Ambient hydrogenation of solid aromatics enabled by a high entropy alloy nanocatalyst

Zekun Jing, Yakun Guo, Qi Wang, Xinrong Yan, Guozong Yue, Zhendong Li, Hanwen Liu, Ruixuan Qin, Changyin Zhong, Mingzhen Li, Dingguo Xu (), Yunxi Yao (), Yonggang Yao () and Maobing Shuai ()
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Zekun Jing: Science and Technology on Surface Physics and Chemistry Laboratory
Yakun Guo: Science and Technology on Surface Physics and Chemistry Laboratory
Qi Wang: Science and Technology on Surface Physics and Chemistry Laboratory
Xinrong Yan: Sichuan University
Guozong Yue: China Academy of Engineering Physics
Zhendong Li: Science and Technology on Surface Physics and Chemistry Laboratory
Hanwen Liu: Huazhong University of Science and Technology
Ruixuan Qin: Xiamen University
Changyin Zhong: China Academy of Engineering Physics
Mingzhen Li: Science and Technology on Surface Physics and Chemistry Laboratory
Dingguo Xu: Sichuan University
Yunxi Yao: China Academy of Engineering Physics
Yonggang Yao: Huazhong University of Science and Technology
Maobing Shuai: China Academy of Engineering Physics

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract Hydrogenation is a versatile chemical process with significant applications in various industries, including food production, petrochemical refining, pharmaceuticals, and hydrogen carriers/safety. Traditional hydrogenation of aromatics, hindered by the stable π-conjugated phenyl ring structures, typically requires high temperatures and pressures, making ambient hydrogenation a grand challenge. Herein, we introduce a PdPtRuCuNi high entropy alloy (HEA) nanocatalyst, achieving an exceptional 100% hydrogenation of carbon-carbon unsaturated bonds, including alkynyl and phenyl groups, in solid 1,4-bis(phenylethynyl)benzene (DEB) at 25 °C under ≤1 bar H2 and solventless condition. This results in a threefold higher hydrogen uptake for DEB-contained composites compared to conventional Pd catalysts, which can only hydrogenate the alkynyl groups with a ~ 27% conversion of DEB. Our experimental results, complemented by theoretical calculations, reveal that PdPtRu alloy is highly active and crucial in enabling the hydrogenation of phenyl groups, while all five elements work synergistically to regulate the reaction rate. Remarkably, this newly developed catalyst also achieves nearly 100% reactivity for ambient hydrogenation of a broad range of aromatics, suggesting its universal effectiveness. Our research uncovers a novel material platform and catalyst design principle for efficient and general hydrogenation. The multi-element synergy in HEA also promises unique catalytic behaviors beyond hydrogenation applications.

Date: 2024
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DOI: 10.1038/s41467-024-50009-5

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