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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

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

Activity origin and alkalinity effect of electrocatalytic biomass oxidation on nickel nitride

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Journal of Energy Chemistry 2021年第10期30卷 179-185,I0006页

作者： Bo Zhou Chung-Li Dong Yu-Cheng Huang Nana Zhang Yandong Wu yuxuan lu Xu Yue Zhaohui Xiao Yuqin Zou Shuangyin Wang State Key Laboratory of Chem/Bio-Sensing and Chemometrics Provincial Hunan Key Laboratory for Graphene Materials and DevicesCollege of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082HunanChina Department of Physics Tamkang UniversityNew Taipei City 25137TaiwanChina

Electro-oxidation of 5-hydroxymethylfurfural(HMFOR)is a promising green approach to realize the conversion of biomass into value-added ***,considering the complexity of the molecular structure of HMF,an in-depth understanding of the electrocatalytic behavior of HMFOR has rarely been ***,the electrocatalytic mechanism of HMFOR on nickel nitride(Ni3 N)is elucidated by operando X-ray absorption spectroscopy(XAS),in situ Raman,quasi in situ X-ray photoelectron spectroscopy(XPS),and operando electrochemical impedance spectroscopy(EIS),*** activity origin is proved to be Ni^(2+δ)N(OH)ads generated by the adsorbed hydroxyl ***,HMFOR on Ni3 N relates to a two-step reaction:Initially,the applied potential drives Ni atoms to lose electrons and adsorb OH-after 1.35 VRHE,giving rise to Ni^(2+δ)N(OH)ads with the electrophilic oxygen;then Ni^(2+δ)N(OH)ads seizes protons and electrons from HMF and leaves as H_(2) O ***,the high electrolyte alkalinity favors the HMFOR process due to the increased active species(Ni^(2+δ)N(OH)ads)and the enhanced adsorption of HMF on the Ni3 N *** work could provide an in-depth understanding of the electrocatalytic mechanism of HMFOR on Ni3 N and demonstrate the alkalinity effect of the electrolyte on the electrocatalytic performance of HMFOR.

关键词： Biomass electro-oxidation Activity origin Alkalinity effect Operando techniques HMF

Preparation and Characterization of Porous Carbon from Mixed Leaves for High-Performance Supercapacitors

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Chinese Journal of Chemistry 2021年第2期39卷 353-359页

作者： Xiaoxiang Yang Jie Xu Xin Chen Yuli Lei Lingling Wang Siyu Cheng Yan Li yuxuan lu Yupeng Zhu Na Chen East China University of Science&Technology No.130Meilong RoadXuhui DistrictShanghai200237 China

With the increasing demand of sustainable and eco-friendly resources,it is very attractive to use waste leaves for activated carbon(AC)preparation that can be used in *** the practically collected leaves are commonly in mixed nature,and extra efforts are needed to sort these mixtures,we here report the first preparation of AC using mixed leaves from different plants,including Platanus acerifolia(PA),Firmiana platanifolia(FP)and Pistia stratiotes(PS),and compared the results with single leaves-derived AC *** leave-derived AC samples were characterized with FESEM,EDS,FTIR and Raman spectroscopy,and electrochemical *** AC derived from mixed leaves(PA3FP1PS2AC)showed a good specific capacitance of 246 F·g−1 at 1 A·g−1 in aqueous 3 mol·L^(-1)*** sample further showed the largest specific capacitance of 201 F·g−1 at 5 A·g−1,as compared with the non-mixed AC samples,and a good stability of 100.0%capacitance retention over 1000 *** mixed leaves for AC preparation is not only demonstrated to be a promising approach of low cost and high-performance AC production for supercapacitor applications,but may also help environmental protection by reducing the invasive species problem.

关键词： Biomass Activated carbon Supercapacitor Electrochemistry Energy conversion

Promoting surface reconstruction of NiFe layered double hydroxides via intercalating[Cr(C_(2)O_(4))_(3)]^(3-)for enhanced oxygen evolution

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Journal of Energy Chemistry 2022年第11期31卷 140-148,I0005页

作者： Yujie Wu Minglei Song Yu-Cheng Huang Chung-Li Dong Yingying Li yuxuan lu Bo Zhou Dongdong Wang Jianfeng Jia Shuangyin Wang Yanyong Wang State Key Laboratory of Chemo/Bio-Sensing and Chemometrics College of Chemistry and Chemical Engineeringthe National Supercomputing Center in ChangshaHunan UniversityChangsha 410082HunanChina Department of Physics Tamkang UniversityNew Taipei City 25137TaiwanChina Key Laboratory of Magnetic Molecules and Magnetic Information Materials(Ministry of Education) School of Chemistry and Material ScienceShanxi Normal UniversityTaiyuan 030031ShanxiChina

