APPLIED SURFACE SCIENCE
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2022
·
IF 7.392
Chong Jia,Ying Wu,Lijie Xu,Shuguang Han,Lu Gan
Herein, binary composite catalysts based on MnO 2 and CoFe 2 O 4 were prepared to degrade bisphenol A (BPA) and dimethyl phthalate (DMP) by coupling with peroxymonosulfate (PMS), in which CoFe 2 O 4 was located either at the outer (MnO 2 @CoFe 2 O 4 ) or at the inner (CoFe 2 O 4 @MnO 2 ) positioning. The catalysts possessed higher degradation efficiency than both pristine CoFe 2 O 4 and MnO 2 , in which MnO 2 @CoFe 2 O 4 provided the highest PMS activation capability. The positioning of each component influenced significantly the variety and intensity of the generated reactive oxidative species, in which MnO 2 @CoFe 2 O 4 generated more hydroxyl radical ( OH) whereas CoFe 2 O 4 @MnO 2 generated more non-radical singlet oxygen ( 1 O 2 ). Therefore, MnO 2 @CoFe 2 O 4 could degrade both BPA and DMP with high degradation rate, while CoFe 2 O 4 @MnO 2 only exhibited promising degradation efficiency towards BPA since DMP was inert to 1 O 2 . Comparatively, CoFe 2 O 4 @MnO 2 had better catalytic stability and water matrix adaptability than MnO 2 @CoFe 2 O 4 when degrading BPA, since OH was vulnerable water with complicated compositions. This study provides a new insight for the design and selection of composite catalyst towards the degradation of organic pollutants with discrepant structures and properties.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Da Wang,Shiwen Dong,Siqi Fu,Yi Shen,Tao Zeng,Weiti Yu,Xiaohui Lu,Lizhang Wang,Shuang Song,Jun Ma
It is a feasible strategy to prepare reliable biochar catalysts for heterogeneous catalytic ozonation (HCO) processes by using inexpensive, high quality, and easily available raw materials. Here, an environmentally friendly, simple, and green biochar catalyst rich in nitrogen (N) and sulfur (S) has been prepared by the pyrolysis of kelp. Compared with directly carbonized kelp biomass (KB), acid-activated KB (KBA) and base-activated KB (KBB) have higher specific surface areas and more extensive porous structures, although only KBB displays effective ozone activation. Imazapic (IMZC), a refractory organic herbicide, was chosen as the target pollutant, which has apparently not hitherto been investigated in the HCO process. Second-order rate constants ( k ) for the reactions of IMZC with three different reactive oxygen species (ROS), specifically k O3, IMZC , k OH, IMZC , and k 1O2, IMZC , have been determined as 0.974, 2.48 × 10 9 , and 6.23 × 10 5 M −1 s −1 , respectively. The amounts of graphitic N and thiophene S derived from the intrinsic N and S showed good correlations with the IMZC degradation rate, implicating them as the main active sites. OH and O 2 − and 1 O 2 were identified as main ROS in heterogeneous catalytic ozonation system for IMZC degradation. This study exemplified the utilization of endogenous N and S in biological carbon, and provided more options for the application of advanced oxidation processes and the development of marine resources.
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高影响因子
Polymers
·
2022
·Vol. 14
·期 23
·5135
·
IF 4.967
Xu Han,Yun Tao,Chao Xu,Yicong Deng,Zisen Meng,Zhenhao Dou,Peng Wang,Quan Feng
Hemin possesses great potential in eliminating organic pollutants due to its mild reaction condition, light-harvesting efficiency, and environmental friendliness. However, it has drawbacks such as being easy to aggregate and hard to recycle, and poor stability should be improved in practical application. Herein, the subject developed an electrospinning approach to enable the hemin particulates to be immobilized onto polyacrylonitrile (PAN) nanofibers stably. Hydrogen peroxide (H2O2) was adopted as an oxidant in the system to simulate the enzymatic catalysis of hemin in an organism. Scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), UV-Vis diffuse reflection spectroscopy (DRS), and electron spin resonance spectroscopy (ESR) analysis was employed to discuss the morphology, structure, and mechanism of the prepared n-hemin/PAN nanocomposite membranes, and 0.02 mmol L−1of the rhodamine B (RhB) removal activity in different conditions was also verified with these membranes. The kinetic studies showed that n-hemin/PAN nanocomposite membranes maintained excellent properties both in adsorption and degradation. Around 42% RhB could be adsorbed in the dark, while 91% RhB decolorized under xenon lamp irradiation in 110 min, suggesting the catalytic performance of n-hemin/PAN was greatly driven by light irradiation. Differing from the axial coordinated hemin complexes, n-hemin/PAN would catalyze hydrogen peroxide into •OH radicals rather than •OOH and high-valent metal-oxo species. This work provides an effective way to support hemin as nanocomposite membranes, in which the molecular interaction between polymer and hemin made their light adsorption an obvious red shift.Keywords:polyacrylonitrile;hemin;photocatalysis;enzyme-like catalysis;electrospinning
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CHEMOSPHERE
·
2022
·
IF 8.943
Mengxue Wang,Yuge Wang,Jiahao Sun,Jianzheng Zhen,Weiyang Lv
