Synthesis of Bifunctional Porphyrin Polymers for Catalytic Conversion of Dilute CO2 to Cyclic Carbonates,ACS Applied Materials & Interfaces

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Synthesis of Bifunctional Porphyrin Polymers for Catalytic Conversion of Dilute CO2 to Cyclic Carbonates
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-06-16 , DOI: 10.1021/acsami.1c04624
Lina Liu _{1,

2} , Sanjeevi Jayakumar ₁ , Jian Chen ₃ , Lin Tao _{1,

2} , He Li ₁ , Qihua Yang ₁ , Can Li ₁

Affiliation

Development of efficient solid catalysts for catalytic conversion of dilute CO₂ is of extreme importance for carbon capture and utilization. We report the synthesis of bifunctional polymers co-incorporated with porphyrin-Zn as Lewis acid sites and Br^– as nucleophiles for the cycloaddition of dilute CO₂ with epoxides in this work. It was found that the Br^–/Zn ratio has a volcano relation with the activity of bifunctional polymers in a cycloaddition reaction, indicating the synergy effect between Lewis acid sites and nucleophiles. The turnover frequency (TOF) of the bifunctional polymer is more than four-fold that of the physical mixture of tetrabutylammonium bromide and porphyrin-Zn-incorporated polymer, implying the enhanced cooperation between Br^– and porphyrin-Zn in the polymer network. The bifunctional polymer with optimized Br^–/Zn afforded 99% conversion, 99% selectivity, and a TOF as high as 12,000 h^–1 for the cycloaddition of CO₂ and propylene oxide, which is among the most active solid catalysts ever reported. Furthermore, the bifunctional polymer could efficiently catalyze the cycloaddition of epichlorohydrin with dilute CO₂ (7.5% CO₂ balanced by N₂) even under ambient conditions, demonstrating its potential application in industrial-scale production.

中文翻译：

稀二氧化碳催化转化为环状碳酸酯的双功能卟啉聚合物的合成

开发用于稀CO ₂催化转化的高效固体催化剂对于碳捕获和利用极其重要。在这项工作中，我们报告了双功能聚合物的合成，其中卟啉-Zn 作为路易斯酸位点，Br ^-作为亲核试剂，用于稀 CO ₂与环氧化物的环加成。研究发现，Br- ^/ Zn 比值与环加成反应中双功能聚合物的活性呈火山关系，表明路易斯酸位点与亲核试剂之间存在协同效应。双功能聚合物的转换频率（TOF）是四丁基溴化铵和卟啉-Zn掺入聚合物的物理混合物的四倍多，这意味着聚合物网络中^Br-和卟啉-Zn之间的合作增强。具有优化的 Br ^– /Zn 的双功能聚合物为 CO ₂和环氧丙烷的环加成提供了 99% 的转化率、99% 的选择性和高达 12,000 h ^–1的 TOF，这是迄今为止报道的最活跃的固体催化剂之一。此外，即使在环境条件下，该双功能聚合物也能有效催化环氧氯丙烷与稀CO ₂ （7.5％CO ₂由N ₂平衡）的环加成反应，展示了其在工业规模生产中的潜在应用。

更新日期：2021-06-30

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