Electronically Engineering Water Resistance in Methane Combustion with an Atomically Dispersed Tungsten on PdO Catalyst. (5th May 2022)

• Record Type: Journal Article
• Authors: Hou, Zhiquan; Dai, Lingyun; Deng, Jiguang; Zhao, Guofeng; Jing, Lin; Wang, Yueshuai; Yu, Xiaohui; Gao, Ruyi; Tian, Xinrong; Dai, Hongxing; Wang, Dingsheng; Liu, Yuxi
• Is Part Of: Angewandte Chemie. Volume 134:Number 27(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-05-05
• Subjects: Electronic Metal-Support Interactions -- Metal Nanoparticles -- Methane Combustion -- Single-Atom Catalysts -- Water Resistance; Chemistry -- Periodicals; 540
• DOI: 10.1002/ange.202201655
• Languages: English
• ISSNs: 0044-8249

Abstract

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−W1 ‐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. Abstract : Methane combustion generates less CO2 emissions than coal and oil, making it a cleaner alternative to other fossil fuels. A PdW1 /Al2 O3 single‐atom catalyst shows enhanced H2 O‐resistance during CH4 combustion. The results show that catalytic CH4 combustion involves water and proceeds via a hydroperoxyl‐promoted reaction on the catalyst surface. An upshift of the d‐band center of Pd aids the adsorption and activation of oxygen on the catalyst.