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Unraveling the advantages of Pd/CeO_(2)single-atom catalysts in the NO+CO reaction by model catalysts

Nano Research 2023年第7期16卷 8882-8892页

作者： Qian Xu Xingwang Cheng Ningqiang Zhang Yi Tu Lihui Wu Haibin Pan Jun Hu Honghe Ding Junfa Zhu Yadong Li Department of Chemistry Tsinghua UniversityBeijing 100084China National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029China College of Chemistry and Materials Science Anhui Normal UniversityWuhu 241002China

Selective catalytic reduction of NO by CO is challenging in environmental catalysis but attractive owing to the advantage of simultaneous elimination of NO and CO.Here,model catalysts consisting of Pd nanoparticles(NPs)and single-atom Pd supported on a CeO_(2)(111)film grown on Cu(111)(denoted as Pd NPs/CeO_(2)and Pd_(1)/CeO_(2),respectively)were successfully prepared and characterized by synchrotron radiation photoemission spectroscopy(SRPES)and infrared reflection absorption spectroscopy(IRAS).The NO+CO adsorption/reaction on the Pd_(1)/CeO_(2)and Pd NPs/CeO_(2)catalysts were carefully investigated using SRPES,temperature-programmed desorption(TPD),and IRAS.It is found that the reaction products on both model catalysts are in good agreement with those on real catalysts,demonstrating the good reliability of using these model catalysts to study the reaction mechanism of the NO+CO reaction.On the Pd NPs/CeO_(2)surface,N_(2)is formed by the combination of atomic N coming from the dissociation of NO on Pd NPs at higher temperatures.N_(2)O formation occurs probably via chemisorbed NO combined with atomic N on the surface.While on the single-atom Pd_(1)/CeO_(2)surface,no N_(2)O is detected.The 100%N_(2)selectivity may stem from the formation of O-N-N-O^(*)intermediate on the surface.Through this study,direct experimental evidence for the reaction mechanisms of the NO+CO reaction is provided,which supports the previous density functional theory(DFT)calculations.

关键词： NO+CO reaction Pd/CeO_(2) model catalysts reaction mechanisms

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Morphology-Dependent Catalysis of CeO_(2)-Based Nanocrystal model catalysts

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Chinese Journal of Chemistry 2022年第15期40卷 1856-1866页

作者： Yang Wen Qiuyu Huang Zhenhua Zhang Weixin Huang Key Laboratory of the Ministry of Education for Advanced Catalysis Materials Zhejiang Key Laboratory for Reactive Chemistry on Solid SurfacesInstitute of Physical ChemistryZhejiang Normal UniversityJinhuaZhejiang 321004China Hefei National Laboratory for Physical Sciences at the Microscale Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes and Department of Chemical PhysicsUniversity of Science and Technology of ChinaHefeiAnhui 230026China Dalian National Laboratory for Clean Energy Chinese Academy of SciencesDalianLiaoning 116023China

Comprehensive Summary Recent progress in colloidal synthesis has realized the preparations of uniform nanocrystal(NC)model catalysts with rich and well-controlled morphologies that were employed to explore structure-activity relationships of powder catalysts,similar to single-crystal-based model catalysts under ultrahigh vacuum conditions but can work at the same conditions as powder catalysts without the"materials gap"and"pressure gap".In this perspective,the CeO_(2)-based NC model catalysts with various morphologies are included and their relevant progresses are critically reviewed.The detailed descriptions of morphology-controlled synthesis and characterizations of uniform CeO_(2)NCs.

关键词： CeO_(2)naocrystals model catalysts Surface chemistry Heterogeneous catalysis Structure-activity relationships

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SIMULATION modelING ON THE COORDINATION MECHANISM OF ETHYLENE MONOMER ON VARIOUS PREREDUCED Cr（Ⅱ）Ox/SiO2 PHILLIPS POLYETHYLENE model catalysts

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Chinese Journal of Polymer Science 2008年第5期26卷 579-587页

作者：刘柏平 State Key Lab of Chemical Engineering East China University of Science and TechnologyMei Long Road 130Shanghai 200237China

As one of the most important catalysts in polyethylene industry,Phillips catalyst(CrO_x/SiO_2)was quite unique for its activation by ethylene monomer without using any activator like alkyl-aluminium or MAO.In this work,the density functional theory(DFT)calculation combined with paired interacting orbitals(PIO)method was applied for the theoretical studies on coordination reaction mechanism between ethylene monomer and two model catalysts namely Cr(Ⅱ)(OH)_2(M1) and silsesquioxane-supported Cr(Ⅱ)(M2)as surfac...

关键词： Phillips catalyst（CrO_x/SiO_2） Polyethylene model catalysts Density functional theory（DFT） Paired interacting orbitals（PIO）.

