Boosting Selectivity toward Long-Chain α-Olefins in CO 2 Hydrogenation through Strengthening ZnO–Fe Interactions with Favorable Iron Phase Regulation for Fischer–Tropsch Synthesis

作者：Zhaobo Fan, Zhangshi Li, Yong Li, Qiang Li, Siyang Yan, Guanze Nie, Dezheng Li, Changxu Wang, Huan He, Jiaxu Liu, Bing Liu, X. L. Liu · 发表于：JACS Au · 年份：2026 · DOI：10.1021/jacsau.5c01605 · 被引用次数：4 · 研究领域：Catalysts for Methane Reforming、Carbon dioxide utilization in catalysis、CO2 Reduction Techniques and Catalysts

High Resolution Image Download MS PowerPoint Slide Developing excellent catalysts for CO 2 hydrogenation to long-chain linear α-olefins (LAOs) offers a promising route toward value-added chemicals. However, it remains a considerable challenge to achieve high CO 2 conversion along with superior selectivity to LAOs. In this study, we prepared a series of Zn-modified iron-based catalysts using urea precipitation for the CO 2 hydrogenation reaction, and they exhibited a much higher selectivity to C 4+ LAOs of 61.7%, with a CO 2 conversion of 38.5%, over Fe2Zn1-U catalyst, compared to the selectivity of 50.5% over Fe2Zn1-A catalyst with same elemental composition prepared using ammonia precipitation. A lower selectivity to methane was obtained, from 13.7% to 8.8%. Moreover, this process resulted in a record-breaking space-time yield (STY) of 0.544 g C4+LAOs ·g cat –1 ·h –1 . HRTEM characterization over spent catalysts showed that Fe2Zn1-U exhibited smaller-size mixed iron-phase particles (Fe 3 O 4, χ-Fe 5 C 2, and θ-Fe 3 C) where the ZnO phase was more homogeneously dispersed and had stronger interactions with Fe species compared to the observations for Fe2Zn1-A. In situ XPS analysis suggested that this structure promoted Zn-to-Fe electron donation along with intimate interaction over Fe2Zn1-U. XANES spectra demonstrated a more difficult reduction of Fe species with weaker Fe–C coordination for carburization, thereby resulting in a higher Fe 3 O 4 content in spent Fe2Zn1-U. In sit...