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The feasibility study of the indium oxide supported silver catalyst for selective hydrogenation of CO_(2)to methanol

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Green Energy & Environment 2022年第4期7卷 807-817页

作者： Kaihang Sun Zhitao Zhang Chenyang Shen Ning Rui Chang-jun Liu School of Chemical Engineering and Technology Tianjin UniversityTianjin300072China

Silver catalyst has been extensively investigated for photocatalytic and electrochemical CO_(2) reduction.However,its high activity for selective hydrogenation of CO_(2) to methanol has not been confirmed.Here,the feasibility of the indium oxide supported silver catalyst was investigated for CO_(2) hydrogenation to methanol by the density functional theoretical(DFT)study and then by the experimental investigation.The DFT study shows there exists an intense Ag-In_(2)O_(3) interaction,which causes silver to be positively charged.The positively charged Ag species changes the electronic structure of the metal,facilitates the formation of the Ag-In_(2)O_(3) interfacial site for activation and dissociation of carbon dioxide.The promoted CO_(2) dissociation leads to the enhanced methanol synthesis via the CO hydrogenation route as CO_(2)^(*)→CO^(*)→HCO^(*)→H_(2)CO^(*)→H_(3)CO^(*)→H_(3)COH^(*).The Ag/In_(2)O_(3)catalyst was then prepared using the deposition-precipitation method.The experimental study confirms the theoretical prediction.The methanol selectivity of CO_(2) hydrogenation on Ag/In_(2)O_(3) reaches 100.0%at reaction temperature of 200℃.It remains more than 70.0%between 200 and 275℃.At 300℃and 5 MPa,the methanol selectivity still keeps 58.2%with a CO_(2) conversion of 13.6%and a space-time yield(STY)of methanol of 0.453 g_(methanol)g_(cat)^(-1)h^(-1),which is the highest methanol STY ever reported for silver catalyst.The catalyst characterization confirms the intense Ag-In_(2)O_(3)interaction as well,which causes high Ag dispersion,increases and stabilizes the oxygen vacancies and creates the active Ag-In_(2)O_(3)interfacial site for the enhanced CO_(2)hydrogenation to methanol.

关键词： Carbon dioxide Hydrogenation Methanol indium oxide Silver

Correlating the crystal structure and facet of indium oxides with their activities for CO_(2)electroreduction

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Fundamental Research 2024年第3期4卷 635-641页

作者： Jiajun Wang Guangjin Wang Han Wu Fei Liu Xixi Ren Yidu Wang Yanhui Cao Qi Lu Xuerong Zheng 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 School of Materials Science and Energy Engineering Foshan UniversityFoshan 528000China 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

Constructing structure-function relationships is critical for the rational design and development of efficient catalysts for CO2 electroreduction reaction(CO2RR).In2O3 is well-known for its specific ability to produce formic acid.However,how the crystal phase and surface affect the CO_(2)RR activity is still unclear,making it difficult to further improve the intrinsic activity and screen for the most active structure.In this work,cubic and hexagonal In_(2)O_(3) with different stable surfaces((111)and(110)for cubic,(120)and(104)for hexagonal)are investigated for CO_(2)RR.Theoretical results demonstrate that the adsorption of reactants on cubic In_(2)O_(3) is stronger than that on hexagonal In_(2)O_(3),with the cubic(111)surface being the most active for CO_(2)RR.In experiments,synthesized cubic In_(2)O_(3) nanosheets with predominantly exposed(111)surfaces exhibited a high HCOO^(-)Faradaic efficiency(87.5%)and HCOO^(–)current density(–16.7 mA cm^(-2))at–0.9 V vs RHE.In addition,an aqueous Zn-CO_(2) battery based on a cubic In2O3 cathode was assembled.Our work correlates the phases and surfaces with the CO_(2)RR activity,and provides a fundamental understanding of the structure-function relationship of In_(2)O_(3),thereby contributing to further improvements in its CO_(2)RR activity.Moreover,the results provide a principle for the directional preparation of materials with optimal phases and surfaces for efficient electrocatalysis.

