicals

Nano Research 2024年第3期17卷 1327-1336页

作者： Yongping Yang Chuhao Liu Tinglu Song Mufan Li Zipeng Zhao Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications Experimental Center of Advanced MaterialsSchool of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Beijing National Laboratory for Molecular Sciences College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

Electrolytic water splitting by renewable energy is a technology with great potential for producing hydrogen(H_(2))without carbon emission,but this technical route is hindered by its huge energy(electricity)cost,which is mainly wasted by the anode oxygen evolution reaction(OER)while the value of the anode product(oxygen)is very *** the high-energy-cost OER with a selective organic compound electrooxidation carried out at a relatively lower potential can reduce the electricity cost while producing value-added ***,H_(2) generation coupled with synthesis of value-added organic compounds faces the challenge of low selectivity and slow generation rate of the anodic ***-dimensional(1D)nanocatalysts with a unique morphology,well-defined active sites,and good electron conductivity have shown excellent performance in many electrocatalytic *** rational design and regulation of 1D nanocatalysts through surface engineering can optimize the adsorption energy of intermediate molecules and improve the selectivity of organic electrooxidation ***,we summarized the recent research progress of 1D nanocatalysts applied in different organic electrooxidation reactions and introduced several different fabrication strategies for surface engineering of 1D ***,we focused on the relationship between surface engineering and the selectivity of organic electrooxidation reaction ***,future challenges and development prospects of 1D nanocatalysts in the coupled system consisting of organic electrooxidation and hydrogen evolution reactions are briefly outlined.

关键词： hydrogen generation organic compound electrooxidation one-dimensional(1D)nanocatalysts surface engineering selectivity

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Cryogenic transmission electron microscopy on beam-sensitive materials and quantum science

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Chinese Physics B 2024年第8期33卷 9-29页

作者：王刚林君浩 Department of Physics and Shenzhen Key Laboratory of Advanced Quantum Functional Materials and Devices Southern University of Science and TechnologyShenzhen 518055China Quantum Science Center of Guangdong–Hong Kong–Macao Greater Bay Area(Guangdong) Shenzhen 518045China

Transmission electron microscopy(TEM)offers unparalleled atomic-resolution imaging of complex materials and heterogeneous ***,high-energy imaging electrons can induce structural damage,posing a challenge for electron-beam-sensitive *** TEM(Cryo-TEM)has revolutionized structural biology,enabling the visualization of biomolecules in their near-native states at unprecedented *** low electron dose imaging and stable cryogenic environment in Cryo-TEM are now being harnessed for the investigation of electron-beam-sensitive materials and low-temperature quantum ***,we present a systematic review of the interaction mechanisms between imaging electrons and atomic structures,illustrating the electron beam-induced damage and the mitigating role of *** review then explores the advancements in low-dose Cryo-TEM imaging for elucidating the structures of organic-based ***,we showcase the application of Cryo-TEM in the study of strongly correlated quantum materials,including the detection of charge order and novel topological spin ***,we discuss the future prospects of Cryo-TEM,emphasizing its transformative potential in unraveling the complexities of materials and phenomena across diverse scientific disciplines.

关键词： cryogenic TEM low dose imaging quantum materials

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Ablation resistance of ZrC coating modified by polymer-derived SiHfOC ceramic microspheres at ultrahigh temperature

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Journal of Materials science & technology 2024年第15期182卷 119-131页

作者： Xuemeng Zhang Yuyu Zhang Lingxiang Guo Bing Liu Yuqi Wang Hongbin Li Hejun Li Jia Sun Shaanxi Key Laboratory of Fiber Reinforced Light Composite Materials State Key Laboratory of Solidification ProcessingNorthwestern Polytechnical UniversityXi’an 710072China China Aerodynamics Research and Development Center Mianyang 621000China Science and Technology on Advanced Ceramic Fibers and Composites Laboratory National University of Defense TechnologyChangsha 410073China

Polymer-derived ceramics(PDCs)method opens up new possibilities for the preparation of novel multi-phase ceramic nanocomposites owing to the molecular design of the precursors at the nanoscale *** the current work,ZrC coatings incorporated with polymer-derived ceramic microspheres(CMS),SiH-fOC_CMS,were deposited to enhance the ablation resistance by supersonic atmosphere plasma *** 10.0 MW·m^(-2) plasma ablation at above 3000℃,the linear ablation rate of ZrC-SiHfOC_CMS coat-ing was reduced to 0.20μm·s^(-1),62%lower than that of the pristine ZrC *** improvement was ascribed to the presentence of viscous SiO_(2)/HfO_(2) molten mixed phase,rather than HfSiO4,which can ef-fectively seal pinholes and ***,the in-situ generated crystalline SiO_(2) had a lower oxygen diffusion rate than amorphous SiO_(2),meanwhile,m-HfO_(2) could improve the stability of SiO_(2) glassy film,thus further enhancing the ablation resistance.

