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通过调整普鲁士蓝类似物中的钴/锰含量实现高析氧反应性能

Achieving High OER Performance by Tuning the Co/Mn Content in Prussian Blue Analogues.

作者信息

Wu Chang, Wang JinSong, Li Jiayang, Zhang Hang, Sharma Shailendra, Titheridge Laura, Tiffin Campbell, Fan Yameng, Zhao Lingfei, Yang Weishen, Li Zhengtao, Peng Jian, Wang Jiazhao, Marshall Aaron T

机构信息

Chemical and Process Engineering Department, University of Canterbury, Christchurch 8401, New Zealand.

Faculty of Materials Science and Engineering, Kunming University of Science and Technology, Kunming 650092, China.

出版信息

ACS Appl Mater Interfaces. 2024 Oct 30;16(43):58703-58710. doi: 10.1021/acsami.4c13199. Epub 2024 Oct 17.

Abstract

The need for efficient, economical, and clean energy systems is increasing, and as a result, interest in water-splitting techniques to produce green hydrogen is also increasing. However, the sluggish kinetics of the oxygen evolution reaction (OER) hinders the practical application and widespread use of water-splitting technologies; therefore, to address this challenge, it is essential to develop cost-effective and efficient OER catalysts. In this work, we have synthesized an inexpensive and tunable FeCoMn Prussian blue analogue (PBAs) as an efficient OER catalyst via a straightforward process. The ratio of the Co and Mn to optimize the electrochemical performance, and as a result, the FeCoMn PBA catalyst demonstrated the best electrochemical performance (260/304 mV overpotential at 10/50 mA cm, a low Tafel slope of 48 mV dec and a good stability of 72 h at 10 mA cm). Additionally, X-ray absorption spectroscopy (XAS) measurements and density functional theory (DFT) calculations suggest that the FeCoMn PBA possesses the optimized electronic density distribution at the active site (Co), and the doping of Mn and Fe can not only increase the electricity conductivity but also activate the critical HO deprotonation step.

摘要

对高效、经济且清洁的能源系统的需求不断增加,因此,对通过水分解技术生产绿色氢气的兴趣也在增加。然而,析氧反应(OER)缓慢的动力学阻碍了水分解技术的实际应用和广泛使用;因此,为应对这一挑战,开发具有成本效益且高效的OER催化剂至关重要。在这项工作中,我们通过一种简单的方法合成了一种廉价且可调谐的铁钴锰普鲁士蓝类似物(PBAs)作为高效的OER催化剂。优化钴和锰的比例以实现电化学性能,结果,铁钴锰PBA催化剂展现出最佳的电化学性能(在10/50 mA cm时过电位为260/304 mV,低塔菲尔斜率为48 mV dec,在10 mA cm时具有72 h的良好稳定性)。此外,X射线吸收光谱(XAS)测量和密度泛函理论(DFT)计算表明,铁钴锰PBA在活性位点(Co)处具有优化的电子密度分布,并且锰和铁的掺杂不仅可以提高电导率,还能激活关键的HO去质子化步骤。

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