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Tunable Perylene-based Donor–Acceptor Conjugated Microporous Polymer to Significantly Enhance Photocatalytic Uranium Extraction from Seawater
Chemical Engineering Journal ( IF 15.1 ) Pub Date : 2020-10-29 , DOI: 10.1016/j.cej.2020.127558
Fengtao Yu , Zhiqiang Zhu , Shiping Wang , Yukai Peng , Zhenzhen Xu , Yuan Tao , Jianbo Xiong , Qiangwen Fan , Feng Luo

Herein, we present a molecular engineering strategy to boost the photocatalysis performance of donor-acceptor conjugated microporous polymers (CMPs) for U(VI) reduction under visible-light. With perylene as donor and tailoring acceptors from 9H-fluoren-9-one to dibenzo[b,d]thiophene 5,5-dioxide, two new CMPs, named ECUT-CO and ECUT-SO, were obtained. Notably, both experiments and DFT calculations certificated the high dependence of photocatalytic activity upon the acceptors. Consequently, ECUT-SO with the strongest acceptor enables ultrahigh photocatalytic performance for uranium (VI) reduction, giving 97.8% reduction efficiency within 60 min, surpassing most reported photocatalysis materials for such use. The excellent photocatalysis ability was mainly due to that D-A configuration ECUT-SO affords optimized visible-light response, excellent photo-exciton separation and stronger coordination sites for UO22+. Importantly, by means of this photocatalytic technology, ultrahigh uranium extraction capacity of 1.78 g/g with a nearly 100% extraction efficiency was achieved in U(VI)-spiked real seawater, suggesting its superior application in extraction of uranium from seawater.



中文翻译:

可调谐Per基供体-受体共轭微孔聚合物,可显着增强海水中光催化铀的提取

在这里,我们提出了一种分子工程策略,以提高供体-受体共轭微孔聚合物(CMP)在可见光下还原U(VI)的光催化性能。以per为供体,将9H-芴-9-一为二苯并[b,d]噻吩5,5-二氧化物的定制受体,获得了两种新的CMP,分别称为ECUT-COECUT-SO。值得注意的是,实验和DFT计算均证明了光催化活性对受体的高度依赖性。因此,ECUT-SO具有最强受体的化合物能够实现超高的铀(VI)还原光催化性能,在60分钟内达到97.8%的还原效率,超过了大多数报道的此类光催化材料。优异的光催化能力主要是由于DA构型ECUT-SO提供了优化的可见光响应,出色的光激子分离和更强的UO 2 2+配位点。重要的是,通过这种光催化技术,在掺有U(VI)的真实海水中实现了1.78 g / g的超高铀提取能力,具有近100%的提取效率,表明其在从海水中提取铀方面具有卓越的应用价值。

更新日期:2020-10-30
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