Jie Zhao, Yue Guo, Zhiqi Zhang, Xilin Zhang, Qianqian Ji, Hua Zhang, Zhaoqi Song, Dongqing Liu, Jianrong Zeng, Chenghao Chuang, Erhuan Zhang, Yuhao Wang, Guangzhi Hu, Muhammad Asim Mushtaq, Waseem Raza, Xingke Cai, Francesco Ciucci
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引用次数: 0
摘要
单原子催化剂的进步对于提高氧进化反应（OER）性能并减少贵金属用量至关重要。全面了解潜在的机理将进一步加快这一进程。在此，我们报告了氢氧化钴铁上与二甲基咪唑（MI）平面外配位的 Ir 单原子（Ir1/(Co,Fe)-OH/MI）。这种Ir1/(Co,Fe)-OH/MI催化剂采用简单的浸泡法制备，在电流密度为10 mA cm-2时具有179 mV的超低过电位，在电流密度为600 mA cm-2时具有257 mV的超低过电位，以及24 mV dec-1的超小塔菲尔斜率。此外，Ir1/(Co,Fe)-OH/MI 的总质量活性比商用二氧化铱高出 58.4 倍。Ab initio 模拟表明，MI 的配位导致电子在 Ir 位点周围重新分布。这导致相邻 Ir 和 Co 位点的 d 带中心发生正向移动，从而为 OER 提供了最佳的能量途径。
Out-of-plane coordination of iridium single atoms with organic molecules and cobalt–iron hydroxides to boost oxygen evolution reaction
Advancements in single-atom-based catalysts are crucial for enhancing oxygen evolution reaction (OER) performance while reducing precious metal usage. A comprehensive understanding of underlying mechanisms will expedite this progress further. Here we report Ir single atoms coordinated out-of-plane with dimethylimidazole (MI) on CoFe hydroxide (Ir1/(Co,Fe)-OH/MI). This Ir1/(Co,Fe)-OH/MI catalyst, which was prepared using a simple immersion method, delivers ultralow overpotentials of 179 mV at a current density of 10 mA cm−2 and 257 mV at 600 mA cm−2 as well as an ultra-small Tafel slope of 24 mV dec−1. Furthermore, Ir1/(Co,Fe)-OH/MI has a total mass activity exceeding that of commercial IrO2 by a factor of 58.4. Ab initio simulations indicate that the coordination of MI leads to electron redistribution around the Ir sites. This causes a positive shift in the d-band centre at adjacent Ir and Co sites, facilitating an optimal energy pathway for OER.
期刊介绍：
Nature Nanotechnology is a prestigious journal that publishes high-quality papers in various areas of nanoscience and nanotechnology. The journal focuses on the design, characterization, and production of structures, devices, and systems that manipulate and control materials at atomic, molecular, and macromolecular scales. It encompasses both bottom-up and top-down approaches, as well as their combinations.
Furthermore, Nature Nanotechnology fosters the exchange of ideas among researchers from diverse disciplines such as chemistry, physics, material science, biomedical research, engineering, and more. It promotes collaboration at the forefront of this multidisciplinary field. The journal covers a wide range of topics, from fundamental research in physics, chemistry, and biology, including computational work and simulations, to the development of innovative devices and technologies for various industrial sectors such as information technology, medicine, manufacturing, high-performance materials, energy, and environmental technologies. It includes coverage of organic, inorganic, and hybrid materials.
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