ENVIRONMENTAL RESEARCH
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2021
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IF 6.498
Lei Chen,He Wang,Yanping Sun,Yue Zhao,Huixiang Shi
Ferrihydrite (Fh), a precursor of more crystalline Fe (hydr)oxides, exhibits decent catalytic behavior; however, the instability of its amorphous structure limits its engineering applications. Siliceous ferrihydrite (FhSi) was readily synthesized in this study by co-precipitation. The formation of Fe–O–Si linkages did not alter the amorphous state of pure Fh, but increased the surface area (S BET ), reduced the point of zero charge (pH ZPC ), and prevented the leaching of more iron. X-ray diffraction, Mössbauer and pyridine-Fourier transform infrared (FTIR) spectroscopies, and potentiometric titration revealed the presence of silicon-occupied portions of growth sites on the Fh surface, which increased the coordination symmetry around the Fe atom and inhibited the transition of Fh to more stable crystalline Fe (hydr)oxides during repeated use. Meanwhile, the density of surface hydroxyl groups (Ds) and the total acid content of the catalytic system after five cycles of catalytic ozonation were 56.75 % and 63.58 % higher than those of freshly prepared system, thereby benefiting the catalysis of ozone for generating ·OH. In addition, the lower pH ZPC of the FhSi/O 3 system compared to that of the Fh/O 3 system promoted the generation of neutral surface-hydroxyl species on the surface of FhSi, which enabled a decent catalytic performance in alkaline solutions, regardless of the catalytic cycle. Moreover, the removal of humic acids (HA) followed a hydroxy radical reaction, which involved self-decomposition (14.15 %), catalytic ozonation (21.58 %), and peroxone and Fenton-like reactions (64.27 %).
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高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2021
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IF 6.789
Guanjun Wang,Dongdong Ge,Lu Bai,Yanting Dong,Chang Bian,Jiajia Xu,Nanwen Zhu,Haiping Yuan
Sludge dewatering , as one of the most important steps of sludge treatment , can facilitate transportation and improve disposal efficiency by reducing the volume of sludge . This study investigated the effects of electrolysis-activated persulfate oxidation on improving sludge dewaterability. The results indicated that the sludge capillary suction time (CST) and water content of dewatered sludge cake (Wc) reduced from 93.7 s and 87.8% to 9.7 s and 68.3% respectively at the optimized process parameters: electrolysis voltage of 40 V, electrolysis time of 20 min, and 1.2 mmol/g TS S 2 O 8 2− . Correlation analysis revealed that the enhancement of sludge dewaterability was closely associated with the increased floc size and zeta potential , decreased protein content in three-layers extracellular polymeric substances (EPS) and viscosity ( R = −0.868, p = 0.002; R = −0.703, p = 0.035; R ≥ 0.961, p < 0.001; R = 0.949, p < 0.001). Four protein fluorescence regions in EPS were analyzed by three-dimensional excitation-emission matrix parallel factor (3D-EEM-PARAFAC). The protein secondary structure was changed after the treatment, and the reduction of α-helix/(β-sheet + random coil) indicated that more hydrophobic sites were exposed. Analysis by X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FTIR) and rheological test demonstrated that the hydrophilic functional groups of the sludge were decreased and the sludge mobility was significantly enhanced after the treatment with electrolysis-activated persulfate oxidation. Moreover, bound water was converted to free water during SO 4 · − and ·OH generated by electrolysis-activated persulfate degraded EPS and attacked sludge cells. Meanwhile, scanning electron microscopy (SEM) images revealed that the treated sludge formed porous channel structures, which promoted the flowability of the water. These findings provide a new insight based on electrolysis-activated persulfate oxidation in sludge treatment for enhancing sludge dewaterability.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Quanfa Zhong,Qintie Lin,Wenjie He,Hengyi Fu,Zhuofan Huang,Yupeng Wang,Libin Wu
Tetracycline (TC) is a kind of refractory pollutant and widely exists in environment, and it is urgent to develop effective methods for TC treatment. In this study, nitrogen-doped biochar (N-BCX) was successfully synthesized and was used to activate persulfate (PS) to degrade TC. The materials were characterized by XPS, Raman spectrum, SEM, BET and FT-IR. SEM and BET results showed that the catalyst had an obvious pore structure and large specific surface area, which increased with increasing pyrolysis temperature. Nitrogen doping could increase the content of graphite-N in biochar; the defect edge of the material increased, further formed the graphitization structure, and enhanced the catalytic performance of the material. TC (20 mg/L) could be completely removed within 120 min under the optimal conditions of 200 mg/L of catalyst dosage, 2 mM of PS dosage and initial pH of 7. The results of EPR, quenching experiments and electrochemical experiments showed that the degradation of TC in the system did not depend on the action of radicals, the electron transfer between TC and PS on the surface of biochar maybe the main pathway. Efficient and environmentally friendly nitrogen-doped biochar can provide a reference for the related antibiotic wastewater treatment.
