Rostami Shahrbanoo, Tayebee Reza, Mahdavi Behnam
Department of Chemistry, School of Sciences, Hakim Sabzevari University Sabzevar Iran
RSC Adv. 2023 Oct 26;13(45):31303-31313. doi: 10.1039/d3ra03921h.
The production of ammonia as an important raw material in the chemical, agricultural, and food industries has been always a significant concern. However, conventional ammonia production methods require high energy consumption and costs. The photocatalytic rotes use green light sources and cost-effective photocatalysts to obtain ammonia from water under aerobic conditions and preventing production of greenhouse gases in the environment. To produce an effective heterogeneous catalyst, a new tetraphenylporphyrin-heteropolyacid (TPP-HPA) nanohybrid material is synthesized and loaded onto Ni nanoparticles in this work. Then, FE-SEM, EDS, XRD, and FT-IR analyses were applied to characterize the prepared nanohybrid material Ni@TPP-HPA. After that, the new inorganic-organic nanohybrid photocatalyst was introduced as an effective, environmental friendly, and recyclable mediator for N photofixation. The results showed that Ni@TPP-HPA is a good photocatalyst for the N fixation reaction and can be easily recycled without losing its activity for at least five runs. The Ni@TPP-HPA nanocomposite demonstrated the maximum ammonia generation by 2760 μmol L g under mild conditions when using methanol as a hole scavenger. Additionally, effects of solvent type, temperature, reaction time, irradiation source, solution pH, and other electron scavengers on the rate of NH production were investigated and discussed.
氨作为化学、农业和食品工业中的一种重要原料,其生产一直备受关注。然而,传统的氨生产方法需要高能耗和高成本。光催化路线利用绿色光源和具有成本效益的光催化剂,在有氧条件下从水中获取氨,并防止环境中温室气体的产生。在这项工作中,合成了一种新型的四苯基卟啉-杂多酸(TPP-HPA)纳米杂化材料,并将其负载到镍纳米颗粒上,以制备一种有效的多相催化剂。然后,应用场发射扫描电子显微镜(FE-SEM)、能谱仪(EDS)、X射线衍射仪(XRD)和傅里叶变换红外光谱仪(FT-IR)对制备的纳米杂化材料Ni@TPP-HPA进行表征。之后,将这种新型的无机-有机纳米杂化光催化剂作为一种有效、环保且可回收的氮光固定介质引入。结果表明,Ni@TPP-HPA是一种用于氮固定反应的良好光催化剂,并且可以很容易地回收利用,至少经过五次循环仍不会失去其活性。当使用甲醇作为空穴清除剂时,Ni@TPP-HPA纳米复合材料在温和条件下表现出最大氨生成量为2760 μmol L⁻¹ g⁻¹。此外,还研究并讨论了溶剂类型、温度、反应时间、辐照源、溶液pH值以及其他电子清除剂对氨生成速率的影响。