Yang Xinyu, Liu Yifeng, Chen Qianqiao, Yu Wanchin, Zhong Qin
School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, China.
Wanhua Chemical Group Co., Ltd., Yantai Development Zone,Yantai 264002, Shandong, China.
Langmuir. 2024 Nov 19;40(46):24605-24612. doi: 10.1021/acs.langmuir.4c03343. Epub 2024 Nov 6.
Urea oxidation reaction (UOR) is an attractive alternative anodic reaction to oxygen evolution reaction (OER) for its low thermodynamic potential (0.37 V vs RHE). A major challenge that prohibits its practical application is the six-electron transfer process during UOR, demanding enhancements in the catalytic activity. Herein, a Fe-doped NiS catalyst with a uniform flower-like structure is synthesized on nickel foam via a simple one-step hydrothermal method. The electrochemical properties of Fe-NiS are significantly improved since a current density of 10 mA cm only requires a 1.33 V potential and remains stable for 60 h. The structural characterization demonstrates a strong interaction between Fe and NiS. After Fe doping, the active site increases, which promotes the formation of NiOOH on the catalyst surface, thus speeding up the UOR process. These changes are beneficial to charge transfer and optimize the adsorption energy of the intermediates. EIS further confirms that Fe promotes electron transfer during the UOR process, reduces the interface resistance between the catalyst and the electrolyte, and lowers the driving voltage.
尿素氧化反应（UOR）因其较低的热力学电位（相对于可逆氢电极，RHE为0.37 V），是一种有吸引力的替代析氧反应（OER）的阳极反应。阻碍其实际应用的一个主要挑战是UOR过程中的六电子转移过程，这需要提高催化活性。在此，通过简单的一步水热法在泡沫镍上合成了具有均匀花状结构的铁掺杂硫化镍催化剂。铁掺杂硫化镍（Fe-NiS）的电化学性能显著提高，因为10 mA cm²的电流密度仅需1.33 V的电位，并且在60小时内保持稳定。结构表征表明铁与硫化镍之间存在强相互作用。铁掺杂后，活性位点增加，促进了催化剂表面NiOOH的形成，从而加速了UOR过程。这些变化有利于电荷转移，并优化了中间体的吸附能。电化学阻抗谱（EIS）进一步证实，铁在UOR过程中促进电子转移，降低了催化剂与电解质之间的界面电阻，并降低了驱动电压。
