Polyoxometalates Immobilized on Covalent Triazine Framework as Efficient Catalysts for Deep Oxidative Desulfurization
Polyoxometalates Immobilized on Covalent Triazine Framework as Efficient Catalysts for Deep Oxidative Desulfurization
复制标题
固定在共价三嗪骨架上的多金属氧酸盐作为深度氧化脱硫的高效催化剂
DOI：
10.1002/cctc.202200021
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发表时间：
2022
期刊：
影响因子：
4.5
通讯作者：
Changwen Hu
中科院分区：
文献类型：
--
作者：
Chengpeng Liu;Zhen Li;Huifang Liu;Jing Dong;Yingnan Chi;Changwen Hu
具有均匀分散的催化位点、两亲表面和优异的可回收性的固定化多金属氧酸盐（POM）在许多重要反应中是非常需要的。在此，通过静电组装H3PMo12O40（PMo12）与多孔阳离子共价三嗪骨架（CTF）成功制备了PMo12@CTF，其中PMo12均匀分散在载体上。合成的PMo12@CTF对柴油氧化脱硫具有很高的活性，二苯并噻吩（DBT）在双相体系中在温和条件（40°C）下可在2 h内完全转化。令人印象深刻的是，多相PMo12@CTF（转化率：100%）的催化活性远高于均相PMo12（转化率：20%）。控制实验和接触角测量表明，CTF赋予PMo12@CTF较大的比表面积和两亲特性，催化剂能够有效地与萃取相中的氧化剂H2O2和油相中的DBT接触。此外，PMo12@CTF具有鲁棒性，十个循环后其催化活性基本保持。
The immobilized polyoxometalates (POMs) with evenly dispersed catalytic sites, amphiphilic surface, and excellent recyclability are highly desired in many important reactions. Herein, PMo12@CTF has been successfully fabricated by the electrostatic assembly of H3PMo12O40 (PMo12) with porous cationic covalent triazine framework (CTF), where PMo12 are evenly dispersed on the support. The synthesized PMo12@CTF is highly active for oxidative desulfurization of diesel fuel and dibenzothiophene (DBT) can be completely converted in 2 h under mild conditions (40 °C) in a biphasic system. Impressively, the catalytic activity of heterogeneous PMo12@CTF (conversion: 100 %) is much higher than that of homogeneous PMo12 (conversion: 20 %). The control experiments and contact angle measurements reveal that the CTF endows PMo12@CTF with large surface area and amphiphilic feature and the catalyst can effectively contact with both oxidant H2O2 in extraction phase and DBT in oil phase. Moreover, PMo12@CTF is robust and its catalytic activity is basically maintained after ten cycles.