Unlocking the Potential of Mn‐based Catalyst for Durable Two‐electron Oxygen Reduction in Acid at High Current Densities
Electrochemical synthesis of H<sub>2</sub>O<sub>2</sub> by two-electron oxygen reduction (2e<sup>-</sup> ORR) often shows limited stability at high current densities in acidic media. Mn-based catalysts have been demonstrated highly stable for four-electron ORR thanks to their intrinsically low rate constant for Fenton-like reactions. However, their activity toward acidic 2e<sup>-</sup> ORR remains low because of too strong adsorption to *OOH. Here, we report a diatomic Mn catalyst with high-spin Mn<sup>II</sup> centers to enable high onset potential (0.69 V), high selectivity (>90%), and outstanding stability (240 h under 300 mA cm<sup>-2</sup>) toward H<sub>2</sub>O<sub>2</sub> electrosynthesis in acid. Theoretical calculations and in situ spectroscopies reveal that the diatomic Mn sites have downshifted d-band center and thus weakened adsorption strength for *OOH. Moreover, the inertia of the Mn<sup>II</sup> sites toward the troublesome Fenton-like reactions leads to the long-term stability at high current densities. We further demonstrate the functionalization of waste polyethylene (PE) using the high-concentration H<sub>2</sub>O<sub>2</sub> as produced, which provides a sustainable route toward on-site upcycling of plastic waste.
Authors
- Xin Tang (ORCID: https://orcid.org/0000-0003-0979-5455)
- Zhiqiang Niu (ORCID: https://orcid.org/0000-0002-9122-4880)
- Yanfen Wu
- Kaiqi Nie (ORCID: https://orcid.org/0000-0002-1150-8024)
- Zhengwen Li (ORCID: https://orcid.org/0009-0007-4486-0386)
- Xiaohang Sun (ORCID: https://orcid.org/0009-0000-3142-6192)
- Mingze Sun (ORCID: https://orcid.org/0000-0003-0027-0003)
- Yu‐Xiao Zhang (ORCID: https://orcid.org/0000-0002-9112-9947)
- Jun He (ORCID: https://orcid.org/0000-0003-1671-2283)
- Jinjie Fang
- Zhongbin Zhuang (ORCID: https://orcid.org/0000-0001-7187-1266)
- Liang Zhang (ORCID: https://orcid.org/0000-0002-3446-3172)
- Yuqi Wang (ORCID: https://orcid.org/0000-0001-6230-0330)
- Kai Chen (ORCID: https://orcid.org/0000-0002-1892-8195)
- Helai Huang (ORCID: https://orcid.org/0009-0006-0633-5110)
- Haiyong Wang (ORCID: https://orcid.org/0000-0002-0787-3678)
- Qikun Hu (ORCID: https://orcid.org/0000-0003-1607-420X)
- Yizhen Che
Institutions
- Harbin Institute of Technology (CN)
- Inner Mongolia University (CN)
- State Key Laboratory of Vehicle NVH and Safety Technology (CN)
- State Key Laboratory of Chemical Engineering (CN)
- Beijing University of Chemical Technology (CN)
- Tsinghua University (CN)
Publication Details
- Journal
- Angewandte Chemie International Edition
- Published
- 2025-06-11
- DOI
- https://doi.org/10.1002/anie.202511844
- Citations
- 6
- Primary Topic
- Electrocatalysts for Energy Conversion
- Type
- article
- Field-Weighted Citation Impact
- 2.18
Funders
- National Natural Science Foundation of China
- Natural Science Foundation of Beijing Municipality