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通过铅-氮化学作用将溴化铯铅锚定在一维多孔管状石墨相氮化碳上以增强光催化二氧化碳还原性能

Pb-N Chemically Anchors CsPbBr on 1D Porous Tubular g-CN for Enhanced Photocatalytic CO Reduction.

作者信息

Li Dong, Wang Kaixuan, Chen Ying, Li Renyi, Tang Jiahong, Zhao Yizhou, Guo Wei, Chen Qi, Li Yujing

机构信息

Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, Experimental Center of Advanced Materials, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081, P. R. China.

Key Laboratory of Advanced Optoelectronic Quantum Architecture and Measurement (MOE), Frontiers Science Center for High Energy Material (MOE), State Key Laboratory of Explosion Science and Technology, School of Physics, Beijing Institute of Technology, Beijing, 100081, P. R. China.

出版信息

ChemSusChem. 2025 Mar 3;18(5):e202401638. doi: 10.1002/cssc.202401638. Epub 2024 Nov 12.

Abstract

Halide perovskite CsPbBr (CPB) quantum dots (QDs) are considered as a promising candidate for solar-driven CO conversion for their unique optoelectronic properties and suitable band structures. However, the CO conversion efficiency of pristine CsPbBr quantum dots is severely limited due to their rapid electron-hole pair recombination and insufficient active sites. In this study, by immobilizing CPB QDs onto one-dimensional (1D) porous tubular g-CN (TCN), an effective 0D/1D CPB@TCN heterojunction photocatalyst for CO reduction is fabricated. Density functional theory (DFT) calculations combined with experimental studies demonstrate that CPB QDs are uniformly anchored on the surface of TCN through Pb-N chemical bonding, resulting in efficient separation and transfer of photogenerated carriers in CPB@TCN photocatalysts. The resultant CPB@TCN photocatalysts exhibit significantly enhanced photocatalytic activity for CO reduction with the highest conversion rate of 22.62 μmol g h, which is 5.33-times higher than that of pristine CPB QDs. This work unveils the interfacial bonding mechanism of CPB@TCN heterojunction through Pb-N chemical bond, which provides new insights for the development perovskite-based heterojunction photocatalysts.

摘要

卤化物钙钛矿CsPbBr₃(CPB)量子点(QDs)因其独特的光电特性和合适的能带结构,被视为太阳能驱动CO₂转化的一种有前景的候选材料。然而,由于原始CsPbBr₃量子点的电子 - 空穴对快速复合以及活性位点不足,其CO₂转化效率受到严重限制。在本研究中,通过将CPB量子点固定在一维(1D)多孔管状g - C₃N₄(TCN)上,制备了一种用于CO₂还原的高效0D/1D CPB@TCN异质结光催化剂。密度泛函理论(DFT)计算与实验研究相结合表明,CPB量子点通过Pb - N化学键均匀地锚定在TCN表面,从而实现了CPB@TCN光催化剂中光生载流子的有效分离和转移。所得的CPB@TCN光催化剂对CO₂还原表现出显著增强的光催化活性,最高转化率为22.62 μmol g⁻¹ h⁻¹,比原始CPB量子点高5.33倍。这项工作揭示了通过Pb - N化学键形成的CPB@TCN异质结的界面键合机制,为基于钙钛矿的异质结光催化剂的开发提供了新的见解。

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