Highly-stable cobalt metal organic framework with sheet-like structure for ultra-efficient water oxidation at high current density

Zhenjie Lu; Wenzhi Luo; Xinning Huang; Huixuan Yu; Zhiwei Li; Guocheng Liu; Jianwen Liu; Xingxing Chen

doi:10.1016/j.jcis.2021.12.132

Highly-stable cobalt metal organic framework with sheet-like structure for ultra-efficient water oxidation at high current density

J Colloid Interface Sci. 2022 Apr:611:599-608. doi: 10.1016/j.jcis.2021.12.132. Epub 2021 Dec 22.

Authors

Zhenjie Lu¹, Wenzhi Luo², Xinning Huang¹, Huixuan Yu³, Zhiwei Li⁴, Guocheng Liu⁵, Jianwen Liu⁶, Xingxing Chen⁷

Affiliations

¹ Research Group of Functional Materials for New Energy, School of Chemical Engineering, University of Science and Technology Liaoning, Qianshan Middle Road 185, Anshan 114051, PR China.
² College of Materials Science and Engineering, Shenzhen University, Shenzhen 518600, PR China.
³ College of Chemistry and Chemical Engineering, Professional Technology Innovation Center of Liaoning Province for Conversion Materials of Solar Cell, Bohai University, Jinzhou 121013, PR China.
⁴ National Supercomputing Center in Shenzhen, Shenzhen 518055, PR China.
⁵ College of Chemistry and Chemical Engineering, Professional Technology Innovation Center of Liaoning Province for Conversion Materials of Solar Cell, Bohai University, Jinzhou 121013, PR China. Electronic address: lgch1004@sina.com.
⁶ College of Materials Science and Engineering, Shenzhen University, Shenzhen 518600, PR China. Electronic address: jwliu@szu.edu.cn.
⁷ Research Group of Functional Materials for New Energy, School of Chemical Engineering, University of Science and Technology Liaoning, Qianshan Middle Road 185, Anshan 114051, PR China. Electronic address: xingchenstar79@163.com.

PMID: 34973656
DOI: 10.1016/j.jcis.2021.12.132

Abstract

The development of efficient and robust non-precious electrocatalysts for water oxidation at a mild condition is extremely desirable for industrial water splitting. Herein we developed a facile solvothermal strategy to synthesize cobalt metal organic frameworks (Co-MOFs) with sheet-like structure, which showed highly promising performance for electrocatalytic oxygen evolution. The best Co-MOF sample afforded an ultra-high oxygen evolution current density of 63.4 mA cm^-2 at 1.75 V in 1 M KOH with a catalyst loading of only 0.21 mg cm^-2. Notably, its electrochemical performance remained unchanged after 10,000 cyclic voltammograms indicating very promising long-term stability. Detailed study of the mechanism of the oxygen evolution by density functional theory (DFT) indicated that the strong π-conjugation formed between the central cobalt ion and adjacent aromatic rings favored the high electrocatalytic performance. The solvothermally synthesized MOFs proposed in this paper are expected to inspire the rational design of high-performance electrocatalysts for water oxidation with atomic and molecular level structural control and the exploration of structure-performance relationships to understand the electrocatalytic origin.

Keywords: Density functional theory (DFT); Metal organic framework (MOF); Solvothermal synthesis; Water oxidation; π-conjugation effect.