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7. Metallic Active Sites on MoO2(110) Surface to Catalyze Advanced Oxidation Processes for Efficient Pollutant Removal

Author

Ji, Jiahui, Aleisa, Rashed M, Duan, Huan, Zhang, Jinlong, Yin, Yadong, and Xing, Mingyang

Subjects
Catalysis, Inorganic Chemistry, Water Resources Engineering
Abstract

Advanced oxidation processes (AOPs) based on sulfate radicals (SO4⋅-) suffer from low conversion rate of Fe(III) to Fe(II) and produce a large amount of iron sludge as waste. Herein, we show that by using MoO2 as a cocatalyst, the rate of Fe(III)/Fe(II) cycling in PMS system accelerated significantly, with a reaction rate constant 50 times that of PMS/Fe(II) system. Our results showed outstanding removal efficiency (96%) of L-RhB in 10 min with extremely low concentration of Fe(II) (0.036 mM), outperforming most reported SO4⋅--based AOPs systems. Surface chemical analysis combined with density functional theory (DFT) calculation demonstrated that both Fe(III)/Fe(II) cycling and PMS activation occurred on the (110) crystal plane of MoO2, whereas the exposed active sites of Mo(IV) on MoO2 surface were responsible for accelerating PMS activation. Considering its performance, and non-toxicity, using MoO2 as a cocatalyst is a promising technique for large-scale practical environmental remediation. more...

Published
2020

11. Non-metallic iodine single-atom catalysts with optimized electronic structures for efficient Fenton-like reactions.

Author

Pei, Junjun, Liu, Jianbin, Fu, Kaixing, Fu, Yukui, Yin, Kai, Luo, Shenglian, Yu, Deyou, Xing, Mingyang, and Luo, Jinming

Subjects
PHYSICAL & theoretical chemistry, ACTIVATION energy, CHARGE exchange, WATER purification, POLLUTANTS
Abstract

In this study, we introduce a highly effective non-metallic iodine single-atom catalyst (SAC), referred to as I-NC, which is strategically confined within a nitrogen-doped carbon (NC) scaffold. This configuration features a distinctive C-I coordination that optimizes the electronic structure of the nitrogen-adjacent carbon sites. As a result, this arrangement enhances electron transfer from peroxymonosulfate (PMS) to the active sites, particularly the electron-deficient carbon. This electron transfer is followed by a deprotonation process that generates the peroxymonosulfate radical (SO5•−). Subsequently, the SO5•− radical undergoes a disproportionation reaction, leading to the production of singlet oxygen (1O2). Furthermore, the energy barrier for the rate-limiting step of SO5•− generation in I-NC is significantly lower at 1.45 eV, compared to 1.65 eV in the NC scaffold. This reduction in energy barrier effectively overcomes kinetic obstacles, thereby facilitating an enhanced generation of 1O2. Consequently, the I-NC catalyst exhibits remarkable catalytic efficiency and unmatched reactivity for PMS activation. This leads to a significantly accelerated degradation of pollutants, evidenced by a relatively high observed kinetic rate constant (kobs ~ 0.436 min−1) compared to other metallic SACs. This study offers valuable insights into the rational design of effective non-metallic SACs, showcasing their promising potential for Fenton-like reactions in water treatment applications. Electronic structure modulation of active sites is important for Fenton-like catalysis. A non-metallic iodine single-atom catalyst with C-I coordination is reported here, which can effectively activate peroxymonosulfate into 1O2 for water treatment. [ABSTRACT FROM AUTHOR] more...

Published
2025
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