Research Center for Solar Driven Carbon Neutrality, The College of Physics Science and Technology, Institute of Life Science and Green Development, Hebei University, Baoding, 071002, P. R. China.
TJU-NIMS International Collaboration Laboratory, School of Materials Science and Engineering, Tianjin University, Tianjin, 300072, P. R. China.
Angew Chem Int Ed Engl. 2023 Jun 5;62(23):e202302253. doi: 10.1002/anie.202302253. Epub 2023 May 3.
Solar-driven CO hydrogenation into multi-carbon products is a highly desirable, but challenging reaction. The bottleneck of this reaction lies in the C-C coupling of C intermediates. Herein, we construct the C-C coupling centre for C intermediates via the in situ formation of Co -Co interface double sites on MgAl O (Co-CoO /MAO). Our experimental and theoretical prediction results confirmed the effective adsorption and activation of CO by the Co site to produce C intermediates, while the introduction of the electron-deficient state of Co can effectively reduce the energy barrier of the key CHCH* intermediates. Consequently, Co-CoO /MAO exhibited a high C hydrocarbons production rate of 1303 μmol g h ; the total organic carbon selectivity of C hydrocarbons is 62.5 % under light irradiation with a high ratio (≈11) of olefin to paraffin. This study provides a new approach toward the design of photocatalysts used for CO conversion into C products.
太阳能驱动的 CO 加氢反应生成多碳产物是一种非常理想但极具挑战性的反应。该反应的瓶颈在于 C 中间体的 C-C 偶联。在此，我们通过在 MgAlO 上原位形成 Co-Co 界面双位点（Co-CoO/MAO）构建了 C 中间体的 C-C 偶联中心。我们的实验和理论预测结果证实，Co 位可有效吸附和活化 CO 生成 C 中间体，而 Co 的缺电子态的引入可有效降低关键 CHCH*中间体的能垒。因此，Co-CoO/MAO 在光照下表现出高达 1303 μmol·g-1·h-1 的 C 烃产率；C 烃的总有机碳选择性为 62.5%，其中烯烃与烷烃的比例（≈11）较高。该研究为设计用于 CO 转化为 C 产物的光催化剂提供了一种新途径。
