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International Journal of Minerals,Metallurgy and Materials 2024年第4期31卷 803-811页

作者： Xiaoyan Wang Safeer Jan Zhiyong Wang Xianbo Jin College of Chemistry and Molecular Sciences Hubei Key Laboratory of Electrochemical Power SourcesWuhan UniversityWuhan 430072China Engineering Research Center of Organosilicon Compounds&Materials Ministry of EducationWuhan 430072China

CO_(2) electrochemical reduction(CO_(2)ER)is an important research area for carbon neutralization.However,available catalysts for CO_(2) reduction are still characterized by limited stability and activity.Recently,metallic bismuth(Bi)has emerged as a promising catalyst for CO_(2) ER.Herein,we report the solid cathode electroreduction of commercial micronized Bi2O3as a straightforward approach for the preparation of nanostructured Bi.At-1.1 V versus reversible hydrogen electrode in a KHCO3aqueous electrolyte,the resulting nanostructure Bi delivers a formate current density of~40 mA·cm^(-2) with a current efficiency of~86%,and the formate selectivity reaches97.6% at-0.78 V.Using nanosized Bi2O3as the precursor can further reduce the primary particle sizes of the resulting Bi,leading to a significantly increased formate selectivity at relatively low overpotentials.The high catalytic activity of nanostructured Bi is attributable to the ultrafine and interconnected Bi nanoparticles in the nanoporous structure,which exposes abundant active sites for CO_(2) electrocatalytic reduction.

关键词： bismuth carbon dioxide electrocatalysis formate solid electroreduction

High-entropy selenides: A new platform for highly selective oxidation of glycerol to formate and energy-saving hydrogen evolution in alkali-acid hybrid electrolytic cell

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Nano Research 2023年第8期16卷 10832-10839页

作者： Hu Yao Yibo Wang Yinan Zheng Xin Yu Junjie Ge Yonghong Zhu Xiaohui Guo Key Lab of Synthetic and Natural Functional Molecule Chemistry of Ministry of Education The College of Chemistry and Materials ScienceNorthwest UniversityXi’an 710069China Changchun Institute of Applied Chemistry Changchun 130022China School of Chemical Engineering Northwest UniversityXi’an 710069China

Glycerol oxidation reaction(GOR)coupled with hydrogen generation simultaneously is a promising strategy for developing sustainable energy conversion technologies,but the complexity of glycerol oxidation products and the high coupling hydrogen evolution potential limit its wide application.In this paper,a self-supported high-entropy selenide electrode can be fabricated via a simple hydrothermal process.Then,the prepared electrode as an advanced catalyst displays optimal catalytic activity(1.20 V at 10 mA·cm^(−2))and high selectivity for the formation of formate in GOR.The results show that the lattice distortion effect of high entropy materials composed of multiple elements is mainly responsible for the greatly improved catalytic activity and selectivity for GOR.Moreover,an advanced alkali-acid hybrid electrolytic cell was assembled that enables efficient energy-saving hydrogen generation and GOR simultaneously.Herein,the electrolyzer requires only 0.5 V applied voltage to reach 10 mA·cm^(−2) for hydrogen generation and maintains long-term operation stability.

关键词： high-entropy selenides lattice distortion glycerol oxidation reaction(GOR) formate activity

Regulating Ni site in NiV LDH for efficient electrocatalytic production of formate and hydrogen by glycerol electrolysis

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Rare Metals 2022年第5期41卷 1583-1594页

作者： Lin Dong Guan-Ru Chang Yi Feng Xian-Zhi Yao Xin-Yao Yu Key Laboratory of Structure and Functional Regulation of Hybrid Materials Institutes of Physical Science and Information TechnologyAnhui UniversityMinistry of Education.Hefei 230601China School of Chemistry and Chemical Engineering Huangshan UniversityHuangshan 245041China Department of Polymer Materials and Engineering Academy of Chemical EngineeringHebei University of TechnologyTianjin 300130China Ningbo Research Institute of Ecological and Environmental Sciences Ningbo 315000China Energy Materials and Devices Key Laboratory of Anhui Province for Photoelectric Conversion Anhui UniversityHefei 230601China

