Song Fujiao, Gao Jia, Yang Bairen, Cao Yan, Liu Huanhuan, Xu Qi
Key Laboratory Under Construction for Volatile Organic Compounds Controlling of Jiangsu Province, School of Environmental Science and Engineering, Yancheng Institute of Technology, Yancheng, China.
School of Chemistry and Chemical Engineering, Jiangsu University, Zhengjiang, China.
Front Chem. 2023 May 23;11:1187762. doi: 10.3389/fchem.2023.1187762. eCollection 2023.
CuInZr-O-C catalysts with CuIn alloy structure were prepared by using the sol-gel method. CuInZr-O-PC and CuInZr-O-CP catalysts were obtained from plasma-modified CuInZr-O-C before and after calcination, respectively. Under the conditions of reaction temperature 270°C, reaction pressure 2 MPa, CO/H = 1/3, and GHSV = 12,000 mL/(g h), CuInZr-O-PC catalyst has a high CO conversion of 13.3%, methanol selectivity of 74.3%, and CHOH space-time yield of 3.26 mmol/gcat/h. The characterization results of X-ray diffraction (XRD), scanning electron microscopy (SEM), and temperature-programmed reduction chemisorption (H-TPR) showed that the plasma-modified catalyst had a low crystallinity, small particle size, good dispersion, and excellent reduction performance, leading to a better activity and selectivity. Through plasma modification, the strong interaction between Cu and In in CuInZr-O-CP catalyst, the shift of Cu 2p orbital binding energy to a lower position, and the decrease in reduction temperature all indicate that the reduction ability of CuInZr-O-CP catalyst is enhanced, and the CO hydrogenation activity is improved.
采用溶胶-凝胶法制备了具有CuIn合金结构的CuInZr-O-C催化剂。CuInZr-O-PC和CuInZr-O-CP催化剂分别是由等离子体改性的CuInZr-O-C在煅烧前后获得的。在反应温度270°C、反应压力2MPa、CO/H = 1/3、气体时空速(GHSV)= 12000 mL/(g h)的条件下,CuInZr-O-PC催化剂具有13.3%的高CO转化率、74.3%的甲醇选择性和3.26 mmol/gcat/h的CHOH时空产率。X射线衍射(XRD)、扫描电子显微镜(SEM)和程序升温还原化学吸附(H-TPR)的表征结果表明,等离子体改性催化剂具有低结晶度、小粒径、良好的分散性和优异的还原性能,从而具有更好的活性和选择性。通过等离子体改性,CuInZr-O-CP催化剂中Cu与In之间的强相互作用、Cu 2p轨道结合能向较低位置的移动以及还原温度的降低均表明CuInZr-O-CP催化剂的还原能力增强,CO加氢活性提高。