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Plasma induced grain boundaries to boost electrochemical reduction of CO2 to formate

Journal of Energy Chemistry 2024年第8期95卷 636-643页

作者： Guan Wang Shengtao Zhong Xiaoqian Xiong Jing Li Fangyuan Wang Li Huo Daoxiong Wu Xingqi Han Zhitong Wang Qi Chen Xinlong Tian Peilin Deng School of marine Science and Engineering State Key Laboratory of Marine Resource Utilization in South China Sea Hainan University

Bismuth-based catalysts are highly promising for the electrochemical carbon dioxide reduction reaction（eCO2RR） to formate product.However,achieving high activity and selectivity towards formate and ensuring long-term stability remains challenging.This work reports the oxygen plasma inducing strategy to construct the abundant grain boundaries of Bi/BiOxon ultrathin two-dimensional Bi nanosheets.The oxygen plasma-treated Bi nanosheet（OP-Bi） exhibits over 90% Faradaic efficiency（FE） for formate at a wide potential range from-0.5 to-1.1 V,and maintains a great stability catalytic performance without significant decay over 30 h in flow cell.Moreover,membrane electrode assembly（MEA） device with OPBi as catalyst sustains the robust current density of 100 mA cm-2over 50 h,maintaining a formate FE above 90%.In addition,rechargeable Zn-CO2battery presents the peak power density of1.22 mW cm-2with OP-Bi as bifunctional catalyst.The mechanism experiments demonstrate that the high-density grain boundaries of OP-Bi provide more exposed active sites,faster electron transfer capacity,and the stronger intrinsic activity of Bi atoms.In situ spectroscopy and theo retical calculations further elucidate that the unsaturated Bi coordination atoms between the grain boundaries can effectively activate CO2molecules through elongating the C-O bond,and reducing the formation energy barrier of the key intermediate（*OCOH）,thereby enhancing the catalytic performance of eCO2RR to formate product.

关键词： Bi nanosheet CO2 electroreduction Grain boundary MEA device Unsaturation Bi atoms

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A universal and ultrafast method for fabricating a library of nanocellulose-supported metal nanoparticles

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Progress in Natural Science:Materials International 2024年第2期34卷 389-395页

作者： Ziyi Luo Xiaoyang Wang Baihua Cui Hao Luo Tao Zhang Jia Ding Yanan Chen Yida Deng Wenbin Hu School of Materials Science and Engineering Tianjin University Department of Chemistry National University of Singapore state key laboratory of marine resource utilization in south china sea School of Materials Science and Engineering Hainan University

Using nanocatalysts to catalyze water electrolysis for hydrogen production is an ideal solution to address the energy crisis.The most well-adopted fabrication methods for nanocatalysts are tube furnace annealing,Hydrothermal method,etc.,hardly satisfying the trade-off among coarsening,dispersity,and particle size due to mutual restrictions.Herein,a universal,ultrafast and facile cellulose nanometer whiskers-high temperature shock（CNWHTS） method was reported for fabricating a library of ultrafine metal nanoparticles with uniform dispersion and narrow size distribution.The metal-anchor functional groups in CNW（i.e.,-OH and-COOH） and the characteristics of the HTS method for ultrafast heating and powerful quenching synergistically contribute to the successful synthesis of metal nanoparticles.As an initial demonstration,the as-prepared Pt nanocatalyst(η10 mA cm-2=51.8 mV) shows more excellent catalytic hydrogen evolution reaction（HER） performance than the Pt catalyst prepared in the tubular furnace(η10 mA cm-2=169.4 mV).This rapid and universal CNW-HTS method can pave the way for nanomanufacturing to produce high-quality metal nanoparticles,thereby expanding applications of energy conversion and electrocatalysis.

