Acidic Hydrogen Evolution Electrocatalysis at High‐Entropy Alloys Correlates with its Composition‐Dependent Potential of Zero Charge
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The vast possibilities in the elemental combinations of high‐entropy alloys (HEAs) make it essential to discover activity descriptors for establishing rational electrocatalyst design principles. Despite the increasing attention on the potential of zero charge (PZC) of hydrogen evolution reaction (HER) electrocatalyst, neither the PZC of HEAs nor the impact of the PZC on the HER activity at HEAs has been described. Here, we use scanning electrochemical cell microscopy (SECCM) to determine the PZC and the HER activities of various elemental compositions of a Pt−Pd−Ru−Ir−Ag thin‐film HEA materials library (HEA‐ML) with high statistical reliability. Interestingly, the PZC of Pt−Pd−Ru−Ir−Ag is linearly correlated with its composition‐weighted average work function. The HER current density in acidic media positively correlates with the PZC, which can be explained by the preconcentration of H + in the electrical double layer at potentials negative of the PZC.
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The double-layer capacitance (Cdl) values present a positive correlation with the electrochemically active surface area (ECSA).
“Typically, the double-layer capacitance (Cdl) values present a positive correlation with the electrochemically active surface area (ECSA),[37,38]”
From Constructing Novel High‐Entropy Alloy Aerogels Platform for pH‐Universal Hydrogen Evolution Reaction with High Electrocatalytic Activity and Stability (2026) · cites this paper as [37]
The Introduction discusses using double-layer capacitance (Cdl) to determine the potential of zero charge, and the Pt/Au measurement section describes its potential dependence. Neither passage addresses a positive correlation between Cdl and electrochemically active surface area; searches for ECSA and surface-area proportionality found no such statement in our copy. (LLM, conf=0.73)
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Research works printed but not linked: 54
- G. Feng, F. Ning, J. Song, H. Shang, K. Zhang, Z. Ding, P. Gao, W. Chu, D. Xia, J. Am. Chem. Soc. 2021, 143, 17117- 17127. · DOI
- R. Q. Yao, Y.-T. Zhou, H. Shi, W.-B. Wan, Q.-H. Zhang, L. Gu, Y.-F. Zhu, Z. Wen, X.-Y. Lang, Q. Jiang, Adv. Funct. Mater. 2021, 31, 2009613. · DOI · Paper page
- T. Löffler, H. Meyer, A. Savan, P. Wilde, A. Garzón Manjón, Y.-T. Chen, E. Ventosa, C. Scheu, A. Ludwig, W. Schuhmann, Adv. Energy Mater. 2018, 8, 1802269. · DOI
- J. K. Pedersen, C. M. Clausen, O. A. Krysiak, B. Xiao, T. A. A. Batchelor, T. Löffler, V. A. Mints, L. Banko, M. Arenz, A. Savan, W. Schuhmann, A. Ludwig, J. Rossmeisl, Angew. Chem. Int. Ed. 2021, 60, 24144-24152. · DOI
- T. A. A. Batchelor, T. Löffler, B. Xiao, O. A. Krysiak, V. Strotkötter, J. K. Pedersen, C. M. Clausen, A. Savan, Y. Li, W. Schuhmann, J. Rossmeisl, A. Ludwig, Angew. Chem. Int. Ed. 2021, 60, 6932-6937. · DOI
- M. W. Glasscott, A. D. Pendergast, S. Goines, A. R. Bishop, A. T. Hoang, C. Renault, J. E. Dick, Nat. Commun. 2019, 10, 2650.
- Z.-J. Chen, T. Zhang, X.-Y. Gao, Y.-J. Huang, X.-H. Qin, Y.- F. Wang, K. Zhao, X. Peng, C. Zhang, L. Liu, M.-H. Zeng, H.- B. Yu, Adv. Mater. 2021, 33, 2101845. · DOI
- D. Wu, K. Kusada, T. Yamamoto, T. Toriyama, S. Matsumura, S. Kawaguchi, Y. Kubota, H. Kitagawa, J. Am. Chem. Soc. 2020, 142, 13833-13838. · DOI
- H. Li, Y. Han, H. Zhao, W. Qi, D. Zhang, Y. Yu, W. Cai, S. Li, J. Lai, B. Huang, L. Wang, Nat. Commun. 2020, 11, 5437.
- T. Löffler, A. Savan, A. Garzón-Manjón, M. Meischein, C. Scheu, A. Ludwig, W. Schuhmann, ACS Energy Lett. 2019, 4, 1206-1214. · DOI
- A. Goyal, M. T. M. Koper, Angew. Chem. Int. Ed. 2021, 60, 13452-13462. · DOI
- S. Ringe, C. G. Morales-Guio, L. D. Chen, M. Fields, T. F. Jaramillo, C. Hahn, K. Chan, Nat. Commun. 2020, 11, 33.
