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Etching oxide overlayers of NiFe phosphide to facilitate surface reconstruction for oxygen evolution reaction

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Green Energy & Environment 2022年第3期7卷 365-371页

作者： Tehua wang Xian-Zhu Fu shuangyin wang College of Materials Science and Engineering Shenzhen UniversityShenzhen518055China College of Physics and Optoelectronic Engineering Shenzhen UniversityShenzhen518060China State Key Laboratory of Chem/Bio-sensing and Chemometrics College of Chemistry and Chemical EngineeringHunan UniversityChangsha410082China

Transition-metal phosphides have been of concern as efficient electrocatalysts for oxygen evolution reaction(OER)due to its high conductivity and earth-abundance ***,oxide overlayers formed on their surface by spontaneously atmospheric oxidation are usually neglected,thus confusing the establishment of structure–performance ***,we successfully etched the oxide overlayers of NiFe phosphide(NiFeP)by a dielectric barrier discharge(DBD)plasma technique,aiming to reveal the influence of the oxide overlayers on its electrocatalytic performance for *** is found that etching the oxide overlayers can accelerate the surface reconstruction process of NiFeP and facilitate the formation of metal hydroxides,which are key intermediate phases for ***,the etched NiFeP-DBD material shows remarkably enhanced OER activity with an overpotential of 265 mV at a current density of 10 mA cm^(-2).The finding of this work probably brings a significant impact to understand the structure–performance relationship of metal phosphide in electrooxidation reaction.

关键词： surface oxide evolution

Transforming Co3O4 nanosheets into porous N-doped CoxOy nanosheets with oxygen vacancies for the oxygen evolution reaction

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Journal of Energy Chemistry 2019年第8期28卷 24-29,I0002页

作者： Lei Xu Yuqin Zou Zhaohui Xiao shuangyin wang State Key Laboratory of Chem/Bio-Sensing and Chemometrics College of Chemistry and Chemical Engineering Hunan University

Cobalt oxides have been widely investigated as promising replacements for noble metal-based catalysts for oxygen evolution reaction(OER). Herein, we, for the first time, have obtained porous CoxOy nanosheets with N-doping and oxygen vacancies by etching Co3O4 nanosheets with NH3 plasma. Comparing with the pristine Co3O4 nanosheets(1.79 V), the porous CoxOy nanosheets with N-doping and oxygen vacancies have a much lower potential of 1.51 V versus RHE to reach the current density of 10 mA cm-2. The obtained sample has a lower Tafel slope of 68 m V dec-1 than the pristine Co3O4 nanosheets(234 mV dec-1).The disclosed Co^2+, which is responsible for the formation of active sites(CoOOH), N-doping and oxygen vacancies, gives rise to better performance of OER.

关键词： Electrocatalysts Oxygen evolution reaction Cobalt oxides N doping Oxygen vacancies

A Pair-Electrosynthesis for Formate at Ultra-Low Voltage Via Coupling of CO_(2) Reduction and Formaldehyde Oxidation

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Nano-Micro Letters 2022年第12期14卷 415-431页

作者： Mengyu Li Tehua wang Weixing Zhao shuangyin wang Yuqin Zou State Key Laboratory of Chemo/Bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringAdvanced Catalytic Engineering Research Center of the Ministry of EducationHunan UniversityChangsha 410082People’s Republic of China School of Chemistry and Chemical Engineering Jishou UniversityJishou 416000HunanPeople’s Republic of China

Formate can be synthesized electrochemically by CO_(2) reduction reaction(CO_(2)RR)or formalde-hyde oxidation reaction(FOR).The CO_(2)RR approach suffers from kinetic-sluggish oxygen evolution reac-tion at the *** this end,an electrochemical sys-tem combining cathodic CO_(2)RR with anodic FOR was developed,which enables the formate electrosynthesis at ultra-low *** CO_(2)RR employing the BiOCl electrode in H-cell exhibited formate Faradaic efficiency(FE)higher than 90% within a wide potential range from−0.48 to−1.32 V_(RHE).In flow cell,the current density of 100 mA cm^(−2) was achieved at−0.67 V_(RHE).The anodic FOR using the Cu_(2)O electrode displayed a low onset potential of−0.13 V_(RHE) and nearly 100%formate and H_(2) selectivity from 0.05 to 0.35 V_(RHE).The CO_(2)RR and FOR were constructed in a flow cell through membrane electrode assembly for the electrosynthesis of formate,where the CO_(2)RR//FOR delivered an enhanced current density of 100 mA cm^(−2) at 0.86 *** work provides a promising pair-electrosynthesis of value-added chemicals with high FE and low energy consumption.

