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Porous Metal Nanocrystal Catalysts:Can Crystalline Porosity Enable catalytic selectivity?

CCS Chemistry 2022年第6期4卷 1829-1842页

作者： Xiaowen Min Hao Lv Yusuke Yamauchi Ben Liu Key Laboratory of Green Chemistry and Technology of the Ministry of Education College of ChemistrySichuan UniversityChengdu 610064 Australian Institute for Bioengineering and Nanotechnology(AIBN) School of Chemical EngineeringThe University of QueenslandBrisbaneQLD 4072 JST-ERATO Yamauchi Materials Space-Tectonics Project International Research Centre for Materials Nanoarchitechtonics(WPI-MANA)National Institute for Materials Science(NIMS)TsukubaIbaraki 305-0044

catalytic selectivity is a central issue in the efficiency of catalytic processes.A large number of strategies have been developed to improve the catalytic selectivity of metal catalysts at the atomic and molecular levels,for instance,alloying secondary elements,fabricating metal-support interactions,and introducing surface ***,macro/mesoscopic pores and cavities have been demonstrated as an alternative route to promote catalytic selectivity of metal nanocrystal *** promotion effects of continuous crystalline porosity include(1)more catalytically active sites that accelerate the favorable catalytic routes to targeted products,(2)confined spaces that increase the retention time of key intermediates and remarkably promote the selective catalysis toward desired products,and(3)an optimized electronic structure and coordination environment of active metal sites that tailor the reaction trends of selective catalysis toward desired *** this minireview,we summarize recent advances in porosity-enabled catalytic selectivity of metal nanocrystal catalysts with focused discussions of CO_(2) reduction electrocatalysis and selective hydrogenation *** mechanisms that allow for the continuous porosity that enables the catalytic selectivity of metal nanocrystal catalysts are discussed in *** end this minireview by proposing current challenges and offering future opportunities in this research field.

关键词： porous metal continuous crystalline porosity structural synergy confinement catalytic selectivity

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Accurate Description of catalytic selectivity:Challenges and Opportunities for the Development of Density Functional Approximations

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CCS Chemistry 2021年第11期3卷 136-143页

作者： Zhe-Ning Chen Tonghao Shen Yizhen Wang Igor Ying Zhang Collaborative Innovation Center of Chemistry for Energy Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsMOE Key Laboratory of Computational Physical SciencesShanghai Key Laboratory of Bioactive Small MoleculesDepartment of ChemistryFudan UniversityShanghai 200433 State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002

An accurate description of catalytic selectivity poses an enormous challenge for theoretical *** to the absence of a well-defined benchmark set on the catalytic selectivity,the performance of even the widely used density functional approximations(DFAs)is yet to be *** work reports a test set based on the selective hydrogenation ofα,β-unsaturated aldehydes catalyzed by ruthenium(Ru)hydride *** attention is paid to benchmark the regioselectivity of aldehydes to either unsaturated alcohols or saturated *** reference data were calculated by the massive parallel implementation of the coupled-cluster single,double,and perturbative triple excitations[CCSD(T)]approach,based completely on set ***,we performed the microkinetic simulation based on the CCSD(T)energy profiles,serving the most direct criteria for the performance of DFAs on catalytic selectivity of hydrogenation *** this test set,we uncovered the intrinsic difficulty of semilocal and hybrid functionals for such a *** the context of the XYG3-type double hybrid(xDH)framework,we showed that this particular challenge could be addressed by the top rung functionals only when the many-body nondynamic correlation effect was accounted for adequately.A recently proposed xDH,namely scsRPA,showed unprecedented accuracy with only 5%error on *** predicted kinetic selectivity by scsRPA is in close agreement with the reference value,revealing a unique versatility of the top rung DFAs for a reliable description of catalytic selectivity of hydrogenation reactions.

