| Full text | |
| Author(s): |
Khiarak, Behnam Nourmohammadi
;
da Silva, Gelson T. S. T.
;
Crane, Jackson
;
O'Brien, Colin P.
;
Pepe, Michael R.
;
Gabardo, Christine M.
;
Golovanova, Viktoria
;
de Arquer, F. Pelayo Garcia
;
Dinh, Cao-Thang
Total Authors: 9
|
| Document type: | Journal article |
| Source: | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION; v. N/A, p. 10-pg., 2025-07-17. |
| Abstract | |
Carbon dioxide (CO2) electroreduction directly from a reactive carbon solution (e.g., (bi)carbonate) provides a promising approach for integrating CO2 capture and conversion. Compared to CO2 conversion in gas-fed systems, this system typically suffers from low Faradaic efficiency (FE), especially for multicarbon (C2+) products. Here, we report an engineered material structuring to selectively produce C2+ products directly from a N2-saturated bicarbonate solution. Multiphysics modeling studies reveal the critical role of local current density distribution and the spatio-selective evolution of C2+ products, which is favored in thinner catalysts (240 mu m thickness). By jointly tailoring catalyst configuration and mass transport in bicarbonate electroreduction, adjusting the thickness, porosity, and surface oxidation of copper (Cu) mesh catalysts, as well as catholyte composition, we achieved a maximum C2H4 FE of 39% and total C2+ FE over 55% at 150 mA cm-2 with a 240 mu m thick Cu mesh. The system is also stable for over 160 h at 100 mA cm-2 with maintained C2H4 FE over 20%. Our electrolysis system converts bicarbonate to C2+ with over 90% CO2 utilization efficiency, reducing regeneration and separation costs. Optimizing catalyst pore structure, and copper surface oxide is a key to maximizing C2H4 production from bicarbonate solutions. (AU) | |
| FAPESP's process: | 23/10268-2 - Developing metal phosphide catalysts for selective and high-rate CO2 electroreduction |
| Grantee: | Gelson Tiago dos Santos Tavares da Silva |
| Support Opportunities: | Scholarships abroad - Research Internship - Post-doctor |
| FAPESP's process: | 13/07296-2 - CDMF - Center for the Development of Functional Materials |
| Grantee: | Elson Longo da Silva |
| Support Opportunities: | Research Grants - Research, Innovation and Dissemination Centers - RIDC |