Enhanced conversion of syngas to high-quality diesel fuel over ZrO2 and acidized carbon nanotube bifunctional catalyst
Enhanced conversion of syngas to high-quality diesel fuel over ZrO2 and acidized carbon nanotube bifunctional catalyst
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DOI：
10.1016/j.fuproc.2023.107920
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发表时间：
2023-07-21
影响因子：
7.5
通讯作者：
Liu，Shanjian
中科院分区：
文献类型：
--
作者：
Zao，Huijie;Liu，Jing;Liu，Shanjian
合成气直接转化为柴油因其可利用非石油碳源而成为一条极具吸引力的途径。然而，由于Anderson-Schulz-Flory（ASF）限制，通过常规费-托方法对柴油烃（C9-C22）的选择性有限，约为36%。在此，由分散在多壁碳纳米管（CNT）上的二氧化锆（ZrO 2）组成的双功能催化剂（ZrO 2/CNT）被成功地设计并应用于合成气直接转化为柴油，其选择性远远超过ASF限制。在350 °C、3 MPa、H2/CO = 2、气时空速为2400 mL·h-1·gcat-1的条件下，ZrO 2/CNT催化剂的C9-C22选择性为50.74%，CO单程转化率为43.86%，与未改性的ZrO 2/CNT催化剂相比，具有较好的催化活性ZnO/CNT和ZnO-ZrO_2/CNT的复合材料中，ZnO/CNT的复合材料中，ZrO_2/CNT的复合材料中，ZrO_2/CNT的复合材料中，ZnO/CNT的复合材料中，ZrO_2/CNT的复合材料中，ZnO/CNT的复合材料中，ZrO_2/CNT的复合材料中，ZrO_2/CNT的复合材料中，ZrO_2/CNT的复合材料中，ZnO/CNT的复合材料中，ZrO_2/CNT的复合材料中，ZrO_2/CNT的复合材料中，ZrO_2/ZnO的复合材料中，ZrO_2/CNT的复合材料中，ZrO_2/CNT的复合材料中，ZrO_2/CNT的复合材料中，ZrO_2/ZnO的复合材料中，ZrO_2/CNT的复合材料中，ZrO_2/CNT的复合材料中，ZrO_2/ZnO的复合材料中，ZrO_2/CNT的复合材料中，ZrO_2/CNT的复合材料中，ZrO_ C9-C22异构烷烃/正构烷烃比高达16。催化剂在100 h后仍表现出良好的催化活性，CO转化率为40.61%，柴油烃选择性为42.27%，甲烷选择性为7.67%，副产物CO2选择性稳定在3.77%左右。
Direct syngas conversion for diesel fuel becomes an attractive route for its possibility of utilizing non-petroleum carbon resources. However, there is a limited selectivity of around 36% for diesel hydrocarbons (C9-C22) via the conventional Fischer-Tropsch process due to the Anderson-Schulz-Flory (ASF) constraint. Herein, bifunctional catalysts composed of zirconium dioxide (ZrO2) dispersed on multi-walled carbon nanotubes (CNT) (ZrO2/CNT) were successfully designed and applied for direct conversion of syngas into diesel with selectivity far beyond the ASF limitation. At 350 °C with the pressure of 3 MPa, H2/CO of 2 and gas hourly space velocity of 2400 mL·h−1·gcat−1, ZrO2/CNT gave an unexceptionable C9-C22selectivity of 50.74% at a single pass CO conversion of 43.86% compared with those (9.11% and 20.55%, respectively) of ZnO/CNT and those (14.07% and 25.76%, respectively) of ZnO-ZrO2/CNT. The iso/n-paraffin ratio in the C9-C22reached up to 16. Moreover, after 100 h of operation, the catalyst still showed remarkable catalytic activity with CO conversion remaining at 40.61%, diesel hydrocarbon selectivity, and methane selectivity at 42.27% and 7.67%, respectively, while the by-product CO2selectivity was also stable at about 3.77%.