Polyoxometalate-modified reduced graphene oxide foam as a monolith reactor for efficient flow catalysis of epoxide ring-opening reactions
Polyoxometalate-modified reduced graphene oxide foam as a monolith reactor for efficient flow catalysis of epoxide ring-opening reactions
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多金属氧酸盐改性还原氧化石墨烯泡沫作为整体式反应器，用于环氧化物开环反应的高效流动催化
DOI：
10.1039/d0ta11188k
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发表时间：
2021-04-07
影响因子：
11.9
通讯作者：
Hu, Changwen
中科院分区：
文献类型：
--
作者：
Jing, Xiaoting;Li, Zhen;Hu, Changwen
连续流催化反应由于其相对于传统间歇反应的显著优点而引起了人们极大的兴趣。在这项工作中，已经开发了一种简单和广谱的水热方法来构建聚氧乙烯酸酯改性的还原氧化石墨烯（POM@rGO）泡沫，其作为整体式反应器用于有效的连续流动催化环氧化物开环反应。rGO泡沫的多孔结构允许POM催化剂通过静电相互作用高度分散到基底上。具体地，磷钨酸（H3 PW 12 O 40，表示为PW 12）改性的rGO（PW12@rGO）整体式反应器对与醇的环氧化物开环反应表现出显著的催化活性和耐久性，在环境条件下在10分钟内实现99%的转化率和92%的甲醇分解产物的选择性而无需搅拌。值得注意的是，当与微注射泵耦合时，这种PW12@rGO泡沫可以作为有效的连续流动反应器，以99%的转化率和超过90%的选择性对氧化苯乙烯进行甲醇分解38 h，达到高达28 044的周转数（TON）。
Continuous flow catalysis has been attracting significant interest due to its remarkable advantages over traditional batch reactions. In this work, a facile and broad-spectrum hydrothermal approach has been developed to construct polyoxometalate-modified reduced graphene oxide (POM@rGO) foam, which worked as a monolith reactor for efficient continuous flow catalysis of epoxide ring-opening reactions. The porous structures of rGO foam allow the high dispersion of the POM catalyst onto the substrate through electrostatic interactions. Specifically, a phosphotungstic acid (H3PW12O40, denoted as PW12)-modified rGO (PW12@rGO) monolith reactor exhibits remarkable catalytic activity and durability towards epoxide ring-opening reactions with alcohols, achieving 99% conversion and 92% selectivity for the methanolysis product in 10 min under ambient conditions without stirring. Notably, while coupling with a micro-injection pump, such PW12@rGO foam can work as an efficient continuous flow reactor towards methanolysis of styrene oxide for 38 h with 99% conversion and over 90% selectivity, reaching a turnover number (TON) as high as 28 044.