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Single-atom catalysts for the electrochemical reduction of carbon dioxide into hydrocarbons and oxygenates

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Carbon Energy 2024年第3期6卷 64-117页

作者： Karl Adrian Gandionco Juwon Kim Lieven Bekaert Annick Hubin Jongwoo Lim department of chemistry Seoul National UniversitySeoulRepublic of Korea research Group Electrochemical and Surface Engineering(SURF) Department of Materials and ChemistryVrije Universiteit BrusselBrusselsBelgium

The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel *** this technology,an electrocatalytic material and renewable energy-generated electricity drive the conversion of carbon dioxide into high-value chemicals and carbon-neutral *** the past few years,single-atom catalysts have been intensively studied as they could provide near-unity atom utilization and unique catalytic ***-atom catalysts have become one of the state-of-the-art catalyst materials for the electrochemical reduction of carbon dioxide into carbon ***,it remains a challenge for single-atom catalysts to facilitate the efficient conversion of carbon dioxide into products beyond carbon *** this review,we summarize and present important findings and critical insights from studies on the electrochemical carbon dioxide reduction reaction into hydrocarbons and oxygenates using single-atom *** is hoped that this review gives a thorough recapitulation and analysis of the science behind the catalysis of carbon dioxide into more reduced products through singleatom catalysts so that it can be a guide for future research and development on catalysts with industry-ready performance for the electrochemical reduction of carbon dioxide into high-value chemicals and carbon-neutral fuels.

关键词： electrocatalysis electrochemical CO_(2)reduction hydrocarbons oxygenates single-atom catalysts

Polarization engineering in porous organic polymers for charge separation efficiency and its applications in photocatalytic aerobic oxidations

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Science China chemistry 2024年第3期67卷 1000-1007页

作者： Kun Wu Pei-Wen Cheng Xin-Yi Liu Ji Zheng Xiao-Wei Zhu Mo Xie Puxin Weng Weigang Lu Dan Li College of chemistry and materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China Guangdong Rare Earth Photofunctional materials Engineering Technology research center School of Chemistry and EnvironmentJiaying UniversityMeizhou 514015China

Photocatalytic aerobic oxidation reactions are largely governed by the efficiency of charge separation and subsequent reactive oxygen species(ROS) generation. Herein, we report a polarization engineering strategy to promote the charge separation and ROS generation efficiency by substituting the benzene unit with furan/thiophene in porous organic polymers(POPs). Benefiting from the extent of local polarization, the thiophene-containing POP(JNU-218) exhibits the best photocatalytic performance in aerobic oxidation reactions, with a yield much higher than those for the furan-containing POP(JNU-217) and the benzenecontaining POP(JNU-216). Experimental studies and theoretical calculations reveal that the increase of local polarization can indeed reduce the exciton binding energy, and therefore facilitate the separation of electron-hole pairs. This work demonstrates a viable strategy to tune charge separation and ROS generation efficiency by modulating the dipole moments of the building blocks in porous polymeric organic semiconductors.

关键词： porous organic polymer local polarization photocatalytic aerobic oxidation charge separation reactive oxygen species exciton binding energy

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Stable operation of highly loaded pure Si-Fe anode under ambient pressure via carboxy silane-directed robust solid electrolyte interphase

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Journal of Energy chemistry 2024年第7期94卷 568-576页

作者： Guntae Lim Dong Guk Kang Hyeon Gyu Lee Yen Hai Thi Tran Kihun An Junghyun Choi Kwang Chul Roh Do Youb Kim Seung-Wan Song department of Chemical Engineering&Applied chemistry Chungnam National University Daejeon 34134Republic of Korea Energy Storage materials center Korea Institute of Ceramic Engineering&TechnologyJinju 52851Republic of Korea Advanced Energy materials research center Korea Research Institute of Chemical TechnologyDaejeon 34114Republic of Korea

Incorporation of higher content Si anode material beyond 5 wt% to Li-ion batteries(LIBs)is challenging,owing to large volume change,swelling,and solid electrolyte interphase(SEI)instability ***,a strategy of diacetoxydimethylsilane(DAMS)additive-directed SEI stabilization is proposed for a stable operation of Si-0.33FeSi_(2)(named as Si-Fe)anode without graphite,which provides siloxane inorganics and organics enrichment that compensate insufficient passivation of fluoroethylene carbonate(FEC)additive and reduce a dependence on *** stable cycling performance of highly loaded(3.5 mA h cm^(-2))pure Si-Fe anode is achieved with 2 wt%DAMS combined with 9 wt%FEC additives under ambient pressure,yielding high capacity 1270 mA h g^(-1)at 0.5 C and significantly improved capacity retention of 81% after 100 cycles,whereas short circuit and rapid capacity fade occur with FEC only ***-directed robust SEI layer dramatically suppresses swelling and particles crossover through separator,and therefore prevents short circuit,demonstrating a possible operation of pure Si or Sidominant anodes in the next-generation high-energy-density and safe LIBs.

