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Communication

Engineering the high-entropy phase of Pt-Au-Cu nanowire for electrocatalytic hydrogen evolution

Yanan Yu1,§, Guangdong Liu2,§, Shuaihu Jiang1,§, Ruya Zhang1, Huiqiu Deng2, Eric A. Stach3, Shujuan Bao4, Zhenhua Zeng5( ), Yijin Kang1( )
Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
School of Physics and Electronics, Hunan University, Changsha 410082, China
Department of Materials Science and Engineering, University of Pennsylvania, Philadelphia, PA 19104, USA
Institute for Clean Energy & Advanced Materials, School of Materials and Energy, Southwest University, Chongqing 400715, China
Davidson School of Chemical Engineering, Purdue University, West Lafayette, IN 47907, USA

§ Yanan Yu, Guangdong Liu, and Shuaihu Jiang contributed equally to this work.

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Graphical Abstract

Alloy phase Pt-Au-Cu was identified as one of the most promising electrocatalysts for hydrogen evolution reaction. However, electrocatalyst with such phase was not available due to the competition of phase segregation in synthesis, until now.

Abstract

Hydrogen economy, as the most promising alternative energy system, relies on the hydrogen production through sustainable water splitting which in turn relies on the high efficiency electrocatalysts. PtAuCu A1-phase alloy has been predicted to be a promising electrocatalyst for the hydrogen evolution. As such preferred phase of Pt-Au-Cu is not thermodynamically favored, herein, we stabilize PtAuCu alloy by engineering the high-entropy phase in the form of nanowire. Density functional theory (DFT) calculations indicate that, in comparison with the ordered phase and segregated phases with discrete hydrogen binding energy, the high-entropy phase provides a diverse combination of site composition to continuously tune the hydrogen binding energy, and thus generate a series of highly active sites for the hydrogen evolution. Reflecting the theoretical prediction, electrochemical tests show that the A1-phase PtAuCu nanowire significantly outperforms its nanoparticle counterpart with phase segregation, toward the electrocatalysis of hydrogen evolution, offering one of the best hydrogen evolution electrocatalysts.

Keywords

hydrogen evolution reactionphase engineeringhigh entropy alloys

Electronic Supplementary Material

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References

[1]

Vesborg, P. C. K.; Seger, B.; Chorkendorff, I. Recent development in hydrogen evolution reaction catalysts and their practical implementation. J. Phys. Chem. Lett. 2015, 6, 951–957.
Crossref Google Scholar
[2]

Li, Y. J.; Sun, Y. J.; Qin, Y. N.; Zhang, W. Y.; Wang, L.; Luo, M. C.; Yang, H.; Guo, S. J. Recent advances on water-splitting electrocatalysis mediated by noble-metal-based nanostructured materials. Adv. Energy Mater. 2020, 10, 1903120.
Crossref Google Scholar
[3]

Subbaraman, R.; Tripkovic, D.; Strmcnik, D.; Chang, K. C.; Uchimura, M.; Paulikas, A. P.; Stamenkovic, V.; Markovic, N. M. Enhancing hydrogen evolution activity in water splitting by tailoring Li+-Ni(OH)2-Pt interfaces. Science 2011, 334, 1256–1260.
Crossref Google Scholar
[4]

Yao, Y. G.; Huang, Z. N.; Xie, P. F.; Lacey, S. D.; Jacob, R. J.; Xie, H.; Chen, F. J.; Nie, A. M.; Pu, T. C.; Rehwoldt, M. et al. Carbothermal shock synthesis of high-entropy-alloy nanoparticles. Science 2018, 359, 1489–1494.
Crossref Google Scholar
[5]

Yang, T. T.; Zhu, H.; Wan, M.; Dong, L.; Zhang, M.; Du, M. L. Highly efficient and durable PtCo alloy nanoparticles encapsulated in carbon nanofibers for electrochemical hydrogen generation. Chem. Commun. 2016, 52, 990–993.
Crossref Google Scholar
[6]

Greeley, J.; Jaramillo, T. F.; Bonde, J.; Chorkendorff, I.; Nørskov, J. K. Computational high-throughput screening of electrocatalytic materials for hydrogen evolution. Nat. Mater. 2006, 5, 909–913.
Crossref Google Scholar
[7]

Sheng, W. C.; Myint, M.; Chen, J. G.; Yan, Y. S. Correlating the hydrogen evolution reaction activity in alkaline electrolytes with the hydrogen binding energy on monometallic surfaces. Energy Environ. Sci. 2013, 6, 1509–1512.
Crossref Google Scholar
[8]

Danilovic, N.; Subbaraman, R.; Strmcnik, D.; Chang, K. C.; Paulikas, A. P.; Stamenkovic, V. R.; Markovic, N. M. Enhancing the alkaline hydrogen evolution reaction activity through the bifunctionality of Ni(OH)2/metal catalysts. Angew. Chem. 2012, 124, 12663–12666.
Crossref Google Scholar
[9]

