Dou Yuhai, Yuan Ding, Yu Linping, Zhang Weiping, Zhang Lei, Fan Kaicai, Al-Mamun Mohammad, Liu Porun, He Chun-Ting, Zhao Huijun
Centre for Catalysis and Clean Energy, Gold Coast Campus, Griffith University, Gold Coast, 4222, Australia.
Shandong Institute of Advanced Technology, Jinan, 250100, China.
Adv Mater. 2022 Jan;34(2):e2104667. doi: 10.1002/adma.202104667. Epub 2021 Nov 18.
Electronic structure engineering via integrating two defect structures with opposite modulation effects holds the key to fully unlocking the power of a catalyst. Herein, an interpolation principle is proposed to activate CoOOH via W doping and Co vacancies for the oxygen evolution reaction. Density functional theory suggests opposite roles for the W dopant and the Co vacancy but a synergy between them in tuning the electronic states of the Co site, leading to near-ideal intermediate energetics and dramatically lowered catalytic overpotential. Experimental studies confirm the modulation of the electronic structure and validate the greatly enhanced catalytic activity with a small overpotential of 298.5 mV to drive 50 mA cm . The discovery of the interpolation between dopants and vacancies opens up a new methodology to design efficient catalysts for various electrochemical reactions.
通过整合具有相反调制效应的两种缺陷结构来进行电子结构工程是充分释放催化剂潜力的关键。在此,提出了一种内插原理,通过W掺杂和Co空位来激活CoOOH以用于析氧反应。密度泛函理论表明W掺杂剂和Co空位具有相反的作用,但它们在调节Co位点的电子态方面具有协同作用,从而导致接近理想的中间体能量学并显著降低催化过电位。实验研究证实了电子结构的调制,并验证了在298.5 mV的小过电位下驱动50 mA cm时催化活性大大增强。掺杂剂和空位之间内插的发现为设计用于各种电化学反应的高效催化剂开辟了一种新方法。