Yang Jun, Jing Jianfang, Zhu Yongfa
Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China.
Adv Mater. 2021 Aug;33(31):e2101026. doi: 10.1002/adma.202101026. Epub 2021 Jul 8.
A full-spectrum (300-850 nm) responsive donor-acceptor (D-A) supramolecular photocatalyst tetraphenylporphinesulfonate/fullerene (TPPS/C ) is successfully constructed. The theoretical spectral efficiency of TPPS/C is as high as 70%, offering the possibility of full-solar-spectrum light harvesting. The TPPS/C performs a highly efficient photocatalytic H evolution rate of 276.55 µmol h (34.57 mmol g h ), surpassing many reported organic photocatalysts. The D-A structure effectively promotes electron transfer from TPPS to C , which is beneficial to the photocatalytic reaction. Specifically, a giant internal electric field in the D-A structure is built via the enhanced molecular dipole, which dramatically promotes the charge separation (CS) efficiency by 2.35 times. Transient absorption spectra results show a long-lived CS state TPPS -C in the D-A structure, which effectively promotes participation of photogenerated electrons in the reduction reaction. Briefly, this work provides a novel approach for designing high-performance photocatalytic materials via enhancing the interfacial electric field.
成功构建了一种全光谱（300 - 850纳米）响应的供体-受体（D-A）超分子光催化剂四苯基卟啉磺酸盐/富勒烯（TPPS/C）。TPPS/C的理论光谱效率高达70%，为全太阳能光谱光捕获提供了可能性。TPPS/C的光催化析氢速率高达276.55微摩尔/小时（34.57毫摩尔/克·小时），超过了许多已报道的有机光催化剂。D-A结构有效地促进了电子从TPPS转移到C，这有利于光催化反应。具体而言，通过增强分子偶极在D-A结构中构建了一个巨大的内电场，使电荷分离（CS）效率显著提高了2.35倍。瞬态吸收光谱结果表明，D-A结构中存在长寿命的CS态TPPS -C，这有效地促进了光生电子参与还原反应。简而言之，这项工作通过增强界面电场为设计高性能光催化材料提供了一种新方法。