关键词： Structure-function relationship CO_(2)electroreduction indium oxide Reactionmechanism Catalyst design

Synthesis and Characterization of indium Niobium oxide Thin Films via Sol—Gel Spin Coating Method

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Journal of Materials Science & Technology 2013年第10期29卷 923-928页

作者： Saeed Mohammadi Mohammad Reza Golobostanfard Hossein Abdizadeh School of Metallurgy and Materials Engineering College of EngineeringUniversity of Tehran Center of Excellence for High Performance Materials University of Tehran

In the present study, niobium-doped indium oxide thin films were prepared by sol-gel spin coating technique. The effects of different Nb-doping contents on structural, morphological, optical, and electrical properties of the films were characterized by means of X-ray diffraction （XRD）, field emission scanning electron microscopy （FESEM）, atomic force microscopy （AFM）, UV-Vis spectroscopy, and four point probe methods. XRD analysis confirmed the formation of cubic bixbyite structure of In203 with a small shift in major peak position toward lower angles with addition of Nb. FESEM micrographs show that grain size decreased with increasing the Nb-doping content. Optical and electrical studies revealed that optimum opto-electronic properties, including minimum electrical resistivity of 119.4 × 10^-3 Ω cm and an average optical transmittance of 85% in the visible region with a band gap of 3.37 eV were achieved for the films doped with Nb-doping content of 3 at.%. AFM studies show that addition of Nb at optimum content leads to the formation of compact films with smooth surface and less average roughness compared with the prepared ln2O3 films.

关键词： indium oxide Nb-doping Sol-gel spin coating Transparent conductive oxide Opto-electronic properties

MOF-Transformed In_(2)O_(3-x)@C Nanocorn Electrocatalyst for Efficient CO_(2)Reduction to HCOOH

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Nano-Micro Letters 2022年第10期14卷 219-234页

作者： Chen Qiu Kun Qian Jun Yu Mingzi Sun Shoufu Cao Jinqiang Gao Rongxing Yu Lingzhe Fang Youwei Yao Xiaoqing Lu Tao Li Bolong Huang Shihe Yang Guangdong Key Lab of Nano-Micro Material Research School of Chemical Biology and BiotechnologyPeking University Shenzhen Graduate SchoolShenzhen 518055People’s Republic of China Department of Chemistry and Biochemistry Northern Illinois UniversityDeKalbIL 60115USA Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic UniversityHung HomKowloonHong Kong SARPeople’s Republic of China School of Materials Science and Engineering China University of PetroleumQingdaoShandong 266580People’s Republic of China Shenzhen International Graduate School Tsinghua UniversityShenzhenPeople’s Republic of China X-Ray Science Division and Joint Center for Energy Storage Research Argonne National LaboratoryLemontIL 60439USA Institute of Biomedical Engineering Shenzhen Bay LaboratoryShenzhen 518107People’s Republic of China

For electrochemical CO_(2) reduction to HCOOH,an ongoing challenge is to design energy efficient electrocatalysts that can deliver a high HCOOH current density(JHCOOH)at a low overpotential.indium oxide is good HCOOH production catalyst but with low con-ductivity.In this work,we report a unique corn design of In_(2)O_(3-x)@C nanocatalyst,wherein In_(2)O_(3-x)nanocube as the fine grains dispersed uniformly on the carbon nanorod cob,resulting in the enhanced conductivity.Excellent performance is achieved with 84%Faradaic efficiency(FE)and 11 mA cm^(−2)JHCOOH at a low potential of−0.4 V versus RHE.At the current density of 100 mA cm^(−2),the applied potential remained stable for more than 120 h with the FE above 90%.Density functional theory calculations reveal that the abundant oxygen vacancy in In_(2)O_(3-x) has exposed more In^(3+) sites with activated electroactivity,which facilitates the formation of HCOO*intermediate.Operando X-ray absorp-tion spectroscopy also confirms In^(3+) as the active site and the key intermediate of HCOO*during the process of CO_(2) reduction to HCOOH.

