Liu Shike, Yang Kun, Ren Qixia, Liu Fei, Yao Mengqin, Ma Jun, Geng Shuo, Cao Jianxin
Department of Chemical Engineering, School of Chemistry and Chemical Engineering, Guizhou University, Guiyang, Guizhou, 550025, China.
Guizhou Key Laboratory for Green Chemical and Clean Energy Technology, Guizhou University, Guiyang, Guizhou, 550025, China.
Chemistry. 2024 Jul 11;30(39):e202400223. doi: 10.1002/chem.202400223. Epub 2024 Jun 17.
We proposed a new strategy for CO hydrogenation to prepare light olefins by introducing Zn into GaZrO to construct ZnGaZrO ternary oxides, which was combined with SAPO-34 to prepare a high-performance ZnGaZrO/SAPO-34 tandem catalyst for CO hydrogenation to light olefins. By optimizing the Zn doping content, the ratio and mode of the two-phase composite, and the process conditions, the 3.5 %ZnGaZrO/SAPO-34 tandem catalyst showed excellent catalytic performance and good high-temperature inhibition of the reverse water-gas shift (RWGS) reaction. The catalyst achieved 26.6 % CO conversion, 82.1 % C -C selectivity and 11.8 % light olefins yield. The ZnGaZrO formed by introducing an appropriate amount of Zn into GaZrO significantly enhanced the spillover H effect and also induced the generation of abundant oxygen vacancies to effectively promote the activation of CO. Importantly, the RWGS reaction was also significantly suppressed at high temperatures, with the CO selectivity being only 46.1 % at 390 °C.
我们提出了一种用于CO加氢制备轻质烯烃的新策略，即通过将Zn引入GaZrO中构建ZnGaZrO三元氧化物，并将其与SAPO-34结合，制备用于CO加氢制轻质烯烃的高性能ZnGaZrO/SAPO-34串联催化剂。通过优化Zn掺杂量、两相复合比例和方式以及工艺条件，3.5%ZnGaZrO/SAPO-34串联催化剂表现出优异的催化性能以及对逆水煤气变换（RWGS）反应良好的高温抑制性能。该催化剂实现了26.6%的CO转化率、82.1%的C-C选择性和11.8%的轻质烯烃收率。通过向GaZrO中引入适量的Zn形成的ZnGaZrO显著增强了溢流H效应，还诱导产生了大量氧空位，从而有效促进了CO的活化。重要的是，高温下RWGS反应也得到了显著抑制，在390℃时CO选择性仅为46.1%。
