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Data-Driven Design of Single-Atom Electrocatalysts with Intrinsic Descriptors for Carbon Dioxide Reduction Reaction

Transactions of Tianjin University 2024年第5期30卷 459-469页

作者： Xiaoyun Lin Shiyu Zhen Xiaohui Wang Lyudmila V.Moskaleva Peng Zhang zhi-jian zhao Jinlong Gong Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Collaborative Innovation Center of Chemical Science and Engineering(Tianjin) Tianjin 300072China School of Economics and Management Tianjin University of Technology and EducationTianjin 300222China Department of Chemistry University of the Free StateP.O.Box 339Bloemfontein 9301South Africa Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China National Industry-Education Platform of Energy Storage Tianjin UniversityTianjin 300350China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207FujianChina

The strategic manipulation of the interaction between a central metal atom and its coordinating environment in single-atom catalysts(SACs)is crucial for catalyzing the CO_(2)reduction reaction(CO_(2)RR).However,it remains a major *** density-functional theory calculations serve as a powerful tool for catalyst screening,their time-consuming nature poses *** paper presents a machine learning(ML)model based on easily accessible intrinsic descriptors to enable rapid,cost-effective,and high-throughput screening of efficient SACs in complex *** ML model comprehensively captures the influences of interactions between 3 and 5d metal centers and 8 C,N-based coordination environments on CO_(2)RR activity and *** reveal the electronic origin of the different activity trends observed in early and late transition metals during coordination with N *** extreme gradient boosting regression model shows optimal performance in predicting binding energy and limiting potential for both HCOOH and CO *** confirm that the product of the electronegativity and the valence electron number of metals,the radius of metals,and the average electronegativity of neighboring coordination atoms are the critical intrinsic factors determining CO_(2)RR *** developed ML models successfully predict several high-performance SACs beyond the existing database,demonstrating their potential applicability to other *** work provides insights into the low-cost and rational design of high-performance SACs.

关键词： Density functional theory Machine learning CO_(2) reduction reaction Electrocatalysts High-throughput screening

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Kinetically rate-determining step modulation by metal-support interactions for CO oxidation on Pt/CeO_(2)

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Science China Chemistry 2022年第10期65卷 2038-2044页

作者： Yanan Wang Chunlei Pei zhi-jian zhao Jinlong Gong Collaborative Innovation Center of Chemical Science and Engineering Key Laboratory for Green Chemical Technology of Ministry of EducationSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300072China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207China

Rational design and performance promotion are eternal topics and ultimate goals in catalyst *** contrast,trial–and–error is still the common method people ***,it is important to develop methods to intrinsically enhance the performance of *** most effective solutions are the one from a kinetic perspective based on clear knowledge of the reaction *** paper describes rate-determining step cognition and modulation to promote CO oxidation on highly dispersed Pt on CeO_(2).The different degrees of metal–support interactions due to variation of hydroxyl density of support could alter the structure of active species and the ability of oxygen activation apparently,further shift the rate-determining step from oxygen activation to oxygen reverse spillover *** transformation of rate-determining step could enhance the intrinsic activity significantly,and decrease the T_(50) approximately 140℃.The findings of this research exemplify the universal and effective method of performance elevation by rate-determining step modulation,which is promising for application in different systems.

关键词： highly dispersed Pt/CeO_(2)catalysts single atom catalysis CO oxidation performance promotion rate-determining step modulation reaction kinetics

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调控氧传输以实现甲烷化学链部分氧化表面和体相速率的匹配

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Science China Materials 2024年第4期67卷 1217-1224页

作者：杨婷婷罗冉石向成张先华吴仕灿裴春雷赵志坚巩金龙 Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering&TechnologyTianjin UniversityCollaborative Innovation Center of Chemical Science and EngineeringTianjin 300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China National Industry-Education Plaform of Energy Storage Tianjin UniversityTianjin 300350China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou 350207China Department of Chemistry National University of SingaporeScience Drive 3Singapore 117543Republic of Singapore

