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 and
Yujie Xiong ()
Additional contact information
Qiaoxi Liu: University of Science and Technology of China
Wenjie Xu: University of Science and Technology of China
Hao Huang: University of Science and Technology of China
Hongwei Shou: University of Science and Technology of China
Jingxiang Low: University of Science and Technology of China
Yitao Dai: University of Science and Technology of China
Wanbing Gong: University of Science and Technology of China
Youyou Li: University of Science and Technology of China
Delong Duan: University of Science and Technology of China
Wenqing Zhang: University of Science and Technology of China
Yawen Jiang: University of Science and Technology of China
Guikai Zhang: Chinese Academy of Sciences
Dengfeng Cao: University of Science and Technology of China
Kecheng Wei: University of Science and Technology of China
Ran Long: University of Science and Technology of China
Shuangming Chen: University of Science and Technology of China
Li Song: University of Science and Technology of China
Yujie Xiong: University of Science and Technology of China
Nature Communications, 2024, vol. 15, issue 1, 1-9
Abstract:
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.
Date: 2024
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DOI: 10.1038/s41467-024-46923-3
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