Advanced Materials Interfaces
·
2021
·Vol. 8
·期 11
·2100178
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IF 6.147
Limei Dong,Yiming Li,Xiuping Chen,Dan Zhang,Yihao Guan
Poor sorption capacity and low biodegradability of carbamazepine (CBZ) lead to the difficulties in CBZ removal from water. Sulfate radical-based advanced oxidation process shows great potential for organic pollutant removal. Metal organic frameworks (MOFs) demonstrate great potential in catalytic field due to their excellent properties. Hence, cobalt-based metal organic framework (ZIF-67) nanoparticles are loaded on Fe 3 O 4 -MnO 2 composite, and then this composite is applied as peroxymonosulfate (PMS) activator for CBZ degradation. The prepared catalyst exhibits excellent catalytic performance because of the central metal cobalt of ZIF-67 and the synergistic effect between MnO 2 and ZIF-67. 81% of CBZ with a high initial concentration of 20 mg L −1 is rapidly removed from water within 2.5 min. The prepared catalyst can be convenient to recycle under magnetic field while maintaining its high catalytic stability. Degradation mechanism analysis indicates that both • OH and SO 4 •− contribute to CBZ degradation, but SO 4 •− is the main radical species. XPS spectra reveal that Co(II)/Co(III), Mn(II)/Mn(III)/Mn(IV), and Fe(II)/Fe(III) are involved in PMS activation. The degradation pathway is put forward based on the detection of intermediates. This study provides a new inspiration for the fabrication of magnetic metal oxide-MOFs catalysts with outstanding recycling performance for PMS activation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Xiaohui Fan,Heng Lin,Jinjin Zhao,Yican Mao,Jiaxing Zhang,Hui Zhang
Activation of peroxymonosulfate (PMS) for organic-contaminated water remediation is a promising strategy. In this study, a sludge-derived biochar (SBC) was prepared as an efficient and low-cost metal-free catalyst to activate PMS for the abatement of bisphenol A (BPA) in water. The results demonstrate that BPA could be rapidly oxidized by the combination of SBC and PMS. Compared with the slight adsorption (8.1%) by SBC alone and limited direct oxidation (2.4%) by sole PMS, the removal efficiency of BPA was boosted to 94.5% within 60 min in the presence of both SBC and PMS. Active species participating in the rapid elimination of BPA were investigated via both chemical quenching experiment and electron paramagnetic resonance (EPR) technique. The results indicate that non-radical rather than radical process plays an important role in BPA abatement in the SBC/PMS system. The electron-transfer non-radical process was further verified by the open circuit potential test. It is proposed that PMS is bound to SBC to form a surface reactive complex (SBC-PMS*), which would abstract the electrons from the adsorbed BPA through the conductive carbon tunnel. The present work provides an alternative of controlling waste by waste.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 32
·17366-17379
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IF 12.732
Junjie Zhang,Wenran Gao,Yamei Yue,Wei Wang,Fatang Tan,Xinyun Wang,Xueliang Qiao,Po Keung Wong
Herein, biactive centers of Fe0-anchored graphitic N-rich graphene (Fe-GNG) were constructed via coordination and hydrogen bonding assemblies followed by calcination. The obtained Fe-GNG exhibited excellent peroxymonosulfate (PMS) activation ability to degrade diverse organic pollutants, accompanied by very low activation energy. Electron paramagnetic resonance and quenching experiments indicated that ˙OH and 1O2 were the predominant reactive species responsible for organics degradation, and were generated from PMS activation mainly at Fe0 and graphitic N sites, respectively. The degradation process had wide pH (2.2–10.3) and temperature (5–45 °C) application ranges, and a high tolerance to common matrix species, which enabled application to natural water systems. Furthermore, the magnetic Fe-GNG catalyst exhibited high stability and reusability, still degrading over 90% organics after five runs. This work provides a feasible strategy to construct multiple active sites for PMS activation, and clarifies the synergistic effect of metal and carbonaceous materials in radical and nonradical activation processes.
