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Construction of pH-Triggered DNA Hydrogels Based on Hybridization Chain Reactions

chemical Research in Chinese Universities 2020年第2期36卷 243-246页

作者： LI Yujie CHEN Jie DONG Yuanchen LIU Huajie LIU Dongsheng Key Laboratory of Organic Optoelectronics&Molecular Engineering Ministry of EducationDepartment of ChemistryTsinghua UniversityBeijing 100084P.R.China School of Chemical Science and Engineering Shanghai Research Institute for Intelligent Autonomous SystemsKey Laboratory of Advanced Civil Engineering MaterialsMinistry of EducationTongji UniversityShanghai 200092P.R.China Division of Physical Biology CAS Key Laboratory of Interfacial Physics and TechnologyShanghai Institute of Applied PhysicsChinese Academy of SciencesShanghai 201800P.R.China CAS Key Laboratory of Colloid Interface and Chemical ThermodynamicsInstitute of ChemistryChinese Academy of SciencesBeijing 100190P.R.China

As a novel type of bio-functional material,DNA hydrogels have attracted more and more attention due to their successful applications in 3D cell culturing and tissue engineering for the designable and programmable ***,we have developed a pH-triggered DNA hydrogel based on a clamped hybridization chain reaction(C-HCR).In this system,a DNA switch was designed,which can release the initiator strand in a controllable way via the formation of the C-G-C4 triplex under the pH *** the pre-gelation solution is stable in neutral environment,the C-HCR will trigger the sol-gel transition as the pH decreased to *** strategy has endowed the DNA hydrogel with good controllability for triggering,which also shows potential in intellectual responsiveness to certain stimuli.

关键词： DNA hydrogel pH-Triggered Hybridization chain reaction Sol-gel phase transition

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Thermal transport in a 2D amorphous material

arXiv

引用

arXiv 2024年

作者： Wang, Yuxi Zhang, Xingxing Yan, Wujuan Liang, Nianjie He, Haiyu Tao, Xinwei Li, Ang Yang, Fuwei Li, Buxuan Liu, Te-Huan Zhu, Jia Zhou, Wu Wang, Wei Zhou, Lin Song, Bai College of Engineering Peking University Beijing100871 China National Key Laboratory of Advanced MicroNanoManufacture Technology Peking University Beijing100871 China Beijing Innovation Center for Engineering Science and Advanced Technology Peking University Beijing100871 China School of Chemistry and Chemical Engineering Frontiers Science Centre for Transformative Molecules Shanghai Jiao Tong University Shanghai200240 China School of Physical Sciences CAS Key Laboratory of Vacuum Physics University of Chinese Academy of Sciences Beijing100049 China Center for Nano and Micro Mechanics Tsinghua University Beijing100084 China Department of Mechanical Engineering Massachusetts Institute of Technology 77 Massachusetts Avenue CambridgeMA02139 United States School of Energy and Power Engineering Huazhong University of Science and Technology Hubei Wuhan430074 China College of Engineering and Applied Sciences Nanjing University Nanjing210093 China School of Integrated Circuits Peking University Beijing100871 China

Two-dimensional (2D) crystals proved revolutionary soon after graphene was discovered in 2004. However, 2D amorphous materials only became accessible in 2020 and remain largely unexplored. In particular, the thermophysical properties of amorphous materials are of great interest upon transition from 3D to 2D. Here, we probe thermal transport in 2D amorphous carbon. A cross-plane thermal conductivity () down to 0.079 Wm-1K-1 is measured for van der Waals stacked multilayers at room temperature, which is among the lowest reported to date. Meanwhile, an unexpectedly high in-plane is obtained for freestanding monolayers which is a few times larger than what is predicted by conventional wisdom for 3D amorphous carbon with similar sp2 fraction. Our molecular dynamics simulations reveal the role of disorder and highlight the impact of dimensionality. Amorphous materials at the 2D limit open up new avenues for understanding and manipulating heat at the atomic scale. Amorphous materials such as glass have captured human imagination for thousands of years and continue to be of immense value for diverse technologies including advanced manufacturing, high-performance electronics, and thermal barrier coatings, in light of their intriguing structures and fascinating properties1,2. In particular, recent years have witnessed substantial progress in terms of fabrication, characterization, and simulation. For example, the atomic structures of glassy solids (e.g., silica and high-entropy alloy) have finally been directly observed3-5 ever since Zachariasen6 proposed the continuous-random-network (CRN) model in 1932. Further, extreme mechanical and dielectric properties have been realized in amorphous carbon and boron nitride, respectively7,8. Moreover, ab initio and machine-learning-assisted calculations have markedly facilitated the mechanistic understandings of amorphous materials9-11. Among all the endeavors, the synthesis of two-dimensional (2D) amorphous carbon in 2020 down to a si

