ENVIRONMENTAL POLLUTION
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2023
·
IF 8.9
Zhuoyue Wang,Ji Li,Wei Song,Jingxin Yang,Wenyi Dong,Xiaolei Zhang
Recently, it has been reported that chlorine dioxide (ClO 2 ) and (bi)sulfite/ClO 2 showed excellent performance in micropollutant removal from water; however, the degradation mechanisms and application boundaries of the two system have not been identified. In this study, bisphenol A (BPA) was chosen as the target contaminant to give multiple comparisons of ClO 2 and S(IV)/ClO 2 process regarding the degradation performance of contaminant, generation of reactive species, transformation of products and toxicity variation. Both ClO 2 and S(IV)/ClO 2 can degrade BPA within 3 min. The BPA degradation mechanism was mainly based on direct oxidation in ClO 2 process while it was attributed to radicals (especially SO 4 · - ) generation in S(IV)/ClO 2 process. Meanwhile, the effect of pH and coexisting substances (Cl − , Br − , HCO 3 − and HA) were evaluated. It was found that ClO 2 preferred the neutral and alkaline condition and S(IV)/ClO 2 preferred the acidic condition for BPA degradation. An unexpected speed-up of BPA degradation was observed in ClO 2 process in the presence of Br − , HCO 3 − and HA . In addition, the intermediate products in BPA degradation were identified. Three exclusive products were found in ClO 2 process, in which p-benzoquinone was considered to be the reason of the acute toxicity increase in ClO 2 process.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xi Chen,Yunfeng Chen,Songrong Li,Cheng Xue,Dongfang Liu,Wenli Huang
Phthalic acid esters (PAEs) pose serious health risks to humans and are difficult to remove by conventional sewage treatment processes. Herein, Fe 2 Mo 3 O 8 /MoO 2 /Mo 2 N composite (FMON) derived from bimetallic organic framework was used to activate peroxymonosulfate (PMS) for dibutyl phthalate (DBP) degradation. FMON exhibited an excellent catalytic effect with DBP removal efficiency of 92.4 % within 60 min. Mo 2 N showed a superior ability in promoting Fe 3+ /Fe 2+ redox cycle. The reduction efficiencies of Fe 3+ by Mo 2 N/MoO 2 composite and MoO 2 were 67 %–94 % and 11 %–23 %, respectively, in the homogeneous comparative experiment. Moreover, the ratio of Fe 2+ /Fe 3+ in FMON increased significantly after the catalytic reaction. Fe element doping also enhanced the reuse stability and reduced the metal ion leaching of the catalyst. The degradation of DBP was mediated by a variety of reactive species, of which SO 4 − , OH and O 2 − were dominant. Fe element, Mo element and O vacancies were confirmed to exert significant contributions as active sites in the catalytic process. Three degradation pathways of DBP were obtained by DFT calculation and HPLC-MS analysis. And the toxicity of DBP degradation products was significantly reduced based on the assessment result of Toxicity Estimation Software Tool (T.E.S.T.). This study explored a novel Fe/Mo bimetallic catalyst with friendly Fe 3+ /Fe 2+ cycling for environmental catalysis and provided new ideas for the treatment of PAEs wastewater.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Afang Wang,Yang Shi,Yang Liu,Wei Li,Heng Zhang,Xiaoqiang Dai,Li Luo,Gang Yao,Bo Lai
Traditional Fenton and Fenton-like processes are affected by the sluggish kinetics of Fe(II) regeneration and Fe(III) accumulation. This research revealed that the degradation efficiency of pollutants was significantly increased by adding Fe(III) to the Vis/PS system. A mechanism is proposed in which photosensitivity pollutants can boost Fe(III) to produce Fe(II) under visible light irradiation. Intriguingly, Fe(III) rapidly combines with LVF in aqueous environments to form Fe(III)-LVF complexes. This research confirms that Fe(III)-pollutant complexes are generated. The proportion of complexes are calculated using mathematical models. Furthermore, the production of Fe(IV) is verified in the Vis/PS/Fe(III) system, which also plays a vital role in boosting LVF degradation. Overall, this study provides comprehensive insights into the degradation mechanism of micropollutants, involving hydroxyl radical ( OH ∙ ), Fe(IV), and Fe(III)-LVF complexes, providing an efficient and green strategy for contaminant removal during wastewater treatment .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Chaoyi Zhou,Guojun Lv,Xuyang Zou,Jiangzhang Wang,Yan Chen,Jialing Shen,Shihao Su,Weilong Xing,Deling Fan,Yangbin Shen
