Local CO2 reservoir layer promotes rapid and selective electrochemical CO2 reduction

Subhabrata Mukhopadhyay, Muhammad Saad Naeem, G. Shiva Shanker, Arnab Ghatak, Alagar R. Kottaichamy, Ran Shimoni, Liat Avram, Itamar Liberman, Rotem Balilty, Raya Ifraemov, Illya Rozenberg, Menny Shalom, Núria López () and Idan Hod ()
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Subhabrata Mukhopadhyay: Ben-Gurion University of the Negev
Muhammad Saad Naeem: The Barcelona Institute of Science and Technology (BIST)
G. Shiva Shanker: Ben-Gurion University of the Negev
Arnab Ghatak: Ben-Gurion University of the Negev
Alagar R. Kottaichamy: Ben-Gurion University of the Negev
Ran Shimoni: Ben-Gurion University of the Negev
Liat Avram: Department of Chemical Research Support Weizmann Institute of Science
Itamar Liberman: Ben-Gurion University of the Negev
Rotem Balilty: Ben-Gurion University of the Negev
Raya Ifraemov: Ben-Gurion University of the Negev
Illya Rozenberg: Ben-Gurion University of the Negev
Menny Shalom: Ben-Gurion University of the Negev
Núria López: The Barcelona Institute of Science and Technology (BIST)
Idan Hod: Ben-Gurion University of the Negev

Nature Communications, 2024, vol. 15, issue 1, 1-14

Abstract: Abstract Electrochemical CO2 reduction reaction in aqueous electrolytes is a promising route to produce added-value chemicals and decrease carbon emissions. However, even in Gas-Diffusion Electrode devices, low aqueous CO2 solubility limits catalysis rate and selectivity. Here, we demonstrate that when assembled over a heterogeneous electrocatalyst, a film of nitrile-modified Metal-Organic Framework (MOF) acts as a remarkable CO2-solvation layer that increases its local concentration by ~27-fold compared to bulk electrolyte, reaching 0.82 M. When mounted on a Bi catalyst in a Gas Diffusion Electrode, the MOF drastically improves CO2-to-HCOOH conversion, reaching above 90% selectivity and partial HCOOH currents of 166 mA/cm2 (at −0.9 V vs RHE). The MOF also facilitates catalysis through stabilization of reaction intermediates, as identified by operando infrared spectroscopy and Density Functional Theory. Hence, the presented strategy provides new molecular means to enhance heterogeneous electrochemical CO2 reduction reaction, leading it closer to the requirements for practical implementation.

Date: 2024
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DOI: 10.1038/s41467-024-47498-9

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