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Coupling Value-Added Methanol Oxidation with CO₂ Electrolysis by Low-Coordinated Atomic Ni Sites

ACS Nano 2025年第21期19卷 20001-20011页

作者： Lian, Kang Gao, Sanshuang Liu, Wenxian Liu, Qian Feng, Yanhong Luo, Jun Hu, Guangzhi Chu, Ke Wang, Dingsheng Liu, Xijun MOE Key Laboratory of New Processing Technology for Nonferrous Metals and Materials Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials School of Resources Environment and Materials Guangxi University Guangxi Nanning 530004 China Institute for New Energy Materials & Low-Carbon Technologies School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China College of Materials Science and Engineering Zhejiang University of Technology Hangzhou 310014 China Institute for Advanced Study Chengdu University Sichuan Chengdu 610106 China ShenSi Lab Shenzhen Institute for Advanced Study University of Electronic Science and Technology of China Shenzhen 518110 China Institute for Ecological Research and Pollution Control of Plateau Lakes School of Ecology and Environmental Science Yunnan University Kunming 650504 China School of Materials Science and Engineering Lanzhou Jiaotong University Lanzhou 730070 China Department of Chemistry Tsinghua University Beijing 100084 China

The combination of CO2 fixation and small organic molecule oxidation offers a promising solution to increasing severe environmental issues and energy crises. Here, low-coordinated NiN3 sites were anchored onto nitroge... 详细信息

The combination of CO₂ fixation and small organic molecule oxidation offers a promising solution to increasing severe environmental issues and energy crises. Here, low-coordinated NiN₃ sites were anchored onto nitrogen-doped ordered mesoporous carbon (Ni-SAs/NOMC), which is capable of efficiently catalyzing the coupled methanol oxidation reaction and CO₂ reduction reaction (MOR||CO₂RR), thereby reducing the energy required for CO₂ conversion and enhancing the economic value of the CO₂ electrolytic system. In the membrane electrode assembly electrolyzer-based MOR||CO₂RR, Ni-SAs/NOMC achieved Faradaic efficiencies (FEs) of 95.4% for formate at the anode and 96.3% for CO at the cathode. Moreover, at a current density of 0.8 A cm^-2, Ni-SAs/NOMC demonstrated stable electrolysis for up to 100 h, with FEs at both the anode and cathode remaining stable at approximately 90%. In situ spectroscopy analyses and theoretical calculations identified the formation of critical intermediate species and the origin of activity improvement, guiding the development of efficient electrosynthesis of valuable chemicals. © 2025 American Chemical Society.

关键词： carbon dioxide fixation hybrid electrolysis system low-coordinated atomic Ni sites methanol oxidation reaction value-added chemicals

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In Situ Transmission Electron Microscopy and Three-Dimensional Electron Tomography for Catalyst Studies

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Chinese Journal of Structural Chemistry 2022年第10期41卷 56-76页

作者： Chen Sun Kuo Liu Jian Zhang Qian Liu Xijun Liu Lili Han College of Chemistry Fuzhou UniversityFuzhou 350116China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Key Laboratory of Spin Electron and Nanomaterials of Anhui Higher Education Institutes Suzhou UniversitySuzhou 234000China Institute for Advanced Study Chengdu UniversityChengdu 610106 China MOE Key Laboratory of New Processing Technology for Non-Ferrous Metals and Materials and Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured MaterialsSchool of ResourceEnvironments and MaterialsGuangxi UniversityNanning 530004China

An in-depth understanding of the catalytic reaction mechanism is the key to designing efficient and stable catalysts. In situ transmission electron microscope(TEM) is the most powerful tool to visualize and analyze the microstructures of catalysts during catalysis. In situ TEM combined with three-dimensional(3D) electron tomography(ET) reconstruction technique enables interrogations of catalysts’ structural dynamics and chemical changes in high temporal and spatial dimensions. In this review, we discuss and summarize the recent advances in in situ TEM together with 3D ET for catalyst studies. Topics include the latest research progress of in situ TEM imaging as well as 3D visualization and quantitative analysis of catalysts. We also pay particular attention to artificial intelligence(AI)-enhanced smart 3D ET. These include deep learning(DL)-based data compression and storage for the analysis of large TEM data, recovery of wedge-shaped information lost in 3D ET reconstructions, and DL models for reducing residual artifacts in 3D reconstructed images. Finally, the challenges and development prospects of current in situ TEM and 3D ET research are discussed.

