当前位置: X-MOL 学术Nat. Chem. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Single-atom gold oxo-clusters prepared in alkaline solutions catalyse the heterogeneous methanol self-coupling reactions.
Nature Chemistry ( IF 19.2 ) Pub Date : 2019-10-21 , DOI: 10.1038/s41557-019-0345-3
Sufeng Cao 1 , Ming Yang 1 , Ahmed O Elnabawy 2 , Antonios Trimpalis 1 , Sha Li 2 , Chongyang Wang 1 , Florian Göltl 2 , Zhihengyu Chen 3 , Jilei Liu 1 , Junjun Shan 1 , Mengwei Li 1 , Terry Haas 1 , Karena W Chapman 3 , Sungsik Lee 4 , Lawrence F Allard 5 , Manos Mavrikakis 2 , Maria Flytzani-Stephanopoulos 1
Affiliation  

In an effort to obtain the maximum atom efficiency, research on heterogeneous single-atom catalysts has intensified recently. Anchoring organometallic homogeneous catalysts to surfaces creates issues with retaining mononuclearity and activity, while the several techniques developed to prepare atomically dispersed precious metals on oxide supports are usually complex. Here we report a facile one-pot synthesis of inorganometallic mononuclear gold complexes formed in alkaline solutions as robust and versatile single-atom gold catalysts. The complexes remain intact on impregnation onto supports or after drying in air to give a crystalline powder. They can be used to interrogate the nuclearity of the catalytically active gold site for reactions known to be catalysed by oxidized gold species. We show that the [Au1–Ox]– cluster directs the heterogeneous coupling of two methanol molecules to methyl formate and hydrogen with a 100% selectivity below 180 °C. The reaction is industrially important as well as the key step in methanol steam reforming on gold catalysts.



中文翻译:

在碱性溶液中制备的单原子金氧基团簇可催化非均相甲醇自偶联反应。

为了获得最大的原子效率,近来加强了对非均相单原子催化剂的研究。将有机金属均相催化剂固定在表面上会产生保留单核和活性的问题,而开发用于在氧化物载体上制备原子分散的贵金属的几种技术通常很复杂。在这里,我们报告了一种在碱溶液中形成的稳健的一锅法合成无机金属单核金络合物,作为健壮且用途广泛的单原子金催化剂。络合物在浸渍到载体上或在空气中干燥后保持完整,得到结晶粉末。它们可用于询问已知由氧化金物质催化的反应的催化活性金部位的核。我们证明[Au 1 –Ox ] –团簇在180°C以下以100%的选择性引导两个甲醇分子与甲酸甲酯和氢的异质偶联。该反应在工业上很重要,也是在金催化剂上进行甲醇蒸汽重整的关键步骤。

更新日期:2019-10-21
down
wechat
bug