Atomically Dispersed Dual Metal Sites Boost the Efficiency of Olefins Epoxidation in Tandem with CO2 Cycloaddition
Atomically Dispersed Dual Metal Sites Boost the Efficiency of Olefins Epoxidation in Tandem with CO2 Cycloaddition
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原子分散的双金属位点提高了烯烃环氧化与 CO2 环加成串联的效率
DOI：
10.1021/acs.nanolett.2c03087
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发表时间：
2022
期刊：
影响因子：
10.8
通讯作者：
Liang Chen
中科院分区：
文献类型：
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作者：
Yinming Wang;Ziqi Tian;Qihao Yang;Kaicheng Tong;Xuan Tang;Nian Zhang;Jing Zhou;Linjuan Zhang;Qiuju Zhang;Sheng Dai;Yichao Lin;Zhiyi Lu;Liang Chen
串联催化为精细化学品的生产提供了经济和节能的方法。本工作中，我们证明了一种合理合成的具有原子分散的双Fe-Al中心的碳基催化剂（ADD-Fe-Al）对烯烃的一锅氧化羧化反应具有上级催化活性（转化率> 97%，选择性> 91%），其中目标产物的产率在ADD-Fe-Al上至少比单一催化剂高62%。动力学结果表明，Fe（氧化位）和Al位（环加成位）的协同作用使催化剂的催化性能显著提高，Al位（3.91wt%）的存在下，CO2与环氧化合物的环加成反应使Fe位（0.89wt%）上的氧化平衡向烯烃环氧化反应转变.本工作不仅为烯烃氧化羧化反应提供了一种先进的催化剂，而且为今后串联催化反应多功能催化剂的合理设计开辟了一条途径。
Tandem catalysis provides an economical and energy-efficient process for the production of fine chemicals. In this work, we demonstrate that a rationally synthesized carbon-based catalyst with atomically dispersed dual Fe–Al sites (ADD-Fe-Al) achieves superior catalytic activity for the one-pot oxidative carboxylation of olefins (conversion ∼97%, selectivity ∼91%), where the yield of target product over ADD-Fe-Al is at least 62% higher than that of monometallic counterparts. The kinetic results reveal that the excellent catalytic performance arises from the synergistic effect between Fe (oxidation site) and Al sites (cycloaddition site), where the efficient CO2cycloaddition with epoxides in the presence of Al sites (3.91 wt %) positively shifts the oxidation equilibrium to olefin epoxidation over Fe sites (0.89 wt %). This work not only offers an advanced catalyst for oxidative carboxylation of olefins but also opens up an avenue for the rational design of multifunctional catalysts for tandem catalytic reactions in the future.