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Enhancing perovskite electrocatalysis through synergistic functionalization of B-site cation for efficient water splitting

Journal Article · · Chemical Engineering Journal
 [1];  [2];  [3];  [4];  [5];  [4];  [2];  [5]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Changji Univ., Changji (China)
  2. Xiamen Univ., Xiamen (China). National Engineering Laboratory for Green Chemical Productions of Alcohols, Ethers and Esters
  3. Indiana State Univ., Terre Haute, IN (United States)
  4. Univ. of Alberta, Edmonton, AB (Canada)
  5. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
The family of perovskite oxides is a promising class of catalysts for diverse energy conversion processes including water splitting. In this work, a facile two-step manipulation (in-situ exsolution and post-sulfurization) strategy was proposed and applied to LaCo0.2Fe0.8O3 (LCF) perovskite parent, through which, the electronic state, spatial immersion and intrinsic activity of B-site cobalt (Co) were stepwise tuned at nanoscale proximity accordingly (i.e., lattice Co ions segregated Co0→ embedded CoS2). Impressively, the as-prepared catalyst (S-LCF) obtains an emergent oxygen deficient microstructure seamlessly pinned with uniformly distributed CoS2 nanoparticles (NPs), which demonstrates enhanced performance toward both oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), and shows good stability in overall water splitting. The density functional theory (DFT) calculations illustrate the optimized metal-oxygen covalency and hydrogen adsorption Gibbs free energy (Δ GH*) on S-LCF, which further buttresses the prominence of our B-site cation engineering tactics.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
Indiana State University; National Natural Science Foundation of China (NSFC); USDOE; USDOE Office of Science (SC); Xiamen University
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1788245
Alternate ID(s):
OSTI ID: 1779520
Journal Information:
Chemical Engineering Journal, Journal Name: Chemical Engineering Journal Vol. 401; ISSN 1385-8947
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

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