Journal of Environmental Chemical Engineering
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2020
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IF 4.3
Yali Song,Shanshan Gao,Jiayu Tian,Hongzhong Zhang
To ensure efficient removal of SIX, Ag/g-C 3 N 4 with uniform-sized Ag nanoparticles was synthesized. With the employment of poly vinylpyrrolidone in synthesis process, Ag sizes were controlled and the photoabsorption ability of Ag/g-C 3 N 4 for visible-light was improved. In comparison with g-C 3 N 4, the degradation kinetic constant of SIX was increased by 1.75 times when Ag content was optimized (5 wt.% in this work, i.e. Ag/g-C 3 N 4 -5). The primary species for SIX degradation by Ag/g-C 3 N 4 -5 were holes and ·O 2 − in the presence of visible radiation. Besides, the intermediate products generated in reaction processes were identified and the transformed pathways were proposed in photocatalytic process of SIX by Ag/g-C 3 N 4 -5, including the rupture of the chemical bond between S and benzene ring, the rupture of S N bond, the hydroxylation and nitration of benzene ring. Finally, the photocatalytic degradation of SIX in two authentic water bodies revealed the efficient removal of SIX can still be realized by Ag/g-C 3 N 4 -5.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Kun Wu,Meng Wang,Angzhen Li,Zixuan Zhao,Ting Liu,Xiaodan Hao,Shengjiong Yang,Pengkang Jin
Mn-oxide-containing adsorbents have shown outstanding performances for the removal of As(III) through an “oxidation-adsorption” process. In this study, a new adsorbent of Fe-Mn-Cu ternary oxide (FMCTO) was fabricated to improve the redox reaction rate and to enhance the recovery of oxidative ability. FMCTO exhibited a stronger ability for As(III) removal than most of other adsorbents, because it has better oxidative capability for As(III) oxidation. The state of dynamic equilibrium for As(III) removal by FMCTO could be basically achieved within 3 h, and the As removal efficiency reached 98.9% at time = 24 h. The Langmuir As adsorption capacity of FMCTO was determined to be 204.8 mg/g. The As(III) removal efficiency of FMCTO was further boosted by 7% through oxygen gas aeration and decreased by 19% with nitrogen gas in the ambient during the first 3 h, indicating the positive effect of oxygen on As(III) oxidation. EPR and UV spectra methods were used to confirm the generation of superoxide radical (O 2 − ) and the enhanced production of Mn(III) soluble species on FMCTO surfaces, thus achieving a better As(III) oxidation performance. The XPS analysis results showed that the electron transfer from Cu(I) to Mn(IV) could improve the stability of Mn(III) within FMCTO. Meanwhile, Mn(II) ions could be oxidized to Mn(III) by O 2 − . Hence, the formation of a redox cycle between Mn(II) and Mn(III) along with the production of O 2 − plays a vital role in the upgraded As(III) removal mechanisms. This study provides new insights into the promotion of the capability of Mn-containing adsorbents for achieving the improved removal of As from As(III)-contaminated water.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2020
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IF 6.551
Yong Liu,Yang Zhao,Jianlong Wang
In this study, a novel Cu 0 -Cu 2 O@CNTs composite was synthesized, characterized and applied to activate peroxydisulfate (PDS) for the degradation of 2, 4-dichlorophenol (2,4-DCP) in contaminated lake water. The results indicated that Cu 0 -Cu 2 O@CNTs can effectively activate PDS to produce O 2 • − radical, which has high selectivity to degrade organic pollutants in actual contaminated water. The efficiency of 2,4-DCP degradation and mineralization was 99.27% and 66.90%, respectively under the optimal condition. In the presence of Cl − , HCO 3 − and natural organic matters (NOMs) or in real wastewater containing 2,4-DCP, Cu 0 -Cu 2 O@CNTs/PDS system had a good selectivity for 2,4-DCP degradation. O 2 • − was the dominant reactive species in Cu 0 -Cu 2 O@CNTs/PDS system for 2,4-DCP degradation. The possible degradation pathway of 2,4-DCP was proposed. It was concluded that Cu 0 -Cu 2 O@CNTs composite could overcome the shortcomings of PDS activation by Cu 0 and Cu 2 O alone, such as low activating capability of Cu 0 and instability of Cu 2 O, which was high efficient for activating PDS. Cu 0 -Cu 2 O@CNTs composite can be used as an efficient catalyst to activate PDS for the degradation of toxic organic pollutants in water and wastewater.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Yingjie Gao,Qi Zhao,Yunhe Li,Yuanqing Li,Jianfeng Gou,Xiuwen Cheng