Iron-based layered double hydroxides (LDHs) have drawn tremendous attention as a promising peroxymonosulfate (PMS) activators, but they still suffer from low efficiencies limited by electrostatic agglomeration and low electronic conductivity. Herein, a MgFeAl layered double hydroxide/carbonitride (LDH/CN) heterostructure was constructed via triggering the interlayer reaction of citric acid (CA) and urea. CA as a structure-directing agent regulated the interlayer anion of MgFeAl-LDH, which enabled an interfacial tuning in the process of coupling with CN. The obtained LDH/CN heterostructure, as an efficient PMS activator, achieved nearly 100% bisphenol A (BPA) removal rate in 10 min with high specific activity (0.146 L min −1 ·m −2 ). Electron paramagnetic resonance (EPR) tests, quenching experiments, electrochemical characterization and X-ray photoelectrons spectroscopy (XPS) tests were applied to clarify the mechanism of BPA degradation. The results unraveled that the activity of the catalyst originated from the heterostructure of LDH and CN with an efficient interfacial electron transfer , which promoted the fast generation of O 2 •- for rapid pollutant degradation . In addition, the catalyst exhibited excellent applicability in realistic wastewater. This work offered a rational strategy for forming a heterostructure catalyst with a fine interface engineering in actual environmental cleanup .
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Gen Wang,Ke Wang,Zhuoyue Liu,Youyou Feng,Shengjiong Yang,Yaqiong Su,Xufang Qian,Pengkang Jin,Jing Wei
Nonradical activation of peroxydisulfate (PDS) is promising for wastewater decontamination but suffers from insufficient decomposition efficiency toward organics. Herein, NiO nanospheres with hollow multi-shelled structure (HoMS) and tunable shell numbers are designed as a nanoreactor of PDS activation to enhance the decomposition efficiency. Study on bis-phenol A (BPA) degradation reveals that 3-shelled NiO HoMS exhibits enhanced kinetic rate (0.08 min 1 ) and mineralization degree (79.2%) compared to 2-shelled NiO HoMS (0.04 min −1 , 50%) and NiO nanoparticles (0.01 min −1 , 29.8%). The degradation of BPA over NiO HoMS follows electron transfer regime with oxygen vacancy ( V O ) acted as the active site. The hollow multi-shelled structure not only increases the accessibility of V O but also enriches local concentration of reactants in the void spaces due to the nanoconfinement effect, and thus mainly contributes to the enhanced catalytic efficiency. This work provides a distinct case for developing efficient nonradical oxidation technique for water purification .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Ming Liu,Mei Lin,Pan Wu,Gary Owens,Zuliang Chen
A green tea extract was used as a natural reducing agent to prepare three different manganese oxides (Mn 3 O 4 , Mn 2 O 3 and MnO) which after carbonization in different atmospheres, were evaluated for their ability to degrade estriol (E3). Catalytic ability of the three manganese oxides varied in the order Mn 2 O 3 > Mn 3 O 4 > MnO; corresponding to E3 degradation efficiencies of 100, 100 and 92.5 % after 180 min. After calcination, no new functional groups were observed on the surface of three manganese oxides, except the corresponding spectra. The morphology of the manganese oxides was primarily olive-shaped, with numerous small cubic particles stacked at the nanoscale, with a uniform distribution of elements. Free radicals and Mn ion leaching was observed from the prepared manganese oxides where leaching of manganese ions was related to the intensity of singlet oxygen. Advanced material characterization showed while green synthesis resulted in materials being doped with a small amounts of elements such as C and S, the broad crystal structure of the three materials was still the main factor affecting the removal efficiency of E3; with Mn(III) playing a major role in the catalytic peroxydisulfate (PDS) process.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Lijun Gao,Dongmei Han,Zhihua Wang,Fubo Gu
Tubular carbon-covered cobalt-doped bi-crystalline phase In 2 O 3 (denoted as CoInO-x) was synthesized by one-step calcination of the metal-organic framework cobalt-doped MIL-68(In)-NH 2 precursor. The photocatalytic activity of CoInO-x was investigated using tetracycline hydrochloride (TCH) degradation. The removal of TCH by CoInO-500 obtained by calcination at 500 °C under visible light irradiation was 90.1% after 70 min, which was significantly higher than that of In 2 O 3 . The reaction rate constant of CoInO-500 was 11.02 times higher than that of In 2 O 3 and could maintain a better photocatalytic performance after four cycles. The effects of photocatalyst dosing, pH, and inorganic anions on photocatalytic degradation were studied. The mechanism of photocatalytic degradation was analyzed in detail by reactive radical trapping experiments, Mott-Schottky measurements, and electron paramagnetic resonance (EPR) signal characterization. Enhanced photocatalytic performance is mostly attributed to the cobalt doping creating impurity energy levels and narrowing the forbidden bandwidth of In 2 O 3 , enhancing the visible light utilization and the photogenerated charge separation efficiency. Carbon covering can serve as a bridge for charge transport, accelerating the rapid transport of photogenerated charges.