关键词： in situ TEM catalyst electron tomography 3D reconstruction artificial intelligence machine learning

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Edge atomic Fe sites decorated porous graphitic carbon as an efficient bifunctional oxygen catalyst for Zinc-air batteries

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Journal of Energy Chemistry 2023年第8期83卷 602-611,I0014页

作者： Ruihui Gan Yali Wang Xiangwu Zhang Yan Song Jingli Shi Chang Ma Tianjin Municipal Key Lab of Advanced Fiber and Energy Storage Technology Tiangong UniversityTianjin 300387China Fiber and Polymer Science Program Department of Textile EngineeringChemistry and ScienceWilson College of TextilesNorth Carolina State UniversityRaleighNC 27695-8301uNITED sTATES CAS Key Laboratory of Carbon Materials Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001ShanxiChina

The development of advanced bifunctional oxygen electrocatalysts for oxygen reduction and evolution reactions(ORR and OER) is critical to the practical application of zinc-air batteries(ZABs). Herein, a silica-assisted method is reported to integrate numerous accessible edge Fe-Nx sites into porous graphitic carbon(named Fe-N-G) for achieving highly active and robust oxygen electrocatalysis. Silica facilitates the formation of edge Fe-Nx sites and dense graphitic domains in carbon by inhibiting iron *** purification process creates a well-developed mass transfer channel for Fe-N-G. Consequently,Fe-N-G delivers a half-wave potential of 0.859 V in ORR and an overpotential of 344 m V at10 m A cm^(-2)in OER. During long-term operation, the graphitic layers protect edge Fe-Nx sites from demetallation in ORR and synergize with Fe OOH species endowing Fe-N-G with enhanced OER *** functional theory calculations reveal that the edge Fe-Nx site is superior to the in-plane Fe-Nx site in terms of OH* dissociation in ORR and OOH* formation in OER. The constructed ZAB based on Fe-N-G cathode shows a higher peak power density of 133 m W cm^(-2)and more stable cycling performance than Pt/C + RuO2counterparts. This work provides a novel strategy to obtain high-efficiency bifunctional oxygen electrocatalysts through space mediation.

关键词： Bifunctionality EdgeFe-Nxsites Oxygen catalysis Graphitic domains Zinc-air batteries

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A case study of comparing two dimerized acceptor molecules built by different branch-connected and terminal-connected approaches

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Science China Chemistry 2024年第5期67卷 1687-1696页

作者： Kangqiao Ma Huazhe Liang Yuxin Wang Tengfei He Tainan Duan Xiaodong Si Wendi Shi Guankui Long Xiangjian Cao Zhaoyang Yao Xiangjian Wan Chenxi Li Bin Kan Yongsheng Chen State Key Laboratory and Institute of Elemento-Organic Chemistry Frontiers Science Center for New Organic MatterThe Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer MaterialsInstitute of Polymer ChemistryRenewable Energy Conversion and Storage Center(RECAST)College of ChemistryNankai UniversityTianjin 300071China School of Materials Science and Engineering National Institute for Advanced MaterialsRenewable Energy Conversion and Storage Center(RECAST)Nankai UniversityTianjin 300350China Chongqing Institute of Green and Intelligent Technology Chongqing SchoolUniversity of Chinese Academy of Sciences(UCAS Chongqing)Chinese Academy of SciencesChongqing 400015China

