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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

Trace Cobalt Doping and Defect Engineering of High Surface Area α-Ni(OH)_(2) for Electrocatalytic Urea Oxidation

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Energy & Environmental Materials 2024年第2期7卷 111-118页

作者： Yi Liu Zhihui Yang yuqin zou Shuangyin Wang Junying He School of Metallurgy and Environment Central South UniversityChangsha 410083China State Key Laboratory of Chem/Bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China

Owing to the intrinsically sluggish kinetics of urea oxidation reaction(UOR)involving a six-electron transfer process,developing efficient UOR electrocatalyst is a great challenge remained to be ***,by taking advantage of 2-Methylimidazole,of which is a kind of alkali in water and owns strong coordination ability to Co^(2+)in methanol,trace Co(1.0 mol%)addition was found to induce defect engineering onα-Ni(OH)_(2)in a dual-solvent system of water and *** characterization results revealed that the synthesized electrocatalyst(WM-Ni_(0.99)Co_(0.01)(OH)_(2))was a kind of defective nanosheet with thickness around 5-6 nm,attributing to the synergistic effect of Co doping and defect engineering,its electron structure was finely altered,and its specific surface a rea was tremendously enlarged from 68 to 172.3 m^(2)g^(-1).With all these merits,its overpotential to drive 10 mA cm^(-2)was reduced by 110 ***,the interfacial behavior of UOR was also well deciphered by operando electrochemical impedance spectroscopy.

关键词： defect engineering electrocatalysis small molecule oxidation

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

Recent Progress on Electrocatalytic Valorization of Biomass-Derived Organics

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Energy & Environmental Materials 2022年第4期5卷 1117-1138页

作者： Ming Yang Zhenran Yuan Rixin Peng Shuangyin Wang yuqin zou State Key Laboratory of Chem/Bio-Sensing and Chemometrics Provincial Hunan Key Laboratory for Graphene Materials and DevicesCollege of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China E-mail:yuqin_zou@***

Electrocatalytic valorization of biomass derivatives can be powered by electricity generated from renewable sources such as solar and wind energy.A shift from centralized,high-temperature,and energy-intensive processes to decentralized,low-temperature conversions is achieved,which meets the requirement of sustainable energy *** approach provides an efficient,green,and additive-free strategy for biomass derivative valorization,in which product selectivity could be easily regulated by the applied potential and electrocatalyst ***,a scale-up application is still far from being completed due to the inability of conversion rates and selectivity to meet the industrialization requirements.A better understanding of the reaction mechanism and the development of highefficiency and high-selectivity electrocatalysts are required to pave the path toward larger industrialization ***,we summarize the recent research progress in the electrocatalytic oxidation and hydrogenation of platform compounds such as furanic compounds and *** the literature,these three research areas are integrated to realize the scale-up application of the processes as mentioned *** investigations of the mechanism are based on in situ techniques,theoretical calculations,and advanced electrocatalyst ***,the challenges and prospects in this topic are *** expect that this review will provide the fundamental understanding and design guidelines to achieve efficient and high-selectivity catalysts and further facilitate the scale-up application of the electrocatalytic conversion of biomass derivatives.

关键词： electrocatalyst electrochemical hydrogenation electrochemical oxidation furanic compound glycerol

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

Defect engineered electrocatalysts for C-N coupling reactions toward urea synthesis

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Chinese Chemical Letters 2024年第8期35卷 7-14页

作者： Shengkai Li yuqin zou Chen Chen Shuangyin Wang Zhao-Qing Liu Guangzhou Key Laboratory for Clean Energy and Materials/Key Laboratory for Water Quality and Conservation of the Pearl River Delta Ministry of EducationGuangzhou UniversityGuangzhou 510006China 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 410082China

Urea is extensively used in agriculture and chemical industry,and it is produced on an industrial scale from CO_(2)and Haber-Bosch NH_(3)under relatively high temperature and high pressure conditions,which demands high energy input and generates masses of carbon *** conversion of CO_(2)and N sources(such as NO_(2)^(−),NO_(3)^(−),and N_(2))through electrocatalytic reactions under ambient conditions is a promising alternative to realize efficient urea *** note,the design of electrocatalyst is one of the key factors that can improve the efficiency and selectivity of C-N coupling *** engineer-ing is an intriguing strategy for regulating the electronic structure and charge density of electrocatalysts,which endows electrocatalysts with excellent physicochemical properties and optimized adsorption en-ergy of the reaction intermediates to reduce the kinetic *** this minireview,recent advances of defect engineered electrocatalysts in urea electrosynthesis from CO_(2)and various N reactants are firstly *** discussions of C-N coupling in these advances are presented,with the aim of directing future investigations on improving the urea ***,the prospects and challenges of de-fect engineered electrocatalysts for urea synthesis are *** overview is expected to provide in-depth understanding of structure-reactivity relationship and shed light on future electrocatalytic C-N coupling reactions.

