ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2022
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IF 11.357
Xiao-Chi Feng,Zi-Jie Xiao,Hong-Tao Shi,Bai-Qin Zhou,Yong-Mei Wang,Hui-Zhong Chi,Xiao-Hang Kou,Nan-Qi Ren
Current research has widely applied heteroatom doping for the promotion of catalyst activity in peroxymonosulfate (PMS) systems; however, the relationship between heteroatom doping and stimulated activation mechanism transformation is not fully understood. Herein, we introduce nitrogen and sulfur doping into a Co@rGO material for PMS activation to degrade tetracycline (TC) and systematically investigate how heteroatom doping transformed the activation mechanism of the original Co@rGO/PMS system. N was homogeneously inserted into the reduced graphene oxide (rGO) matrix of Co@rGO, inducing a significant increase in the degradation efficiency without affecting the activation mechanism transformation. Additionally, S doping converted Co3O4 to Co4S3 in Co@rGO and transformed the cooperative oxidation pathway into a single non-radical pathway with stronger intensity, which led to a higher stability against environmental interferences. Notably, based on density functional theory (DFT) calculations, we demonstrated that Co4S3 had a higher energy barrier for PMS adsorption and cleavage than Co3O4, and therefore, the radical pathway was not easily stimulated by Co4S3. Overall, this study not only illustrated the improvement due to the heteroatom doping of Co@rGO for TC degradation in a PMS system but also bridged the knowledge gap between the catalyst structure and degradation performance through activation mechanism transformation drawn from theoretical and experimental analyses.
研究领域:
环境科学
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材料科学
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理论化学
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产品关联
DOI
PubMed
高影响因子
Nanomaterials
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2023
·Vol. 14
·期 1
·74
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IF 5.3
Xin Zhong,Meihuan Ji,Wenxin Wu,Caicai Lu,Wenping Liu,Fubin Jiang
In this work, the heterojunctions of CuInS2embedded in the g-C3N4materials (xCuInS2/g-C3N4, abbreviated as xCIS/GCN) was successfully prepared for peroxymonosulfate (PMS) activation under visible light. The catalysts are characterized by different techniques, such as XRD, FTIR, SEM, TEM, and UV-vis. The unique heterojunction composites can suppress the recombination of photogenerated pairs. The catalytic results showed that the 3CIS/GCN exhibited excellent catalytic levofloxacin (LVF) degradation efficiency, while more than 98.9% of LVF was removed in 60 min over a wide pH range. SO4•−, O2•−, OH•, and1O2were verified as the main reactive species for LVF degradation via the quenching experiments and electron paramagnetic resonance technology (EPR). The synergetic effect of xCIS/GCN, PMS, and visible light irradiation was discussed. The possible LVF degradation pathway was proposed through byproducts analysis (LC-MS). Moreover, the 3CIS/GCN/vis-PMS system has very low metal leaching. Owing to xCIS/GCN having good properties for PMS activation, it has potential applications for LVF or other hazardous pollutants degradation.Keywords:peroxymonosulfate;visible-light-assisted PMS activation;antibiotics
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
Nanoscale
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2023
·Vol. 15
·期 16
·7352-7364
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IF 6.7
Xiaojuan Bai,Wei Song,Xuan Ling,Linlong Guo,Derek Hao,Xiao Zhang
The rational design of photocatalytic nanomaterials with unique structures is critical for remediating environmental problems and thus reducing ecological risks. In this work, we employed H2 temperature-programmed reduction to modify MFe2O4 (M = Co, Cu, and Zn) photocatalysts for obtaining additional oxygen vacancies. After activation of PMS, naphthalene and phenanthrene degradation rates in the soil phase were increased by 3.24-fold and 1.39-fold, respectively, and 1.38-fold for naphthalene in the aqueous phase by H-CoFe2O4−x. The extraordinary photocatalytic activity is attributed to the oxygen vacancies on the H-CoFe2O4−x surface, which promote electron transfer and thus enhance the redox cycle from Co(III)/Fe(III) to Co(II)/Fe(II). In addition, oxygen vacancies are used as electron traps to hinder the recombination of photogenerated carriers and accelerate the generation of hydroxyl and superoxide radicals. Quenching tests showed that the addition of p-benzoquinone resulted in the greatest decrease in the degradation rate of naphthalene (inhibition of about 85.5%), demonstrating that O2˙− radicals are the main active species in the photocatalytic degradation of naphthalene. H-CoFe2O4−x showed improved degradation performance in synergy with PMS (82.0%, kapp = 0.00714 min−1) while maintaining excellent stability and reusability. Hence, this work provides a promising approach for the design of efficient photocatalysts to degrade persistent organic pollutants in soil and aqueous environments.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
