journal article·2024-11-08Open access

Asymmetric Bipolar Membrane for High Current Density Electrodialysis Operation with Exceptional Stability

Éowyn Lucas, Justin C. Bui, Timothy Nathan Stovall, Monica Hwang, Kaiwen Wang, Emily R. Dunn, Ellis Spickermann, Lily Shiau, Ahmet Kusoglu, Adam Z. Weber, Alexis T. Bell, Shane Ardo, Harry A. Atwater, Chengxiang Xiang

ACS Energy Letters· Volume 9· Issue 11

Abstract

Bipolar membranes (BPMs) enable isolated acidic/alkaline regions in electrochemical devices, facilitating optimized environments for electrochemical separations and catalysis. For economic viability, BPMs must attain stable, high current density operation with low overpotentials in a freestanding configuration. We report an asymmetric, graphene oxide (GrOx)-catalyzed BPM capable of freestanding electrodialysis operation at 1 A cm –2 with overpotentials <250 mV. Use of a thin anion-exchange layer improves water transport while maintaining near unity Faradaic efficiency for acid and base generation. Voltage stability exceeding 1100 h with an average drift of 70 μV/h at 80 mA cm –2 and 100 h with an average drift of −300 μV/h at 500 mA cm –2 and implementation in an electrodialysis stack demonstrate real-world applicability. Continuum modeling reveals that water dissociation in GrOx BPMs is both catalyzed and electric-field enhanced, where low p K a moieties on GrOx enhance local electric fields and high p K a moieties serve as active sites for surface-catalyzed water dissociation. These results establish commercially viable BPM electrodialysis and provide fundamental insight to advance design of next-generation devices.
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Research context

OpenAlex topics: Membrane-based Ion Separation Techniques · Fuel Cells and Related Materials · Advanced battery technologies research

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

Affiliations

Division of Engineering and Applied Science, California Institute of Technology, 1200 E California Blvd, Pasadena, California 91125, United States

Department of Chemical and Biomolecular Engineering, University of California, Berkeley, University Avenue and Oxford St, Berkeley, California 94720, United States

Chemical Sciences Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Rd, Berkeley, California 94720, United States

Department of Chemistry, University of California, Berkeley, University Avenue and Oxford St, Berkeley, California 94720, United States

Energy Technologies Area, Lawrence Berkeley National Laboratory, 1 Cyclotron Rd, Berkeley, California 94720, United States

Division of Chemistry and Chemical Engineering, California Institute of Technology, 1200 E California Blvd, Pasadena, California 91125, United States

Department of Chemistry, Department of Chemical & Biomolecular Engineering, and Department of Materials Science & Engineering

University of California Irvine

Funding

National Science Foundation Graduate Research Fellowship Program · Basic Energy Sciences · Advanced Research Projects Agency - Energy · National Defense Science and Engineering Graduate

References (60)

