In Situ Identification of Zinc Sites as Potential-Dependent Selectivity Switch over Dual-Atom Catalysts for H<sub>2</sub>O<sub>2</sub> Electrosynthesis
Controllably breaking the activity-selectivity trade-offs in the electrocatalytic oxygen reduction reaction to produce H<sub>2</sub>O<sub>2</sub> has long been a challenge in renewable energy technologies. Herein, by assigning the activity and selectivity requirements to two independent single-atom sites, we deliberately engineered a Co-Zn DAC for promising H<sub>2</sub>O<sub>2</sub> electrosynthesis, from which the Co sites provided the activity response for oxygen reduction, and the Zn sites regulated the reaction selectivity toward the 2e<sup>-</sup> pathway. Through multidimensional in situ characterizations, a potential-dependent switching function of the Zn sites was revealed, which made the increase in H<sub>2</sub>O<sub>2</sub> production at various reaction stages controllable. As a result, efficient H<sub>2</sub>O<sub>2</sub> selectivity switching from 11.1% in the single Co atom catalyst to 94.8% in the Co-Zn DAC was realized, with a prominent turnover frequency of 2.7 s<sup>-1</sup> among the reported H<sub>2</sub>O<sub>2</sub>-producing catalysts. Notably, a similar effect was also observed in M-Zn DACs (M = Pt, Ru, or Ni), which demonstrated the universal switcher role of the Zn sites. The real-time catalytic site behavior insights gained through this integrated experimental and theoretical study are envisioned to be valuable not only for the ORR but also for other energy catalysis reactions involving activity-selectivity trade-off issues.
Authors
- Qizheng An
- Xin Chen (ORCID: https://orcid.org/0000-0002-5120-1983)
- Xupeng Qin
- Jianglong Guo (ORCID: https://orcid.org/0000-0002-9997-6059)
- Dingsheng S. Wang (ORCID: https://orcid.org/0000-0003-0074-7633)
- Yuanli Li (ORCID: https://orcid.org/0000-0002-0816-8575)
- Weiren Cheng (ORCID: https://orcid.org/0000-0001-6938-6296)
- Xuan Sun (ORCID: https://orcid.org/0000-0002-8338-3654)
- Jing Zhang (ORCID: https://orcid.org/0000-0002-4706-8630)
- Yuhao Zhang (ORCID: https://orcid.org/0000-0002-5131-8591)
- Qinghua Liu (ORCID: https://orcid.org/0000-0003-4090-3311)
- Xu Zhang (ORCID: https://orcid.org/0000-0003-3112-4789)
- Kun Zheng (ORCID: https://orcid.org/0000-0001-7556-0203)
- Hui Zhang (ORCID: https://orcid.org/0000-0003-2210-5674)
- Baojie Li (ORCID: https://orcid.org/0000-0002-1211-5222)
- Yaling Jiang
- Jingjing Jiang (ORCID: https://orcid.org/0000-0002-5390-9715)
Institutions
- Shihezi University (CN)
- University of Science and Technology of China (CN)
- Southwest University of Science and Technology (CN)
- Southwest Petroleum University (CN)
- Xinjiang Production and Construction Corps (CN)
- Beijing University of Technology (CN)
- State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation (CN)
- Nuclear and Radiation Safety Center (CN)
- National Synchrotron Radiation Laboratory (CN)
- Green Chemistry (PL)
- Intelligent Decision Systems (Spain) (ES)
- Tsinghua University (CN)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2025-03-25
- DOI
- https://doi.org/10.1021/jacs.5c01449
- Citations
- 43
- Primary Topic
- Electrocatalysts for Energy Conversion
- Type
- article
- Field-Weighted Citation Impact
- 15.63
Funders
- National Natural Science Foundation of China
- China Postdoctoral Science Foundation
- Southwest University of Science and Technology
- University of Science and Technology of China