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水相 Au-Pd 胶体在温和条件下,以 O2 为氧化剂,催化 CH 选择性氧化生成 CHOH。

Aqueous Au-Pd colloids catalyze selective CH oxidation to CHOH with O under mild conditions.

机构信息

Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, UK.

Department of Materials Science and Engineering, Lehigh University, 5 East Packer Avenue, Bethlehem, PA 18015, USA.

出版信息

Science. 2017 Oct 13;358(6360):223-227. doi: 10.1126/science.aan6515. Epub 2017 Sep 7.

Abstract

The selective oxidation of methane, the primary component of natural gas, remains an important challenge in catalysis. We used colloidal gold-palladium nanoparticles, rather than the same nanoparticles supported on titanium oxide, to oxidize methane to methanol with high selectivity (92%) in aqueous solution at mild temperatures. Then, using isotopically labeled oxygen (O) as an oxidant in the presence of hydrogen peroxide (HO) we demonstrated that the resulting methanol incorporated a substantial fraction (70%) of gas-phase O More oxygenated products were formed than the amount of HO consumed, suggesting that the controlled breakdown of HO activates methane, which subsequently incorporates molecular oxygen through a radical process. If a source of methyl radicals can be established, then the selective oxidation of methane to methanol using molecular oxygen is possible.

摘要

甲烷的选择性氧化是催化领域的一个重要挑战,而甲烷是天然气的主要成分。我们使用胶体金-钯纳米粒子,而不是负载在氧化钛上的相同纳米粒子,在温和的温度下,于水溶液中将甲烷高选择性(92%)氧化为甲醇。然后,在过氧化氢(HO)存在下,使用同位素标记的氧(O)作为氧化剂,我们证明生成的甲醇中掺入了大量(70%)的气相 O。形成的含氧产物比消耗的 HO 多,这表明 HO 的受控分解激活了甲烷,随后通过自由基过程掺入了分子氧。如果可以建立甲基自由基的来源,那么使用分子氧将甲烷选择性氧化为甲醇是可能的。

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