CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Chao Liu,ShanShan Dong,Yinguang Chen
Effective interface contact between components in heterojunction is crucial to realize high photocatalytic performance of photocatalyst. In this paper, the improvement of heterojunction contact by forming new ternary heterostructure via calcining the mixture of tetracycline and melamine to obtain the graphene-like carbon plane grafted g-C 3 N 4 and then coupling it with TiO 2 is reported. The unique carbon plane, which is anchored into g-C 3 N 4 basal domains, acts as a significant role to achieve the sufficient ternary heterojunction contact in the novel carbon plane/g-C 3 N 4 /TiO 2 nanostructure system. Under visible-light irradiation, the new ternary nanocomposite exhibits excellent photocatalytic activity for efficient removal of aqueous organic contaminants: methylene blue (98.6%), tetracycline (94.0%), and norfloxacin (95.3%), with the corresponding degradation rate constants of 0.0441, 0.0302, and 0.0125 min −1 , respectively, which are 54.1, 9.8, and 9.4 times higher than that of the pure g-C 3 N 4 . The mechanism study indicates that the excellent photocatalytic activity is attributed to the effective heterojunction, which can successfully extend visible-light absorption, promote charge separation efficiency, and suppress recombination of the photocatalytic electron-hole pairs. Moreover, the electron spin resonance (ESR) assay and radical scavenger experiments demonstrate that the photogenerated holes (h + ), superoxide anion radicals ( O 2 − ), and hydroxyl radical ( OH) play vital roles in photocatalytic degradation process. Importantly, this work may open up novel insights into the design of ternary heterostructure with highly efficacious photocatalytic performance, which suggests attractive applications in environment protection.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Fanqing Meng,Wei Ma,Chunying Duan,Xin Liu,Zhen Chen,Moyan Wang,Jian Gao,Zhe Zhang
Two dimensional transition metal dichalcogenides as potential catalysts to solve energy and environmental crises have caused significant research interests in recent years. In this work, edge-selectively Fe@3D-WS 2 nanoflowers with the abundant single-layer were efficiently prepared by dry ball milling for levofloxacin (LEVO) elimination. Together with the advantages of the single-layer active edges and the stretch of W S bond, the as-prepared Fe@3D-WS 2 showed the ultra-high degradation efficiency for LEVO under ball-milling condition. This high degradation activity was demonstrated to be originated from piezo-catalysis, rather than adsorption or thermocatalysis. In addition, the Fe@3D-WS 2 also showed an ultra-high reusability during the cyclic tests, which is due to its special “self-renewing” behavior under ball milling condition. The degradation efficiency of the Fe@3D-WS 2 still reached ˜ 99% after ten cyclic tests. Both oxygen radicals ( 1 O 2 , O 2 ·− ) and ·OH radicals were generated and took part in the LEVO degradation, while oxygen radicals were more contributed to the LEVO degradation. The present work not only provides an important insight for designing efficient catalysts, but also extends the possible application areas of ball milling technique.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Deyou Yu,Lubiao Li,Minghua Wu,John C. Crittenden
The photocatalytic activity of metal-organic frameworks (MOFs) is drawing great attention in the field of environmental remediation. However, the efficiency of MOFs still remains low because of the rapid recombination of valence band holes and conduction band electrons (a.k.a., charge carriers). The combination of photocatalysis and electron acceptors such as ozone are believed to be an efficient strategy to reduce the charge carrier recombination. Herein, we report that photocatalytic ozonation (PCO) using an Fe-based MOF (MIL-88A(Fe)) has greater destruction than photocatalysis and/or catalytic ozonation in terms of 4-nitrophenol (4-NP) degradation and mineralization. It is worth noting that our Fe-based MOF has a large number of Lewis acid sites (LAS). The pseudo-first order kinetic rate constants ( k ) of 4-NP degradation using PCO, photocatalysis and catalytic ozonation systems are 0.1632, 0.0143 and 0.0840 min −1 , respectively. The TOC removal of 4-NP in the PCO system is approximately 75.4% ([4-NP] = 100 ppm, ozone input dosage = 1.5 mg/min-L, UV light intensity = 3.46 × 10 -6 Einstiens/L-s, treatment time = 30 min) and this is much greater than those of photocatalysis (17.6%) and catalytic ozonation (38.7%). Most importantly, both the k value and TOC removal in the PCO system are much higher than the sum of those in other two processes, implying a strong synergistic effect in the PCO process. Mechanistic studies were conducted using electrochemical impedance spectroscopy (EIS) and photoluminescence (PL) measurements and demonstrate that the synergistic effect may originate from the enhanced photoinduced carrier separation using ozone as an electron acceptor. Furthermore, OH, O 2 − , and 1 O 2 are found to be the principal reactive oxygen species (ROS) for 4-NP degradation and mineralization. Integrating the analysis of band structure, EPR and scavenging experiment results, ozone is not only able to reduce charge carrier recombination but also can be catalytically decomposed to generate more ROS on the LAS of MIL-88A(Fe). This study provides deep insights into the use of MOFs as effective advanced oxidation processes (AOPs).
