TY - JOUR
T1 - Sintering Activated Atomic Palladium Catalysts with High-Temperature Tolerance of ∼1,000°C
AU - Yang, Nating
AU - Zhao, Yonghui
AU - Zhang, Hao
AU - Xiang, Weikai
AU - Sun, Yuhan
AU - Yang, Shuai
AU - Sun, Yu
AU - Zeng, Gaofeng
AU - Kato, Kenichi
AU - Li, Xiaopeng
AU - Yamauchi, Miho
AU - Jiang, Zheng
AU - Li, Tong
N1 - Funding Information:
XAS studies were carried out at the BL14W1 beamline in the Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, China (16ssrf00787). The synchrotron radiation XRD experiments were performed at BL44B2 in SPring-8 with the approval of RIKEN. The authors would like to acknowledge the financial support from the China Ministry of Science and Technology ( 2016YFA0202802 ) and Youth Innovation Promotion Association CAS . N.Y. acknowledges financial support from the National Natural Science Foundation of China ( 22002182 ). X.L. acknowledges financial support from the National Natural Science Foundation of China ( 21972163 ), the Fundamental Research Funds for the Central Universities , DHU Distinguished Young Professor Program , and the development fund for Shanghai talents. W.X. and T.L. would like to thank Deutsche Forschungsgemeinsschaft (DFG) for financial support ( 407513992 ) and Zentrumfür Grenzflächendominierte Höchstleistungswerkstoffe (ZGH) at Ruhr University Bochum for the access to infrastructure (FEI Helios G4 CX FIB/SEM and Cameca LEAP 5000 XR).
Funding Information:
XAS studies were carried out at the BL14W1 beamline in the Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, China (16ssrf00787). The synchrotron radiation XRD experiments were performed at BL44B2 in SPring-8 with the approval of RIKEN. The authors would like to acknowledge the financial support from the China Ministry of Science and Technology (2016YFA0202802) and Youth Innovation Promotion Association CAS. N.Y. acknowledges financial support from the National Natural Science Foundation of China (22002182). X.L. acknowledges financial support from the National Natural Science Foundation of China (21972163), the Fundamental Research Funds for the Central Universities, DHU Distinguished Young Professor Program, and the development fund for Shanghai talents. W.X. and T.L. would like to thank Deutsche Forschungsgemeinsschaft (DFG) for financial support (407513992) and Zentrumf?r Grenzfl?chendominierte H?chstleistungswerkstoffe (ZGH) at Ruhr University Bochum for the access to infrastructure (FEI Helios G4 CX FIB/SEM and Cameca LEAP 5000 XR). N.Y. Y.Z. and H.Z. contributed equally to the work. N.Y. X.L. G.Z. and Y.S. conceived the idea and designed experiments. N.Y. performed the catalysts preparation, catalysis, and general characterization experiments. Y.Z. performed the DFT calculations. H.Z. S.Y. and Z.J. performed the XAS experiments and analysis. S.Y. K.K. and M.Y. performed the synchrotron radiation XRD and Rietveld refinement. W.X. and T.L. performed the APT experiments and analysis. N.Y. Y.Z. H.Z. X.L. and Y.S. wrote the manuscript. All the authors contributed to the data interpretation, discussion, and manuscript revision. Y.S. directed the research. The authors declare no competing interests.
Publisher Copyright:
© 2020 The Author(s)
PY - 2021/1/20
Y1 - 2021/1/20
N2 - Sintering-induced aggregation of active metals is a major cause of catalyst deactivation. Catalysts that can operate above 800°C are rare. Here, we report an unusual noble metal catalyst with sintering-induced activation at temperatures up to 1,000°C. The catalyst consists of atomically dispersed palladium embedded in a reducible SnO2 support designated for lean methane combustion. High temperature reaction simultaneously causes favorable changes of palladium ensemble state combining synergistically with lattice oxygen activation. Such changes lead to at least one order of magnitude improvement of the intrinsic reactivity, which compensates the surface area loss. Extensive characterizations such as atom probe tomography, X-ray absorption spectroscopy, and isotope tracking together with theoretical calculations illustrate the structure and surface chemistry changes and their impacts on the reaction mechanism. The catalyst also shows notable long-term stability and facile regeneration after poisoning. Our work may provide new insights into designing active and thermally stable catalysts.
AB - Sintering-induced aggregation of active metals is a major cause of catalyst deactivation. Catalysts that can operate above 800°C are rare. Here, we report an unusual noble metal catalyst with sintering-induced activation at temperatures up to 1,000°C. The catalyst consists of atomically dispersed palladium embedded in a reducible SnO2 support designated for lean methane combustion. High temperature reaction simultaneously causes favorable changes of palladium ensemble state combining synergistically with lattice oxygen activation. Such changes lead to at least one order of magnitude improvement of the intrinsic reactivity, which compensates the surface area loss. Extensive characterizations such as atom probe tomography, X-ray absorption spectroscopy, and isotope tracking together with theoretical calculations illustrate the structure and surface chemistry changes and their impacts on the reaction mechanism. The catalyst also shows notable long-term stability and facile regeneration after poisoning. Our work may provide new insights into designing active and thermally stable catalysts.
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U2 - 10.1016/j.xcrp.2020.100287
DO - 10.1016/j.xcrp.2020.100287
M3 - Article
AN - SCOPUS:85100427600
SN - 2666-3864
VL - 2
JO - Cell Reports Physical Science
JF - Cell Reports Physical Science
IS - 1
M1 - 100287
ER -