Rationally manipulating surface reconstruction of catalysts for water oxidation,inducing formation and dynamic accumulation of catalytically active centers still face numerous ***,the introduction of[Cr(C_(2)O_(4))_(3)]^(3-)into NiFe LDHs by intercalation engineering to promote surface reconstruction achieves an advanced oxygen evolution reaction(OER)*** view of the weak electronegativity of Cr^(3+) in[Cr(C_(2)O_(4))_(3)]^(3-),the intercalation of[Cr(C_(2)O_(4))_(3)]^(3-)is expected to result in an electron-rich structure of Fe sites in NiFe LDHs,and higher valence state of Ni can be formed with the charge transfer between Fe and *** optimized electronic structure of NiFe-[Cr(C_(2)O_(4))_(3)]^(3-)-LDHs with more active Ni^(3+) species and the expedited dynamic generation of Ni^(3+) (Fe)OOH phase during the OER process contributed to its excellent catalytic property,revealed by in situ X-ray absorption spectroscopy,Raman spectroscopy,and quasi-in situ X-ray photoelectron *** the modulated electronic structure of metal sites,NiFe-[Cr(C_(2)O_(4))_(3)]^(3-)-LDHs exhibited promoted OER property with a lower overpotential of 236 mV at the current density of 10 mA cm^(-2).This work illustrates the intercalation of conjugated anion to dynamically construct desired Ni^(3+) sites with the optimal electronic environment for improved OER electrocatalysis.

关键词： NiFe layered double hydroxides [Cr(C_(2)O_(4))_(3)]^(3-)intercalation Dynamic restructuring Operando spectroscopies Oxygen evolution reaction

Hierarchically nanostructured Ni O-Co3O4 with rich interface defects for the electro-oxidation of 5-hydroxymethylfurfural

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Science China Chemistry 2020年第7期63卷 980-986页

作者： yuxuan lu Chung-Li Dong Yu-Cheng Huang Yuqin Zou Yanbo Liu Yingying Li Nana Zhang Wei Chen Ling Zhou Hongzhen Lin Shuangyin Wang State Key Laboratory of Chem/Bio-Sensing and Chemometrics Provincial Hunan Key Laboratory for Graphene Materials and DevicesCollege of Chemistry and Chemical Engineeringthe National Supercomputer Centers in ChangshaHunan UniversityChangsha 410082 Department of Physics Tamkang UniversityTaipei 25137 i-LAB Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123

Ni-based electrocatalysts with strong redox abilities are active for the electrochemical oxidation of 5-hydroxymethylfurfural(HMF). Interface engineering is an efficient way to modulate the electronic structure, tune the intermediate adsorption, and expose more active sites. Herein, we increased the concentration of interfacial sites with rich defects in a 3D hierarchical nanostructured NiO-Co3O4 electrocatalyst and investigated its catalytic performance for HMF electro-oxidation. The interface effect created abundant cation vacancies, modulated the electronic properties of Co and Ni atoms, and raised the oxidation state of Ni species. The NiO-Co3O4 catalysts show superb HMF oxidation activities with a low onset potential of 1.28 ***, in-situ surface-selective vibrational spectroscopy of sum-frequency generation was performed to study the reaction pathway during the oxidation process on the electrocatalysts. The current study offers an efficient way to create cation vacancies and proves the decisive role of cation vacancies in catalyzing the HMF electro-oxidation.

关键词： interface effect cation vacancies in-situ vibrational spectroscopy electrochemical biomass conversion 3D hierarchical nanostructure

Promoting the electrochemical hydrogenation of furfural by synergistic Cu^(0)−Cu^(+) active sites

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Science China Chemistry 2022年第12期65卷 2588-2595页

作者： Zhongcheng Xia Yingying Li Jingcheng Wu Yu-Cheng Huang Weixing Zhao yuxuan lu Yuping Pan Xu Yue Yanjing Wang Chung-Li Dong 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 UniversityChangsha410082China Research Center for X-ray Science&Department of Physics Tamkang UniversityNew Taipei City25137China School of Chemistry and Chemical Engineering Jishou UniversityJishou416000China

Electrochemical hydrogenation(ECH)of furfural,which uses the proton from water and avoids the usage of gaseous hydrogen and high pressure,is an efficient way to utilize biomass ***-based catalysts are promising catalysts for the ECH of ***,their active sites and reaction mechanism have not been fully understood *** work unveils the active oxidation state of Cu-based electrocatalysts for the ECH of *** co-existence of Cu^(+)and Cu^(0) on the CuO surface under the working potential is confirmed by a series of in situ *** poisoning experiment shows that the performance decreased heavily after the Cu^(+)was complexed with SCN−,indicating the decisive role of Cu^(+).Finally,the density functional theory(DFT)calculation suggests that the Cu^(0)−Cu^(+)synergistic effect is beneficial to both kinetics and thermodynamics:Cu^(+)accelerates the second step hydrogenation process of furfural,and Cu^(0) reduces the energy barrier for the desorption of furfuryl *** work demonstrates the synergistic effect of Cu^(0) and Cu^(+)states for the electrochemical hydrogenation of furfural and provides a deeper understanding of the furfural hydrogenation mechanism.

