Ziyi Wan, Ping Tang, Luwei Dai, Yao Yang, Lu Li, Jun Liu, Min Yang, Guowei Deng
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引用次数: 1
摘要
合理设计镍基催化剂是实现高效、可持续能源转化的关键。然而,对于碱性电解质中的电催化材料,活性位点的原子水平控制是必不可少的。此外,明确的表面结构有助于更深入地了解催化机理。在这里,我们报道了在丝绸炭化后加载缺陷镍钴层状双氢氧化物纳米片(Ni2Co-LDH@C)。在催化活性位点局部配位环境的精确调控和缺陷的存在下,Ni2Co-LDH@C可以在10 mA cm−2下为析氢反应(HERs)提供164.8 mV的超低过电位,超过了商用Pt/C催化剂的过电位。密度泛函理论计算表明,Ni2Co-LDH@C优化了中间体的吸附能,促进了析氧反应中活性位点的O-O偶联。当使用Ni2Co-LDH@Cs作为阴极和阳极来实现整体的水分解时,需要1.63 V的低电压来实现10 mA cm−2的电流密度。Ni2Co-LDH@C作为一种理想模型,具有优异的水裂解性能,具有开发水碱电催化剂的潜力。
Highly Effective Electrochemical Water Splitting with Enhanced Electron Transfer between Ni2Co Layered Double Hydroxide Nanosheets Dispersed on Carbon Substrate
A reasonable design of nickel-based catalysts is key to efficient and sustainable energy conversion. For electrocatalytic materials in alkaline electrolytes, however, atomic-level control of the active sites is essential. Moreover, the well-defined surface structure contributes to a deeper understanding of the catalytic mechanism. Here, we report the loading of defective nickel–cobalt layered double hydroxide nanosheets (Ni2Co-LDH@C) after carbonization of silk. Under the precise regulation of the local coordination environment of the catalytic active site and the presence of defects, Ni2Co-LDH@C can provide an ultra-low overpotential of 164.8 mV for hydrogen evolution reactions (HERs) at 10 mA cm−2, exceeding that of commercial Pt/C catalysts. Density functional theory calculations show that Ni2Co-LDH@C optimizes the adsorption energy of the intermediate and promotes the O-O coupling of the active site in the oxygen evolution reaction. When using Ni2Co-LDH@Cs as cathodes and anodes to achieve overall water splitting, a low voltage of 1.63 V is required to achieve a current density of 10 mA cm−2. As an ideal model, Ni2Co-LDH@C has excellent water splitting properties and has the potential to develop water–alkali electrocatalysts.