Room-temperature ambient air is cheap and easy to obtain, hence the application of room-temperature ambient air as sole oxidant for pollutant degradation is extremely fascinating. In this work, core–shell coordination sponge-Fe 0 @Cu-Pd trimetal catalyst was synthesized via a simple step displacement plating process employing first displacement of Cu and the subsequent displacement of Pd, and applied as heterogeneous catalyst for synergistic catalytic degradation of composite pollutants including TC and PNP. The prepared s-Fe 0 @Cu-Pd trimetal sample was characterized with XRD, SEM, TEM, VSM and XPS. The characterization results revealed the obtained s-Fe 0 @Cu-Pd trimetal sample was a 20 ∼ 30 nm core–shell spherical morphology composed of Fe 0 aggregates core wrapped by a Cu-Pd shell layer. The obtained sponge-Fe 0 @Cu-Pd trimetal catalyst could efficiently activate room-temperature dissolved ambient oxygen and achieve the largest TC removal rate of 99.08 % and PNP removal rate of 97.16 % as well as the biggest removal rate constant of 8.76 min −1 for TC degradation and 7.55 min −1 for PNP degradation within 60 min at experimental conditions: [TC] = 30 mg/L, [PNP] = 30 mg/L, [Catalyst] = 25.52 g/L, pH = 3, 298 K ascribed to the strongest oxidation and reduction ability confirmed by CV characterizations, the lowest charge transfer and contact resistance affirmed by EIS measurements, the strongest O 2 activation ability verified by O 2 -TPD characterizations and DFT analyses, the largest external surface area and mesoporous volume validated by Nitrogen adsorption and desorption characterizations as well as the synergistic catalysis effect for wrapped Cu and Pd. Quenching experiments and EPR characterizations revealed that •OH, •O 2 − , 1 O 2 and •H are all the reactive species and meanwhile •O 2 − served as the main reactive oxygen species. Furthermore, possible mechanisms of TC and PNP degradation via sponge-Fe 0 @Cu-Pd trimetal catalyst were proposed.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Mingyi Liu,Hanchun Chen,Pengfei Xiao,Haodong Ji
Copper-manganese composite metal oxides (CuMnO y ) were prepared by hydrolysis-driven oxidation-reduction method and used to activate sulfite to degrade chlortetracycline hydrochloride (CTC) for the first time. The Jahn-Teller ions Mn 3+ and Cu 2+ exist in CuMnO y , which form a solid electric charge transport redox system and ensure the continuous generation of reactive oxygen species (ROS). Through the systematic study of the experimental parameters such as sulfite concentration, catalyst metal molar ratio, catalyst amounts and initial pH, the optimal degradation rate of CTC could reach 91.74% within 10 min and 94.46% after 30 min. The major reactive radicals were determined by radical quenching experiments and electron paramagnetic resonance (EPR) trapping techniques, and it was confirmed that SO 4 •- and •O 2 - played a nonnegligible role in the process of degrading CTC. Density functional theory (DFT) calculations show that higher Fukui indices ( f - and f 0 ) of CTC sites are more vulnerable to free radical attack. CuMnO y has low CTC degradation intermediate toxicity, high catalytic performance, good anti-interference ability, reusability and stability, and possesses decent application potential in the actual water treatment field.
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ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Longjie Liu,Zeyang Lu,Wanling Cai,Gary Owens,Zuliang Chen
Reduced graphene oxide/iron nanoparticles (rGO/FeNPs) synthesized by the chemical method have been used in Fenton oxidation of organic contaminants , yet little is known about biosynthesized rGO/FeNPs using green tea extract (GT) as how to activate persulfate in sulfate radical-based advanced oxidation processes . In this study, rGO/FeNPs were used to activate peroxydisulfate (PDS) for 17β-estradiol (βE 2 ) and estriol (E 3 ) removal. The rGO/FeNPs-PDS system removed 83.6% of βE 2 and 62.5% of E 3 within 240 min, which was confirmed by a combination of adsorption and degradation via both radical and non-radical pathways. Four main reactive species in βE 2 and E 3 degradation were observed, i.e., hydroxyl radical (·OH), sulfate radical (SO 4 ·− ), singlet oxygen ( 1 O 2 ) and electron transfer , with the respective contributions of ·OH (32.9 and 34.7%), SO 4 ·− (16.1 and 19.7%), 1 O 2 (12.2 and 14.1%) and electron transfer (8.0 and 7.2%). Analysis of X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FTIR), Electron Paramagnetic Resonance (EPR) and electrochemical measurements all indicated that beside the well-known role of Fe, C O from rGO through the generation of ·OH, SO 4 ·− , 1 O 2 and electron transfer, as well as GT through electron transfer also participated in the activation of PDS. Finally, the degradation pathways of βE 2 /E 3 were proposed. Overall, this study provides a new insight into the biosynthesis of rGO/FeNPs to activate PDS for the oxidation of mixed emerging contaminants .