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Nanomaterials
·
2023
·Vol. 13
·期 1
·216
·
IF 5.3
Wenxi Wang,Junjie Zhang,Zhiran Hou,Pei Chen,Xu Zhou,Wei Wang,Fatang Tan,Xinyun Wang,Xueliang Qiao
Carbon nanotubes (CNTs) were considered a promising activator for persulfates due to their high electrical conductivity, large specific surface area and low toxicity. The functional groups and surface defects of CNTs could significantly affect their activation performance. In this study, CNTs with high C=O ratio and defect density (CNT-O-H) were prepared through a facile treatment of raw CNTs with HNO3oxidation followed by calcination at 800 °C under an argon atmosphere. X-ray photoelectron spectroscopy (XPS) and Raman results showed that the C=O proportion and defect degree (ID/IG) rose to 75% and 1.53, respectively. The obtained CNT-O-H possessed a superior performance towards peroxydisulfate (PDS) activation, and the degradation efficiency of tetracycline (TC) in the CNT-O-H/PDS system was increased to 75.2% from 56.2% of the raw CNTs/PDS system within 40 min. Moreover, the activity of CNT-O-H after use could be easily recovered with re-calcination. In addition, the CNT-O-H/PDS system exhibited high adaptabilities towards wide solution pH (2–10), common coexisting substances and diverse organic pollutants. Singlet oxygen (1O2) was confirmed to be the dominant reactive oxygen species (ROS) generated in the CNT-O-H/PDS system. It was inferred that surface C=O groups and defects of CNTs were the key site to activate PDS for TC degradation.Keywords:carbon nanotube;carbonyl group;surface defect;peroxydisulfate activation;singlet oxygen;tetracycline degradation
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Materials Research Express
·
2022
·Vol. 9
·期 12
·126101
·
IF 2.025
Jing Wang,Li Ma,Zhengwei Pan,Tingyun Li
A high-efficient and stable catalyst is highly desired to catalyze ozone for refractory organic pollutants removal. In this work, Mn-Ce bimetallic oxide loaded CNT@Fe3C (Mn0.7Ce0.3Ox/CNT@Fe3C) was synthesized with Mn0.7Ce0.3Ox as the active component and magnetic CNT@Fe3C as the support. The catalytic performance of Mn0.7Ce0.3Ox/CNT@Fe3C towards catalytic ozonation was evaluated. The TOC removal efficiency of phenol degradation after 45 min of reaction was 98%, which was 1.5 times and 1.8 times that of monometallic CeO2/CNT@Fe3C (65%) and MnxOy/CNT@Fe3C (54%), respectively. The synthesized-Mn0.7Ce0.3Ox/CNT@Fe3C possessed good reusability during five successive cycles and remained efficient over a wide range of pH 4.2–8.3. The results of EPR measurements and quenching experiments demonstrated that hydroxyl radicals (·OH) were the dominant reactive oxidation species (ROS) for phenol mineralization in the Mn0.7Ce0.3Ox/CNT@Fe3C/O3 system. Moreover, the magnetic Mn0.7Ce0.3Ox/CNT@Fe3C is easily recovered and reused.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Zhiran Hou,Wei Wang,Ningning Dong,Pei Chen,Lifa Ge,Fatang Tan,Xinyun Wang,Xueliang Qiao,Po Keung Wong
In this study, a dual-oxidant advanced oxidation process (AOP) system containing calcium peroxide (CaO 2 ) and peroxymonosulfate (PMS) was developed for the first time to efficiently degrade refractory organic pollutants . It was found that the system with 0.1 g/L CaO 2 and 0.3 g/L PMS could degrade more than 91% of 50 mg/L tetracycline (TC) within 4 min at room temperature, and the degradation process much followed the pseudo second-order kinetic model. The presented AOP system exhibited strong anti-interference capabilities towards coexisting inorganic anions (Cl − , SO 4 2– , NO 3 – , HCO 3 – and HPO 4 2– ) and humic acid (HA), even at high concentrations. Moreover, the system could efficiently work in a wide pH (3−12) range, suitable for natural waterbodies and various organic pollutants. The results of quenching experiments and electron paramagnetic resonance (EPR) tests demonstrated that singlet oxygen ( 1 O 2 ) was the dominate reactive oxygen species (ROS) responsible for organics degradation. A synergistic mechanism of the dual-oxidant system was confirmed by a series of comparative experiments, where CaO 2 continuously provided OH − and H 2 O 2 , and then combined with PMS to produce predominant 1 O 2 and inferior O 2 •– , respectively. Further, the possible pathways of TC degradation were deduced based on analyses of the intermediates.