Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Shaoru Liu,Weizi Zhang,Peng Zhu,Songlin Zuo,Haian Xia
The study reports a facile synthesis of Ag-g-C 3 N 4 /AC composites with highly photocatalytic activity and good adsorption capacity by an impregnation-thermal polycondensation process. The resulting Ag-g-C 3 N 4 /AC composites were used for treatment of different pollutants in water including Rhodamine B (RhB), Cr(VI) ions and pathogens . When the precursor mass ratio of urea and AC was 2:2, the resultant Ag-g-C 3 N 4 /AC catalyst showed the best photocatalytic performances. In particular, the composite photocatalysts exhibited highly bactericidal efficiency, which could reach 99.9% after 120 min of irradiation. The higher photocatalytic performances of Ag-g-C 3 N 4 /AC composites were attributed to the surface plasmon resonance (SPR) effect of Ag nanoparticles (NPs) together with the interfacial synergistic effects. Meanwhile, AC not only exhibited excellent adsorption capacity, but also decreased aggregation of g-C 3 N 4 , which could enhance the separation efficiency of photogenerated charge carriers. It was uncovered through Electron Spin Resonance (ESR) and radical scavenger experiments that • OH radicals, • O 2 − and h + participate in the RhB degradation under the visible light. This work shows that the high-efficient and stable Ag-g-C 3 N 4 /AC composites have a great potential in the treatment of organic pollutants , toxic heavy metals and pathogenic bacteria by adsorption/photocatalysis for practical water treatment .
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ACS Omega
·
2021
·
IF 3.512
Yuqing Zhao,Hang Yang,Jianfa Sun,Yi Zhang,Shibin Xia
In this study, the utilization of secondary pyrolysis oil-based drilling cuttings ash (OBDCA-sp) to activate peroxymonosulfate (PMS) for pollutant removal was investigated. The chemical and physical properties of OBDCA-sp were explicitly analyzed via multiple characterization. The activation efficiency of OBDCA-sp for PMS was tested using humic acid (HA) as the target pollutant. 92% of HA and 52% of total organic carbon in solution could be removed using OBDCA-sp-activated PMS under optimal conditions: OBDCA-sp dosage at 4 g/L, PMS concentration at 4 mmol/L, HA concentration at 10 mg/L, and pH value at 7. After four cycles, 84% removal rate of HA could still be achieved using OBDCA-sp to activate PMS. The main catalysis elements for PMS activation in OBDCA were postulated to be Fe(III), Co(III), and Mn(III), based on X-ray photoelectron spectroscopy and X-ray diffraction results. The results of the quenching experiment indicated that SO4•–, •OH, and 1O2 were the main reactive oxygen species (ROS) and that 1O2 was the dominant ROS in the HA removal process. Radical trapping experiments indicated the presence of SO4•–, •OH, and 1O2 in the reaction system. This study presented a novel utilization path of OBDCA in the field of environmental remediation.
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CHEMOSPHERE
·
2021
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IF 7.086
Yu Li,Yong Feng,Bin Yang,Zequn Yang,Kaimin Shih
The activation of persulfate by ferrous iron (Fe(II)) is of great interest to the environmental remediation community, but the reduction of ferric iron (Fe(III)) to Fe(II) is slow and the accumulation of iron sludge resulted from the precipitation of Fe(III) is a great concern. Here, molybdenum disulfide (MoS 2 ) was studied as a co-catalyst to improve the activation of peroxymonosulfate (PMS) by Fe(III) for sulfadiazine (SDZ) degradation and different characterization technologies were used to reveal the reactive species. The results showed that a strong synergy existed between MoS 2 and Fe(III); approximately 94.3% of the SDZ was removed by MoS 2 -Fe(III)-PMS after reaction for 30 min, while only 8.5% and 56.4% of the SDZ was removed by Fe(III)-PMS and MoS 2 -PMS, respectively. Both hydroxyl radicals and sulfate radicals were generated and the latter was the primary species. In addition to the radicals, singlet oxygen was found to be generated and contributed to the degradation of SDZ. The chemical probe reaction with methyl phenyl sulfoxide showed that the generation of high-valent iron-oxo species was not obvious by MoS 2 -Fe(III)-PMS under both acidic and neutral conditions. MoS 2 had good stability. No noticeable deactivation was observed during the 1st to 5th run and no obvious oxidation of surface Mo(IV) occurred. Based on the characterization of catalyst and oxidizing species, a mechanism for the activation of PMS by MoS 2 -Fe(III) was proposed. The results from this study are expected to clarify the reactive species and deepen the understanding of MoS 2 -promoted persulfate activation by Fe(II)/Fe(III).
