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锰掺杂的CsPbX(X = Cl,Br)钙钛矿纳米晶体作为全解水的电催化剂的缺陷钝化

Defect Passivation of Mn-Doped CsPbX(X=Cl,Br) Perovskite Nanocrystals as Electrocatalyst for Overall Water Splitting.

作者信息

Zhou Haiyun, Li Pingping, Zhong Tingting, Teng Yunzhen, Li Siqi, Luo Xiaofeng, Wang Xinning, Yang Min, Deng Guowei

机构信息

College of Chemistry and Life Science, Sichuan Provincial Key Laboratory for Structural Optimization and Application of Functional Molecules, Chengdu Normal University, Chengdu, 611130, China.

出版信息

Chem Asian J. 2024 Dec 16;19(24):e202400798. doi: 10.1002/asia.202400798. Epub 2024 Nov 7.

DOI:10.1002/asia.202400798
PMID:39344932
Abstract

Mn doping has been used to improve the physical chemistry of lead halide perovskite nanocrystals such as CsPbX, where X is a halogen ion. In this paper, a two-phase method for Mn-doped CsPbX nanosheets (where X=Br, Cl), namely water-hexane system, is reported. Compared to conventional catalyst arrays, the band gap of CsPbBr nanocrystalline is easily tuned, the carrier diffusion distance is remote, the band edge position of the band structure is favorable for a wide range of electrocatalytic redox reactions, and the catalytic active site is maximally exposed, providing a larger electrolyte contact area. The porous hierarchical structure also accelerates the release of hydrogen bubbles. The results showed that the optimized Mn : CsPbBr catalyst exhibited excellent electrolytic performance of aquatic hydrogen in alkaline electrolyte (1 mol/L KOH). The overpotentials of the oxygen evolution reaction (OER) at the current densities of 10 and 100 mA cm are only 114.4 and 505.4 mV, respectively, with a Tafel slope of 43 mV dec. At a current density of 10 mA cm, the excess potential required for the hydrogen evolution reaction (HER) is 158.6 mV and it exhibits excellent electrochemical stability. The Mn : CsPbBr nanocrystalline consists of two electrodes for hydrolysis of water, requiring only a voltage of 1.45 V. This provides implications for the optimization of electrocatalysts in alkaline electrolytes with the aim of developing next generation 2D electrocatalysts for overall water splitting.

摘要

锰掺杂已被用于改善卤化铅钙钛矿纳米晶体(如CsPbX,其中X为卤素离子)的物理化学性质。本文报道了一种用于锰掺杂CsPbX纳米片(其中X = Br、Cl)的两相法,即水 - 己烷体系。与传统催化剂阵列相比,CsPbBr纳米晶体的带隙易于调节,载流子扩散距离较远,能带结构的带边位置有利于广泛的电催化氧化还原反应,且催化活性位点最大程度暴露,提供了更大的电解质接触面积。多孔分级结构还加速了氢气泡的释放。结果表明,优化后的Mn : CsPbBr催化剂在碱性电解质(1 mol/L KOH)中表现出优异的析氢电解性能。在电流密度为10和100 mA cm时,析氧反应(OER)的过电位分别仅为114.4和505.4 mV,塔菲尔斜率为43 mV dec。在电流密度为10 mA cm时,析氢反应(HER)所需的过电位为158.6 mV,且表现出优异的电化学稳定性。Mn : CsPbBr纳米晶体由两个用于水解水的电极组成,仅需1.45 V的电压。这为优化碱性电解质中的电催化剂以开发用于全水分解的下一代二维电催化剂提供了启示。

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