Asymmetric Ru-In atomic pairs promote highly active and stable acetylene hydrochlorination

Yurui Fan, Haomiao Xu (), Guanqun Gao, Mingming Wang, Wenjun Huang, Lei Ma, Yancai Yao (), Zan Qu (), Pengfei Xie (), Bin Dai and Naiqiang Yan
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Yurui Fan: Shanghai Jiao Tong University
Haomiao Xu: Shanghai Jiao Tong University
Guanqun Gao: Shanghai Jiao Tong University
Mingming Wang: Shanghai Jiao Tong University
Wenjun Huang: Shanghai Jiao Tong University
Lei Ma: Shanghai Jiao Tong University
Yancai Yao: Shanghai Jiao Tong University
Zan Qu: Shanghai Jiao Tong University
Pengfei Xie: Zhejiang University
Bin Dai: Shihezi University
Naiqiang Yan: Shanghai Jiao Tong University

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

Abstract: Abstract Ru single-atom catalysts have great potential to replace toxic mercuric chloride in acetylene hydrochlorination. However, long-term catalytic stability remains a grand challenge due to the aggregation of Ru atoms caused by over-chlorination. Herein, we synthesize an asymmetric Ru-In atomic pair with vinyl chloride monomer yield (>99.5%) and stability (>600 h) at a gas hourly space velocity of 180 h−1, far surpassing those of the Ru single-atom counterparts. A combination of experimental and theoretical techniques reveals that there is a strong d-p orbital interaction between Ru and In atoms, which not only enables the selective adsorption of acetylene and hydrogen chloride at different atomic sites but also optimizes the electron configuration of Ru. As a result, the intrinsic energy barrier for vinyl chloride generation is lowered, and the thermodynamics of the chlorination process at the Ru site is switched from exothermal to endothermal due to the change of orbital couplings. This work provides a strategy to prevent the deactivation and depletion of active Ru centers during acetylene hydrochlorination.

Date: 2024
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DOI: 10.1038/s41467-024-50221-3

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