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Cited by 180Electrocatalysts for Energy ConversionCO2 Reduction Techniques and CatalystsHydrogen Storage and Materials

Methanol-Enhanced Low-Cell-Voltage Hydrogen Generation at Industrial-Grade Current Density by Triadic Active Sites of Pt1–Pdn–(Ni,Co)(OH)x

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Pei, An, Xie, Ruikuan, Zhu, Lihua, Wu, Fengshun, Huang, Zinan, Pang, Yongyu, Chang, Yu-Chung, Chai, Guoliang +8 more·2025·Journal of the American Chemical Society
DOI 10.1021/jacs.4c12665PMC PMC11803621
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Abstract

Methanol (ME) is a liquid hydrogen carrier, ideal for on-site-on-demand H 2 generation, avoiding its costly and risky distribution issues, but this “ME-to-H 2 ” electric conversion suffers from high voltage (energy consumption) and competitive oxygen evolution reaction. Herein, we demonstrate that a synergistic cofunctional Pt 1 Pd n /(Ni,Co)(OH) x catalyst with Pt single atoms (Pt 1 ) and Pd nanoclusters (Pd n ) anchored on OH-vacancy(V OH )-rich (Ni,Co)(OH) x nanoparticles create synergistic triadic active sites, allowing for methanol-enhanced low-voltage H 2 generation. For MOR, OH* is preferentially adsorbed on Pd n and then interacts with the intermediates (such as *CHO or *CHOOH) adsorbed favorably on neighboring Pt 1 with the assistance of hydrogen bonding from the surface hydrogen of (Ni,Co)(OH) x . The enhanced selectivity of the *CHOOH pathway, instead of *CO, sustains the MOR activity to a practically high current density. For HER, triadic Pt 1, Pd n, and OH-vacancy sites on (Ni,Co)(OH) x create an “acid–base” microenvironment to facilitate water adsorption and splitting, forming H* species on Pt 1 and Pd n, and *OH at the vacancy, to promote efficient H 2 evolution from the asymmetric Pt 1 and Pd n sites via the Tafel mechanism. The triadic-site synergy opens new avenues for the design and synthesis of highly efficient and stable cofunctional catalysts for “on-site-on-demand” H 2 production, here facilitated by liquid methanol.

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  • Pt-based electrocatalysts are still recognized as the most effective catalysts for both alkaline HER and alkaline MOR.

    “Currently, Pt-based electrocatalysts are still recognized as the most effective catalysts for both alkaline HER and alkaline MOR.16,20–22”

    From Tuning the local environment of atomic Pt shells of Pt <sub>3</sub> Fe@Pt nanoparticles enables energy-saving hydrogen production (2026) · cites this paper as [16]

    The Introduction says Pt(Pd)-based catalysts activate alkaline MOR at low voltage and Pt single atoms have excellent HER activity. The Results and Discussion report that this particular Pt–Pd–hydroxide catalyst outperforms tested benchmarks for both reactions. Those findings support the importance of Pt-based catalysts, but not the broader claim that the class is recognized as the most effective for both alkaline HER and MOR. (LLM, conf=0.83)

    Experimental — accuracy not yet measured

  • Alkaline HER at the cathode can be coupled with the methanol oxidation reaction (MOR) to replace the corresponding OER at the anode.

    “For example, alkaline HER at the cathode is coupled with the methanol oxidation reaction (MOR) to replace the corresponding OER at the anode.16–19”

    From Tuning the local environment of atomic Pt shells of Pt <sub>3</sub> Fe@Pt nanoparticles enables energy-saving hydrogen production (2026) · cites this paper as [16]

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Cited by

Sorted by citations

Authors
Pei, A., Xie, R., Zhu, L., Wu, F., Huang, Z., Pang, Y., Chang, Y.-C., Chai, G., Pao, C.-W., Gao, Q., Shang, C., Li, G., Ye, J., Zhu, H., Yang, Z., & Guo, Z.
Affiliations
  • Jiangxi University of Science and Technology (CN)
  • Chinese Academy of Sciences (CN)
  • Jinan University (CN)
  • National Synchrotron Radiation Research Center (TW)
  • University of Hong Kong (HK)
  • Xiamen University (CN)
  • Ji Hua Laboratory (CN)
Corresponding author
  • Zhu, Lihua
  • Chai, Guoliang
  • Gao, Qingsheng
  • Guo, Zhengxiao
ORCID
Venue
Journal of the American Chemical Society
Publisher
American Chemical Society (ACS)
Published
2025-01-13
Volume
147
Issue
4
Pages
3185-3194
ISSN
  • 0002-7863 (ISSN-L)
  • 1520-5126
DOI
10.1021/jacs.4c12665
PMC
PMC11803621
OpenAlex
W4406323640
Cited by
180
References
3
Citations by year
2026: 98 · 2025: 82
FWCI
24.84
Type
journal article
Language
en
Open access
Licence
Locations
  • Journal of the American Chemical Society (publishedVersion, cc-by)
  • PubMed Central (publishedVersion, cc-by)
  • PubMed (publishedVersion)
  • The HKU Scholars Hub (University of Hong Kong) (submittedVersion, cc-by-nc-nd)
Funders
  • Research Grants Council, University Grants Committee (T23-713/22-R)
  • National Key Research and Development Program of China (2017YFA0700103, 2018YFA0704502)
  • University of Hong Kong
  • Government of Guangdong Province (2020B0101370003)
  • Jiangxi University of Science and Technology (JXUSTQJBJ2019002)
  • University Grants Committee (E-HKU701/23)
  • National Natural Science Foundation of China (21703248, 22162012, 22175077, 22202089)
  • Environment and Conservation Fund (109/2022, 152/2021)
  • Program of Qingjiang Excellent Young Talents
  • Hong Kong Quantum AI Lab
  • Program of Technology Innovation Talents of Ganzhou
  • Youth Jinggang Scholars Program in Jiangxi Province ([2019]57)
  • Natural Science Foundation of Jiangxi Province for Distinguished Young Scholars (20224ACB213005)
  • Thousand Talents Plan of Jiangxi Province (jxsq2019201083)
Topics
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
  • Physical Sciences › Materials Science › Materials Chemistry › Hydrogen Storage and Materials
Keywords
methanol-to-hydrogen conversion, methanol oxidation, hydrogen evolution reaction, Pt single atoms, Pd nanoclusters, on-site hydrogen production, oxygen evolution suppression

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