Yu Xinru, Qiu Peng, Wang Yongchao, He Bing, Xu Xiangran, Zhu Huiling, Ding Jian, Liu Xueqin, Li Zhen, Wang Yang
Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430074, PR China.
Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430074, PR China.
J Colloid Interface Sci. 2023 Jun 15;640:775-782. doi: 10.1016/j.jcis.2023.03.010. Epub 2023 Mar 7.
Photocatalytic ammonia synthesis technology has become one of the effective methods to replace the Haber method for nitrogen fixation in the future for its low energy consumption and green environment. However, limited by the weak adsorption/activation ability of N molecules at the photocatalyst interface, the efficient nitrogen fixation still remains a daunting job. Defect-induced charge redistribution as a catalytic site for N molecules is the most prominent strategy to enhance the adsorption/activation of N molecules at the interface of catalysts. In this study, MoO nanowires containing asymmetric defects were prepared by a one-step hydrothermal method via using glycine as a defect inducer. It is shown that at the atomic scale, the defect-induced charge reconfiguration can significantly improve the nitrogen adsorption and activation capacity and enhance the nitrogen fixation capacity; at the nanoscale, the charge redistribution induced by asymmetric defects effectively improved the photogenerated charge separation. Given the charge redistribution on the atomic and nanoscale of MoO nanowires, the optimal nitrogen fixation rate of MoO reached 200.35 µmol gh.
光催化氨合成技术因其低能耗和环境友好,已成为未来替代哈伯固氮法的有效方法之一。然而,受光催化剂界面处N分子吸附/活化能力较弱的限制,高效固氮仍然是一项艰巨的任务。缺陷诱导的电荷重新分布作为N分子的催化位点,是增强催化剂界面处N分子吸附/活化的最突出策略。在本研究中,通过一步水热法,以甘氨酸作为缺陷诱导剂制备了含有不对称缺陷的MoO纳米线。结果表明,在原子尺度上,缺陷诱导的电荷重新配置可显著提高氮吸附和活化能力,并增强固氮能力;在纳米尺度上,不对称缺陷诱导的电荷重新分布有效改善了光生电荷分离。鉴于MoO纳米线在原子和纳米尺度上的电荷重新分布,MoO的最佳固氮速率达到200.35 µmol g⁻¹ h⁻¹。