关键词： density functional theory catalytic selectivity doubly hybrid approximation nondynamic correlation

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A facile strategy to construct MOF-based nanocatalyst with enhanced activity and selectivity in oxytetracycline degradation

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Nano Research 2024年第7期17卷 5863-5871页

作者： Yanjing Ke Jiaxing Zhang Xin Peng Zhiyi Zhang Xu Wang Wei Qi Mengfan Wang School of Life Sciences Faculty of MedicineSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China The Co-Innovation Centre of Chemistry and Chemical Engineering of Tianjin Tianjin 300072China Tianjin Key Laboratory of Membrane Science and Desalination Technology Tianjin 300350China

Recently,many efforts have been dedicated to construct artificial catalysts with enzyme-like ***,it is still a big challenge to endow artificial catalysts with specific substrate *** this study,we developed a facile strategy to construct a MIL-53(Fe)-based nanocatalyst with designable selectivity in the degradation of oxytetracycline(OTC).Through the Fe–O–P conjunction,oxytetracycline aptamer(OA)can be easily anchored on MIL-53(Fe)to provide the specific site for OTC *** verified that the obtained MIL-53(Fe)-Apt nanocatalyst displayed enhanced catalytic ability in the degradation of OTC,whereas obvious suppression toward other substrate *** performance therefore brings about an anticipated selectivity toward ***,we highlighted that the configuration of aptamers on MIL-53(Fe)can be modulated through varying conjunction ***–function analysis revealed that aptamer configuration affects the local concentration of substrate around catalytic site,which thus decides the catalytic performance toward *** work presented a facile and promising strategy for developing artificial catalysts with designable selectivity.

关键词： MIL-53(Fe) aptamer Fe-O-P catalytic selectivity oxytetracycline

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Compressive strain in Cu catalysts: Enhancing generation of C2+ products in electrochemical CO2 reduction

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SCIENCE BULLETIN 2024年第18期69卷 2881-2891页

作者： Fan, Qikui Yan, Pengxu Liu, Fuzhu Xu, Zhongshuang Liang, Pengfei Cao, Xi Ye, Chenliang Liu, Moxuan Zhao, Lingyi Ren, Shan Miao, Huanran Zhang, Xiai Yang, Zhimao Ding, Xiangdong Yang, Jian Kong, Chuncai Wu, Yuen Xi An Jiao Tong Univ Sch Phys MOE Key Lab Nonequilibrium Synth & Modulat Condens Key Lab Adv Mat & Mesoscop Phys Shaanxi Prov Xian 710049 Peoples R China Xi An Jiao Tong Univ State Key Lab Mech Behav Mat Xian 710049 Peoples R China Anhui Normal Univ Coll Chem & Mat Sci Wuhu 241002 Peoples R China North China Elect Power Univ Dept Power Engn Beijing 102206 Peoples R China Xian Univ Sci & Technol Coll Chem & Chem Engn Xian 710054 Peoples R China Chinese Acad Sci Shenzhen Inst Adv Technol Ctr Mat & Interfaces Shenzhen 518055 Peoples R China Univ Sci & Technol China Collaborat Innovat Ctr Chem Energy Mat iChEM Sch Chem & Mat Sci Hefei Natl Lab Phys Sci Microscale Hefei 230026 Peoples R China Univ Sci & Technol China Natl Synchrotron Radiat Lab Hefei 230026 Peoples R China

Elastic strain in Cu catalysts enhances their selectivity for the electrochemical CO2 reduction reaction (eCO(2)RR), particularly toward the formation of multicarbon (C2+) products. However, the reasons for this selectivity and the effect of catalyst precursors have not yet been clarified. Hence, we employed a redox strategy to induce strain on the surface of Cu nanocrystals. Oxidative transformation was employed to convert Cu nanocrystals to CuxO nanocrystals; these were subsequently electrochemically reduced to form Cu catalysts, while maintaining their compressive strain. Using a flow cell configuration, a current density of 1 A/cm(2) and Faradaic efficiency exceeding 80% were realized for the C2+ products. The selectivity ratio of C2+/C1 was also remarkable at 9.9, surpassing that observed for the Cu catalyst under tensile strain by approximately 7.6 times. In-situ Raman and infrared spectroscopy revealed a decrease in the coverage of K+ ion-hydrated water (KH2O) on the compressively strained Cu catalysts, consistent with molecular dynamics simulations and density functional theory calculations. Finite element method simulations confirmed that reducing the coverage of coordinated KH2O water increased the probability of intermediate reactants interacting with the surface, thereby promoting efficient C-C coupling and enhancing the yield of C2+ products. These findings provide valuable insights into targeted design strategies for Cu catalysts used in the eCO(2)RR. (c) 2024 Science China Press. Published by Elsevier B.V. and Science China Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.