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CHEMOSPHERE
·
2021
·
IF 7.086
Xiaoping Liao,Jinru Cao,Ying Hu,Caixiang Zhang,Lisong Hu
Although various activated peroxymonosulfate (PMS) processes have been applied widely for the destruction of recalcitrant organics due to its high generation potential of various electrophiles reactive oxygen species (e.g., sulfate and hydroxyl radicals and singlet oxygen), non-radical-based PMS reactions with pollutants are poorly understood. Especially, relatively little information exists on the reactivity of PMS towards organic ester compounds such an organophosphorus pesticides (OPPs). Herein, we systematically studied the unactivated PMS-induced transformation of methyl parathion, a stubborn and toxic OPP. Specifically, direct reaction rather than electrophile radical-based oxidation was responsible for the rapid degradation of methyl parathion. The contribution of the produced singlet oxygen ( 1 O 2 ) from the self-decomposition of PMS to methyl parathion degradation can be neglected. The degradation rate constant ( k obs ) was strongly dependent on PMS loading and solution pH. The implication of the PMS reaction with methyl parathion for environment treatment was further evaluated by investigating the effects of common water matrices such as sediment humic acids , Cl − , and natural water. The identified metabolic products revealed that exposure to PMS resulted in hydrolysis and oxidation to methyl parathion. Further study demonstrated that PMS was also capable of effectively oxidizing other typical OPPs without explicit activation. This study provides novel insights into the reaction of methyl parathion with PMS, which indicate feasibility for the decontamination of OPP-contaminated environments.
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GONDWANA RESEARCH
·
2021
·
IF 6.051
Zhuozhi Ouyang,Zhiping Zhang,Yao Jing,Linjie Bai,Manyi Zhao,Xinrui Hao,Xiaoqin Li,Xuetao Guo
Microplastics (MPs) pollution is becoming a global environmental problem due to the ubiquity. Knowledge about transformation process of MPs under ultraviolet (UV) irradiation was critical to understanding the environmental fate of these particles. In this study, the photo-aging characteristics and mechanisms of polyvinyl chloride (PVC) under different UV irradiations in the air or water condition were comprehensively investigated. When the PVC was exposed to the UVA, UVB and UVC irradiation, the surface morphology, functional group, crystal structure, and elemental composition of PVC were systematically characterized. With the increasing of aging time, the PVC was identified as more oxygen-containing functional groups, higher carbonyl index, and higher crystallinity, especially under the UVC irradiation. Based on the Two-dimensional correlation Fourier transform infrared spectroscopy (2D-FTIR-COS), the active sites and aging sequence of functional groups were confirmed under UVA, UVB and UVC irradiation. The reactive oxygen species (ROS) were produced and increased with the aging time as the whole. Corresponding to the aging results, the intensity of ROS and toxicity from leaching under UVC irradiation was greater than that under UVA or UVB. These findings provide direct evidences of photo-aging processes of MPs and the potential ecological risks resulting from aging in the aquatic environments.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Zhijie Guan,Yanping Guo,Zhenhua Huang,Xiaojian Liao,Shaojin Chen,Xuelian Ou,Shuiyu Sun,Jialin Liang,Yongfeng Cai,Wenren Xie,Jiao Xian
In the industrial electroless metal plating process, efficient removal of organic-Ni and -Cu complexes from electroless plating effluent (EPE) remains a huge challenge. In this study, a novel and feasible process of heterogeneous catalytic ozonation combined with heavy metal chelation is proposed for the effective removal of organic-Ni and -Cu complexes from EPE. The method was evaluated in a continuous pilot-scale system (CPSS). Results show that the adoption of synchronous bi-directional flow enhanced the removal of total Ni and Cu. Under optimal conditions, the total Ni and Cu in the effluent decreased to 0.1 and 0.3 mg L −1 , respectively, meeting the Chinese discharge standard requirements. The CPSS indicated that efficient removal of total Ni and Cu ( > 95%) was consistently achieved for 300 days using the proposed process. Mechanistic analysis demonstrated that ethylenediamine tetraacetic acid-Ni (EDTA-Ni) and citrate-Cu (CA-Cu) were the main complexes present in EPE. Furthermore, there were 10 transformation products and their related pathways were also identified. The decomplexation of EDTA-Ni was found to be difficult, with its final products principally existing in the complexed states, while CA-Cu was readily broken down, releasing Cu (II) that can be easily chelated. Overall, these findings provide valuable and novel insights into the removal of organic-Ni and -Cu, supporting the practical application of the proposed process in advanced EPE treatment and other industrial wastewater treatment systems.
