Microwave shock motivating the Sr substitution of 2D porous GdFeO3 perovskite for highly active oxygen evolution

IF 14 1区 化学 Q1 CHEMISTRY, APPLIED 能源化学 Pub Date : 2023-09-27 DOI:10.1016/j.jechem.2023.09.016
Jinglin Xian , Huiyu Jiang , Zhiao Wu , Huimin Yu , Kaisi Liu , Miao Fan , Rong Hu , Guangyu Fang , Liyun Wei , Jingyan Cai , Weilin Xu , Huanyu Jin , Jun Wan
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Abstract

The incorporation of partial A-site substitution in perovskite oxides represents a promising strategy for precisely controlling the electronic configuration and enhancing its intrinsic catalytic activity. Conventional methods for A-site substitution typically involve prolonged high-temperature processes. While these processes promote the development of unique nanostructures with highly exposed active sites, they often result in the uncontrolled configuration of introduced elements. Herein, we present a novel approach for synthesizing two-dimensional (2D) porous GdFeO3 perovskite with A-site strontium (Sr) substitution utilizing microwave shock method. This technique enables precise control of the Sr content and simultaneous construction of 2D porous structures in one step, capitalizing on the advantages of rapid heating and cooling (temperature ∼1100 K, rate ∼70 K s−1). The active sites of this oxygen-rich defect structure can be clearly revealed through the simulation of the electronic configuration and the comprehensive analysis of the crystal structure. For electrocatalytic oxygen evolution reaction application, the synthesized 2D porous Gd0.8Sr0.2FeO3 electrocatalyst exhibits an exceptional overpotential of 294 mV at a current density of 10 mA cm−2 and a small Tafel slope of 55.85 mV dec−1 in alkaline electrolytes. This study offers a fresh perspective on designing crystal configurations and the construction of nanostructures in perovskite.

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微波冲击激发二维多孔GdFeO3钙钛矿Sr取代高活性氧析出
在钙钛矿氧化物中加入部分a位取代是精确控制电子构型和提高其内在催化活性的一种有前途的策略。传统的a位取代方法通常涉及长时间的高温过程。虽然这些过程促进了具有高度暴露活性位点的独特纳米结构的发展,但它们往往导致引入元素的不受控制的配置。本文提出了一种利用微波激波法合成具有a位锶取代的二维(2D)多孔GdFeO3钙钛矿的新方法。该技术能够精确控制Sr含量,并在一步中同时构建2D多孔结构,利用快速加热和冷却(温度~ 1100 K,速率~ 70 K s−1)的优势。通过电子构型的模拟和晶体结构的综合分析,可以清楚地揭示这种富氧缺陷结构的活性位点。在电催化析氧反应中,合成的二维多孔Gd0.8Sr0.2FeO3电催化剂在10 mA cm−2电流密度下具有294 mV的过电位,在碱性电解质中具有55.85 mV dec−1的Tafel斜率。该研究为钙钛矿晶体结构的设计和纳米结构的构建提供了新的视角。
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CiteScore
23.60
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2875
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