Chem ( IF 19.1 ) Pub Date : 2022-02-04 , DOI: 10.1016/j.chempr.2022.01.004 Sen Wang 1, 2 , Li Zhang 1, 3 , Pengfei Wang 1 , Xingchen Liu 1 , Yanyan Chen 1 , Zhangfeng Qin 1 , Mei Dong 1 , Jianguo Wang 1, 2 , Lin He 2, 4 , Unni Olsbye 5 , Weibin Fan 1
Conversion of CO2 into light olefins is an effective strategy for sustainable utilization of fossil energy and biomass. However, highly selective production of specific olefin, such as ethene, from CO2 hydrogenation is a challenge. Thus, a new catalyst consisting of Cr2O3(SG) oxide and H-SAPO-34 zeolite is fabricated. It shows C2=−C4= selectivity in hydrocarbons as high as 95.7% at 370°C and 0.5 MPa. More interestingly, around 74% of light olefins are ethene, with an ethene/propene (E/P) ratio of 3.1, which is three times that of previously reported results. This catalytic performance is well maintained for at least 600 h. In situ spectroscopy, DFT calculation, and MD simulation results reveal that ethanol, in addition to methanol, is produced on Cr2O3(SG) through successive hydrogenations of CH3COO∗ intermediate, which is generated through the reaction of H3CO∗ with CO2 and H∗. The ethanol is quickly converted into ethene on H-SAPO-34 and is responsible for the primary light olefin distribution.
中文翻译:
将二氧化碳高效转化为富含乙烯的轻质烯烃
将CO 2转化为轻质烯烃是可持续利用化石能源和生物质的有效策略。然而,从 CO 2加氢中高选择性地生产特定烯烃(例如乙烯)是一项挑战。因此,制备了由Cr 2 O 3 (SG) 氧化物和H-SAPO-34 沸石组成的新型催化剂。它表明在 370°C 和 0.5 MPa 条件下,C 2 = -C 4 =在烃类中的选择性高达 95.7%。更有趣的是,大约 74% 的轻质烯烃是乙烯,乙烯/丙烯 (E/P) 比为 3.1,是先前报道结果的三倍。这种催化性能可以很好地保持至少 600 小时。原位光谱、DFT 计算和 MD 模拟结果表明,除了甲醇之外,乙醇还通过 CH 3 COO* 中间体的连续氢化在 Cr 2 O 3 (SG)上生成,该中间体通过 H 3 CO* 与CO 2和 H*。乙醇在 H-SAPO-34 上迅速转化为乙烯,并负责初级轻烯烃的分布。