PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2023
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IF 7.8
Wei Zhang,Heng Li,Siqiang Xiao,Jianfei Wu,Chuanhu Wang,Xiaobin Liu,Qingbiao Li,Yanmei Zheng
Controllable delivery of persulfate (PS) and the enhancement of oxidative availability of pollutants in in-situ oxidative remediation of low-permeability polycyclic aromatic hydrocarbons (PAHs) contaminated soil are crucial. To tackle the above challenges, the coupling of Tween 80 solubilization enhanced oxidation of phenanthrene (PHE) in low-permeability soil under electrokinetic remediation (EKR) was proposed. Firstly, batch degradation experiments showed that the addition of Tween 80 significantly inhibited the degradation of PHE in soil under thermally activated PS, as the dosage of Tween 80 increased from 0 % to 1 % with the corresponding removal rate declining from 99.19 % to 40.90 %. Accordingly, in-situ electrokinetic delivery of Tween 80 and PS was regulated in further EKR, intending to reduce unproductive consumption. PS was more uniformly delivered to the whole remediation regions from the cathode chamber by electromigration , while Tween 80 was transported into the soil from the anode chamber by electroosmosis , which made Tween 80 solubilization and PS oxidation achieve synergistic effect . And the total removal rate of PHE reached 64.90 % under this strategy, which had increased by 415.90 % and 8.76 %− 130.14 % compared with only EKR or EKR coupling single enhanced technology , respectively. After further thermal activation of transported PS at 50 ℃ by electrical resistance heating, the total removal rate of PHE increased to 71.58 %. EPR spectrum indicated that SO 4 . - and OH . were responsible for the degradation of PHE.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Yaling Wang,Maolin Wang,Qing Xie,Xiyun Cai
We report new activated persulfate systems with cyclodextrin (CD)-coated Fe 3 O 4 @Fe 0 nanoparticles (Fe 3 O 4 @Fe 0 -CD) that are characterized by both highly activating persulfates and rapidly accessing hydrophobic PAHs. Fe 3 O 4 @Fe 0 -β-CD displays chain-like structure of core–shell Fe 3 O 4 @Fe 0 nanoparticles coated with a CD layer (about 5.9 nm). CD coating stabilizes the polycrystalline structure of Fe 3 O 4 @Fe 0 nanoparticles and accelerates mass transfer of PAHs in water, thereby making Fe 3 O 4 @Fe 0 -β-CD intrinsically stable and reactive. Fe 3 O 4 @Fe 0 -β-CD/PS, featured by high yields of highly reactive Fe(IV), had about 30-fold rate constants of naphthalene (Nap) in water as much as Fe 3 O 4 @Fe 0 /PS. Fe 3 O 4 @Fe 0 -β-CD/PS completely removed Nap in water during 13 of total 18 supplementations of Nap and/or PS, whereas Fe 3 O 4 @Fe 0 /PS completely removed Nap only at the first supplementation of Nap. Likewise, Fe 3 O 4 @Fe 0 -β-CD/PS completely removed Nap in simulated groundwater, and degraded four PAHs in soils by >63%. This study may provide a technical basis for the developments of new PS activators to remove recalcitrant hydrophobic contaminants in water and soils.
