Steering the Electronic Microenvironment of Ruthenium Sites via Boron Buffering Enables Enhanced Hydrogen Evolution under a Universal pH Range
Optimizing the microenvironment of active sites is crucial for enhancing the catalytic activity of the hydrogen evolution reaction (HER) across various pH conditions. Here, guided by theoretical predictions of boron (B)-doping's electronic buffering effect on ruthenium (Ru) at the atomic scale, a highly efficient and universal-pH Ru-based HER electrocatalyst (Ru-NBC) by introducing B and nitrogen (N) into a carbon (C) matrix was designed. The Ru-NBC catalyst demonstrated exceptional HER activity, requiring overpotentials of 27, 40, and 68 mV in 1 M KOH, 0.5 M H<sub>2</sub>SO<sub>4</sub>, and 1 M phosphate buffer solution (PBS), respectively, to achieve a current density of 10 mA cm<sup>-2</sup>. <i>In situ</i> Raman spectroscopy, ambient-pressure X-ray photoelectron spectroscopy, and potential of zero charge measurements revealed that B-doping modulates the local Ru microenvironment, restructuring the distribution balance of the interfacial water hydrogen-bond network within the electrochemical double layer and thereby facilitating water adsorption and dissociation. Density functional theory calculations further verified that the electronic buffering effect of B optimizes hydrogen adsorption in acidic media and water activation in alkaline conditions, resultantly contributing to the universal-pH HER performance. This study could provide guidance for the design of advanced electrocatalysts through modulation of the local microenvironment of active sites for energy storage and conversion.
Authors
- Jianfeng Huang (ORCID: https://orcid.org/0000-0001-9871-6303)
- Jingxiang Zhao (ORCID: https://orcid.org/0000-0001-6023-8887)
- Ying Wei (ORCID: https://orcid.org/0000-0002-2965-8274)
- Yongqiang Feng (ORCID: https://orcid.org/0000-0002-7026-7152)
- Dantong Zhang (ORCID: https://orcid.org/0000-0002-4859-9898)
- Wenjie Zhu (ORCID: https://orcid.org/0000-0001-5218-7602)
- Lu Zhao (ORCID: https://orcid.org/0000-0002-6835-8397)
- Qingqing Liu (ORCID: https://orcid.org/0000-0001-7482-2523)
- Li Xu
- Liping Lin (ORCID: https://orcid.org/0009-0003-8741-263X)
- Yifan Ye (ORCID: https://orcid.org/0000-0003-4123-9387)
- Jilong Xu
- Bin Wu (ORCID: https://orcid.org/0009-0007-6652-2601)
- Qunzhi Ma
- Qiwen Su
- Ying Wang (ORCID: https://orcid.org/0009-0008-3662-2692)
Institutions
- University of Science and Technology of China (CN)
- Harbin Normal University (CN)
- Chinese Academy of Sciences (CN)
- Helmholtz-Zentrum Berlin für Materialien und Energie (DE)
- China University of Geosciences (CN)
- China University of Geosciences (Beijing) (CN)
- Shenzhen Institutes of Advanced Technology (CN)
- Materials Research Center (IN)
- National Synchrotron Radiation Laboratory (CN)
- Shaanxi University of Science and Technology (CN)
Publication Details
- Journal
- ACS Nano
- Published
- 2025-02-22
- DOI
- https://doi.org/10.1021/acsnano.4c14866
- Citations
- 31
- Primary Topic
- Electrocatalysts for Energy Conversion
- Type
- article
- Field-Weighted Citation Impact
- 11.27
Funders
- Volkswagen Foundation
- National Natural Science Foundation of China
- Xi'an Municipal Bureau of Science and Technology
- University of Science and Technology of China
- National Key Research and Development Program of China
- Key Research and Development Projects of Shaanxi Province