关键词： Strain effect CO2 electroreduction to C2+ catalytic selectivity Copper catalyst Water coverage SPECTROSCOPY REVEALS CARBON-MONOXIDE COPPER selectivity ETHYLENE OPERANDO

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selectivity control in alkyne semihydrogenation:Recent experimental and theoretical progress

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Chinese Journal of Catalysis 2022年第8期43卷 1991-2000页

作者： Xiao-Tian Li Lin Chen Cheng Shang Zhi-Pan Liu Collaborative Innovation Center of Chemistry for Energy Material Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsKey Laboratory of Computational Physical ScienceDepartment of ChemistryFudan UniversityShanghai 200433China

Researchers have been attempting to characterize heterogeneous catalysts in situ in addition to correlating their structures with their activity and selectivity in spite of many ***,we review recent experimental and theoretical advances regarding alkyne selective hydrogenation by Pd‐based catalysts,which are an important petrochemical *** catalytic selectivity for the reaction of alkynes to alkenes is influenced by the composition and structure of the *** progress achieved through experimental studies and atomic simulations has provided useful insights into the origins of the *** important role of the subsurface species(H and C)was revealed by monitoring the catalyst surface and the related catalytic *** atomic structures of the Pd catalytic centers and their relationship with selectivity were established through atomic *** combined knowledge gained from experimental and theoretical studies provides a fundamental understanding of catalytic mechanisms and reveals a path toward improved catalyst design.

关键词： Alkyne semihydrogenation catalytic selectivity Surface science Machine learning Neural network potential

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Cobalt sandwich complex-based covalent organic frameworks for chemical fixation of CO

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Science China Materials 2022年第5期65卷 1377-1382页

作者： Yang Li Xiaoyu Song Guang Zhang Weihua Chen Lei Wang Yi Liu Long Chen Shenzhen Key Laboratory of Polymer Science and Technology Guangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Materials Science and EngineeringShenzhen UniversityShenzhen 518060China College of Physics and Optoelectronic Engineering Shenzhen UniversityShenzhen 518060China Tianjin Key Laboratory of Molecular Optoelectronic Science Department of ChemistryTianjin UniversityTianjin 300072China College of Chemistry and Green Catalysis Center Zhengzhou UniversityZhengzhou 450001China

Carbon dioxide as a notorious greenhouse gas triggers severe global warming which is threatening the balance of ecosystem. In this respect, effectively capturing and transforming CO_(2)into value-added chemicals are essential but still challenging tasks. As a kind of emerging crystalline porous material, covalent organic frameworks(COFs) have been demonstrated to be able to adsorb gases and function as catalysts to facilitate chemical transformations. Herein, we report an imine-linked, cobalt sandwich complex-based COF(Co-BD-COF) with high crystallinity and large surface ***-BD-COF can efficiently catalyze the transformation of CO_(2)into cyclic carbonates due to abundant metal sites and high porosity. In addition, Co-BD-COF exhibits high catalytic selectivity toward small ethylene oxide derivatives in cycloaddition reaction due to the large steric hindrance around the cobalt complexes rendered by the peripheral phenyl *** new metal sandwich-type building block provides a new strategy for improving catalytic selectivity of COFs.

关键词： covalent organic frameworks cobalt sandwich complex carbon dioxide heterocatalysis catalytic selectivity

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Selective photocatalytic reduction of CO2 to CO mediated by a[FeFe]-hydrogenase model with a 1,2-phenylene S-to-S bridge

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Chinese Journal of Catalysis 2021年第2期42卷 310-319页

作者： Minglun Cheng Xiongfei Zhang Yong Zhu Mei Wang State Key Laboratory of Fine Chemicals Dalian University of TechnologyDalian 116024LiaoningChina