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JOURNAL OF MEMBRANE SCIENCE
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2021
·
IF 8.742
Jiaojiao Chen,Senqing Fan,Yu Chen,Yilin Wang,Ke Bai,Zenghui Mai,Zeyi Xiao
An electrocatalytic composite membrane with deep-permeation nano structure (DPNS) has been fabricated by flowing synthesis. The nano electrocatalyst MnO 2 is in situ successfully assembled in membrane pores and uniformly immobilized in membrane pores along the direction of membrane thickness. The size of MnO 2 nanoparticles immobilized in membrane pores is in the range of 33–35 nm, which is one-tenth of that immobilized on the membrane surface. The increased current density and the lower charge transfer resistance of the electrocatalytic composite membrane implied that a fast electron transfer can be achieved. As a concept-of-proof, the removal of phenol was applied to test the catalytic performance of the electrocatalytic composite membrane under the flow-through reaction mode, and the removal rate of phenol of being over 97% can be achieved under the condition of membrane flux of being 13.5 L m −2 h −1 . The apparent reaction rate constant could be increased by 2–3 orders of magnitude, owing to the enhanced contact by uniform distribution of membrane pores, as well as the confined space effect of membrane pores and the flow-through synergism enhancing mass transfer. The species of free radical can be determined as ·OH via ESR measurements for phenol oxidation . This electrocatalytic composite membrane (ECCM) with DPNS has good reusability and can provide a promising prospect for industrial application.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Shuzhao Pei,Han Shi,Jinna Zhang,Shengli Wang,Nanqi Ren,Shijie You
This study reports fluorine-doped titanium suboxide anode for electrochemical mineralization of hydrophobic micro-contaminant, tetrabromobisphenol A. Fluorinated TiSO anode promoted electro-generated hydroxyl radicals (•OH) with higher selectivity and activity, due to increased O 2 evolution potential and more loosely interaction with hydrophobic electrode surface. For electro-oxidation process, fluorine doping had an insignificant impact on outer-sphere reaction and exerted inhibition on inner-sphere reaction, as indicated by cyclic voltammogram performed on Ru(NH 3 ) 6 3+/2+ , Fe(CN) 6 3−/4− and Fe 3+/2+ redox couple. This facilitated electrochemical conversion of TBBPA and intermediates via more efficient outer-sphere reaction and hydroxylation route. Additionally, generated O 2 micro-bubbles could be stabilized on hydrophobic F-doped TiSO anode, which extended the three-phase boundary available for interfacial enrichment of TBBPA and subsequent mineralization. Under action of these comprehensive factors, 0.5% F-doped TiSO electrochemically reactive membrane could achieve 99.7% mineralization of TBBPA upon energy consumption of 0.52 kWh m −3 at current density of 7.8 ± 0.24 mA cm −2 (3.75 V vs SHE) and flow rate of 1628 LHM based on flow-through electrolysis. The modified anode exhibited superior performances compared with un-modified one with more efficient TBBPA removal, less toxic intermediate accumulation and lower energy consumption. The results may have important implications for electrochemical removal and detoxification of hydrophobic micro-pollutants.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Min Yu,Changduo Sun,Luhan Wang,Kun Zang,Mingzhe Li,Lei Zhou,Yian Zheng
Semi-coke (SC) is a solid waste of coal chemical process, and the comprehensive utilization of SC is a challenging issue. Based on physicochemical characteristics, SC was firstly utilized as a mineral biochar for activating persulfate (PS) to promote simultaneous degradation of sulfadiazine (SDZ) and tetracycline (TC) in a binary mixture. The influencing parameters were systematically investigated. The dominant reactive oxygen species (ROS) were identified by combination of quenching experiments and electron spin resonance (EPR) analysis. Subsequently, possible activation mechanism and degradation pathways were also proposed. With the evolution of SDZ and TC in SC/PS system, the Vibrio fischeri was used to examine the acute toxicity to explore the detoxification efficiency. The experimental results indicated that in such a binary system, a mutually promoted degradation occurred between SDZ and TC, and at optimized conditions of 0.75 g/L PS, 0.50 g/L SC, pH 3.0 and 30 ℃, the developed SC/PS system had high degradation ability for simultaneous removal of SDZ (97.8%) and TC (97.2%). The polar groups and defects of SC were conducive to the adsorption; the oxygen-containing functional groups, pyridine N and graphite C on SC surface could be used as active sites for activating PS to produce ROS. During the degradation process, both radical (•OH and SO 4 •− ) and non-radical ( 1 O 2 ) pathways coexisted. SC exhibited an excellent reusability, with the degradation efficiency of 84.5% for SDZ and 95.9% for TC after 4 cycles, and high mineralization efficiency of 67.5% after 4 h, demonstrating that such a unique SC/PS system exhibited a great potential for simultaneously efficient removal of different kinds of antibiotics in actual wastewaters.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Zhiyuan Feng,Qingling Tian,Qianqian Yang,Yanbo Zhou,Hongying Zhao,Guohua Zhao