Advanced Oxidation Processes (AOPs) play a critical role in the elimination of antibiotics, in which it is essential to explore an environmentally friendly, cheap and effective catalyst. In this study, Ag 2 O-g/eggshell catalyst had been synthesized in a simple strategy, combining with peroxymonosulfate (PMS) to simultaneous remove sulfamethoxazole (SMX). Then, physicochemical properties of catalyst were investigated by series of techniques. Results indicated the Ag species was featured with a spherical-like structure and homogeneously distributed on the surface of eggshell. In addition, Ag 2 O-Ag/eggshell exhibited high degradation efficiency of SMX by activation of PMS (94.6%) under the optimized conditions of 0.1 g•L −1 Ag 2 O-Ag/eggshell, 0.16 mM PMS, 10 mg•L −1 SMX and initial pH 6.42. Moreover, several parameters such as the dosage of catalyst, PMS and the effect of pH, co-existing anions, humic acid (HA) and water matrices on SMX degradation were systematically studied. Besides, scavenging experiments were conducted to distinguish the active radicals. Furthermore, to improve the reusability of powder Ag 2 O-Ag/eggshell, corresponding Microporous Filter Membrane had been synthesized. Subsequently, possible reaction mechanism was proposed. Consequently, these results revealed that the waste eggshell was considered as a promising supporting material for the metal catalyst for the catalytic degradation of antibiotics in water.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2020
·Vol. 30
·期 42
·2004108
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IF 16.836
Jingyu Sun,Jinghong Wen,Guizhu Wu,Ze Zhang,Xue Chen,Guichang Wang,Mingyang Liu
Due to the unique surface atomic arrangement, exposed facets and defects of nanomaterials play critical roles in their physicochemical properties. Herein, BiOI nanosheets with the same type of defects on different exposed facets such as {001} (BI-001) and {110} (BI-110) are engineered to harmonize the electronic structures for antibacterial applications. Results demonstrate that BI-110 exhibits higher activity in killing Escherichia coli under 808 nm light irradiation than that of BI-001 due to its superior electronic structures. The density functional theory calculations show that BI-110 with its excellent geometric effect exhibits stronger adsorption to O 2, leading to the formation of highly concentrated single oxygen species, which causes excellent antibacterial performance. This work with the combination of facets engineering and vacancy engineering will inspire future studies on antibacterial photodynamic therapy.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
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IF 7.489
Zhuoqian Li,Kai Li,Shuanglong Ma,Bingjun Dang,Yi Li,Haichao Fu,Jinge Du,Qingxiang Meng
A convenient and efficient method to fabricate isolated Fe single-atom catalysts deposited on Myriophyllum aquaticum -based biochar (ISA-Fe/MC) is reported for peroxymonosulfate-based organics degradation. Firstly, the Fe nanoparticles anchored on the hierarchical porous biochar (nano-Fe/MC) can be obtained by utilizing K 2 FeO 4 as a synchronous activation and graphitization agent. Subsequently, ISA-Fe/MC was achieved by HCl etching of nano-Fe/MC to remove the excess Fe nanoparticles. Compared with nano-Fe/MC, ISA-Fe/MC demonstrated outperformed catalytic capacity towards PMS activation for phenol degradation. The combination of super high surface area, hierarchical porous structure, graphitization structure and atomically dispersed Fe species should be responsible for prominent catalytic oxidation ability and outstanding resistance to common anions and humic acid. Based on the chemical scavengers, EPR experiments and electrochemistry tests, the SO 4 •– dominated radical degradation pathway for nano-Fe/MC and electron transfer reigned non-radical degradation pathway for ISA-Fe/MC was revealed. In contrast to nano-Fe/MC, density functional theory calculations demonstrated the enhanced density of states around Fermi level in ISA-Fe/MC meaning the increased catalytic performance and more electron transfer between single-atom Fe to adjacent graphitic C and N which could serve as electron transfer channel for PMS activation.
