Atomic layer deposited Pt-Ru dual-metal dimers and identifying their active sites for hydrogen evolution reaction

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Abstract

Single atom catalysts exhibit particularly high catalytic activities in contrast to regular nanomaterial-based catalysts. Until recently, research has been mostly focused on single atom catalysts, and it remains a great challenge to synthesize bimetallic dimer structures. Herein, we successfully prepare high-quality one-to-one A-B bimetallic dimer structures (Pt-Ru dimers) through an atomic layer deposition (ALD) process. The Pt-Ru dimers show much higher hydrogen evolution activity (more than 50 times) and excellent stability compared to commercial Pt/C catalysts. X-ray absorption spectroscopy indicates that the Pt-Ru dimers structure model contains one Pt-Ru bonding configuration. First principle calculations reveal that the Pt-Ru dimer generates a synergy effect by modulating the electronic structure, which results in the enhanced hydrogen evolution activity. This work paves the way for the rational design of bimetallic dimers with good activity and stability, which have a great potential to be applied in various catalytic reactions.

Abstract

Atomically precise control over elemental distributions presents a challenge in the preparation of catalytic nanomaterials. Here the authors report Pt-Ru bimetallic dimer structures through atomic layer deposition process and identify the roles of Pt and Ru in hydrogen evolution reaction.

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Most cited references 26

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Single-Atom Catalysts: Synthetic Strategies and Electrochemical Applications

Yuanjun Chen, Qing Peng, Yadong Li … (2018)

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Climbing the density functional ladder: nonempirical meta-generalized gradient approximation designed for molecules and solids.

Jianmin Tao, John P Perdew, Viktor N. Staroverov … (2003)

The electron density, its gradient, and the Kohn-Sham orbital kinetic energy density are the local ingredients of a meta-generalized gradient approximation (meta-GGA). We construct a meta-GGA density functional for the exchange-correlation energy that satisfies exact constraints without empirical parameters. The exchange and correlation terms respect two paradigms: one- or two-electron densities and slowly varying densities, and so describe both molecules and solids with high accuracy, as shown by extensive numerical tests. This functional completes the third rung of "Jacob's ladder" of approximations, above the local spin density and GGA rungs.

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Low-temperature hydrogen production from water and methanol using Pt/α-MoC catalysts

Lili Lin, Yao-Wu Zhou, Rui Gao … (2017)

Polymer electrolyte membrane fuel cells (PEMFCs) running on hydrogen are attractive alternative power supplies for a range of applications, with in situ release of the required hydrogen from a stable liquid offering one way of ensuring its safe storage and transportation before use. The use of methanol is particularly interesting in this regard, because it is inexpensive and can reform itself with water to release hydrogen with a high gravimetric density of 18.8 per cent by weight. But traditional reforming of methanol steam operates at relatively high temperatures (200–350 degrees Celsius), so the focus for vehicle and portable PEMFC applications has been on aqueous-phase reforming of methanol (APRM). This method requires less energy, and the simpler and more compact device design allows direct integration into PEMFC stacks. There remains, however, the need for an efficient APRM catalyst. Here we report that platinum (Pt) atomically dispersed on α-molybdenum carbide (α-MoC) enables low-temperature (150–190 degrees Celsius), base-free hydrogen production through APRM, with an average turnover frequency reaching 18,046 moles of hydrogen per mole of platinum per hour. We attribute this exceptional hydrogen production—which far exceeds that of previously reported low-temperature APRM catalysts—to the outstanding ability of α-MoC to induce water dissociation, and to the fact that platinum and α-MoC act in synergy to activate methanol and then to reform it.

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Author and article information

Contributors

Li-Min Liu:

ORCID: http://orcid.org/0000-0003-3925-5310

liminliu@buaa.edu.cn

Gianluigi A. Botton:

ORCID: http://orcid.org/0000-0002-8746-1146

gbotton@mcmaster.ca

Xueliang Sun: xsun@eng.uwo.ca

Journal

Journal ID (nlm-ta): Nat Commun

Journal ID (iso-abbrev): Nat Commun

Title: Nature Communications

Publisher: Nature Publishing Group UK (London )

ISSN (Electronic): 2041-1723

Publication date (Electronic): 30 October 2019

Publication date PMC-release: 30 October 2019

Publication date Collection: 2019

Volume: 10

Electronic Location Identifier: 4936

Affiliations

[1 ]ISNI 0000 0004 1936 8884, GRID grid.39381.30, Department of Mechanical and Materials Engineering, , The University of Western Ontario, ; London, ON N6A 5B9 Canada

[2 ]ISNI 0000 0004 0586 4246, GRID grid.410743.5, Beijing Computational Science Research Center, ; Beijing, 100193 China

[3 ]ISNI 0000 0000 9999 1211, GRID grid.64939.31, School of Physics, , Beihang University, ; Beijing, 100083 China

[4 ]ISNI 0000 0004 1936 8227, GRID grid.25073.33, Department of Materials Science and Engineering, , McMaster University, ; Hamilton, ON L8S 4L8 Canada

[5 ]ISNI 0000 0004 0443 7584, GRID grid.423571.6, Canadian Light Source Inc, ; Saskatoon, SK S7N 2V3 Canada

[6 ]GRID grid.263817.9, Department of Materials Science and Engineering, , Southern University of Science and Technology, ; Shenzhen, 518055 China

[7 ]ISNI 0000 0004 1936 8884, GRID grid.39381.30, Department of Chemistry, , University of Western Ontario, ; London, ON N6A 5B7 Canada

Author information

Zhiqiang Wang http://orcid.org/0000-0003-0628-5222

Jiatang Chen http://orcid.org/0000-0002-9705-6523

Mohammad Norouzi Banis http://orcid.org/0000-0002-6144-6837

Li-Min Liu http://orcid.org/0000-0003-3925-5310

Gianluigi A. Botton http://orcid.org/0000-0002-8746-1146

Article

Publisher ID: 12887

DOI: 10.1038/s41467-019-12887-y

PMC ID: 6821730

PubMed ID: 31666505

SO-VID: 2641a58e-b6a2-4d9d-89d6-57e306ba55ed

License:

Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

History

Date received : 6 May 2019

Date accepted : 25 September 2019

Funding

Funded by: FundRef https://doi.org/10.13039/501100001804, Canada Research Chairs (Chaires de recherche du Canada);

Funded by: FundRef https://doi.org/10.13039/501100004381, Western University (University of Western Ontario);

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ScienceOpen disciplines: Uncategorized

Keywords: catalyst synthesis,hydrogen fuel,electrocatalysis

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ScienceOpen disciplines: Uncategorized

Keywords: catalyst synthesis, hydrogen fuel, electrocatalysis

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Atomic layer deposited Pt-Ru dual-metal dimers and identifying their active sites for hydrogen evolution reaction

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Most cited references 26

Single-Atom Catalysts: Synthetic Strategies and Electrochemical Applications

Climbing the density functional ladder: nonempirical meta-generalized gradient approximation designed for molecules and solids.

Low-temperature hydrogen production from water and methanol using Pt/α-MoC catalysts

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Cited by 181

Most referenced authors 1,324