Spectroscopic visualization of reversible hydrogen spillover between palladium and metal–organic frameworks toward catalytic semihydrogenation

Qiaoxi Liu; Wenjie Xu; Hao Huang; Hongwei Shou; Jingxiang Low; Yitao Dai; Wanbing Gong; Youyou Li; Delong Duan; Wenqing Zhang; Yawen Jiang; Guikai Zhang; Dengfeng Cao; Kecheng Wei; Ran Long; Shuangming Chen; Li Song; Yujie Xiong

doi:10.1038/s41467-024-46923-3

Nature Communications (Mar 2024)

Spectroscopic visualization of reversible hydrogen spillover between palladium and metal–organic frameworks toward catalytic semihydrogenation

Qiaoxi Liu,
Wenjie Xu,
Hao Huang,
Hongwei Shou,
Jingxiang Low,
Yitao Dai,
Wanbing Gong,
Youyou Li,
Delong Duan,
Wenqing Zhang,
Yawen Jiang,
Guikai Zhang,
Dengfeng Cao,
Kecheng Wei,
Ran Long,
Shuangming Chen,
Li Song,
Yujie Xiong

Affiliations

Qiaoxi Liu: Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, School of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, University of Science and Technology of China
Wenjie Xu: Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, School of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, University of Science and Technology of China
Hao Huang: Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, School of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, University of Science and Technology of China
Hongwei Shou: Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, School of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, University of Science and Technology of China
Jingxiang Low: Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, School of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, University of Science and Technology of China
Yitao Dai: Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, School of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, University of Science and Technology of China
Wanbing Gong: Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, School of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, University of Science and Technology of China
Youyou Li: Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, School of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, University of Science and Technology of China
Delong Duan: Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, School of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, University of Science and Technology of China
Wenqing Zhang: Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, School of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, University of Science and Technology of China
Yawen Jiang: Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, School of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, University of Science and Technology of China
Guikai Zhang: Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences
Dengfeng Cao: Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, School of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, University of Science and Technology of China
Kecheng Wei: Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, School of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, University of Science and Technology of China
Ran Long: Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, School of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, University of Science and Technology of China
Shuangming Chen: Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, School of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, University of Science and Technology of China
Li Song: Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, School of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, University of Science and Technology of China
Yujie Xiong: Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, School of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, University of Science and Technology of China

DOI: https://doi.org/10.1038/s41467-024-46923-3
Journal volume & issue: Vol. 15, no. 1
pp. 1 – 9

Abstract

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Abstract Hydrogen spillover widely occurs in a variety of hydrogen-involved chemical and physical processes. Recently, metal–organic frameworks have been extensively explored for their integration with noble metals toward various hydrogen-related applications, however, the hydrogen spillover in metal/MOF composite structures remains largely elusive given the challenges of collecting direct evidence due to system complexity. Here we show an elaborate strategy of modular signal amplification to decouple the behavior of hydrogen spillover in each functional regime, enabling spectroscopic visualization for interfacial dynamic processes. Remarkably, we successfully depict a full picture for dynamic replenishment of surface hydrogen atoms under interfacial hydrogen spillover by quick-scanning extended X-ray absorption fine structure, in situ surface-enhanced Raman spectroscopy and ab initio molecular dynamics calculation. With interfacial hydrogen spillover, Pd/ZIF-8 catalyst shows unique alkyne semihydrogenation activity and selectivity for alkynes molecules. The methodology demonstrated in this study also provides a basis for further exploration of interfacial species migration.

Published in Nature Communications

ISSN: 2041-1723 (Online)
Publisher: Nature Portfolio
Country of publisher: United Kingdom
LCC subjects: Science
Website: https://www.nature.com/ncomms/

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