Intikhab, S.; Snyder, J. D.; Tang, M. H. Adsorbed hydroxide does not participate in the volmer step of alkaline hydrogen electrocatalysis. ACS Catal. 2017, 7, 8314–8319.
Crossref Google Scholar
[10]

Wang, T.; Guo, Y. R.; Zhou, Z. X.; Chang, X. H.; Zheng, J.; Li, X. G. Ni-Mo nanocatalysts on N-doped graphite nanotubes for highly efficient electrochemical hydrogen evolution in acid. ACS Nano 2016, 10, 10397–10403.
Crossref Google Scholar
[11]

Wang, H. P.; Li, X. B.; Gao, L.; Wu, H. L.; Yang, J.; Cai, L.; Ma, T. B.; Tung, C. H.; Wu, L. Z.; Yu, G. Three-dimensional graphene networks with abundant sharp edge sites for efficient electrocatalytic hydrogen evolution. Angew. Chem., Int. Ed. 2018, 57, 192–197.
Crossref Google Scholar
[12]

Wang, X. S.; Zhu, Y. H.; Vasileff, A.; Jiao, Y.; Chen, S. M.; Song, L.; Zheng, B.; Zheng, Y.; Qiao, S. Z. Strain effect in bimetallic electrocatalysts in the hydrogen evolution reaction. ACS Energy Lett. 2018, 3, 1198–1204.
Crossref Google Scholar
[13]

Wang, D. L.; Xin, H. L.; Hovden, R.; Wang, H. S.; Yu, Y. C.; Muller, D. A.; DiSalvo, F. J.; Abruña, H. D. Structurally ordered intermetallic platinum-cobalt core–shell nanoparticles with enhanced activity and stability as oxygen reduction electrocatalysts. Nat. Mater. 2013, 12, 81–87.
Crossref Google Scholar
[14]

Jiang, B. B.; Tang, Z. Y.; Liao, F.; Lin, H. P.; Lu, S. K.; Li, Y. Y.; Shao, M. W. Powerful synergy: Efficient Pt-Au-Si nanocomposites as state-of-the-art catalysts for electrochemical hydrogen evolution. J. Mater. Chem. A 2017, 5, 21903–21908.
Crossref Google Scholar
[15]

Cao, Z. M.; Chen, Q. L.; Zhang, J. W.; Li, H. Q.; Jiang, Y. Q.; Shen, S. Y.; Fu, G.; Lu, B. A.; Xie, Z. X.; Zheng, L. S. Platinum-nickel alloy excavated nano-multipods with hexagonal close-packed structure and superior activity towards hydrogen evolution reaction. Nat. Commun. 2017, 8, 15131.
Crossref Google Scholar
[16]

Shen, Y.; Zhou, Y. F.; Wang, D.; Wu, X.; Li, J.; Xi, J. Y. Nickel-copper alloy encapsulated in graphitic carbon shells as electrocatalysts for hydrogen evolution reaction. Adv. Energy Mater. 2018, 8, 1701759.
Crossref Google Scholar
[17]

Wei, M.; Huang, L.; Huang, S. L.; Chen, Z. Y.; Lyu, D.; Zhang, X. R.; Wang, S. B.; Tian, Z. Q.; Shen, P. K. Highly efficient Pt-Co alloy hollow spheres with ultra-thin shells synthesized via Co-B-O complex as intermediates for hydrogen evolution reaction. J. Catal. 2020, 381, 385–394.
Crossref Google Scholar
[18]

Huang, L. L.; Chen, P. C.; Liu, M. H.; Fu, X. B.; Gordiichuk, P.; Yu, Y. N.; Wolverton, C.; Kang, Y. J.; Mirkin, C. A. Catalyst design by scanning probe block copolymer lithography. Proc. Natl. Acad. Sci. USA 2018, 115, 3764–3769.
Crossref Google Scholar
[19]

Chen, Y.; Lai, Z. C.; Zhang, X.; Fan, Z. X.; He, Q. Y.; Tan, C. L.; Zhang, H. Phase engineering of nanomaterials. Nat. Rev. Chem. 2020, 4, 243–256.
Crossref Google Scholar
[20]

Cheng, H. F.; Yang, N. L.; Lu, Q. P.; Zhang, Z. C.; Zhang, H. Syntheses and properties of metal nanomaterials with novel crystal phases. Adv. Mater. 2018, 30, 1707189.
Crossref Google Scholar
[21]

Wang, J. L.; Wei, Y.; Li, H.; Huang, X.; Zhang, H. Crystal phase control in two-dimensional materials. Sci. China Chem. 2018, 61, 1227–1242.
Crossref Google Scholar
[22]

Chen, P. C.; Du, J. S.; Meckes, B.; Huang, L. L.; Xie, Z.; Hedrick, J. L.; Dravid, V. P.; Mirkin, C. A. Structural evolution of three-component nanoparticles in polymer nanoreactors. J. Am. Chem. Soc. 2017, 139, 9876–9884.
Crossref Google Scholar
[23]

