CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Le Zhang,Ting Liu,Meng Zhu,Yong Liu
Persulfate (PS)-based advanced oxidation processes (SR-AOPs) is a promising approach for the removal of ammonia nitrogen (NH 3 -N) from wastewater, but it suffered from the low removal efficiency and the excessive oxidation of NH 3 -N to nitrate (NO 3 − ) or nitrite (NO 2 − ) in the absence of in-situ generated chlorine radicals. Therefore, it is still a challenge to improve the efficiency of NH 3 -N removal and the selectivity of NH 3 -N oxidation products towards dinitrogen (N 2 ) by SR-AOPs without chlorine radicals. Herein, a novel photo-assisted activation of SR-AOPs involving sodium silicate (Na 2 SiO 3 ) and sodium sulfite (Na 2 SO 3 ) was developed for NH 3 -N removal from wastewater. In this system, Na 2 SiO 3 was acted as a green buffer to maintain NH 3 -N in the form of un-ionized ammonia (NH 3 ) with strong reducibility, promoting the efficiency of NH 3 -N removal as well as ensuring the neutral effluent by receiving the H + from PS activation. Na 2 SO 3 could inhibit the excessive oxidation of NH 3 -N by regulating the redox potential of the solution and generating hydrated electrons (e aq − ) under light ( hv) irradiation, enhancing the selectivity of NH 3 -N oxidation products towards N 2 . 100 % of NH 3 -N removal efficiency and more than 98 % of N 2 selectivity were obtained after 30 min at the initial pH of 3–9 and the initial NH 3 -N concentration of 30 mg N/L. Based on the quenching experiment, EPR test and probe experiment, the HO and SO 4 − were the main reactive oxygen species (ROS) to be responsible for NH 3 -N oxidation. This study proposed a new approach for treatment of wastewater containing NH 3 -N by SR-AOPs.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Shilong Jiang,Song Cheng,Jiashun Cao,Cailiang Yue,Jianglei Xiong,Cong Jiang,Hongzhan Cai,Jianhua Wu
The removal of trace urea presents a significant challenge in the production of electronic-grade ultra-pure water (UPW). This study proposed a simple strategy to regulate the low-coordination of a single-atom cobalt catalyst (R y Co-CN 0.20 ) for the efficient removal of trace urea via peroxymonosulfate (PMS) activation. The optimal R 0.50 Co-CN 0.20 with low-coordination Co-N 3 sites was constructed by in-situ reduction of NaBH 4 and significantly enhanced the PMS activation. The removal efficiency of trace urea achieved 94 % within 5 mins. The k obs of trace urea degradation in R 0.50 Co-CN 0.20 /PMS system reached 0.4576 min −1 , which was much higher than previous reported systems. Experiments of free radical quenching and electron paramagnetic resonance demonstrated that singlet oxygen species were the dominant free radical. The corresponding steady concentration of singlet oxygen species in the R 0.50 Co-CN 0.20 /PMS system was enhanced to be 16.361 × 10 –6 μM, which was twice of Co-CN 0.20 /PMS. Density functional theory calculations revealed that the optimized electron distribution of the Co center in the Co-N 3 sites processed a higher d band center (−1.08 eV) and richer electron transfer number (0.75 e − ) compared with Co-N 4 sites, hence realizing the stronger PMS activation. Continuous operation verified that R 0.50 Co-CN 0.20 /PMS could maintain the removal rate of trace urea above 80 % after 150 h operation. Moreover, R 0.50 Co-CN 0.20 /PMS in the pilot UPW production process effectively reduced the pollution caused by trace urea and ensured the quality of the terminal UPW (Total organic carbon <1 μg/L). This study provides a new approach for the removal of trace urea through PMS activation by low-coordination single-atom catalysts.
