期刊
NATURE CATALYSIS
卷 3, 期 4, 页码 376-385出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41929-020-0431-3
关键词
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资金
- ETH research grant [ETH-40 17-1]
- Swiss National Science Foundation [200021-169679]
- MINECO La Caixa Severo Ochoa [SEV 2013 0319]
- Micromeritics Grant Program
- Swiss National Science Foundation (SNF) [200021_169679] Funding Source: Swiss National Science Foundation (SNF)
The worldwide replacement of the toxic mercuric chloride catalyst in vinyl chloride manufacture via acetylene hydrochlorination is slowed by the limited durability of alternative catalytic systems at high space velocities. Here, we demonstrate that platinum single atoms on carbon carriers are substantially more stable (up to 1,073 K) than their gold counterparts (up to 473 K), enabling facile and scalable preparation and precise tuning of their coordination environment by simple temperature control. By combining kinetic analysis, advanced characterization, and density functional theory, we assess how the Pt species determines the catalytic performance and thereby identify Pt(ii)-Cl as the active site, being three times more active than Pt nanoparticles. We show that Pt single atoms exhibit outstanding stability in acetylene hydrochlorination and surpass the space-time yields of their gold-based analogues after 25 h time-on-stream, qualifying them as a candidate for sustainable vinyl chloride production. Platinum nanoparticles have been neglected as a catalyst for acetylene hydrochlorination due to their limited activity. Here, the authors show that nanostructuring to the single-atom level renders platinum on carbonaceous supports a superior catalyst for this important industrial process.
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