journal article·2024-05Open access

Steering CO2 Electroreduction to C2+ Products via Enhancing Localized *CO Coverage and Local Pressure in Conical Cavity

Congcong Li, Tingting Zhang, Heng Liu, Zhongyuan Guo, Zhongliang Liu, Haojun Shi, Jialin Cui, Hao Li, Huihui Li, Chunzhong Li

Advanced Materials· Volume 36· Issue 18

Abstract

Abstract The electrochemical carbon dioxide (CO2) reduction reaction (CO2RR) involves a multistep proton‐coupled electron transfer (PCET) process that generates a variety of intermediates, making it challenging to transform them into target products with high activity and selectivity. Here, a catalyst featuring a nanosheet‐stacked sphere structure with numerous open and deep conical cavities (OD‐CCs) is reported. Under the guidance of the finite‐element method (FEM) simulations and theoretical analysis, it is shown that exerting control over the confinement space results in diffusion limitation of the carbon intermediates, thereby increasing local pressure and subsequently enhancing localized *CO coverage for dimerization. The nanocavities exhibit a structure‐driven shift in selectivity of multicarbon (C2+) product from 41.8% to 81.7% during the CO2RR process.
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Research context

OpenAlex topics: CO2 Reduction Techniques and Catalysts · Ionic liquids properties and applications · Electrocatalysts for Energy Conversion

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Key Laboratory for Ultrafine Materials of Ministry of Education School of Chemical Engineering East China University of Science and Technology Shanghai 200237 China

Advanced Institute for Materials Research (WPI‐AIMR) Tohoku University Sendai 980–8577 Japan

College of Environmental and Resource Sciences Zhejiang University Hangzhou 310058 China

Shanghai Engineering Research Center of Hierarchical Nanomaterials School of Materials Science and Engineering East China University of Science and Technology Shanghai 200237 China

Funding

National Natural Science Foundation of China · Science and Technology Commission of Shanghai Municipality · Shanghai Rising-Star Program · Iwatani Naoji Foundation

References (34)

Show source-provided references
1. 10.1038/nature1147510.1038/nature11475 ↗
2. 10.1002/anie.20211283510.1002/anie.202112835 ↗
3. 10.1126/science.aav350610.1126/science.aav3506 ↗
4. 10.1038/s41560-019-0374-610.1038/s41560-019-0374-6 ↗
5. 10.1039/D1CS00535A10.1039/D1CS00535A ↗
6. 10.1016/j.ccr.2021.21398310.1016/j.ccr.2021.213983 ↗
7. 10.1021/acsnano.0c1069710.1021/acsnano.0c10697 ↗
8. 10.1039/D2SE01174C10.1039/D2SE01174C ↗
9. 10.1021/acs.jpclett.5b0072210.1021/acs.jpclett.5b00722 ↗
10. 10.1126/sciadv.aay311110.1126/sciadv.aay3111 ↗
11. 10.1021/acscatal.1c0147810.1021/acscatal.1c01478 ↗
12. 10.1038/s41929-022-00751-010.1038/s41929-022-00751-0 ↗
13. 10.1038/s41467-023-36530-z10.1038/s41467-023-36530-z ↗
14. 10.1021/jacs.0c0169910.1021/jacs.0c01699 ↗
15. 10.1016/j.apcatb.2022.12111110.1016/j.apcatb.2022.121111 ↗
16. 10.1002/anie.20211349810.1002/anie.202113498 ↗
17. 10.1038/s41929-018-0168-410.1038/s41929-018-0168-4 ↗
18. 10.1039/b924097g10.1039/b924097g ↗
19. 10.1038/s41586-020-2783-x10.1038/s41586-020-2783-x ↗
20. 10.1002/anie.20211065710.1002/anie.202110657 ↗
21. Kim J. Y. · Angew. Chem., Int. Ed. · 2022 · 34
22. 10.1038/s41467-022-29428-910.1038/s41467-022-29428-9 ↗
23. 10.1021/acscatal.7b0434710.1021/acscatal.7b04347 ↗
24. 10.1016/j.joule.2021.02.00810.1016/j.joule.2021.02.008 ↗
25. 10.1021/jacs.9b0741510.1021/jacs.9b07415 ↗
26. 10.1002/anie.20201515910.1002/anie.202015159 ↗
27. 10.1038/s41467-020-17690-810.1038/s41467-020-17690-8 ↗
28. Kim Y. · Environ. Sci. · 2020 · 13 · 4301
29. 10.1021/acscatal.5b0254310.1021/acscatal.5b02543 ↗
30. 10.1038/s41557-018-0092-x10.1038/s41557-018-0092-x ↗
31. 10.1021/jacs.9b0212410.1021/jacs.9b02124 ↗
32. 10.1063/1.132967210.1063/1.1329672 ↗
33. 10.1063/1.132322410.1063/1.1323224 ↗
34. 10.1021/jacs.9b0212410.1021/jacs.9b02124 ↗