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FUEL
·
2023
·
IF 7.4
Yanqing Shi,Cai Guo,Huajing Zhou,Liang He,Shaoyun Shan,Tianding Hu
Rational modulation of the local electron density of Cu active site is the key to improve the efficient transfer hydrogenation (CTH) of furfural (FF) on the surface of catalysts with low Cu-loadings. In this paper, a CuMgAl/LSC catalyst with lower Cu content (<3.5 % wt ) was prepared by using porous biochar as a carrier and exploiting the local dispersion and electron-modulation effects of structural elements of hydrotalcite laminates. CTH experiments showed that the conversion of FF and the selectivity of FA could reach more than 99.0 % in isopropanol solution at 170 °C and within 1 h. Catalyst characterization and density functional theory (DFT) calculations demonstrated that the Cu(I) species was the main active site during the CTH process of FF. Doping laminate metals (i.e., Mg, Al) can not only form electron-rich centers by local electron modulation of the active site through the coordination structure of Cu-O-M, lowering its D-band center and achieving higher catalytic activity; Due to the Jahn-Teller effect, the local spatial misalignment of Cu sites formed, which can reduce the risk of over-hydrogenation and improve the FA selectivity. In addition, it can be also found that the Coulomb tractive force of reactive intermediates can lead to the crystal surface reconstruction and structure deterioration of Cu species. The new discovery of the deactivation mechanism can provide a reference for the future design of copper-based catalysts in CTH process of FF.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Xuefeng Zhang,Xiaowen Kang,Junyou Wu,Qin Yang,Yuejie Zhang,Jiahao He,Chao Zheng,Yingchun Yang,Zhixiang Ye
High energy consumption is the bottleneck in advanced oxidation processes (AOPs) for applying in eliminating refractory organic contaminants . Fenton catalysis is deemed to be the promising technology of AOPs to produce super-active hydroxyl radical ( ·OH) for tackling serious water environment pollution issues. Here, magnetic mesoporous sulfur-doped ferric oxide (PS-Fe) composite, prepared through simple co-precipitation method, was creatively introduced to activate hydrogen peroxide (H 2 O 2 ) to generate ·OH for degrading emerging antibiotic moxifloxacin (MOX). The catalytic activity of PS-Fe was significantly elevated by sulfurization to achieve a degradation efficiency of 97 % and total organic carbon removal exceeding 44 % (within 30 min). Besides, we investigated the effects of catalyst dosage and H 2 O 2 concentration, initial pH value, temperature, and humic acid concentration on MOX degradation. Quenching experiments results indicate that ·OH, O 2 · – , and 1 O 2 participated in the degradation process of MOX, and ·OH plays the predominant role. Additionally, possible activation mechanism is proposed and possible reaction intermediates are speculated. This work can offer a novel and reasonable interpretation for designing heterogeneous iron-based materials in activating H 2 O 2 to degrade pollutants.
