Confining lead-free perovskite quantum dots in metal–organic frameworks for visible light-driven proton reduction,Materials Chemistry Frontiers

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Confining lead-free perovskite quantum dots in metal–organic frameworks for visible light-driven proton reduction
Materials Chemistry Frontiers ( IF 6.0 ) Pub Date : 2021-09-03 , DOI: 10.1039/d1qm01006a
Yao-Yao Wang ₁ , Xue-Yang Ji ₁ , Meng Yu ₁ , Jun Tao ₁

Affiliation

Inhibition of the recombination of photo-induced electrons and holes is critical for light harvesting and enhancing the photocatalytic efficiency of hydrogen production in metal–organic frameworks (MOFs). Herein, Cs₃Bi₂I₉ (CBI) quantum dots (QDs) were firstly loaded into the inner pores of MOF NH₂-UiO-66 (U6N) through an anti-solvent recrystallization (ASR) method. The light adsorption wavelength of the MOF composite was significantly extended to the visible region, and remarkably, the complementary electronic band structures between MOF and CBI resulted in spatial separation of photogenerated electron–hole pairs in this material. Thereby, under visible light irradiation, the prepared catalysts exhibited high H₂ production activity of 32.21 μmol g⁻¹ h⁻¹ that originated from photocatalytic proton reduction without introducing noble metals, far surpassing the MOF and CBI counterparts. In addition, under the synergistic effect of CBI QDs and low-coordination Pt metal clusters, the photocatalytic hydrogen production rate can be further improved to 141.87 μmol g⁻¹ h⁻¹ with a TON value of 17.74. The electron migration mechanism among CBI and U6N, and the microstructure of low coordination Pt clusters was also investigated through transient absorption spectra (TAS) and X-ray absorption spectra (XAS).

中文翻译：

将无铅钙钛矿量子点限制在金属有机框架中用于可见光驱动的质子还原

抑制光致电子和空穴的复合对于光收集和提高金属有机框架（MOF）中产氢的光催化效率至关重要。在此，Cs ₃ Bi ₂ I ₉ (CBI) 量子点(QDs) 首先通过反溶剂重结晶(ASR) 方法加载到MOF NH ₂ -UiO-66 (U6N)的内孔中。MOF 复合材料的光吸收波长显着扩展到可见光区，并且显着地，MOF 和 CBI 之间的互补电子能带结构导致该材料中光生电子 - 空穴对的空间分离。因此，在可见光照射下，制备的催化剂表现出高 H ₂32.21 μmol g ^-1 h ^{-1 的}生产活性源于光催化质子还原而不引入贵金属，远远超过 MOF 和 CBI 对应物。此外，在CBI QDs和低配位Pt金属簇的协同作用下，光催化产氢速率可进一步提高至141.87 μmol g ^-1 h ^-1，TON值为17.74。还通过瞬态吸收光谱（TAS）和X射线吸收光谱（XAS）研究了CBI和U6N之间的电子迁移机制以及低配位Pt簇的微观结构。

更新日期：2021-09-22

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