journal article·2025-09-12Open access

The Intricacies of Computational Electrochemistry

Nitish Govindarajan, Georg Kastlunger, Joseph A. Gauthier, Jun Cheng, Ivo Filot, Arthur Hagopian, Heine Anton Hansen, Jun Huang, Piotr M. Kowalski, Jinwen Liu, Juan M. Lombardi, Mikael Maraschin, Andrew Peterson, Hemanth S. Pillai, Hector Prats, Conor J. Price, René van Roij, Jan Rossmeisl, Ranga Rohit Seemakurthi, Seung-Jae Shin, Audrey Smith, Jia-Xin Zhu, Katharina Doblhoff-Dier

ACS Energy Letters· Volume 10· Issue 9

Abstract

Computational electrochemistry is hardanybody who has ever tried will know. We argue that the reasons for its complexity lie not only in the multiscale nature of electrochemical processes but also in the rapid, ongoing method development in the field. This has resulted in a lack of clear guidelines and many open discussions in the community. These issues were also the topic of a recent Lorentz Center workshop, the key take-away messages of which are highlighted in this Perspective. In particular, we discuss why the choice between constant potential and constant charge simulations is less trivial than it may seem, why interpreting electrochemical reaction free energy diagrams can be challenging, why the Poisson-Nernst-Planck equation is not all there is, and why we desperately need more benchmarking in the field.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Electrochemical Analysis and Applications · Electrocatalysts for Energy Conversion · Machine Learning in Materials Science

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

Affiliations

School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 21 Nanyang Link, Singapore, 637371 Singapore

Catalysis Theory Center, Department of Physics

Technical University of Denmark (DTU)

Department of Chemical Engineering

Texas Tech University

State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, College of Chemistry and Chemical Engineering

Xiamen University

Laboratory of AI for Electrochemistry (AI4EC)

IKKEM

Institute of Artificial Intelligence

Laboratory of Inorganic Materials and Catalysis, Department of Chemistry and Chemical Engineering

Eindhoven University of Technology

Leiden Institute of Chemistry

Leiden University

Department of Energy Conversion and Storage

Technical University of Denmark

Forschungszentrum Jülich GmbH, Institute of Energy Technologies, Theory and Computation of Energy Materials (IET-3), 52425 Jülich, Germany

Fritz-Haber-Institut der Max-Planck-Gesellschaft. Faradayweg 4-6, 14195 Berlin, Germany

School of Engineering, Brown University, Hope Street, Providence, Rhode Island 02912, United States

Department of Chemistry, Physical and Theoretical Chemistry Laboratory, University of Oxford, South Parks Road, Oxford OX1 3QZ, U.K.

Institute for Theoretical Physics, Utrecht University, Princetonplein 5, Utrecht 3584 CC, The Netherlands

Center for High Entropy Alloy Catalysis, Department of Chemistry

University of Copenhagen

Institute of Chemical Research of Catalonia (ICIQ-CERCA), The Barcelona Institute of Science and Technology, Av. Països Catalans 16, Tarragona 43007 Spain

School of Energy and Chemical Engineering

Funding

Danmarks Tekniske Universitet · Lorentz Center · Universiteit Leiden · Nederlandse Organisatie voor Wetenschappelijk Onderzoek · Software for Chemistry and Materials B.V.

References (100+)