Energy-saving glycerol electrolysis with lower potential than water spitting endows a promising way for the concurrent production of value-added formate and high-purity hydrogen. However, there is still lack of efficient electrocatalysts at both anode and cathode for glycerol electrolysis. Herein, we report the activation of Ni site in NiV layered double hydroxide(LDH) by electrochemical and N_(2)/H_(2) plasma regulations for boosting the activity of glycerol oxidation reaction(GOR) and hydrogen evolution reaction(HER), respectively. Specifically, boosted GOR performance with a low overpotential(1.23 V at 10 mA·cm^(-2)) and a high Faradic efficiency(94%) is demonstrated by electrochemically regulated NiV LDH(ENiV LDH) with elevated valence state of Ni site. In situ Raman spectrum reveals the generation of Ni(Ⅲ) species by electrochemical regulation, and the highly active Ni(Ⅲ)can be regenerated with the process of electrochemical oxidation. Additionally, the possible reaction pathway is speculated based on the in situ Fourier transform infrared spectroscopy(FTIR) and high-performance liquid chromatography results. The plasma-regulated NiV LDH(PNiV LDH) with lower valence state of Ni site exhibits outstanding HER activity, displaying a low overpotential of 45 m V to deliver 10 mA·cm^(-2).When employing E-NiV LDH and P-NiV LDH as anode and cathode electrocatalyst, respectively, the assembled electrolyzer merely needs 1.25 V to achieve 10 m A·cm^(-2) for simultaneous production of formate and hydrogen, demonstrating remarkable 320 mV of lower potential than water electrolysis.

关键词： Glycerol electrolysis Glycerol oxidation reaction Hydrogen evolution reaction NiV LDH formate

In-situ constructing Cu_(1)Bi_(1)bimetallic catalyst to promote the electroreduction of CO_(2)to formate by synergistic electronic and geometric effects

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Journal of Energy Chemistry 2023年第4期79卷 263-271页

作者： Houan Ren Xiaoyu Wang Xiaomei Zhou Teng Wang Yuping Liu Cai Wang Qingxin Guan Wei Li College of Chemistry State Key Laboratory of Elemento-Organic ChemistryKey Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)Nankai UniversityTianjin 300071China

Electrochemical CO_(2)reduction to formate is a potential approach to achieving global carbon neutrality.Here,Cu1Bi1bimetallic catalyst was prepared by a co-precipitation method.It has a ginger like composite structure(CuO/CuBi_(2)O_(4))and exhibited a high formate faradaic efficiency of 98.07%at–0.98 V and a large current density of–56.12 mA.cm^(-2)at–1.28 V,which is twice as high as Bi2O3catalyst.Especially,high selectivity(FE^(–)_(HCOO)>85%)is maintained over a wide potential window of 500 mV.In-situ Raman measurements and structure characterization revealed that the reduced Cu1Bi1bimetallic catalyst possesses abundant Cu-Bi interfaces and residual Bi-O structures.The abundant Cu-Bi interface structures on the catalyst surface can provide abundant active sites for CO_(2)RR,while the Bi-O structures may stabilize the CO_(2)^(*–)intermediate.The synergistic effect of abundant Cu-Bi interfaces and Bi-O species promotes the efficient synthesis of formate by following the OCHO^(*)pathway.

关键词： CO_(2)electroreduction Bimetallic catalyst formate Cu-Bi interfaces Bi-O structure

In-situ electrochemical restructuring of Cu_(2)BiS_(x)solid solution into Bi/Cu_(x)S_(y)heterointerfaces enabling stabilization intermediates for high-performance CO_(2)electroreduction to formate

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Nano Research 2023年第5期16卷 7974-7981页

作者： Xiaofeng Yang Qinru Wang Feiran Chen Hu Zang Changjiang Liu Nan Yu Baoyou Geng College of Chemistry and Materials Science the Key Laboratory of Electrochemical Clean Energy of Anhui Higher Education InstitutesAnhui Provincial Engineering Laboratory for New-Energy Vehicle Battery Energy-Storage MaterialsAnhui Normal UniversityWuhu 241002China Institute of Energy Hefei Comprehensive National Science CenterHefei 230031China

Bismuth-based materials are prevalent catalysts for CO_(2)electroreduction to formate,enduring high hydrogen evolution reactions and inadequate activity and stability.Herein,we reveal that in-situ electrochemical transformation of Cu_(2)BiS_(x)solid solution into Bi/Cu_(x)S_(y)heterointerfaces,which can stabilize the intermediates and achieve highly selective and consistent CO_(2)electroreduction.It shows over 85%Faraday efficiency(FE)of formate with a potential window of−0.8 to−1.2 VRHE(RHE:reversible hydrogen electrode)and a stability above 90%over 27 h in H-type cell at−0.9 VRHE.It maintains more than 85%of FEformate at the current density of−25 to−200 mA·cm^(−2),has stability of about 80%of FEformate at least 10 h at−150 mA·cm^(−2)in flow cell.In-situ Fourier transform infrared(FT-IR)spectroscopy measurement confirms that the preferred route of catalytic reaction is to generate *CO_(2)^(−) and *OCHO intermediates.The density functional theory(DFT)calculations illustrate that heterointerfaces facilitate the prior process of CO_(2)to HCOOH through *OCHO by additional Bi hybrid orbitals.This study is expected to open up a new idea for the design of CO_(2)electroreduction catalyst.

