Yingqiang Li, Xinmiao Yu, Yifan Liu, Chao Liu, Jing Jin, Libin Hao, Tao Zhang, Xiang Tang, Pan Xiong, Junwu Zhu
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引用次数: 0
Abstract
Single-atom catalysts exhibit high efficiency and durability in oxygen reduction reactions (ORR). Among the factors influencing ORR activity, the spin configuration of single-atom catalysts can be effectively tuned through heteroatom doping, diatomic synergy, and coordination number regulation. However, systematic investigations into how atomic clusters modulate the spin configuration and catalytic behavior of single atoms in electrocatalysis remain scarce. Herein, Mn atomic clusters are employed to regulate the spin configuration of Mn single atoms, thereby enhancing their intrinsic activity as the primary active sites for high-performance zinc-air batteries. A porous carbon-based two-dimensional (2D) nanosheet (MnSA/MnAC-NSC) was synthesized, featuring co-existence of Mn atomic clusters and Mn single atoms. The involvement of Mn clusters induces a spin-state transition of Mn single atoms from high-spin to low-spin, which leads to σ* orbital occupation, facilitated OH⁻ desorption, and consequently accelerated reaction kinetics of the rate-determining step. MnSA/MnAC-NSC exhibited a high half-wave potential (0.85 V) for ORR, surpassing that of the Mn single atom counterpart (Mn-NSC) (0.81 V) and commercial Pt/C (0.75 V). Besides, a zinc-air battery with the MnSA/MnAC-NSC cathode could deliver a power density of 152.8 mW cm⁻2 and maintain enduring stability for over 80 h. This work paves the way for designing high-performance single-atom catalysts through cluster-induced spin-state modulation.
期刊介绍:
Nano Energy is a multidisciplinary, rapid-publication forum of original peer-reviewed contributions on the science and engineering of nanomaterials and nanodevices used in all forms of energy harvesting, conversion, storage, utilization and policy. Through its mixture of articles, reviews, communications, research news, and information on key developments, Nano Energy provides a comprehensive coverage of this exciting and dynamic field which joins nanoscience and nanotechnology with energy science. The journal is relevant to all those who are interested in nanomaterials solutions to the energy problem.
Nano Energy publishes original experimental and theoretical research on all aspects of energy-related research which utilizes nanomaterials and nanotechnology. Manuscripts of four types are considered: review articles which inform readers of the latest research and advances in energy science; rapid communications which feature exciting research breakthroughs in the field; full-length articles which report comprehensive research developments; and news and opinions which comment on topical issues or express views on the developments in related fields.