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Polaron and bipolaron induced charge carrier transportation for enhanced photocatalytic H2 production.
Nanoscale ( IF 5.8 ) Pub Date : 2020-06-10 , DOI: 10.1039/d0nr02950e
T R Naveen Kumar 1 , P Karthik , B Neppolian
Affiliation  

Photocatalysis is one of the facile approaches for efficient solar energy conversion and storage. However, rapid charge carrier recombination considerably decreases solar to energy conversion efficiency. Herein, polaron and bipolaron rich polypyrrole (PPy) has been utilized as a solid support for effective photogenerated charge carrier separation. Simple oxidative polymerization using a high concentration of ammonium persulfate (APS) induces radical cation/bipolaron formation in PPy due to the cleavage of π-bonds as confirmed by electron paramagnetic resonance spectroscopy (EPR). The formation of radical cations led to an increase of the dielectric constant which retards the charge carrier recombination and thereby enhances the conductivity. Moreover, the polarons and bipolarons induced charge carrier separation in photocatalytic H2 production was studied with the well-known g-C3N4 photocatalyst. It is worth mentioning that compared to bare g-C3N4, the PPy supported system showed a drastically enhanced photocatalytic H2 production rate. A maximum H2 production rate of 1851 μmoles per g is achieved, which is ∼51 times higher than that of the bare g-C3N4 catalyst due to efficient charge carrier separation assisted by radical cations/bipolarons. Thus, utilizing this simple polaron and bipolaron rich PPy solid support could be an effective strategy and alternative for using noble metal cocatalysts to enhance charge carrier separation.

中文翻译:

极化子和双极化子诱导电荷载流子传输,以增强光催化氢气的产生。

光催化是有效的太阳能转换和存储的简便方法之一。然而,快速的载流子复合大大降低了太阳能到能量的转换效率。在本文中,富含极化子和双极化子的聚吡咯(PPy)已被用作有效分离光生载流子的固体载体。如电子顺磁共振波谱(EPR)所证实的,使用高浓度的过硫酸铵(APS)进行的简单氧化聚合会由于π键的裂解而在PPy中引发自由基阳离子/双极化子的形成。自由基阳离子的形成导致介电常数的增加,这阻碍了电荷载流子的复合,从而提高了电导率。此外,极化子和双极化子在光催化H中引起电荷载流子分离用众所周知的gC 3 N 4光催化剂研究了2的产生。值得一提的是,与裸露的gC 3 N 4相比,PPy支撑的系统显示出光催化H 2的生产速率大大提高。由于自由基阳离子/双极化子的有效载流子分离,H 2的最大生产率达到了每克1851μmoles,比裸gC 3 N 4催化剂高出约51倍。因此,利用这种简单的富含极化子和双极化子的PPy固体载体可能是使用贵金属助催化剂增强电荷载流子分离的有效策略和替代方法。
更新日期:2020-07-09
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