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Hetero‑Interfaces on Cu Electrode for Enhanced Electrochemical Conversion of CO_(2)to Multi‑Carbon Products

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Nano-Micro Letters 2022年第8期14卷 181-193页

作者： Xiaotong Li Jianghao Wang Xiangzhou Lv Yue Yang Yifei Xu Qian Liu hao bin wu Institute for Composites Science Innovation(InCSI)and State Key Laboratory of Silicon Materials School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China

Electrochemical CO_(2)reduction reaction(CO_(2)RR)to multi-carbon products would simultaneously reduce CO_(2)emission and produce high-value ***,we report Cu electrodes modified by metal–organic framework(MOF)exhibiting enhanced electrocatalytic performance to convert CO_(2) into ethylene and *** Zr-based MOF,UiO-66 would in situ transform into amorphous ZrOx nanoparticles(a-ZrO_(x)),constructing a-ZrOx/Cu hetero-interface as a dual-site *** Faradaic efficiency of multi-carbon(C2+)products for optimal UiO-66-coated Cu(0.5-UiO/Cu)electrode reaches a high value of 74%at−1.05 V versus *** intrinsic activity for C2+products on 0.5-UiO/Cu electrode is about two times higher than that of Cu *** situ surface-enhanced Raman spectra demonstrate that UiO-66-derived a-ZrO_(x)coating can promote the stabilization of atop-bound CO^(*)intermediates on Cu surface during CO_(2)electrolysis,leading to increased CO^(*)coverage and facilitating the C–C coupling *** present study gives new insights into tailoring the adsorption configurations of CO_(2)RR intermediate by designing dual-site electrocatalysts with hetero-interfaces.

关键词： CO_(2)reduction reaction Metal–organic frameworks Copper Hetero-interfaces Multi-carbon products

Janus Quasi‑Solid Electrolyte Membranes with Asymmetric Porous Structure for High‑Performance Lithium‑Metal Batteries

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Nano-Micro Letters 2024年第6期16卷 221-232页

作者： Zerui Chen Wei Zhao Qian Liu Yifei Xu Qinghe Wang Jinmin Lin hao bin wu Institute for Composites Science Innovation(InCSI)and State Key Laboratory of Silicon and Advanced Semiconductor Materials School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China

Quasi-solid electrolytes(QSEs)based on nanoporous materials are promising candidates to construct high-performance Limetal batteries(LMBs).However,simultaneously boosting the ionic conductivity(σ)and lithium-ion transference number(t^(+)) of liquid electrolyte confined in porous matrix remains ***,we report a novel Janus MOFLi/MSLi QSEs with asymmetric porous structure to inherit the benefits of both mesoporous and microporous *** Janus QSE composed of mesoporous silica and microporous MOF exhibits a neat Li^(+) conductivity of 1.5.10^(–4)S cm^(−1) with t^(+) of 0.71.A partially de-solvated structure and preference distribution of Li^(+)near the Lewis base O atoms were depicted by MD ***,the nanoporous structure enabled efficient ion flux regulation,promoting the homogenous deposition of Li^(+).When incorporated in Li||Cu cells,the MOFLi/MSLi QSEs demonstrated a high Coulombic efficiency of 98.1%,surpassing that of liquid electrolytes(96.3%).Additionally,NCM 622||Li batteries equipped with MOFLi/MSLi QSEs exhibited promising rate performance and could operate stably for over 200 cycles at 1 *** results highlight the potential of Janus MOFLi/MSLi QSEs as promising candidates for next-generation LMBs.

