SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Xiaohui Fan,Jinjin Zhao,Cheng Cheng,Yin Xu,Hui Zhang
Efficient and low-cost catalysts are important for contaminant remediation in peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs). In this study, a solid waste, generated by the polyferric chloride coagulation of the phenol-saturated powder activated carbon from an industrial wastewater treatment plant, was used to prepare metal/carbon composites under different pyrolysis temperatures (650–950 °C). The catalyst pyrolyzed at 950 °C (FeAC-950) exhibited the highest reactive activity for PMS activation as demonstrated by a series of electrochemical techniques. Nearly complete BPA elimination can be achieved within 60 min by 0.1 g L –1 FeAC-950 and 0.5 mM PMS. The results of electron paramagnetic resonance (EPR), chemical quenching and open circuit potential (OCPT) experiments demonstrate a combined radical and non-radical oxidation mechanism in the FeAC-950/PMS process and BPA was removed dominantly through radical pathway. Various persistent organic pollutants can be efficiently eliminated in the FeAC-950/PMS system. In addition, the present system showed good tolerance to natural organic matter as well as some common anions such as chloride and nitrate. This study dedicated a simple method to prepare an efficient solid waste-based catalyst in environmental catalysis. The outcomes will not only provide a value-added reuse approach for waste management but also facilitate the FeAC-950 applications in wastewater remediation technologies.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Xiaoyue Wang,Jin Wang,Shanjun Liu,Mengmeng Dou,Boru Gao
The sterilization effect of photocatalysis and biotoxicity of nanomaterial catalysts have attracted high attention. In this study, the novel visible-driven defective carbon nitride (VL/DCN) system exhibits non-photoreactivation, non-toxic superior performance compared with traditional ultraviolet radiation (UV) and UV/titanium dioxide (UV/TiO 2 ). The inactivation of antibiotic-resistant bacteria (ARB) by novel VL/DCN still reached 7 log within 4 h, and the reduction rates of aminoglycoside gene strB and tetracycline gene tetA exceeded 0.8 log and 1.2 log, respectively. Further, the sterilization mechanism and nanotoxicity were contrastively and systematically analyzed among above three systems as following. Firstly, in the VL/DCN system, reactive oxygen species (ROSs) generated from photocatalytic process leads to the destruction of cell membranes, resulting in dissolving out of potassium ion (K + ), protein and cell membrane ATP content. Thus, resistant bacteria were completely inactivated and photoreactivation disappears. In contrast, the UV only acted on bacterial DNA and existed the light resurrection. The UV/TiO 2 strictly dependent on ultraviolet light and can be used in limited scenarios. Secondly, in cell viability analysis by human lung cell line BEAS-2B experiments, the 10% inhibition of cell growth when DCN was 600 mg/L much lower than 28% inhibition of cell growth when TiO 2 was only 200 mg/L. The expression of pro-inflammatory cytokines (( Interleukin, IL) -6), IL-8, IL-1β ) under the effect of DCN was 1.5-fold, 5.7-fold and 3.7-fold lower than TiO 2 , respectively. Meanwhile, DCN induced cells to produce less ROSs, malondialdehyde (MDA), and more superoxide dismutase (SOD). Above results demonstrated that DCN has far lower cytotoxicity than TiO 2 . This study provides theoretical support for the application of photocatalytic sterilization technology and the exploration of the toxicity of nanomaterials. Environmental Implication In this study, the novel visible-driven defective carbon nitride (VL/DCN) system exhibits non-photoreactivation, non-toxic superior performance compared with traditional ultraviolet radiation (UV) and UV/titanium dioxide (UV/TiO 2 ). The VL/DCN exhibited excellent sterilization efficiency and a high rate of reduction of the E. coli resistance gene strB. The inactivation of ARB reached 7 log within 4 h without the occurrence of photoreactivation. The reduction rates of the aminoglycoside gene strB and tetracycline gene tetA exceeded 0.8 log and 1.2 log, respectively. This study provides a valuable theoretical basis for the development of a new sustainable and environmentally friendly visible light catalytic sterilization technologies.