Dimerized small-molecule acceptors(SMAs) built by the conventional connection of terminal groups of monomers have contributed to exciting long-term stabilities of organic solar cells(OSCs). However, device efficiencies, especially fill factors(FFs), still need to be improved. This probably originates from unsymmetrical molecular structure/conformation-determined less compact/ordered molecular stackings, such as ineffective stackings of constraint terminals. Herein, an exotic dimerized SMA of BC-Th is established by bridging the branched groups(BC-type, branch coupling) of two monomers rather than conventional terminal units(TC-type, terminal coupling). Benefiting from the three-dimensional conformation and more uncurbed terminals,BC-Th exhibits multiple molecular orientations along with a larger dielectric constant and electron mobility compared with TCTh. Finally, an efficiency of 17.43% is achieved by BC-Th-based OSCs, along with the highest FF of 79.13% among all dimerized SMAs-based OSCs to date. When introducing L8-BO as the third component, overall enhanced efficiency of 18.05%and FF of 80.11% are further afforded. Contrarily, TC-Th-based OSCs exhibit much inferior PCE of 16.29% and FF of 74.81%,demonstrating the great advantages of “branch coupling” over “terminal coupling” when building dimerized SMAs.

关键词： organic solar cells dimerized acceptor molecules branch coupling morphology control stability

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Simulation of Weft Knitted Fabric Using Three-Dimensional Yarn Loops and Grid and Spring Mass Models

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Advances in materials Science and Engineering 2023年第1期2023卷

作者： Hu, Haodong Li, Tong Ke, Wei Wang, Lijing Deng, Zhongmin State Key Laboratory of New Textile Materials and Advanced Processing Technology Wuhan Textile University Hubei Wuhan430200 China School of Fashion and Textiles RMIT University 25 Dawson St MelbourneVIC3056 Australia

The existing knitted fabric simulation methods cannot be effectively applied to three-dimensional (3D) modeling and simulation of weft knitted garments due to the lack of simple and convenient 3D dynamic simulation models for weft knitted fabrics. This paper presents a method of constructing a loop model by coupling the grid model with the spring mass model. The simulation of weft knitted fabric with real effects was achieved through the coupled model construction of the loop model combined with the yarn simulation generation algorithm and yarn collision response algorithm. The method presented in this paper can quickly and simply simulate the design of weft knitted clothing with loop structure. It provides a reference for the 3D simulation design of weft knitted fabric. © 2023 Haodong Hu et al.

关键词： Wool

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Multiscale strain alleviation of Ni-rich cathode guided by in situ environmental transmission electron microscopy during the solid-state synthesis

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Journal of Energy Chemistry 2023年第9期84卷 467-475页

作者： Fengyu Zhang Yunna Guo Chenxi Li Tiening Tan Xuedong Zhang Jun Zhao Ping Qiu Hongbing Zhang Zhaoyu Rong Dingding Zhu Lei Deng Zhangran Ye Zhixuan Yu Peng Jia Xiang Liu Jianyu Huang Liqiang Zhang School of New Energy and Materials China University of Petroleum BeijingBeijing 102249China Clean Nano Energy Center State Key Laboratory of Metastable Materials Science and Technology Yanshan UniversityQinhuangdao 066004HebeiChina School of Materials Science and Engineering Beihang UniversityBeijing 100191China Sichuan New Energy Vehicle Innovation Center Yibin 644000SichuanChina School of Materials Science and Engineering Xiangtan UniversityXiangtan 411105HunanChina Peking University Institute of Advanced Agricultural Sciences Shandong Laboratory of Advanced Agricultural Sciences at WeifangWeifang 261000ShandongChina China Oil&Gas Pipeline Network Corporation Department of Engineering Beijing 100026China Hebei Key Laboratory of Applied Chemistry College of Environmental and Chemical EngineeringYanshan UniversityQinhuangdao 066004HebeiChina Key Laboratory of Low Dimensional Materials and Application Technology of Ministry of Education School of Materials Science and EngineeringXiangtan UniversityXiangtan 411105HunanChina

