CoChat
Sign Up
Cited by 146Electrocatalysts for Energy ConversionCatalytic Processes in Materials ScienceFuel Cells and Related Materials

Pt Single Atom Electrocatalysts at Graphene Edges for Efficient Alkaline Hydrogen Evolution

Open access
Tsounis, Constantine, Subhash, Bijil, Kumar, Priyank V., Bedford, Nicholas M., Zhao, Yufei, Shenoy, Joel, Ma, Zhipeng, Zhang, Ding +7 more·2022·Advanced Functional Materials
DOI 10.1002/adfm.202203067
Open this paper in CoChat — free accountOpen PDF

Abstract

Graphene edges exhibit a highly localized density of states that result in increased reactivity compared to its basal plane. However, exploiting this increased reactivity to anchor and tune the electronic states of single atom catalysts (SACs) remains elusive. To investigate this, a method to anchor Pt SACs with ultra‐low mass loadings at the edges of edge‐rich vertically aligned graphene (as low as 0.71 µg Pt cm–2) is developed. Angle‐dependent X‐ray absorption spectroscopy and density‐functional theory calculations reveal that edge‐anchored Pt SACs has a robust coupling with the π‐electrons of graphene. This interaction results in a higher occupancy of the Pt 5d orbital, shifting the d‐band center toward the Fermi level, improving the adsorption of *H for the hydrogen evolution reaction (HER). Pt primarily coordinated to the graphene edge shows improved alkaline HER performance compared to Pt coordinated in mixed environments (turnover frequencies of 22.6 and 10.9 s–1 at an overpotential of 150 mV, respectively). This work demonstrates an effective route to engineering the coordination environment of Pt SACs by using the graphene edge for enhanced energy conversion reactions.

The claims and statistics of this paper haven’t been checked yet.

Run the check — free, no account needed. It reads the open-access text and checks the sources it cites.

A few free checks a day · papers already verified open instantly · results are public

Integrity signals

Registry

Crossref · 10.1002/adfm.202203067

Cites

3 of 3 references verified0 citation errors · 0 not checkable

Statistics

Claims the paper makes

The claims and statistics of this paper haven’t been checked yet.

Run the check — free, no account needed. It reads the open-access text and checks the sources it cites.

A few free checks a day · papers already verified open instantly · results are public

Claims other papers make about this one

Each is checked against this paper’s own text: does it say what the citing paper says it does?

  • The anchoring of Pt onto GA through O-Pt interactions can be confirmed by the appearance of component peaks in the resolved O 1s spectra of Pt-GA-x.

    “Moreover, the anchoring of Pt onto GA through O-Pt interactions can be confirmed by the appearance of component peaks in the resolved O 1s spectra of Pt-GA-x (Fig. 3c) [38, 39].”

    From Synergistic interaction of monodisperse Pt nanoparticles with defect‐rich graphene aerogel for efficient acidic hydrogen evolution (2025) · cites this paper as [39]

    Section 2.1 reports Pt anchored on graphene and identifies a mixture of Pt–O and Pt–C coordination by EXAFS. Section 2.3 describes oxygen-bridge interactions as likely, but the paper studies Pt/VG Ar samples, not Pt-GA-x, and does not confirm anchoring from resolved O 1s component peaks. Its reported XPS peaks are Pt 4f peaks. (LLM, conf=0.86)

    Experimental — accuracy not yet measured

Self-check

Percentages, sums and reported differences re-computed from the paper’s own numbers.

The self-check needs the paper’s full text.