Show source-provided references
1. Center for Scientific Workshops in All Disciplines - Multiscale Modeling of Electrochemical Processes. https://www.lorentzcenter.nl/multiscale-modeling-of-electrochemical-processes.html, Accessed: 2025-05-13.
2. 10.1016/j.jcat.2016.01.01010.1016/j.jcat.2016.01.010 ↗
3. 10.1016/j.jcat.2022.12.02510.1016/j.jcat.2022.12.025 ↗
4. 10.1021/acs.jpcc.1c0617010.1021/acs.jpcc.1c06170 ↗
5. 10.1039/C9CY02338K10.1039/C9CY02338K ↗
6. 10.1021/ja992723s10.1021/ja992723s ↗
7. 10.1103/PhysRevLett.83.181410.1103/PhysRevLett.83.1814 ↗
8. 10.1021/acscatal.9b0079610.1021/acscatal.9b00796 ↗
9. 10.1038/s41467-018-05544-310.1038/s41467-018-05544-3 ↗
10. 10.1002/cphc.20230095910.1002/cphc.202300959 ↗
11. 10.1016/0022-0728(93)80005-310.1016/0022-0728(93)80005-3 ↗
12. 10.1126/science.aaf505010.1126/science.aaf5050 ↗
13. 10.1016/j.electacta.2010.04.05510.1016/j.electacta.2010.04.055 ↗
14. 10.1016/j.electacta.2007.02.08210.1016/j.electacta.2007.02.082 ↗
15. 10.1039/b803956a10.1039/b803956a ↗
16. 10.1021/acs.jpclett.6b0125410.1021/acs.jpclett.6b01254 ↗
17. 10.1038/s41467-023-38758-110.1038/s41467-023-38758-1 ↗
18. 10.1021/jp047349j10.1021/jp047349j ↗
19. 10.1246/bcsj.64.12310.1246/bcsj.64.123 ↗
20. 10.1002/anie.20210280310.1002/anie.202102803 ↗
21. 10.1039/D1SC04775B10.1039/D1SC04775B ↗
22. 10.1021/acsenergylett.2c0250010.1021/acsenergylett.2c02500 ↗
23. 10.1021/acsenergylett.4c0189710.1021/acsenergylett.4c01897 ↗
24. 10.1038/s41467-022-33199-810.1038/s41467-022-33199-8 ↗
25. 10.1021/acscatal.9b0279910.1021/acscatal.9b02799 ↗
26. 10.1103/PhysRevLett.131.23800310.1103/PhysRevLett.131.238003 ↗
27. 10.1021/acs.jpcc.8b0246510.1021/acs.jpcc.8b02465 ↗
28. 10.1063/5.017630810.1063/5.0176308 ↗
29. 10.1063/1.505458010.1063/1.5054580 ↗
30. 10.1016/j.softx.2017.10.00610.1016/j.softx.2017.10.006 ↗
31. 10.1063/5.017630810.1063/5.0176308 ↗
32. 10.1021/acs.jpclett.2c0358810.1021/acs.jpclett.2c03588 ↗
33. 10.1002/cphc.20230095010.1002/cphc.202300950 ↗
34. 10.1021/acs.jpcc.3c0795410.1021/acs.jpcc.3c07954 ↗
35. 10.1063/5.013819710.1063/5.0138197 ↗
36. 10.1016/j.electacta.2024.14465910.1016/j.electacta.2024.144659 ↗
37. 10.1063/1.500302210.1063/1.5003022 ↗
38. 10.1063/1.311963910.1063/1.3119639 ↗
39. 10.1016/j.electacta.2023.14209510.1016/j.electacta.2023.142095 ↗
40. 10.1103/PhysRevB.96.11542910.1103/PhysRevB.96.115429 ↗
41. 10.1021/acs.jctc.2c0095910.1021/acs.jctc.2c00959 ↗
42. 10.1103/PhysRevLett.126.13680310.1103/PhysRevLett.126.136803 ↗
43. 10.3389/fenrg.2022.109619010.3389/fenrg.2022.1096190 ↗
44. 10.1088/1361-648X/ac1aa210.1088/1361-648X/ac1aa2 ↗
45. 10.1063/1.497697110.1063/1.4976971 ↗
46. 10.1021/acs.jpclett.6b0035810.1021/acs.jpclett.6b00358 ↗
47. 10.1021/acscatal.8b0279310.1021/acscatal.8b02793 ↗
48. 10.1021/jacs.1c0218610.1021/jacs.1c02186 ↗