Ni-rich layered oxides are one of the most promising cathode materials for Li-ion batteries due to their high energy ***,the chemomechanical breakdown and capacity degradation associated with the anisotropic lattice evolution during lithiation/delithiation hinders its practical ***,by utilizing the in situ environmental transmission electron microscopy(ETEM),we provide a real time nanoscale characterization of high temperature solid-state synthesis of LiNi_(0.8)CO_(0.1)Mn_(0.1)O_(2)(NCM811) cathode,and unprecedentedly reveal the strain/stress formation and morphological evolution mechanism of primary/second ary particles,as well as their influence on electrochemical *** show that stress inhomogeneity during solid-state synthesis will lead to both primary/secondary particle pulverization and new grain boundary initiation,which are detrimental to cathode cycling stability and rate *** to alleviate this multiscale strain during solid-state synthesis,we introduced a calcination scheme that effectively relieves the stress during the synthesis,thus mitigating the primary/secondary particle crack and the detrimental grain boundaries formation,which in turn improves the cathode structural integrity and Li-ion transport kinetics for long-life and high-rate electrochemical *** work remarkably advances the fundamental understanding on mechanochemical properties of transition metal oxide cathode with solid-state synthesis and provides a unified guide for optimization the Ni-rich oxide cathode.

关键词： Ni-rich cathode In situ ETEM Solid-state synthesis Multiscale strain alleviation

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Comparative coherence between layered and traditional semiconductors: unique opportunities for heterogeneous integration

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International Journal of Extreme Manufacturing 2023年第4期5卷 1-35页

作者： Zhuofan Chen Xiaonan Deng Simian Zhang Yuqi Wang Yifei Wu Shengxian Ke Junshang Zhang Fucheng Liu Jianing Liu Yingjie Liu Yuchun Lin Andrew Hanna Zhengcao Li Chen Wang State Key Laboratory of New Ceramics and Fine Processing Key Laboratory of Advanced Materials of Ministry of EducationSchool of Materials Science and EngineeringTsinghua UniversityBeijing 100084People’s Republic of China Beijing Advanced Innovation Center for Integrated Circuits Beijing 100084People’s Republic of China

As Moore’s law deteriorates,the research and development of new materials system are crucial for transitioning into the post Moore *** semiconductor materials,such as silicon,have served as the cornerstone of modern technologies for over half a *** has been due to extensive research and engineering on new techniques to continuously enrich silicon-based materials system and,subsequently,to develop better performed silicon-based ***,in the emerging post Moore era,layered semiconductor materials,such as transition metal dichalcogenides(TMDs),have garnered considerable research interest due to their unique electronic and optoelectronic properties,which hold great promise for powering the new era of next generation *** a result,techniques for engineering the properties of layered semiconductors have expanded the possibilities of layered semiconductor-based ***,there remain significant limitations in the synthesis and engineering of layered semiconductors,impeding the utilization of layered semiconductor-based devices for mass *** a practical alternative,heterogeneous integration between layered and traditional semiconductors provides valuable opportunities to combine the distinctive properties of layered semiconductors with well-developed traditional semiconductors materials ***,we provide an overview of the comparative coherence between layered and traditional semiconductors,starting with TMDs as the representation of layered *** highlight the meaningful opportunities presented by the heterogeneous integration of layered semiconductors with traditional semiconductors,representing an optimal strategy poised to propel the emerging semiconductor research community and chip industry towards unprecedented advancements in the coming decades.

关键词： heterogeneous integration van der Waals heterostructure post Moore era layered semiconductor transition metal dichalcogenide layered-traditional semiconductor heterostructure

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Ultralight Ppy@Pva/Bc/Mxene Composite Aerogels for High-Performance Supercapacitor Electrodes and Pressure Sensors

SSRN

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SSRN 2023年

作者： Zheng, Wenfeng Yang, Yuan Fan, Lingling Ye, Dezhan Xu, Weilin Xu, Jie State Key Lab for Hubei New Textile Materials and Advanced Processing Technology College of Materials Science & Engineering College of Textile Science & Engineering Wuhan Textile University Wuhan430200 China