关键词： Formate pair-electrolysis Electrochemical CO_(2)reduction Formaldehyde oxidation reaction Membrane electrode assembly Flow cell

Prospects of fuel cell technologies

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National Science Review 2017年第2期4卷 163-166页

作者： shuangyin wang San Ping Jiang State Key Laboratory of Chem/Bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringHunan University Fuels and Energy Technology Institute and Department of Chemical Engineering Curtin University

Fuel cells(FCs) are efficient and clean devices to electrochemically convert the chemical energy of fuels such as hydrogen,natural gas(NG),methanol,ethanol and hydrocarbons to electric energy with significantly high e... 详细信息

关键词： cell Prospects of fuel cell technologies PAFC PEMFC

The Nano Research Young Innovators(NR45)Awards in nanocatalysis

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Nano Research 2022年第12期15卷 9961-9966页

作者： Tierui Zhang shuangyin wang Ding Ma Key Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing100190China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing100049China State Key Laboratory of Chem/Bio-Sensing and Chemometrics Provincial Hunan Key Laboratory for Graphene Materials and DevicesCollege of Chemistry and Chemical EngineeringThe National Supercomputing Center in ChangshaHunan UniversityChangsha410082China Beijing National Laboratory for Molecular Sciences College of Chemistry and Molecular Engineering and College of Engineering and BIC-ESATPeking UniversityBeijing100871China

Nano Research Young Innovators(NR45)Awards aims to recognize young researchers under the age of 45 for their distinguished accomplishments and/or their great potential to make substantial contributions in various fields of nanoscience and *** the inaugural NR45 Awards launched in 2018,over a hundred innovators in nanobiotechnology,nanoenergy,and two-dimensional materials have been selected by the journal's editorial board[1-3].The 2022 NR45 Awards highlight the research topic of *** outstanding young innovators were selected for their extraordinary contributions to the development of well-designed metals,metal oxides,single-atoms,and carbon-based nanocatalysts for important catalytic reactions related to energy *** to all the 30 awardees in 2022!

关键词： journal accomplishment oxides

Defect engineering of electrocatalysts for organic synthesis

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Nano Research 2023年第2期16卷 1890-1912页

作者： Yuxuan Lu Ling Zhou shuangyin wang Yuqin Zou Key Laboratory of Chemo/Bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringAdvanced Catalytic Engineering Research Center of the Ministry of EducationHunan UniversityChangsha 410082China School of Chemistry and Chemical Engineering Jishou UniversityJishou 416000China

Electrocatalytic organic synthesis has attracted considerable research attention because it is an efficient and eco-friendly strategy for converting energy sources to value-added *** engineering is a promising strategy for regulating the electronic structure and charge density of *** endows electrocatalysts with excellent physical and physicochemical properties and optimizes the adsorption energy of the reaction intermediates to reduce the kinetic barriers of the electrosynthesis ***,the recent advances related to the use of electrocatalysts for organic synthesis with respect to defects are systematically *** roles of defects in anodic and cathodic reactions,such as the syntheses of alkanes,alkenes,alcohols,aldehydes,amides,and carboxylic acids,are ***,the relationship between the defective structure and electrocatalytic activity is discussed by combining experimental results and theoretical ***,the challenges,opportunities,and development prospects of defective electrocatalysts are examined to promote the development of the field of electrocatalytic organic *** review is expected to help understand the vital role of defects in catalytic processes and the controllable synthesis of efficient electrocatalysts for the production of high-value chemicals.

