Fine-Tuning the Coordinatively Unsaturated Metal Sites of Metal−Organic Frameworks by Plasma Engraving for Enhanced Electrocatalytic Activity

Jiang, Zongrui and Ge, Lei ORCID: https://orcid.org/0000-0003-2989-0329 and Zhuang, Linzhou and Li, Mengran and Wang, Zhanke and Zhu, Zhonghua (2019) Fine-Tuning the Coordinatively Unsaturated Metal Sites of Metal−Organic Frameworks by Plasma Engraving for Enhanced Electrocatalytic Activity. ACS Applied Materials & Interfaces, 11 (47). pp. 44300-44307. ISSN 1944-8244


Abstract

Metal−organic frameworks (MOFs) have recently emerged as promising electrocatalysts because of their atomically dispersed metal sites and porous structures. The active sites of MOF catalysts largely exist as coordinatively unsaturated metal sites (CUMSs). In this study, facile microwave-induced plasma engraving is applied to finetune the CUMSs of cobalt-based MOF (Co-MOF-74) without destroying its phase integrity by controlling the plasma engraving species, intensity, and duration. The electrochemical activity of the engraved MOF is found to be quantitatively correlated to the coordination geometry of the metal centers corresponding to CUMSs. Specifically, the hydrogen plasma-engraved Co-MOF-74 shows an enhanced catalytic activity of oxygen evolution reaction, which exhibits a low overpotential (337 mV at 15 mA cm−2), high turnover frequency (0.0219 s−1), and large mass activity (54.3 A g−1). The developed CUMS control strategy and the revealed CUMSs activity correlation can inspire the further microstructure tuning of MOFs for various applications.


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Item Type: Article (Commonwealth Reporting Category C)
Refereed: Yes
Item Status: Live Archive
Additional Information: Files associated with this item cannot be displayed due to copyright restrictions.
Faculty/School / Institute/Centre: Current - Institute for Advanced Engineering and Space Sciences - Centre for Future Materials (1 Jan 2017 -)
Faculty/School / Institute/Centre: Current - Institute for Advanced Engineering and Space Sciences - Centre for Future Materials (1 Jan 2017 -)
Date Deposited: 27 Jan 2020 23:50
Last Modified: 29 Jan 2020 05:31
Uncontrolled Keywords: metal−organic framework; oxygen evolution reaction; coordinatively unsaturated metal site; defect; plasma engraving
Fields of Research : 03 Chemical Sciences > 0303 Macromolecular and Materials Chemistry > 030304 Physical Chemistry of Materials
09 Engineering > 0904 Chemical Engineering > 090402 Catalytic Process Engineering
Socio-Economic Objective: B Economic Development > 86 Manufacturing > 8606 Industrial Chemicals and Related Products > 860601 Industrial Gases
Identification Number or DOI: 10.1021/acsami.9b15794
URI: http://eprints.usq.edu.au/id/eprint/37418

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