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Nano Today
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2021
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IF 20.722
Jiawei Zhao,Yugang Wang,Wenjing Wang,Ying Tian,Zhongdong Gan,Yanlei Wang,Hongyan He,Wei Chen,Xiao Zhang,Yuanbin Wu,Rongrong Jia,Min Shi,Wei Wei,Guanghui Ma
Reactive oxygen species (ROS) are key contributors to inflammatory progression and damage. Upon clinical and experimental observation of vascular abnormalities in acute inflammatory diseases, we explore cellular vesicles as templates and carriers to elevate therapeutic performance of nano-antioxidant. Specifically, we develop a mild one-pot approach for in situ growth of cerium oxide (Ce) nanocrystals onto nano-sized red blood cells vesicles (ReVs). Besides excellent biocompatibility, Ce-ReVs have very high ROS-scavenging activity, which is experimentally and theoretically explained by discovering the unique functions of membrane lipids in optimizing Ce nanocrystals with ultrasmall size (~ 3 nm) and ultrahigh Ce(III) content (~ 60.8%). In colitis and acute liver injury models, Ce-ReVs notably enhance accumulation at the inflamed sites and confer strong ROS elimination. Moreover, we upgrade the system by hybridizing ReVs with mesenchymal stem cell-derived exosomes and demonstrate additional repair function of highly damaged tissues, further verifying the satisfactory flexibility and therapeutic efficacy.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Jun Li,Zu-E Hu,Yun-Jie We,Yan-Hong Liu,Na Wang,Xiao-Qi Yu
To minimize unwanted reactions with high concentrations of reduced glutathione (GSH) in the tumor microenvironment (TME) during chemodynamic therapy (CDT), a simple and effective strategy was developed to fabricate a TME stimuli-responsive theranostic nanomedicine ( Fe-CD ) for fluorescence imaging-guided GSH depletion and cancer therapy by combining fluorescent imaging carbon dots ( CD ) and Fe(III). Introducing Fe(III) into Fe-CD not only quenched the fluorescence of CD while reacting with and consuming intracellular GSH for fluorescence imaging of the depletion of GSH but also provided a source of metal ions to generate more abundant hydroxyl radicals (•OH) with hydrogen peroxide (H 2 O 2 ) through the Fenton reaction to improve CDT. Fe-CD showed promising •OH generation under H 2 O 2 to effectively degrade methylene blue in vitro and obviously activate the green fluorescence of the reactive oxygen species (ROS) probe in cells. Benefiting from the fluorescence enhancement in response to TME stimulation, Fe-CD greatly enhanced CDT cytotoxicity while monitoring successful GSH depletion by fluorescence imaging. Fe-CD has the potential to act as a theranostic nanomedicine for fluorescence imaging-guided GSH depletion to amplify CDT.