关键词： Amorphous carbon

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Exciton dynamics uncovering electron fractionalization in superconducting cuprates

arXiv

引用

arXiv 2022年

作者： Singh, Amol Huang, H.Y. Xie, J.D. Okamoto, J. Chen, C.T. Watanabe, T. Fujimori, A. Imada, M. Huang, D.J. National Synchrotron Radiation Research Center Hsinchu30076 Taiwan Department of Electrophysics National Yang Ming Chiao Tung University Hsinchu30093 Taiwan Graduate School of Science and Technology Hirosaki University Aomori Hirosaki036-8561 Japan Department of Physics National Tsing Hua University Hsinchu30013 Taiwan Department of Physics University of Tokyo Bunkyo-ku Tokyo113-0033 Japan Waseda Research Institute for Science and Engineering Waseda University Shinjuku Tokyo169-8555 Japan Toyota Physical and Chemical Research Institute Aichi Nagakute480-1192 Japan

Electron quasiparticles play a crucial role in simplifying the description of many-body physics in solids with surprising success. Conventional Landau's Fermi-liquid and quasiparticle theories for high-temperature superconducting cuprates have, however, received skepticism from various angles. A path-breaking framework of electron fractionalization has been established to replace the Fermi-liquid theory for systems that show the fractional quantum Hall effect and the Mott insulating phenomena;whether it captures the essential physics of the pseudogap and superconducting phases of cuprates is still an open issue. Here, we show that excitonic excitation of optimally doped Bi2Sr2CaCu2O8+δ with energy far above the superconducting-gap energy scale, about 1 eV or even higher, is unusually enhanced by the onset of superconductivity. Our finding proves the involvement of such high-energy excitons in superconductivity. Therefore, the observed enhancement in the spectral weight of excitons imposes a crucial constraint on theories for the pseudogap and superconducting mechanisms. A simple two-component fermion model which embodies electron fractionalization in the pseudogap state well explains the change, pointing toward a novel route for understanding the electronic structure of superconducting cuprates. © 2022, CC BY.

关键词： Electrons

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Construction status and prospects of the Hyper-Kamiokande project

Construction status and prospects of the Hyper-Kamiokande pr...

