Li Huabo, Cui Yuanyuan, Liu Yixin, Wang Songlin, Dai Wei-Lin
School of Chemistry and Chemical Engineering, Henan Institute of Science and Technology, Xinxiang 453003, Henan Province, People's Republic of China.
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200433, People's Republic of China.
Nanotechnology. 2022 Aug 5;33(43). doi: 10.1088/1361-6528/ac8233.
The hydrogenation of CO-derived carbonates to methanol is an alternative route for the indirect utilization of abundant C1 sources. Various Cu/SiOcatalysts with different copper loading content prepared by using an ammonia evaporation hydrothermal method are implemented to evaluate the catalytic performance of ethylene carbonate (EC) hydrogenation to methanol and ethylene glycol (EG). The Cu loading content was identified to significantly affect the Cu nanoparticles (NPs) size and metal-support interaction. Highly dispersed Cu NPs restricted and embedded in copper phyllosilicate presented a smaller average particle size than the impregnated Cu/SiO-IM catalyst. TheCu/SiOcatalyst with ultrafine Cu NPs showed abundant Cu-O-Si interfaces, acidic sites, and coherent Cuand Cuspecies. The 5Cu/SiOcatalyst achieved methanol yield of 76% and EG yield of 98% at EC conversion of 99%, and no obvious deactivation was observed after long-term operation. The superior catalytic performance of the 5Cu/SiOcatalyst is attributed to the synergetic effect between the appropriate Cusurface area which provides sufficient active hydrogen, and the atomic ratio of Cufor the polarization and activation of carbon-oxygen bonds.
将源自一氧化碳的碳酸盐加氢制甲醇是间接利用丰富的C1资源的一条替代途径。采用氨蒸发水热法制备了不同铜负载量的各种Cu/SiO催化剂,用于评价碳酸乙烯酯(EC)加氢制甲醇和乙二醇(EG)的催化性能。结果表明,铜负载量显著影响铜纳米颗粒(NPs)的尺寸和金属-载体相互作用。高度分散且嵌入层状硅酸铜中的Cu NPs的平均粒径比浸渍法制备的Cu/SiO-IM催化剂更小。具有超细Cu NPs的Cu/SiO催化剂具有丰富的Cu-O-Si界面、酸性位点以及相干的Cu和Cu物种。5Cu/SiO催化剂在EC转化率为99%时,甲醇产率达到76%,EG产率达到98%,并且在长期运行后未观察到明显失活。5Cu/SiO催化剂优异的催化性能归因于提供充足活性氢的合适Cu表面积与用于碳-氧键极化和活化的Cu原子比之间的协同效应。