Synergetic effect of hollowrization and sulfonation on improving the photocatalytic performance of covalent porphyrin polymers in the reduction of CO2,Materials Chemistry Frontiers

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Synergetic effect of hollowrization and sulfonation on improving the photocatalytic performance of covalent porphyrin polymers in the reduction of CO2
Materials Chemistry Frontiers ( IF 6.0 ) Pub Date : 2020-07-13 , DOI: 10.1039/d0qm00314j
Yue Zhang _{1,

2,

3,

4,

5} , Yuting Wang _{1,

2,

3,

4,

5} , Lian-Cai An _{1,

2,

3,

4,

5} , Juanjuan Chen _{4,

6,

7,

8} , Tianhao Zhang _{4,

8,

9,

10,

11} , Ying-Hui Zhang _{1,

2,

3,

4,

5}

Affiliation

As a new kind of photocatalytic system, covalent organic polymers (COPs) exhibit wide spectral absorption and high surface area, but poorer photocatalytic performance relative to traditional inorganic semiconductor materials due mainly to the lower separation efficiency of photogenerated carriers. Herein, a tetrabiphenylporphyrin-based COP (COP-P) was investigated in photocatalyzing the reduction of CO₂, and nearly exclusive production of CO was observed with a rate of 1.55 μmol g⁻¹ within one hour, which is a little higher than commercial TiO₂ (P25) with a rate of 0.92 μmol g⁻¹. Meanwhile, hollowrization and post-sulfonation were utilized to modulate the photocatalytic performance of COP-P, resulting in just moderately improved and slightly deteriorated performance, respectively. Surprisingly, the synergistic action of these two modulations gives 4.8 times enhanced production of CO (7.54 μmol g⁻¹ within 1 hour). Its revealed that post-sulfonation would improve the separation and transfer ability of photogenerated carriers based on transient amperometric I–t curve analyses, but reduces significantly the surface area of COP-P polymers and thereby decreases CO₂ uptake through gas adsorption analyses, which fortunately could be remedied by hollowrization, leading to much improved photocatalytic production of CO. This work reveals the complicated influences of post-modification and paves a facile way to optimize the photocatalytic efficiency of organic polymers through synergetic effects.

中文翻译：

中和和磺化的协同作用对提高共价卟啉聚合物在减少二氧化碳中的光催化性能

作为一种新型的光催化体系，共价有机聚合物（COP）表现出宽光谱吸收和高表面积，但相对于传统的无机半导体材料而言，光催化性能较差，这主要是由于光生载流子的分离效率较低。在本文中，研究了基于四联苯基卟啉的COP（COP-P）在光催化还原CO _2时，在一小时内观察到几乎独家的CO生成，速率为1.55μmolg ^-1，这比商用TiO ₂（P25）的比率为0.92μmolg ^-1。同时，中和和后磺化被用来调节COP-P的光催化性能，分别导致适度改善和稍微恶化的性能。令人惊讶地，这两个调节的协同作用使CO的产生提高了4.8倍（1小时内为7.54μmolg ^-1）。其结果表明，基于瞬时安培I – t曲线分析，后磺化将改善光生载流子的分离和转移能力，但会显着减少COP-P聚合物的表面积，从而降低CO _2。通过气体吸附分析的吸收，幸运的是可以通过中空处理来弥补，从而大大改善了CO的光催化生成。这项工作揭示了后改性的复杂影响，并为通过协同效应优化有机聚合物的光催化效率提供了一种简便的方法。

更新日期：2020-08-27

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