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CATALYSIS LETTERS
·
2023
·
IF 2.8
Su Zheng,Sun Yu,Zhang Qi,Wang Jia,Zhou Wenqi,Zhou Suyin,Zhang Jinlong,Liu Yongdi,Zhou Liang,Lei Juying
Photocatalytic cofactor regeneration often encounters the problem of insufficient stability of reduced nicotinamide adenine dinucleotide hydrogen (NADH) regeneration due to the influence of reactive oxygen species. Here, we obtained Pt-loaded CdS nanorods (CdS NRs) with a one-dimensional (1D) rod-like structure by simple hydrothermal and photo-deposition methods. The yield of NADH improved by 52.54% within 40 min. Superoxide radical (·O 2 − ) had been proven to be the main reactive species that leaded to unwanted oxidation after NADH regeneration. After loading Pt, the formation of Schottky junctions between Pt and CdS NRs promoted the separation and migration of photogenerated carriers, resulting in a tendency of ·O 2 − to shift toward hydroxyl radical (·OH). ·OH produces additional intermediates in the oxidation of NADH compared to ·O 2 − , which inhibits the unwanted oxidation of NADH. Meanwhile, the conduction band position of Pt/CdS shifted positively and the ability to reduce O 2 was weakened, thus the ·O 2 − in the system was reduced, which weakened the oxidation of NADH and significantly improved the stability of NADH regeneration. These studies provide a new reference for applying loaded metal catalysts to the stable regeneration of NADH. Graphical Abstract
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xu Chen,Linfeng Su,Shaojie Zhang,Li Yi,Hao Yang,Yingjie Wen,Jie Sun,Zhiyi Lu
The aluminosilicate-based heterogeneous catalysts hold great promise for industrial catalytic ozonation ; however, the lack of exploration into novel active sites and mechanism studies has impeded their development. In this work, we demonstrate that labile oxygen (O lab ) can be generated in mullite (mullite-O lab ) by the introduction of extra Al-O 4 tetrahedral units. In our experiments, mullite-O lab exhibits excellent performance in terms of catalytic ozone activation, with a degradation rate of 87.4 % within 15 min for nonbiodegradable atrazine, corresponding to a high quasi-first-order rate constant ( k , 0.112 min −1 ), while the degradation constant is close to 0 for mullite without O lab . Operando Raman and density functional theory (DFT) simulations further reveal that O lab activates ozone via a novel surface peroxide pathway to generate surface O lab -O* species with a high oxidizing ability. The mullite-O lab is stable with an average Al 3+ leaching of 0.339 ppm during cycling, meeting the effluent discharge standard of the total Al. Moreover, we achieve the kilogram synthesis of mullite-O lab , which shows promising activity in the catalytic ozonation of acrylic fiber wastewater, with the chemical oxygen demand (COD) and total organic carbon (TOC) removal rates of 46.0 %±4.8 % and 24.9 %±2.8 % for 5 cycles. This work is the first to demonstrate the role of O lab in ozone activation and provides an advanced mullite-O lab catalyst for future nonbiodegradable wastewater treatment .
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Shuang Liu,Hong Wu,Huaili Zheng,Weizhen Zhang,Wei Ding,Hong Li,Chao Liu
Sulfite (S(IV))-based advanced oxidation process has attracted widespread attention due to the generation of strongly oxidizing sulfate radicals (SO 4 •− ) and hydroxyl radicals (HO • ) for contaminants remediation. However, the contaminant degradation by singlet oxygen ( 1 O 2 ) through a nonradical pathway was still unclear in the S(IV) activation system. Herein, a magnetic Fe 3 O 4 /g-C 3 N 4 (MCN) composite was synthesized for the utilization as a visible-light catalyst to activate S(IV) under visible-LED (Vis-LED) for the organic degradation . The incorporation of Fe 3 O 4 in g-C 3 N 4 up-regulated the photocatalytic performance in the S(IV) activation for X-3B degradation, and > 98% of X-3B (20 mg L −1 ) was degraded with the degradation rate constant ( k obs ) of 0.110 min −1 within 30 min. The SO 4 •− and 1 O 2 produced in the MCN/S(IV)/Vis-LED system were identified as the primary reactive species through the quenching experiments and electron spin resonance. Interestingly, the light-induced generation of superoxide radical (O 2 •− ) played a negligible role in the formation of 1 O 2 , and most of 1 O 2 was corroborated to be originated from SO 4 •− besides SO 5 •− , which was rarely reported in other S(IV) activation processes. The catalysts before and after utilization were characterized to further elucidate the mechanisms for the S(IV) activation. There were two possible pathways for the S(IV) activation: the electron transfer from S(IV) to the photo-generated holes and the ligand-to-metal charge-transfer (LMCT) within the surface Fe(III)−S(IV) complexes. Furthermore, the MCN/S(IV)/Vis-LED system was of high resistance to complex water matrixes (pH, inorganic anions, etc.), demonstrating its application perspective in the purification of wastewater containing organic pollutants .
