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Modular monomers with adjustable solubility: Synthesis of block copolymers for improved photocatalysis by RAFT for the synthesis of atomic nickel co-catalysts
Molecular Catalysis ( IF 3.9 ) Pub Date : 2021-08-25 , DOI: 10.1016/j.mcat.2021.111834
Bo Zhang 1 , Guohua Wu 2 , Baohua Zhang 3
Affiliation  

Using the high incompatibility between the neutral stabilizer body and the block polyelectrolyte to drive phase separation during polymerization-induced self-assembly, a modular approach to systematically adjust ionic monomer/polymer solubility was developed to effectively identify monomers suitable for RAFT aqueous dispersion polymerization, with strong phase separation ability to form worm phases over a wide range of compositions and even at very low solids content. The block copolymer PMPS-MPS-P([META+][PF6]), prepared by this method, acts as a "nano bridge" and achieves Ni loading on TiO2 with the help of sol-gel method + thermal reduction. The atomic loading of Ni on TiO2 is achieved through strong covalent bonding, metallic bonding and the natural physical intertwining effect of silane coupling agent. Interestingly, it was unexpectedly found that the TiC stable structure generated by this process, the ionization of part of the block polyelectrolyte after the thermal reduction treatment at 773 K and the loading process of Ni all can promote the formation of oxygen vacancy Ov, which facilitates the charge transfer and hydrogen precipitation reaction. It has superior photocatalytic ability and cheaper cost compared to the conventional impregnation dispersion method. These findings provide a new idea to modify the manipulated photocatalysts by defect engineering to achieve efficient photocatalytic efficiency and capability.



中文翻译:

具有可调节溶解度的模块化单体:合成嵌段共聚物以通过 RAFT 改进光催化,用于合成原子镍助催化剂

利用中性稳定剂主体与嵌段聚电解质之间的高度不相容性在聚合诱导自组装过程中驱动相分离,开发了一种系统地调节离子单体/聚合物溶解度的模块化方法,以有效识别适用于 RAFT 水分散聚合的单体,具有强大的相分离能力,可在广泛的成分范围内甚至在非常低的固体含量下形成蠕虫相。通过该方法制备的嵌段共聚物PMPS-MPS-P([META + ][PF 6 - ])充当“纳米桥”,并借助溶胶-凝胶法+热还原在TiO 2上实现Ni负载. Ni在TiO 2上的原子负载是通过强共价键、金属键和硅烷偶联剂的天然物理交织作用实现的。有趣的是,意外地发现该过程产生的 TiC 稳定结构、773 K 热还原处理后部分嵌段聚电解质的电离和 Ni 的加载过程都可以促进氧空位 Ov 的形成,这有利于电荷转移和析氢反应。与传统的浸渍分散方法相比,它具有优越的光催化能力和更便宜的成本。这些发现为通过缺陷工程修饰操纵的光催化剂以实现高效的光催化效率和能力提供了新的思路。

更新日期:2021-08-26
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