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Journal of Water Process Engineering
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2023
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IF 7
Lu Qin,Dongqi Wang,Cong Liu,Guodong Chai,Mingliang Fang,Jiake Li,Hui Wang,Zhe Wang,Haiyu Meng,Xing Zheng,Mengbo Huang,Yi Xiao,Yishan Lin,Long Chen
Aqueous pathogenic microorganisms pose a significant risk to public health, but conventional disinfection methods present numerous drawbacks. By employing bactericidal tests, radical quenching experiments, and quantitative toxicogenomic assay, this study aimed to evaluate the effectiveness and associated cellular mechanism of a novel disinfection process combining recyclable copper ferrite (CuFe 2 O 4 ) nanoparticles with sulfite. At the optimal CuFe 2 O 4 (800 mg/L) and sulfite (4 mM) concentrations determined, the CuFe 2 O 4 /sulfite system inactivated 4.65-log (>99.99 %) of Escherichia coli cells at an initial concentration of 10 8 colony-forming units (CFU)/mL in 3 h. Meanwhile, the E. coli cells at the initial concentration of 10 4 − 10 6 CFU/mL were 100 % inactivated within 1–2 h. Cuprous ions (Cu(I)) rather than sulfate radicals (SO 4 •− ) played the dominant role in the inactivation process, by breaking the cell membrane, damaging intracellular components (such as adenosine triphosphate and nicotinamide adenine dinucleotide), and stimulating increased reactive oxygen species production. Correspondingly, the toxicogenomics-based toxicity assessment indicated the induction of oxidative damage to exposed cells as a dominant molecular-level disinfection mechanism of the CuFe 2 O 4 /sulfite system. Moreover, the CuFe 2 O 4 /sulfite system exhibited comparable inactivation efficiency against three other bacterial species, while gram-positive strains ( Staphylococcus aureus and Bacillus subtilis ) were more susceptible to this system than gram-negative ones ( Pseudomonas aeruginosa and E. coli ). The magnetic recyclable CuFe 2 O 4 /sulfite system is a promising water disinfection method owing to its efficacy, convenience, and environmental sustainability.
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CHEMOSPHERE
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2023
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IF 8.8
Wei Zhang,Wenjie Wu,Jianfei Wu,Xiaobin Liu,Jian Tian,Heng Li,Qingbiao Li,Yanmei Zheng
Although advanced oxidation processes (AOPs) based on persulfate (PS) is an attractive approach for repairing polycyclic aromatic hydrocarbons (PAHs) contaminated soils, limited oxidizability of PAHs and efficient in-situ activation of PS hinder its practical applications. In this study, we comprehensively examined the contributions of five representative surfactants on the oxidative remediation of PAHs-contaminated soil in terms of degradation kinetics of the pollutants, and further proposed an innovative coupling strategy of surfactant-enhanced thermally activated PS remediating PAHs-contaminated soil. The results showed that the degradation process of PAHs in soil was significantly facilitated only via adding sodium dodecyl benzenesulfonate (SDBS) and fitted the pseudo-first-order kinetic pattern. The removal of phenanthrene (PHE) reached 98.56% at 50 mM PS, 50 °C, 5 g L −1 SDBS and 48 h reaction time, accompanying an increase of 25% in reaction rate constant from 0.0572 h −1 (without SDBS) to 0.0715 h −1 . More importantly, SDBS-enhanced thermally activated PS degrading PAHs with higher benzene rings were more effective as the reaction rate constants of pyrene (PYR) and benzo(a)anthracene (BaA) were significantly increased by 49.40% and 56.86%. Additionally, only appropriate dosages (5–10 g L −1 ) of SDBS facilitated the oxidative degradation of PHE, as well as the aging time of contaminant-soil contact slowed down the enhancement of oxidative degradation of PHE by SDBS. Scavenger experiments demonstrated that SO 4 ·- and 1 O 2 were the dominant reactive oxygen species . Finally, a possible oxidative degradation pathway of PHE was proposed, and the toxicity of derived intermediates got alleviation by the assessment using the Toxicity Estimation Software Tool . This investigation was promising for in situ scale-up remediation of PAHs-contaminated soil.
