Xu Xiaolong, Liu Xuejing, Zhao Jinxiu, Wu Dan, Du Yu, Yan Tao, Zhang Nuo, Ren Xiang, Wei Qin
Key Laboratory of Interfacial Reaction & Sensing Analysis in Universities of Shandong, School of Chemistry and Chemical Engineering, University of Jinan, Jinan, Shandong 250022, China.
Key Laboratory of Interfacial Reaction & Sensing Analysis in Universities of Shandong, School of Chemistry and Chemical Engineering, University of Jinan, Jinan, Shandong 250022, China; Collaborative Innovation Center for Green Chemical Manufacturing and Accurate Detection, Jinan, Shandong 250022, China.
J Colloid Interface Sci. 2022 Jan 15;606(Pt 2):1374-1379. doi: 10.1016/j.jcis.2021.08.099. Epub 2021 Aug 18.
The electrocatalytic reduction of nitrogen (N) to ammonia (NH) has broad prospects for green and sustainable NH production. Due to the electrocatalytic nitrogen reduction reaction (eNRR) performance of transition metal compound may be restricted with low yield rate, we develop transition metal interface engineering to improve the eNRR performance. Although the edge of MoS catalyst is active, the MoS(001) surface is inert for N electroreduction. Through the hydrothermal and electrodeposition methods, Fe(OH) as N and H channels coated on MoS nanosheets array (MoS@Fe(OH)/CC) is synthesized. Such catalyst exhibits excellent eNRR performance in 0.1 M NaSO with high Faradaic efficiency (2.76%) and NH yield rate (4.23 × 10 mol s cm) at - 0.45 V (vs. RHE). This work may provide a new electrocatalyst synthesis pathway for artificial N fixation. Density functional theory calculations show that electrodeposition Fe(OH) can accelerate eNRR process rate of MoS.
将氮气（N）电催化还原为氨（NH₃）在绿色可持续的氨生产方面具有广阔前景。由于过渡金属化合物的电催化氮还原反应（eNRR）性能可能因产率低而受到限制，我们开展了过渡金属界面工程以改善eNRR性能。尽管MoS₂催化剂的边缘具有活性，但MoS₂(001)表面对氮电还原是惰性的。通过水热和电沉积方法，合成了作为氮和氢通道的Fe(OH)₃包覆在MoS₂纳米片阵列上（MoS₂@Fe(OH)₃/CC）。这种催化剂在0.1 M Na₂SO₄中表现出优异的eNRR性能，在-0.45 V（相对于可逆氢电极，RHE）时具有高法拉第效率（2.76%）和氨产率（4.23×10⁻¹¹ mol s⁻¹ cm⁻²）。这项工作可能为人工固氮提供一种新的电催化剂合成途径。密度泛函理论计算表明，电沉积Fe(OH)₃可以加速MoS₂的eNRR过程速率。
