Interfacing with Carbonaceous Potassium Promoters Boosts Catalytic CO2 Hydrogenation of Iron

作者：Yu Han, Chuanyan Fang, Xuewei Ji, Jian Hua Wei, Qingjie Ge, Jian Sun · 发表于：ACS Catalysis · 年份：2020 · DOI：10.1021/acscatal.0c03215 · 被引用次数：200 · 研究领域：Carbon dioxide utilization in catalysis、Catalysts for Methane Reforming、CO2 Reduction Techniques and Catalysts

Directly converting carbon dioxide into high-valued olefins (ethylene, propylene, and linear α-olefins) with regenerative hydrogen could be a way of reducing CO 2 emissions and replacing fossil fuels. However, precise control of C–O activation and subsequent C–C coupling toward those olefins remain a challenge, due to the unclear catalytic mechanism on active sites and surrounding promoters. Herein, we demonstrate that the carbonaceous series K-promoters from K 2 CO 3, CH 3 COOK, KHCO 3, and KOH can induce Fe/C catalysts to form a more active and distinct Fe 5 C 2 –K 2 CO 3 interface in nanoscale via CO 2 hydrogenation, which boosts the production of high-valued olefins by facilitating electron transfer from potassium to iron species. A high olefin selectivity of near 75% in hydrocarbons is realized at a conversion of more than 32%. The maximum yield of high-valued olefins reaches up to 20.1%, which is the record-breaking highest value among all Fe based CO 2 hydrogenation in the literature. More interestingly, the appropriate proximity between carbonaceous K-promoters and Fe/C catalyst endow the catalytic system with an outstanding high-valued olefin yield and high catalytic stability. These findings enrich the chemistry of CO 2 conversion and provide a strategy to design highly selective catalysts for high-valued chemicals.