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CHEMOSPHERE
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2023
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IF 8.8
Yaxiong Zeng,Qizheng Zhuo,Liyan Dai,Baohong Guan
The molecular nest structured catalysts have demonstrated better performance than the traditional supported catalysts. However, they have not been tried in antibiotics or other organic pollutants removal from water by advanced oxidation processes (AOPs). Here we synthesized Mn anchored zeolite molecular nest (Mn@ZN) for the catalytic ozonation of cephalexin (CLX), which is the widely used antibiotic and also a refractory pollutant in water. The ozonation catalyzed by Mn@ZN achieves 97% of CLX degradation in only 2 min and a reaction rate constant of 0.2454 L·mg −1 ·s −1 , which is 79.2 times higher than that of the non-catalytic ozonation. Even after ten cycles, the 0.46Mn@ZN/O 3 still achieves a CLX degradation efficiency higher than 88% in 2 min, presenting an excellent stability. Mn ions stabilized by the molecular nests facilitate Lewis acid sites and oxygen vacancies, providing active sites for O 3 sorption and decomposition into ·O 2− and 1 O 2 through electrons transfer for the radical reaction with CLX. DFT calculation indicates that both the oxygen vacancy formation energy and the O 3 adsorption energy of Mn@ZN are reduced by the Mn species introduction. This study finds a fascinating catalyst of Mn@ZN for the catalytic ozonation of antibiotics, and also a smart design strategy for zeolite confined metals catalysts for water treatment .
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INORGANIC CHEMISTRY
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2023
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IF 4.6
Xuan Jiang,Zhaodong Nan
Multiple oxidation states of first-row transition-metal cations were always doped in g-C3N4 to enhance the catalytic activity by the synergistic action between the cations in the Fenton-like reaction. It remains a challenge for the synergistic mechanism when the stable electronic centrifugation (3d10) of Zn2+ was used. In this work, Zn2+ was facilely introduced in Fe-doped g-C3N4 (named xFe/yZn-CN). Compared with Fe-CN, the rate constant of the tetracycline hydrochloride (TC) degradation increased from 0.0505 to 0.0662 min–1 for 4Fe/1Zn-CN. The catalytic performance was more outstanding than those of similar catalysts reported. The catalytic mechanism was proposed. With the introduction of Zn2+ in 4Fe/1Zn-CN, the atomic percent of Fe (Fe2+ and Fe3+) and the molar ratio of Fe2+ to Fe3+ at the catalyst’s surface increased, where Fe2+ and Fe3+ were the active sites for adsorption and degradation. In addition, the band gap of 4Fe/1Zn-CN decreased, leading to enhanced electron transfer and conversion from Fe3+ to Fe2+. These changes resulted in the excellent catalytic performance of 4Fe/1Zn-CN. Radicals •OH, •O2–, and 1O2 formed in the reaction and took different actions under various pH values. 4Fe/1Zn-CN exhibited excellent stability after five cycles under the same conditions. These results may give a strategy for synthesizing Fenton-like catalysts.
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Advanced Healthcare Materials
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2023
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IF 10
Yi Lu,Xinni Pan,Cheng Cao,Shanshan Fan,Haisong Tan,Shengsheng Cui,Yanlei Liu,Daxiang Cui
As one of the most widely used drugs, acetaminophen, is the leading cause of acute liver injury. In addition, acetaminophen-induced liver injury (AILI) has a strong relationship with the overproduced reactive oxygen species, which can be effectively eliminated by nanozymes. To address these challenges, mesoporous PdPt@MnO 2 nanoprobes (PPM NPs) mimicking peroxide, catalase, and superoxide dismutase-like properties are synthesized. They demonstrate nontoxicity, high colloidal stability, and exceptional reactive oxygen species (ROS)-scavenging ability. By scavenging excessive ROS, decreasing inflammatory cytokines, and inhibiting the recruitment and activation of monocyte/macrophage cells and neutrophils, the pathology mechanism of PPM NPs in AILI is confirmed. Moreover, PPM NPs’ therapeutic effect and good biocompatibility may facilitate the clinical treatment of AILI.
