Coupling Ni Single Atomic Sites with Metallic Aggregates at Adjacent Geometry on Carbon Support for Efficient Hydrogen Peroxide Electrosynthesis

Xin Wang; Run Huang; Xin Mao; Tian Liu; Panjie Guo; Hai Sun; Zhelin Mao; Chao Han; Yarong Zheng; Aijun Du; Jianwei Liu; Yi Jia; Lei Wang

doi:10.1002/advs.202402240

Coupling Ni Single Atomic Sites with Metallic Aggregates at Adjacent Geometry on Carbon Support for Efficient Hydrogen Peroxide Electrosynthesis

Adv Sci (Weinh). 2024 Apr 11:e2402240. doi: 10.1002/advs.202402240. Online ahead of print.

Authors

Xin Wang¹, Run Huang¹, Xin Mao², Tian Liu³, Panjie Guo¹, Hai Sun¹, Zhelin Mao¹, Chao Han¹, Yarong Zheng⁴, Aijun Du², Jianwei Liu³, Yi Jia^{5

6}, Lei Wang¹

Affiliations

¹ College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310014, P. R. China.
² School of Chemistry, Physics and Mechanical Engineering, Queensland University of Technology, Brisbane, QLD, 4000, Australia.
³ Division of Nanomaterials & Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, Institute of Energy, Hefei Comprehensive National Science Center, Department of Chemistry, Institute of Biomimetic Materials & Chemistry, Anhui Engineering Laboratory of Biomimetic Materials, University of Science and Technology of China, Hefei, 230026, P. R. China.
⁴ Anhui Province Key Laboratory of Advanced Catalytic Materials and Reaction Engineering, School of Chemistry and Chemical Engineering, Hefei University of Technology, Hefei, 230041, P. R. China.
⁵ Petroleum and Chemical Industry Key Laboratory of Organic Electrochemical Synthesis, College of Chemical Engineering, Zhejiang Carbon Neutral Innovation Institute, Zhejiang University of Technology (ZJUT), Hangzhou, 310014, P. R. China.
⁶ Moganshan Institute ZJUT, Deqing, 313200, P. R. China.

PMID: 38605604
DOI: 10.1002/advs.202402240

Abstract

Single atomic catalysts have shown great potential in efficiently electro-converting O₂ to H₂O₂ with high selectivity. However, the impact of coordination environment and introduction of extra metallic aggregates on catalytic performance still remains unclear. Herein, first a series of carbon-based catalysts with embedded coupling Ni single atomic sites and corresponding metallic nanoparticles at adjacent geometry is synthesized. Careful performance evaluation reveals Ni_SA/Ni_NP-NSCNT catalyst with precisely controlled active centers of synergetic adjacent Ni-N₄S single sites and crystalline Ni nanoparticles exhibits a high H₂O₂ selectivity over 92.7% within a wide potential range (maximum selectivity can reach 98.4%). Theoretical studies uncover that spatially coupling single atomic NiN₄S sites with metallic Ni aggregates in close proximity can optimize the adsorption behavior of key intermediates ^*OOH to achieve a nearly ideal binding strength, which thus affording a kinetically favorable pathway for H₂O₂ production. This strategy of manipulating the interaction between single atoms and metallic aggregates offers a promising direction to design new high-performance catalysts for practical H₂O₂ electrosynthesis.

Keywords: heteroatom doped carbon matrix; hydrogen peroxide electrosynthesis; nanoparticles; single atoms; synergistic effect.

Abstract

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