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JOURNAL OF MOLECULAR LIQUIDS
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2021
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IF 6.165
Adeel Ahmed,Muhammad Usman,Bing Yu,Youqing Shen,Hailin Cong
Seeking an effective strategy to develop inexpensive and highly stable photocatalyst materials for dye degradation is of great significance to resolve the global environmental problems caused by dye abuse. Herein, we have reported the environmental-friendly synthesis of exceptionally efficient and highly sustainable hematite nanoparticles (α-Fe 2 O 3 NPs) using Punica granatum seed extract biomolecules. The morphology and phase purity of the synthesized α-Fe 2 O 3 NPs were executed through a series of characterization techniques. FESEM and TEM analysis exhibited that the synthesized α-Fe 2 O 3 NPs were irregular-shaped with an average size of 26.53 nm, while the BET surface area of nanoparticles was estimated to be 31.52 m 2 /g with an average pore diameter of 5.54 nm. α-Fe 2 O 3 NPs exhibited typical ferromagnetic behavior at room temperature. The oxidation states of elements in α-Fe 2 O 3 NPs were confirmed through X-ray photoelectron spectroscopy (XPS) analysis, while the charge on α-Fe 2 O 3 NPs was found to be −10.6 mV. The as-prepared α-Fe 2 O 3 NPs were utilized in solar-light driven photocatalytic degradation of anionic Congo red (CR) and Bromophenol blue (BPB) dye. Experimental results indicated the remarkable photocatalytic activity of α-Fe 2 O 3 NPs, and approximately 89.42% of CR and 87.96% of BPB was degraded in 240 min under sunlight irradiation at ambient conditions. The photocatalytic degradation experiments were also performed under different reaction conditions which followed the pseudo-first-order kinetics. The presence of reactive species generated in the reaction system liable for the CR and BPB degradation were corroborated through radical quenching experiments and further confirmed by EPR analysis. The excellent photocatalytic potential of α-Fe 2 O 3 NPs suggested that the synthesized nanoparticles could effectually be applied to remove organic dyes from the wastewater.
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Environmental Science-Water Research & Technology
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2021
·Vol. 7
·期 9
·1563-1575
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IF 4.251
Xuan-Yuan Pei,Hong-Yu Ren,De-Feng Xing,Guo-Jun Xie,Guang-Li Cao,Jia Meng,Nan-Qi Ren,Bing-Feng Liu
There is an urgent need for the development of efficient and economical persulfate activators in persulfate-based advanced oxidation processes for wastewater treatment. Accordingly, in this work, sewage sludge from a wastewater treatment plant was carbonized at different pyrolysis temperatures in the range of 400–800 °C via a one-pot synthesis method, which was used to activate peroxydisulfate (PDS) for the degradation of sulfamethoxazole (SMX). Among the samples, biochar pyrolyzed at 800 °C (BC800) showed the best catalytic performance for the removal of SMX (85.3% in 60 min reaction). In the initial pH range of 5.0–11.0, PDS could be activated (0.75 g L−1) efficiently by BC800 for the degradation of SMX. Combined with electron paramagnetic resonance (EPR) spectroscopy, quenching experiment, steady-state kinetics experiment and electrochemical results, the degradation of SMX in the BC800/PDS system was proposed to be a degradation mechanism involving electron transfer as the main pathway. Through the analysis of the intermediates, the possible SMX degradation pathways were predicted. This study provides new insights into the mechanism for the sewage sludge-derived biochar activation of peroxydisulfate and its potential applications for the treatment of SMX wastewater.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Ning Liu,Na Lu,HongTao Yu,Shuo Chen,Xie Quan
In recent years, the excellent performance of sulfate radical (SO 4 · − ) in advanced oxidation process has attracted more and more attention. However, it requires the consumption of expensive persulphate (PMS/PDS), and the resulting sulfate ion (SO 4 2− ) requires subsequent processing procedures, which limits its practical application value. In this work, a Z-scheme heterojunction g-C 3 N 4 /BiPO 4 (CNB x ) photocatalyst was constructed to in-situ activate the residual SO 4 2− , H 2 O and dissolved O 2 in organic wastewater simultaneously and produce SO 4 · − , ·OH and O 2 · − efficiently, so as to realize enhanced organic pollutant treatment by using clean and renewable solar energy resources. Under the condition of 10 mM SO 4 2− addition and 100 mW·cm −1 illumination, the degradation rate of BPA ( C 0 = 20 mg·L −1 ) by optimized CNB 150 catalyst was 0.30 min −1 , which was 50% higher than that without SO 4 2− (0.20 min −1 ). Detailed characterizations shown that a direct Z-scheme heterojunction was formed between g-C 3 N 4 and BiPO 4 , which could be simultaneously stimulated by light, and then effective charge separation and migration could be achieved through the internal electric field caused by the Fermi-level difference between the g-C 3 N 4 (-0.12 eV) and BiPO 4 (0.01 eV). In general, this study makes full use of renewable solar energy and provides a feasible path for promoting the simultaneous in-situ utilization of small molecules (SO 4 2− , H 2 O and O 2 ) that originally exist in water, which makes organic wastewater treatment more economic, eco-friendly and sustainable.