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yuxuan He,Yueming Zhu,Jin Qian,Peifang Wang,Yuhang Zhang,Kailin Xu,Bianhe Lu,Yin Liu,Junwei Shen
The composite catalysts with different morphologies (nanorods, nanocubes, nano-polyhedra and nanosphere) of ceria as loadings are prepared by using spinel as the carrier to investigate the crystal plane effect of ceria on the formation of oxygen vacancies in the catalyst and the activation efficiency of peroxymonosulfate (PMS). The results show that the CeO 2 nanocubic-based composite (CFOC-C) with more (1 0 0) crystal phase has superior catalytic performance in each individual condition, providing rapid activation of PMS and pollutant degradation. Through characterizations, the largest oxygen vacancy concentration is observed on the CFOC-C surface and the strongest reactive oxygen detection signal is obtained in the CFOC-C/PMS system. Moreover, the more active (1 0 0) crystal phase on the CeO 2 surface promotes the electron delocalization at Ce sites, accelerating the adsorption of PMS molecules and the cleavage of O-O bonds, subsequently generating more active species. With levofloxacin as the target, the main degradation intermediates and the degradation pathways in the CFOC-C/PMS system are analyzed in detail. The toxicity estimation results suggest that the toxicity of the degradation products decreases progressively with the reaction.
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WATER RESEARCH
·
2023
·
IF 12.8
Qiang Liu,Xiaojun Niu,Dongqing Zhang,Xingyao Ye,Peibing Tan,Ting Shu,Zhang Lin
Phosphite, an essential component in the biogeochemical phosphorus cycle, may make significant contributions to the bioavailable phosphorus pool as well as water eutrophication. However, to date, the potential impacts of coexisting photochemically active substances on the environmental fate and transformation of phosphite in aquatic environments have been sparsely elucidated. In the present study, the effect of zinc oxide nanoparticles (ZnO NPs), a widely distributed photocatalyst in aquatic environments, on phosphite phototransformation under simulated solar irradiation was systematically investigated. The physicochemical characteristics of the pristine and reacted ZnO NPs were thoroughly characterized. The results showed that the presence of ZnO NPs induced the indirect phototransformation of phosphite to phosphate, and the reaction rate increased with increasing ZnO NPs concentration. Through experiments with quenching and trapping free radicals, it was proved that photogenerated reactive oxygen species (ROS), such as hydroxyl radical (•OH), superoxide anion (O 2 •− ), and singlet oxygen ( 1 O 2 ), made substantial contributions to phosphite phototransformation. In addition, the influencing factors such as initial phosphite concentration, pH, water matrixes (Cl − , F − , Br − , SO 4 2− , NO 3 − , NO 2 − , HCO 3 − , humic acid (HA) and citric acid (CA)) were investigated. The component of generated precipitates after the phosphite phototransformation induced by ZnO NPs was still dominated by ZnO NPs, while the presence of amorphous Zn 3 (PO 4 ) 2 was identified. This work explored ZnO NPs-mediated phosphite phototransformation processes, indicating that nanophotocatalysts released into aquatic environments such as ZnO NPs may function as photosensitizers to play a beneficial role in the transformation of phosphite to phosphate, thereby potentially mitigating the toxicity of phosphite to aquatic organisms while exacerbating eutrophication. The findings of this study provide a novel insight into the comprehensive assessment of the environmental fate, potential ecological risk, and biogeochemical behaviors of phosphite in natural aquatic environments under the condition of combined pollution.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Xin Liu,Peng Xu,Zhuoyu Yang,Pengfei Zhu,Jingwei Ma,Qiulai He,Baolin Hou