引用

37th International Cosmic Ray Conference, ICRC 2021

作者： Itow, Yoshitaka Abe, K. Adrich, P. Aihara, H. Akutsu, R. Alekseev, I. Ali, A. Alj Hakim, Y.I. Ameli, F. Anthony, L.H.V. Araya, A. Asaoka, Y. Aushev, V. Ballester, F. Bandac, I. Barbi, M. Barr, G. Batkiewicz-Kwasniak, M. Bellato, M. Berardi, V. Bernard, L. Bernardini, E. Berns, L. Bhadra, S. Bian, J. Blanchet, A. Blondel, A. Boiano, A. Bolognesi, S. Bonavera, L. Booth, N. Bordoni, S. Borjabad, S. Boschi, T. Bose, D. Boyd, S.B. Bozza, C. Bravar, A. Bronner, C. Brown, L. Bubak, A. Buchowicz, A. Buizza Avanzini, M. Cafagna, F.S. Calabria, N.F. Calvo-Mozota, J.M. Cao, S. Carroll, A. Catanesi, M.G. Cebriàn, S. Chakraborty, S. Choi, J.H. Choubey, S. Cicerchia, M. Coleman, J. Collazuol, G. Cuen-Rochin, S. Danilov, M. Díaz López, G. De la Fuente, E. de Perio, P. De Rosa, G. Dealtry, T. Densham, C.J. Dergacheva, A. Deshmukh, N. Devi, M.M. Di Lodovico, F. Di Meo, P. Di Palma, I. Doyle, T.A. Drakopoulou, E. Drapier, O. Dumarchez, J. Eklund, L. El Hedri, S. Ellis, J. Emery, S. Esmaili, A. Esteve, R. Fedotov, S. Feng, J. Fernandez, P. Fernández-Martinez, E. Ferrario, P. Ferrazzi, B. Finch, A. Finley, C. Fiorillo, G. Fitton, M. Friend, M. Fujii, Y. Fujisawa, C. Fukuda, Y. Galinski, G. Gao, J. Garde, C. Garfagnini, A. Garode, S. Gialanella, L. Giganti, C. Gomez-Cadenas, J.J. Gonin, M. González-Nuevo, J. Gorin, A. Gornea, R. Gousy-Leblanc, V. Gramegna, F. Grassi, M. Grella, G. Guigue, M. Hadley, D.R. Harada, M. Hartz, M. Hassani, S. Hastings, N.C. Hayato, Y. Hernando-Morata, J.A. Herrero, V. Hiraide, K. Holin, A. Hoshina, K. Hultqvist, K. Iacob, F. Ichikawa, A.K. Idrissi Ibnsalih, W. Ieki, K. Ikeda, M. Ioannisian, A. Ishida, T. Ishidoshiro, K. Ishino, H. Ishitsuka, M. Israel, H.T. Ito, H. Itow, Y. Izumi, N. Izumiyama, S. Jakkapu, M. Jamieson, B. Jang, J.S. Jo, H.S. Jonsson, P. Joo, K.K. Kajita, T. Kakuno, H. Kameda, J. Kaneshima, R. Kano, Y. Karlen, D. Kataoka, Y. Kato, A. Katori, T. Kazarian, N. Khabibullin, M. Institute for Space-Earth Environmental Research Kobayashi-Maskawa Institute for the Origin of Particles and the Universe Nagoya University Aichi Nagoya Japan University of Tokyo Institute for Cosmic Ray Research Kamioka Observatory Kamioka Japan University of Tokyo Institutes for Advanced Study Kashiwa Japan University of Tokyo Next-generation Neutrino Science Organization Kamioka Japan National Centre for Nuclear Research Warsaw Poland University of Tokyo Department of Physics Tokyo Japan TRIUMF VancouverBC Canada P.N.Lebedev Physical Institute of the Russian Academy of Sciences Moscow Russia Kyoto University Department of Physics Kyoto Japan Imperial College London Department of Physics London United Kingdom INFN Sezione di Roma Università Sapienza Dipartimento di Fisica Roma Italy University of Tokyo Earthquake Research Institute Tokyo Japan Kyiv National University Department of Nuclear Physics Kyiv Ukraine Valencia Spain Laboratorio Subterráneo de Canfranc Estación Canfranc Spain University of Regina Department of Physics ReginaSK Canada Oxford University Department of Physics Oxford United Kingdom H. Niewodniczański Institute of Nuclear Physics PAN Cracow Poland INFN Sezione di Padova Università di Padova Dipartimento di Fisica Padova Italy INFN Sezione di Bari Università e Politecnico di Bari Bari Italy Ecole Polytechnique IN2P3-CNRS Laboratoire Leprince-Ringuet Palaiseau France Tokyo Institute of Technology Department of Physics Tokyo Japan York University Department of Physics and Astronomy TorontoON Canada University of California Irvine Department of Physics and Astronomy IrvineCA United States Laboratoire de Physique Nucleaire et de Hautes Energie IN2P3 CNRS Sorbonne Universitè Paris France INFN Sezione di Napoli Napoli Italy IRFU CEA Universitè Paris-Saclay Gif-sur-Yvette France University of Oviedo Applied Mathematical Modeling Group Department of Physics Oviedo Spain University of Victoria Department of

