Nanostructuring unlocks high performance of platinum single-atom catalysts for stable vinyl chloride production.,Nature Catalysis

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Nanostructuring unlocks high performance of platinum single-atom catalysts for stable vinyl chloride production.
Nature Catalysis ( IF 42.8 ) Pub Date : 2020-03-02 , DOI: 10.1038/s41929-020-0431-3
Selina K Kaiser ₁ , Edvin Fako ₂ , Gabriele Manzocchi ₁ , Frank Krumeich ₁ , Roland Hauert ₃ , Adam H Clark ₄ , Olga V Safonova ₄ , Núria López ₂ , Javier Pérez-Ramírez ₁

Affiliation

A worldwide replacement of the toxic mercuric chloride catalyst in vinyl chloride manufacture via acetylene hydrochlorination is slowed down 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 1073 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 characterisation, 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. Remarkably, 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 as candidate for sustainable vinyl chloride production.

中文翻译：

纳米结构释放了铂单原子催化剂的高性能，用于稳定氯乙烯生产。

由于替代催化系统在高空速下的耐用性有限，因此通过乙炔氢氯化作用在氯乙烯制造中替代有毒氯化汞催化剂的全球范围被减缓。在这里，我们证明了碳载体上的铂单原子比它们的金对应物（高达 473 K）要稳定得多（高达 1073 K），通过简单的温度控制能够轻松和可扩展地制备和精确调整其配位环境。通过结合动力学分析、高级表征和密度泛函理论，我们评估了 Pt 物种如何决定催化性能，从而确定 Pt(II)-Cl 作为活性位点，其活性是 Pt 纳米颗粒的三倍。值得注意的是，

更新日期：2020-04-24

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