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Yang Zong,Hua Zhang,Yufei Shao,Wenjie Ji,Yunqiao Zeng,Longqian Xu,Deli Wu
Periodate (PI)-based advanced oxidation processes have recently received increasing attentions. Herein, PI was readily activated by nano zero-valent iron (nZVI) and subsequently led to the enhanced oxidation of organic contaminants , with the removal performance of sulfadiazine (SDZ) in the nZVI/PI process even higher than that in the nZVI/peroxydisulfate process under identical conditions. Kinetic experiments indicated that the decay of SDZ was susceptible to the dosage of nZVI and PI, but was barely affected by pH values (4.0–7.0) under buffered conditions, suggesting the promising performance of the nZVI/PI process in a relatively wide pH range. Selective degradation of contaminants and 18 O-isotope labeling assays collectively demonstrated that iodate radical ( • IO 3 ), high-valent iron-oxo species (Fe(IV)) and hydroxyl radical ( • OH) were responsible for the abatement of organic contaminants . More importantly, due to the relatively weak steric hindrance effect of PI, PI easily adsorbed on the surface of nZVI and no iron leaching was detected throughout the reaction, implying that PI activation induced by nZVI was a surface-mediated process. Besides, PI was not transformed into harmful reactive iodine species. This study proposed an environmental-friendly approach for PI activation and shed new lights on the PI-based processes.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Yunjin Yao,Huanhuan Hu,Hongda Zheng,Hongwei Hu,Yinghao Tang,Xiaoyan Liu,Shaobin Wang
Bimetallic Fe- and Mo-embedded N-enriched porous biochar (Fe-Mo@N-BC) is developed and serves as a cost-effective and highly efficient catalyst for mineralization of non-biodegradation organic contaminants . Fe-Mo@N-BC was prepared by pyrolysis of complex Fe/Mo -containing precursors. Transmission electron microscopy and elemental mapping suggested that Fe and Mo are uniformly dispersed in nitrogen-doped biochar with hierarchical mesopores . In comparison to Fe@N-BC and Mo@N-BC, Fe-Mo@N-BC exhibited a superior activity for activating peroxymonosulfate (PMS). The stable activity was ascribed to N-doping and synergistic effect of Fe and Mo species, where both Fe-N x and Mo-N x can simultaneously serve as the active sites and N-BC can act as a carrier and an activator as well as an electron mediator. Electron paramagnetic resonance and quenching experiments indicated that H O • , O 2 • − and 1 O 2 were responsible for organic degradation . The effects of PMS dosage, initial Orange II concentration, temperature, solution pH, coexisting anions and humic acids on organic degradation were also investigated. With the assistance of an external magnet, Fe-Mo@N-BC can be easily separated after reaction and remains stable in the reusability tests. This work demonstrates a feasible strategy towards the fabrication of Fe, Mo-embedded N-enriched porous biochar catalysts for the detoxification of organic contaminants.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Jiayi Li,Zhaokun Xiong,Yahan Yu,Xinhao Wang,Hongyu Zhou,Bingkun Huang,Zelin Wu,Chunxiu Yu,Tingting Chen,Zhicheng Pan,Gang Yao,Bo Lai
In this study, the removal efficiency of carbamazepine (CBZ) was significantly improved in an electro-Fenton system without any extra oxidant (e.g., O 2 or H 2 O 2 ) in the presence of sodium molybdate (EF-Na 2 MoO 4 system). The slow release of iron ions of EF-Na 2 MoO 4 system greatly reduced the generation of iron sludge and effectively promoted the utilization of iron ions. The pseudo-first-order rate constants ( k obs ) for CBZ removal by EF-Na 2 MoO 4 process (0.0417 min −1 ) was much higher than those of sole electrolysis (0.0007 min −1 ) and EF-Na 2 SO 4 systems (0.0044 min −1 ). Meanwhile, the total iron concentration in EF-Na 2 MoO 4 process was 4.93 mg/L for 60 min, which was extremely lower than that of EF-Na 2 SO 4 process (271.22 mg/L). Besides, the primary reactive species was proposed to be superoxide radical (O 2 − ), while hydroxyl radical ( OH) and MoO 2 (O 2 ) 2 2− acted as the secondary reactive species. Our work elucidated the possible mechanism that the slow release of iron ions promotes pollutants degradation.
