Journal
ACS CATALYSIS
Volume 10, Issue 10, Pages 5623-5630Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b05470
Keywords
covalent organic frameworks (COFs); thiadiazole moiety; metal-free electrocatalyst; oxygen evolution reaction (OER); water splitting
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Funding
- DST-SERB, New Delhi [CRG/2018/000230]
- EPSRC [EP/S015868/1]
- HPC resources on Thomas via the Materials Chemistry Consortium [EP/P020194]
- UGC, New Delhi
- MNRE, New Delhi
- BRNS, Mumbai, India
- CSIR, New Delhi, India
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Covalent organic frameworks (COFs) have attracted surging interest lately due to their wide potential in several frontline application areas like gas storage, sensing, photovoltaics, fuel cells, active catalyst supports, and so on. However, only very few reports are available for the metal-free electrocatalysis over COFs. Herein, we developed a new thiadiazole-based COF, C4-SHz COF, through the reaction between 1,3,5-tris(4-formylphenyl)benzene and 2,5-dihydrazinyl- 1,3,4-thiadiazole that possesses a very high specific surface area of 1224 m(2) g(-1), unique molecular architecture, high porosity, and abundant active sites. The synthesized C4-SHz COF displayed superior electrocatalytic oxygen evolution reaction (OER) activity and excellent long-term durability. The electrocatalytic performance of the C4-SHz COF achieved a current density of 10 mA/cm(2) at an overpotential of 320 mV. The higher activity of the C4-SHz COF could be attributed to the high Brunauer-Emmett-Teller surface area, porosity, and network structure of the pi-conjugated organic building blocks, which allowed fast charge and mass transport processes. This work validates the promising potential of a metal-free COF electrocatalyst toward the OER and its capability to replace carbon-based electrocatalysts.
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