Mohammad Nafeezuddin, Aravamudhan Shyam, Kuila Debasish
Department of Nanoengineering, Joint School of Nanoscience and Nanoengineering, Greensboro, NC 27401, USA.
Department of Chemistry, North Carolina A&T State University, Greensboro, NC 27411, USA.
Nanomaterials (Basel). 2022 Jul 15;12(14):2425. doi: 10.3390/nano12142425.
In recent years, rising environmental concerns have led to the focus on some of the innovative alternative technologies to produce clean burning fuels. Fischer-Tropsch (FT) synthesis is one of the alternative chemical processes to produce synthetic fuels, which has a current research focus on reactor and catalyst improvements. In this work, a cobalt nanofilm (~4.5 nm), deposited by the atomic layer deposition (ALD) technique in a silicon microchannel microreactor (2.4 cm long × 50 µm wide × 100 µm deep), was used as a catalyst for atmospheric Fischer-Tropsch (FT) synthesis. The catalyst film was characterized by XPS, TEM-EDX, and AFM studies. The data from AFM and TEM clearly showed the presence of polygranular cobalt species on the silicon wafer. The XPS studies of as-deposited and reduced cobalt nanofilm in silicon microchannels showed a shift on the binding energies of Co 2p spin splits and confirmed the presence of cobalt in the Co chemical state for FT synthesis. The FT studies using the microchannel microreactor were carried out at two different temperatures, 240 °C and 220 °C, with a syngas (H:CO) molar ratio of 2:1. The highest CO conversion of 74% was observed at 220 °C with the distribution of C-C hydrocarbons. The results showed no significant selectivity towards butane at the higher temperature, 240 °C. The deactivation studies were performed at 220 °C for 60 h. The catalyst exhibited long-term stability, with only ~13% drop in the CO conversion at the end of 60 h. The deactivated cobalt film in the microchannels was investigated by XPS, showing a weak carbon peak in the XPS spectra.
近年来,对环境问题的日益关注促使人们将焦点转向一些用于生产清洁燃烧燃料的创新替代技术。费托(FT)合成是生产合成燃料的替代化学工艺之一,目前的研究重点是反应器和催化剂的改进。在这项工作中,通过原子层沉积(ALD)技术在硅微通道微反应器(长2.4厘米×宽50微米×深100微米)中沉积的钴纳米膜(约4.5纳米)被用作常压费托(FT)合成的催化剂。通过XPS、TEM-EDX和AFM研究对催化剂膜进行了表征。AFM和TEM的数据清楚地表明硅片上存在多颗粒钴物种。对硅微通道中沉积态和还原态钴纳米膜的XPS研究表明,Co 2p自旋分裂的结合能发生了位移,并证实了FT合成中钴以Co化学态存在。使用微通道微反应器进行的FT研究在240℃和220℃两个不同温度下进行,合成气(H:CO)摩尔比为2:1。在220℃下观察到最高CO转化率为74%,同时有C-C烃类分布。结果表明,在较高温度240℃下对丁烷没有明显的选择性。失活研究在220℃下进行60小时。催化剂表现出长期稳定性,在60小时结束时CO转化率仅下降约13%。通过XPS对微通道中失活的钴膜进行了研究,结果显示XPS光谱中有一个弱碳峰。