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ENVIRONMENTAL RESEARCH
·
2021
·
IF 6.498
Lingxiao Xue,Lijing Hao,Hui Ding,Rui Liu,Dan Zhao,Jianfeng Fu,Mengling Zhang
Glyphosate , a common broad-spectrum herbicide, is a serious environmental pollutant that causes a significant threat to humans. Hence, there is a pressing task to remove glyphosate from the environment. Here, we report an excellent Fe 3 Ce 1 O x catalyst synthesized via the one-step co-precipitation method for activating peroxymonosulfate (PMS) to degrade glyphosate at 25 °C. As a result, glyphosate is completely degraded with a high degradation rate of 400 mg L −1 ·h −1 , and the TOC and TN removals are 85.6% and 80.8%, respectively. As proven by systematic characterizations, the Fe–Ce synergistic effect plays a significant role in promoting PMS activation . The main reactive oxygen species for glyphosate oxidation are surface-bound SO 4 − · and ·OH, produced by activating PMS by electron transfer between Fe 2+ /Fe 3+ and Ce 3+ /Ce 4+ of Fe 3 Ce 1 O x . In light of the products determined, the possible degradation process of glyphosate is also speculated: C–N and C–P bonds of glyphosate molecules are attacked to form aminomethylphosphonic acid (AMPA) and orthophosphate (PO 4 3− ) by surface-bound SO 4 − · and ·OH that continuously mineralize and dephosphorylate AMPA to generate small molecules and inorganic ions, such as H 2 O and PO 4 3− . The results of this work suggest that Fe 3 Ce 1 O x /PMS could provide a potential candidate for efficiently removing organic compounds containing nitrogen or phosphorus from wastewater.
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Frontiers in Chemistry
·
2021
·
IF 5.221
Shi Jiaqi,Long Tao,Zhou Yuxuan,Wang Lei,Jiang Cuiping,Pan Dongguo,Zhu Xin
Quinones and quinone-containing organics have potential of activating persulfate to produce sulfate radical. In this work, the optimal condition for quinone activation of persulfate was investigated. It was found representative monoaromatics were degraded fastest in alkaline environment (pH 10.0), but excessive alkalinity restrained the reaction instead. The mechanisms to explain this phenomenon were speculated. The effect of initial quinone concentration on persulfate oxidation was also investigated at pH 10.0. In addition, a quantitative structure-activity relationship model was established with 15 kinds of monoaromatics, which revealed the most negative atomic net charges on carbon atom played an important role on degradation rates. Chemicals with a smaller qC- were easier oxidized in quinone-activate system. This finding helps further exploration of effective activator in alkaline environment.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Yezi Jin,Xianjie Feng,Anqi Yang,Zihui Jia,Yu Guo,Xiaoxia Li,Aihua Xu
The development of mixed metal oxides with excellent activity and stability for pollutants degradation via peroxymonosulfate (PMS) activation is highly desired in recent years. In this work, the brownmillerite-type oxide, Ca 2 Co 2 O 5 (CCO) with unique Ca 2 CoO 3 and CoO 2 layer structure and multiple oxidation states such as Co(II), Co(III) and Co(IV), was prepared and used to degrade organic pollutants with PMS as oxidant for the first time. It was found that CCO exhibited higher activity than other Co-based catalysts such as Co 2+ and Co 3 O 4 , and more than 93% of acid orange 7 (50 μM) was degraded after 7.5 min under mild reaction conditions. The catalysts were also stable during five successive runs. The easy oxidation of Co(II) species, the strong interactions among CCO, PMS and the pollutants, and the synergistic effect between Co and Ca were identified by several technologies and contributed to the high performance of the catalyst. Moreover, different from the conventional mechanism, radicals produced from low valent Co species oxidation by PMS, as well as the direct electron transfer process through the high valent Co species contributed the degradation reaction simultaneously. These findings provide an ideal bimetallic heterogeneous catalyst and a new mechanism for PMS-mediated reaction.
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