Cites

Flagged first, then by citations

Research works printed but not linked: 49

  1. R. Daiyan, I. MacGill, R. Amal, ACS Energy Lett. 2020, 5, 3843.
  2. K. L. Zhou, Z. Wang, C. B. Han, X. Ke, C. Wang, Y. Jin, Q. Zhang, J. Liu, H. Wang, H. Yan, Nat. Commun. 2021, 12, 3783.
  3. I. Vincent, A. Kruger, D. Bessarabov, Int. J. Hydrogen Energy 2017, 42, 10752.
  4. J. N. Hansen, H. Prats, K. K. Toudahl, N. M. Secher, K. Chan, J. Kibsgaard, I. Chorkendorff, ACS Energy Lett. 2021, 6, 1175.
  5. W. Sheng, M. Myint, J. G. Chen, Y. Yan, Energy Environ. Sci. 2013, 6, 1509.
  6. C. C. L. McCrory, S. Jung, I. M. Ferrer, S. M. Chatman, J. C. Peters, T. F. Jaramillo, J. Am. Chem. Soc. 2015, 137, 4347.
  7. J. Kibsgaard, I. Chorkendorff, Nat. Energy 2019, 4, 430.
  8. X.-P. Yin, H.-J. Wang, S.-F. Tang, X.-L. Lu, M. Shu, R. Si, T.-B. Lu, Angew. Chem., Int. Ed. 2018, 57, 9382.
  9. D. Liu, X. Li, S. Chen, H. Yan, C. Wang, C. Wu, Y. A. Haleem, S. Duan, J. Lu, B. Ge, P. M. Ajayan, Y. Luo, J. Jiang, L. Song, Nat. Energy 2019, 4, 512.
  10. F. Abild-Pedersen, J. Greeley, F. Studt, J. Rossmeisl, T. R. Munter, P. G. Moses, E. Skúlason, T. Bligaard, J. K. Nørskov, Phys. Rev. Lett. 2007, 99, 016105.
  11. W. Sheng, H. A. Gasteiger, Y. Shao-Horn, J. Electrochem. Soc. 2010, 157, B1529.
  12. I. Ledezma-Yanez, W. D. Z. Wallace, P. Sebastián-Pascual, V. Climent, J. M. Feliu, M. T. M. Koper, Nat. Energy 2017, 2, 17031.
  13. B. Hammer, J. K. Norskov, Nature 1995, 376, 238.
  14. Q. Cheng, C. Hu, G. Wang, Z. Zou, H. Yang, L. Dai, J. Am. Chem. Soc. 2020, 142, 5594.
  15. J. Li, Y. Zhou, W. Tang, J. Zheng, X. Gao, N. Wang, X. Chen, M. Wei, X. Xiao, W. Chu, Appl. Catal., B 2021, 285, 119861.
  16. Y. Cheng, S. Zhao, H. Li, S. He, J.-P. Veder, B. Johannessen, J. Xiao, S. Lu, J. Pan, M. F. Chisholm, S.-Z. Yang, C. Liu, J. G. Chen, S. P. Jiang, Appl. Catal., B 2019, 243, 294.
  17. T. Sun, W. Zang, H. Yan, J. Li, Z. Zhang, Y. Bu, W. Chen, J. Wang, J. Lu, C. Su, ACS Catal. 2021, 11, 4498.
  18. J. Ge, D. Zhang, Y. Qin, T. Dou, M. Jiang, F. Zhang, X. Lei, Appl. Catal., B 2021, 298, 120557.
  19. Z. Xiang, Q. Dai, J.-F. Chen, L. Dai, Adv. Mater. 2016, 28, 6253.
  20. A. Shen, Y. Zou, Q. Wang, R. A. W. Dryfe, X. Huang, S. Dou, L. Dai, S. Wang, Angew. Chem., Int. Ed. 2014, 53, 10804.
  21. Y. Kobayashi, K.-i. Fukui, T. Enoki, K. Kusakabe, Phys. Rev. B 2006, 73, 125415.
  22. S. Fujii, M. Ziatdinov, M. Ohtsuka, K. Kusakabe, M. Kiguchi, T. Enoki, Faraday Discuss. 2014, 173, 173.
  23. K. Nakada, M. Fujita, G. Dresselhaus, M. S. Dresselhaus, Phys. Rev. B 1996, 54, 17954.
  24. C. Tsounis, X. Lu, N. M. Bedford, B. Subhash, L. Thomsen, Q. Zhang, Z. Ma, K. Ostrikov, A. Bendavid, J. A. Scott, R. Amal, Z. Han, ACS Nano 2020, 14, 11327.
  25. Z. Ma, C. Tsounis, P. V. Kumar, Z. Han, R. J. Wong, C. Y. Toe, S. Zhou, N. M. Bedford, L. Thomsen, Y. H. Ng, R. Amal, Adv. Funct. Mater. 2020, 30, 1910118.