关键词： ZrC Polymer-derived ceramics(PDCs) Carbon/Carbon composites Plasma spraying Plasma ablation

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Electrolyte and interphase engineering through solvation structure regulation for stable lithium metal batteries

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Chinese Chemical Letters 2023年第12期34卷 401-408页

作者： Hai Su Haikuo Zhang Zifeng Chen Mengjie Li Jiwei Zhao Haiyan Xun Jie Sun Yunhua Xu School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining Technology(Ministry of Education)and Tianjin Key Laboratory of Composite and Functional MaterialsTianjin UniversityTianjin 300072China State Key Laboratory of Silicon Materials School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027China Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Lithium metal batteries(LMBs)are considered to be one of the most promising high-energy-density battery ***,their practical application in carbonate electrolytes is hampered by lithium dendrite growth,resulting in short cycle ***,an electrolyte regulation strategy is developed to improve the cyclability of LMBs in carbonate electrolytes by introducing LiNO3 using trimethyl phosphate with a slightly higher donor number compared to NO_(3)^(-)as a *** not only allows the formaion of Li^(+)-coordinated NO3 but also achieves the regulation of electrolyte solvation structures,leading to the formation of robust and ion-conductive solid-electrolyte interphase films with inorganic-rich inner and organic-rich outer layers on the Li metal *** a result,high Coulombic efficiency of 99.1%and stable plating/stripping cycling of Li metal anode in LilCu cells were ***,excellent performance was also demonstrated in Li||LiNi_(0.83)Co_(0.11)Mn_(0.06)O_(2)(NCM83)full cells and Cul/NCM83 anodefree cells using high mass-loading *** work provides a simple interphase engineering strategy through regulating the electrolyte solvation structures for high-energy-density LMBs.

关键词： Lithium metal batteries Lithium nitrate Trimethyl phosphate Solvation structures Solid-electrolyte interphases

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Catalyst-Free Four-Component Spiropolymerization for the Construction of Spirocopolymers with Tunable Photophysical Properties

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Chinese Journal of Polymer science 2023年第10期41卷 1525-1532页

作者： Luo-Jie Zhu Gui-Nan Zhu Wen-Ya Yan Peng Sun Jian-Bing Shi Jun-Ge Zhi Bin Tong Zheng-Xu Cai Yu-Ping Dong Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing100081China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing100081China Key Laboratory of Cluster Science of Ministry of Education School of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing100081China

Spiropolymers have gained a great deal of interest from both academic and industrial fields by virtue of their unique geometric structures and physical ***,we prepared a series of spirocopolymers through the catalyst-free four-component spiropolymerization of diisocyanides,activated alkynes,and two different kinds of monomers with reactive carbonyl *** is found that the polymerization reactivity of monomers,feeding modes,and feed ratios play significant roles in *** with high reactivity and feeding reactive monomers first contribute to improving the molecular weights and yields of the *** constructed copolymers have two different kinds of spiro structures,which is confirmed by the nuclear magnetic *** addition,the spirocopolymers display the unique cluster-triggered emission and aggregation-induced emission properties,and their emission properties can be well-modulated by altering the ratio of *** is highly anticipated that this line of research will enrich the methodology of multi-component spiropolymerization,and provide a new insight into developing spiropolymers with various spiro structures and tunable properties.