关键词： Electrocatalysis High-temperature shock Hydrogen evolution reaction (HER) Nanocellulose Nanomanufacturing Nanoparticles

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Accurate identification of glass crystallization helps in selecting high electronic conductivity materials

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Progress in Natural Science:Materials International 2024年第3期34卷 503-511页

作者： Fanhou Kong Shuli Li Suoqi Zhao Huiwen Li Lin Li Zhenting Zang Rui Zhang Hongrui Liu Lehan Wang Changjiu Li Keng H.Chung Dongying key laboratory of New Energy Materials and Devices & School of Chemical Engineering Shandong Institute of Petroleum and Chemical Technology Special Glass key Lab of Hainan Province & state key laboratory of marine resource utilization in south china sea Hainan University

Though the current research on vanadium-based glass electrodes has made great progress, the conductivity theory of V-based glasses has not been obviously improved and crystals cannot be positioned precisely. The changes in the valence state of V3+, V4+and V5+are regulated by the strong reducing agent Fe2P to realize valence bond transformation of the amorphous electrode, explore the redox process of multi-electron reactions and further optimize the conductivity of electrode materials. VPFe2 and VPFe3 precipitate VO2crystals and VPFe4 precipitates VO2and V6O11crystals. Electron back-scattered diffraction was used to accurately identify the distribution and specific positions of both types of crystals. V6O11crystals exhibit a strong texture according to pole figure and inverse pole figure. XPS reveals that Fe2P and V2O5, undergo a redox reaction during the hightemperature melting process, where V5+is reduced to V4+and V3+and V4+renders a positive influence on conductivity. The addition of Fe2P increases the content of V4+in the glass and VPFe3 glass contains the highest content of V4+, leading to the highest electronic conductivity. V2O5transforms into VO2crystals and VO2transforms into V6O11with the increase of Fe2P content. The type of nanocrystal precipitation in glass affects electronic conductivity.

关键词： Electron back-scattered diffraction Electronic conductivity Glass crystallization Multi-electron reactions V2O5

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Graphdiyne oxide substrate-enhanced peroxidase-mimicking performance of Ru nanoparticles with physiological pH preference

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Nano Research 2024年第3期17卷 1123-1131页

作者： Cong Xu Wenjie Ma Haozhi Wang Leihou Shao Weiqi Li Ping Yu Lanqun Mao Beijing National laboratory for Molecular Science Key Laboratory of Analytical Chemistry for Living BiosystemsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China state key laboratory of marine resource utilization in south china sea School of Materials Science and EngineeringHainan UniversityHaikou 570228China College of Chemistry Beijing Normal UniversityBeijing 100875China

Modulating electronic structure of metal nanoparticles via metal–support interaction has attracted intense interest in the field of catalytic science.However,the roles of supporting substrates in regulating catalytic properties of nanozymes remain elusive.In this study,we find that the use of graphdiyne oxide(GDYO)as the substrate for self-terminating growth of Ru nanoparticles(Ru@GDYO)endows the peroxidase-like activity of Ru nanoparticles with intrinsic physiological pH preference and natural horseradish peroxidase(HRP)comparable performance.Ru nanoparticles electrolessly deposited onto GDYO possess a partially oxidized electronic structure owing to limited charge transfer between Ru and GDYO,contributing to the intrinsic physiological pH preference of the peroxidase-mimicking nanozyme.More importantly,the substrate GDYO plays an influential factor in enhancing catalytic activity,that is,the activity of Ru@GDYO is much higher than that of Ru nanoparticles deposited on other carbon substrates including graphene oxides and graphdiyne.To demonstrate the application of Ru@GDYO nanozyme in neutral solutions,we employ Ru@GDYO with nicotinamide adenine dinucleotide(NAD+)-dependent dehydrogenases in physiological conditions to realize a sustainable cascade reaction by means of forming continuous NAD^(+)/dihydronicotiamide adenine dinucleotide(NADH)recycling.Our finding represents a promising perspective on designing high-performance peroxidase-mimicking nanozymes with broader applicability,raising fundamental understanding of structure–activity relationship,and investigating new applications of nanozymes in biological systems.