The Hyper-Kamiokande project is a 258-kton Water Cherenkov together with a 1.3-MW high-intensity neutrino beam from the Japan Proton Accelerator Research Complex (J-PARC). The inner detector with 186-kton fiducial volume is viewed by 20-inch photomultiplier tubes (PMTs) and multi-PMT modules, and thereby provides state-of-the-art of Cherenkov ring reconstruction with thresholds in the range of few MeVs. The project is expected to lead to precision neutrino oscillation studies, especially neutrino CP violation, nucleon decay searches, and low energy neutrino astronomy. In 2020, the project was officially approved and construction of the far detector was started at Kamioka. In 2021, the excavation of the access tunnel and initial mass production of the newly developed 20-inch PMTs was also started. In this paper, we present a basic overview of the project and the latest updates on the construction status of the project, which is expected to commence operation in 2027. © Copyright owned by the author(s).

关键词： Photomultipliers

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Friction and wear behaviors of MoS2-multi-walled-carbonnanotube hybrid reinforced polyurethane composite coating

引用

Friction 2019年第4期7卷 316-326页

作者： Zhaozhu ZHANG Mingming YANG Junya YUAN Fang GUO Xuehu MEN State Key Laboratory of Solid Lubrication Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou730000China University of Chinese Academy of Sciences Beijing100039China School of Physical Science and Technology Lanzhou UniversityLanzhou730000China

MoS2-multi-walled-carbon-nanotube(MWCNT)hybrids containing two-dimensional MoS2 and one-dimensional MWCNTs were synthesized through a one-step hydrothermal reaction.X-ray-diffraction and transmission-electron-microscopy results demonstrated that MoS2 nanosheets were successfully synthesized,and uniformly anchored on the MWCNTs’***,the effects of the Mo S2-MWCNT hybrids on the tribological performances of polyurethane composite coatings were investigated using a UMT-2MT *** and wear test results revealed that the friction coefficient and wear rate of a 3 wt%Mo S2-MWCNT-1 filled polyurethane composite coating were reduced by 25.6% and 65.5%,*** outstanding tribological performance of the MoS2-MWCNT-1 reinforced polyurethane composite coating was attributed to the excellent load-carrying capacity of the MWCNTs and good lubricant ability of *** surface morphologies of the worn surfaces and counterpart ball surfaces were investigated to reveal the wear mechanisms.

关键词： adhesion coating friction wear polyurethane

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Kinetic analysis of thermally induced polymorphic transition in HMX using terahertz spectroscopy

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Spectrochimica acta. Part A, Molecular and biomolecular spectroscopy 2025年 343卷 126515页

作者： Quancheng Liu Hang Su Xiaoxia Li Zhengwen Zhang Lingdi Li Qi Zhang School of Information and Control Engineering Southwest University of Science and Technology Mianyang 621010 China Tianfu Institute of Research and Innovation Southwest University of Science and Technology Chengdu 610200 China. Electronic address: Liuqc@***. School of Information and Control Engineering Southwest University of Science and Technology Mianyang 621010 China. Physical and Chemical Testing Center Gansu Yinguang Chemical Group Co. Ltd. Baiyin 730900 China. Institute of Chemical Materials China Academy of Engineering Physics Mianyang 621022 China. Electronic address: jackzhang531@***.

Understanding the kinetics of polymorphic transitions is critical for predicting and controlling phase behavior in functional materials. Although terahertz spectroscopy has been established as a reliable technique for identifying polymorphic forms, its application in analyzing transition kinetics remains underexplored. In this study, terahertz time-domain spectroscopy (THz-TDS) was employed to monitor the thermally induced β-to-δ polymorphic transition in HMX. Principal component analysis enabled segmentation of the spectral evolution, allowing precise identification of intermediate transformation stages. Density functional theory calculations, combined with analysis of thermally activated anharmonic vibrational modes, revealed that nitro-group motion facilitates the transition by lowering activation barriers. A logistic relationship between absorption intensity and transformation time was observed, consistent with a cooperative nucleation-and-growth mechanism governed by thermal input. These results demonstrate the capacity of THz spectroscopy to dynamically monitor polymorphic transition kinetics at the molecular level.