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Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Lei Chen,Jiankun Zhang,Qingxue Li,Yangyang Zhang,Jiajia Huangpu,Jiaqi Shen,Mingye Gu,Jiaxiang Yang
Straw biochar loaded zero-valent iron nanoparticles were prepared by co-precipitation method using agricultural waste straw biochar as a carrier for the removal of p-nitrophenol (PNP) by activated sodium persulfate (PS). The physicochemical properties of BC@nZVI were characterized using SEM, EDS, FTIR, BET, and RAMAN. The effects of PS concentration, catalyst concentration, initial pH, coexisting anions, and different activation systems on the degradation of PNP were investigated. The results showed that the best activation effect was exhibited at pH= 7, BC@nZVI dosage of 2 g/L, and PS concentration of 1 mM, and the removal of 40 mg/L PNP reached 91.7 % in 10 min. The high concentration of PS (4 mM) triggered free radical competition to inhibit the degradation, and the removal rate was only 74.5 % at 1 mM. In addition, bicarbonate ions (0–20 M) had a significant inhibitory effect on this system. Electron spin resonance (ESR) demonstrated that SO 4 ⋅ − and·OH were the major radicals, and SO 4 ⋅ − was preferentially generated. The intermediate products were identified by LC-MS, XRD and XPS characterization, which showed that adsorption and redox were the main degradation mechanisms, with p-benzoquinone was the oxidized product and substances such as 4-heptanone and propionic acid were the reduced products. This study proves that BC@nZVI activated PS is an efficient and excellent means of removing PNP and a good way to reuse agricultural waste.
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ACS Applied Nano Materials
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2023
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IF 5.9
Qian-Qian Li,Fei Wang,Hui-Yuan Bai,Yan Cui,Ming Ma,Yu Zhang
The most effective treatment for acute myeloid leukemia relies on high-dose chemotherapeutic agents. However, this therapy is prone to serious adverse effects due to the lack of targeted selectivity. The CXC chemokine receptor 4 (CXCR4) overexpressed on the surface of acute myeloid leukemia cells is closely associated with poor prognosis and is an important clinical target. In this study, we report the construction of a biomimetic nanomedicine with targeted effects based on the CXCR4/CXC chemokine ligand 12 (CXCL12) biological axis by coating bone marrow stromal cell membranes (CMs) on the surface of hollow mesoporous Prussian blue nanoparticles (HMPB NPs) loaded with daunorubicin (DNR), namely, HMPB(DNR)@CM NPs, which inherit the CXCL12 of mouse bone marrow stromal (MS-5) cells. Due to the inherent CXCL12, HMPB(DNR)@CM NPs exhibit prominent advantages in targeted delivery, which enhances the killing of acute myeloid leukemia cells, and the migration and adhesion of acute myeloid leukemia cells to MS-5 cells are inhibited after treatment with nanocarriers. These CMs biomimicry also endows the nanocarrier with immune evasion as a property. More importantly, PB nanocarriers with reactive oxygen species scavenging activity and slow drug release can effectively alleviate the damage caused by chemotherapeutic drugs to hepatocytes. As a result of this research, the construction of safer and more effective chemotherapy strategies is expected to be facilitated, and the prognosis of acute myeloid leukemia patients is expected to be improved.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Jue-Lin Xiang,Jun-Jie Wang,Zhi-Jing Wu,Bao-Jun Xu,Hai-Sheng Du,Ying Chen,Min Liu,Min-Yong Lee,Wen-Long Wang,Ye Du
Microwave discharge electrodeless lamp (MDEL) is a novel ultraviolet (UV) light source. Synergistic disinfection using UV light emitted by MDEL (MWUV) coupled with ozone (O 3 ) at an ultra-low dose was investigated. Escherichia coli and Bacillus subtilis were deactivated more effectively by MWUV/O 3 than by either MWUV or O 3 alone. MWUV/O 3 treatment using an O 3 concentration of 0.4 mg/L gave an E. coli inactivation rate of 5.52 log. The photoreactivation degree and rate of E. coli were lower after inactivation by MWUV/O 3 treatment than after MWUV treatment alone. The maximum photoreactivation rates after the MWUV/O 3 and MWUV treatments were 2.90% and 16.08%, respectively. MWUV/O 3 disinfection also inhibited dark resurrection of E. coli and gave a maximum dark resurrection rate of 0.0036%. Electron paramagnetic resonance spectroscopy indicated that more hydroxyl radicals were generated during MWUV/O 3 treatment. Scanning electron microscopy and laser confocal scanning microscopy observations indicated that O 3 played a key role in breaking down the cell structure. MWUV/O 3 treatment gave a good disinfection effect on fecal coliform bacteria in actual domestic wastewater. The results indicated that inactivation of bacteria can be more effectively achieved by MWUV treatment with O 3 .
