共 - 共界面双位点介导 C-C 偶联用于 CO 光热转化为轻烯烃。
Co -Co Interface Double-Site-Mediated C-C Coupling for the Photothermal Conversion of CO into Light Olefins.
机构信息
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.
出版信息
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。
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