Cheng Shaoan, Li Chaochao, Yu Zhen, Sun Yi, Li Longxin, Yang Jiawei
State Key Laboratory of Clean Energy Utilization, Department of Energy Engineering, Zhejiang University Hangzhou 310027 PR China
RSC Adv. 2020 Mar 6;10(17):9814-9823. doi: 10.1039/d0ra00155d.
The electroreduction of nitrogen (N) has gained increasing attention as a promising route to achieve green and sustainable ammonia (NH) production. However, the construction of an active and durable electrocatalyst for N reduction reaction (NRR) remains a significant challenge. Herein, we, for the first time, report that S/N co-doped carbon cloth (CC) with abundant defects can serve as an efficient NRR electrocatalyst at ambient conditions. The S/N co-doped CC was prepared through a novel one-step method by using ammonium persulfate (APS) as the source of nitrogen and sulfur. The catalyst prepared at 800 °C (CC-APS 800) showed abundant defects and heteroatoms as the active and stable electrocatalytic sites for NH electrosynthesis. Based on this, a sizeable NH yield of 9.87 × 10 mol s cm and high faradaic efficiency of 8.11% were obtained in 0.05 M HSO at -0.3 V ( reversible hydrogen electrode, RHE), respectively. Furthermore, the electrocatalytic mechanism on CC-APS 800 was elucidated using the electrochemical Fourier transform infrared technique, and follows an associative reaction pathway. Our work would provide a new guideline for designing metal-free self-standing electrocatalysts for the NRR and other applications.
作为实现绿色可持续氨（NH₃）生产的一条有前景的途径，氮（N₂）的电还原受到了越来越多的关注。然而，构建一种用于氮还原反应（NRR）的活性和耐久性电催化剂仍然是一项重大挑战。在此，我们首次报道具有大量缺陷的硫/氮共掺杂碳布（CC）可在环境条件下作为高效的NRR电催化剂。硫/氮共掺杂CC是通过一种新颖的一步法制备的，使用过硫酸铵（APS）作为氮和硫的来源。在800℃制备的催化剂（CC-APS 800）表现出大量缺陷和杂原子，作为NH₃电合成的活性和稳定电催化位点。基于此，在-0.3V（可逆氢电极，RHE）的0.05M H₂SO₄中分别获得了9.87×10⁻¹⁰mol s⁻¹ cm⁻²的可观NH₃产率和8.11%的高法拉第效率。此外，使用电化学傅里叶变换红外技术阐明了CC-APS 800上的电催化机理，并遵循缔合反应途径。我们的工作将为设计用于NRR和其他应用的无金属自支撑电催化剂提供新的指导方针。