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高影响因子
CHEMOSPHERE
·
2020
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IF 5.778
Xuefeng Liu,Guoshuai Liu,Shijie You
Advanced reduction process (ARP) has drawn an increasing interest as a new manner for removing oxidative pollutants in water. In this paper, we demonstrate the possibility of in-situ reduction of Cr(VI) by CO 2 ·- produced from formate originally existing in leather wastewater by visible-light-driven ARP containing black TiO 2 photocatalyst. The prepared black TiO 2 with nanotube structure achieves remarkable enhanced the reduction rate of Cr(VI) as high as 96.2% (k = 0.0114 min −1 ) in the presence of formate, which is approximately 4.75 times than that of 56.3% (k = 0.0024 min −1 ) in the absence under 120 min visible-light irradiate at unadjusted pH. The results exhibit a distinct contrast with commercial TiO 2 (P25). A series of control experiments are also performed, indicating that formate is able to convert the oxidative environment into a highly reductive one, and the formate concentration, black TiO 2 dosage and pH may greatly impact on the Cr(VI) reduction rate. According to the electron spin resonance (ESR) measurement, CO 2 ·- radicals can be directly verified as dominate radical in this system. Moreover, this system appears to be attractive for creating photochemical systems where in-situ production of CO 2 ·- radicals may be realized by using formate. Then this in-situ ARP system will provide a new perspective for the Cr(VI) removing, which makes leather wastewater treatment much easier and more sustainable in the future.
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APPLIED SURFACE SCIENCE
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2020
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IF 6.182
Yifei Wang,Jing Niu,Xin Gao,Yanlin Zhang
In this study, Y-doped Ag 3 PO 4 , carbon quantum dots (CQDs), BiVO 4 were used to synthesize Z-scheme Y-Ag 3 PO 4 /CQDs/BiVO 4 . X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FT-IR) and UV–vis diffuse reflectance spectra (DRS) were employed to probe into the crystalline structure, morphology, optical property and chemical composition of Y-Ag 3 PO 4 /CQDs/BiVO 4 . The kinetic constant of the prepared Y-Ag 3 PO 4 /CQDs/BiVO 4 was approximately 2.8 times that of pristine Ag 3 PO 4 for atenolol degradation. The degradation of atenolol mainly depended on the excited holes, •OH and •O 2 − . The photocatalysis mechanism of Y-Ag 3 PO 4 /CQDs/BiVO 4 conforms to the Z-scheme mechanism deduced by reactive species trapping experiment, electron spin resonance (ESR) and photoelectrochemical measurement (photocurrent response and EIS). The introduction of yttrium, CQDs and BiVO 4 significantly promoted the photogenerated carriers separation of Ag 3 PO 4 and inhibited the photogenerated electron-holes pairs recombination of Ag 3 PO 4 during the degradation of atenolol. Oxygen defects caused by the doping of Y 3+ into Ag 3 PO 4 were the centers of capture of photogenerated electrons to generate •O 2 − , inhibiting the recombination of photogenerated electron-holes pairs and the photocorrosion of Ag 3 PO 4 .
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CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Xuheng Li,Chunli Wang,Feng Liu,Zhihao Zhang,Jafar Ali,Qingwen Long,Jing Zhang
Electrochemical reduction and treatment of Cr(VI)-contaminated wastewater normally suffer from a high overpotential, due to the extravagant consumption of electrons by the adverse reactions of hydrogen evolution and oxygen reduction. In this work, the MoS 2 film electrode prepared by electrochemical deposition-annealing method was applied into the electrochemical reduction of Cr(VI), with the aim to suppress the over-potential of the reduction and improve the utilization of electrons. Results demonstrated that the 2H/1T′ heterostructure of MoS 2 enhanced the reduction efficiency of Cr(VI) up to 99% at a lower potential of −1.0 V vs. Ag/AgCl. The in-situ electrochemically generated hydrogen peroxide was found to play a critical role in accelerating the reduction of Cr(VI). Selective oxygen reduction reaction (ORR) via a two-electron pathway on the MoS 2 cathode was responsible for the formation of hydrogen peroxide, where the MoS 2 film electrode annealed at 700 °C can obtain a high productivity of 360 μM hydrogen peroxide within 60 min. The plenty of preserved interfaces between 2H and 1 T′ in the heterophase MoS 2 were crucial to the selective electrocatalytic activity. In addition, this electrode also presented an excellent electrocatalytic activity in hydrogen evolution reaction (HER), which could form atomic hydrogen on the surface of cathode to facilitate the reduction of Cr(VI) under the anoxic condition. This study paves a novel pathway to in-situ deposit the MoS 2 film electrode for the sustainable electrochemical reduction and treatment of Cr(VI)-containing wastewater.
