Journal
ADVANCED MATERIALS
Volume 33, Issue 10, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202004393
Keywords
CO2 reduction reaction; conductive metal-organic frameworks; electrocatalysis
Categories
Funding
- National Science Foundation DMREF [1729420]
- NSF CBET [1800357]
- Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division
- U.S. Department of Energy Office of Science laboratory [DE-AC02-06CH11357]
- CATSS project from the Knut and Alice Wallenberg Foundation [KAW 2016.0072]
- Swedish Research Council (VR) [2017-04321, 2016-04625]
- Directorate For Engineering
- Div Of Chem, Bioeng, Env, & Transp Sys [1800357] Funding Source: National Science Foundation
- Swedish Research Council [2016-04625] Funding Source: Swedish Research Council
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A 2D copper-based conductive MOF, Cu-THQ, exhibits excellent catalytic activity for aqueous CO2 reduction reaction (CO2RR) with low overpotentials. The material shows high CO production rate and current density at low overpotentials, making it a promising candidate for practical applications in CO2RR.
Metal-organic frameworks (MOFs) are promising materials for electrocatalysis; however, lack of electrical conductivity in the majority of existing MOFs limits their effective utilization in the field. Herein, an excellent catalytic activity of a 2D copper (Cu)-based conductive MOF, copper tetrahydroxyquinone (Cu-THQ), is reported for aqueous CO2 reduction reaction (CO2RR) at low overpotentials. It is revealed that Cu-THQ nanoflakes (NFs) with an average lateral size of 140 nm exhibit a negligible overpotential of 16 mV for the activation of this reaction, a high current density of approximate to 173 mA cm(-2) at -0.45 V versus RHE, an average Faradaic efficiency (F.E.) of approximate to 91% toward CO production, and a remarkable turnover frequency as high as approximate to 20.82 s(-1). In the low overpotential range, the obtained CO formation current density is more than 35 and 25 times higher compared to state-of-the-art MOF and MOF-derived catalysts, respectively. The operando Cu K-edge X-ray absorption near edge spectroscopy and density functional theory calculations reveal the existence of reduced Cu (Cu+) during CO2RR which reversibly returns to Cu2+ after the reaction. The outstanding CO2 catalytic functionality of conductive MOFs (c-MOFs) can open a way toward high-energy-density electrochemical systems.
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