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DALTON TRANSACTIONS
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2023
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IF 4
Si-Man Li,Ji-Lei Wang,Jiu-Lin Zhou,Xin-Ying Xiang,Ya-Ting Yu,Qun Chen,Hua Mei,Yan Xu
It is a major challenge to perform one-pot hydroxylation of benzene to phenol under mild conditions, which replaces the environmentally harmful cumene method. Thus, finding highly efficient heterogeneous catalysts that can be recycled is extremely significant. Herein, a (POM)-based hybrid compound {[FeII(pyim)2(C2H5O)][FeII(pyim)2(H2O)][PMoV2MoVI9VIV3O42]}·H2O (pyim = 2-(2-pyridyl)benzimidazole) (Fe2-PMo11V3) was successfully prepared by hydrothermal synthesis using typical Keggin POMs, iron ions and pyim ligands. Single-crystal diffraction shows that the Fe-pyim unit in Fe2-PMo11V3 forms a stable double-supported skeleton by Fe–O bonding to the polyacid anion. Remarkably, due to the introduction of vanadium, Fe2-PMo11V3 forms a divanadium-capped conformation. Benzene oxidation experiments indicated that Fe2-PMo11V3 can catalyze the benzene hydroxylation reaction to phenol in a mixed solution of acetonitrile and acetic acid containing H2O2 at 60 °C, affording a phenol yield of about 16.2% and a selectivity of about 94%.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Yue Wang,Zhenglong Liu,Pan Huang,Baoliang Lei,Lele Qiao,Tielong Li,Kun-Yi Andrew Lin,Haitao Wang
Transition metal and carbon nanomaterials are well-known for their peroxymonosulfate (PMS) activation capabilities. However, metal-based materials often suffer from ion leakage and poor reusability, while carbon-based materials have limited catalytic efficiency. To overcome these challenges and leverage the strengths of both, we introduce carbon-coated Fe/Mn composites (FeMn@BC), that establish strong interactions between metal components and the carbon substrate. FeMn@BC exhibited exceptional selectivity for 1 O 2 generation via PMS activation. In practical applications, FeMn@BC efficiently degraded tetracycline by activating PMS, achieving 99.1% removal in just 30 min. Importantly, FeMn@BC demonstrated remarkable stability, especially under visible light exposure. XPS analyses revealed strong interactions between FeMn components and the biochar shell, enhancing the electron transfer capacity of FeMn@BC through Fe(III)/Fe(II) and Mn(III)/Mn(II) redox pairs. In-situ attenuated total reflection Fourier-transform infrared (ATR-FTIR) analysis highlighted abundant hydroxyl groups in FeMn@BC as crucial active sites for electron transfer. Quenching experiments and electron paramagnetic resonance (EPR) measurements unveiled that FeMn@BC catalyzed 1 O 2 generation primarily through the disproportionation of O 2 − and energy transfer from oxygen vacancy to O 2 . Our work demonstrates the possibility of simple ball milling of biomass in the presence of iron salts for iron-catalyzed mechanochemical synthesis of biochar-based catalysts. This study not only presents a novel strategy for large-scale biochar-encapsulated transition metal catalyst synthesis but also explores the potential use of agricultural waste for value-added applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Junjie Zhang,Yongjia Hong,Xu Tang,Yong Chen,Wenran Gao,Yuncheng Cai,Ningning Dong,Jiazi Xu,Li Zhang,Quli Fan,Bin Sun
The rational design of active sites in nanocarbons are the long-term pursuit for their practical applications. However, N, as the most potential active site, still encounters the problems of low atom utilization efficiency and stability in practical environmental remediation. Herein, we successfully constructed synergistic active sites consisting of graphitic N, pyridinic N, and thiophene S in heavy S, N co-doped hollow graphene spheres (HSNGS). The HSNGS exhibited exceptional efficiency in degrading tetracycline in real water, with a turnover frequency of 6.24 min −1 , which is among the highest reported. Moreover, tetracycline dissolved in practical water could be continuously and rapidly eliminated by passing through a column filled with HSNGS, maintaining its high performance even after 40 consecutive cycles. In the synergistic active