Electronic structure reconfiguration of nickel–cobalt layered double hydroxide nanoflakes via engineered heteroatom and oxygen-vacancies defect for efficient electrochemical water splitting

氢氧化物 双功能 杂原子 电化学 材料科学 分解水 析氧 过电位 化学工程 塔菲尔方程 无机化学 化学 冶金 催化作用 电极 有机化学 戒指(化学) 工程类 物理化学 光催化
作者
Kai Chen,Yonghua Cao,Sunny Yadav,Gyu-Cheol Kim,Zheng Han,Wenmeng Wang,Weijin Zhang,Dung Van Dao,In-Hwan Lee
出处
期刊:Chemical Engineering Journal [Elsevier BV]
卷期号:463: 142396-142396 被引量:94
标识
DOI:10.1016/j.cej.2023.142396
摘要

The development of earth-abundant and high-efficiency bifunctional electrocatalysts is extremely desirable for electrochemical water splitting, but there are some critical challenges that need to be addressed. The coordinated tailoring of electronic structure and Bader charge transference by heteroatom doping and oxygen vacancy defects are one of the strongest tactics to enhance the oxygen and hydrogen evolution reactions (OER and HER) of catalysts. Herein, a novel Mo-decorated nickel–cobalt layered double hydroxides 3D honeycomb nanoflake on Ni foam (labeled as Mo-NiCo LDHs(Vo)) as bifunctional electrode materials with enriched oxygen vacancy defects, excellent geometric stability, and enriched active sites was successfully fabricated through a facile hydrothermal reaction strategy. Density functional theory computations and experimental results confirmed that the electrocatalytic intrinsic activity of Mo-NiCo LDHs(Vo) was optimized not only because of the provision of new active sites by the Mo dopants via the construction of defects and oxygen vacancies but also because of the activation of the local electronic structures of the surrounding Ni and Co sites. Consequently, Mo-NiCo LDHs(Vo) exhibited outstanding electrocatalytic performance with an overpotential of 258 mV for OER and 194 mV for HER at a current density of 10 mA/cm2 in an alkaline medium. In addition, the catalyst exhibited excellent long-term stability after 100 h of use as a bifunctional electrode for overall water splitting. This work provides a facile means to fabricate superior, efficient noble metal-free catalysts with well-designed defects at the atomic-level using electronic structure engineering for energy-related applications.
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