关键词： nanozyme graphdiyne reactive oxygen species electroless deposition metal–support interaction

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How the surface Cu layer affected the activity of Ni foil for alkaline hydrogen evolution

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Journal of Materials Science & Technology 2024年第2期169卷 11-18页

作者： Qingfeng Hu Yuan Liu Xuerong Zheng Jinfeng Zhang Jiajun Wang Xiaopeng Han Yida Deng Wenbin Hu School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of EducationTianjin UniversityTianjin 300072China state key laboratory of marine resource utilization in south china sea School of Materials Science and EngineeringHainan UniversityHaikou 570228China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207China

Synthesizing bimetallic nanomaterials,with noble metals as the surface layers and inert metals as the substrates,has been proven to be an effective way to reduce the use of noble metals with maintained catalytic activity.However,an atomic diffusion from the inert substrate to the surface during the long-term operation has been reported to significantly decrease the activity.In this work,a series of catalysis-inert Cu-coated Ni foil were fabricated through electrodeposition and their activities for alkaline hydrogen evolution were investigated.Notably,the Ni/Cu-60 sample showed a similar catalytic property with pure Ni foil and only a slight decrease in HER activity was observed.The X-ray photoelectron spectroscopy(XPS)results indicated a decreased electron concentration of Cu in Ni/Cu-60,and theoretical calculations further demonstrated the electron transfer between the Ni substrate and Cu layer.Our results reveal that a specific composition or structure of an inert metal layer might not significantly decrease the electrocatalytic activity of active metals.Moreover,there are more possibilities for the rational design of metal-based catalysts for electrocatalysis.

关键词： Bimetallic heterostructure Charge redistribution Water splitting Alkaline hydrogen evolution

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Phase transfer-based high-efficiency recycling of precious metal electrocatalysts

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Green Chemical Engineering 2024年第1期5卷 68-74页

作者： Qing Zeng Shaonan Tian Yu Zhang Hui Liu Dong Chen Xinlong Tian Chaoquan Hu Jun Yang state key laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing100190China state key laboratory of marine resource utilization in south china sea Hainan Provincial Key Lab of Fine ChemistrySchool of Chemical Engineering and TechnologyHainan UniversityHaikou570228China Nanjing IPE Institute of Green Manufacturing Industry Nanjing211100China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing100049China

Recycling precious metals with high-efficiency is undoubtedly beneficial to optimize resource utilization for environmental remediation and sustainable development.Herein,we report an efficient route to recycle the palladium(Pd)and platinum(Pt)electrocatalysts using a phase transfer method.This strategy involves acidic dissolution of deactivated precious metal(Pd/Pt)electrocatalysts from their loading substrates,mixing with an ethanolic solution of dodecylamine(DDA),subsequent extraction of metal ions into a non-polar organic phase,and final reduction by sodium borohydride to reproduce high-performance electrocatalysts towards typical electrochemical reactions,e.g.,oxygen reduction reaction(ORR)and ethanol oxidation reaction(EOR).In specific,the transfer efficiencies are up to 98%and the final recovery rate is over 85%for Pd and Pt electrocatalysts in each cycle.This approach symbolizes a facile and efficient way to recover precious metals,which might be applied to recycling a wide range of metals in various realms after appropriate modifications.

关键词： Precious metal Phase transfer Extraction Recovery Electrocatalyst

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Polyp-Canal Reconstruction Reveals Evolution Toward Complexity in Corals

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Research 2024年第1期2023卷 417-428页

作者： Yixin Li Xin Liao Xin Wang Yuanchao Li Hongwei Zhao Yunpeng Zhao Junyuan Chen Chunpeng He Zuhong Lu state key laboratory of Bioelectronics School of Biological Science and Medical EngineeringSoutheast UniversityNanjing 210096China state key laboratory of Coastal and Offshore Engineering Dalian University of TechnologyDalian 116024China Guangxi key Lab of Mangrove Conservation and utilization Guangxi Mangrove Research CenterGuangxi Academy of SciencesBeihai 536000China Hainan Academy of Ocean and Fishery Sciences Haikou 571126China state key laboratory of marine resources utilization in south china sea Hainan UniversityHaikou 570228China Nanjing Institute of Geology and Palaeontology Chinese Academy of Sciences39 East Beijing RoadNanjing 210008China