关键词： Metal-organic frameworks Mesoporous silicas Quasi-solid electrolytes Janus structure Lithium-metal battery

Phosphorus-doping and oxygen vacancy endowing anatase TiO_(2) with excellent sodium storage performance

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Rare Metals 2022年第4期41卷 1284-1293页

作者： Hong-Shun Zhao Yan-Li Qi Kang Liang Wei-Kai Zhu hao-bin wu Jian-bin Li Yu-Rong Ren School of Materials Science and Engineering Changzhou UniversityChangzhou 213164China Changzhou Key Laboratory of Intelligent Manufacturing and Advanced Technology for Power Battery Changzhou 213164China Jiangsu Province Engineering Research Center of Intelligent Manufacturing Technology for the New Energy Vehicle Power Battery Changzhou 213164China Institute for Composites Science Innovation(InCSI) School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027China

Titanium dioxide is considered to be promising anode for sodium-ion batteries due to stable structure during the charge/discharge ***,its practical application is hindered by the slow electron/ion ***,phosphorus-doped anatase TiO_(2) nanoparticles with oxygen vacancies are successfully synthesized and utilized as high-performance sodium-storage *** dual strategy of phosphorus-doping and oxygen vacancies can concurrently boost electronic conductivity and adjust ion diffusion *** significantly contribute to the improved rate performance(167 mAh·g^(-1) at 20.0C)and stable cycling(95.9%after 2000 cycles at 20.0C).The proposed dual strategy can be potentially used to improve other oxide anodes for rechargeable batteries.

关键词： Titanium dioxide Phosphorus doping Oxygen vacancy Anode Sodium-ion batteries

Metal–Organic Framework-Assisted Synthesis of Compact Fe_2O_3 Nanotubes in Co_3O_4 Host with Enhanced Lithium Storage Properties

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Nano-Micro Letters 2018年第3期10卷 70-78页

作者： Song Lin Zhang Bu Yuan Guan hao bin wu Xiong Wen David Lou School of Chemical and Biomedical Engineering Nanyang Technological University School of Materials Science and Engineering Zhejiang University

Transition metal oxides are promising candidates for the high-capacity anode material in lithium-ion *** electrochemical performance of transition metal oxides can be improved by constructing suitable composite architectures. Herein, we demonstrate a metal–organic framework(MOF)-assisted strategy for the synthesis of a hierarchical hybrid nanostructure composed of Fe_2O_3 nanotubes assembled in Co_3O_4 host. Starting from MOF composite precursors(Fe-based MOF encapsulated in a Cobased host matrix), a complex structure of Co_3O_4 host and engulfed Fe_2O_3 nanotubes was prepared by a simple annealing treatment in air. By virtue of their structural and compositional features, these hierarchical composite particles reveal enhanced lithium storage properties when employed as anodes for lithium-ion batteries.

关键词： Metal–organic framework(MOF) Hierarchical structures Fe2O3 nanotubes Co3O4 Lithium-ion batteries(LIBs)

Zeolite-mediated hybrid Cu^(+)/Cu~0 interface for electrochemical nitrate reduction to ammonia

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Journal of Energy Chemistry 2023年第12期87卷 136-143,I0005页

作者： Jiabao Lv Angjian wu Liang Wang Yunhao Zhong Zhihao Zeng Qunxing Huang Xiaoqing Lin hao Zhang Shaojun Liu Qian Liu Songqiang Zhu Xiaodong Li Jianhua Yan Zhifu Qi hao bin wu State Key Laboratory of Clean Energy Utilization Zhejiang UniversityHangzhou 310027ZhejiangChina Baima Lake Laboratory Hangzhou 310053ZhejiangChina Laboratory of Clean Energy and Carbon Neutrality of Zhejiang Province Jiaxing Research InstituteZhejiang UniversityJiaxing 314031ZhejiangChina Key Lab of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027ZhejiangChina Institute for Composites Science Innovation(InCSI)and State Key Laboratory of Silicon Materials School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027ZhejiangChina

The electrocatalytic conversion of reactive nitrogen species to ammonia is a promising strategy for efficient NH_(3) *** this study,we reveal that the hybrid Cu^(+)/Cu~0 interface is catalytically active for electrochemical ammonia synthesis from nitrate *** maintain the hybrid Cu^(+)/Cu~0 state at negative reaction potentials,hydrophilic zeolite is used to modify Cu/Cu_(2)O electrocatalyst,which demonstrates an impressive NH_(3) production rate of 41.65 mg h^(-1) cm^(-2)with ~100% Faradaic efficiency of ammonia synthesis at-0.6 V ***-situ Raman spectroscopy unveil the high activity originates from the zeolite reconstruction at the electrode–electrolyte interface,which protects the valence state of Cu~0/Cu^(+) site under negative potential and promotes electrochemical activity towards NH_(3) synthesis.