Processes
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2023
·Vol. 11
·期 3
·903
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IF 3.5
Yajie Wang,Xin Dong,Chengfeng Liu,Peng Cheng,Gilles Mailhot
The decolorization of azo dye Orange II using a UVA-Fe3+-PMS-oxalate system was studied. A series of experiments was performed to investigate the effects of several variables, including the pH, PMS dosage, Fe3+concentration, oxalate concentration, and coexisting anions. The results revealed that a lower pH facilitated the decolorization, and relatively high decolorization efficiency (97.5%) could be achieved within 5 min at pH 3.0. The electron paramagnetic resonance (ESR) and radical quenching experiments revealed that SO4•−played a crucial role in the decolorization of Orange II (85.8%),•OH was of secondary importance (9%), and1O2made a small contribution to the decolorization (5.2%). Furthermore, the formation of•OH in the experimental system strongly depended on HO2•/O2•−. These reactive oxidants were able to directly attack the azo bond of the luminescent group in Orange II and initiate the decolorization process. The efficient UVA-Fe3+-PMS-oxalate system showed great application potential in the treatment of wastewater contaminated by azo dyes.Keywords:PMS activation;Orange II;decolorization;UVA irradiation;Fe3+-oxalate complexes
研究领域:
环境科学
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化学工程
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
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2023
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IF 6.7
Guanwei Peng,Yanyu Xie,Ying Wang,Qi Yu,Youyi Huang,Shuwu Liu,Limin Lu
Peroxymonosulfate (PMS)-assisted photocatalytic processes are economical and green strategies for the treatment of pesticide pollution. However, its degradation efficiency is severely hindered by the sluggish kinetics of active centers regeneration and low charge-transfer. Herein, S-scheme Bi 2 Fe 4 O 9 /BiOBr heterogeneous material was designed to activate PMS for thiabendazole (TBZ) degradation. Bi 2 Fe 4 O 9 and BiOBr have similar structural unit of [Bi 2 O 2 ] 2+ to share the Bi-O bonds, which is favorable to form asymmetric interface and enhance the polarization. Based on these unique characteristics between Bi 2 Fe 4 O 9 and BiOBr, a robust internal electric field in the S-scheme heterojunction is built, which could provide driving force to boost the electron-transfer process and encourage the sustainable regeneration of Fe 2+ . After optimizing the proportion of Bi 2 Fe 4 O 9 on the composite, it was found that 50 wt% Bi 2 Fe 4 O 9 /BiOBr (BFB-50) exhibits the best TBZ removal efficiency after 30 min visible light irradiation, which is 2.25 and 12 folds compared to Bi 2 Fe 4 O 9 and BiOBr, respectively. Furthermore, electron paramagnetic resonance (EPR) and radical trapping experiments indicate that 1 O 2 and SO 4 •- involving oxidation mechanism impart maximum contribution towards TBZ degradation. The possible pathways of TBZ degradation are reasonably proposed by the HPLC-MS and the toxicity evolution of TBZ is appraised using the ECOSAR software. This study provides an insight into the fabrication of S-scheme heterojunction for environment remediation through the photocatalysis/sulfate-mediated advanced oxidation process.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2025
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IF 7.8
Zhongsen Yan,Binbin Li,Guohui Liu,Zhenyu Lu,Haiqing Chang,Juxiang Jin,Wenxin Dai,Yao Qu,Fangshu Qu
Humic acid (HA), a widely prevalent natural organic matter in aquatic environments, poses serious health risks due to its potential to form carcinogenic by-products during water treatment. While the photo-Fenton process can be employed for HA degradation, its effectiveness is often hindered by the poor catalytic performance of conventional catalysts. In this study, Co 3 O 4 was modified with nitrogen-doped carbon quantum dots (NCDs) and immobilized on a PVDF membrane. Compared with Co 3 O 4 /PVDF, Co 3 O 4 /NCDs/PVDF system achieved 85.1 % HA removal and 66 % mineralization within 60 min through photocatalytic peroxymonosulfate (PMS) activation as well as showed excellent stability in cycle experiments. The incorporation of NCDs enhanced the synergistic effect between light and PMS, improved light absorption due to the narrowed bandgap of Co 3 O 4 /NCDs/PVDF, and played a significant role in generating the primary reactive species, 1 O 2 . Additionally, Co 3 O 4 /NCDs/PVDF effectively controlled Co ions leaching. Finally, the degradation intermediates were identified, and the degradation pathways were proposed. The photo-Fenton degradation of HA preferentially broke unsaturated bonds and degraded aromatic ring compounds. The Co 3 O 4 /NCDs/PVDF photo-Fenton catalytic system serves as an effective approach for boosting the efficiency of photo-Fenton degradation.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
