Synthesis of tetrahedrally coordinated CoO for higher alcohol synthesis directly from syngas  

作　　者：Zhuoshi Li Han Yang Xiaofeng Pei Jiahui Li Jing Lv Shouying Huang Yue Wang Xinbin Ma 

机构地区：[1]Key Laboratory for Green Chemical Technology of Ministry of Education,Collaborative Innovation Center of Chemical Science and Engineering,School of Chemical Engineering and Technology,Tianjin University,Tianjin 300072,China [2]Joint School of National University of Singapore and Tianjin University,International Campus of Tianjin University,Binhai New City,Fuzhou 350207,China [3]Haihe Laboratory of Sustainable Chemical Transformations,Tianjin 300192,China

出　　处：《Frontiers of Chemical Science and Engineering》2024年第8期99-109,共11页化学科学与工程前沿（英文版）

基　　金：support from the National Natural Science Foundation of China(Grant Nos.22108199,22278317,and 22022811);the China Postdoctoral Science Foundation(Grant No.2021TQ0239)。

摘　　要：Higher alcohol synthesis directly from syngas is highly desirable as one of the efficient non-petroleum energy conversion routes.Co^(0)–CoO catalysts showed great potential for this reaction,but the alcohol selectivity still needs to be improved and the crystal structure effect of Co^(0)on catalytic behaviors lacks investigation.Here,a series of tetrahedrally coordinated Co^(0)polymorphs were prepared by a thermal decomposition method,which consisted of wurtzite CoO and zinc blende CoO with varied contents.After diluting with SiO_(2),the catalyst showed excellent performance for higher alcohol synthesis with ROH selectivity of 45.8%and higher alcohol distribution of 84.1 wt%under the CO conversion of 38.0%.With increasing the content of wurtzite CoO,the Co^(0)/Co^(2+)ratio gradually increased in the spent catalysts,while the proportion of highly active hexagonal close packed cobalt in Co^(0)decreased,leading to first decreased then increased CO conversion.Moreover,the higher content of zinc blende CoO in fresh catalyst facilitated the retention of more Co^(2+)sites in spent catalysts,promoting the ROH selectivity but slightly decreasing the distribution of higher alcohols.The catalyst with 40%wurtzite CoO obtained the optimal performance with a space time yield toward higher alcohols of 7.9 mmol·gcat^(-1)·h^(-1).

关 键 词：higher alcohol synthesis CO hydrogenation wurtzite CoO zinc blende CoO hexagonal-closest-packed Co 

分 类 号：O64[理学—物理化学]