49. 10.1021/acs.jctc.5c0040610.1021/acs.jctc.5c00406 ↗
50. 10.1039/D1SC00354B10.1039/D1SC00354B ↗
51. 10.1002/cphc.20190053610.1002/cphc.201900536 ↗
52. 10.1021/acscatal.1c0552010.1021/acscatal.1c05520 ↗
53. 10.1126/sciadv.abb121910.1126/sciadv.abb1219 ↗
54. 10.1021/jacsau.1c0010810.1021/jacsau.1c00108 ↗
55. 10.1021/acs.jctc.8b0117410.1021/acs.jctc.8b01174 ↗
56. 10.1021/acs.jctc.9b0071710.1021/acs.jctc.9b00717 ↗
57. 10.1021/acs.jpclett.5b0104310.1021/acs.jpclett.5b01043 ↗
58. 10.1021/ar500268y10.1021/ar500268y ↗
59. 10.1063/5.012365610.1063/5.0123656 ↗
60. 10.1021/acscatal.9b0026810.1021/acscatal.9b00268 ↗
61. 10.1038/ncomms1543810.1038/ncomms15438 ↗
62. 10.1038/s41467-018-07970-910.1038/s41467-018-07970-9 ↗
63. 10.1021/jp410060810.1021/jp4100608 ↗
64. 10.1021/acscatal.4c0441310.1021/acscatal.4c04413 ↗
65. 10.1021/acscatal.3c0022810.1021/acscatal.3c00228 ↗
66. 10.1515/pac-2014-502610.1515/pac-2014-5026 ↗
67. 10.1016/j.cattod.2012.05.04410.1016/j.cattod.2012.05.044 ↗
68. 10.1021/acs.jpclett.2c0136710.1021/acs.jpclett.2c01367 ↗
69. 10.1002/anie.20221647710.1002/anie.202216477 ↗
70. 10.1016/j.jcat.2021.08.04310.1016/j.jcat.2021.08.043 ↗
71. 10.1021/acs.jpcc.9b0383010.1021/acs.jpcc.9b03830 ↗
72. 10.1038/s41565-021-00974-510.1038/s41565-021-00974-5 ↗
73. 10.1016/j.joule.2022.01.00710.1016/j.joule.2022.01.007 ↗
74. 10.1149/1.277969210.1149/1.2779692 ↗
75. 10.1039/C9EE02697E10.1039/C9EE02697E ↗
76. 10.1021/acscatal.1c0132510.1021/acscatal.1c01325 ↗
77. 10.1016/j.electacta.2024.14427010.1016/j.electacta.2024.144270 ↗
78. 10.1021/jp970284i10.1021/jp970284i ↗
79. 10.1016/j.joule.2023.05.00710.1016/j.joule.2023.05.007 ↗
80. 10.1126/science.adh435510.1126/science.adh4355 ↗
81. 10.1039/D2CP04424B10.1039/D2CP04424B ↗
82. 10.3389/fchem.2019.0020210.3389/fchem.2019.00202 ↗
83. 10.1063/5.008325110.1063/5.0083251 ↗
84. 10.1039/C9EE02485A10.1039/C9EE02485A ↗
85. 10.1038/s41467-019-13777-z10.1038/s41467-019-13777-z ↗
86. 10.1103/PRXEnergy.2.03301010.1103/PRXEnergy.2.033010 ↗
87. 10.1126/science.125379310.1126/science.1253793 ↗
88. 10.1103/PhysRevLett.120.26450210.1103/PhysRevLett.120.264502 ↗
89. 10.1038/s41467-021-24270-x10.1038/s41467-021-24270-x ↗
90. 10.1073/pnas.172198711510.1073/pnas.1721987115 ↗
91. 10.1063/5.011303510.1063/5.0113035 ↗
92. 10.1103/PhysRevResearch.7.01332810.1103/PhysRevResearch.7.013328 ↗
93. 10.1016/j.coelec.2023.10125810.1016/j.coelec.2023.101258 ↗
94. 10.1021/acs.jpcc.1c0489510.1021/acs.jpcc.1c04895 ↗
95. 10.1021/acs.jpclett.2c0023010.1021/acs.jpclett.2c00230 ↗
96. 10.1039/D3EY00126A10.1039/D3EY00126A ↗
97. 10.1039/C6FD00144K10.1039/C6FD00144K ↗
98. 10.1149/1945-7111/ac315910.1149/1945-7111/ac3159 ↗
99. 10.1016/j.jpowsour.2023.23327310.1016/j.jpowsour.2023.233273 ↗
100. 10.1016/j.jpowsour.2024.23420910.1016/j.jpowsour.2024.234209 ↗