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Edge-Rich Pt-O-Ce Sites in CeO2 Supported Patchy Atomic-Layer Pt Enable a Non-CO Pathway for Efficient Methanol Oxidation.
Xu, Airong; Liu, Tong; Liu, Dong; Li, Wenzhi; Huang, Hui; Wang, Sicong; Xu, Li; Liu, Xiaokang; Jiang, Shuaiwei; Chen, Yudan; Sun, Mei; Luo, Qiquan; Ding, Tao; Yao, Tao.
Affiliation
  • Xu A; School of Nuclear Science and Technology, Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, P.R. China.
  • Liu T; School of Nuclear Science and Technology, Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, P.R. China.
  • Liu D; School of Nuclear Science and Technology, Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, P.R. China.
  • Li W; School of Nuclear Science and Technology, Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, P.R. China.
  • Huang H; School of Nuclear Science and Technology, Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, P.R. China.
  • Wang S; School of Nuclear Science and Technology, Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, P.R. China.
  • Xu L; School of Nuclear Science and Technology, Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, P.R. China.
  • Liu X; School of Nuclear Science and Technology, Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, P.R. China.
  • Jiang S; School of Nuclear Science and Technology, Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, P.R. China.
  • Chen Y; School of Nuclear Science and Technology, Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, P.R. China.
  • Sun M; School of Nuclear Science and Technology, Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, P.R. China.
  • Luo Q; Institutes of Physical Science and Information Technology, Anhui University, Hefei, 230601, P.R. China.
  • Ding T; School of Nuclear Science and Technology, Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, P.R. China.
  • Yao T; School of Nuclear Science and Technology, Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, P.R. China.
Angew Chem Int Ed Engl ; 63(40): e202410545, 2024 Oct 01.
Article in En | MEDLINE | ID: mdl-38940407
ABSTRACT
Rational design of efficient methanol oxidation reaction (MOR) catalyst that undergo non-CO pathway is essential to resolve the long-standing poisoning issue. However, it remains a huge challenge due to the rather difficulty in maximizing the non-CO pathway by the selective coupling between the key *CHO and *OH intermediates. Here, we report a high-performance electrocatalyst of patchy atomic-layer Pt epitaxial growth on CeO2 nanocube (Pt ALs/CeO2) with maximum electronic metal-support interaction for enhancing the coupling selectively. The small-size monolayer material achieves an optimal geometrical distance between edge Pt-O-Ce sites and *OH absorbed on CeO2, which well restrains the dehydrogenation of *CHO, resulting in the non-CO pathway. Meanwhile, the *CHO/*CO intermediate generated at inner Pt-O-Ce sites can migrate to edge, inducing the subsequent coupling reaction, thus avoiding poisoning while promoting reaction efficiency. Consequently, Pt ALs/CeO2 exhibits exceptionally catalytic stability with negligible degradation even under 1000 s pure CO poisoning operation and high mass activity (14.87 A/mgPt), enabling it one of the best-performing alkali-stable MOR catalysts.
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Full text: 1 Collection: 01-internacional Database: MEDLINE Language: En Journal: Angew Chem Int Ed Engl Year: 2024 Document type: Article Country of publication:
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Full text: 1 Collection: 01-internacional Database: MEDLINE Language: En Journal: Angew Chem Int Ed Engl Year: 2024 Document type: Article Country of publication: