CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Peng Chen,Yejing Gou,Jiaming Ni,Yumeng Liang,Bingqiao Yang,Feifei Jia,Shaoxian Song
Base on the strong activation activity and affinity of transition metal ions and MoS 2 for peroxymonosulfate (PMS), respectively, Co(Ⅱ)-doped MoS 2 nano-flowers (Co-MoS 2 NFs) with a great photo-response property was facilely synthesized to achieve a more efficient PMS activation for ofloxacian (OFX) degradation. It was found that Co-MoS 2 NFs exhibits superior catalytic activity for OFX degradation under visible-light irradiation, which was attributed to the synergetic effect of doped Co(Ⅱ) and photo-generated carriers to PMS activation. Besides, Co-MoS 2 NFs was able to efficiently degrade OFX within 4 cycles in the presence of PMS while leaked minute amount of Mo and Co ions, implying the excellent cycle stability of Co-MoS 2 NFs. Furthermore, SO 4 •− and 1 O 2 were detected as the primary reactive radicals for OFX degradation in the Co-MoS 2 NFs-PMS system through EPR and quenching tests. This new strategy of coupling doped Co(Ⅱ) and photo-generated carriers for more efficient PMS activation, which will greatly benefit the development of SO 4 •− -based AOPs as well as cater to the demand for environmental remediation in the future.
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Journal of Environmental Sciences
·
2020
·
IF 4.302
Changsheng Feng,Chen Chen,Yu Zhu,Qi Cao,Chao Chen,Caiyun Jiang,Yuping Wang
Nitrogen-rich graphitized carbon microspheres (NGCs) with hierarchically porous were constructed by self-assembly. Under different heat treatment conditions, the structure, morphology and properties of NGCs were studied by using multiple characterization techniques. The results showed that the chemical microenvironments (e.g. surface chemistry, degree of graphitization and defective, etc.) and microstructures properties (e.g. morphology, specific surface area, particle size, etc.) could be delicately controlled via thermal carbonization processes. The degradation of ofloxacin (OFLX) by NGCs activated peroxymonosulfate (PMS) was studied systematically. It was found that the synergistic coupling effect between optimum N or O bonding species configuration ratio (graphitic N and C=O) and special microstructure was the main reason for the enhanced catalytic activity of NGC-800 (calcination temperature at 800°C). Electron paramagnetic resonance (EPR) experiments and radical quenching experiments indicated that the hydroxyl ( • OH), sulfate (SO 4 •− ) and singlet oxygen ( 1 O 2 ) were contributors in the NGC-800/PMS systems. Further investigation of the durability of chemical structures and surface active sites revealed that undergo N bonding species configuration reconstruction and cannibalistic oxidation during PMS activation reaction. The used NGC-800 physicochemical properties could be recovered by heat treatment to achieve the ideal catalytic performance. The findings proposed a valuable insight for catalytic performance and controllable design of construction.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2020
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IF 7.864
Wenxiao Zheng,Liuyi Zhu,Sheng Liang,Jinshao Ye,Xin Yang,Zhenchao Lei,Zhang Yan,Yongdong Li,Chaohai Wei,Chunhua Feng
Inorganic constituents in real wastewater, such as halides and carbonates/bicarbonates, may have negative effects on the performance of electrochemical systems because of their capability of quenching HO•. However, we discovered that the presence of Cl– and HCO3– in an electrochemical system is conducive to the formation of ClO•, which plays an important role in promoting the simultaneous elimination of biorefractory organics and nitrogen in secondary coking wastewater effluent. The 6-h operation of the coupled electrochemical system (an undivided electrolytic cell with a PbO2/Ti anode and a Cu/Zn cathode) at a current density of 37.5 mA cm–2 allowed the removal of 87.8% of chemical oxygen demand (COD) and 86.5% of total nitrogen. The electron paramagnetic resonance results suggested the formation of ClO• in the system, and the probe experiments confirmed the predominance of ClO•, whose steady-state concentrations (8.08 × 10–13 M) were 16.4, 26.5, and 1609.5 times those of Cl2•– (4.92 × 10–14 M), HO• (3.05 × 10–14 M), and Cl• (5.02 × 10–16 M), respectively. The rate constant of COD removal and the Faradaic efficiency of anodic oxidation obtained with Cl– and HCO3– was linearly proportional to the natural logarithm of the ClO• concentration, and the specific energy consumption was inversely correlated to it, demonstrating the crucial role of ClO• in pollutant removal.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Xiao-Cong Zhang,Song-Hai Wu,Shao-Yi Jia,Cong Wang,Shi-Wei Sun,Xiang-Ming Wang,Zi-He Meng,Yi-Ying Lin,Yong Liu,Hai-Tao Ren,Xu Han
Turning heterocyclic contaminants into polymers from industrial wastewater is a promising method that opens a new door for feasible and cost-effective treatment for aromatic wastewater. In this study, CuO shows the high reactivity in the catalytic oxidation of thiophene by persulfate (PS) under pH-neutral condition, and the observed rate constant ( k obs ) in the PS-CuO system is about 10 times of that in the PS-alone system at pH 7.0. The linear relationship between the consumed PS and the removed thiophene reveals that a complete removal of 1.0 mM thiophene from solution requires 1.11 mM PS in the PS-CuO system, indicating that thiophene has not been completely mineralized into CO 2 and H 2 O. Quenching experiments and EPR analysis rule out contributions of O 2 •− and 1 O 2 to thiophene oxidation, and suggest that although both SO 4 •− and •OH contribute to thiophene oxidation to some extent, they are not the primary oxidants in the PS-CuO system at pH 7.0. Meanwhile, the presence of thiophene radical cation indicates that electron abstraction from thiophene is an important pathway in the oxidation. The produced thiophene radical cations are then polymerized into polymers. Solid characterizations further confirm that polythiophene S,S -dioxide is the primary oxidation product. The electrochemical analysis indicates that the produced polythiophene S,S -dioxide polymers show pseudocapacitive characteristics and can be used for capacitors.
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ADVANCED FUNCTIONAL MATERIALS
·
2020
·Vol. 30
·期 22
·2000189
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IF 16.836
Chao Zhang,Donglin Xia,Jiahao Liu,Da Huo,Xiqun Jiang,Yong Hu
Myeloid-derived suppressor cells (MDSCs) are garnering increasing attention given their role in tumor development. Herein, a nano-enabled strategy is demonstrated for the eradication of tumor-infiltrated MDSCs by reversing hypoxia. Oxygen-independent photodynamic bismuth tungstate nanoparticles (Bi 2 WO 6 NPs) are loaded into reactive oxygen species (ROS) responsive platelet membranes (PMs) to form a hybrid (PM-BiW NPs). P-Selectin on PMs endows PM-BiW NPs with selectivity toward cancer cells. Once in the tumor, laser illumination stimulates the Bi 2 WO 6 NPs photothermally and photodynamically, which produces enormous quantities of hydroxyl radicals. These hydroxyl radicals help rupture the PM and mitigate hypoxia with the assistance of ionizing radiation. This effectively remodels the tumor microenvironment toward one disfavoring the recruitment of MDSCs and contributes to better prognosis. To better understand the mechanism, the expression levels of a set of markers are monitored. It is found that the downregulations of hypoxia-inducible factor-1α, ectonucleoside triphosphate diphosphohydrolase 2, and adenosine-5-phosphoricacid are behind the blocked infiltration of MDSCs. This platform strategy offers a promising approach to overcome the immunosuppression caused by MDSCs through a trimodal therapy integrating the power of photothermal and photodynamic therapy in addition to radiation therapy.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Qiong Lin,Yue-Hua Li,Ming-Yu Qi,Jing-Yu Li,Zi-Rong Tang,Masakazu Anpo,Yoichi M.A. Yamada,Yi-Jun Xu
The photocatalytic coupling reaction can be conducted in one pot to realize the simultaneous utilization of electrons and holes, thereby obtaining value-added fine chemicals and fuels. Herein, we report a binary nickel modified ZnIn 2 S 4 (Ni:ZIS) for highly efficient photocatalytic selective oxidation of benzyl alcohol (BA) to benzaldehyde (BAD) integrated with hydrogen (H 2 ) evolution, in which Ni can promote photogenerated charge transfer for enhancing photoactivity. Particularly, the products of converting BA to aromatic compounds over blank ZnIn 2 S 4 (ZIS) and Ni:ZIS show a marked difference under the same reaction conditions. Hydrobenzoin (HB) is the primary product over blank ZIS. After the introduction of Ni, the formation of HB is dramatically suppressed, resulting in higher selectivity of BAD, because the introduction of Ni facilitates the α-H abstraction. In addition, an analogous phenomenon has been observed on Ni-based compounds modified ZIS, such as Ni x P and NiS. It is hoped that this work would provide a feasible paradigm for modifying the surface of photocatalysts to tune the selectivity of product-oriented alcohols oxidation coupled with H 2 evolution in water.
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APPLIED MICROBIOLOGY AND BIOTECHNOLOGY
·
2020
·Vol. 104
·期 9
·3947-3957
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IF 3.53
Qu Yuejun,Yang Yue,Du Renjie,Zhao Min
A sensing methodology that combines Au, tobacco mosaic virus (TMV), and folic acid for selective, sensitive, and colorimetric detection of tumor cells based on the peroxidase-like activity was reported in this study. Gold nanowires with a high aspect ratio were synthesized using TMV as a template. Au@TMV nanowire (AT) complex was obtained with diameter of 4 nm and length between 200 and 300 nm. In addition, since TMV was biocompatible and had many amino and carboxyl groups on its surface, AT was conjugated by folate to form a folic acid (FA)–conjugated AT composite (ATF) and tested by FTIR measurements. Furthermore, the peroxidase-like properties were studied and the optimal conditions for mimic enzyme activity were optimized. Finally, HeLa and other tumor cells expressed excessive receptors of folate on the surface, which can specifically bind to folic acid. As the specific binding of ATF with HeLa cells, the peroxidase properties of ATF were used for detection of cancer cells (Scheme 1). The cancer cells were detected not only qualitatively but also quantitatively. In this study, as low as 2000 cancer cells/mL could be detected using the current method.
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JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Xiaojun Zhou,Lingshuai Kong,Zongyu Jing,Shuqing Wang,Yongchao Lai,Meng Xie,Long Ma,Zhenyu Feng,Jinhua Zhan
In this study, superparamagnetic β-CD-MnFe 2 O 4 with a large surface area was synthesized via a facile co-precipitation method, with β-cyclodextrin (β-CD) acting as a coating agent. The as-prepared β-CD-MnFe 2 O 4 exhibited better catalytic performance than bare MnFe 2 O 4 in terms of activating peroxymonosulfate (PMS) to degrade 2,4-dichlorophenol (2,4-DCP) over a broad pH range of 5–11. Electron spin resonance spectroscopy (ESR) and free radical quenching experiments indicate that various active species (SO 4 − / OH/O 2 − / 1 O 2 ) are generated in the β-CD-MnFe 2 O 4 /PMS system and that pollutants trapped in the cyclodextrin cavity are quickly degraded. Various reaction parameters of the β-CD-MnFe 2 O 4 /PMS system and the stability of β-CD-MnFe 2 O 4 were also investigated. The results indicate that β-CD-MnFe 2 O 4 is promising for use in water purification owing to its excellent magnetic separation and recovery properties and good resistance to humic acid (HA).
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Environmental Science-Nano
·
2020
·Vol. 7
·期 5
·1444-1453
·
IF 7.683
Shang Yanan,Xu Xing,Qinyan Yue,Baoyu Gao,Yanwei Li
In this work, the carbon nanotubes (CNTs) encapsulating Zn and Fe bimetallic nanoparticles (FeZn@NC) were synthesized through a one-pot pyrolytic strategy. The persulfate (PS) activation ability of FeZn@NC with various ratios of Fe and Zn was determined by sulfamethoxazole (SMX) degradation. The results indicated that the iron played a key role in forming external CNTs and the catalytic activity of FeZn@NC was mainly based on the encapsulated FeZn nanoparticles. In addition, PS activation was greatly strengthened by the heterostructure of FeZn@NC. Free radical quenching experiments and electron paramagnetic resonance (EPR) spectra suggested that the singlet oxygen was the key reactive oxygen species for SMX degradation. The activity of pyridinic-N, pyrrolic-N and graphitic-N on external CNTs was analyzed by theoretical calculations, which showed the pyridinic-N possessed strong adsorptive ability to activate PS to degenerate sulfate radicals.