Ye, Y. F.; Wang, Q.; Lu, J.; Liu, C. T.; Yang, Y. High-entropy alloy: Challenges and prospects. Mater. Today 2016, 19, 349–362.
Crossref Google Scholar
[24]

Aikens, D. A. Electrochemical methods, fundamentals and applications. J. Chem. Educ. 1983, 60, A25.
Crossref Google Scholar
[25]

Holze, R. Book review: Electrochemical methods. fundamentals and applications (2nd edition). By Allen J. Bard and Larry R. Faulkner. Angew. Chem., Int. Ed. 2002, 41, 655–657.
Crossref Google Scholar
[26]

Chen, C.; Kang, Y. J.; Huo, Z. Y.; Zhu, Z. W.; Huang, W. Y.; Xin, H. L.; Snyder, J. D.; Li, D. G.; Herron, J. A.; Mavrikakis, M. et al. Highly crystalline multimetallic nanoframes with three-dimensional electrocatalytic surfaces. Science 2014, 343, 1339–1343.
Crossref Google Scholar
[27]

Lombardo, D.; Calandra, P.; Pasqua, L.; Magazù, S. Self-assembly of organic nanomaterials and biomaterials: The bottom-up approach for functional nanostructures formation and advanced applications. Materials 2020, 13, 1048.
Crossref Google Scholar
[28]

Kang, Y. J.; Murray, C. B. Synthesis and electrocatalytic properties of cubic Mn-Pt nanocrystals (nanocubes). J. Am. Chem. Soc. 2010, 132, 7568–7569.
Crossref Google Scholar
[29]

Kang, Y. J.; Qi, L.; Li, M.; Diaz, R. E.; Su, D.; Adzic, R. R.; Stach, E.; Li, J.; Murray, C. B. Highly active Pt3Pb and core–shell Pt3Pb-Pt electrocatalysts for formic acid oxidation. ACS Nano 2012, 6, 2818–2825.
Crossref Google Scholar
[30]

Zhan, W. C.; Wang, J. L.; Wang, H. F.; Zhang, J. S.; Liu, X. F.; Zhang, P. F.; Chi, M. F.; Guo, Y. L.; Guo, Y.; Lu, G. Z. et al. Crystal structural effect of AuCu alloy nanoparticles on catalytic CO oxidation. J. Am. Chem. Soc. 2017, 139, 8846–8854.
Crossref Google Scholar
[31]

Kang, Y. J.; Snyder, J.; Chi, M. F.; Li, D. G.; More, K. L.; Markovic, N. M.; Stamenkovic, V. R. Multimetallic core/interlayer/shell nanostructures as advanced electrocatalysts. Nano Lett. 2014, 14, 6361–6367.
Crossref Google Scholar
[32]

Yang, Z. B.; Sun, J.; Lu, S.; Vitos, L. A comparative study of solid-solution strengthening in Cr-Co-Ni complex concentrated alloys: The effect of magnetism. Comput. Mater. Sci. 2021, 192, 110408.
Crossref Google Scholar
[33]

Nørskov, J. K.; Bligaard, T.; Logadottir, A.; Kitchin, J. R.; Chen, J. G.; Pandelov, S.; Stimming, U. Trends in the exchange current for hydrogen evolution. J. Electrochem. Soc. 2005, 152, J23–J26.
Crossref Google Scholar
[34]

Kresse, G.; Hafner, J. Ab initio molecular dynamics for open-shell transition metals. Phys. Rev. B 1993, 48, 13115–13118.
Crossref Google Scholar
[35]

Kresse, G.; Furthmüller, J. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys. Rev. B 1996, 54, 11169–11186.
Crossref Google Scholar
[36]

Kresse, G.; Joubert, D. From ultrasoft pseudopotentials to the projector augmented-wave method. Phys. Rev. B 1999, 59, 1758–1775.
Crossref Google Scholar
[37]

Perdew, J. P.; Burke, K.; Ernzerhof, M. Generalized gradient approximation made simple. Phys. Rev. Lett. 1996, 77, 3865–3868.
Crossref Google Scholar
[38]

Monkhorst, H. J.; Pack, J. D. Special points for Brillouin-zone integrations. Phys. Rev. B 1976, 13, 5188–5192.
Crossref Google Scholar
Nano Research
Volume 16 Issue 8,
August 2023
Pages 10742-10747
DOI: 10.1007/s12274-023-5868-7
Cite this article:
Yu Y, Liu G, Jiang S, et al. Engineering the high-entropy phase of Pt-Au-Cu nanowire for electrocatalytic hydrogen evolution. Nano Research, 2023, 16(8): 10742-10747. https://doi.org/10.1007/s12274-023-5868-7
Topics:
Electrocatalysis

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Received: 23 March 2023
Revised: 02 May 2023
Accepted: 24 May 2023
Published: 19 June 2023
© Tsinghua University Press 2023
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