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APPLIED SURFACE SCIENCE
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2021
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IF 6.707
Dashi Lei,Juanqin Xue,Xiangyu Peng,Shuhao Li,Qiang Bi,Changbin Tang,Liang Zhang,Jing Zhang
Inorganic arsenic threatens human health due to its high mobility and toxicity. In this work, rapid and effective treatment of As(III) wastewater was achieved by Z-Scheme photocatalyst (ZnFe 2 O 4 /Ag/AgCl). By means of peroxymonosulfate (PMS) activation, 50 mg/L As(III) was completely removed within 20 min under light irradiation. During photocatalytic system, free radicals ( SO 4 − , OH, O 2 − ) and non-radicals ( 1 O 2 ) were responsible for As(III) removal. The fast PMS activation was attributed to the loop conversion of Fe(III)/Fe(II) and Ag 0 /Ag + . Besides, density functional theory (DFT) calculations exhibited that Fe atoms were active sites for As(III) adsorption and Ag nanoparticles were spots for PMS activation. Specially, the dual active sites on photocatalyst could effectively minimize the distance between oxidizing product with arsenite molecular and thus facilitate As(III) fast oxidation.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Rui Ma,Xueqian Yan,Xiaohui Mi,Yaoguo Wu,Jin Qian,Qiuyu Zhang,Guang-Hao Chen
In this study, the Mg-Fe-LDH@biochar composite was firstly fabricated and applied for effectively activation peroxymonosulfate (PMS) for aqueous doxycycline (DOX) degradation. The physiochemical properties of the as-synthesized composite were thoroughly characterized. In the developed Mg-Fe-LDH@biochar/PMS system, the catalytic DOX degradations were evaluated under different conditions. Under the optimal condition (0.75 g/L catalyst loading, 0.75 g/L PMS dosage, pH = 7.0), about 88.76% DOX (35 mg/L) was removed within 120 mins. The results of quenching test and electron paramagnetic resonance (EPR) illustrated that the •OH, SO 4 • - and •O 2 – radicals all contributed to the DOX degradation in the Mg-Fe-LDH@biochar/PMS system, whereas the 1 O 2 -based non-radical degradation played the dominant role in DOX removal. The developed system was almost not adversely affected by the high-strength anions and exhibited high DOX decomposition rates in a wide pH range from 3.0 to 9.0, indicating the great potential in the practical application. The satisfactory reusability of the composite catalyst was demonstrated in the recycling test, with the DOX removal efficiency slightly declined from 90.08 to 84.42% after five runs. Based on the generation of reactive oxidative species and the transformation intermediates identified by HPLC-MS, the possible degradation pathways and reaction mechanism of DOX degradation in Mg-Fe-LDH@biochar/PMS system were proposed.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Bing Wang,Carlota Bozal-Ginesta,RuiQing Zhang,Bo Zhou,HaiXia Ma,LinYu Jiao,Long Xu,EnZhou Liu,Chen Wang,Zhuo Li
The development of stable, efficient molecular-inorganic photocatalysts for organic pollutants degradation in wastewater remains a major challenge. Herein, a novel axially substituted supramolecular nanocrystalline subphthalocyanine H 12 SubPcB–OPhCOPh (SubPc-4) was successfully synthesized. By self-assembling supramolecular SubPc-4 on TiO 2 via dimeric concave-ligand π-interaction, an molecular-inorganic Z -scheme photocatalytic system (SubPc-4/TiO 2 ) was prepared exhibiting high photoactivity and stability towards the degradation of tetracycline (TC), methyl orange (MO) and bromophenol blue (BB). The photocatalytic degradation efficiency of TC, MO and BB with SubPc-4/TiO 2 was 96.2 %, 98.0 % and 100 % within 180 min, approximately 3.2, 19.7 and 6.6 times larger than pristine TiO 2 , respectively. The constructed SubPc-4/TiO 2 hybrid kept 88.5 % of its original photocatalytic activity toward TC after five photocatalytic cycles with respect to the first cycle, while bare TiO 2 only kept 23.2 %. We reveal that this high photoactivity and photostability arises from the formation of an effective charge separation Z -scheme. This work demonstrates the potential of the SubPc-4/TiO 2 molecular-inorganic Z -scheme photocatalyst in wastewater treatment.
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CHEMOSPHERE
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2021
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IF 7.086
Ji'an Sun,Lixin Wang,Yuge Wang,Weiyang Lv,Yuyuan Yao
The morphology and specific surface area of layered double hydroxide (LDH) are of great significance for optimizing the application of LDH in sewage treatment . Herein, we present a study of the relation between the catalytic property and the morphology of LDH via activating peroxymonosulfate (PMS) for degradation of organic pollutants. The results demonstrated that LDH nanoscrolls possessed a superior performance for methylene blue (MB) degradation, which achieved almost 100% removal in 40 min and the calculated apparent rate constant was about 2.1, 4.5 and 11.5 times higher than that of LDH nanosheets, Co 2+ and Co 3 O 4 , respectively. According to the results of X-ray photoelectrons spectroscopy (XPS) and electron paramagnetic resonance (EPR), 1 O 2 was confirmed to play a dominant role in the MB degradation, where the redox cycle of Co 3+ /Co 2+ provided the impetus for the reaction. Moreover, the pH and ion tolerance abilities of LDH nanoscrolls in PMS activating process were determined as well. Remarkably, CO 3 2− and H 2 PO 4 − could even promote the generation of •OH and 1 O 2 to facilitate the progress of reaction. Overall, these findings in the study may provide more opportunities in the preparation of high-efficiency catalysts and give insight into the accelerated degradation of refractory contaminants with surrounding anions.