关键词： in-situ electrochemical restructuring heterointerfaces CO_(2)electroreduction formate current density

反钙钛矿结构氮化铜纳米片实现高效电催化甲醇氧化转化为甲酸盐

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Science China Materials 2023年第5期66卷 1820-1828页

作者：赵磊孙啟焦李懋钟亚霏沈沛祺林运祥徐坤 School of Chemistry and Chemical Engineering Key Laboratory of Functional Inorganic Material Chemistry of Anhui ProvinceAnhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized MaterialsKey Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationAnhui UniversityHefei 230601China Institutes of Physical Science and Information Technology Anhui UniversityHefei 230601China

钙钛矿氧化物具有灵活的组成和电子结构,在电催化水氧化反应中具有很大的应用潜力.然而,钙钛矿氧化物在电催化有机小分子转化中的应用研究较少,这可能是由于其导电性差,表面重构产生活性物种所需的能垒高.在本文中,我们报道了具有典型... 详细信息

钙钛矿氧化物具有灵活的组成和电子结构,在电催化水氧化反应中具有很大的应用潜力.然而,钙钛矿氧化物在电催化有机小分子转化中的应用研究较少,这可能是由于其导电性差,表面重构产生活性物种所需的能垒高.在本文中,我们报道了具有典型反钙钛矿结构的氮化铜纳米片作为甲醇选择性转化为甲酸盐的电催化剂,其形成甲酸盐的法拉第效率超过90%.原位电化学质谱和原位红外反射吸收光谱进一步证实了制备的氮化铜样品在较宽的电位范围内具有较高的甲酸盐选择性.此外,高分辨率透射电镜、X射线吸收光谱和原位拉曼光谱表明,该催化剂在电催化过程中发生表面重构形成了氧化态铜物种壳,从而提升了其整体甲醇氧化性能,而原始的氮化铜核则利于在催化剂内部的电子传递.本研究不仅为甲醇的高选择性转化提供了一种有意义的方案,而且为有机小分子的电化学转化提供了一种新型的非氧化物钙钛矿材料模型.

关键词： antiperovskite copper nitride methanol oxidation reaction formate

Unraveling the interfacial effect of PdBi bimetallic catalysts on promoting CO_(2)electroreduction to formate

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Nano Research 2023年第8期16卷 10822-10831页

作者： Wenhui Liu Lingtong Ding Minmin Liu Xiao Wang Zhengrong Zhang Tian-Wen Jiang Shengjuan Huo Wen-Bin Cai International Joint Laboratory of Catalytic Chemistry Department of ChemistryInstitute for Sustainable EnergyCollege of SciencesShanghai UniversityShanghai 200444China Shenzhen Key Laboratory of Nanobiomechanics Shenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055China Paul C.Lauterbur Research Center for Biomedical Imaging Shenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055China Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Collaborative Innovation Center of Chemistry for Energy MaterialsDepartment of ChemistryFudan UniversityShanghai 200438China

Through interface engineering and content control strategy,a PdBi bimetallic interface structure was constructed for the first time to selectively convert CO_(2)to formate with a remarkably high Faraday efficiency(FEformate)of 94%and a partial current density(jformate)of 34 mA·cm^(−2)at−0.8 V vs.reversible hydrogen electrode(RHE)in an H-cell.Moreover,the PdBi interface electrocatalyst even exhibited a high current density of 180 mA·cm^(−2)with formate selectivity up to 92%in a flow cell and could steadily operate for at least 20 h.Electrochemical in-situ attenuated total reflection surface enhanced infrared absorption spectroscopy(ATR-SEIRAS)confirmed that the PdBi interface could greatly weaken the adsorption of*CO intermediates due to electronic and geometric effects.Density functional theory(DFT)calculations also established that the PdBi interface regulated the CO_(2)-to-formate pathway by reducing the energy barrier toward HCOOH and largely weakening the adsorption of*CO intermediates on the catalyst surface.This study reveals that the unique PdBi bimetallic interface can provide a novel platform to study the reaction mechanism through combining in-situ ATR-SEIRAS and DFT calculations.