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Tianyao Shen,Xiaojing Wang,Jiaqin Li,Chunyan Yang,Peng Xu,Hua Chai,Peng Wang,Guangshan Zhang
Dielectric barrier discharge plasma (DBDP) has attracted much attention because of its energy saving, high efficiency, and simultaneous production of various active substances. In this work, a three-dimensional (3D) ZnFe-layered double hydroxides (LDH)/nickel foam (NiF) was rationally engineered and synthesized to overcome the problem of active substances insufficient use and clogged pipes in DBDP. With the assistance of ZnFe-LDH/NiF, the removal efficiency of diuron (DUR) increased from 85.98 % to 96.52 %, and the energy efficiency increased from 1074 mg·kWh −1 to 1281 mg·kWh −1 . In various circumstances, the DBDP + ZnFe-LDH/NiF process performed a strong anti-interference ability, high stability, and reusability. The improvement of catalytic degradation ability could be attributed to the combined action of the Fenton-like process and O 3 catalysis, all three elements participating in the electron transfer. With the help of quenching experiments, reactive oxygen species (ROS, including OH, 1 O 2 , and O 2 − ) were identified as the dominant active substance, significantly contributing to DUR elimination. Density functional theory calculation (DFT) and quadrupole-time of flight-liquid chromatography/mass spectrometry (Q-TOF-LC/MS) reached the same conclusion that C N and C−Cl were the main sites attacked by electrophiles and radicals. In summary, the combination of DBDP and ZnFe-LDH/NiF sheds new light on catalyst design and DBDP application.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 47
·期 4
·1935-1944
·
IF 3.925
Hancheng Tan,Xiaolan Zhou,Haiyan Zhu,Wenxiu Gu
A micro/nano hierarchical flower-like ZnS/FeS2 direct Z-scheme heterojunction visible-light catalyst was in situ derived from a Prussian blue analogue cube (Zn–Fe PBA) using a facile one-pot hydrothermal sulfidation strategy. The as-prepared ZnS/FeS2 catalyst shows extraordinarily boosted visible-light photocatalytic degradability for Rhodamine B (RhB) with the synergism of peroxydisulfate (PDS). Under visible-light illumination, 98.5% degradation efficiency can be achieved within 15 min and 100% within 20 min with excellent structural stability of ZnS/FeS2. The degradation kinetic constant of ZnS/FeS2 + PDS is 9.33 times that of ZnS/FeS2, 23.02 times that of p-ZnS/FeS2, 24.05 times that of FeS2, and 28.25 times that of ZnS, respectively. The ZnS/FeS2 heterojunction shows significant synergistic benefits in the photocatalytic degradation reaction. More advantageously, ZnS/FeS2 + PDS shows excellent photocatalytic degradation performance in a wide pH range (1–10). A reasonable direct Z-scheme heterojunction mechanism for visible-light responsive photocatalytic degradation of RhB with ˙OH, h+, ˙O2−, and ˙SO4− as the crucial active species is recommended for the ZnS/FeS2 + PDS composite system. The micro/nano hierarchical flower-like structure of ZnS/FeS2 simultaneously combines the high activity of nano-materials with the advantages of easy recycling of micro-sized materials. The in situ transformation characteristics of ZnS/FeS2 from the PBA template contribute to the advantageous high performance and structural stability.
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