关键词： Electrocatalysis Defective electrocatalyst Co-reduction C-N coupling Urea synthesis

Sulfonic groups functionalized Zr-metal organic framework for highly catalytic transfer hydrogenation of furfural to furfuryl alcohol

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Journal of Energy Chemistry 2022年第8期31卷 411-417,I0011页

作者： Jingcheng Wu Dong Liang Xiangbo Song Tingsen Liu Tianyi Xu Shuangyin Wang yuqin zou State Key Laboratory of Chem/Bio-Sensing and Chemometrics Advanced Catalytic Engineering Research Center of the Ministry of EducationCollege of Chemistry and Chemical Engineeringthe National Supercomputer Centers in ChangshaHunan UniversityChangsha 410082HunanChina Shenzhen Institute of Hunan University Shenzhen 518057GuangdongChina School of Physical and Electronic Sciences Chuxiong Normal UniversityChuxiong 675099YunnanChina

The highly selective catalytic transfer hydrogenation(CTH)of furfural(FF)to furfuryl alcohol(FOL)is a significant route of biomass ***,a series microporous Zr-metal organic framework(ZrMOF)functionalized by sulfonic groups are *** on the comprehensive structural characterizations by means of X-ray diffraction(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM),N2 physisorption,Thermogravimetric(TG)and Fourier transformed infrared spectroscopy(FTIR),we find that sulfonic acid(–SO_(3)H)functional groups are tethered on the UIO-66 without affecting the structure of the *** characterizations(NH_(3)-TPD,CO_(2)-TPD,and in-situ FTIR)demonstrate that modifying of sulfonic groups on UIO-66 results in the formation of stronger Lewis acidic-basic and Brnsted acidis *** cooperative role of the versatile Lewis acidic-basic and Brnsted acidic sites in 60%mol fraction of sulfonic acid-containing UIO-66(UIO-S_(0.6))retain high surface area and exhibit excellent catalytic performance of 94.7%FOL yield and 16.9 h^(-1).turnover number(TOF)under mild *** experiments reveal that the activation energy of the CTH of furfural(FF)over UIO-S_(0.6) catalyst is as low as 50.8 k J mol^(-1).Besides,the hydrogen transfer mechanism is investigated through isotope labeling experiments,exhibiting that theβ-H in isopropanol is transferred to the a-C of FF by forming six-membered intermediates on the Lewis acidic-basic and Brnsted acidic sites of the UIO-S_(0.6),which is the rate-determining step in the formation of FOL.

关键词： Hydrogenation Biomass Metal organic framework Biorefinery

Understanding the surface segregation behavior of bimetallic CoCu toward HMF oxidation reaction

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Journal of Energy Chemistry 2022年第11期31卷 85-90,I0004页

作者： Yanwei Zhu Jianqiao Shi Yingying Li Yuxuan Lu Bo Zhou Shuangyin Wang yuqin zou State Key Laboratory of Chem/Bio-Sensing and Chemometrics Advanced Catalytic Engineering Research Center of the Ministry of EducationCollege of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082HunanChina School of Chemistry and Chemical Engineering Jishou UniversityJishou 416000HunanChina

Surface segregation is ubiquitous in multi-component materials and is of great important for catalysis but little is known on the surface structure under graphene ***,we show that the graphene encapsulated CoCu performs well for the electrocatalytic oxidation of 5-hydroxymethylfurfural(HMF)to2,5-furandicarboxylic acid(FDCA)with the onset potential before 1.23 VRHEand a nearly 100%selectivity of FDCA under 1.4 *** the experimental results,the unprecedented catalytic performance was attributed to local structural distortion and sub-nanometer lattice composition of the CoCu *** accurately show the dispersed Cu doped Co_(3)O_(4) nano-islands with a lot of edge sites on the bimetallic Co-Cu ***,the gradient components effectively facilitate the establishment of built-in electric field and accelerate the charge *** and experimental results reveal that the surface Co and neighbouring Cu atoms in sub-nanometer lattice synergistically promote the catalysis of *** work offers new insights into surface segregation in tuning the element spatial distribution for catalysis.

关键词： CoCu alloy Surface segregation Sub-nanometer lattice Electrocatalysis HMF oxidation

Rational design of three-phase interfaces for electrocatalysis

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Nano Research 2019年第9期12卷 2055-2066页

作者： yuqing Wang yuqin zou Li Tao Yanyong Wang Gen Huang Shiqian Du Shuangyin Wang State Key Laboratory of Chem/Bio-Sensing and Chemometrics Provincial Hunan Key Laboratory for Graphene Materials and De vicesCollege oj Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China

Gas-involving electrochemical reactions,like oxygen reduction reaction (ORR),oxygen evolution reaction (OER),and hydrogen evolution reaction (HER),are critical processes for energy-saving,environment-friendly energy conversion and storage technologies which gain increasing *** development of according electrocatalysts is key to boost their electrocatalytic *** efforts have been put into the development of advanced electrocatalysts to overcome sluggish *** the other hand,the electrode interfaces-architecture construction plays an equally important role for practical applications because these imperative electrode reactions generally proceed at triple-phase interfaces of gas,liquid electrolyte,and solid electrocatalyst.A desirable architecture should facilitate the complicate reactions occur at the triple-phase interfaces,which including mass diffusion,surface reaction and electron *** this review,we will summarize some design principles and synthetic strategies for optimizing triple-phase interfaces of gas-involving electrocatalysis systematically,based on the electrode reaction process at the three-phase *** can be divided into three main optimization directions:exposure of active sites,promotion of mass diffusion and acceleration of electron ***,we especially highlight several remarkable works with comprehensive optimization about specific energy conversion devices,including metal-air batteries,fuel cells,and water-splitting devices are demonstrated with superb *** the last section,the perspectives and challenges in the future are proposed.

关键词： triple-phase irderfaces gas-involving electrocatalysis mass diffusion exposure of active sites electron transfer