Zero-valent copper (Cu(0))-triggered hydrogen peroxide (Cu(0)/H 2 O 2 ) process was used to eliminate and mineralize contamination, while its oxidation efficacy was limited by the reaction of Cu(I) with O 2 . In this study, ferric ion (Fe(III)) was spiked into the Cu(0)/H 2 O 2 (Fe(III)/Cu(0)/H 2 O 2 ) system, and the degradation rate of paracetamol decreased from 24.9% to 95.4%. In the Fe(III)/Cu(0)/H 2 O 2 system, the reaction of Cu(0) and Cu(I) with Fe(III) expedited the conversion from Fe(III) to Fe(II). The reaction of Cu(I) with O 2 was weakened by the competition reaction between Cu(I) and Fe(III), promoting the generation of reactive oxygen species and increasing the utilization of Cu(0). The main reactive oxygen species for pH 4.0 was •OH and Fe(IV) with the contribution rate of •OH and Fe(IV) being 92.3% and 7.7%, but the dominant reactive oxygen species at pH 3.0 was only •OH in the Fe(III)/Cu(0)/H 2 O 2 process. Especially, the contribution of Fe(IV) rose and the contribution of •OH decreased, when the concentrations of 20–80 μmol/L Fe(III), 0.05–0.3 g/L Cu(0) and 50–300 μmol/L H 2 O 2 incremented. In the Fe(III)/Cu(0)/H 2 O 2 process.After we increased the pH of end solution to 7.0/7.5/8.0 and leaching, the total copper in reaction solution was under 6.4/3.3/1.5 μmol/L. In addition, Ni(II) (57.7%), Fe(II) (100%) and Mn(II) (72.4%) obviously enhanced the degradation of paracetamol in the Cu(0)/H 2 O 2 process.
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MOLECULES
·
2023
·Vol. 28
·期 16
·6064
·
IF 4.6
Shuai Xu,Shiyue Zhang,Yutong Li,Jiyang Liu
Visual detection based on nanozymes has great potential for the rapid detection of metabolites in clinical analysis or home-based health management. In this work, iron and nitrogen co-doped carbon dots (Fe,N-CDs) were conveniently synthesized as a nanozyme for the visual detection of glucose (Glu) or cholesterol (Chol). Using inexpensive and readily available precursors, Fe,N-CDs with peroxidase-like activity were conveniently prepared through a simple hydrothermal method. Co-doping of Fe and N atoms enhanced the catalytic activity of the nanozyme. The nanozyme had a low Michaelis constant (Km) of 0.23 mM when hydrogen peroxide (H2O2) was used as the substrate. Free radical trapping experiments revealed that the reactive oxygen species (ROS) generated in the nanozyme-catalyzed process were superoxide anion radicals (•O2−), which can oxidize colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to generate blue oxidation product (ox-TMB) with characteristics absorbance at 652 nm. Based on this mechanism, a colorimetric sensor was constructed to detect H2O2ranging from 0.1 μM to 200 μM with a detection limit (DL) of 75 nM. In the presence of glucose oxidase (Gox) or Chol oxidase (Chox), Glu or Chol was oxidized, respectively, and generated H2O2. Based on this, indirect detection of Glu and Chol was realized with linear detection ranges of 5–160 μM and 2–200 μM and DLs of 2.8 μM and 0.8 μM, respectively. A paper-based visual detection platform was fabricated using Fe,N-CDs as nanozyme ink to prepare testing paper by inkjet printing. Using a smartphone to record the RGB values of the testing paper after the reaction, visual detection of Glu and Chol can be achieved with linear detection ranges of 5–160 μM (DL of 3.3 μM) and 2–200 μM (DL of 1.0 μM), respectively.Keywords:visual detection;colorimetric sensor;nanozyme;carbon dots;metabolite detection
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ACS Nano
·
2023
·
IF 17.1
Wanrui Shi,Wenjie Feng,Siyuan Li,Yanqi Cui,Shuwei Liu,Huan Jiang,Yi Liu,Hao Zhang
