Journal
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
Volume 167, Issue 14, Pages -Publisher
ELECTROCHEMICAL SOC INC
DOI: 10.1149/1945-7111/abc4f5
Keywords
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Funding
- National Science Foundation, CBET [0933141, 1511390]
- U.S. Department of Energy (DOE), Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-SC0001531]
- National Science Foundation [ACI-1053575]
- Directorate For Engineering
- Div Of Chem, Bioeng, Env, & Transp Sys [1511390] Funding Source: National Science Foundation
- Directorate For Engineering
- Div Of Chem, Bioeng, Env, & Transp Sys [0933141] Funding Source: National Science Foundation
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The spinel oxide, Cu1.5Mn1.5O4 (CMO) is a promising precious group metal-free electrocatalyst (EC) known for acid-mediated oxygen evolution reaction (OER). By employing density functional theory (DFT) based Bader analysis for active sites identification, the effective electronic charges of constituent ions in the ordered-disordered crystal structures were calculated. Accordingly, for DFT result validation, structurally disordered Cu1.5Mn1.5O4 ECs were experimentally synthesized by heat treatment to 200 degrees C (CMO-200). The disorder-order transitions of CMO related change in surface atomic arrangement and alteration in the Mn3+/Mn4+ and Cu2+/Cu1+ states are modulated via corresponding heat treatment (200 degrees C-800 degrees C) of CMO, revealing significant influence on OER electrocatalytic activity and durability. The measured higher electrocatalytic activity of disordered CMO-200 contrasted with ordered CMO is attributed to higher Mn3+/Mn4+ and Cu2+/Cu1+ states, signifying the beneficial role of Mn3+ and Cu2+ for facilitating OER. The ordered CMO structures containing lower Mn3+/Mn4+ and Cu2+/Cu1+ ratios albeit reveal higher electrochemical stability than the disordered CMO. The present study, thus, provides fundamental insights into the influence of ordered-disordered structures and rearrangement of the oxidation state of active species and their combined synergistic effects on the electrochemical performance for engineering high-performance ECs for acidic OER. (c) 2020 The Electrochemical Society (ECS). Published on behalf of ECS by IOP Publishing Limited.
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