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Correlation between the structure of gold and silver model catalysts and their CO oxidation,NOX reduction activities

Correlation between the structure of gold and silver model c...

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第18届国际真空大会

作者： Krisztina Frey Gábor Pet Ferenc Tanczikó László Guczi Institute of Isotopes HASH-1525 BudapestP.O.Box 77Hungary KFKI Research Institute for Particle and Nuclear Physics H-1525 BudapestP.O.Box. 49Hungary

Automotive exhaust gas contains high concentrations of NOx, CO, and hydrocarbons, which are harmful to human health. Although these components can be reduced drastically by the use of a three-way catalyst, nitrous oxide, N2O, which has a strong greenhouse effect, is produced during the catalytic reaction. The present work is aimed at developing a novel family of catalysts, based on gold and silver, to replace the more expensive platinum and rhodium metals.

关键词： model catalysts XPS nanoparticles oxides

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Combination of a reaction cell and an ultra-high vacuum system for the in situ preparation and characterization of a model catalyst

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Nuclear Science and Techniques 2023年第5期34卷 13-21页

作者： Yi-Jing Zang Shu-Cheng Shi Yong Han Hui Zhang Wei-Jia Wang Peng Liu Mao Ye Zhi Liu State Key Laboratory of Functional Materials for Informatics Shanghai Institute of Microsystem and Information TechnologyChinese Academy of SciencesShanghai 200050China School of Physical Science and Technology ShanghaiTech UniversityShanghai 201210China Center for Transformative Science ShanghaiTech UniversityShanghai 201210China University of Chinese Academy of Sciences Beijing 100049China

An in-depth understanding of the structure-activity relationship between the surface structure,chemical composition,adsorption and desorption of molecules,and their reaction activity and selectivity is necessary for the rational design of high-performance catalysts.Herein,we present a method for studying catalytic mechanisms using a combination of in situ reaction cells and surface science techniques.The proposed system consists of four parts:preparation chamber,temperatureprogrammed desorption(TPD)chamber,quick load-lock chamber,and in situ reaction cell.The preparation chamber was equipped with setups based on the surface science techniques used for standard sample preparation and characterization,including an Ar+sputter gun,Auger electron spectrometer,and a low-energy electron diffractometer.After a well-defined model catalyst was prepared,the sample was transferred to a TPD chamber to investigate the adsorption and desorption of the probe molecule,or to the reaction cell,to measure the catalytic activity.A thermal desorption experiment for methanol on a clean Cu(111)surface was conducted to demonstrate the functionality of the preparation and TPD chambers.Moreover,the repeatability of the in situ reaction cell experiment was verified by CO_(2) hydrogenation on the Ni(110)surface.At a reaction pressure of 800 Torr at 673 K,turnover frequencies for the methanation reaction and reverse water-gas shift reaction were 0.15 and 7.55 Ni atom^(-1) s^(-1),respectively.

关键词： Surface science model catalysts Ultra-high vacuum Temperature-programmed desorption In situ reaction cell

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Unraveling the Dynamic Structural Evolution of Phthalocyanine catalysts during CO_(2) Electroreduction

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Chinese Journal of Structural Chemistry 2022年第10期41卷 82-88页

作者： Jianing Mao Bingbao Mei Ji Li Shuai Yang Fanfei Sun Siyu Lu Wei Chen Fei Song Zheng Jiang Shanghai Institute of Applied Physics Chinese Academy of SciencesShanghai 201204China University of Chinese Academy of Sciences Beijing 100049China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China College of Chemistry College of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450000China Low-Carbon Conversion Science and Engineering Center Shanghai Advanced Research InstituteChinese Academy of ScienceShanghai 201210China Innovation Academy for Green Manufacture Chinese Academy of SciencesBejing 100190China

Understanding the atomic and electronic changes of active sites promotes the whole new sight into electrochemical carbon dioxide reduction reaction(CO_(2)RR),which provides a feasible strategy to achieve carbon neutrality.Here we employ operando high-energy resolution fluorescence-detected Xray absorption spectroscopy(HERFD-XAS)to track the structural evolution of Ni(II)phthalocyanine(NiPc),considered as the model catalysts with uniform Ni-N_(4)-C_(8) moiety,during the CO_(2)RR.The HERFD-XAS method is in favor of elucidating the interaction of the reactant/catalyst interface from the atomic electronic structure dimension,facilitating the establishment of the catalytic mechanism and the dynamic structure changes.Based on operando measurement,surface sensitive difference spectra(△μ)and spectroscopy simulation,the interfacial interactions between the active sites of NiPc and reactants are monitored and the Ni species gradually reduced by increasing the applied potential is discovered.HERFD-XAS method offers an advanced and powerful tool for elucidating the complex catalytic mechanism in further various systems.

关键词： CO_(2)electrochemical reduction HERFD-XAS model catalysts difference spectra structural evolution

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