  26. Z. J. Han, S. Pineda, A. T. Murdock, D. H. Seo, K. Ostrikov, A. Bendavid, J. Mater. Chem. A 2017, 5, 17293.
  27. P. Ahlberg, F. O. L. Johansson, Z.-B. Zhang, U. Jansson, S.-L. Zhang, A. Lindblad, T. Nyberg, APL Mater. 2016, 4, 046104.
  28. Y. Kobayashi, K.-i. Fukui, T. Enoki, K. Kusakabe, Y. Kaburagi, Phys. Rev. B 2005, 71, 193406.
  29. S. Fang, X. Zhu, X. Liu, J. Gu, W. Liu, D. Wang, W. Zhang, Y. Lin, J. Lu, S. Wei, Y. Li, T. Yao, Nat. Commun. 2020, 11, 1029.
  30. K. Yamazaki, Y. Maehara, C.-C. Lee, J. Yoshinobu, T. Ozaki, K. Gohara, J. Phys. Chem. C 2018, 122, 27292.
  31. F. Jiang, C. Li, H. Fu, X. Guo, G. Wu, S. Chen, Phys. Chem. Chem. Phys. 2016, 18, 19259.
  32. J. Y. Howe, C. J. Rawn, L. E. Jones, H. Ow, Powder Diffr. 2003, 18, 150.
  33. A. C. Ferrari, D. M. Basko, Nat. Nanotechnol. 2013, 8, 235.
  34. R. Garg, S. K. Rastogi, M. Lamparski, S. C. de la Barrera, G. T. Pace, N. T. Nuhfer, B. M. Hunt, V. Meunier, T. Cohen-Karni, ACS Nano 2017, 11, 6301.
  35. C. Casiraghi, A. Hartschuh, H. Qian, S. Piscanec, C. Georgi, A. Fasoli, K. S. Novoselov, D. M. Basko, A. C. Ferrari, Nano Lett. 2009, 9, 1433.
  36. M. Pan, E. C. Girão, X. Jia, S. Bhaviripudi, Q. Li, J. Kong, V. Meunier, M. S. Dresselhaus, Nano Lett. 2012, 12, 1928.
  37. D. Zhang, C. Tsounis, Z. Ma, D. Djaidiguna, N. M. Bedford, L. Thomsen, X. Lu, D. Chu, R. Amal, Z. Han, Small 2021, 18, 2105082.
  38. X. Zhang, T. Schiros, D. Nordlund, Y. C. Shin, J. Kong, M. Dresselhaus, T. Palacios, Adv. Funct. Mater. 2015, 25, 4163.
  39. V. Lee, R. V. Dennis, B. J. Schultz, C. Jaye, D. A. Fischer, S. Banerjee, J. Phys. Chem. C 2012, 116, 20591.
  40. A. M. Shikin, A. G. Rybkin, D. Marchenko, A. A. Rybkina, M. R. Scholz, O. Rader, A. Varykhalov, New J. Phys. 2013, 15, 013016.
  41. B. Hwang, J. Hwang, J. K. Yoon, S. Lim, S. Kim, M. Lee, J. H. Kwon, H. Baek, D. Sung, G. Kim, S. Hong, J. Ihm, J. A. Stroscio, Y. Kuk, Sci. Rep. 2016, 6, 31160.
  42. Y. Y. Li, M. X. Chen, M. Weinert, L. Li, 2D Mater. 2019, 6, 025038.
  43. J. Wang, F. Xu, H. Jin, Y. Chen, Y. Wang, Adv. Mater. 2017, 29, 1605838.
  44. C. Wei, R. R. Rao, J. Peng, B. Huang, I. E. L. Stephens, M. Risch, Z. J. Xu, Y. Shao-Horn, Adv. Mater. 2019, 31, 1806296.
  45. F. D. Speck, M. T. Y. Paul, F. Ruiz-Zepeda, M. Gatalo, H. Kim, H. C. Kwon, K. J. J. Mayrhofer, M. Choi, C. H. Choi, N. Hodnik, S. Cherevko, J. Am. Chem. Soc. 2020, 142, 15496.
  46. J. Greeley, T. F. Jaramillo, J. Bonde, I. Chorkendorff, J. K. Nørskov, Nat. Mater. 2006, 5, 909.
  47. T. Kondo, Y. Iwasaki, Y. Honma, Y. Takagi, S. Okada, J. Nakamura, Phys. Rev. B 2009, 80, 233408.
  48. J. K. Nørskov, F. Abild-Pedersen, F. Studt, T. Bligaard, Proc. Natl. Acad. Sci. USA 2011, 108, 937.
  49. E. Gann, C. R. McNeill, A. Tadich, B. C. C. Cowie, L. Thomsen, J. Synchrotron Radiat. 2016, 23, 374.