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JOURNAL OF MEMBRANE SCIENCE
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2020
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IF 7.183
Yang Yang,Zhu Xiong,Zhu Wang,Yi Liu,Zijun He,Akun Cao,Li Zhou,Lijing Zhu,Shuaifei Zhao
Carbon nanotube (CNT) based adsorbents have attracted extensive research interest for aqueous pollutants removal. However, such adsorbents face the problems of limited adsorption capacities and costly regeneration. Here, we report a highly adsorptive photo-regenerable CNT based multifunctional membrane with excellent self-cleaning properties via the facile vacuum filtration method, followed by FeOOH in-situ anchoring and silver-amino reaction. Various dyes (Rhodamine B, methylene blue, eosin Y and acid orange 7) and emerging contaminants (bisphenol A, amoxicillin and p-nitrophenol) were tested with the CNT based membrane. Our membrane exhibited superior adsorption performance to dyes among CNT based adsorbents reported in literature. In particular, the CNT based composite membrane displayed even better adsorption performance to cationic dyes. The adsorption capacities of the membrane for Rhodamine B and methylene blue were up to 181 and 247 mg/g, respectively. The membrane also had excellent self-cleaning and photo-regenerable properties after severe organic fouling. Our multifunctional CNT based membrane combined the features of adsorption, membrane separation , and catalytic degradation into one system, showing great promise for dye polluted wastewater purification. This study also offers a new strategy to engineer robust adsorptive, self-cleaning and regenerable membranes for wastewater treatment .
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Lele Cui,Zhiwen Li,Qingqing Li,Meifei Chen,Wenheng Jing,Xuehong Gu
The development of transition metal oxide-based integrated carbonaceous materials for use as bifunctional electrodes of high stability and activity in the heterogeneous electro-Fenton (EF) process is supposed to have great potential in environmental governance. Herein, Cu/CuFe 2 O 4 (CCFO) with different Cu 0 ratios were synthesized by a facile one-step solvothermal approach. These materials were subsequently used to fabricate modified graphite felt through the polytetrafluoroethylene (PTFE)-bonding technique. Importantly, with its hydrophobicity PTFE effectively inhibited metal leaching from the thus obtained cathodes and improved the oxygen utilization rate. Cathode performance in EF-based tetracycline (TC) degradation was found to increase with Cu 0 ratio. The observed increase in activity was attributed to Cu 0 enhancing the 2-electron oxygen reduction reaction selectivity (i.e., H 2 O 2 production) and endowing the cathode with abundant electron-rich centers that accelerated active Fe(II) regeneration, causing rapid conversion of H 2 O 2 to hydroxyl radical ( OH). The possible TC mineralization pathway was inferred by liquid chromatography–mass spectrometry (LC–MS) analysis, and a catalytic mechanism of the heterogeneous EF process was proposed. The most effective cathode fabricated displayed high stability even at pH 3 (0.84 ± 0.11 mg/L Fe and 1.35 ± 0.17 mg/L Cu leaching) and exhibited nearly 80% TC removal efficiency after five oxidation cycles, demonstrating its potential use in heterogeneous EF technology for efficient and durable wastewater treatment.
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JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Xiaoping Yu,Wenlei Qin,Xiangjuan Yuan,Lei Sun,Fei Pan,Dongsheng Xia
The present research systematically investigates the atenolol (ATL) degradation in integrated UV/Ozone (O 3 )/peroxymonosulfate (PMS) process focusing on the synergistic mechanism, reaction kinetics, pollutant degradation pathway and antibacterial activity. The results manifested that the integrated UV/O 3 /PMS process showed the noteworthy superiority to ATL degradation compared with UV/PMS, UV/O 3 and O 3 /PMS systems. Simultaneously, the impacts of operating parameters like PMS dosage, initial ATL concentration, solution pH and water matrix were comprehensively explored. The ATL elimination efficiency increased linearly with PMS dose and significantly enhanced in alkaline conditions. The • OH and SO 4 •− were the primary reactive radicals for ATL oxidation in UV/O 3 /PMS system based on the radical scavenging experiments and electron paramagnetic resonance characterization. Besides, a simplified kinetic model on the basis of the dominant reactions and the steady-state assumption was established to foretell the relative contributions of reactive oxidants for ATL elimination in UV/O 3 /PMS process. Main transformation products were determined via UPLC-QTOF-MS to infer the possible degradation pathways of ATL. Furthermore, the UV/O 3 /PMS process could distinctly mitigate the antibacterial activity of ATL and its intermediates to E. coli and B. subtilis . Our findings may have critical implications for the development of novel oxidation processes for recalcitrant contaminants mitigation in water purification .
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