关键词： Electrochemical nitrate reduction reaction Ammonia synthesis In-situ Raman spectroscopy Zeolite Density functional theory

Solvent sieving separators implement dual electrolyte for highvoltage lithium-metal batteries

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Nano Research 2023年第4期16卷 4901-4907页

作者： Yan Liu Qianqian Liu Youran Hong Yifei Xu Zerui Chen Wei Zhao Zhikun Hu Jiangwei Wang hao bin wu School of Materials Science and Engineering Zhejiang UniversityHangzhou 310027China

Lithium-metal batteries(LMBs)based on high-voltage cathodes would deliver high specific energy density to meet the demand of future energy ***,developing liquid electrolytes with wide electrochemical window for high-energy LMBs is intrinsically ***,we demonstrate metal-organic framework-functionalized separators(PE@MOF)with solvent sieving capability that implement dual electrolyte for *** capability of PE@MOF separator to block the diffusion of liquid electrolytes has been *** PE@MOF separator notably suppresses solvents shuttling,enabling the independent optimization of cathode-electrolyte and anode-electrolyte *** adapting commercial carbonate and ether electrolytes on cathode and anode sides,respectively,robust cathode-electrolyte interphase(CEI)and solid electrolyte interface(SEI)have been built on both *** lifespan of LiCoO_(2)(LCO)|Li full cell has been notably extended when using dual electrolyte and the solvent-sieving PE@MOF *** work demonstrates a new strategy to separately optimize the local environments at electrodes and to develop high-energy LMBs using low-cost and commercially available electrolytes.

关键词： dual electrolyte metal-organic framework lithium metal battery

Electrocatalytic CO_(2) reduction to C_(2)H_(4): From lab to fab

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Journal of Energy Chemistry 2024年第3期90卷 540-564,I0012页

作者： Zeyu Guo Fabao Yang Xiaotong Li Huiwen Zhu Hainam Do Kam Loon Fow Jonathan D.Hirst Tao wu Qiulin Ye Yaqi Peng hao bin wu Angjian wu Mengxia Xu Department of Chemical and Environmental Engineering and New Materials InstituteUniversity of Nottingham Ningbo ChinaNingbo 315100ZhejiangChina Key Laboratory of Carbonaceous Waste Processing and Process Intensification of Zhejiang Province University of Nottingham Ningbo ChinaNingbo 315100ZhejiangChina Nottingham Ningbo China Beacons of Excellence Research and Innovation Institute University of Nottingham Ningbo ChinaNingbo 315100ZhejiangChina State Key Laboratory of Clean Energy Utilization Department of Energy EngineeringZhejiang UniversityHangzhou 310027ZhejiangChina Institute for Composites Science Innovation(InCSI)and State Key Laboratory of Silicon and Advanced Semiconductor Materials School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027ZhejiangChina School of Chemistry University of NottinghamUniversity ParkNottingham NG72RDUK Baima Lake Laboratory Hangzhou 310053ZhejiangChina

The global concerns of energy crisis and climate change,primarily caused by carbon dioxide(CO_(2)),are of utmost ***,the electrocatalytic CO_(2) reduction reaction(CO_(2)RR) to high value-added multi-carbon(C_(2+)) products driven by renewable electricity has emerged as a highly promising solution to alleviate energy shortages and achieve carbon *** these C_(2+) products,ethylene(C_(2)H_(4))holds particular importance in the petrochemical ***,this review aims to establish a connection between the fundamentals of electrocatalytic CO_(2) reduction reaction to ethylene(CO_(2)RRto-C_(2)H_(4)) in laboratory-scale research(lab) and its potential applications in industrial-level fabrication(fab).The review begins by summarizing the fundamental aspects,including the design strategies of high-performance Cu-based electrocatalysts and advanced electrolyzer ***,innovative and value-added techniques are presented to address the inherent challenges encountered during the implementations of CO_(2)RR-to-C_(2)H_(4) in industrial ***,case studies of the technoeconomic analysis of the CO_(2)RR-to-C_(2)H_(4) process are discussed,taking into factors such as costeffectiveness,scalability,and market *** review concludes by outlining the perspectives and challenges associated with scaling up the CO_(2)RR-to-C_(2)H_(4) *** insights presented in this review are expected to make a valuable contribution in advancing the CO_(2)RR-to-C_(2)H_(4) process from lab to fab.