Show source-provided references
1. 10.1021/acsaem.0c0112710.1021/acsaem.0c01127 ↗
2. 10.1016/j.memsci.2022.12066010.1016/j.memsci.2022.120660 ↗
3. 10.1039/d1ta00747e10.1039/d1ta00747e ↗
4. 10.1021/acs.est.9b0502410.1021/acs.est.9b05024 ↗
5. 10.1021/acsenergylett.6b0031710.1021/acsenergylett.6b00317 ↗
6. 10.1038/s41467-020-18232-y10.1038/s41467-020-18232-y ↗
7. 10.1016/j.cclet.2022.10807510.1016/j.cclet.2022.108075 ↗
8. 10.1038/s41467-022-29791-710.1038/s41467-022-29791-7 ↗
9. 10.1016/j.isci.2022.10515310.1016/j.isci.2022.105153 ↗
10. Climate Change 2022: Mitigation of Climate Change . https://www.ipcc.ch/report/ar6/wg3/?itid=lk_inline_enhanced-template (accessed 2022-12-04).
11. 10.1126/science.abn795010.1126/science.abn7950 ↗
12. 10.1038/s41558-018-0091-310.1038/s41558-018-0091-3 ↗
13. 10.1021/acsenergylett.0c0207810.1021/acsenergylett.0c02078 ↗
14. 10.1039/C8SE00118A10.1039/C8SE00118A ↗
15. 10.1002/aenm.20160037910.1002/aenm.201600379 ↗
16. 10.1002/cssc.20140253510.1002/cssc.201402535 ↗
17. 10.1021/acsami.2c0768010.1021/acsami.2c07680 ↗
18. 10.3389/fenrg.2022.100168410.3389/fenrg.2022.1001684 ↗
19. 10.1002/cssc.20150053810.1002/cssc.201500538 ↗
20. 10.1039/D1EE03523A10.1039/D1EE03523A ↗
21. 10.1016/j.isci.2022.10399010.1016/j.isci.2022.103990 ↗
22. 10.1016/j.jclepro.2019.03.08610.1016/j.jclepro.2019.03.086 ↗
23. 10.2139/ssrn.428296910.2139/ssrn.4282969 ↗
24. 10.1021/acs.iecr.2c0088910.1021/acs.iecr.2c00889 ↗
25. 10.1021/acs.iecr.2c0088910.1021/acs.iecr.2c00889 ↗
26. 10.1021/acs.iecr.9b0564110.1021/acs.iecr.9b05641 ↗
27. 10.1016/j.memsci.2020.11853810.1016/j.memsci.2020.118538 ↗
28. 10.1021/acs.chemmater.0c0282910.1021/acs.chemmater.0c02829 ↗
29. 10.1016/j.joule.2021.06.01610.1016/j.joule.2021.06.016 ↗
30. 10.1038/s44286-023-00009-x10.1038/s44286-023-00009-x ↗
31. 10.1016/S0009-2614(98)00877-X10.1016/S0009-2614(98)00877-X ↗
32. 10.1016/S0032-3861(99)00886-110.1016/S0032-3861(99)00886-1 ↗
33. 10.1016/S0376-7388(96)00185-810.1016/S0376-7388(96)00185-8 ↗
34. 10.1021/acs.jpcc.1c0827610.1021/acs.jpcc.1c08276 ↗
35. 10.1016/0011-9164(96)00021-510.1016/0011-9164(96)00021-5 ↗
36. 10.1016/j.joule.2023.06.01110.1016/j.joule.2023.06.011 ↗
37. 10.1016/j.joule.2023.03.00510.1016/j.joule.2023.03.005 ↗
38. 10.1126/science.aaz148710.1126/science.aaz1487 ↗
39. 10.1039/C7EE00345E10.1039/C7EE00345E ↗
40. 10.1021/acsaem.9b0125710.1021/acsaem.9b01257 ↗
41. 10.1039/D1SE00201E10.1039/D1SE00201E ↗
42. 10.1021/acsami.0c1268610.1021/acsami.0c12686 ↗
43. 10.1021/acsaem.1c0015110.1021/acsaem.1c00151 ↗
44. 10.1021/acsami.1c1254410.1021/acsami.1c12544 ↗
45. 10.1039/C8EE01192C10.1039/C8EE01192C ↗
46. 10.1039/D3EE00885A10.1039/D3EE00885A ↗
47. 10.1021/jz300236w10.1021/jz300236w ↗
48. 10.1016/j.jcis.2016.01.01310.1016/j.jcis.2016.01.013 ↗
49. Ardo, S.; White, W.; Renna, L.; Bhide, R.; Schultz, L.; Phun, G. Membranes for Enhancing Rates of Water Dissociation and Water Formation. U.S. Patent WO 20210046423A1. February 18, 2021.
50. 10.1038/s41560-019-0372-810.1038/s41560-019-0372-8 ↗
51. 10.1021/am503242v10.1021/am503242v ↗
52. 10.1039/c1ee01336j10.1039/c1ee01336j ↗
53. 10.1016/j.memsci.2019.11768010.1016/j.memsci.2019.117680 ↗
54. 10.1016/j.memsci.2021.11999010.1016/j.memsci.2021.119990 ↗
55. 10.1039/C7RA00294G10.1039/C7RA00294G ↗
56. 10.1021/acs.langmuir.8b0234210.1021/acs.langmuir.8b02342 ↗
57. 10.1038/srep3383510.1038/srep33835 ↗
58. 10.1038/s41467-022-31429-710.1038/s41467-022-31429-7 ↗
59. 10.1021/acs.iecr.2c0088910.1021/acs.iecr.2c00889 ↗
60. Craig, N. P. Electrochemical Behavior of Bipolar Membranes, 2013. https://escholarship.org/uc/item/8058x81t (accessed 2022-12-28).