sites, graphitic N and pyridinic N species accepted electrons from peroxymonosulfate, generating singlet oxygen for tetracycline degradation. Simultaneously, thiophene S coordinated with metal ions present in the practical water, synergistically enhancing the degradation of tetracycline. Additionally, the coordinated metal ions provided protection for the synergistic active sites during peroxymonosulfate activation, preventing their oxidation and enabling the continuous and rapid degradation of tetracycline. This work opens up possibilities for the industrial application of nanocarbon materials in environmental remediation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Caixia Chen,Shumei Wang,Fang Han,Xiaoying Zhou,Benxia Li
The reasonable construction of composite membranes with dual functions of rapid adsorption and photo-Fenton-like oxidation degradation holds great significance in the field of wastewater purification. Herein, a poly(vinylidene fluoride)-based composite membrane (denoted as CFT/PVDF) was meticulously prepared through a nonsolvent induced phase separation (NIPS) process with the introduction of cobalt-iron metal–organic framework (CoFe-MOF) and TiO 2 (Degussa P25). The composite membrane exhibited an excellent adsorption ability for removing a variety of organic pollutants from water. With the integration of adsorptive filtration and in situ photo-Fenton-like degradation, the removal efficiency of tetracycline hydrochloride reached up to 92.9% through the CFT/PVDF membrane in one filtration process, and the remarkable performance could be maintained after ten consecutive cycles. Moreover, a group of CFT/PVDF membranes was connected in series to realize the fast and continuous wastewater treatment. The photo-Fenton-like oxidation mechanism and possible degradation pathways were proposed on the basis of active-species detections and degradation intermediates analysis. The toxicological analysis indicated that tetracycline was in situ degraded into less toxic intermediates and even nontoxic substances by the CFT/PVDF composite membrane. This work provides some valuable guidance on the construction of self-cleaning membranes for sustainable wastewater remediation and potential applications.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Yi Ren,Bo Tan,Chao Liu,Chenghan Ji,Bo Lai,Weiming Zhang,Jun Li
In this study, a new Fe(VI)/I(V) system was developed to efficiently strengthen utilization efficiency of generated Fe(IV)/Fe(V). This system could effectively degrade sulfamethoxazole, carbamazepine, bisphenol A and tetracycline within 4 min with k 1 values of 0.60648 min −1 , 1.39726 min −1 , 0.65921 min −1 and 0.93298 min −1 , which were 21–66 times higher than the sum of k 1 values of I(V) alone and Fe(VI) alone systems, and also much better than H 2 O 2 , peroxydisulfate, and peroxymonosulfate strengthened Fe(VI) systems. In addition, Fe(VI)/I(V) exhibited favorable anti-interference, that high-salinity and high organic showed negligible inhibition on pollutant degradation. More importantly, I(V), as an excellent catalyst, hardly decayed during treatment process, which broadens the application field of Fe(VI)/I(V) in different contaminated environmental media and provides a distinguished efficiency for recycling use in contaminated sediment with only consumed Fe(VI) supplement. Fe(VI) consumption in Fe(VI)/I(V) system was not enhanced compared with Fe(VI) alone system, and thus saving agent costs is another significant advantage of Fe(VI)/I(V) system. Above multiple superiorities are still obvious even compared with the systems of other oxidants enhancing Fe(VI) developed in recent years. The main active species was identified as Fe(IV)/Fe(V). The mechanisms of I(V) strengthening Fe(VI) were determined as Fe(IV)/Fe(V) oxidation enhancement, rather than Fe(VI) decay enhancement. Utilization efficiency of Fe(IV)/Fe(V) was improved by oxidation reactivity modulation with I(V) complexes formation, thereby strengthening decontamination significantly. This study proposed a strategy for decontamination in different mediums with high treatment efficiency, high selectivity , satisfactory reusability, and low consumption of agents.
