Issue 10, 2023

Medium-entropy state quinary keplerate clusters as a remarkable electrocatalyst for small molecule electrooxidation

Abstract

The synthesis of discrete polyoxometalate clusters composed of more than 3 metallic elements has always been attractive but seldom successful. For the first time, we have developed a de novo synthetic route to quinary Cu–Ni–Co–Mn–Zn Keplerate clusters with a nuclearity of 20. Seven single-crystalline quinary Keplerates in a medium-entropy state with various compositions have been obtained. A systematic study reveals that the different ions’ ability to be incorporated into the Keplerates is governed by the Irving–Williams series, and they are stabilized in a medium entropy state. More intriguingly, these quinary Keplerate clusters represent an analogue of the Ship of Theseus at the molecular level, i.e., the global features of the {M20} Keplerates are intact, while the constitution can be altered by tuning the synthesis conditions. Our further investigation reveals that the quinary elements {M20} compared to mono-component and binary Keplerate clusters exhibit much superior electrochemical performance, therefore shedding light on the design of multimetallic clusters in high-entropy states as novel electrocatalysts.

Graphical abstract: Medium-entropy state quinary keplerate clusters as a remarkable electrocatalyst for small molecule electrooxidation

Supplementary files

Article information

Article type
Research Article
Submitted
18 Febr. 2023
Accepted
04 Apr. 2023
First published
05 Apr. 2023

Inorg. Chem. Front., 2023,10, 3047-3057

Medium-entropy state quinary keplerate clusters as a remarkable electrocatalyst for small molecule electrooxidation

M. Cao, H. Ye, Y. Liu, J. Wang, Y. Zhou, X. Wang, S. Wu, F. Xu and Y. Wu, Inorg. Chem. Front., 2023, 10, 3047 DOI: 10.1039/D3QI00316G

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