关键词： carbon dioxide reduction reaction bimetallic PdBi interface engineering formate in-situ attenuated total reflection surface enhanced infrared absorption spectroscopy(ATR-SEIRAS)

Hydrogenation of CO_(2) to formate catalyzed by SBA-15-supported cyclic(alkyl)(amino)carbene-iridium

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Chinese Journal of Chemical Engineering 2022年第10期50卷 283-291页

作者： Lei Zhou Lingling Peng Xingbang Hu College of Chemistry and Chemical Engineering Yangzhou Polytechnic InstituteYangzhou 225127China School of Chemistry and Chemical Engineering Nanjing UniversityNanjing 210093China

Recently,cyclic(alkyl)(amino)carbenes(CAACs)have been widely used as ligands to enhance the catalytic reactivity of center metal,but the problem of recycling this expensive ligand remains to be solved.In this work,the heterogeneous SBA-15-CAAC-Ir catalyst was prepared by a covalent attachment method.and using SBA-15 as the carrier.It shows high reactivity for the hydrogenation of CO_(2) to formate.After immobilization,the ordered mesoporous structure and the overall rod-like morphology of the original SBA-15 have been preserved very well.Using SBA-15-CAAC-Ir as catalyst,up to 21050 TON can be obtained at 60℃.In addition,the catalyst can be separated easily by centrifugation,and the catalytic activity of SBA-15-CAAC-Ir can still remain very high after multiple cycles.

关键词： Cyclic(alkyl)(amino)carbenes Carbon dioxide Hydrogenation SBA-15 formate

Self-supported ultrathin NiCo layered double hydroxides nanosheets electrode for efficient electrosynthesis of formate

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Journal of Energy Chemistry 2023年第10期85卷 267-275,I0008页

作者： Haoyuan Chi Jianlong Lin Siyu Kuang Minglu Li Hai Liu Qun Fan Tianxiang Yan Sheng Zhang Xinbin Ma Key Laboratory for Green Chemical Technology of Ministry of Education Collaborative Innovation Centre of Chemical Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

Electrochemical CO_(2)reduction into energy-carrying compounds,such as formate,is of great importance for carbon neutrality,which however suffers from high electrical energy input and liquid products crossover.Herein,we fabricated self-supported ultrathin NiCo layered double hydroxides(LDHs)electrodes as anode for methanol electrooxidation to achieve a high formate production rate(5.89 mmol h^(-1)cm^(-2))coupled with CO_(2)electro-reduction at the cathode.A total formate faradic efficiency of both anode for methanol oxidation and cathode for CO_(2)reduction can reach up to 188%driven by a low cell potential of only 2.06 V at 100 mA cm^(-2)in membrane-electrode assembly(MEA).Physical characterizations demonstrated that Ni^(3+)species,formed on the electrochemical oxidation of Ni-containing hydroxide,acted as catalytically active species for the oxidation of methanol to formate.Furthermore,DFT calculations revealed that ultrathin LDHs were beneficial for the formation of Ni^(3+)in hydroxides and introducing oxygen vacancy in NiCo-LDH could decrease the energy barrier of the rate-determining step for methanol oxidation.This work presents a promising approach for fabricating advanced electrodes towards electrocatalytic reactions.

关键词： CO_(2)reduction Methanol oxidation reaction formate Layered double hydroxides Oxygen vacancies

Boosting CO_(2) electroreduction to formate via bismuth oxide clusters

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Nano Research 2023年第10期16卷 12050-12057页

作者： Xiaole Jiang Le Lin Youwen Rong Rongtan Li Qike Jiang Yaoyue Yang Dunfeng Gao Key Laboratory of Fundamental Chemistry of the State Ethnic Commission School of Chemistry and EnvironmentSouthwest Minzu UniversityChengdu 610041China State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China School of Science Dalian Maritime UniversityDalian 116026China University of Chinese Academy of Sciences Beijing 100049China

Supported metal(oxide)clusters,with both rich surface sites and high atom utilization efficiency,have shown improved activity and selectivity for many catalytic reactions over nanoparticle and single atom catalysts.Yet,the role of cluster catalysts has been rarely reported in CO_(2)electroreduction reaction(CO_(2)RR),which is a promising route for converting CO_(2)to liquid fuels like formic acid with renewable electricity.Here we develop a bismuth oxide(BiOn)cluster catalyst for highly efficient CO_(2)RR to formate.The BiOn cluster catalyst exhibits excellent activity,selectivity,and stability towards formate production,with a formate Faradaic efficiency of over 90%at a current density up to 500 mA·cm^(−2)in an alkaline membrane electrode assembly electrolyzer,corresponding to a mass activity as high as 3,750 A·gBi−1.The electrolyzer with the BiOn cluster catalyst delivers a remarkable formate production rate of 0.56 mmol·min−1 at a high single-pass CO_(2)conversion of 44%.Density functional theory calculations indicate that Bi4O_(3)cluster is more favorable for stabilizing the HCOO^(*)intermediate than Bi(001)surface and single site BiC_(4)motif,rationalizing the improved formate production over the BiOn cluster catalyst.This work highlights the great importance of cluster catalysts in activity and selectivity control in electrocatalytic CO_(2)conversion.

关键词： CO_(2)electroreduction reaction formate bismuth oxide cluster catalyst membrane electrode assembly