关键词： Multi-component spiropolymerization Spirocopolymers Aggregation-induced emissions Clusterization-triggered emissions

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Organic Host-Guest Materials with Bright Red Room-Temperature Phosphorescence for Persistent Bioimaging

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Chinese Journal of Chemistry 2023年第13期41卷 1575-1582页

作者： Yueyue Si Yeyun Zhao Wenbo Dai Shisheng Cui Peng Sun Jianbing Shi Bin Tong Zhengxu Cai Yuping Dong Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing100081 China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing100081 China

Organic room-temperature phosphorescence(RTP)materials have attracted immense attention in bioimaging due to their long emission lifetime and large Stokes *** materials with long emission wavelength can improve the penetration depth for ***,the design of red persistent RTP materials is still *** this study,a fused-ring structure has been proposed to effectively decrease the triplet energy level,thus extending the emission wavelength of *** addition,the fused-ring structure exhibits a high molar extinction coefficient(ɛ)and high luminescence efficiency due to the rigid structure.A new class of crystalline hosts(iminodibenzyl,IDB)are developed to stabilize the triplet excitons that are generated from the fused-ring *** maximum RTP wavelength of doping materials can reach 635 nm with a lifetime of 9.35 ***-disperse nanoparticles are successfully prepared for in vivo time-resolved bioimaging,which eliminates the background fluorescence interference from biological *** reveal a delicate design strategy for the construction of long-wavelength emissive RTP materials for high-resolution bioimaging.

关键词： Room-temperature phosphorescence Fused-ring systems Long-wavelength emission High-resolution bioimaging Luminescence Nanoparticles

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Sabatier principle guiding the design of cathode catalysts for Li-CO_(2) batteries

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Journal of Energy Chemistry 2024年第10期97卷 585-592,I0012页

作者： Haonan Xie Yimin Zhang Biao Chen Chunnian He Chunsheng Shi Enzuo Liu Naiqin Zhao School of Materials Science and Engineering Tianjin Key Laboratory of Composite and Functional MaterialsKey Laboratory of Advanced Ceramics and Machining Technology(Ministry of Education)Tianjin UniversityTianjin 300350China National Industry-Education Platform of Energy Storage Tianjin UniversityTianjin 300350China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou 350207FujianChina

The Sabatier principle has been widely used for designing electrocatalysts for energy conversion applications,but it is rarely mentioned in the research of cathode catalyst of Li-CO_(2) *** our work,the"volcanic"relationship between the catalytic activity and the adsorption energy of the catalyst to the intermediates is first demonstrated based on the first-principles calculation,which meets the Sabatier principle and can be used to design the cathode *** increases in the number of nitrogenvacancy in WN shift the d-band center and increase the interaction with the *** catalytic activity increases first and then decreases with the increase of adsorption energy,which was proved in the *** optimal catalyst for moderate adsorption of intermediate makes the thin LiaCO_(3) distribute *** exhibits a median voltage difference of 0.68 V and an energy efficiency of 84.33%at20μA cm^(-2)with a limited capacity of 200μA h cm^(-2).

关键词： Sabatier principle Bidirectional catalyst Transition metal nitrides Nitrogen-vacancy Li-CO_(2) batteries

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Reconstructing interfacial manganese deposition for durable aqueous zinc-manganese batteries

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National science Review 2023年第10期10卷 139-150页

作者： Yida Hu Zhexuan Liu Lanyan Li Shan Guo Xuefang Xie Zhigao Luo Guozhao Fang Shuquan Liang School of Materials Science and Engineering Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan ProvinceCentral South University School of Science Hunan University of Technology and Business College of Physical Science and Technology Xinjiang University College of Chemistry Xiangtan University

Low-cost,high-satety,and broad-prospect aqueous zinc-manganese batteries（ZMBs） are limited by complex interracial *** solid-liquid interfacial state of the cathode dominates the Mn dissolution/deposition process of aqueous ZMBs,especially the important influence on the mass and charge transfer behavior of Zn2+and Mn2+.We proposed a quasi-eutectic electrolyte（QEE） that would stabilize the reversible behavior of interracial deposition and favorable interracial reaction kinetic of manganese-based cathodes in a long cycle process by optimizing mass and charge *** emphasize that the initial interfacial reaction energy barrier is not the main factor affecting cycling performance,and the good reaction kinetics induced by interfacial deposition during the cycling process is more conducive to the stable cycling of the battery,which has been confirmed by theoretical analysis,quartz crystal microbalance with dissipation monitoring,depth etching X-ray photon-electron spectroscopy,*** a result,the QEE electrolyte maintained a stable specific capacity of 250 mAh g-1at 0.5 A g-1after 350 cycles in zinc-manganese *** energy density retention rate of the ZMB with QEE increased by 174%compared to that of conventional aqueous ***,the multi-stacked soft-pack battery with a cathodic mass load of 54.4 mg maintained a stable specific capacity of 200 mAh g-1for 100 cycles,demonstrating its commercial *** work proves the feasibility of adapting lean-water QEE to the stable aqueous ZMBs.

