Science Bulletin ( IF 18.8 ) Pub Date : 2019-05-16 , DOI: 10.1016/j.scib.2019.05.009 Xiang Gao 1 , Li An 2 , Dan Qu 2 , Wenshuai Jiang 2 , Yanxiao Chai 2 , Shaorui Sun 2 , Xingyuan Liu 3 , Zaicheng Sun 2
Photocatalytic N2 fixation involves a nitrogen reduction reaction on the surface of the photocatalyst to convert N2 into ammonia. Currently, the adsorption of N2 is the limiting step for the N2 reduction reaction on the surface of the catalyst. Based on the concept of photocatalytic water splitting, the photocatalytic efficiency can be greatly enhanced by introducing a co-catalyst. In this report, we proposed a new strategy, namely, the loading of a NiS co-catalyst on CdS nanorods for photocatalytic N2 fixation. Theoretical calculation results indicated that N2 was effectively adsorbed onto the NiS/CdS surface. Temperature programmed desorption studies confirmed that the N2 molecules preferred to adsorb onto the NiS/CdS surface. Linear sweep voltammetry results revealed that the overpotential of the N2 reduction reaction was reduced by loading NiS. Furthermore, transient photocurrent and electrochemical impedance spectroscopy indicated that the charge separation was enhanced by introducing NiS. Photocatalytic N2 fixation was carried out in the presence of the catalyst dispersed in water without any sacrificial agent. As a result, 1.0 wt% NiS/CdS achieved an ammonia production rate of 2.8 and 1.7 mg L−1 for the first hour under full spectrum and visible light (λ > 420 nm), respectively. The catalyst demonstrated apparent quantum efficiencies of 0.76%, 0.39% and 0.09% at 420, 475 and 520 nm, respectively. This study provides a new method to promote the photocatalytic efficiency of N2 fixation.
中文翻译:
通过用助催化剂促进 N2 吸附来增强光催化 N2 固定
光催化N 2固定涉及光催化剂表面上的氮还原反应以将N 2转化为氨。目前,N 2 的吸附是催化剂表面N 2还原反应的限制步骤。基于光催化水分解的概念,通过引入助催化剂可以大大提高光催化效率。在本报告中,我们提出了一种新策略,即在 CdS 纳米棒上负载 NiS 助催化剂用于光催化 N 2固定。理论计算结果表明,N 2被有效地吸附到NiS/CdS表面。程序升温脱附研究证实,N2 个分子优先吸附到 NiS/CdS 表面。线性扫描伏安法结果表明负载NiS降低了N 2还原反应的过电位。此外,瞬态光电流和电化学阻抗谱表明,通过引入 NiS 可以增强电荷分离。在没有任何牺牲剂的情况下,在分散在水中的催化剂存在下进行光催化N 2固定。结果,1.0 wt% NiS/CdS在全光谱和可见光下第一个小时的氨产量分别为 2.8 和 1.7 mg L -1 ( λ > 420 纳米),分别。该催化剂在 420、475 和 520 nm 处的表观量子效率分别为 0.76%、0.39% 和 0.09%。该研究为提高N 2固定的光催化效率提供了一种新方法。