关键词： CO_(2)reduction indium oxide Formate Corn design Active sites

Tailored BiVO_(4)/In_(2)O_(3)nanostructures with boosted charge separation ability toward unassisted water splitting

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Carbon Energy 2023年第6期5卷 45-59页

作者： Mi Gyoung Lee Jin Wook Yang Ik Jae Park Tae Hyung Lee Hoonkee Park Woo Seok Cheon Sol ALee Hyungsoo Lee Su Geun Ji Jun Min Suh Jooho Moon Jin Young Kim Ho Won Jang Department of Materials Science and Engineering Research Institute of Advanced MaterialsSeoul National UniversitySeoulRepublic of Korea Country Department of Applied Physics Sookmyung Women's UniversitySeoulRepublic of Korea Department of Materials Science and Engineering Yonsei UniversitySeoulRepublic of Korea Advanced Institute of Convergence Technology Seoul National UniversitySuwonRepublic of Korea

The development of new heterostructures with high photoactivity is a breakthrough for the limitation of solar-driven water splitting.Here,we first introduce indium oxide(In_(2)O_(3))nanorods(NRs)as a novel electron transport layer for bismuth vanadate(BiVO_(4))with a short charge diffusion length.In_(2)O_(3)NRs reinforce the electron transport and hole blocking of BiVO_(4),surpassing the state-of-the-art photoelectrochemical performances of BiVO_(4)-based photoanodes.Also,a tannin-nickel-iron complex(TANF)is used as an oxygen evolution catalyst to speed up the reaction kinetics.The final TANF/BiVO_(4)/In_(2)O_(3)NR photoanode generates photocurrent densities of 7.1 mAcm^(−2) in sulfite oxidation and 4.2 mA cm^(−2) in water oxidation at 1.23 V versus the reversible hydrogen electrode.Furthermore,the“artificial leaf,”which is a tandem cell with a perovskite/silicon solar cell,shows a solar-to-hydrogen conversion efficiency of 6.2%for unbiased solar water splitting.We reveal significant advances in the photoactivity of TANF/BiVO_(4)/In_(2)O_(3)NRs from the tailored nanostructure and band structure for charge dynamics.

关键词： bismuth vanadate heterojunction indium oxide nanostructure photoelectrochemical water splitting

Synergistic effect of the metal-support interaction and interfacial oxygen vacancy for CO_(2) hydrogenation to methanol over Ni/In_(2)O_(3) catalyst:A theoretical study

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Journal of Energy Chemistry 2022年第2期31卷 623-629页

作者： Chenyang Shen Qianqian Bao Wenjuan Xue Kaihang Sun Zhitao Zhang Xinyu Jia Donghai Mei Chang-jun Liu Collaborative Innovation Center of Chemical Science&Engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China State Key Laboratory of Membrane Separation and Membrane Processes School of Environmental Science and EngineeringTiangong UniversityTianjin 300387China

indium oxide supported nickel catalyst has been experimentally confirmed to be highly active for CO_(2) hydrogenation towards methanol.In this work,the reaction mechanism for CO_(2) hydrogenation to methanol has been investigated on a model Ni/In_(2)O_(3) catalyst,i.e.,Ni_(4)/In_(2)O_(3),via the density functional theory(DFT)study.Three possible reaction pathways,i.e.,the formate pathway,CO hydrogenation and the reverse water-gas-shift(RWGS)pathways,have been examined on this model catalyst.It has been demonstrated that the RWGS pathway is the most theoretically-favored for CO_(2) hydrogenation to methanol.The complete RWGS pathway follows CO_(2)+6 H→COOH+5 H→CO+H_(2)O+4 H→HCO+H_(2)O+3 H→H_(2)CO+H_(2)O+2 H→H_(3)CO+H_(2)O+H→H_(3)COH+H_(2) O.Furthermore,it has been also proved that the interfacial oxygen vacancy can serve as the active site for boosting the CO_(2) adsorption and charge transfer between the nickel species and indium oxide,which synergistically promotes the consecutive CO_(2) hydrogenation towards methanol.

关键词： CO_(2)hydrogenation indium oxide Nickel Methanol synthesis Oxygen vacancy Density functional theory

Metal-Organic Frameworks-derived indium Clusters/Carbon Nanocomposites for Efficient CO_(2) Electroreduction

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Chemical Research in Chinese Universities 2022年第5期38卷 1287-1291页

作者： GONG Yu PAN Jing ZHANG Lingling WANG Xiao SONG Shuyan ZHANG Hongjie State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022P.R.China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026P.R.China Department of Chemistry Tsinghua UniversityBeijing 100084P.R.China