Cited by

Sorted by citations

Authors
Tsounis, C., Subhash, B., Kumar, P. V., Bedford, N. M., Zhao, Y., Shenoy, J., Ma, Z., Zhang, D., Toe, C. Y., Cheong, S., Tilley, R. D., Lu, X., Dai, L., Han, Z., & Amal, R.
Affiliations
  • Commonwealth Scientific and Industrial Research Organisation (AU)
  • UNSW Sydney (AU)
Corresponding author
  • Han, Zhaojun
  • Amal, Rose
ORCID
Venue
Advanced Functional Materials
Publisher
Wiley
Published
2022-07-10
Volume
32
Issue
38
ISSN
  • 1616-301X (ISSN-L)
  • 1616-3028
DOI
10.1002/adfm.202203067
OpenAlex
W4284989416
Cited by
146
References
3
Citations by year
2026: 21 · 2025: 46 · 2024: 47 · 2023: 29 · 2022: 3
FWCI
5.63
Type
journal article
Language
en
Open access
Licence
Locations
Advanced Functional Materials (publishedVersion, cc-by-nc)
Funders
  • U.S. Department of Energy (DE‐ AC02‐06CH11357, AC02‐06CH11357, 06CH11357, DE-AC02-)
  • Australian Nuclear Science and Technology Organisation
  • Analytical Center for the Government of the Russian Federation
  • Australian Institute of Nuclear Science and Engineering
  • Australian Synchrotron
  • University of New South Wales
  • University of Wollongong
  • Office of Science (AC02‐06CH11357, DE-AC02, 06CH11357, DE-AC02-06CH11357)
  • Australian Research Council (IC200100023)
  • Division of Materials Research (DE-AC02-06CH11357)
  • Argonne National Laboratory (DE- AC02-06-CH11357, DE-AC02, AC02–06CH11357, 06CH11357)
Topics
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
  • Physical Sciences › Materials Science › Materials Chemistry › Catalytic Processes in Materials Science
  • Physical Sciences › Engineering › Electrical and Electronic Engineering › Fuel Cells and Related Materials
Keywords
platinum single-atom catalysts, graphene edges, alkaline hydrogen evolution reaction, vertically aligned graphene, d-band center, hydrogen adsorption, coordination environment engineering, density of states

About these checks

Registry, retraction, Cites and statistics results are computed, not judged, with one exception: a printed reference that no index lists is read once by a model before it counts as a citation error. Claims are extracted by a model and kept only when their quote appears verbatim in the text; each cited source is then checked, with a model’s help, for whether it says what the claim relies on. Those verdicts can be wrong — read the claim’s quote and the cited source before relying on one.

Statistics and arithmetic are recomputed, not judged.

Confidence bands are shown only for fields calibrated on our annotated test set. None is calibrated yet, so no band is shown.

What counts as a claim ›How we measure confidence ›How we check this ›

Are you an author, or do you see a problem with this page? Request a review