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一石二鸟:同时提高双相中熵金属硫化物的OER催化活性和稳定性

Two Birds with One Stone: Contemporaneously Enhancing OER Catalytic Activity and Stability for Dual-Phase Medium-Entropy Metal Sulfides.

作者信息

Li Fengqi, Wu Hao, Lv Shaochen, Ma Yujie, Wang Biao, Ren Yilun, Wang Cong, Shi Yuxuan, Ji Hurong, Gu Jian, Tang Shaochun, Meng Xiangkang

机构信息

National Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, College of Engineering and Applied Sciences, Nanjing University, Nanjing, 210093, P. R. China.

College of Electronic and Information Engineering, Tongji University, Shanghai, 201800, P. R. China.

出版信息

Small. 2024 Mar;20(11):e2309025. doi: 10.1002/smll.202309025. Epub 2023 Oct 27.

Abstract

Transition metal-based sulfides exhibit remarkable potential as electrocatalysts for oxygen evolution reaction (OER) due to the unique intrinsic structure and physicochemical characteristics. Nevertheless, currently available sulfide catalysts based on transition metals face a bottleneck in large-scale commercial applications owing to their unsatisfactory stability. Here, the first fabrication of (FeCoNiMn )S dual-phase medium-entropy metal sulfide (dp-MEMS) is successfully achieved, which demonstrated the expected optimization of stability in the OER process. Benefiting from the "cell wall" -like structure and the synergistic effect in medium-entropy systems, (FeCoNiMn )S dp-MEMS delivers an exceptionally low overpotential of 169 and 232 mV at current densities of 10 and 100 mA cm , respectively. The enhancement mechanism of catalytic activity and stability is further validated by density functional theory (DFT) calculations. Additionally, the rechargeable Zn-air batteries integrated with FeCoNiMn )S dp-MEMS exhibit remarkable performance outperforming the commercial catalyst (Pt/C+RuO ). This work demonstrates that the dual-phase medium-entropy metal sulfide-based catalysts have the potential to provide a greater application value for OER and related energy conversion systems.

摘要

基于过渡金属的硫化物由于其独特的内在结构和物理化学特性,在析氧反应(OER)电催化剂方面展现出显著潜力。然而,目前基于过渡金属的硫化物催化剂因其稳定性不尽人意,在大规模商业应用中面临瓶颈。在此,首次成功制备出(FeCoNiMn)S双相中熵金属硫化物(dp-MEMS),其在OER过程中展现出预期的稳定性优化。受益于中熵体系中类似“细胞壁”的结构和协同效应,(FeCoNiMn)S dp-MEMS在电流密度分别为10和100 mA cm时,过电位极低,分别为169和232 mV。催化活性和稳定性的增强机制通过密度泛函理论(DFT)计算得到进一步验证。此外,集成有(FeCoNiMn)S dp-MEMS的可充电锌空气电池表现出卓越性能,优于商业催化剂(Pt/C+RuO)。这项工作表明,基于双相中熵金属硫化物的催化剂有潜力为OER及相关能量转换系统提供更大的应用价值。

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