Modern scleractinian corals are classified into robust,complex,and basal clades through comparative molecular studies.However,only few morphological or biological criteria can systematically determine the evolutionary trajectories of these major scleractinian coral clades.Here,we obtained the structural information of 21 scleractinian coral species representing robust and complex clades:High-resolution micro-computed tomography was used to reconstruct the polyp-canal systems in their colonies and to visualize the dynamic polyp growth processes.We found that the emergence of mesh-like canals may distinguish representatives of complex and robust clades.The differences in polyp-canal connections suggest distinct evolutionary trajectories among coral species:The formation of the canal network promoted the development of more complex coral structures,and coral polyps within this network formed calices of very similar volume,following precise axial growth directions.The influence of individual polyps on the coral colony becomes less significant as coral structures become more complex,and coral species with more complicated polyp-canal systems occupied niches more efficiently.This work supplements current evolutionary studies on reef-building corals,providing insight for further studies on coral growth patterns.

关键词： Coral representing directions

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The corrosion characteristic and mechanism of Mg-5Y-1.5Nd-xZn-0.5Zr(x=0,2,4,6 wt.%)alloys in marine atmospheric environment

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Journal of Magnesium and Alloys 2024年第1期12卷 139-158页

作者： Quantong Jiang Dongzhu Lu Liren Cheng Nazhen Liu Baorong Hou CAS key laboratory of marine Environmental Corrosion and Bio-fouling Institute of OceanologyChinese Academy of SciencesNo.7 Nanhai RoadQingdao 266071PR China state key laboratory of Rare Earth resource utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesNo.5625 Renmin StreetChangchun 130022PR China Open Studio for marine Corrosion and Protection Pilot National Laboratory for Marine Science and Technology(Qingdao)No.1 Wenhai RoadQingdao 266071PR China Sanya Institute of Oceanology South China Sea Institute of OceanologyChinese Academy of SciencesZhenzhou RoadSanya 572000PR China

The microstructure and precipitated phases of as-cast Mg-5Y-1.5Nd-x Zn-0.5Zr(x=0,2,4,6 wt.%)alloys were investigated by optical microscopy,scanning electron microscopy,energy-dispersive spectrometry and X-ray Diffraction.The exposure corrosion experiment of these magnesium alloys was tested in south china sea and KEXUE vessel atmospheric environment.The corrosion characteristic and mechanism of magnesium alloys of Mg-5Y-1.5Nd-x Zn-0.5Zr(x=0,2,4,6 wt.%)alloys were analyzed by weight loss rate,corrosion depth,corrosion products and corrosion morphologies.The electrochemical corrosion tests were also measured in the natural seawater.The comprehensive results showed that Mg-5Y-1.5Nd-4Zn-0.5Zr magnesium alloy existed the best corrosion resistance whether in the marine atmospheric environment and natural seawater environment.That depended on the microstructure,type and distribution of precipitated phases in Mg-5Y-1.5Nd-4Zn-0.5Zr magnesium alloy.Sufficient quantity anodic precipitated phases in the microstructure of Mg-5Y-1.5Nd-4Zn-0.5Zr alloy played the key role in the corrosion resistance.