关键词： defect engineering electrocatalysts electrocatalytic organic synthesis energy conversion

Sub-2 nm IrO_(2)/Ir nanoclusters with compressive strain and metal vacancies boost water oxidation in acid

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Nano Research 2023年第1期16卷 334-342页

作者： Zhijuan Liu Guangjin wang Jinyu Guo shuangyin wang Shuang-Quan Zang Henan Key Laboratory of Crystalline Molecular Functional Materials Henan International Joint Laboratory of Tumor Theranostical Cluster MaterialsGreen Catalysis Centerand College of ChemistryZhengzhou UniversityZhengzhou 450001China Hunan University State Key Laboratory of Chem/Bio-sensing and ChemometricsCollege of Chemistry and Chemical EngineeringChangsha 410082China School of Materials Science and Energy Engineering Foshan UniversityFoshan 528000China

IrO_(2)exhibits good stability but limited electrocatalytic activity for oxygen evolution reaction in *** engineering is an effective strategy to improve the intrinsic ability of electrocatalysts by tailoring their electronic ***,we have successfully synthesized IrO_(2)/Ir heterophase with compressive strain and metal vacancies via a simple substitution-etching *** virtue of the solubility of Cr in strong alkali,metal vacancies could be formed at surface after etching Cr-doped IrO_(2)/Ir in alkali,which leaded to modulated electronic ***,the substitution of Cr with smaller atom radius would induce the formation of compressive strain and the relocated atoms made the d-band center *** the regulated electronic structure and tuned d-band center,the obtained electrocatalyst only needed 285 mV to reach 10 mA·cm^(−2)in 0.1 M *** kinetic has been rapidly accelerated as indicated by the smaller Tafel slope and charge transfer *** calculations revealed that the d-band center and charge density distribution have been regulated with the introduction of defects in IrO_(2)/Ir,which significantly decreased the free energy barrier of rate determining *** work provides a valuable reference to design effective and defects-rich electrocatalysts.

关键词： IrO_(2)/Ir nanoclusters compressive strain metal vacancies d-band center water oxidation in acid

Recent advances in defect electrocatalysts: Preparation and characterization

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Journal of Energy Chemistry 2021年第2期30卷 208-225,I0008页

作者： Zhaohui Xiao Chao Xie Yanyong wang Ru Chen shuangyin wang State Key Laboratory of Chem/Bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082HunanChina

the types and strategies used to prepare defect electrocatalysts will continue to be studied and developed as new defective materials are generated.4. Characterization of defectsThis review briefly summarizes recent progress in defect electrocatalysts, and the synthesis strategies and characterization techniques for defects are systematically discussed. Although challenges in the characterization of defect structures in the electrocatalytic reaction process remain, the dynamic evolution of defect sites is predicted to be helpful for designing and preparing high-performance electrocatalysts for commercial applications. Furthermore, due to an insufficient understanding of the defect-structureproperty relationships, future possibilities for the reasonable design of defect electrocatalysts to obtain desirable performance are suggested.

关键词： Defect Electrocatalysts Vacancies Heteroatom doping

Selective Electrocatalytic Hydrogenation of 5-Hydroxymethylfurfural to 2,5-Dihydroxymethylfuran on Bimetallic PdCu Alloy

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Chinese Journal of Structural Chemistry 2022年第5期41卷 63-69页

作者： Xu Yue Weixing Zhao shuangyin wang Yuqin Zou State Key Laboratory of Chem/Bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringAdvanced Catalytic Engineering Research Center of the Ministry of EducationHunan UniversityChangsha 410082China Shenzhen Institute of Hunan University Shenzhen 518057China

2,5-dihydroxymethylfuran(DHMF),obtained from 5-hydroxymethylfurfural(HMF)by electrochemical method,is a promising building block for ***,one challenge of this process is to reduce initial potential and improve catalytic *** this work,the PdCu bimetallic catalyst is prepared with an onset potential of-0.05 VRHE and a selectivity of 99%.Compared with the single Cu electrocatalyst,the adsorption of HMF and proton is improved by introducing of Pd,which is demonstrated by the electrochemical results and hydrogen production *** work provides an effective strategy to improve the selectivity of Cu-based electrocatalyst and builds a relationship between the adsorption capacity and the electrocatalytic performance.

关键词： biomass 2,5-dihydroxymethylfuran electrocatalyst bimetallic alloy hydrogenation