Rashid, Nusrat;
Dar, Farooq Ahmad;
Bhat, Mohsin Ahmad;
Ingole, Pravin Popinand;
(2023)
Tailoring Motif and Channel Terminating Groups of Conventional Copper MOFs for Their Enhanced Activity, Selectivity, and Stability toward the Electroreduction of CO2 to Hydrocarbons.
ACS Applied Energy Materials
, 6
(3)
pp. 1378-1388.
10.1021/acsaem.2c03237.
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Abstract
Judicious tuning of electronic effects, chemical functionalities, and type and distribution of active sites is a promising strategy to manage the selectivity, efficiency, and electrochemical stability of electrocatalysts toward the electrochemical reduction of CO2 (ERCO2). Herein, we report a simple postsynthetic modification to tune electronic effects and Lewis basicity in copper-based three-dimensional (3D) and two-dimensional (2D) metal-organic frameworks (MOFs) involving the chemical transformation of the free −COOH/-OH groups into amide/amine groups that improves their electrocatalytic stability and performance for hydrocarbon production. Detailed structural and voltammetric characterizations reveal that the unique electronic and structure-enhancing effects in the modified MOFs (especially in 2D MOF) endow them with excellent electrocatalytic performance (overall faradaic efficiency (FE) 81%, with FEC1 = 62% and FEC2 = 19%) and stability toward ERCO2 (>4 h). The significantly high FE for the production of hydrocarbons over the modified MOFs is attributed to the improved Lewis acidity of the open metal centers and confined pores resulting in alternate active sites for *CO adsorption, hydrogenation, and C-O bond dissociation.
| Type: | Article |
|---|---|
| Title: | Tailoring Motif and Channel Terminating Groups of Conventional Copper MOFs for Their Enhanced Activity, Selectivity, and Stability toward the Electroreduction of CO2 to Hydrocarbons |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1021/acsaem.2c03237 |
| Publisher version: | https://doi.org/10.1021/acsaem.2c03237 |
| Language: | English |
| Additional information: | This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
| Keywords: | ADSORPTION, CARBON-DIOXIDE, CATALYSTS, Chemistry, Chemistry, Physical, CO2 reduction, Cu-MOFs, EFFICIENT, ELECTROCATALYTIC REDUCTION, ELECTROCHEMICAL REDUCTION, Energy & Fuels, hydrocarbon production, Materials Science, Materials Science, Multidisciplinary, METAL-ORGANIC-FRAMEWORK, MOF structural stability, NANOPARTICLES, OXIDATION, Physical Sciences, postsynthesis modification, Science & Technology, STRATEGY, Technology |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > MAPS Faculty Office UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > MAPS Faculty Office > Institute for Materials Discovery |
| URI: | https://discovery-pp.ucl.ac.uk/id/eprint/10203286 |
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