Nan Cheng, Yang Huimin, Gao Fanfan, Gao Nan, Zhou Wenjing, Du Haiyan, Liang Zhenhai
College of Chemistry, Taiyuan University of Technology, Taiyuan, 030024, China) (Huimin Yang.
Chempluschem. 2023 Mar;88(3):e202300023. doi: 10.1002/cplu.202300023.
As a green and sustainable strategy, the electrocatalytic N reduction reaction (NRR) has been considered the best potential approach to replace the traditional Haber-Bosch process under ambient conditions. The key is to exploit efficient and low-cost electrocatalysts according to the current situation. Herein, a series of Molybdenum (Mo) doped CeO nanorods (NR) catalysts were successfully fabricated via a hydrothermal reaction coupled with high temperature calcination. The nanorod structures were not altered after Mo atom doping. The obtained 5 %-Mo-CeO nanorods act as a superior electrocatalyst in neutral electrolytes of 0.1 M Na SO . Such electrocatalyst significantly enhances NRR performance with an NH yield of 10.9 μg h mg at -0.45 V vs reversible hydrogen electrode (RHE) and a Faradaic efficiency (FE) of 26.5 % at -0.25 V vs RHE. That outcome is 4 times higher than that of CeO nanorods (2.6 μg h mg ; 4.9 %). Meanwhile, density functional theory (DFT) calculation shows the characteristics after Mo doping: the band gap value lowers, the density of states increases, electrons are more easily excited, and N molecules are more easily adsorbed, thereby enhancing the activity of the electrocatalytic NRR.
作为一种绿色可持续的策略，电催化氮还原反应（NRR）被认为是在环境条件下替代传统哈伯-博施法的最具潜力的方法。关键在于根据当前情况开发高效且低成本的电催化剂。在此，通过水热反应结合高温煅烧成功制备了一系列钼（Mo）掺杂的CeO纳米棒（NR）催化剂。Mo原子掺杂后纳米棒结构未改变。所制备的5%-Mo-CeO纳米棒在0.1 M Na₂SO₄中性电解质中作为优异的电催化剂。这种电催化剂显著提高了NRR性能，在相对于可逆氢电极（RHE）为-0.45 V时NH₃产率为10.9 μg h⁻¹ mg⁻¹，在相对于RHE为-0.25 V时法拉第效率（FE）为26.5%。该结果比CeO纳米棒的结果（2.6 μg h⁻¹ mg⁻¹；4.9%）高4倍。同时，密度泛函理论（DFT）计算表明了Mo掺杂后的特性：带隙值降低，态密度增加，电子更容易被激发，N₂分子更容易被吸附，从而增强了电催化NRR的活性。
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