Wang Yongsheng, Zhao Zhenzhen, Zhao Yunlu, Lan Xiaolin, Xu Weixiang, Chen Li, Guo Dongjie, Duan Zhengkang
College of Chemical Engineering, Xiangtan University Xiangtan 411105 Hunan China
Hunan Collaborative Innovation Center of New Chemical Technologies for Environmental Benignity and Efficient Resource Utilization Xiangtan 411105 Hunan China.
RSC Adv. 2019 Sep 25;9(52):30439-30447. doi: 10.1039/c9ra05458h. eCollection 2019 Sep 23.
The sintering resistance of supported Cu nanoparticle (NP) catalysts is crucial to their practical application in the dehydrogenation of diethanolamine (DEA). In this paper, co-precipitation, hydrothermal synthesis, and sol-gel condensation are used to form a new support material through chemical bonding between graphene oxide and ZrO. The composite carriers prepared by the three methods are mixed with copper nitrate and ground using a ball mill. A series of Cu/ZrO-reduced graphene oxide (RGO) composites were prepared by calcination under nitrogen at 450 °C for 3 h and hydrogen reduction at 250 °C for 4 h. The conversion of DEA to iminodiacetic acid (IDA) reached 96% with the Cu/ZrO-RGO catalyst prepared by hydrothermal synthesis. The conversion rate of DEA is more than 80% following the reuse of the CZG-2 catalyst for twelve cycles. The various physicochemical characterization techniques show that the Cu/ZrO-RGO layered and wrinkled nanostructures can improve catalytic stability and suppress the sintering of the supported Cu NPs during the catalytic dehydrogenation of diethanolamine. A synergistic effect between the RGO and the Cu nanoparticles is observed. The Cu nanoparticles with RGO have a better dispersibility, and a new nano-environment is created, which is the key to improving the efficiency of diethanolamine dehydrogenation. These new Cu/ZrO-RGO catalysts show increased durability compared to commercially produced Cu/ZrO catalysts and show promise for practical applications involving diethanolamine dehydrogenation.
负载型铜纳米颗粒(NP)催化剂的烧结抗性对其二乙醇胺(DEA)脱氢的实际应用至关重要。本文采用共沉淀法、水热合成法和溶胶 - 凝胶缩聚法,通过氧化石墨烯与ZrO之间的化学键合形成一种新型载体材料。用这三种方法制备的复合载体与硝酸铜混合并用球磨机研磨。通过在氮气气氛下450℃煅烧3小时和在250℃氢气还原4小时制备了一系列Cu/ZrO-还原氧化石墨烯(RGO)复合材料。水热合成法制备的Cu/ZrO-RGO催化剂使DEA转化为亚氨基二乙酸(IDA)的转化率达到96%。CZG-2催化剂重复使用十二次后,DEA的转化率超过80%。各种物理化学表征技术表明,Cu/ZrO-RGO层状和褶皱的纳米结构可以提高催化稳定性,并在二乙醇胺催化脱氢过程中抑制负载型Cu NPs的烧结。观察到RGO与铜纳米颗粒之间存在协同效应。具有RGO的铜纳米颗粒具有更好的分散性,并创造了一种新的纳米环境,这是提高二乙醇胺脱氢效率的关键。这些新型Cu/ZrO-RGO催化剂与商业生产的Cu/ZrO催化剂相比,耐久性增强,在涉及二乙醇胺脱氢的实际应用中显示出前景。