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CHEMOSPHERE
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2021
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IF 7.086
Xinghao Liu,Zhaoguang Yang,Ying Yang,Haipu Li
A novel carbon quantum dots (CQDs) sensitized 2D/2D carbon nitride nanosheets and bismuth tungstate composite (CQD-CNs/BWO) was successfully prepared via the facile hydrothermal method and used for the photocatalytic degradation of norfloxacin (NOR). During 120 min irradiation test, CQD-CNs/BWO exhibited 9 and 1.76 times higher photocatalytic activity than CNs and BWO, respectively. CQDs and constructed 2D/2D structure could not only improve the light harvesting but also promote the generation and separation of electron-holes. The existing inorganic ions in solution (e.g. bicarbonate ions, chlorine ions, and sulfate ions) could inhibit NOR degradation. Based on the electron spin resonance and free radicals inhibition tests, the holes and superoxide radicals rather than hydroxyl radicals were the main reactive species. The intermediates and possible pathways were proposed, and the antibacterial activity of the treated solution after the reaction was evaluated via bacteriostatic tests. The prepared composite material with high photocatalytic activity and stability is potentially effective for the degradation of antibiotics in wastewater.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Xin Liu,Peng Xu,Qi Fu,Runhan Li,Chenxi He,Wenxuan Yao,Lei Wang,Shiqi Xie,Zhiyi Xie,Qiulai He,John C. Crittenden
Zero − valent copper activated peroxymonosulfate (Cu(0)/PMS) system had widely studied for degrading contaminant due to being highly efficient. However, the weak reactivity and easy dismutation of Cu(I) in acid condition restrained its efficiency. In our study, ferric ion (Fe(III)) significantly enhanced Cu(0)/PMS system for acetaminophen degradation and total organic carbon removal. Multiple reactive oxidants including Fe(IV), Cu(III) and hydroxyl radical (•OH) were generated in the Fe(III)/Cu(0)/PMS system. In the Fe(III)/Cu(0)/PMS system, Cu(0) generated Cu(I) by hydrogen corrosion and PMS oxidation, and then Fe(III) reacted with Cu(I) and Cu(0) producing Fe(II). At the same time, PMS reduced Cu(II) to Cu(I), and Cu(I) reacted with oxygen with forming hydrogen peroxide (H 2 O 2 ). Finally, both Cu(I) and Fe(II) induced H 2 O 2 and PMS producing reactive oxidants, and meanwhile H 2 O 2 was formed by the reaction of Fe(IV) and •OH. Thereinto, Fe(IV) and •OH made main contribution on the degradation of acetaminophen, while Fe(IV), Cu(III) and •OH were responsible for orange II degradation. Common water matrix including sulfate ion, nitrate ion and carbonate ion had inapparent impact on acetaminophen degradation, but chloride ion and humic acid limited slightly the degradation of acetaminophen. There had a good degradation of acetaminophen in tap water, lake water and well water with the Fe(III)/Cu(0)/PMS system. Adjusting the final reaction solution to pH 8.0 and subsiding, the discharge of total copper was within the II-level environmental quality standards for surface water in China (1 mg/L). The study might provide a new and promising idea based on Cu(0) activated PMS system for enhanced degradation of contaminants.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Shengnan Huang,Fan Tian,Jiawei Dai,Xuesong Tian,Guangfang Li,Yunling Liu,Zhiquan Chen,Rong Chen
Chlorophenols (CPs) treatment in water is a huge challenge due to its native robustness and harmful chlorinated by-products in degradation. In this work, we developed a specific BiO 2-x with high density Bi-O-Bi-O vacancy via a facile hydrothermal process. Extraordinary CPs removal ability under near infrared (NIR, >700 nm) is achieved over the as-prepared product. The presence of vacancies not only induced strong interactions between CPs and photocatalyst, but also promoted singlet oxygen ( 1 O 2 ) and photogenerated holes (h + ) generation. Furthermore, the generated 1 O 2 is found mainly originating from lattice oxygen release and the superoxide radicals ( O 2 − ) oxidation from BiO 2-x . Such performance could be well-maintained under wide pH range as well as in the presence of different constitutes in water matrix. This work unravels a unique function of BiO 2-x photocatalyst for CPs decomposition and provide a rational design of highly efficient photocatalysts toward optimization of pollutants degradations.
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