Unique S-scheme heterojunctions in self-assembled TiO2/CsPbBr3 hybrids for CO2 photoreduction
Unique S-scheme heterojunctions in self-assembled TiO2/CsPbBr3 hybrids for CO2 photoreduction
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自组装 TiO2/CsPbBr3 杂化物中独特的 S 型异质结用于 CO2 光还原
DOI：
10.1038/s41467-020-18350-7
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发表时间：
2020-09-16
影响因子：
16.6
通讯作者：
Yu, Jiaguo
中科院分区：
文献类型：
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作者：
Xu, Feiyan;Meng, Kai;Yu, Jiaguo
探索光催化剂促进CO2光还原为太阳能燃料具有重要意义。我们开发的TiO 2/钙钛矿（CsPbBr 3）S-计划的异质结合成一个简单的静电驱动的自组装方法。密度泛函理论计算结合实验研究证明了CsPbBr 3量子点（QD）与TiO 2之间的电子转移，导致了CsPbBr 3与TiO 2杂化时内部电场的形成。通过原位X射线光电子能谱分析发现，IEF驱动TiO 2中的光激发电子到CsPbBr 3，表明在TiO 2/CsPbBr 3纳米杂化材料中形成了S型异质结，极大地促进了电子-空穴对的分离，从而促进了高效的CO2光还原。与原始TiO 2纳米纤维（4.68 μ mol g（-1）h（-1））相比，混合纳米纤维揭示了更高的CO2还原速率（9.02 μ mol g（-1）h（-1））。同位素（（CO2）-C-13）示踪结果证实还原产物来源于CO2源。
Exploring photocatalysts to promote CO2 photoreduction into solar fuels is of great significance. We develop TiO2/perovskite (CsPbBr3) S-scheme heterojunctions synthesized by a facile electrostatic-driven self-assembling approach. Density functional theory calculation combined with experimental studies proves the electron transfer from CsPbBr3 quantum dots (QDs) to TiO2, resulting in the construction of internal electric field (IEF) directing from CsPbBr3 to TiO2 upon hybridization. The IEF drives the photoexcited electrons in TiO2 to CsPbBr3 upon light irradiation as revealed by in-situ X-ray photoelectron spectroscopy analysis, suggesting the formation of an S-scheme heterojunction in the TiO2/CsPbBr3 nanohybrids which greatly promotes the separation of electron-hole pairs to foster efficient CO2 photoreduction. The hybrid nanofibers unveil a higher CO2-reduction rate (9.02 mu mol g(-1) h(-1)) comparing with pristine TiO2 nanofibers (4.68 mu mol g(-1) h(-1)). Isotope ((CO2)-C-13) tracer results confirm that the reduction products originate from CO2 source.