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JOURNAL OF HAZARDOUS MATERIALS
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2018
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IF 6.434
Ying Liu,Yong Feng,Yunfei Zhang,Shun Mao,Deli Wu,Huaqiang Chu
In this study, the presence of Cu(II) ions was found for the first time to severely inhibit +-dimethyl phthalate (DMP) degradation by ozone due to the formation of the stable complex Cu(II)-DMP. However, 100% DMP removal was rapidly reached when ethylenediamine tetraacetic acid (EDTA) was added with a Cu(II)/EDTA molar ratio of 3:1. Subsequent studies indicated that Cu(II)-DMP is sequestrated by EDTA, then DMP was degraded and Cu(II) was removed by precipitation. The freshly formed Cu-EDTA 2− and organic nitrogen intermediates further decomposed O 3 into OH, which induced to the rapid degradation of DMP. The k obs of Cu-EDTA/O 3 were 9–10 times greater than the k obs of DMP removed by ozonation alone within 10 min. The reaction mechanism involved a OH generation was proposed. The OH and O 2 - are generated from the rapid reaction between ozone and EDTA. Acting as a more strongly negative species, the specific Cu(II) in Cu-EDTA complexes is more inclined to react with O 2 - to give Cu(I), accelerating the forward reaction to produce more OH. The synergistic removal of DMP and Cu(II) can be achieved after reaction. Therefore, this study provides an effective method to dispose metal ion and organic pollutant wastewater.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Chen Li,Hui Lin,Andac Armutlulu,Ruzhen Xie,Yongli Zhang,Xiaoyang Meng
In this study, ferrate (Fe(VI)) was used as catalyst to activate persulfate (PS) for the removal of ciprofloxacin (CIP) from aqueous solution. Hydroxylamine (HA) was used to accelerate the reduction and regeneration of Fe(II) from the Fe(VI) + PS system. It was found that 91.5% of 30 μM CIP was decomposed within 60 min in the PS + Fe(VI)/HA system, which is 25.9% higher than that in the PS + Fe(VI) system. In the PS + Fe(VI)/HA system, the removal of CIP increased with the decrement of initial solution pH, whereas inorganic anions (i.e. HCO 3 − , Cl − , NO 3 − ions) and humic acid had slightly inhibitory effects on CIP removal. The radical scavenging experiments and the electron paramagnetic resonance (ESR) tests confirmed that the addition of HA in the PS + Fe(VI) system can accelerate the generation of reactive oxygen species (ROS) such as sulfate radicals (SO 4 − ) and hydroxyl radicals ( OH), which played important roles for the removal of CIP in the PS + Fe(VI)/HA system. CIP degradation intermediates were also identified and the pathways were proposed. This study suggested a new approach for catalytic degradation of CIP by ferrate.
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Journal of Materials Chemistry B
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2018
·Vol. 7
·期 2
·296-304
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IF 4.776
Yan-Wen Bao,Xian-Wu Hua,Huan-Huan Ran,Jia Zeng,Fu-Gen Wu
Nanomaterial-based enzyme mimics (nanozymes) are attracting increasing attention because of their low production cost, high stability against denaturation, and resistance to high concentrations of substrates. Here, carbon nanoparticles doped with a small amount (<5 mol%) of Pt (denoted as PtCNPs) are synthesized via a facile, cost-effective hydrothermal treatment of p-phenylenediamine (PPD) and K2PtCl4. The obtained PtCNPs possess high aqueous stability, excellent water-dispersibility, and suitable size (∼15 nm). More interestingly, the PtCNPs exhibit an intrinsic peroxidase-like activity that can quickly catalyze 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of hydrogen peroxide (H2O2) and produce a blue color. Importantly, since satisfactory catalytic properties were also observed when K2PtCl4 was replaced with CuCl2, NiCl2, or Na2PdCl4 during the synthesis, the PPD- and inorganic metal salt-involved hydrothermal synthetic approach may be developed as a general and simple way to fabricate new nanozymes. Besides, the steady-state kinetics reveals that the PtCNPs have a stronger affinity for TMB and a weaker affinity for H2O2 compared with horseradish peroxidase. On the basis of the color reaction, a colorimetric detection method for H2O2 and glucose has been successfully established with a detection limit of 0.15 and 0.30 μM, respectively. Further, the method has also been successfully applied for glucose detection in human serum samples. To sum up, this work develops a new synthetic method of metal-doped carbon nanomaterials and demonstrates their capability for the sensitive and selective detection of H2O2 and glucose, which may foster the development of new nanozymes for biosensing applications.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Haichao Fu,Shuanglong Ma,Peng Zhao,Shengjun Xu,Sihui Zhan