关键词： High-energy Li-ion battery Pure Si-Fe anode without graphite Silane additive SEI layer Suppressed swelling

Optimal geometrical configuration and oxidation state of cobalt cations in spinel oxides to promote the performance of Li-O_(2) battery

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Nano research 2024年第1期17卷 221-227页

作者： Yu Zhang Shuting Zhang Mengwei Yuan Yufeng Li Rong Liu Caiyun Nan Chen Chen Engineering research center of Advanced Rare Earth materials Department of ChemistryTsinghua UniversityBeijing 100084China Beijing Key Laboratory of Energy Conversion and Storage materials Institution College of ChemistryBeijing Normal UniversityBeijing 100875China X-ray diffraction Lab Analytical and Testing CenterBeijing Normal UniversityBeijing 100875China

Co_(3)O_(4) is considered as one of promising cathode catalysts for lithium oxygen(Li-O_(2))batteries,which contains both tetrahedral Co^(2+)sites(Co^(2+)Td)and octahedral Co^(3+)sites(Co^(3+)Oh).It is important to reveal the effect of optimal geometric configuration and oxidation state of cobalt ion in Co_(3)O_(4) to improve the performance of Li-O_(2) ***,through regulating the synthesis process,Co^(2+)and Co^(3+)sites in Co_(3)O_(4) were replaced with Zn and Al atoms to form materials with a unique Co *** Li-O_(2) batteries based on ZnCo_(2)O_(4) showed longer cycle life than that of CoAl_(2)O_(4),suggesting that in Co_(3)O_(4),the Co^(3+)Oh site is a relatively better geometric configuration than Co^(2+)Td site for Li-O_(2) *** calculations revealed that Co^(3+)Oh sites provide higher catalysis activity,regulating the adsorption energy of the intermediate LiO_(2) and accelerating the kinetics of the reaction in batteries,which further leads to the change of the morphology of the discharge product and ultimately improves the electrochemical performance of the batteries.

关键词： lithium oxygen(Li-O_(2))batteries geometrical configuration oxidation state lithium peroxide

New opportunities for ferroelectric deep-UV nonlinear optical crystals

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Science China materials 2024年第3期67卷 1004-1005页

作者： Miriding Mutailipu Shilie Pan research center for Crystal materials Xinjiang Technical Institute of Physics and ChemistryChinese Academy of SciencesUrumqi 830011China center of materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

Deep-ultraviolet(deep-UV)light with the wavelength below200 nm is one of the most crucial elements of both laser-driven industrial and scientific applications in recent years[1].DeepUV light has been produced using a variety of techniques,such as gas discharge lamps,synchrotron radiation,excimer lasers,free electron lasers,and nonlinear frequency conversion.

关键词： nonlinear optical ferroelectric

Recent Advances in Asymmetric Structural Composites for Excellent Electromagnetic Interference Shielding: A Review

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Chinese Journal of Polymer Science 2024年第6期42卷 693-710页

作者： Ying Zhou Bai Xue Lan Xie Chang-Mei Wu Qiang Zheng department of Polymer materials and Engineering College of Materials and Metallurgy Guizhou University National Engineering research center for Compounding and Modification of Polymer materials National and Local Joint Engineering Research Center for Functional Polymer Membrane Materials and Membrane Processes State Key Laboratory of Public Big Data Guizhou University department of Polymer Science and Engineering Zhejiang University

Since electromagnetic pollution is detrimental to human health and the environment, numerous efforts have been successively made to achieve excellent electromagnetic interference shielding effectiveness(EMI SE) via designing the hierarchical structures for electromagnetic interference(EMI) shielding polymer composites. Among the plentiful structures, the asymmetric structures are currently a hot spot, principally categorizing into multi-layered, porous, fibrous, and segregated asymmetric structures, which endows the high EMI shielding performance for polymer composites incorporated with magnetic, conductive, and/or dielectric micro/nano-fillers, due to the “absorption-reflection-reabsorption” shielding mechanism. Therefore, this review provides the retrospection and summary of the efforts with respect to abundant asymmetric structures and multifunctional micro/nano-fillers for enhancing EMI shielding properties, which is conducive to the booming development of polymeric EMI shielding materials for the promising prospect in modern electronics and 5-generation(5G) technology.

