Spectroscopic visualization of reversible hydrogen spillover between palladium and metal–organic frameworks toward catalytic semihydrogenation
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 meta...
| Main Authors: | , , , , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2024-03-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-46923-3 |
| _version_ | 1797247142982582272 |
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| author | 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 |
| author_facet | 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 |
| author_sort | Qiaoxi Liu |
| collection | DOAJ |
| description | 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. |
| first_indexed | 2024-04-24T19:54:00Z |
| format | Article |
| id | doaj.art-8ca0fe18c2ee40528360a3bbd844ff0e |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-04-24T19:54:00Z |
| publishDate | 2024-03-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-8ca0fe18c2ee40528360a3bbd844ff0e2024-03-24T12:27:24ZengNature PortfolioNature Communications2041-17232024-03-011511910.1038/s41467-024-46923-3Spectroscopic visualization of reversible hydrogen spillover between palladium and metal–organic frameworks toward catalytic semihydrogenationQiaoxi Liu0Wenjie Xu1Hao Huang2Hongwei Shou3Jingxiang Low4Yitao Dai5Wanbing Gong6Youyou Li7Delong Duan8Wenqing Zhang9Yawen Jiang10Guikai Zhang11Dengfeng Cao12Kecheng Wei13Ran Long14Shuangming Chen15Li Song16Yujie Xiong17Hefei 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 ChinaHefei 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 ChinaHefei 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 ChinaHefei 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 ChinaHefei 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 ChinaHefei 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 ChinaHefei 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 ChinaHefei 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 ChinaHefei 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 ChinaHefei 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 ChinaHefei 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 ChinaBeijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of SciencesHefei 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 ChinaHefei 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 ChinaHefei 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 ChinaHefei 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 ChinaHefei 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 ChinaHefei 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 ChinaAbstract 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.https://doi.org/10.1038/s41467-024-46923-3 |
| spellingShingle | 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 Spectroscopic visualization of reversible hydrogen spillover between palladium and metal–organic frameworks toward catalytic semihydrogenation Nature Communications |
| title | Spectroscopic visualization of reversible hydrogen spillover between palladium and metal–organic frameworks toward catalytic semihydrogenation |
| title_full | Spectroscopic visualization of reversible hydrogen spillover between palladium and metal–organic frameworks toward catalytic semihydrogenation |
| title_fullStr | Spectroscopic visualization of reversible hydrogen spillover between palladium and metal–organic frameworks toward catalytic semihydrogenation |
| title_full_unstemmed | Spectroscopic visualization of reversible hydrogen spillover between palladium and metal–organic frameworks toward catalytic semihydrogenation |
| title_short | Spectroscopic visualization of reversible hydrogen spillover between palladium and metal–organic frameworks toward catalytic semihydrogenation |
| title_sort | spectroscopic visualization of reversible hydrogen spillover between palladium and metal organic frameworks toward catalytic semihydrogenation |
| url | https://doi.org/10.1038/s41467-024-46923-3 |
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