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通过在单层二维TiCT MXene上原位生长提高无铅CsBiBr钙钛矿纳米晶体用于C-H键氧化的光催化活性和稳定性

Boosting Photocatalytic Activity and Stability of Lead-Free CsBiBr Perovskite Nanocrystals via In Situ Growth on Monolayer 2D TiCT MXene for C-H Bond Oxidation.

作者信息

Li Qinglin, Song Tao, Zhang Yinpan, Wang Qi, Yang Yong

机构信息

CAS Key Laboratory of Bio-Based Materials, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China.

University of Chinese Academy of Sciences, Beijing 100049, China.

出版信息

ACS Appl Mater Interfaces. 2021 Jun 16;13(23):27323-27333. doi: 10.1021/acsami.1c06367. Epub 2021 Jun 2.

Abstract

Light-driven selective oxidation of saturated C-H bonds with molecular oxygen, as an alternative to conventional thermochemical catalysis, allows a sustainable and eco-friendly manner to convert solar energy into highly value-added oxygenates. However, the photocatalytic oxidation of hydrocarbons still remains a great challenge owing to the low efficiency in the separation and transfer of photogenerated charge of the currently available photocatalytic materials. Herein, we report a novel perovskite-based heterostructure photocatalyst, in which ligand- and lead-free all-inorganic perovskite CsBiBr nanocrystals (NCs) with uniform crystal size and high crystallinity were homogeneously distributed on the surface of ultrathin two-dimensional (2D) monolayer TiCT MXene nanosheets in an in situ growth manner. The resultant heterostructure featured with intimate interface between CsBiBr NCs and TiCT MXene and strong visible-light adsorption not only exhibits significant enhancement in the performance of photocatalytic oxidation of challenging aromatic and aliphatic alkanes under visible-light irradiation but also greatly improves the stability of CsBiBr NCs under a reaction environment. Comprehensive characterizations reveal that the formation of an intimate interface between CsBiBr NCs and highly conductive ultrathin 2D TiCT MXene nanosheets via strong interaction markedly accelerates the separation and transfer efficiency of photogenerated electron-hole pairs and simultaneously suppresses their recombination, resulting in improved utilization of the excited charges, which account for the highly enhanced photocatalytic performance.

摘要

与传统热化学催化相比,光驱动的饱和C-H键与分子氧的选择性氧化提供了一种可持续且环保的方式,将太阳能转化为高附加值的含氧化合物。然而,由于目前可用的光催化材料在光生电荷的分离和转移方面效率较低,烃类的光催化氧化仍然是一个巨大的挑战。在此,我们报道了一种新型的基于钙钛矿的异质结构光催化剂,其中具有均匀晶体尺寸和高结晶度的无配体和无铅全无机钙钛矿CsBiBr纳米晶体(NCs)以原位生长的方式均匀分布在超薄二维(2D)单层TiCT MXene纳米片的表面。所得的异质结构在CsBiBr NCs和TiCT MXene之间具有紧密的界面以及强烈的可见光吸附,不仅在可见光照射下对具有挑战性的芳香族和脂肪族烷烃的光催化氧化性能有显著增强,而且在反应环境下大大提高了CsBiBr NCs的稳定性。综合表征表明,CsBiBr NCs与高导电性超薄2D TiCT MXene纳米片通过强相互作用形成紧密界面,显著加速了光生电子-空穴对的分离和转移效率,同时抑制了它们的复合,从而提高了激发电荷的利用率,这解释了光催化性能的高度增强。

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