关键词： biomass conversion electrocatalytic hydrogenation furfural CuO synergistic effect

pH-Induced selective electrocatalytic hydrogenation of furfural on Cu electrodes

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Chinese Journal of Catalysis 2022年第12期43卷 3142-3153页

作者： Ling Zhou Yingying Li yuxuan lu Shuangyin Wang Yuqin Zou State Key Laboratory of Chemo/Bio-Sensing and Chemometrics Advanced Catalytic Engineering Research Center of the Ministry of EducationCollege of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082HunanChina Shenzhen Institute of Hunan University Shenzhen 518057GuangdongChina

The efficient and selective electrocatalytic hydrogenation(ECH)of furfural is considered a green strategy for achieving biomass-derived high-value *** an aqueous electrolytic environment,a green hydrogen energy source of water,is significant for improving the selectivity of products and reducing energy *** this study,we systematically investigated the mechanism of pH dependence of product selectivity in the ECH of furfural on Cu *** acidic conditions,the oxygen atom dissociated directly from hydrogenated furfural-derived alkoxyl intermediates,followed by stepwise hydrogenation until H_(2)O formation via a thermodynamically favorable proton-coupled electron transfer process,thereby inducing a high proportion of the hydrogenolysis product(2-methylfuran).However,under partial alkaline conditions,furfural could be directly hydrogenated to furfuryl alcohol(selectivity~98%)due to the high-energy barrier of the deoxidation process via a surface hydride(Had)*** results highlight the vital role of the electrolytic environment in furfural selective conversion and broaden our fundamental understanding of hydrodeoxygenation reactions in ECH.

关键词： Electrocatalytic hydrogenation Biomass pH Dependence Mechanism

Identification of the hydrogen utilization pathway for the electrocatalytic hydrogenation of phenol

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Science China Chemistry 2021年第9期64卷 1586-1595页

作者： Ling Zhou Xiaorong Zhu Hui Su Hongzhen Lin Yanhong Lyu Xu Zhao Chen Chen Nana Zhang Chao Xie Yingying Li yuxuan lu Jianyun Zheng Benrt Johannessen San Ping Jiang Qinghua Liu Yafei Li Yuqin Zou Shuangyin Wang State Key Laboratory of Chem/Bio-Sensing and Chemometrics Provincial Hunan Key Laboratory for Graphene Materials and DevicesCollege of Chemistry and Chemical Engineeringthe National Supercomputer Centers in ChangshaHunan UniversityChangsha410082China College of Chemistry and Materials Science Nanjing Normal UniversityNanjing210023China National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei230026China i-LAB Suzhou Institute of Nano-Tech and Nano-Bionics(SINANO)Chinese Academy of SciencesSuzhou215123China Department of Educational Science Hunan First Normal UniversityChangsha410205China Australian Synchrotron ClaytonVictoria3168Australia Western Australian School of Mines:Minerals Energy and Chemical Engineering and Fuels and Energy Technology InstituteCurtin UniversityPerthWA6102Australia

Electrochemical hydrogenation(ECH)of biomass-derived platform molecules is a burgeoning route for the sustainable utilization of ***,the noble-metal-catalyzed ECH of phenolic compounds suffers from intense competition with hydrogen evolution *** prepared Pt Rh bimetallic nanoparticles dispersed on highly ordered mesoporous carbon nanospheres,which improves the utilization efficiency of adsorbed hydrogen(H_(ad))to ECH in H-UPD region(>0 V ***).Further analysis reveals(i)the strong overlapping between the d-orbitals of Pt and Rh enhances specific adsorption of phenol;(ii)incorporation of Rh devotes an electronic effect on weakening the alloy-H_(ad)interaction to increase the FE of *** calculations confirm the selectivity difference and the ECH parallel pathways:cyclohexanol and cyclohexanone are formed via hydrogenation/dehydrogenation of the intermediate ^(*)C_(6)H_(10) *** findings deepen our fundamental understanding of the ECH process,and cast new light on exploration of highly efficient electrocatalysts for biomass upgrading.

关键词： electrohydrogenation aromatic hydrogenation biomass conversion Pt Rh alloy