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ENVIRONMENTAL RESEARCH
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2023
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IF 8.3
Jiajun Liu,Xionghao Zhang,Junda Li,Yi Feng,Li Feng,Shuai Han,Tingyu Pan,Taiheng Zhang,Shenyu Wu,Zijie Ke,Bingzhi Liu,Huaili Zheng
In this study, an advanced oxidation process with E/Ce(IV) synergistic PMS (E/Ce(IV)/PMS) was established for the efficient removal of Reactive Blue 19 (RB19). The catalytic oxidation performance of different coupling systems was examined and the synergistic effect of E/Ce(IV) with PMS in the system was substantiated. The oxidative removal of RB19 in E/Ce(IV)/PMS was excellent, achieving a removal efficiency of 94.47% and a reasonable power consumption (EE/O value was 3.27 kWh·m −3 ). The effect of pH, current density, Ce(IV) concentration, PMS concentration, initial RB19 concentration and water matrix on the removal efficiency of RB19 were explored. Additionally, quenching and EPR experiments showed that the solution contains different radicals such as SO 4 ·− , HO∙ and 1 O 2 , where 1 O 2 and SO 4 ·− played key roles, but HO∙ just acted a weaker role. Ce ion trapping experiment confirmed that Ce(IV) was involved in the reaction process and played a major role (29.91%). RB19 was subject to three possible degradation pathways, and the intermediate products displayed well biochemical properties. To conclude, the degradation mechanism of RB19 was explored and discussed. In the presence of current, E/Ce(IV)/PMS performed a rapid Ce(IV)/Ce(III) cycle, continuously generating strong catalytic oxidation Ce(IV), The reactive radicals derived from the decomposition of PMS, in conjunction with Ce(IV) and direct electro-oxidation, efficiently destroyed the molecular structure of RB19 and showed an efficient removal rate.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Wei Chen,Xinning Dai,Zhujun Liu,Bin Du,Xinyu Zheng,Dandan Ma,Xianbin Huang
Periodate-based advanced oxidation processes (PI-AOPs) exhibited a promising future for the reduction of emerging refractory organic pollutants . However, the underlying mechanism and the sulfuretted effect of sulfide-modified metal silicate materials for PI activation were still unclear. In this study, sulfide-modified metal silicates (S-CoSi) were first synthesized and applied in the PI-AOPs system. Different from traditional metal silicate materials, sulfurization improved the catalytic performance. The enhanced degradation performance was from the increase in specific surface area and charge transfer efficiency, which derived from the sulfurization in metal silicate. DFT calculations revealed that the enhanced charge densities of Co-S bonds promoted the existence of Co (Ⅱ), which was more conducive to PI activation. Experimental and calculation results further demonstrated that Co was the active site in S-CoSi, and sulfur species strengthened the radical pathway by assisting Co (Ⅱ) regeneration (electron transfer from S to Co) rather than participating in the PI activation. Moreover, sulfurization promoted the generation of 1 O 2 (non-radical pathway) by increasing oxygen vacancy in the metal silicate. This study provided new insights into the effect of sulfurization on the radical and non-radical pathways in the metal silicates PI system.
