Bimetallic Pt-Sn nanocluster from the hydrogenolysis of a well-defined surface compound consisting of [( AlO-)Pt(COD)Me] and [( AlO-)SnPh3] fragments for propane dehydrogenation

Bimetallic Pt-Sn nanocluster from the hydrogenolysis of a well-defined surface compound consisting of [( AlO-)Pt(COD)Me] and [( AlO-)SnPh3] fragments for propane dehydrogenation
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由 [(Al2O-)Pt(COD)Me] 和 [(AlO-)SnPh3] 碎片组成的明确表面化合物氢解产生的双金属 Pt-Sn 纳米簇,用于丙烷脱氢

DOI:
10.1016/j.jcat.2019.04.035
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发表时间:
2019
影响因子:
7.3
通讯作者:
Zhu Haibo
Zhu Haibo
中科院分区:
化学1区
文献类型:
--
作者:
Xu Zhikang;Xu Rui;Yue Yuanyuan;Yuan Pei;Bao Xiaojun;Abou Hamad Edy;Basset Jean Marie;Zhu Haibo

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双金属铂锡催化剂被认为是丙烷脱氢反应中最有效的催化剂,然而,合成具有合金结构的双金属铂锡纳米簇合物(小于1 nm)仍然是一个巨大的挑战。提出了一种基于氧化物概念的表面金属有机化学可控合成铂锡纳米簇合物的方法,它包括两个基本步骤:在脱羟基的θ-Al_2O表面依次接枝铂(COD)Me2和HSnPh_3,形成由[(三键铝单键)铂(COD)Me]和[(三键铝单键)SnPh_3]片段组成的有序的双金属表面化合物,该表面化合物在温和的条件下氢解生成约0.75 nm的超小双金属簇合物。所制得的铂-锡/θ-Al_2O_3催化剂在丙烷脱氢制丙烯反应中具有较高的活性、选择性和稳定性。
The bimetallic Pt-Sn catalysts are known to be the most efficient ones for propane dehydrogenation reaction; however, the synthesis of bimetallic Pt-Sn nanocluster (below 1 nm) with an alloy structure still remains a formidable challenge. An approach for the controllable synthesis of Pt-Sn nanocluster based on Surface Organometallic Chemistry on oxide concept is developed here, which involves two basic steps: the sequential grafting of Pt(COD)Me2and HSnPh3at the surface of dehydroxylated θ-Al2O leading to the formation of well-defined bimetallic surface compound consisting of [(triple bondAlOsingle bond)Pt(COD)Me] and [(triple bondAlOsingle bond)SnPh3] fragments, and the hydrogenolysis of this surface compound under a mild condition giving rise to the ultra-small bimetallic Pt-Sn cluster around 0.75 nm. The achieved Pt-Sn/θ-Al2O3catalysts exhibit high activity, selectivity and stability in propane dehydrogenation to propylene.