- S. Ringe, E. L. Clark, J. Resasco, A. Walton, B. Seger, A. T. Bell, K. Chan, Energy Environ. Sci. 2019, 12, 3001-3014. · DOI
- J. Resasco, L. D. Chen, E. Clark, C. Tsai, C. Hahn, T. F. Jaramillo, K. Chan, A. T. Bell, J. Am. Chem. Soc. 2017, 139, 11277-11287. · DOI
- I. Ledezma-Yanez, W. D. Z. Wallace, P. Sebastián-Pascual, V. Climent, J. M. Feliu, M. T. M. Koper, Nat. Energy 2017, 2, 17031.
- P. Li, Y. Jiang, Y. Hu, Y. Men, Y. Liu, W. Cai, S. Chen, Nat. Catal. 2022, 5, 900-911. · DOI · Paper page
- L. Rebollar, S. Intikhab, J. D. Snyder, M. H. Tang, J. Phys. Chem. Lett. 2020, 11, 2308-2313. · DOI
- K. Ojha, N. Arulmozhi, D. Aranzales, M. T. M. Koper, Angew. Chem. Int. Ed. 2020, 59, 711-715. · DOI
- K. Ojha, K. Doblhoff-Dier, M. T. M. Koper, Proc. Natl. Acad. Sci. USA 2022, 119, e2116016119.
- T. Pajkossy, D. M. Kolb, Electrochim. Acta 2001, 46, 3063- 3071. · DOI
- R. Martínez-Hincapié, V. Climent, J. M. Feliu, Curr. Opin. Electrochem. 2019, 14, 16-22. · DOI
- B. Garlyyev, S. Xue, S. Watzele, D. Scieszka, A. S. Bandar- enka, J. Phys. Chem. Lett. 2018, 9, 1927-1930. · DOI
- S. Xue, B. Garlyyev, A. Auer, J. Kunze-Liebhäuser, A. S. Bandarenka, J. Phys. Chem. C 2020, 124, 12442-12447. · DOI
- L. Banko, O. A. Krysiak, J. K. Pedersen, B. Xiao, A. Savan, T. Löffler, S. Baha, J. Rossmeisl, W. Schuhmann, A. Ludwig, Adv. Energy Mater. 2022, 12, 2103312. · DOI
- N. Ebejer, A. G. G¨uell, S. C. S. Lai, K. McKelvey, M. E. Snowden, P. R. Unwin, Annu. Rev. Anal. Chem. 2013, 6, 329- 351. · DOI
- C. L. Bentley, M. Kang, P. R. Unwin, Curr. Opin. Electrochem. 2017, 6, 23-30. · DOI
- O. J. Wahab, M. Kang, P. R. Unwin, Curr. Opin. Electrochem. 2020, 22, 120-128. · DOI
- Y. Wang, E. Gordon, H. Ren, Anal. Chem. 2020, 92, 2859- 2865. · DOI
- G. J. Clark, T. N. Andersen, R. S. Valentine, H. Eyring, J. Electrochem. Soc. 1974, 121, 618-622. · DOI
- B. B. Berkes, G. Inzelt, W. Schuhmann, A. S. Bondarenko, J. Phys. Chem. C 2012, 116, 10995-11003. · DOI
- R. Rizo, J. Fernández-Vidal, L. J. Hardwick, G. A. Attard, F. J. Vidal-Iglesias, V. Climent, E. Herrero, J. M. Feliu, Nat. Commun. 2022, 13, 2550.
- A. J. Bard, L. R. Faulkner, Electrochemical Methods: Funda- mentals and Applications, Wiley, New York, 2000.
