Asymmetrical facet-oriented anisotropic charge migration of MIL-101(Fe) with internal electric field-steered photogenerated holes for boosting photocatalytic oxidation

Applied Catalysis B: Environment and Energy Pub Date : 2024-09-05 DOI:10.1016/j.apcatb.2024.124564

Yifei Wang, Yan Du, Peiyang Duan, Beibei Li, Junshan Li, Yongfa Zhu

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Abstract

Controllably steering the photogenerated charge behaviors of semiconductor photocatalysts is crucial in improving photocatalytic oxidation. By engineering the primary facet from (101) to (112), the asymmetrical feather of MIL-101(Fe)(112) result in potential difference on varied facets to contribute to anisotropic charge migration, which has been determined by the preferentially photodeposited cocatalysts on facet (112) and facet (119) of the nanocrystal. Thus-observed anisotropic charge migration of MIL-101(Fe)(112) contribute to 10 times stronger internal electric field (IEF) to accelerate charge separation and migration. Also, we demonstrate the lowest unoccupied crystal orbital (LUCO) of MIL-101(Fe)(112) deepened (up to 3.33 eV vs. NHE) and acquire 3.5 times higher photogenerated holes for robust hole oxidation capacities. As a proof-of-concept, the optimal MIL-101(Fe)(112) can acquire 100 % higher degradation rate and 33 % higher mineralization than MIL-101(Fe)(101). This work highlights the importance of unsymmetric facet manipulation in tailoring photocatalysts for efficient photocatalytic oxidation.

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具有内部电场引导的光生空穴的 MIL-101(Fe)非对称面向各向异性电荷迁移，用于促进光催化氧化

可控地引导半导体光催化剂的光生电荷行为对于改善光催化氧化至关重要。MIL-101(Fe)(112) 的主刻面从(101)变为(112)，其不对称羽化导致了不同刻面上的电位差，从而促进了各向异性电荷迁移，这是由纳米晶体刻面(112)和刻面(119)上优先光沉积的共催化剂决定的。由此观察到的 MIL-101(Fe)(112)各向异性电荷迁移有助于产生 10 倍强的内电场 (IEF)，从而加速电荷分离和迁移。此外，我们还证明 MIL-101(Fe)(112)的最低未占晶体轨道（LUCO）加深了（与 NHE 相比高达 3.33 eV），光生空穴增加了 3.5 倍，从而提高了空穴氧化能力。作为概念验证，最佳的 MIL-101(Fe)(112)比 MIL-101(Fe)(101)的降解率高 100%，矿化度高 33%。这项工作凸显了非对称面处理在定制光催化剂以实现高效光催化氧化方面的重要性。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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Applied Catalysis B: Environment and Energy

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