Nanovaccine-based immunotherapy has been considered as a major pillar to stimulate the host immune system to recognize and eradicate tumor cells as well as establish a long-term immune memory to prevent tumor relapse and metastasis. However, the weak specificity and low cross-presentation of antigens, as well as the immunosuppressive microenvironments of tumor tissues, are still the major obstacles on exerting the therapeutic performance of tumor nanovaccines sufficiently. Herein, we design and construct cytosine guanine dinucleotide (CpG) oligodeoxynucleotide (ODN)-loaded aluminum hydroxyphosphate nanoparticles covered by Fe-Shikonin metal-phenolic networks (MPNs) (Alum-CpG@Fe-Shikonin NPs) as personalized in situ nanovaccines for antitumor immunity. Upon internalization by tumor cells, the shell of Fe-Shikonin MPNs will disassemble into Fe2+ and Shikonin to elicit the immunogenic cell death of tumor cells through ferroptosis and necroptosis. Then, dying tumor cell-released autologous tumor cell lysates will be absorbed by Alum NPs and codelivered with CpG ODN to professional antigen-presenting cells temporally and spatially to activate multistep cascade antitumor immune responses, including dendritic cell maturation, antigen cross-presentation, natural killer cell and cytotoxic T lymphocyte infiltrations, and tumor-associated macrophage repolarization. Benefiting from the synergistic effects of Alum NPs, CpG ODN, and Fe-Shikonin MPNs, our Alum-CpG@Fe-Shikonin NPs exhibit drastic cytotoxicity and accurate selectivity on eradicating primary tumor, strong abscopal effect on inhibiting distant tumor, and a long-term immune memory effect on preventing tumor metastasis and recurrence. Because our report provides a feasible strategy to in situ make full use of autologous tumor cell lysates, which present an entire spectrum of the patient’s personal epitopes without complicated ex vivo processes, such as extraction, purification, and sequencing, it may promote the development of personalized nanovaccines for antitumor immunity.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Jiayu Zhang,Shan Qiu,Fengxia Deng
The electro-Fenton (EF) process generates H 2 O 2 through the 2e- oxygen reduction reaction (ORR), which is subsequently activated to •OH by iron-based catalysts. To alleviate the potential risk of external Fe-based catalysts, along with metal dissolution in acidic or neutral environments, in this study we employed oxygen-doped carbon nanotubes (OCNT) as a bifunctional, metal-free cathode to establish a metal-free EF process for organic pollutant degradation. The results demonstrate that the metal-free electrode has excellent H 2 O 2 accumulation (12 mg L −1 cm −1 ) and degrades sulfathiazole (STZ) with 97.05 % efficiency in 180 min with an explanation kinetic of 0.0189 min −1 . For the first time, this enhancement came from the dual active site centers in OCNT: Ⅰ) -COOH and defects active sites were responsible for H 2 O 2 production, Ⅱ) then -C O triggered H 2 O 2 into •OH, avoiding the introduction of metal-based catalysts. These findings suggest that the EF system with in situ oxygen-doped cathodes have great potential for treating antibiotic wastewater.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Zhitong Xu,Ye Qi,Yueguang Fang,Peng Tian,Guiling Ning,Junwei Ye
Core-shell Fe 3 O 4 @UiO-66-NH 2 nanospheres with superior photocatalytic activity and photo-Fenton performance were synthesized using a layer-by-layer growth strategy. The synthesis involved the use of FeCl 3 , trisodium citrate, sodium acetate, ZrCl 4 , and 2-aminoterephthalic acid as raw materials, with mercaptoacetic acid serving as a modifier. Fe 3 O 4 @UiO-66-NH 2 demonstrated improved visible-light-driven photocatalytic performance in the oxidation degradation of Rhodamine B (RhB) in the presence of trace amounts of H 2 O 2 under visible light irradiation. The Fe(II)/Fe(III) cycle was accelerated by the transfer of the photogenerated electrons (e-) from UiO-66-NH 2 to Fe 3 O 4 , which in turn encouraged the Fenton reaction to produce hydroxyl radicals (•OH). With only 10 mmol/L H 2 O 2 , the removal rate of RhB approached 94% in 120 min. Furthermore, when exposed to visible light, Fe 3 O 4 @UiO-66-NH 2 exhibited 99% efficacious antibacterial activity against Escherichia coli and Staphylococcus aureus . Overall, the as-prepared Fe 3 O 4 @UiO-66-NH 2 core-shell nanospheres show promise for practical applications as photocatalysts for the degradation of organic pollutants and the inactivation of bacteria in wastewater.
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