Water
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2023
·Vol. 15
·期 12
·2243
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IF 3.4
Jing Wang,Quanfeng Wang,Pei Gao,Da Sun,Libo Jin,Li Ma,Lan Yang,Jujiao Zhao
Peroxymonosulfate (PMS) activation is an intriguing technology for refractory organic pollutant removal in wastewater treatment. Herein, a highly dispersed Mn-Ce bimetallic oxide on carbon nanotubes (MCC) was synthesized and applied to catalyze PMS for the degradation of phenol. The material was well characterized using a transmission electron microscope (TEM), N2adsorption–desorption isotherms, X-ray powder diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). The synthesized MCC showed superior activity for PMS activation. Thekvalue of phenol removal with MCC is 0.135 min−1, which is greatly superior to that of CNT (6.17 × 10−5min−1) and Mn-Ce bimetallic oxide (3.18 × 10−4min−1). Electron paramagnetic resonance (EPR), along with radical quenching experiments, revealed that the activation of PMS by MCC for phenol degradation involves both radical and non-radical reaction pathways. Moreover, a synergic effect between Mn-Ce bimetallic oxide and CNT was identified to be responsible for the outstanding catalytic activity.Keywords:PMS activation;Mn-Ce bimetallic oxide;CNT;synergic effect
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Ke Xiang,Shaoyi Wu,Tiefeng Xu,Wangyang Lu
The photocatalysis-assisted peroxymonosulfate (PMS) activation process has shown great potential for organic wastewater treatment. Herein, the composite photocatalyst (FeTAPc/PDI/CN) was obtained by grafting graphitic carbon nitride (CN) and amino iron phthalocyanine (FeTAPc) onto both ends of perylene tetracarboxylic anhydride (PTCDA) through an imidization process. Under simulated solar irradiation, the catalyst exhibited a remarkable degradation performance toward the target pollutant by activated PMS over a wide pH range from 3 to 11. The degradation efficiency of SMX reached 100 % in 7 min with the reaction kinetic constant of 0.845 min −1 , which was 13 times higher than that of pure CN. In addition, the removal rate of FeTAPc/PDI/CN-4 for SMX was more than 80 % after 9 cycles. The introduction of phthalocyanine and PDI improved the separation efficiency of photogenerated electron-hole pairs. Furthermore, the active species involved in the SMX degradation were identified as •OH, SO 4 • - , •O 2 – and 1 O 2 . The possible degradation pathways were proposed based on the identified intermediates, in which the oxidation of the amino group on the benzene ring was the main degradation pathway. This study is anticipated to result in a favorable method for designing CN-based photocatalysts with high stability and excellent catalytic activity for environmental remediation.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Xinyi Zhang,Weibao Liu,Yuerong Zhou,Yunhe Li,Ying Yang,Jianfeng Gou,Jiangwei Shang,Xiuwen Cheng
In order to further expand the practical applicability of nano photo-activators, a low-toxicity bismuth ferrite mixture (BFO) combined with MnO 2 were used to construct nano-catalyst@nickel foam (NF) composite material. A variety of characterization methods were applied to determine the physical, chemical and photoelectrochemical properties of BFO/MnO 2 @NF. Subsequently, the performance of BFO/MnO 2 @NF/PMS/Light degradation system was evaluated through the enrofloxacin (ENR) removal experiment. And 87.5% of ENR could achieve removal with 4 cm 2 of BFO/MnO 2 (3:1)@NF and 0.6 g L −1 of peroxymonosulfate (PMS) at the pH of 6.86 in the coupled system. In addition, during the ENR degradation process, the leaching percentages of Bi, Fe, and Mn ions in the BFO/MnO 2 nano powder and BFO/MnO 2 @ NF were 0.041%, 0.29%, 0.12% and 0.035%, 0.068%, 0.084% (0.035% of Ni dissolution), respectively. It could be seen that the leaching concentration of metal ions during the reaction of the nickel foam-supported composite material was much lower than that of the corresponding nano-catalysts powder. Furthermore, the coupled system maintained excellent catalytic performance even after 8 running cycles. Thus, the BFO/MnO 2 @NF was easy to recover from the system and met the needs of practical applications, which would provide more opportunities for the design of nano-catalysts and practical applications in wastewater treatment processes.