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Advanced Healthcare Materials
·
2023
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IF 10
Mengge Feng,Xuelian Zeng,Quan Lin,Yunxiao Wang,Hongjiang Wei,Shanyi Yang,Guangwei Wang,Xingyu Chen,Mengqin Guo,Xin Yang,Jun Hu,Yangge Du,Yanbing Zhao,Yufeng Zhang,Xiangliang Yang
The postoperative periodontal wound is in a complex physiological environment, the bacteria accumulation, the saliva stimulation, and the food residues retention will aggravate the wound deterioration. Commercial periodontal dressings have been widely used for postoperative periodontal treatment, and there still exists some problems, such as poor biocompatibility, weak adhesion, insufficient antibacterial and anti-inflammatory properties. In this study, a chitosan-gallic acid graft copolymer (CS-GA) is synthesized as a potential periodontal dressing hydrogel. CS-GA possesses high swelling rate, adjustable degradability, self-healing ability, biocompatibility, strong adhesion ability, high mechanical properties and toughness. Furthermore, CS-GA has good scavenging ability for ·OH, O 2 − , and 1 O 2. And CS-GA has good inhibition effect on different bacterial through bacterial membranes damage. CS-GA can stop bleeding in a short time and adsorb erythrocytes to form physical blood clots to enhance the hemostatic performance. In addition, CS-GA can reduce inflammatory factors expressions, increase collagen fibers deposition and neovascularization to promote wounds healing, which makes it as a potential periodontal dressing for postoperative tissue restoration. This article is protected by copyright. All rights reserved
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2023
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IF 6
Hongyu Liu,Qingyun Han,Xueyao Zhang,Huan Zhang,Huicai Wang,Junfu Wei
In this work, N-doped biochar balls NBC 3 800 were prepared from waste biomass corn straw. The biochar balls supported by clay have an obvious spherical structure. Clay can enhance the adsorption capacity of the biochar balls to pollutants by its excellent adsorption property. Thus, the clay can speed up the catalytic reaction by strengthening the adsorption function. The biochar balls NBC 3 800 have the best catalytic performance and the removal rate of NC can reach 100% within 100 min. The electron transfer resistance of NBC 3 800 is only 36 Ω indicating a lower resistance value and higher conductivity to transfer electrons compared with carbon nanotube. Electron paramagnetic resonance (EPR) and electrochemical analysis show that sulfate radical (SO 4 •− ), hydroxyl radical (·OH), singlet oxygen ( 1 O 2 ), and electron transfer are all involved in the reaction. The removal rate of NC can still be maintained at 83.41% after being reused five times. Besides, it can be further improved to 100% by high temperature regeneration at 800 ℃. Most importantly, the biochar balls can be separated from the solution very easily which not only extremely improves the recyclability but also avoids secondary pollution to the water body.
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危险品化学品经营许可证（带存储）