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利用原子分散在 PdO 催化剂上的钨对甲烷燃烧进行电子工程防水。

Electronically Engineering Water Resistance in Methane Combustion with an Atomically Dispersed Tungsten on PdO Catalyst.

作者信息

Hou Zhiquan, Dai Lingyun, Deng Jiguang, Zhao Guofeng, Jing Lin, Wang Yueshuai, Yu Xiaohui, Gao Ruyi, Tian Xinrong, Dai Hongxing, Wang Dingsheng, Liu Yuxi

机构信息

Department of Environmental Chemical Engineering, Beijing University of Technology, Beijing, 100124, China.

John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USA.

出版信息

Angew Chem Int Ed Engl. 2022 Jul 4;61(27):e202201655. doi: 10.1002/anie.202201655. Epub 2022 May 5.

Abstract

Improving the low-temperature water-resistance of methane combustion catalysts is of importance for industrial applications and it is challenging. A stepwise strategy is presented for the preparation of atomically dispersed tungsten species at the catalytically active site (Pd nanoparticles). After an activation process, a Pd-O-W -like nanocompound is formed on the PdO surface with an atomic scale interface. The resulting supported catalyst has much better water resistance than the conventional catalysts for methane combustion. The integrated characterization results confirm that catalytic combustion of methane involves water, proceeding via a hydroperoxyl-promoted reaction mechanism on the catalyst surface. The results of density functional theory calculations indicate an upshift of the d-band center of palladium caused by electron transfer from atomically dispersed tungsten, which greatly facilitates the adsorption and activation of oxygen on the catalyst.

摘要

提高甲烷燃烧催化剂的低温耐水性对工业应用具有重要意义,且具有挑战性。本文提出了一种逐步策略,用于在催化活性位点(钯纳米颗粒)上制备原子分散的钨物种。经过活化过程后,在PdO表面形成了具有原子尺度界面的类Pd-O-W纳米化合物。所得负载型催化剂在甲烷燃烧方面比传统催化剂具有更好的耐水性。综合表征结果证实,甲烷的催化燃烧涉及水,通过催化剂表面的氢过氧根促进反应机制进行。密度泛函理论计算结果表明,原子分散的钨的电子转移导致钯的d带中心上移,这极大地促进了催化剂上氧的吸附和活化。

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