Electrochemical conversion of CO2 to syngas with a stable H2/CO ratio in a wide potential range over ligand-engineered metal–organic frameworks
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Wu, X
Liu, Y
Mao, F
Shi, Y
Li, J
Zhu, M
Dai, S
Chen, A
Liu, PF
Yang, HG
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Abstract
The efficient electrochemical conversion of CO2 to value-added chemicals is a promising approach to mitigate the current energy and environmental challenges. In this work, a ligand-engineering strategy was reported to be applied to stabilize CO2 adsorption in metal-organic frameworks (MOFs). Zn-based MOFs (Zn-MOFs) related to two different carboxyl functional ligands, i.e., 1,3,5-benzenetricarboxylic acid (Zn-BTC) and 1,4-benzenedicarboxylate (Zn-BDC), were investigated for the CO2 reduction reaction (CO2RR) in a flow cell electrolyzer. Zn-BTC exhibits a stable H2/CO ratio (≈1 : 2) up to a high current density (−300 mA cm−2) in a wide potential range (−0.96 to −1.96 V vs. RHE) in 1 M KOH. The molar H2/CO ratio is steady in both neutral and alkaline electrolytes. Ex situ experimental results indicate that the carboxyl groups in Zn-BTC are more durable than those in Zn-BDC, which also enhances the absorption of CO2. In situ attenuated total reflection surface-enhanced infrared absorption spectroscopy elucidates that carboxyl groups can stabilize CO2RR intermediates. This work not only verifies the significance of the carboxyl groups in sustaining molecular structures but also offers valuable understandings in electrocatalyst design.
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Journal of Materials Chemistry A
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10
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18
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Chemical engineering
Electrochemical energy storage and conversion
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Cao, L; Wu, X; Liu, Y; Mao, F; Shi, Y; Li, J; Zhu, M; Dai, S; Chen, A; Liu, PF; Yang, HG, Electrochemical conversion of CO2 to syngas with a stable H2/CO ratio in a wide potential range over ligand-engineered metal–organic frameworks, Journal of Materials Chemistry A, 2022, 10 (18), pp. 9954-9959