甲烷化学链部分氧化(CL-POM)是一种有前景的合成气生产技术,具有高选择性和低爆炸风险的优势.然而,开发性能优异、可持续释氧的金属载氧体仍然面临挑战.为此,本研究设计了一种复合载氧体(LaFeO_(3-δ)/Ca_(1-η)Sr_(η)MnO_(3)),通过调... 详细信息

甲烷化学链部分氧化(CL-POM)是一种有前景的合成气生产技术,具有高选择性和低爆炸风险的优势.然而,开发性能优异、可持续释氧的金属载氧体仍然面临挑战.为此,本研究设计了一种复合载氧体(LaFeO_(3-δ)/Ca_(1-η)Sr_(η)MnO_(3)),通过调控Ca_(1-η)Sr_(η)MnO_(3)的氧扩散来维持LaFeO_(3-δ)(121)缺陷表面的活性结构,从而提升了CL-POM的活性和选择性.理论计算结果表明,甲烷在LaFeO_(3-δ)(121)缺陷表面上的反应活性位点主要是Fe-O_(4)(O_(V))和Fe-O_(3)(O_(V))_(2),它们表现出相近的反应能垒(ΔG_(a)=1.44和1.40 eV).氧扩散系数和表面反应速率常数分别由体相氧迁移能垒和表面反应能垒确定,进而计算得到体相氧扩散和表面反应的速率,用以评估两者的匹配程度.最后,本研究证实了LaFeO_(3-δ)/Ca_(0.75)-Sr_(0.25)MnO_(3)是一种有潜力的CL-POM载氧体,其能够实现体相氧扩散速率与表面氧消耗速率的合理匹配,并有效地抑制不利的相变过程.

关键词：反应速率常数表面反应载氧体化学链氧扩散部分氧化活性结构氧化表面

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Exploring the initial oxidation of Pt,Pt_(3)Ni,Pt_(3)Au(111)surfaces:a genetic algorithm based global optimization with density functional theory

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Green Chemical Engineering 2020年第1期1卷 56-62页

作者： Sihang Liu Jie Zong zhi-jian zhao Jinlong Gong School of Chemical Engineering and Technology Key Laboratory for Green Chemical Technology of Ministry of EducationTianjin UniversityTianjin300072China Collaborative Innovation Center of Chemical Science and Engineering Tianjin300072China Department of Chemistry The Pennsylvania State UniversityUniversity ParkPA 16802USA Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou350207China

Noble metal alloys are one of the most commonly used heterogeneous *** many reactions,the surface composition and oxidation states of the noble metal alloy particles have been reported to be *** paper describes a density functional theory study to explore the initial oxidation stages of the Ptbased surfaces,which are widely-used catalysts in various clean energy conversion *** applying a genetic algorithm based global optimization,we identified new surface phases at relatively high O coverages,1 ML and 3/2 ML,on Pt and Pt alloy(111)*** existence of O transforms the metallic surfaces,creating oxide skins with different morphology and *** with higher reducibility are pulled out to the outmost surface,to bind with O *** lattice constant affects the binding strength of O atoms over certain oxide ***,the strain effect plays a crucial role in the formation of oxide overlayers.

关键词： alloy theory optimization

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The role of CO_(2)dissociation in CO_(2)hydrogenation to ethanol on CoCu/silica catalysts

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Nano Research 2023年第5期16卷 6128-6133页

作者： Zhongyan Wang Chengsheng Yang Xianghong Li Xiwen Song Chunlei Pei zhi-jian zhao Jinlong Gong Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyCollaborative Innovation Center of Chemical Science and EngineeringTianjin UniversityTianjin 300072China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou 350207China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

CoCu-based catalysts are widely used in CO_(x) hydrogenation reactions to produce higher alcohols due to the C–C coupling ability of Co and the ability of Cu to produce *** work describes the role of easily happened CO_(2)dissociation on the CoCu surface during the reaction,using different silica support to tune the metal–support interaction,reaches different selectivity to *** supported on mesoporous silica MCM-41 shows ethanol selectivity as high as 85.3%,the ethanol space-time yield(STY)is 0.229 mmol/(gmetal∙h),however,poor selectivity to ethanol as low as 28.8%is observed on CoCu supported on amorphous *** different selectivity is due to the different intensities of CO_(2)dissociation on the *** adsorbed O*produced via CO_(2)dissociation can occupy the cobalt hollow sites on CoCu surfaces,which are also the adsorption sites of C1 intermediates for further C–C coupling.