关键词： CO_(2) electroreduction reaction Ethylene Gas diffusion electrode Machine learning Density functional theory Techno-economic analysis

Quasi-solid electrolyte membranes with percolated metal–organic frameworks for practical lithium-metal batteries

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Journal of Energy Chemistry 2021年第1期30卷 354-360,I0012页

作者： Zijian Li Qianqian Liu Lina Gao Yifei Xu Xueqian Kong Yang Luo Huaxin Peng Yurong Ren hao bin wu School of Materials Science and Engineering Jiangsu Collaborative Innovation Center of Photovolatic Science and EngineeringChangzhou UniversityChangzhou 213164JiangsuChina School of Materials Science and Engineering Zhejiang UniversityHangzhou 310027ZhejiangChina Department of Chemistry Zhejiang UniversityHangzhou 310027ZhejiangChina

High-energy Li-metal batteries (LMBs) suffer from short cycle life and safety issues due to severe parasitic reactions and dendrite growth of Li metal anode (LMA) in liquid electrolytes [1–3].It is generally believed that replacing liquid electrolytes with solidstate electrolytes (SSEs) would be a feasible approach for practical LMBs [4,5]. Conventional SSEs including ceramic and polymer electrolytes have been studied for decades.

关键词： Solid electrolyte Composite membrane Metal-organic framework Lithium metal anode Lithium-metal battery

Quasi‑Solid Electrolyte Interphase Boosting Charge and Mass Transfer for Dendrite‑Free Zinc Battery

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Nano-Micro Letters 2023年第4期15卷 223-237页

作者： Xueer Xu Yifei Xu Jingtong Zhang Yu Zhong Zhongxu Li Huayu Qiu hao bin wu Jie Wang Xiuli Wang Changdong Gu Jiangping Tu State Key Laboratory of Silicon Materials Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang Provinceand School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China Institute for Composites Science Innovation(InCSI)and State Key Laboratory of Silicon Materials School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China Qingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao 266101People’s Republic of China Zhejiang Laboratory Hangzhou 311100People’s Republic of China Department of Engineering Mechanics School of Aeronautics and AstronauticsZhejiang UniversityHangzhou 310027People’s Republic of China

The practical applications of zinc metal batteries are plagued by the dendritic propagation of its metal anodes due to the limited transfer rate of charge and mass at the electrode/electrolyte *** enhance the reversibility of Zn metal,a quasi-solid interphase composed by defective metal-organic framework(MOF)nanoparticles(D-UiO-66)and two kinds of zinc salts electrolytes is fabricated on the Zn surface served as a zinc ions ***,anions in the aqueous electrolytes could be spontaneously anchored onto the Lewis acidic sites in defective MOF *** the synergistic effect between the MOF channels and the anchored anions,Zn^(2+)transport is prompted ***,such quasi-solid interphase boost charge and mass transfer of Zn^(2+),leading to a high zinc transference number,good ionic conductivity,and high Zn^(2+)concentration near the anode,which mitigates Zn dendrite growth ***,unprecedented average coulombic efficiency of 99.8%is achieved in the Zn||Cu cell with the proposed quasi-solid *** cycling performance of D-UiO-66@Zn||MnO_(2)(~92.9%capacity retention after 2000 cycles)and D-UiO-66@Zn||NH_(4)V_(4)O_(10)(~84.0%capacity retention after 800 cycles)prove the feasibility of the quasi-solid interphase.

关键词： Mass transfer Defect engineering Quasi-solid electrolyte interphase Zinc metal anode Zinc batteries