journal article·2023-05-12Open access

Hydrodynamics Change Tafel Slopes in Electrochemical CO 2 Reduction on Copper

Nicholas B. Watkins, Zachary J. Schiffer, Yungchieh Lai, Charles B. Musgrave, Harry A. Atwater, William A. Goddard, Theodor Agapie, Jonas C. Peters, John M. Gregoire

ACS Energy Letters· Volume 8· Issue 5

Abstract

High Resolution Image Download MS PowerPoint Slide The hydrodynamics of electrochemical CO 2 reduction (CO 2 R) systems is an insufficiently investigated area of research that has broad implications on catalyst activity and selectivity. While most previous reports are limited to laminar and CO 2 -sparged systems, herein we address a wide range of hydrodynamics via electrolyte recirculation systems. We find that increased hydrodynamics at the electrode surface results directly in changes to the ethylene and methane Tafel slopes, demonstrating that mass transport is on equal footing with catalyst active sites in determining reaction mechanisms and the ensuing product distribution. Mass transport is traditionally considered to be in the purview of systems-level engineering, yet the present work shows that CO 2 R mechanistic work must be considered in the context of the mass transport conditions. We extend our analysis to organic coatings, demonstrating that the films shield the active sites from variability in hydrodynamics and increase the residence time of CO so that it may be further reduced to desirable products.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: CO2 Reduction Techniques and Catalysts · Ionic liquids properties and applications · Advanced battery technologies research

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

Affiliations

Liquid Sunlight Alliance, California Institute of Technology, Pasadena, California 91125, United States

Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California 91125, United States

Division of Engineering and Applied Science, California Institute of Technology, Pasadena, California 91125, United States

Funding

Basic Energy Sciences

References (36)

Show source-provided references
1. 10.1038/s43017-022-00285-w10.1038/s43017-022-00285-w ↗
2. Foote E. · Am. J. Sci. Arts · 1856 · 22 · 383
3. 10.1246/cl.1986.89710.1246/cl.1986.897 ↗
4. 10.1073/pnas.060339510310.1073/pnas.0603395103 ↗
5. 10.1021/acs.chemrev.8b0070510.1021/acs.chemrev.8b00705 ↗
6. 10.1021/acs.chemrev.1c0090110.1021/acs.chemrev.1c00901 ↗
7. Bard A. J. · 1980 · 2
8. 10.1038/s41467-021-20924-y10.1038/s41467-021-20924-y ↗
9. 10.1021/jacs.8b0398610.1021/jacs.8b03986 ↗
10. 10.1039/D0EE02826F10.1039/D0EE02826F ↗
11. 10.1021/acscatal.1c0552010.1021/acscatal.1c05520 ↗
12. 10.1021/je101116810.1021/je1011168 ↗
13. 10.1021/acsaem.2c0016010.1021/acsaem.2c00160 ↗
14. 10.1021/acssuschemeng.2c0019510.1021/acssuschemeng.2c00195 ↗
15. 10.1039/c2ee21234j10.1039/c2ee21234j ↗
16. 10.1039/C6CP05287H10.1039/C6CP05287H ↗
17. 10.1021/acscatal.8b0134010.1021/acscatal.8b01340 ↗
18. 10.1021/jacs.7b0676510.1021/jacs.7b06765 ↗
19. 10.1021/acs.iecr.1c0185110.1021/acs.iecr.1c01851 ↗
20. 10.1007/s10800-005-9058-y10.1007/s10800-005-9058-y ↗
21. 10.1021/acsaem.9b0079110.1021/acsaem.9b00791 ↗
22. 10.1088/1361-6463/aa635910.1088/1361-6463/aa6359 ↗
23. 10.1021/acs.analchem.9b0499910.1021/acs.analchem.9b04999 ↗
24. 10.1021/jacs.9b1006110.1021/jacs.9b10061 ↗
25. 10.1007/BF0061588310.1007/BF00615883 ↗
26. 10.1016/j.electacta.2017.04.01710.1016/j.electacta.2017.04.017 ↗
27. 10.1002/aic.1760510.1002/aic.17605 ↗
28. 10.1021/acscentsci.1c0086010.1021/acscentsci.1c00860 ↗
29. 10.1063/1.504970410.1063/1.5049704 ↗
30. 10.1002/anie.20180605110.1002/anie.201806051 ↗
31. 10.1021/acs.jpcc.9b0682010.1021/acs.jpcc.9b06820 ↗
32. 10.1021/jacs.9b0700010.1021/jacs.9b07000 ↗
33. 10.1021/acscatal.1c0033810.1021/acscatal.1c00338 ↗
34. 10.1002/anie.20190793510.1002/anie.201907935 ↗
35. 10.1016/j.molliq.2014.01.00410.1016/j.molliq.2014.01.004 ↗
36. Deen W. M. · 2012