- A. Makaraviciute, X. Xu, L. Nyholm, Z. Zhang, ACS Appl. Mater. Interfaces 2017, 9, 26610-26621. · DOI
- L. M. Fischer, M. Tenje, A. R. Heiskanen, N. Masuda, J. Castillo, A. Bentien, J. Émneus, M. H. Jakobsen, A. Boisen, Microelectron. Eng. 2009, 86, 1282-1285. · DOI
- S. Trasatti, J. Electroanal. Chem. 1971, 33, 351-378. · DOI
- P. Xu, A. D. von Rueden, R. Schimmenti, M. Mavrikakis, J. Suntivich, Nat. Mater. 2023, 22, 503-510. · DOI
- J. Huang, A. Malek, J. Zhang, M. H. Eikerling, J. Phys. Chem. C 2017, 121, 26140. · DOI
- U. W. Hamm, D. Kramer, R. S. Zhai, D. M. Kolb, J. Electroa- nal. Chem. 1996, 414, 85-89. · DOI
- A. Frumkin, B. Damaskin, N. Grigoryev, I. Bagotskaya, Electrochim. Acta 1974, 19, 69-74. · DOI
- O. A. Krysiak, S. Schumacher, A. Savan, W. Schuhmann, A. Ludwig, C. Andronescu, Nano Res. 2022, 15, 4780-4784. · DOI
- V. Strotkötter, O. A. Krysiak, J. Zhang, X. Wang, E. Suhr, W. Schuhmann, A. Ludwig, Chem. Mater. 2022, 34, 10291-10303. · DOI
- H. B. Michaelson, J. Appl. Phys. 1977, 48, 4729-4733. · DOI
- P. Li, J. Huang, Y. Hu, S. Chen, J. Phys. Chem. C 2021, 125, 3972-3979. · DOI
- X.-Y. Li, A. Chen, X.-H. Yang, J.-X. Zhu, J.-B. Le, J. Cheng, J. Phys. Chem. Lett. 2021, 12, 7299-7304. · DOI
- F. Gossenberger, T. Roman, K. Forster-Tonigold, A. Groß, Beilstein J. Nanotechnol. 2014, 5, 152-161. · DOI
- V. Briega-Martos, F. J. Sarabia, V. Climent, E. Herrero, J. M. Feliu, ACS Meas. Sci. Au 2021, 1, 48-55. · DOI
- L. J. T. Metzroth, E. M. Miller, A. G. Norman, S. Yazdi, G. M. Carroll, Nano Lett. 2021, 21, 9131-9137. · DOI
- C. Gabrielli, P. P. Grand, A. Lasia, H. Perrot, J. Electrochem. Soc. 2004, 151, A1937. · DOI
- A. Auer, F. J. Sarabia, D. Winkler, C. Griesser, V. Climent, J. M. Feliu, J. Kunze-Liebhäuser, ACS Catal. 2021, 11, 10324- 10332. · DOI
- F. J. Sarabia, P. Sebastián-Pascual, M. T. M. Koper, V. Cli- ment, J. M. Feliu, ACS Appl. Mater. Interfaces 2019, 11, 613- 623. · DOI
- X. Fu, J. Zhang, S. Zhan, F. Xia, C. Wang, D. Ma, Q. Yue, J. Wu, Y. Kang, ACS Catal. 2022, 12, 11955-11959. · DOI
- F. McKay, Y. Fang, O. Kizilkaya, P. Singh, D. D. Johnson, A. Roy, D. P. Young, P. T. Sprunger, J. C. Flake, W. A. Shelton, Y. Xu, J. Phys. Chem. C 2021, 125, 17008-17018. · DOI
- H. Ooka, J. Huang, K. S. Exner, Front. Energy Res. 2021, 9, 654460.
- J. N. Hansen, H. Prats, K. K. Toudahl, N. Mørch Secher, K. Chan, J. Kibsgaard, I. Chorkendorff, ACS Energy Lett. 2021, 6, 1175-1180. Manuscript received: July 14, 2023 Accepted manuscript online: August 3, 2023 Version of record online: August 17, 2023 · DOI · Paper page
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- Authors
- Kim, M., Batsa Tetteh, E., Krysiak, O. A., Savan, A., Xiao, B., Piotrowiak, T. H., Andronescu, C., Ludwig, A., Dong Chung, T., & Schuhmann, W.
- Affiliations
- Seoul National University (KR)
- Analytical Chemistry—Center for Electrochemical Sciences (CES) Faculty of Chemistry and Biochemistry Ruhr University Bochum Universitätsstr. 150 D-44780 Bochum Germany
- Ruhr University Bochum (DE)
- University of Duisburg-Essen (DE)
- Department of Chemistry Seoul National University Seoul 08826 Republic of Korea
- Corresponding author
- Schuhmann, Wolfgang
- ORCID
- Venue
- Angewandte Chemie International Edition
- Publisher
- Wiley
- Published
- 2023-08-17
- Volume
- 62
- Issue
- 39
- Pages
- e202310069-e202310069
- ISSN
- 1433-7851 (ISSN-L)
- 1521-3773
- OpenAlex
- W4385520936
- Cited by
- 63
- References
- 0
- Citations by year
- 2026: 19 · 2025: 25 · 2024: 19
- FWCI
- 3.01
- Type
- journal article
- Language
- en
- Open access
- hybrid
- doi.org
- Licence
- Locations
- Angewandte Chemie International Edition (publishedVersion, cc-by-nc-nd)
- PubMed (publishedVersion)
- Dokumentenrepositorium der RUB (Ruhr University Bochum) (submittedVersion, cc-by-nc-nd)
- Funders
- HORIZON EUROPE European Research Council (CasCat [833408])
- HORIZON EUROPE Marie Sklodowska-Curie Actions (Sentinel [812398])
- National Research Foundation of Korea (2021R1A5A1030054, 2022R1A2C3004327)
- Deutsche Forschungsgemeinschaft (LU1175/26-1, 440951282)
- Topics
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
- Physical Sciences › Engineering › Mechanical Engineering › High Entropy Alloys Studies
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
- Keywords
- high-entropy alloys, hydrogen evolution reaction, potential of zero charge, acidic electrocatalysis, work function, electric double layer, scanning electrochemical cell microscopy, electrocatalyst design
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