The fine-tuning of generating hydroxyl radical ( OH) and singlet oxygen ( 1 O 2 ) was firstly proposed via the selectively photoelectrochemical (PE) reduction of oxygen with Cu-coordinated carbon-nitride-electrode (CuCN). Complete removal efficiency and trace Cu leaching (<0.01 ppm) were achieved during treatment of dimethyl phthalate and atrazine, which were mainly oxidized by OH and 1 O 2 , respectively. Besides, no toxic intermediates was detected in the whole degradation process. The overall oxygen reduction pathway in PE system was demonstrated by electron paramagnetic resonance measurements and quenching tests. The valence band position of CuCN was designed to be more negative (−1.5 V SHE ) for favoring the photocatalytic oxygen reduction. Specifically, Cu-N 2 -C as active sites optimized the Gibbs free energy of intermediate *OOH (ΔG *OOH = 3.99 eV) to improve the reactivity of two-electron oxygen reduction. The CuCN/photoelectrochemical system is applied for treatment of coal water slurry gasification (CWS) wastewater with high concentration of salt. The TOC of CWS was successfully decreased from 127 to 1.9 mg·L −1 in 3 h with a low specific energy consumption of 0.024−0.05 kW·h·g −1 ·TOC −1 . The treated CWS wastewater can be used for recovery and utilization of salt as chemical raw materials. This work highlights the important role of synergistic photo-electro-catalytic effect in regulating the generation of active oxygen species via oxygen reduction pathway, which can be a promising way especially for salinity coal wastewater remediation.
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NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 6
·3298-3310
·
IF 3.591
Zhi-Yu Liang,Ren-Kun Huang,Ruo-Wen Liang,Dan-Hua Xie,Gui-Yang Yan
Nowadays, visible-light-driven photocatalysts are considered to be prospective candidates for solving the crisis of energy shortage and environment pollution. Herein, with the support of WO3 nanorods (NRs), which possess a fast electron transmission and low carrier diffusion, a series of direct Z-scheme ZnIn2S4/WO3 photocatalysts are exquisitely fabricated by an in situ self-assembly route with ZnIn2S4 (ZIS) and WO3 NRs. Photocatalytic activities towards both selective hydrogenation of aromatic nitro compounds and non-selective oxidation of organic compounds demonstrate that these as-fabricated heterostructured nanocomposites exhibit remarkably enhanced photocatalytic activities owing to the highly efficient separation of photogenerated electrons and holes. Furthermore, the characteristics of electron spin resonance (ESR) spectra clearly suggest that the as-fabricated nanocomposites follow the direct Z-scheme-dominated photoredox catalytic mechanism. Additionally, combining the results of ESR and X-ray photoelectron spectroscopy (XPS), it can be concluded that the photo corrosion of ZnIn2S4 is significantly postponed after integration with WO3 NRs. Finally, we will be greatly pleased if this work could afford a theoretical exemplification and synthetic strategy for rationally designing and utilizing direct Z-scheme photocatalysts.
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CHEMOSPHERE
·
2020
·
IF 5.778
Meng Wu,Yun Wang,Bin Lu,Bing Xiao,Rufen Chen,Hui Liu
In this study, the low-cost preparation of iron phosphide by using pickling waste liquor as the initial material was performed through a two-step reaction. The degradation of Orange G was evaluated using iron phosphide coupled with peroxymonosulfate to construct a catalytic system. The removal efficiencies of Orange G and total organic carbon reached 97.4 and 58.4% at 60 min, respectively. Iron phosphide has dual-catalysis centers for the activation of PMS. Multiple free radicals (e.g., SO 4 •− , HO • , SO 5 •− , and O 2 •− ) and singlet oxygen were involved in the pollutant degradation , of which sulfate radicals played the main role. The iron phosphide catalyst exhibited excellent recycling stability, and its catalytic efficiency reached 95% after five cycles. In summary, the Fe 2 P/PMS system—as a Fenton-like catalytic system—has certain advantages, including low cost, high efficiency, sufficient reusability, and good stability, all of which are favorable for its practical application.
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