关键词： marine atmospheric environment Exposure corrosion Magnesium alloy Corrosion rate Corrosion mechanism

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In-situ Generation of Hydroxyl Layers in Coo@FeSe_(2) Catalyst for High Selectivity seawater Electrolysis

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Chinese Journal of Chemistry 2024年第1期42卷 48-54,I0004页

作者： Suyang Feng Peng Rao Xiao Wu Ke Li Anyuan Qi Yanhui Yu Jing Li Peilin Deng Yuliang Yuan Shaolei Wang Xinlong Tian Zhenye Kang state key laboratoryof marine resource utilization in south china sea Hainan Provincial Key Lab of Fine ChemistrySchoolof Chemical Engineering andTechnologyHainan UniversityHaikouHainan 570228China key Laboraory of Polyoxmetalate andReticular Material Chemtry of Ministy of Education School of Chmistry Northeast NormalUniversity ChangchunJilin 130024China National Energy Group Ledong Power Generation Co. Ltd.LedongHainan 572539China

seawater electrolysis holds great promise for hydrogen production in the future,while the development of anodic catalysts has been severely hampered by the side-reaction,chloride evolution reaction.In this work,nano-flower-cluster structured Coo@FeSe_(2)/CF catalysts are synthesized via a scalable electrodeposition technique,and the performance is systematically studied.The oxygen evolution reaction(OER)overpotential of Co0@FeSe_(2)/CF is 267 mV at 100 mA.cm^(-2),which is significantly lower than that of the IrO_(2) catalyst(435 mV).Additionally,the catalyst shows high selectivity for OER(97.9%)and almost no loss of activity after a durability test for 1100 h.The impressive performance is attributed to the dense rod-like structure with abundant active centers after electrochemical activation and the in-situ generated CoOOH and FeOOH that improve the catalytic activity of the catalyst.The synergistic effect induced bythenon-uniform structureendows the catalyst with excellent stability.

关键词： Energy Transfer seawat erelectrolysis Oxygen evolution reaction Electrodeposition method CoO@FeSe_(2)/CF catalyst Nano-flower-cluster structure Catalytic activity

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A strategy based on water soluble coal tar pitches to construct MnO_(2)@C composite materials with high electrochemical performance

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Science china(Technological Sciences) 2024年第1期67卷 311-320页

作者： LIU Bo WANG Kun GUO ZhaoQi HAN BeiBei XU GuiYing JU DongYing AN BaiGang LI YongCheng NI ZhenYong ZHOU WeiMin key laboratory of Energy Materials and Electrochemistry Research Liaoning Province University of Science and Technology LiaoningAnshan 114051China Advanced Science Research laboratory Saitama Institute of TechnologyFusaiji 1690Japan Liaoning Starry Sky Sodium Battery Co. Ltd.Anshan 114051China Sinosteel Anshan Research Institute of Thermo-Energy Co. Ltd.Anshan 114051China state key laboratory of marine resource utilization in south china sea Hainan Provincial Key Lab of Fine ChemistrySchool of Chemical Engineering and TechnologyHainan UniversityHaikou 570228China key laboratory of Advanced Fuel Cells and Electrolyzers Technology of Zhejiang Province Ningbo Institute of Materials Technology and EngineeringChinese Academy of SciencesNingbo 315201China

The water soluble coal tar pitches(WS-CTPs)were successfully prepared and used to construct the MnO_(2)@C composite materials by a hydrothermal method.It is interestingly observed that the structures and morphologies of MnO_(2)@C materials can be controlled by controlling the dosages of WS-CTPs and KMnO4.Meanwhile,it is aware that MnO_(2)exists in the MnO_(2)@C materials in an amorphous state.Compared with MnO_(2),MnO_(2)@C materials output a remarkable improvement in electrochemical performance.For instance,MnO_(2)@C-0.3 shows the storage capacity at 965.7 mA h g^(−1)after 300 cycles at a current density of 0.1 A g^(−1).In addition,after 600 cycles at a current density of 1.0 A g^(−1),the storage capacity of MnO_(2)@C-0.3 still keeps 450.3 mA h g^(−1),indicating that MnO_(2)@C-0.3 owns tremendous cycle stability at a high current density.In view of the fact that the coal tar pitches possess great cost advantages,the strategy of using WS-CTPs as a carbon source to cover the metal oxides is a competitive way to expand the application of metal oxides in the fabrication of electrodes of LIBs.

关键词： water soluble coal tar pitches MnO_(2) composite materials lithium ion batteries(LIBs) energy storage systems(ESSs) coal tar pitches

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