Three novel graphitized hierarchical porous biochar (MX) and MnFe 2 O 4 magnetic composites (MnFe 2 O 4 /MX) have been prepared for degrading organic pollutants by peroxymonosulfate (PMS) activation. MX including MS, ML, MC synthesized using corn stems (S), leaves (L) and cores (C) as raw materials, respectively, possesses hierarchical porous structure, graphitization domains and tremendous surface area. The orange II removal effects of MX and MnFe 2 O 4 /MX outperform the corresponding carbonization products, despite that adsorption probably undertakes the major removal efficiency for MX and degradation contributes the most for MnFe 2 O 4 /MX. A structure-dependent degradation efficiency is discovered for MX and MnFe 2 O 4 /MX, among of which both MS and MnFe 2 O 4 /MS present the best removal effect, by electrochemical impedance spectroscopy (EIS) and X-ray photoelectron spectroscopy (XPS). The lowest EIS owning to its better balance between graphitization degree and specific surface area and micropore volume of MnFe 2 O 4 /MS among MnFe 2 O 4 /MX explains its best catalytic activity. The catalytic degradation occurs by the following three ways. First, the radical-induced oxidation is attained by surface-bound SO 4 − and OH on MnFe 2 O 4 nanoclusters and hierarchical porous carbon nanosheets generated by one-electron reduction of PMS under the participating and coupling of Mn(III)/Mn(II), Fe(III)/Fe(II), O 2 / O 2 − , and active sites on carbon surface. Second, non-radical pathway involves the contribution of 1 O 2 , which is produced in a large quantity by promoted self-decomposition of PMS in presence of MnFe 2 O 4 /MS. Third, non-radical pathway is achieved through electron transfer from organic compounds as electron donator to PMS as electron acceptor mediated by graphitization structures. Taking into consideration the excellent degradation performance, easy magnetic separation, and bulk availability of MnFe 2 O 4 /MS, this work is expected to pave a new way for precision utilization of corn biomass-based biochar for environmental application.
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CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Guangyu Wu,Wenlei Qin,Lei Sun,Xiangjuan Yuan,Dongsheng Xia
The enhancement performance, mechanisms and kinetic study of peroxymonosulfate (PMS) towards ozonation via prometon (PMT) degradation have been comprehensively investigated via the semi-continuous experiments in the present study. The removal of PMT (>97.34%) and the pseudo-first-order rate constant ( k = 0.6095 min −1 ) were achieved after 7 min reaction with 7.5 mg min −1 O 3 and 100 mg L −1 PMS at pH 6.5. Meanwhile, the PMT degradation performance was systematically evaluated in terms of inlet O 3 concentration, PMS dose, solution pH, water matrix species and etc . It was notable that pH played a significant role on the PMT degradation efficiency in O 3 /PMS process, especially under the neutral and alkaline conditions. The mechanism of the synergistic effect was subsequently explored by the radical scavengers and electron paramagnetic resonance experiments, confirming that both OH and SO 4 − were the dominant reactive radicals in O 3 /PMS process. In addition, the second-order rate constants of PMT with OH and SO 4 − were determined to be 1.9 × 10 9 M −1 s −1 and 1.7 × 10 9 M −1 s −1 via competition kinetics for the first time. Moreover, the plausible degradation pathways of PMT were elucidated based on the seventeen transformation by-products detected. Furthermore, a modified kinetic model was put forward to quantify the relative contribution of OH and SO 4 − , in order to accurately predict the degradation rate of PMT in O 3 /PMS process. This investigation could provide a promising alternative in developing more efficient O 3 -based advanced oxidation process and supply a feasible approach for water decontamination.
