Institute of Chemistry for Functionalized Materials School of Chemistry and Chemical Engineering, Liaoning Normal University, Dalian, 116029, China.
College of Chemistry, Nankai University, Tianjin, 300071, China.
Chemphyschem. 2023 Jun 15;24(12):e202200910. doi: 10.1002/cphc.202200910. Epub 2023 Apr 3.
The objective of the tandem hydroformylation-hydrogenation of alkenes to corresponding alcohols was to design an efficient and stable heterogeneous catalyst. To this end, a series of novel heterogeneous graphitic carbon nitride (g-CN) supported bimetallic Rh-Co nanoparticle catalysts (Rh-Co/g-CN) were prepared and subsequently studied for this one-pot two-step reaction. The lamellar structure makes Rh and Co nanoparticles with diameters of <1 nm and 20 nm, respectively, homogeneously deposited on the surface of g-CN layers, exhibit remarkable conversion of styrene (99.9 %) and chemoselectivity for alcohol (87.8 %). More importantly, Co nanoparticles are found to play an important role in the improvement of the chemoselectivity for alcohol due to the formation of catalytic active species [HCo(CO) ]. Besides the detailed investigation of the catalytic properties of Rh-Co/g-CN under different reaction conditions, the reuse of Rh-Co/g-CN was conducted for five times and no evident decrease in the activity and chemoselectivity was observed. Therefore, we expect that this work could offer an initial insight into g-CN-based heterogeneous catalyst on the tandem hydroformylation-hydrogenation reaction.
烯烃的串联氢甲酰化-加氢反应的目的是设计高效稳定的多相催化剂。为此，我们制备了一系列新型的负载双金属 Rh-Co 纳米粒子的石墨相氮化碳（g-CN）负载型催化剂（Rh-Co/g-CN），并对其在一锅两步反应中的性能进行了研究。层状结构使 Rh 和 Co 纳米颗粒分别以<1 nm 和 20 nm 的直径均匀地沉积在 g-CN 层的表面，对苯乙烯的转化率达到 99.9%，对醇的选择性达到 87.8%。更重要的是，由于形成了催化活性物种[HCo(CO) ]，Co 纳米颗粒在提高醇的选择性方面发挥了重要作用。除了在不同反应条件下对 Rh-Co/g-CN 的催化性能进行详细研究外，我们还对 Rh-Co/g-CN 进行了五次重复使用实验，其活性和选择性没有明显下降。因此，我们期望这项工作能够为基于 g-CN 的多相催化剂在串联氢甲酰化-加氢反应中的应用提供初步的认识。
