Shang Xin, Zhuo Hongying, Han Qiao, Yang Xiaofeng, Hou Guangjin, Liu Guodong, Su Xiong, Huang Yanqiang, Zhang Tao
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, No. 457 Zhongshan Road, Dalian, 116023, China.
University of Chinese Academy of Sciences, Beijing, 100049, China.
Angew Chem Int Ed Engl. 2023 Sep 11;62(37):e202309377. doi: 10.1002/anie.202309377. Epub 2023 Aug 4.
Selective synthesis of specific value-added aromatics from CO hydrogenation is of paramount interest for mitigating energy and climate problems caused by CO emission. Herein, we report a highly active composite catalyst of ZnZrO and HZSM-5 (ZZO/Z5-SG) for xylene synthesis from CO hydrogenation via a coupling reaction in the presence of toluene, achieving a xylene selectivity of 86.5 % with CO conversion of 10.5 %. A remarkably high space time yield of xylene could reach 215 mg g h , surpassing most reported catalysts for CO hydrogenation. The enhanced performance of ZZO/Z5-SG could be due to high dispersion and abundant oxygen vacancies of the ZZO component for CO adsorption, more feasible hydrogen activation and transfer due to the close interaction between the two components, and enhanced stability of the formate intermediate. The consumption of methoxy and methanol from the deep hydrogenation of formate by introduced toluene also propels an oriented conversion of CO .
通过CO加氢选择性合成特定的增值芳烃对于缓解由CO排放引起的能源和气候问题至关重要。在此,我们报道了一种用于在甲苯存在下通过偶联反应由CO加氢合成二甲苯的高活性ZnZrO和HZSM-5复合催化剂(ZZO/Z5-SG),二甲苯选择性达到86.5%,CO转化率为10.5%。二甲苯的时空产率显著高达215 mg g h ,超过了大多数报道的用于CO加氢的催化剂。ZZO/Z5-SG性能的提高可能归因于ZZO组分对CO吸附的高分散性和丰富的氧空位、由于两种组分之间的紧密相互作用而更可行的氢活化和转移以及甲酸盐中间体稳定性的增强。引入的甲苯对甲酸盐深度加氢产生的甲氧基和甲醇的消耗也推动了CO的定向转化。