Directional freezing is an efficient approach to design anisotropic materials with surface void and well-defined aligned channels along the freezing direction for charge transmission and ion diffusion. Herein, poly(vinyl alcohol) (PVA)/bacterial cellulose (BC)/MXene (PBM) composite aerogels are prepared via directional freezing. The aligned porous architecture of PBM not only enables uniform loading and high accessibility of PPy through the aerogel network, but also ensures efficient penetration and fast transport of electrolytes. The as-prepared PPy@PVA/BC/MXene (PPy@PBM) aerogel electrodes show a high areal specific capacitance of 3948 mF cm-2 at 0.47 mA cm-2, a desirable energy density 178 μWh cm-2 at a power density of 951 μW cm-2 and excellent cycling stability (105% capacitance retention after 5000 cycles). In addition, the PPy@PBM aerogels demonstrate high sensitivity (313.2 kPa-1 in 200 to 3000 Pa pressure range), ultralow detection limit ( © 2023, The Authors. All rights reserved.

关键词： Aerogels

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N‑Doped Graphene‑Decorated NiCo Alloy Coupled with Mesoporous NiCoMoO Nano‑sheet Heterojunction for Enhanced Water Electrolysis Activity at High Current Density

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Nano-Micro Letters 2021年第5期13卷 77-89页

作者： Guangfu Qian Jinli Chen Tianqi Yu Lin Luo Shibin Yin College of Chemistry and Chemical Engineering MOE Key Laboratory of New Processing Technology for Nonferrous Metals and MaterialsState Key Laboratory of Processing for Non‑Ferrous Metal and Featured MaterialsGuangxi University100 Daxue RoadNanning 530004P.R.China

Developing highly effective and stable non-noble metalbased bifunctional catalyst working at high current density is an urgent issue for water electrolysis(WE).Herein,we prepare the N-doped graphene-decorated NiCo alloy coupled with mesoporous NiCoMoO nano-sheet grown on 3D nickel foam(NiCo@C-NiCoMoO/NF)for water ***@C-NiCoMoO/NF exhibits outstanding activity with low overpotentials for hydrogen and oxygen evolution reaction(HER:39/266 mV;OER:260/390 mV)at±10 and±1000 mA cm^(−2).More importantly,in 6.0 M KOH solution at 60℃ for WE,it only requires 1.90 V to reach 1000 mA cm−2 and shows excellent stability for 43 h,exhibiting the potential for actual *** good performance can be assigned to N-doped graphene-decorated NiCo alloy and mesoporous NiCoMoO nano-sheet,which not only increase the intrinsic activity and expose abundant catalytic activity sites,but also enhance its chemical and mechanical *** work thus could provide a promising material for industrial hydrogen production.

关键词： N-doped graphene-decorated NiCo alloy Catalyst Mesoporous nano-sheet Water electrolysis High current density

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Photocatalytic water splitting versus H_(2) generation coupled with organic synthesis:A large critical review

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Chinese Journal of Catalysis 2025年第3期70卷 44-114页

作者： Oleksandr Savateev Jingru Zhuang Sijie Wan Chunshan Song Shaowen Cao Junwang Tang Department of Chemistry The Chinese University of Hong KongShatinNew TerritoriesHong KongChina State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070HubeiChina Industrial Catalysis Center Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

Photocatalytic water splitting using natural solar light is considered as a sustainable approach to generate H_(2) and O_(2).While H_(2) has high market value,the by-product of water splitting,oxygen,is less *** make H_(2) produced by means of photocatalysis more economically competitive to that generated from methane,its generation is studied together with synthesis of organic compounds that have higher market *** review summarizes and analyzes critically dehydrogenation reactions that were developed since *** dehydrogenation reactions are classified and the results are collected in the online *** of homogeneous and heterogenous photocatalysts in dehydrogenation reactions,such as yield rates of organic products on analytical and preparative scales,and quantum efficiencies are *** limitations of the existing methods and photocatalytic systems are identified and directions for the future developments are outlined.

关键词： Acceptorless dehydrogenation Photocatalysis Photoredox catalysis Hydrogen Organic synthesis

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