关键词： CO_(2)hydrogenation bimetallic catalysts cobalt catalysts CO_(2)dissociation ethanol synthesis

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Neural Network Accelerated Investigation of the Dynamic Structure-Performance Relations of Electrochemical CO_(2) Reduction over SnO_(x),Surfaces

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Research 2023年第2期2023卷 351-360页

作者： Lulu Li zhi-jian zhao Gong Zhang Dongfang Cheng Xin Chang Xintong Yuan Tuo Wang Jinlong Gong School of Chemical Engineering and Technology Key Laboratory for Green Chemical Technology of Ministry of EducationTianjin UniversityTianjin 300072China Collaborative Innovation Center for Chemical Science and Engineering(Tianjin) Tianjin 300072China National Industry-Education Platform of Energy Storage Tianjin UniversityTianjin 300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207China

Heterogeneous catalysts,especially metal oxides,play a curial role in improving energy conversion efficiency and production of valuable ***,the surface structure at the atomic level and the nature of active sites are still ambiguous due to the dynamism of surface structure and difficulty in structure characterization under electrochemical conditions.

关键词： conditions structure difficulty

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Chemical looping oxidative propane dehydrogenation controlled by oxygen bulk diffusion over FeVO_(4)oxygen carrier pellets

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Chinese Journal of Chemical Engineering 2023年第1期53卷 409-420页

作者： Hongbo Song Wei Wang Jiachen Sun Xianhui Wang Xianhua Zhang Sai Chen Chunlei Pei zhi-jian zhao Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Collaborative Innovation Center of Chemical Science and Engineering Tianjin 300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China Zhejiang Institute of Tianjin University Ningbo 315201China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207China Department of Chemistry National University of Singapore3 Science Drive 3117543Singapore

The oxygen distribution and evolution within the oxygen carrier exert significant influence on chemical looping *** paper describes the influence of oxygen bulk diffusion within FeVO4 oxygen carrier pellets on the chemical looping oxidative propane dehydrogenation(CL-ODH).During CL-ODH,the oxygen concentration at the pellet surface initially decreased and then maintained stable before the final *** the stage with the stable surface oxygen concentration,the reaction showed a stable C3H6 formation rate and high C3H6 ***,based on Fick’s second law,the oxygen distribution and evolution in the oxygen carrier at this stage were further *** was found that main reactions of selective oxidation and over-oxidation were controlled by the oxygen bulk diffusion.C3H8 conversion rate kept decreasing during this stage due to the decrease of the oxygen flux caused by the decline of oxygen gradient within the oxygen carrier,while C3H6 selectivity increased due to the decrease of *** addition,reaction rates could increase with the propane partial pressure due to the increase of the oxygen gradient within the oxygen carrier until the bulk transfer reached its limit at higher propane partial *** study provides fundamental insights for the diffusion-controlled chemical looping reactions.

