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铱掺杂调节花状磷化物的电子结构用于水氧化。

Ir Doping Modulates the Electronic Structure of Flower-Shaped Phosphides for Water Oxidation.

作者信息

Sun Huiyu, Yu Shudi, Yin Jiongting, Li Jie, Yu Jun, Liu Tianpeng, Liang Wanyu, Zhang Nannan, Zhang Yangping, Ye Changqing, Hu Mengyun, Du Yukou

机构信息

College of Chemistry, Chemical Engineering and Materials Science, Soochow University, 199 Renai Road, Suzhou 215123, China.

Jiangsu Key Laboratory for Environment Functional Materials, School of Materials Science and Engineering, Suzhou University of Science and Technology, Suzhou 215009, China.

出版信息

Inorg Chem. 2024 Nov 4;63(44):21283-21292. doi: 10.1021/acs.inorgchem.4c03771. Epub 2024 Oct 22.

Abstract

Electrolysis of water to produce hydrogen is an efficient, clean, and environmentally friendly hydrogen production method with unlimited development prospects. However, its overall efficiency is hampered by the slow oxygen evolution reaction (OER) with complex electron transfer processes. Therefore, designing efficient and low-cost OER catalysts is the key to solving this problem. In this paper, Ir-doped CoP/FeP (abbreviated as Ir-CoFeP/NF) was grown on nickel foam through the strategies of low amount noble-metal doping and mild phosphating. Phosphide derived from a floral metal-organic framework (MOF) exhibits regular three-dimensional (3D) morphology and large active area, avoiding the stacking of active sites. The addition of Ir can effectively adjust the electronic structure, change the position of the d-band center, and increase active sites, thus enhancing the catalytic activity. Hence, the optimized catalyst exhibits unexpected electrocatalytic OER activity with an ideal overpotential of 213 mV at 10 mA cm, as well as a low Tafel slope of 40.63 mV dec. Coupling with Pt/C for overall water splitting (OWS), the entire device only needs an ultralow cell voltage of 1.50 V to achieve a current density of 10 mA cm. Besides, the OWS can be maintained for more than 70 h. This study demonstrates the superiority of Ir-doped phosphide in accelerating water oxidation.

摘要

电解水制氢是一种高效、清洁、环保的制氢方法,具有无限的发展前景。然而,其整体效率受到析氧反应(OER)缓慢且电子转移过程复杂的限制。因此,设计高效且低成本的OER催化剂是解决这一问题的关键。本文通过少量贵金属掺杂和温和磷化策略,在泡沫镍上生长了Ir掺杂的CoP/FeP(简称为Ir-CoFeP/NF)。源自花状金属有机框架(MOF)的磷化物呈现规则的三维(3D)形态和大的活性面积,避免了活性位点的堆积。Ir的加入可以有效调节电子结构,改变d带中心位置,并增加活性位点,从而提高催化活性。因此,优化后的催化剂表现出意想不到的电催化OER活性,在10 mA cm时理想过电位为213 mV,塔菲尔斜率低至40.63 mV dec。与Pt/C耦合用于全水分解(OWS)时,整个装置仅需1.50 V的超低电池电压即可实现10 mA cm的电流密度。此外,OWS可维持70 h以上。本研究证明了Ir掺杂磷化物在加速水氧化方面的优越性。

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