2D Copper Tetrahydroxyquinone Conductive Metal–Organic Framework for Selective CO 2 Electrocatalysis at Low Overpotentials
Abstract
Abstract 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 (CuTHQ), is reported for aqueous CO 2 reduction reaction (CO 2 RR) at low overpotentials. It is revealed that CuTHQ 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 ≈173 mA cm −2 at −0.45 V versus RHE, an average Faradaic efficiency (F.E.) of ≈91% toward CO production, and a remarkable turnover frequency as high as ≈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 CO 2 RR which reversibly returns to Cu 2+ after the reaction. The outstanding CO 2 catalytic functionality of conductive MOFs (c‐MOFs) can open a way toward high‐energy‐density electrochemical systems.
- Authors:
-
[1];
[1]
- Department of Mechanical and Industrial Engineering University of Illinois at Chicago Chicago IL 60607 USA
- Materials Science Division Argonne National Laboratory Lemont IL 60439 USA
- Department of Chemistry University of Illinois at Chicago Chicago IL 60607 USA
- Department of Materials and Environmental Chemistry Stockholm University Stockholm 10691 Sweden
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1785880
- Grant/Contract Number:
- DE‐AC02‐06CH11357
- Resource Type:
- Publisher's Accepted Manuscript
- Journal Name:
- Advanced Materials
- Additional Journal Information:
- Journal Name: Advanced Materials Journal Volume: 33 Journal Issue: 10; Journal ID: ISSN 0935-9648
- Publisher:
- Wiley Blackwell (John Wiley & Sons)
- Country of Publication:
- Germany
- Language:
- English
Citation Formats
Majidi, Leily, Ahmadiparidari, Alireza, Shan, Nannan, Misal, Saurabh N., Kumar, Khagesh, Huang, Zhehao, Rastegar, Sina, Hemmat, Zahra, Zou, Xiaodong, Zapol, Peter, Cabana, Jordi, Curtiss, Larry A., and Salehi‐Khojin, Amin. 2D Copper Tetrahydroxyquinone Conductive Metal–Organic Framework for Selective CO 2 Electrocatalysis at Low Overpotentials. Germany: N. p., 2021.
Web. doi:10.1002/adma.202004393.
Majidi, Leily, Ahmadiparidari, Alireza, Shan, Nannan, Misal, Saurabh N., Kumar, Khagesh, Huang, Zhehao, Rastegar, Sina, Hemmat, Zahra, Zou, Xiaodong, Zapol, Peter, Cabana, Jordi, Curtiss, Larry A., & Salehi‐Khojin, Amin. 2D Copper Tetrahydroxyquinone Conductive Metal–Organic Framework for Selective CO 2 Electrocatalysis at Low Overpotentials. Germany. https://doi.org/10.1002/adma.202004393
Majidi, Leily, Ahmadiparidari, Alireza, Shan, Nannan, Misal, Saurabh N., Kumar, Khagesh, Huang, Zhehao, Rastegar, Sina, Hemmat, Zahra, Zou, Xiaodong, Zapol, Peter, Cabana, Jordi, Curtiss, Larry A., and Salehi‐Khojin, Amin. Mon .
"2D Copper Tetrahydroxyquinone Conductive Metal–Organic Framework for Selective CO 2 Electrocatalysis at Low Overpotentials". Germany. https://doi.org/10.1002/adma.202004393.
@article{osti_1785880,
title = {2D Copper Tetrahydroxyquinone Conductive Metal–Organic Framework for Selective CO 2 Electrocatalysis at Low Overpotentials},
author = {Majidi, Leily and Ahmadiparidari, Alireza and Shan, Nannan and Misal, Saurabh N. and Kumar, Khagesh and Huang, Zhehao and Rastegar, Sina and Hemmat, Zahra and Zou, Xiaodong and Zapol, Peter and Cabana, Jordi and Curtiss, Larry A. and Salehi‐Khojin, Amin},
abstractNote = {Abstract 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 (CuTHQ), is reported for aqueous CO 2 reduction reaction (CO 2 RR) at low overpotentials. It is revealed that CuTHQ 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 ≈173 mA cm −2 at −0.45 V versus RHE, an average Faradaic efficiency (F.E.) of ≈91% toward CO production, and a remarkable turnover frequency as high as ≈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 CO 2 RR which reversibly returns to Cu 2+ after the reaction. The outstanding CO 2 catalytic functionality of conductive MOFs (c‐MOFs) can open a way toward high‐energy‐density electrochemical systems.},
doi = {10.1002/adma.202004393},
journal = {Advanced Materials},
number = 10,
volume = 33,
place = {Germany},
year = {Mon Feb 01 00:00:00 EST 2021},
month = {Mon Feb 01 00:00:00 EST 2021}
}
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