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Catalysts
·
2023
·Vol. 13
·期 3
·469
·
IF 3.9
Hongzhong Zhang,Zhaoya Fan,Qingqing Chai,Jun Li
In this work, a Z-scheme Bi2WO6/BiO2−xheterojunction was successfully prepared using a self-assembly strategy. Various characterization techniques demonstrated that the formation of the heterojunction not only accelerated the separation of photoinduced carriers but also weakened the recombination rate of photogenerated electron–hole pairs-. The Bi2WO6/BiO2−xcomposites had a wider absorption edge than Bi2WO6in the range of 200–800 nm, which improved the photocatalytic performance of ciprofloxacin (CIP) degradation under xenon lamps. As a result, the Z-scheme heterojunction Bi2WO6/BiO2−xcomposite exhibited excellent photocatalytic activity. Catalyzed by the optimal 20% Bi2WO6/BiO2−x(0.5 g/L), the removal rate of CIP (10.0 mg/L) was 91.8% within 2 h irradiated by visible light, which was 2.37 times that of the BiO2−xcatalyst. This work will provide a fresh perspective on the construction of visible-driven Z-scheme photocatalysts for wastewater treatment.Keywords:photocatalysis;ciprofloxacin;Bi2WO6;BiO2−x;Z-scheme heterostructure
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Catalysts
·
2023
·Vol. 13
·期 4
·715
·
IF 3.9
Dongrui Hou,Jing Luo,Qinggong Sun,Mengyang Zhang,Jianfeng Wang
In this study, Co-modified alkalinized g-C3N4(named Co-CNK-OH) was prepared for the Fenton-like photocatalytic degradation of tetracycline (TC) via a simple yet effective calcination–impregnation method. In all samples of CNK-OH with different Co2+loadings, Co-CNK-OH catalyst with the optimal content (9%) exhibited the highest catalytic activity, with 87.1% tetracycline removal and 50% removal efficiency of the total organic carbon (TOC). Mechanism studies revealed that the 9%Co-CNK-OH catalyst had the lower electrical resistance after alkalization treatment and Co2+modification, leading to a significantly accelerated interfacial charge transfer to the electron acceptor as well as effectively separating electrons and holes. The intermediates generated during the TC degradation in the photo-Fenton process were detected by HPLC-MS, which proved that the holes, superoxide radicals, and singlet oxygen are the key reactive species in the Fenton-like photocatalysis. This study provides a new option for the treatment of TC in wastewater.Keywords:Fenton-like photocatalysis;Co-CNK-OH;tetracycline;reactive oxygen species
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Ke Du,Zhizheng Sheng,He Li,Lou Gao,Tianlan Yan,Jiayu Yu,Di Pan,Zhichao Tan,Songhai Xie,Jing Ju,Yahong Zhang,Yi Tang
Constructing zeolite catalysts with excellent mass transfer and active site accessibility is the key to improving their catalytic efficiencies. Herein, a zeolite subcrystal catalyst with high short-range ordering but X-ray amorphism is prepared to minimize the existing molecular mass-transfer barrier of conventional zeolite catalysts. Various characterizations confirm its size of smaller than 10 nm, definite MFI framework, complete opened micropore channel, and abundant accessible acid sites. Moreover, physical and chemisorption results reveal that the high short-range ordering MFI zeolite subcrystal possesses negligible intracrystalline diffuse limitation and utmost accessibility for the active site. As anticipated, the zeolite subcrystal catalyst not only demonstrates high cracking efficiency in polyolefin cracking reactions but also exhibits outstanding catalytic activity and resistance to carbon deposition in macromolecular furfuryl alcohol etherification reaction. The controlled MFI zeolite subcrystal catalyst synthesis strategy is expected to extend to a variety of microporous materials.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Shuang Liu,Hong Wu,Huaili Zheng,Weizhen Zhang,Wei Ding,Hong Li,Chao Liu
Sulfite (S(IV))-based advanced oxidation process has attracted widespread attention due to the generation of strongly oxidizing sulfate radicals (SO 4 •− ) and hydroxyl radicals (HO • ) for contaminants remediation. However, the contaminant degradation by singlet oxygen ( 1 O 2 ) through a nonradical pathway was still unclear in the S(IV) activation system. Herein, a magnetic Fe 3 O 4 /g-C 3 N 4 (MCN) composite was synthesized for the utilization as a visible-light catalyst to activate S(IV) under visible-LED (Vis-LED) for the organic degradation . The incorporation of Fe 3 O 4 in g-C 3 N 4 up-regulated the photocatalytic performance in the S(IV) activation for X-3B degradation, and > 98% of X-3B (20 mg L −1 ) was degraded with the degradation rate constant ( k obs ) of 0.110 min −1 within 30 min. The SO 4 •− and 1 O 2 produced in the MCN/S(IV)/Vis-LED system were identified as the primary reactive species through the quenching experiments and electron spin resonance. Interestingly, the light-induced generation of superoxide radical (O 2 •− ) played a negligible role in the formation of 1 O 2 , and most of 1 O 2 was corroborated to be originated from SO 4 •− besides SO 5 •− , which was rarely reported in other S(IV) activation processes. The catalysts before and after utilization were characterized to further elucidate the mechanisms for the S(IV) activation. There were two possible pathways for the S(IV) activation: the electron transfer from S(IV) to the photo-generated holes and the ligand-to-metal charge-transfer (LMCT) within the surface Fe(III)−S(IV) complexes. Furthermore, the MCN/S(IV)/Vis-LED system was of high resistance to complex water matrixes (pH, inorganic anions, etc.), demonstrating its application perspective in the purification of wastewater containing organic pollutants .
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