关键词： quasi-eutectic electrolyte aqueous zinc −manganese batteries solid −liquid interfacial state mass transfer charge transfer

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Thermal response, oxidation and ablation of ultra–high temperature ceramics, C/SiC, C/C, graphite and graphite–ceramics

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Journal of Materials science & technology 2022年第7期102卷 137-158页

作者： Xinghong Zhang Baihe Du Ping Hu Yuan Cheng Jiecai Han National Key Laboratory of Science and Technology on Advanced Composites in Special Environments and Center for Composite Materials and StructuresHarbin Institute of TechnologyHarbin 150001China

Various thermal protection materials exhibit obviously different and complicated thermal response,oxidation and ablation behavior,which are very important for the appropriate design and ***,the relative researches are very few *** this work,the thermal response,oxidation and ablation behavior of representative thermal protection materials including ultra-high temperature ceramics,C/SiC,C/C, graphite and graphite-ceramic were investigated systematically in strong heat flux,high enthalpy and low-pressure *** response of these materials was analyzed based on experimental results and thermal energy balance that accounts for all of the heat transfer processes transporting energy into and out of the *** factors were playing important roles in the thermal response including thermal conductivity,volumetric heat capacity,catalytic efficiency,emissivity and oxidation characteristics of the *** importance of each factor not only depends on the material characteristics such as material composition and phase content but also environment parameters including heat flux,enthalpy,pressure and testing *** comparisons and relationships of oxidation and ablation behaviors for these materials under extreme environments were also illustrated in ***,thermal response and ablation behaviors of pre-oxidized material or repeated tests were also performed to evaluate the effect of pre-treatment on the performance and reusability of thermal protection *** work offers guiding significance for the appropriate design and selection of thermal protection materials.

关键词： Thermal protection materials Ceramic Thermal response Oxidation Ablation

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Polaron interfacial entropy as a route to high thermoelectric performance in DAE-doped PEDOT:PSS films

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National science Review 2024年第3期11卷 259-270页

作者： Jiajia Zhang Caichao Ye Genwang Wei Liang Guo Yuhang Cai Zhi Li Xinzhi Wu Fangyi Sun Qikai Li Yupeng Wang Huan Li Yuchen Li Shuaihua Wang Wei Xu Xuefeng Guo Wenqing Zhang Weishu Liu Department of Materials Science and Engineering Southern University of Science and Technology Academy for Advanced Interdisciplinary Studies and Guangdong Provincial Key Laboratory of Computational Science and Material Design Southern University of Science and Technology Department of Mechanical and Energy Engineering Southern University of Science and Technology Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences College of Chemistry and Molecular Engineering National Biomedical Imaging Centre Peking University Guangdong Provincial Key Laboratory of Functional Oxide Materials and Devices Southern University of Science and Technology

Enhancing the thermoelectric transport properties of conductive polymer materials has been a long-term challenge, in spite of the success seen with molecular doping strategies. However, the strong coupling between the thermopower and the electrical conductivity limits thermoelectric performance. Here, we use polaron interfacial occupied entropy engineering to break through this intercoupling for a PEDOT:PSS(poly（3,4-ethylenedioxythiophene）-poly（4-styrenesulfonate）) thin film by using photochromic diarylethene（DAE） dopants coupled with UV-light modulation. With a 10-fold enhancement of the thermopower from 13.5 μV K-1to 135.4 μV K-1and almost unchanged electrical conductivity, the DAE-doped PEDOT:PSS thin film achieved an extremely high power factor of 521.28 μW m-1K-2from an original value of 6.78 μW m-1K-2. The thermopower was positively correlated with the UV-light intensity but decreased with increasing temperature, indicating resonant coupling between the planar closed DAE molecule and PEDOT. Both the experiments and theoretical calculations consistently confirmed the formation of an interface state due to this resonant coupling. Interfacial entropy engineering of polarons could play a critical role in enhancing the thermoelectric performance of the organic film.

关键词： thermoelectric PEDOT: PSS interfacial occupied entropy resonant coupling UV-light modulation

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