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CHINESE JOURNAL OF CATALYSIS
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2020
·
IF 6.146
Sufeng An,Guanghui Zhang,Jiaqiang Liu,Keyan Li,Gang Wan,Yan Liang,Donghui Ji,Jeffrey T. Miller,Chunshan Song,Wei Liu,Zhongmin Liu,Xinwen Guo
Heterogeneous catalysts with ultra-small clusters and atomically dispersed (USCAD) active sites have gained increasing attention in recent years. However, developing USCAD catalysts with high-density metal sites anchored in porous nanomaterials is still challenging. Here, through the template-free S-assisted pyrolysis of low-cost Fe-salts with melamine (MA), porous alveolate Fe/g-C 3 N 4 catalysts with high-density (Fe loading up to 17.7 wt%) and increased USCAD Fe sites were synthesized. The presence of a certain amount of S species in the Fe-salts/MA system plays an important role in the formation of USCAD S-Fe-salt/CN catalysts; the S species act as a “sacrificial carrier” to increase the dispersion of Fe species through Fe-S coordination and generate porous alveolate structure by escaping in the form of SO 2 during pyrolysis . The S-Fe-salt/CN catalysts exhibit greatly promoted activity and reusability for degrading various organic pollutants in advanced oxidation processes compared to the corresponding Fe-salt/CN catalysts, due to the promoted accessibility of USCAD Fe sites by the porous alveolate structure. This S-assisted method exhibits good feasibility in a large variety of S species (thiourea, S powder, and NH 4 SCN) and Fe salts, providing a new avenue for the low-cost and large-scale synthesis of high-density USCAD metal/g-C 3 N 4 catalysts.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2020
·
IF 6.551
Zhendong Li,Dongfang Liu,Wenli Huang,Xiaocheng Wei,Weiwei Huang
Biochar supported copper oxide composite (BC-CuO) was synthesized and attempted to activate peroxymonosulfate (PMS) for treating highly saline (100–400 mM) wastewater. In the BC-CuO/PMS system, rapid removals of Methylene Blue (MB), Acid Orange 7, Rhodamine B, Atrazine and Ciprofloxacin from the highly saline system were observed within 30 min, attaining a high efficiency of 99.68%, 100%, 100%, 100% and 78.27%, respectively. Meanwhile, the BC-CuO/PMS can remove >88.61% of MB in other salt systems containing one or more salt components and 68.43% of COD from landfill leachate . Experimental results confirmed that sulfate radical (SO 4 ▪- ), hydroxyl radical ( ▪ OH) and singlet oxygen ( 1 O 2 ) all contributed to the pollutants degradation , but 1 O 2 was dominated in highly saline systems. On the basis of the characterization and analysis data, possible activation mechanisms of the oxygenated functional groups of biochar and hydroxylation of CuO surface accelerating the generation of 1 O 2 were proposed. BC-CuO activating PMS is a promising technique for the removal of organic pollutants from highly saline wastewater or complex background.
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ATMOSPHERIC ENVIRONMENT
·
2020
·
IF 4.039
Xuewen Guo,Nan Zhang,Xin Hu,Yue Huang,Zhuhong Ding,Yijun Chen,Hong-zhen Lian
PM 2.5 –bound toxic elements and organic pollutants have been extensively investigated, while limited information is available for environmental persistent free radicals (EPFRs) associated with PM 2.5 , which may lead to oxidative stress in the human lung when exposed to PM 2.5 . In this study, the levels and types of PM 2.5 –bound EPFRs present in Nanjing, a mega–city in China, were analyzed. PM 2.5 –bound EPFRs were found to mainly be a mixture of carbon– and oxygen–centered radicals. The concentration of PM 2.5 –bound EPFRs ranged from 2.78 × 10 12 to 1.72 × 10 13 spins m −3 , with an average value of 7.61 × 10 12 spins m −3 . The half–life of the PM 2.5 –bound EPFRs was calculated to be an average of 83.5 days when stored at room temperature, with only weak correlations observed between EPFRs and conventional air pollutants (NO 2 , O 3 , CO and PM 2.5 )/PM 2.5 –bound transition metals (Cu, Zn, Cr, Mn, V, Cd, and Ni) and significant correlations between EPFRs and SO 2 /PM 2.5 –bound Fe. PM 2.5 –bound EPFRs can induce the formation of reactive oxygen species (ROS) in both water and a H 2 O 2 solution, which are used to simulate lung solution of a healthy person and patient, respectively. Therefore, PM 2.5 –bound EPFRs can lead to potential oxidative stress in humans. Overall, PM 2.5 –bound EPFRs show an obvious temporal variation and can pose potential health risks to humans via the induction of ROS in the lung solution.
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