化学
固氮
固定(群体遗传学)
超短脉冲
氮气
动能
光谱学
化学反应
猝灭(荧光)
离解(化学)
化学过程
反应机理
光化学
固碳
动力学同位素效应
同位素
大气压力
气泡
同位素标记
热力学平衡
化学工程
激光器
光解
化学物理
化学平衡
分析化学(期刊)
作者
Weiwei Cao,Yinwu Li,Bo Yan,Zhiping Zeng,Pu Liu,Rui Li,Jiuxing Jiang,Zhuofeng Ke,Guowei Yang
摘要
Ultrafast N2 fixation reactions are quite challenging. Currently used methods for N2 fixation are limited, and strong dinitrogen bonds usually need to be activated via extreme temperature or pressure or by the use of an energy-consuming process with sophisticated catalysts. Herein, we report a novel laser-based chemical method for N2 fixation under ambient conditions without catalysts, this method is called laser bubbling in liquids (LBL), and it directly activates N2 in water (H2O) and efficiently converts N2 into valuable NH3 (max: 4.2 mmol h-1) and NO3- (0.17 mmol h-1). Remarkably, the highest yields of NH3 and NO3- are 4 orders of magnitude greater than the best values for electrocatalysis reported to date. Notably, we further validate the experimental mechanism by using optical emission spectroscopy to detect the production of intermediate plasma and by employing isotope tracing. We also establish that an extremely high-temperature environment far from thermodynamic equilibrium inside a laser-induced bubble and the kinetic process of rapid quenching of bubbles is crucial for N2 activation and fixation to generate NH3 and NOx via LBL. Based on these results, it is shown that LBL is a simple, safe, efficient, green, and sustainable technology that enables the rapid conversion of the renewable feedstocks H2O and N2 to NH3 and NO3-, facilitating new prospects for chemical N2 fixation.
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