Single-Atom Cr-N4 Sites Designed for Durable Oxygen Reduction Catalysis in Acid Media

Ergui Luo; Hao Zhang; Xian Wang; Liqin Gao; Liyuan Gong; Tuo Zhao; Zhao Jin; Junjie Ge; Zheng Jiang; Changpeng Liu; Wei Xing

doi:10.1002/anie.201906289

Single-Atom Cr-N₄ Sites Designed for Durable Oxygen Reduction Catalysis in Acid Media

Angew Chem Int Ed Engl. 2019 Sep 2;58(36):12469-12475. doi: 10.1002/anie.201906289. Epub 2019 Aug 1.

Authors

Ergui Luo^{1

2}, Hao Zhang^{3

4}, Xian Wang^{1

2}, Liqin Gao¹, Liyuan Gong^{1

2}, Tuo Zhao^{1

2}, Zhao Jin¹, Junjie Ge^{1

2}, Zheng Jiang^{3

5}, Changpeng Liu^{1

2}, Wei Xing^{1

2}

Affiliations

¹ Laboratory of Advanced Power Sources, Jilin Province Key Laboratory of Low Carbon Chemical Power Sources, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, Jilin, 130022, P. R. China.
² School of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
³ Shanghai Institute of Applied Physics, Chinese Academy of Science, Shanghai, 201800, P. R. China.
⁴ University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.
⁵ Shanghai Synchrotron Radiation Facility, Zhangjiang Lab, Shanghai Advanced Research Institute, Chinese Academy of Science, Shanghai, 201210, P. R. China.

PMID: 31290248
DOI: 10.1002/anie.201906289

Abstract

Single-atom catalysts (SACs) are attracting widespread interest for the catalytic oxygen reduction reaction (ORR), with Fe-N_x SACs exhibiting the most promising activity. However, Fe-based catalysts suffer serious stability issues as a result of oxidative corrosion through the Fenton reaction. Herein, using a metal-organic framework as an anchoring matrix, we for the first time obtained pyrolyzed Cr/N/C SACs for the ORR, where the atomically dispersed Cr is confirmed to have a Cr-N₄ coordination structure. The Cr/N/C catalyst exhibits excellent ORR activity with an optimal half-wave potential of 0.773 V versus RHE. More excitingly, the Fenton reaction is substantially reduced and, thus, the final catalysts show superb stability. The innovative and robust active site for the ORR opens a new possibility to circumvent the stability issue of the non-noble metal ORR catalysts.

Keywords: Fenton reaction; chromium; heterogeneous catalysis; oxygen reduction; single-atom catalysts.

Abstract

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