研究领域:
环境科学
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材料科学
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水处理技术
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Yizhou Wu,Wenqi Zhou,Liang Zhou,Su-Il In,Juying Lei,Lingzhi Wang,Jinlong Zhang,Yongdi Liu
The utilization of near-infrared (NIR) light with strong photothermal effect in photo-Fenton or Fenton-like systems for the degradation of organic pollutants is always ignored. In this study, we have synthesized a novel photothermal Fenton-like catalyst (Co 3 O 4 /PDA) to activate peroxymonosulfate (PMS) for the degradation of antibiotics. The Co 3 O 4 in the nanocomposite acts as a PMS activator, while unexpectedly, PDA was found to accelerate the redox cycle of Co 2+ /Co 3+ . Both Co 3 O 4 and PDA are black-colored photothermal materials with excellent NIR absorption properties. During the degradation process, the light-to-heat conversion ability of Co 3 O 4 and PDA enables a higher temperature, which innovatively boosts the rate of PMS catalytic activation. Mechanistic studies revealed that the increased temperature effectively promotes the heterogeneous catalytic PMS activation by Co 3 O 4 /PDA. As a result, the Co 3 O 4 /PDA + PMS + NIR system exhibits greatly enhanced degradation performance. Furthermore, this degradation system demonstrates strong tolerance to different operation conditions, and the catalyst exhibits good stability in cycling tests. These results demonstrate the favorable application prospects of this photothermal Fenton-like system in environmental water remediation. The findings also contribute valuable insights towards the development of efficient strategies for the photothermal activation of PMS.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Siyuan Diao,Lili Meng,Lanlan Feng
The application of peroxymonosulfate (PMS)-based advanced oxidation processes , facilitated by the incorporation of metal-deposited MoS 2 catalyst, has attracted considerable interest in recent years within the scientific community. Nevertheless, investigating the structure-performance relationship between MoS 2 and deposited metal still presents a formidable challenge, yet a highly desirable pursuit. In this study, a Cu-MoS 2 single-atom catalyst (SAC) was successfully synthesized by a photo-deposition method, wherein Cu ions were deposited on the MoS 2 surface. The Cu-MoS 2 /PMS system exhibits exceptional degradation performance for tetracycline (TC), with a removal efficiency reaching 96% at 60 min. Furthermore, the density functional theory (DFT) is applied to investigate the coordination microenvironment of the catalyst by depositing of Cu. Experimental and theoretical calculations results exhibit that, on one hand, the introduction of Cu decreases the adsorption energy barrier and enhances the adsorption capacity of the catalyst for PMS. On the other hand, the abundant presence of Cu on the surface of the MoS 2 facilitates an accelerated transfer of electron , availing the formation of reactive oxygen species (ROS) via the distinct pathway: MoS 2 → transition metal → PMS. Concurrently, the synergistic interaction between Mo and Cu expedites rapid valence evolution of Mo 4+ /Mo 5+ /Mo 6+ and Cu + /Cu 2+ , thereby further enhancing the PMS activation. Hence, adjusting the coordination microenvironment of the catalyst represents a promising strategy for enhancing the catalytic activity.
研究领域:
环境科学
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催化材料
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理论化学
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产品关联
DOI
高影响因子
WATER RESEARCH
·
2021
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IF 11.236
Xiangyu Chen,Juanjuan Yao,Hongsen Dong,Mingjian Hong,Naiyun Gao,Zhi Zhang,Wenchao Jiang
A collaborative system including peroxymonosulfate (PMS) activation in a photocatalytic fuel cell (PFC) with an BiOI/TiO 2 nanotube arrays p-n type heterojunction as photoanode under visible light (PFC(BiOI/TNA)/PMS/vis system) was established. Xenon lamp was used as the light source of visible light. A 4.6 times higher pseudo-first-order bezafibrate (BZF) degradation rate constant was achieved in this system compared with the single PFC(BiOI/TNA)/vis system. The radical quenching experiments revealed that the contribution of reactive oxidative species (ROS) followed the order of 1 O 2 ≈ h + >> •OH > SO 4 •− >>O 2 •− . The EPR tests demonstrated that PMS addition enlarged the formation of 1 O 2 , •OH and SO 4 •− , but suppressed O 2 •− yield. Interestingly, 1 O 2 was further proved to dominantly originated from the priority reaction between positive photoinduced holes ( h + ) and negatively charged PMS. Besides, N 2 -purging tests and density functional theory calculation indicated that PMS probably reacted with residual photoinduced electron ( e − ) on the more negative conduction band (CB) of BiOI to form •OH and SO 4 •− , but competed with dissolved oxygen. Other e − transferred to the less negative CB of TNA through p-n junction will efficiently move to cathode through the external circuit. The greatly promoted power generation of PFC system was observed after PMS addition due to extra h + consumption and efficient e − separation and transfer. Besides, three possible pathways for BZF degradation were proposed including hydroxylation, fibrate chain substituent and amino bond fracture. This study can provide new insights into the mechanisms of PMS assisted photocatalysis and accompanying energy recovery.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）