Interface Engineering of Co(OH)2 Nanosheets Growing on the KNbO3 Perovskite Based on Electronic Structure Modulation for Enhanced Peroxymonosulfate Activation

化学 电子结构 密度泛函理论 钙钛矿(结构) 费米能级 电子转移 催化作用 化学吸附 反键分子轨道 物理化学 光化学 计算化学 原子轨道 结晶学 电子 有机化学 物理 量子力学
作者
Juanjuan Qi,Xiaoyong Yang,Po-Yueh Pan,Taobo Huang,Xudong Yang,Chong‐Chen Wang,Wen Liu
出处
期刊:Environmental Science & Technology [American Chemical Society]
卷期号:56 (8): 5200-5212 被引量:310
标识
DOI:10.1021/acs.est.1c08806
摘要

Material-enhanced heterogonous peroxymonosulfate (PMS) activation on emerging organic pollutant degradation has attracted intensive attention, and a challenge is the electron transfer efficiency from material to PMS for radical production. Herein, an interface architecture of Co(OH)2 nanosheets growing on the KNbO3 perovskite [Co(OH)2/KNbO3] was developed, which showed high catalytic activity in PMS activation. A high reaction rate constant (k1) of 0.631 min–1 and complete removal of pazufloxacin within 5 min were achieved. X-ray photoelectron spectroscopy, X-ray absorption near edge structure spectra, and density functional theory (DFT) calculations revealed the successful construction of the material interface and modulated electronic structure for Co(OH)2/KNbO3, resulting in the hole accumulation on Co(OH)2 and electron accumulation on KNbO3. Bader topological analysis on charge density distribution further indicates that the occupations of Co-3d and O-2p orbitals in Co(OH)2/KNbO3 are pushed above the Fermi level to form antibonding states (σ*), leading to high chemisorption affinity to PMS. In addition, more reactive Co(II) with the closer d-band center to the Fermi level results in higher electron transfer efficiency and lower decomposition energy of PMS to SO4•–. Moreover, the reactive sites of pazufloxacin for SO4•– attack were precisely identified based on DFT calculation on the Fukui index. The pazufloxacin pathways proceeded as decarboxylation, nitroheterocyclic ring opening reaction, defluorination, and hydroxylation. This work can provide a potential route in developing advanced catalysts based on manipulation of the interface and electronic structure for enhanced Fenton-like reaction such as PMS activation.
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