关键词： Density functional theory HMX Kinetics Polymorphic transition Terahertz spectroscopy

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Mechanistic insights of evaporation-induced actuation in supramolecular crystals (Sept, 10.1038/s41563-020-0799-0, 2020)

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NATURE MATERIALS 2021年第3期20卷 434-434页

作者： Piotrowska, Roxana Hesketh, Travis Wang, Haozhen Martin, Alan R. G. Bowering, Deborah Zhang, Chunqiu Hu, Chunhua T. McPhee, Scott A. Wang, Tong Park, Yaewon Singla, Pulkit McGlone, Thomas Florence, Alastair Tuttle, Tell Ulijn, Rein V. Chen, Xi Advanced Science Research Center (ASRC) at the Graduate Center of the City University of New York New York NY USA PhD Program in Chemistry The Graduate Center of the City University of New York New York NY USA Department of Pure and Applied Chemistry University of Strathclyde Glasgow UK PhD Program in Physics The Graduate Center of the City University of New York New York NY USA EPSRC Continuous Manufacturing and Crystallisation Future Research Hub c/o Strathclyde Institute of Pharmacy and Biomedical Sciences Technology Innovation Centre University of Strathclyde Glasgow UK Department of Chemistry New York University New York NY USA Department of Chemistry and Biochemistry Hunter College City University of New York New York NY USA Department of Chemical Engineering The City College of New York New York NY USA

A Correction to this paper has been published: https://***/10.1038/s41563-021-00950-3.

关键词： Condensed-matter physics Materials science Soft materials

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Ternary oxides of s- and p-block metals for photocatalytic solar-to-hydrogen conversion

arXiv

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arXiv 2023年

作者： Gelin, Simon Kirchner-Hall, Nicole E. Katzbaer, Rowan R. Theibault, Monica J. Xiong, Yihuang Zhao, Wayne Khan, Mohammed M. Andrewlavage, Eric Orbe, Paul Baksa, Steven M. Cococcioni, Matteo Timrov, Iurii Campbell, Quinn Abruña, Héctor Schaak, Raymond E. Dabo, Ismaila Department of Materials Science and Engineering Materials Research Institute The Pennsylvania State University University ParkPA16802 United States Science & Technology Corning Incorporated CorningNY United States Department of Chemistry The Pennsylvania State University University ParkPA16802 United States Department of Chemistry and Chemical Biology Cornell University 245 Feeney Way IthacaNY14850 United States Department of Materials Science and Engineering University of California Berkeley BerkeleyCA94720 United States Physical Sciences and Engineering Division King Abdullah University of Science and Technology Thuwal23955-6900 Saudi Arabia Department of Physics University of Pavia via Bassi 6 PaviaI-27100 Italy LausanneCH-1015 Switzerland Center for Computing Research Sandia National Laboratories AlbuquerqueNM United States Department of Chemistry Department of Chemical Engineering Materials Research Institute The Pennsylvania State University University ParkPA16802 United States

Oxides containing metals or metalloids from the p-block of the periodic table (e.g., In, Sn, Sb, Pb, Bi) are of technological interest as transparent conductors and light absorbers for solar energy conversion due to the tunability of their electronic conductivity and optical absorption. Comparatively, these oxides have found limited applications in hydrogen photoelectrolysis primarily due to their high electronegativity, which impedes electron transfer for reducing protons into hydrogen. We have shown recently that inserting s-block cations into p-block metal oxides is effective at lowering electronegativities while affording further control of band gaps. Here, we explain the origins of this dual tunability by demonstrating the mediator role of s-block cations in modulating orbital hybridization while not contributing to frontier electronic states. From this result, we carry out a comprehensive computational study of 109 ternary oxides of s- and p-block metal elements as candidate photocatalysts for solar hydrogen generation. We downselect the most desirable materials using band gaps and band edges obtained from Hubbard-corrected density-functional theory with Hubbard parameters computed entirely from first principles, evaluate the stability of these oxides in aqueous conditions, and characterize experimentally four of the remaining materials, synthesized with high phase uniformity, to validate and further develop the computational models. We thus propose nine oxide semiconductors, including CsIn3O5, Sr2In2O5, and KSbO2 which, to the extent of our literature review, have not been previously considered as water-splitting photocatalysts. Copyright © 2023, The Authors. All rights reserved.

