Facilitating OH* Generation on Atomic Pd–Cu Dual Sites towards Efficient Glycerol Electrooxidation to Formate
The electrocatalytic glycerol oxidation reaction (GOR) represents a mild and sustainable pathway to produce value-added chemicals such as formate. However, the rational design and controlled synthesis of efficient catalysts to achieve highly selective C-C bond cleavage of glycerol towards formate remains a great challenge. Herein, atomic Pd doped Cu<sub>3</sub>N hollow nanocubes with Pd-Cu dual sites were prepared via the unique Kirkendall process, exhibiting superior electrocatalytic GOR activity and selectivity towards formate with a maximum Faraday efficiency of 91.6 %. In situ spectroscopic characterization and theoretical calculations reveal that Pd atoms located in partial Cu substituent sites could facilitate the generation of active *OH and enhance the adsorption of glycerol molecule on adjacent Cu sites, while Pd atoms located in Cu<sub>3</sub>N unit center could effectively reduce the energy barrier of C-C bond cleavage for the rate determining step. Our work provides new insights into the development of well-defined dual-site catalysts to boost glycerol electrooxidation to formate.
Authors
- Yi Ding (ORCID: https://orcid.org/0000-0002-0948-4991)
- Hui Zhang (ORCID: https://orcid.org/0000-0002-5602-9879)
- Yu Fu (ORCID: https://orcid.org/0000-0003-0962-7152)
- Yuchen Qin (ORCID: https://orcid.org/0000-0002-2680-9217)
- Dingsheng S. Wang (ORCID: https://orcid.org/0000-0003-0074-7633)
- Yizhen Zhang (ORCID: https://orcid.org/0000-0003-0755-2767)
- Yuanmiao Sun (ORCID: https://orcid.org/0000-0003-4650-5226)
- Junjun Li (ORCID: https://orcid.org/0000-0002-4080-5458)
- Zhicheng Zhang (ORCID: https://orcid.org/0000-0002-5333-1394)
- Zhenhua Li (ORCID: https://orcid.org/0000-0002-4101-2767)
- Qi Zhou (ORCID: https://orcid.org/0000-0002-6549-9362)
- Liya Zhang (ORCID: https://orcid.org/0000-0002-3496-3126)
- Le Yu (ORCID: https://orcid.org/0009-0004-2481-7426)
- Jiangrong Yang
Institutions
- Tianjin University (CN)
- Southwest Petroleum University (CN)
- Chinese Academy of Sciences (CN)
- Beijing Jiaotong University (CN)
- Shenzhen Institutes of Advanced Technology (CN)
- Henan Agricultural University (CN)
- Beijing University of Chemical Technology (CN)
- Tsinghua University (CN)
Publication Details
- Journal
- Angewandte Chemie International Edition
- Published
- 2025-02-16
- DOI
- https://doi.org/10.1002/anie.202425006
- Citations
- 27
- Primary Topic
- Electrocatalysts for Energy Conversion
- Type
- article
- Field-Weighted Citation Impact
- 9.81