关键词： Asymmetric structure Microano functional filler Polymer composite Electromagnetic interference shielding

Atomically Dispersed Ruthenium Catalysts with Open Hollow Structure for Lithium-Oxygen Batteries

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Nano-Micro Letters 2024年第2期16卷 154-164页

作者： Xin Chen Yu Zhang Chang Chen Huinan Li Yuran Lin Ke Yu Caiyun Nan Chen Chen Beijing Advanced Innovation center for materials Genome Engineering Institute of Solid State ChemistryUniversity of Science and Technology BeijingBeijing 100083People’s Republic of China Engineering research center of Advanced Rare Earth materials Department of ChemistryTsinghua UniversityBeijing 100084People’s Republic of China Beijing Key Laboratory of Energy Conversion and Storage materials Institution College of ChemistryBeijing Normal UniversityBeijing 100875People’s Republic of China

Lithium–oxygen battery with ultrahigh theoretical energy density is considered a highly competitive next-generation energy storage device,but its practical application is severely hindered by issues such as difficult decomposition of discharge products at ***,we have developed N-doped carbon anchored atomically dispersed Ru sites cathode catalyst with open hollow structure(h-RuNC)for Lithium–oxygen *** one hand,the abundance of atomically dispersed Ru sites can effectively catalyze the formation and decomposition of discharge products,thereby greatly enhancing the redox *** the other hand,the open hollow structure not only enhances the mass activity of atomically dispersed Ru sites but also improves the diffusion efficiency of catalytic ***,the excellent activity from atomically dispersed Ru sites and the enhanced diffusion from open hollow structure respectively improve the redox kinetics and cycling stability,ultimately achieving a high-performance lithium–oxygen battery.

关键词： Atomically dispersed Open hollow structure Discharge product Lithium Oxygen battery

Layered kagome compound Na_(2)Ni_(3)S_(4)with topological flat band

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Chinese Physics B 2024年第5期33卷 153-159页

作者：叶君耀林益浩王浩哲宋志达冯济谢韦伟贾爽 International center for Quantum materials School of PhysicsPeking UniversityBeijing 100871China department of chemistry Michigan State UniversityMI48824USA Hefei National Laboratory Hefei 230088China Interdisciplinary Institute of Light-Element Quantum materials and research center for Light-Element Advanced materials Peking UniversityBeijing 100871China

We report structural and electronic properties of Na_(2)Ni_(3)S_(4),a quasi-two-dimensional compound composed of alternating layers of[Ni_(3)S_(4)]^(2-)and Na^(+).The compound features a remarkable Ni-based kagome lattice with a square planar configuration of four surrounding S atoms for each Ni *** and electrical measurements reveal a weak paramagnetic insulator with a gap of about 0.5 *** band structure calculation highlights a set of topological flat bands of the kagome lattice derived from the rotated dxz-orbital with C_(3)+T symmetry in the presence of crystal-field splitting.

关键词： kagome lattice flat band

A review on transition metal oxides based photocatalysts for degradation of synthetic organic pollutants

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Journal of Environmental Sciences 2024年第5期139卷 389-417页

作者： Athira Krishnan Anna Swarnalal Divine Das Midhina Krishnan Viswanathan S.Saji SMAShibli department of chemistry Amrita Vishwa VidyapeethamAmritapuriKerala690525India Interdisciplinary research center for Advanced materials King Fahd University of Petroleum&MineralsDhahran31261Saudi Arabia department of chemistry University of KeralaKariavattom CampusThiruvananthapuramKerala695581India

This review provides insight into the current research trend in transition metal oxides(TMOs)-based photocatalysis in removing the organic colouring matters from *** easy understanding,the research progress has been presented in four generations according to the catalyst composition and mode of application,viz:single component TMOs(the firstgeneration),doped TMOs/binary TMOs/doped binary TMOs(the second-generation),inactive/active support-immobilized TMOs(the third-generation),and ternary/quaternary compositions(the fourth-generation).The first two generations represent suspended catalysts,the third generation is supported catalysts,and the fourth generation can be suspended or *** review provides an elaborated comparison between suspended and supported catalysts,their general/specific requirements,key factors controlling degradation,and the methodologies for performance *** the plausible fundamental and advanced dye degradation mechanisms involved in each generation of catalysts were *** existing challenges in TMOs-based photocatalysis and how the researchers approach the hitch to resolve it effectively are *** research trends are also presented.

关键词： Photocatalysis Dye degradation Transition metal oxides and composites Supported catalysts Suspended catalysts