关键词： Electronegativity

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First-principles kinetics study of carbon monoxide promoted Ostwald ripening of Au particles on FeO/Pt(111)

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Journal of Energy Chemistry 2019年第3期28卷 108-113页

作者： Sulei Hu Runhai Ouyang Wei-Xue Li State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Department of Chemical Physics School of Chemistry and Materials ScienceiCHeMCAS Excellence Center for NanoscienceUniversity of Science and Technology of ChinaHefei 230026AnhuiChina Hefei National Laboratory for Physical Sciences at the Microscale Hefei 230026AnhuiChina University of Chinese Academy of Sciences Beijing 100049China

The dynamic and kinetic evolution of supported metal particles in the presence of reactants is decisive in shaping the nature of the catalytic active sites and the deactivation process. Ostwald ripening of FeO/Pt(111) supported Au particles in the presence of carbon monoxide is addressed here by firstprinciples kinetics. It is found that CO stabilizes the ripening monomer(Au atom) by forming favorable Au carbonyls with lower total activation energy, and corresponding phase diagram at wide range of temperature and CO pressures is constructed. Evolution of particle number, dispersion and particle size distribution of supported Au particles are explored. Great influence of CO promotion on ripening kinetics is revealed and explored in details, and mbar range of CO can lower the onset temperature of ripening by a few hundred kelvins. The present work reveals the crucial role of the metal-reactant complexes formed under reaction conditions on ripening of metal catalysts.

关键词： Carbon monoxide Au particles Ostwald ripening First-principles kinetics FeO/Pt(111)

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Zinc Oxide Morphology-Dependent Pd/ZnO Catalysis in Base-Free CO₂ Hydrogenation into Formic Acid

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ChemCatChem 2020年第21期12卷 5540-5547页

作者： Zhang, Jing Fan, Liping Zhao, Feiyue Fu, Yanghe Lu, Ji-Qing Zhang, Zhenhua Teng, Botao Huang, Weixin Key Laboratory of the Ministry of Education for Advanced Catalysis Materials Institute of Physical Chemistry Zhejiang Normal University Zhejiang 321004 Jinhua China Hefei National Laboratory for Physical Sciences at Microscale Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes CAS Key Laboratory of Materials for Energy Conversion Department of Chemical Physics University of Science and Technology of China Hefei 230026 China

Pd/ZnO catalysts with ca. 2 wt.% Pd loading employing ZnO nanocrystals with various morphologies as supports, including ZnO nanoplates (p−ZnO) predominantly exposing polar {002} facets, ZnO nanorods (r−ZnO) predominantly exposing nonpolar {100} and {101} facets, and commercial ZnO (c−ZnO) exposing random facets, have been prepared as catalysts for the catalytic reaction of CO₂ hydrogenation into formic acid (FA) without the addition of base under mild conditions. A remarkable morphology-dependence of zinc oxide in the Pd/ZnO catalysts was observed. Catalytic activities of various Pd/ZnO catalysts in CO₂ hydrogenation into FA follow an order of Pd/r−ZnO>Pd/p−ZnO>Pd/c−ZnO, and all the catalysts are stable. Kinetic study, CO₂-TPD analysis, and in situ DRIFTS spectra provide evidence that all the Pd/ZnO catalysts follow a similar catalytic mechanism that CO₂ activation is the rate-determining step. Consequently, r−ZnO, possessing a higher density of weak basic sites than p−ZnO and c−ZnO, can act as a superb support to prepare Pd/r−ZnO catalyst, which is more active than Pd/p−ZnO and Pd/c−ZnO catalysts for the production of FA. These findings nicely demonstrate the crystal-plane engineering of the metal oxide support in tuning the catalytic performance of Pd-based catalysts for CO₂ hydrogenation into FA. © 2020 Wiley-VCH GmbH

关键词： Basicity of support Catalytic mechanism CO2 hydrogenation into formic acid Pd/ZnO catalysts ZnO nanocrystals

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