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Biomaterials Science
·
2019
·Vol. 7
·期 9
·3886-3897
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IF 5.251
Zhengxi Guo,Xiaohong Zhou,Cheng Hou,Zhaoyang Ding,Changchun Wen,Lai-Jun Zhang,Bang-Ping Jiang,Xing-Can Shen
Specific targeting capabilities and effective phototherapeutic functions are the key demands for precise cancer phototherapeutic agents. Herein, a bioinspired nanoplatform composed of Cu(II)-chlorophyll–hyaluronic acid nanoparticles (Cu(II)Chl–HA NPs) was developed for targeting cancer and synergistic photodynamic/photothermal therapy. Inspired by the photonic biosystem of the chloroplast, Cu(II) chlorophyll was used as a photosensitive substituent to covalently connect with a hydrophilic HA tail rather than a natural phytol tail, and this conjugate further assembled into a nanoparticle-like morphology under non-covalent interaction. Time-dependent density functional theory calculations reveal that the Cu(II) chlorophyll has a much smaller energy gap between an excited singlet and excited triplet, and theoretically leads to rapid electron intersystem crossing that would benefit the PDT effect. In addition, a series of experiments have proven that, under 650 nm laser irradiation, the nanoplatform of Cu(II)Chl–HA can produce a high amount of singlet oxygen and exhibit an outstanding photothermal conversion capability. More interestingly, owing to the specific interactions between the HA component and the CD44 receptor on the cell membrane, the HA tails impart Cu(II)Chl–HA NPs an excellent receptor-mediated targeting performance toward CD44-overexpressing cancer cells. Based on these features, the nanoplatform of Cu(II)Chl–HA NPs presents active targeting and outstanding dual modality synergistic PDT/PTT performance of cancer both in vitro and in vivo. Thus, this work opens up a new strategy to fabricate a bioinspired multifunctional cancer phototherapy nanoplatform.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Yizhen Zhang,Lifen Liu,Qiyuan Chen,Yun He,Michael K.H. Leung
A novel system including peroxymonosulfate (PMS) activation process in a photocatalytic fuel cell (PFC) was established, promoting the degradation efficiency of berberine and enhancing the simultaneous electricity generation. The cathode is based on carbon-fiber cloth (CC) and loaded CoFe 2 O 4 with carbon nano-fibers (CNFs), matching well with Ag NPs/ZnO NRs/NiF photo-anode to drive PFC work. The CNFs/CoFe 2 O 4 /CC cathode is multifunctional, it can activate PMS for sulfate radical ( SO 4 - · ) generation, and can simultaneously accept electrons from photo-anode for transform between Co 3+ and Co 2+ . The adding of PMS in PFC system boosts radical formation and cyclic reactions between related species. This PFC-PMS system showed a high antibiotic degradation efficiency and stable electricity generation (93.5% for berberine degradation, 9.18 h −1 for kinetic rate constant, ~0.50 V for cell-voltage at 2000 Ω). In addition, the pollutant removal capacity, influencing factors and the pollutant degradation mechanism in PFC-PMS system were illustrated. The feasible mechanism of berberine degradation was elucidated by the radical trapping and EPR test and these results confirmed that the formation of reactive species, including SO 4 - · , OH, O 2 - · , 1 O 2 radicals and holes. This study suggests that the established PFC-PMS system is more efficient in wastewater treatment and simultaneous energy recovery.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Yake Xu,Lingyu Zeng,Lanqing Li,Yoon-Seok Chang,Jianyu Gong
In this study, we systematically investigated the oxidative degradation of 4-chlorophenol (4-CP) using nano zero valent iron (nZVI, Fe 0 ) cooperated with citric acid (CA), and the role of CA as well as the mechanism of oxidation were deeply evaluated. 56.2% of 4-CP was removed after 60 min under dark condition without any ventilation of oxygen in the presence of Fe 0 and CA. The addition of CA accelerated the release of ferrous ions and promoted the Fenton reaction to generate much more reactive oxygen species (ROS), which was confirmed by EPR. The MINEQL+ 4.6 soft was utilized to calculated the existent species in Fe 0 -CA system, and Fe(II)[Cit] − was found to be the key species playing an important role on the degradation of 4-CP. Fe(II)[Cit] − adsorbed on iron surface accelerated the transportation of electron from Fe 0 to O 2 to produce more OH. This study puts forward the possible mechanism of generating ROS on Fe 0 enhanced by CA and provides an application for the oxidation of pollutants.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
·
IF 14.229
Lingshuai Kong,Guodong Fang,Yufeng Chen,Meng Xie,Feng Zhu,Long Ma,Dongmei Zhou,Jinhua Zhan
In this study, a flower-like Cu 2 FeSnS 4 (CFTS) nanomaterial was applied to the activation of persulfate (PS) for the degradation of bisphenol A (BPA) in model industrial wastewater. The efficiency of PS decomposition by CFTS, and the mechanism of contaminant degradation by SO 4 − were investigated. The results revealed that CFTS catalyzes PS decomposition more efficiently than the monometallic Cu/Fe/Sn sulfides and exhibits activity over a wide pH range. Electron spin resonance spectroscopy, X-ray photoelectron spectroscopy, and free radical quenching experiments revealed a tandem synergistic effect between Cu, Fe, and Sn in their quaternary chalcogenide systems upon PS activation. The intrinsic electron transfer between Cu, Fe and Sn, especially the Fe(II)* species formed upon the complexation of Fe(II) by S on the surface of the CFTS, overcomes the inhibition of the M (n+1)+ /M n+ redox cycle. CFTS shows promise as a catalyst for wastewater treatment.
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