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Journal of Cleaner Production
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2023
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IF 11.1
Zheng Fang,Zifeng Lin,Ping Chen,Mengying Feng,Haijin Liu,Zhenjun Xiao,Zili Lin,Dagaung Li,Dezhu Liu,Yudan Zhang,Wenying Lv,Guoguang Liu
Advanced oxidation processes (AOPs) are highly efficient for the removal of antibiotics from water. The activation of hydrogen peroxide (H 2 O 2 ) by ultraviolet (UV) has garnered increasing attention. This study describes the enhanced photochemical degradation of emerging contaminants in water using a UV-activated calcium peroxide (UV/CaO 2 ) system, wherein CaO 2 can gently produce H 2 O 2 when exposed to UV light . The UV/CaO 2 system can expeditiously and efficiently eradicate ciprofloxacin (CIP), in which hydroxyl radicals (•OH) and superoxide anions (O 2 •- ) played critical roles. The superlative rate constant was 0.024 min −1 at an optimal dosage of 0.1 g L −1 , which was a 16-fold increase over the rate of pure UV photolysis. The UV/CaO 2 system had an excellent defluorination capacity (80% within 60 min). Further, this technology was intensely evaluated over a wide range of pH for the removal of CIP, including H 2 O 2 yields, defluorination rates, as well as correlations with the reactive species generated during the reactions for numerical analysis. The UV/CaO 2 system had an excellent anti-interference capacity over a wide pH range. Three major degradation pathways were proposed for the degradation of CIP, together with predictions of the physiological toxicity of these transformation intermediates. This study provides strong technical support for the promotion of this UV/CaO 2 water treatment platform, as well as the decontamination and defluorination of water matrixes contaminated with fluoroquinolones.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Xin Liu,Peng Xu,Zhuoyu Yang,Pengfei Zhu,Baolin Hou
Zero-valent copper/air process was studied in degrading contaminants owing to in-site generation of hydrogen peroxide and reactive oxygen species, while its oxidation efficacy was restrained by the dismutation of cuprous ion. In this study, when the dosages of paracetamol, ferric ion, chloride ion and zero-valent copper were respectively 10 μM, 40 μM, 2 mM and 0.2 g/L at pH 3.0, the paracetamol elimination was greatly enhanced and increased from 9.2% to 76.5% within 30 min with adding both ferric ion and chloride ion in the zero-valent copper/air process. Hydroxyl radical and reactive chlorine species were identified as the dominant reactive oxygen species, and the contribution rates of hydroxyl radical and reactive chlorine species to eliminating paracetamol were respectively 68.2% and 28.9%. In the proposed system, zero-valent copper and cuprous ion expedited the ferric/ferrous circulation, conducing to the production of reactive oxygen species. Moreover, chloride ion coupled with cuprous ion producing the cuprous chloride complexes, and chloride ion contributed to the comproportionation between zero-valent copper with cupric ion to form cuprous chloride, receding the dismutation of cuprous ion and contributing to the formation of hydrogen peroxide and reactive oxygen species. When zero-valent copper reused for three times in the proposed system, the degradation of paracetamol reached 62%. After we increased the end pH to > 7.0 and leaching, the total copper of reaction solution was under 0.85 mg/L and the acute toxicity had no insignificant increase for discharge water. The study provided a new idea to enhance zero-valent copper/air system for the purification of pollutants.
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JOURNAL OF CONTROLLED RELEASE
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2023
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IF 10.8
Mengsi Zhang,Lu Wang,Hao Jin,Nan Zhao,Yi Liu,Shijie Lan,Shuwei Liu,Hao Zhang
Metal-phenolic networks (MPNs) have been conventionally formed by the coordination of metal ions and polyphenols, which can responsively release metal ions and polyphenols under the trigger of tumor microenvironment (TME), showing high potential in the field of antitumor. However, MPNs are mainly limited to multi-valency polyphenols, and the unavailability of single valency polyphenols greatly hinders their applications even though they have excellent antitumor activity . Herein, we demonstrate a FeOOH assisted preparation method for MPNs antitumor reagent by introducing the complexes of Fe 3+ , H 2 O and polyphenol (Fe(H 2 O) x -polyphenol y ) in the preparation process, which overcomes the shortage of single valency polyphenols. Taking apigenin (Ap) as an example, Fe(H 2 O) x -Ap y complexes are foremost formed, in which the Fe(H 2 O) x is capable of hydrolyzing to generate FeOOH, thus producing Fe 3+ -Ap networks-coated FeOOH nanoparticles ( [email protected] NPs). Under the stimulation of the TME, [email protected] NPs could release Fe 2+ and Ap, realizing ferroptosis and apoptosis for tumor combination therapy. In addition, FeOOH can shorten transverse relaxation time, acting as a T 2 -weighted magnetic resonance imaging contrast agent . The current efforts provide an alternative strategy for constructing MPNs by exploiting single valency polyphenols, which strengthens the potential of MPNs in antitumor applications.
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