Chen Ziliang, Wu Jie, Chen Zhengran, Yang Hongyuan, Zou Kai, Zhao Xiangyong, Liang Ruihong, Dong Xianlin, Menezes Prashanth W, Kang Zhenhui
Institute of Functional Nano and Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-based Functional Materials and Devices, Joint International Research Laboratory of Carbon-Based Functional Materials and Devices, Soochow University, Suzhou, 215123, China.
Department of Chemistry: Metalorganics and Inorganic Materials, Technische Universität Berlin, Straße des 17 Juni 135, Sekr. C2, 10623, Berlin, Germany.
Angew Chem Int Ed Engl. 2022 May 16;61(21):e202200086. doi: 10.1002/anie.202200086. Epub 2022 Mar 23.
The electrochemical oxygen reduction reaction (ORR) offers a most promising and efficient route to produce hydrogen peroxide (H O ), yet the lack of cost-effective and high-performance electrocatalysts have restricted its practical application. Herein, an entropy-enhancement strategy has been employed to enable the low-cost perovskite oxide to effectively catalyze the electrosynthesis of H O . The optimized Pb(NiWMnNbZrTi) O ceramic is available on a kilogram-scale and displays commendable ORR activity in alkaline media with high selectivity over 91 % across the wide potential range for H O including an outstanding degradation property for organic dyes through the Fenton process. The exceptional performance of this perovskite oxide is attributed to the entropy stabilization-induced polymorphic transformation assuring the robust structural stability, decreased charge mobility as well as synergistic catalytic effects which we confirm using advanced in situ Raman, transient photovoltage, Rietveld refinement as well as finite elemental analysis.
电化学氧还原反应（ORR）为生产过氧化氢（H₂O₂）提供了一条最具前景且高效的途径，然而缺乏具有成本效益的高性能电催化剂限制了其实际应用。在此，采用了一种熵增强策略，使低成本的钙钛矿氧化物能够有效地催化H₂O₂的电合成。优化后的Pb(NiW0.5Mn0.5Nb0.2Zr0.1Ti0.2)O₃陶瓷可实现千克级规模生产，在碱性介质中表现出值得称赞的ORR活性，在包括通过芬顿过程对有机染料具有出色降解性能的H₂O₂宽电位范围内，选择性高达91%以上。这种钙钛矿氧化物的优异性能归因于熵稳定诱导的多晶型转变，确保了强大的结构稳定性、降低的电荷迁移率以及协同催化效应，我们使用先进的原位拉曼光谱、瞬态光电压、Rietveld精修以及有限元分析对其进行了确认。
