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串联 InO-Pt/AlO 催化剂用于丙烷脱氢偶联到选择性 H 燃烧。

Tandem InO-Pt/AlO catalyst for coupling of propane dehydrogenation to selective H combustion.

机构信息

Department of Chemistry, Northwestern University, Evanston, IL 60208, USA.

Northwestern University Atomic and Nanoscale Characterization Experimental Center (NUANCE), Northwestern University, Evanston, IL 60208, USA.

出版信息

Science. 2021 Mar 19;371(6535):1257-1260. doi: 10.1126/science.abd4441.

Abstract

Tandem catalysis couples multiple reactions and promises to improve chemical processing, but precise spatiotemporal control over reactive intermediates remains elusive. We used atomic layer deposition to grow InO over Pt/AlO, and this nanostructure kinetically couples the domains through surface hydrogen atom transfer, resulting in propane dehydrogenation (PDH) to propylene by platinum, then selective hydrogen combustion by InO, without excessive hydrocarbon combustion. Other nanostructures, including platinum on InO or platinum mixed with InO, favor propane combustion because they cannot organize the reactions sequentially. The net effect is rapid and stable oxidative dehydrogenation of propane at high per-pass yields exceeding the PDH equilibrium. Tandem catalysis using this nanoscale overcoating geometry is validated as an opportunity for highly selective catalytic performance in a grand challenge reaction.

摘要

串联催化耦联多个反应,并有望改进化学加工,但对反应中间体的精确时空控制仍然难以实现。我们使用原子层沉积在 Pt/AlO 上生长 InO,这种纳米结构通过表面氢原子转移在动力学上使畴耦合,导致丙烷通过铂脱氢(PDH)生成丙烯,然后通过 InO 选择性燃烧氢气,而不会过度燃烧碳氢化合物。其他纳米结构,包括 InO 上的铂或与 InO 混合的铂,由于不能按顺序组织反应,因此有利于丙烷燃烧。净效应是在高单程收率下快速稳定地氧化脱氢丙烷,超过 PDH 平衡。使用这种纳米级覆盖层几何形状的串联催化被验证为在重大挑战反应中实现高选择性催化性能的机会。

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