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Ceria nanocrystals supporting Pd for formic acid electrocatalytic oxidation: prominent polar surface metal support interactions

DOI: 10.1021/acscatal.9b00421 DOI Help

Authors: Lin Ye (The Wolfson Catalysis Centre, University of Oxford) , A. A. Hanif Mahadi (The Wolfson Catalysis Centre, University of Oxford) , Chalathan Saengruengrit (Burapha University) , Jin Qu (The Wolfson Catalysis Centre, University of Oxford) , Feng Xu (The Wolfson Catalysis Centre, University of Oxford) , Simon Fairclough (University of Manchester) , Neil Young (University of Oxford) , Ping-luen Ho (University of Oxford) , Junjun Shan (University of Kansas) , Luan Nguyen (University of Kansas) , Franklin F. Tao (University of Kansas) , Karaked Tedsree (Burapha University) , Shik Chi Edman Tsang (University of Oxford)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Acs Catalysis

State: Published (Approved)
Published: April 2019

Abstract: Ceria has been widely used as support in electrocatalysis for its high degree of oxygen storage, fast oxygen mobility and reduction and oxidation properties at mild conditions. However, it is unclear what are the underlying principles and the nature of surface involved. By controlling the growth of various morphologies of ceria nanoparticles, it is demonstrated that the cubic-form of ceria, predominantly covered with higher energy polar surface (100), as support for Pd gives much higher activity in the electrocatalytic oxidation of formic acid than ceria of other morphologies (rods and spheres) with low indexed facets ((110) and (111)). High resolution TEM confirms the alternating layer-to-layer of cations and anions in (100) surface, the electrostatic repulsion of oxygen anions within the same layers gives intrinsically higher oxygen vacancies on this redox active surface in order to reduce surface polarity. DFT calculations suggest that the properties of fast oxygen mobility to re-oxidize the CO-poisoned Pd may arise from the overdosed oxygens on these ceria surface layers during electro-oxidation hence sustaining higher activity.

Journal Keywords: ceria; noble metal; electrocatalysis; facet; polarity

Subject Areas: Chemistry, Materials

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