Journal of Energy Chemistry ( IF 14.0 ) Pub Date : 2024-01-04 , DOI: 10.1016/j.jechem.2023.12.028
Chongchong Liu , Peifang Wang , Bin Hu , Xiaoli Liu , Rong Huang , Gang Zhou
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Urea oxidation reaction (UOR) is proposed as an exemplary half-reaction in renewable energy applications because of its low thermodynamical potential. However, challenges persist due to sluggish reaction kinetics and complex by-products separation. To this end, we introduce the lattice oxygen oxidation mechanism (LOM), propelling a novel UOR route using a modified CoFe layered double hydroxide (LDH) catalyst termed CFRO-7. Theoretical calculations and in-situ characterizations highlight the activated lattice oxygen (OL) within CFRO-7 as pivotal sites for UOR, optimizing the reaction pathway and accelerating the kinetics. For the urea overall electrolysis application, the LOM route only requires a low voltage of 1.54 V to offer a high current of 100 mA cm−2 for long-term utilization (>48 h). Importantly, the by-product NCO− is significantly suppressed, while the CO2/N2 separation is efficiently achieved. This work proposed a pioneering paradigm, invoking the LOM pathway in urea electrolysis to expedite reaction dynamics and enhance product selectivity.
中文翻译:
![](https://scdn.x-mol.com/jcss/images/paperTranslation.png)
不对称构型通过削弱dp轨道杂化激活晶格氧以实现尿素整体电解中有效的C/N分离
尿素氧化反应(UOR)因其热力学势低而被提议作为可再生能源应用中的示例性半反应。然而,由于反应动力学缓慢和副产物分离复杂,挑战仍然存在。为此,我们引入了晶格氧氧化机制(LOM),使用称为CFRO-7的改性CoFe层状双氢氧化物(LDH)催化剂推动了一种新型UOR路线。理论计算和原位表征强调 CFRO-7 内的活化晶格氧 (O L ) 作为 UOR 的关键位点,优化反应途径并加速动力学。对于尿素整体电解应用,LOM路线仅需要1.54 V的低电压即可提供100 mA cm -2的高电流以供长期使用(>48 h)。重要的是,副产物NCO -被显着抑制,同时有效地实现了CO 2 /N 2分离。这项工作提出了一个开创性的范例,在尿素电解中调用 LOM 途径来加速反应动力学并提高产物选择性。