Electrochemical reduction of carbon dioxide into value-added products is a promising way to recycle the greenhouse gas,thus solving the crisis of global warming.Pressing challenges remain in regulating the catalytic selectivity.In this work,we demonstrated a metal-organic frameworks-assisted approach to synthesizing In species loaded on the surface of N doped carbon matrix.By controlling the particle sizes,the catalytic selectivity can be easily altered.The obtained Inc/NC possesses the outstanding capability for converting CO_(2)into CO.And 80.09%Faraday efficiency(FE)of CO can be achieved at 0.8 V vs.RHE.While the In_(2)O_(3)/C exhibits different catalytic behaviors,the main product is formic acid and the FE is more than 50%at 0.8 V vs.RHE.The selectivity reversal can be attributed to the strong interactions between In clusters and N atoms of carbon supports,which efficiently inhibits the formation of the by-product,formic acid.Our research has paved a new way to modulate catalytic selectivity by manipulating the fine structures of the catalysts.

关键词： indium cluster indium oxide Electrochemical reduction CO_(2)electroreduction

Monolithic bilayered In_(2)O_(3) as an efficient interfacial material for high-performance perovskite solar cells

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Interdisciplinary Materials 2022年第4期1卷 526-536页

作者： Wanjia Tian Peiquan Song Yaping Zhao Lina Shen Kaikai Liu Lingfang Zheng Yujie Luo Chengbo Tian Liqiang Xie Zhanhua Wei Xiamen Key Laboratory of Optoelectronic Materials and Advanced Manufacturing Institute of Luminescent Materials and Information DisplaysCollege of Materials Science and EngineeringHuaqiao UniversityXiamenPeople's Republic of China

Carrier recombination at the buried SnO_(2)/perovskite interface limits the efficiency and stability of n-i-p-structured perovskite solar cells(PSCs).Herein,we report an In_(2)O_(3)interfacial layer with the distinctive structure of the monolithic compact/nanostructured bilayer.The partial hydrolysis nature of the In^(3+)ion enables the formation of nanorods on top of the compact In_(2)O_(3)layer when spin-coating the In(NO_(3))_(3) aqueous solution.This novel interfacial layer reduces the pinholes of the SnO_(2)film and increases the contact area between the perovskite and electron transport material.Therefore,PSCs with the incorporation of the interfacial layer demonstrate enhanced electron extraction and suppressed carrier recombination.Consequently,the champion device achieves a power conversion efficiency of 23.87%with a high fill factor of 82.14%.The optimized device also shows robust operational stability,retaining over 80%of the initial power conversion efficiency after working at the maximum power point for over 500 h under continuous one-sun illumination.

关键词： charge transfer indium oxide interfacial layer perovskite solar cells

Selective hydrogenation of CO2 to methanol over Ni/In2O3 catalyst

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Journal of Energy Chemistry 2020年第11期29卷 409-415页

作者： Xinyu Jia Kaihang Sun Jing Wang Chenyang Shen Chang-jun Liu School of Chemical Engineering and Technology Tianjin UniversityTianjin 300072China

An In2O3 supported nickel catalyst has been prepared by wet chemical reduction with sodium borohydride(NaBH4) as a reducing agent for selective hydrogenation of carbon dioxide to methanol. Highly dispersed Ni species with intense Ni-In2O3 interaction and enhanced oxygen vacancies have been achieved.The highly dispersed Ni species serve as the active sites for hydrogen activation and hydrogen spillover.Abundant H adatoms are thereby generated for the oxygen vacancy creation on the In2O3 surface. The enhanced surface oxygen vacancies further lead to improved CO2 conversion. As a result, an effective synergy between the active Ni sites and surface oxygen vacancies on In2O3 causes a superior catalytic performance for CO2 hydrogenation with high methanol selectivity. Carbon monoxide is the only by product detected. The formation of methane can be ignored. When the reaction temperature is lower than 225 ℃,the selectivity of methanol is 100%. It is higher than 64% at the temperature range between 225 ℃ and 275 ℃. The methanol selectivity is still higher than 54% at 300 ℃ with a CO2 conversion of 18.47% and a methanol yield of 0.55 gMeOHg-1cath-1(at 5 MPa). The activity of Ni/In2O3 is higher than most of the reported In2O3-based catalysts.

关键词： Methanol CO2 hydrogenation indium oxide Ni/In2O3 Oxygen vacancy