Photocatalytic reduction of CO2 to CO is a promising approach for storing solar energy in chemicals and mitigating the greenhouse effect of *** recent studies revealed that[(μ-bdt)Fe2(CO)6](1,bdt=benzene-1,2-dithiolato),a[FeFe]-hydrogenase model with a rigid and conjugate S-to-S bridge,was catalytically active for the selective photochemical reduction of CO2 to CO,while its analogous complex[(μ-edt)Fe2(CO)6](2,edt=ethane-1,2-dithiolato)was *** this study,it was found that the turnover number of 1 for CO evolution reached 710 for the 1/[Ru(bpy)3]2+/BIH(BIH=1,3-dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]-imidazole)system under optimal conditions over 4.5 h of visible-light irradiation,with a turnover frequency of 7.12 min−1 in the first hour,a high selectivity of 97%for CO,and an internal quantum yield of 2.8%.Interestingly,the catalytic selectivity of 1 can be adjusted and even completely switched in a facile manner between the photochemical reductions of CO2 to CO and of protons to H2 simply by adding different amounts of triethanolamine to the catalytic *** electron transfer in the photocatalytic system was studied by steady-state fluorescence and transient absorption spectroscopy,and a plausible mechanism for the photocatalytic reaction was proposed.

关键词： catalytic selectivity Carbon dioxide reduction Carbon monoxide Diiron complex Hydrogenase model Photocatalysis

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Customizing the microenvironment of CO_(2) electrocatalysis via three‐phase interface engineering

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SmartMat 2022年第1期3卷 111-129页

作者： Xianlong Zhou Hao Liu Bao Yu Xia Kostya(Ken)Ostrikov Yao Zheng Shi‐Zhang Qiao School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaideSouth AustraliaAustralia Key Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service FailureWuhanChina National Laboratory for Optoelectronics School of Chemistry and Chemical EngineeringHuazhong University of Science and Technology(HUST)China School of Chemistry and Physics and Centre for Materials Science Queensland University of Technology(QUT)BrisbaneAustralia

Converting CO_(2) into high‐value fuels and chemicals by renewable‐electricitypowered electrochemical CO_(2) reduction reaction(CRR)is a viable approach toward carbon‐emissions‐neutral *** the thermocatalytic hydrogenation of CO_(2) at the solid‐gas interface,the CRR takes place at the three‐phase gas/solid/liquid interface near the electrode surface in aqueous solution,which leads to major challenges including the limited mass diffusion of CO_(2) reactant,competitive hydrogen evolution reaction,and poor product *** we critically examine the various methods of surface and interface engineering of the electrocatalysts to optimize the microenvironment for CRR,which can address the above *** effective modification strategies for the gas transport,electrolyte composition,controlling intermediate states,and catalyst engineering are *** key emphasis is made on the diverse atomic‐precision modifications to increase the local CO_(2) concentration,lower the energy barriers for CO_(2) activation,decrease the H2O coverage,and stabilize intermediates to effectively control the catalytic activity and *** perspectives on the challenges and outlook for the future applications of three‐phase interface engineering for CRR and other gasinvolving electrocatalytic reactions conclude the article.

关键词： catalytic selectivity electrochemical CO_(2)reduction intermediates microenvironment three‐phase interface

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Improve catalytic activity by Tuning Surface Strain of Fe Nanoparticles

Improve Catalytic activity by Tuning Surface Strain of Fe Na...

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第十三届全国量子化学会议

作者： Yin Junqing Wen Xiaodong State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of Sciences University of Chinese A cademy of Sciences Synfuels China Co.Ltd

DFT calculations about CO dissociation and CH formation on the iron surface indicate that higher CO conversion and lower CH production would be obtained on the sites like those on Fe（211） and Fe（310）. Thus, trying to expand the surface area of Fe（211） and Fe（310） may be helpful to suppress CH selectivity. MD simulations on the Fe Wulff structures[ 1 ] reveal that higher temperature would induce the corner and bridge atoms to escape the bulk constraint, producing more under-coordinated atoms（UCAs）. Strain calculations [ 2 ] on the iron surfaces indicate that the UCAs are readily reconstructed and thus create bigger strain. The temperature-strain mechanism can be useful to improve catalytic activity by tuning surface strain of Fe Nanoparticles.

关键词： DFT MD surface strain catalytic selectivity

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