关键词： Chemical looping Diffusion Reaction kinetics Oxygen carriers Oxidation

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Theory assisted design of N-doped tin oxides for enhanced electrochemical CO2 activation and reduction

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Science China Chemistry 2019年第8期62卷 1030-1036页

作者： Congling Hu Lei Zhang Lulu Li Wenjin Zhu Wanyu Deng Hao Dong zhi-jian zhao Jinlong Gong Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityCollaborative Innovation Center of Chemical Science and Engineering (Tianjin)Tianjin 300072China Department of Mechanical and Materials Engineering Western UniversityLondonON N6A 5B9Canada

Clearly understanding the structure-function relationship and rational design of efficient CO2 electrocatalysts are still the *** article describes the molecular origin of high selectivity of formic acid on N-doped SnO2 nanoparticles,which obtained via thermal treatment of g-C3N4 and SnCl2·2H2O *** with density functional theory(DFT)calculations,we discover that N-doping effectively introduces oxygen vacancies and increases the charge density of Sn sites,which plays a positive role in CO2 *** addition,N-doping further regulates the adsorption energy of^*OCHO,^*COOH,^*H and promotes HCOOH *** from above modulation,the obtained N-doped SnO2 catalysts with oxygen vacancies(Ov-N-SnO2)exhibit faradaic efficiency of 93% for C1 formation,88% for HCOOH production and well-suppression of H2 evolution over a wide range of potentials.

关键词： N-doped SnO2 oxygen vacancy charge density CO2 activation electrochemical CO2 reduction

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Fabrication of bilayer Pd-Pt nanocages with sub-nanometer thin shells for enhanced hydrogen evolution reaction

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Nano Research 2019年第9期12卷 2268-2274页

作者： Yihe Wang Lei Zhang Congling Hu Shengnan Yu Piaoping Yang Dongfang Cheng zhi-jian zhao Jinlong Gong Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityCollaborative Innovation Center of Chemical Science and Engin eeringTianjin 300072China

The hydrogen evolution reaction (HER),which generates molecular hydrogen through the electrochemical reduction of water,is an important clean-energy *** (Pt) is an ideal material for HER electrocatalysts in terms of low overpotential and fast *** effective method to improve the atom utilization efficiency of Pt is to fabricate Pt-based core-shell or nanocage structures with ultra-thin *** paper describes the construction of bilayer palladium (Pd)-Pt alloy nanocages catalyst with enhanced HER catalytic *** nanocages were fabricated by etching away the Pd templates of multishelled nanocubes composed of alternate shells of Pd and Pt with well-defined (100) *** bilayer Pd-Pt nanocages with sub-nanometer shells have a high dispersion of the active atoms on the outside and inside surfaces of outer layer and inner layer,***,the Pd-Pt alloy lowers the overpotential for HER and speeds up the reaction rate of HER due to the synergies between Pd and *** rational design of bilayer nanocages provided a novel route for boosting the atom utilization efficiency of Pt catalysts.

关键词： Pd-Pt alloy multishelled nanocubes nanocages hydrogen evolution reaction electrocatalysis

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Defect-mediated reactivity of Pt/TiO2 catalysts:the different role of titanium and oxygen vacancies

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Science China Chemistry 2020年第9期63卷 1323-1330页

作者： Quan Xiao Yanan Wang zhi-jian zhao Chunlei Pei Sai Chen Lijun Gao Rentao Mu Qiang Fu Jinlong Gong Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityCollaborative Innovation Center of Chemical Science and EngineeringTianjin 300072China State Key Laboratory of Catalysis iChEMDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207China

Defects are ubiquitous in oxide supports and can often tune the catalytic property of supported metal *** work describes the distinct role of titanium and oxygen vacancies of TiO2 supports in the catalytic performance of supported Pt catalysts for CO *** was loaded on the TiO2 supports with oxygen vacancies(VO-TiO2)and titanium vacancies(VTiTiO2).It was found that different defects of TiO2 could distinctively modify the electron property of Pt and thereby CO adsorption *** strength of CO adsorption on Pt/VTi-TiO2 is enhanced,while that of Pt/VO-TiO2 becomes ***,the presence of defects would also promote the reducibility of *** the account of the superior redox ability,both Pt/VTi-TiO2 and Pt/VO-TiO2 exhibit a higher activity than Pt supported on normal TiO2 for CO oxidation.

关键词： defects electronic metal-support interaction titanium vacancies oxygen vacancies CO oxidation

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