Discovering Partially Charged Single-Atom Pt for Enhanced Anti-Markovnikov Alkene Hydrosilylation,Journal of the American Chemical Society

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Discovering Partially Charged Single-Atom Pt for Enhanced Anti-Markovnikov Alkene Hydrosilylation
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2018-06-04 , DOI: 10.1021/jacs.8b03121
Yuanjun Chen ₁ , Shufang Ji ₁ , Wenming Sun ₂ , Wenxing Chen ₁ , Juncai Dong ₃ , Junfeng Wen ₁ , Jian Zhang ₁ , Zhi Li ₁ , Lirong Zheng ₃ , Chen Chen ₁ , Qing Peng ₁ , Dingsheng Wang ₁ , Yadong Li ₁

Affiliation

The hydrosilylation reaction is one of the largest-scale application of homogeneous catalysis and is widely used to enable the commercial manufacture of silicon products. However, considerable issues including disposable platinum consumption, undesired side reactions and unacceptable catalyst residues still remain. Here, we synthesize a heterogeneous partially charged single-atom platinum supported on anatase TiO2 (Pt1δ+/TiO2) catalyst via an electrostatic-induction ion exchange and two-dimensional confinement strategy, which can catalyze hydrosilylation reaction with almost complete conversion and produce exclusive adduct. Density functional theory calculations reveal that unexpected property of Pt1δ+/TiO2 originates from atomic dispersion of active species and unique partially positive charge Ptδ+ electronic structure that conventional nanocatalysts do not possess. The fabrication of single-atom Pt1δ+/TiO2 catalyst accomplishes a reasonable use of Pt through recycling and maximum atom-utilized efficiency, indicating the potential to achieve a green hydrosilylation industry.

中文翻译：

发现部分带电单原子 Pt 以增强抗马尔科夫尼科夫烯烃氢化硅烷化

氢化硅烷化反应是均相催化最大规模的应用之一，广泛用于实现硅产品的商业化生产。然而，包括一次性铂消耗、不希望的副反应和不可接受的催化剂残留物在内的相当大的问题仍然存在。在这里，我们通过静电感应离子交换和二维限制策略合成了负载在锐钛矿型 TiO2 (Pt1δ+/TiO2) 催化剂上的多相部分带电单原子铂，该催化剂可以催化几乎完全转化的氢化硅烷化反应并产生专属加合物. 密度泛函理论计算表明，Pt1δ+/TiO2 的意外性质源于活性物质的原子分散和传统纳米催化剂不具备的独特的部分正电荷 Ptδ+ 电子结构。单原子 Pt1δ+/TiO2 催化剂的制备通过回收和最大原子利用效率实现了 Pt 的合理利用，表明实现绿色氢化硅烷化工业的潜力。

更新日期：2018-06-04

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