Mechanisms behind photocatalytic CO2 reduction by CsPbBr3 perovskite-graphene-based nanoheterostructures
Mechanisms behind photocatalytic CO2 reduction by CsPbBr3 perovskite-graphene-based nanoheterostructures
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DOI：
10.1016/j.apcatb.2020.119751
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发表时间：
2021-05-05
影响因子：
22.1
通讯作者：
Pu, Ying-Chih
中科院分区：
文献类型：
--
作者：
Chen, Yu-Hung;Ye, Jin-Kun;Pu, Ying-Chih
我们证明了CsPbBr3纳米颗粒可以分别在半导体氧化石墨烯（GO）和导电少层石墨烯（FLG）表面原位生长。CsPbBr3-GO和CsPbBr3-FLG纳米异质结构（NHSs）的ii型和schottky结类能带结构导致了不同的界面电荷转移（CT）行为。CsPbBr3-GO和CsPbBr3-FLG NHSs的CT速率常数k（CT）可以通过控制它们的GO/FLG组成比来调节。CsPbBr3-GO NHSs的CO2 - CH4转化率（k(CH4)）与kCT呈正相关，而CsPbBr3-FLG NHSs的k（CH4）与k（CT）呈负相关。其机制可能是cspbbr3 -石墨烯基NHSs的不同能带结构为光激发载流子提供了不同的还原电位，从而影响光催化CO2还原性能。这项工作为钙钛矿-石墨烯基NHS的设计提供了重要的见解，该NHS在太阳能驱动的二氧化碳转换方面具有卓越的性能。
We demonstrate the CsPbBr3 nanoparticles can in-situ growth on semiconducting graphene oxide (GO) and conductive few-layer graphene (FLG) surfaces, individually. The type-II and Schottky-junction-like energy band structures of CsPbBr3-GO and CsPbBr3-FLG nanoheterostructures (NHSs) resulted in the varied interfacial charge transfer (CT) behaviors. The CT rate constant (k(CT)) of CsPbBr3-GO and CsPbBr3-FLG NHSs could be modulated by controlling their constituent ratio of GO/FLG. Moreover, the CO2 to CH4 conversion rate (k(CH4)) of CsPbBr3-GO NHSs showed a positive relation with kCT, while the negative correlation between k(CH4) and k(CT) for CsPbBr3-FLG NHSs was observed. The mechanism can be suggested as that the different energy band structures in CsPbBr3-graphehe-based NHSs provide the varied reduction potential for the photoexcited charge carriers to effect the performance in photocatalytic CO2 reduction. This work presents the important insights into the design of perovskite-graphene based NHS with remarkable performance for solar-driven CO2 conversion.