SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Hao Zhu,Shunyan Ning,Zengzhiqiang Li,Xinpeng Wang,Toyohisa Fujita,Yuezhou Wei,Xiangbiao Yin
Here, a nano disc-shaped bimetallic organic framework (NbCo-piperazine) was prepared by the solvothermal method for the activation of PMS for the degradation of contaminants. The effects of Nb/Co ratio, synthesis time and temperature on the morphology, structure and performance of the NbCo-piperazine catalyst were characterized by XRD, FT-IR, SEM-EDS and TEM. The optimum conditions for NbCo-PZ to activate PMS degradation of tetracycline were investigated by adjusting the dosage of catalyst, tetracycline concentration, pH and PMS concentration. The catalytic performance of NbCo-PZ in the presence of co-existing anions (Cl − , NO 3 – , HCO 3 2– , H 2 PO 4 − ) was also evaluated. XPS explained that cyclic changes in the valence states of Nb 4+ /Nb 5+ and Co 2+ /Co 3+ accelerated the activation of the PMS degradation process. EPR results showed the presence of free radicals (SO 4 ·− , ·OH and O 2 ·− ) and non-free radicals ( 1 O 2 ) in the degradation process, with free radicals playing a major role in the degradation process. The degradation rate of tetracycline after three cycles was 92.2%. In addition, NbCo-piperazine showed good catalytic performance for other organic pollutants such as methyl blue, tylosin tartrate and tetracycline with the degradation rate of 97.8%, 95.2% and 95.5%, respectively. Moreover, it also has good catalytic properties in various water systems such as river water and sea water.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Desheng Liu,Pan Jiang,Xin Xu,Jiayu Wu,Yaozhong Lu,Xinzhong Wang,Xiaolong Wang,Weimin Liu
Developing high-performance catalytic filter with both high removal efficiency and ultra-high flux, especially under gravity-driven conditions, is of great significance yet still a fundamental challenge in organic wastewater purification. Herein, a high-efficiency gravity-driven catalytic filter, ZIF-67 decorated sugarcane that is denoted as ZIF-67@SC sponge, is successfully constructed by the in-situ growing ZIF-67 nanoparticles inside the channels of biomass sugarcane skeleton. Pretreatment of cellulose fibers with alkali can set the nucleation sites for the ZIF-67 nanocrystals decoration on the sugarcane skeleton, which originates from the ion exchange between Co 2+ and Na + . The effect of the perforated plate structures of sugarcane on fluid obstruction and the widely distributed ZIF-67 nanoparticles can synergistically enhance the contraction between organic pollutants and ZIF-67 nanoparticles. The resultant ZIF-67@SC sponge therefore exhibits the superior removal efficiency up to 86.99 % for methylene blue (MB) in water with the water treatment flux of ∼ 2720 L m -2 h −1 under the activation of peroxymonosulfate (PMS). Importantly, the ZIF-67@SC sponge catalytic filter can be readily regenerated by a simple methanol washing, maintaining the removal efficiency of 82.09 % after even 10 continuous regeneration cycles. Furthermore, the ZIF-67@SC sponge catalytic filter can be facilely engineer as a continuous-flow catalytic reactor like a water purifier for high throughout wastewater purification. It’s believed that relying on the outstanding catalytic performance of metal–organic frameworks (MOFs) and the unique skeletons of sugarcane and other biomass materials, the present outcomes can be promising by extended to the large-scale water remediation.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Yongsong Ma,Kaifa Du,Yifan Guo,Mengyi Tang,Huayi Yin,Xuhui Mao,Dihua Wang
Greenhouse gases carbon dioxide (CO 2 ) can be converted into high value-added carbon materials by molten salt electrolysis. Herein, we employ CO 2 as the inorganic carbon source to prepare a core–shell catalyst (Co@C) by molten salt electrolysis for the activation of peroxymonosulfate (PMS) to degrade diethyl phthalate (DEP). The electrolytic Co@C catalyst presents a high catalytic performance for the degradation of DEP with a high turnover frequency (TOF) value (2.28 min −1 ), a relatively low catalyst dosage (Cat = 50 mg L –1 ), low oxidant concentration (PMS = 0.46 mM), a wide range of pH applicability (pH = 3–9), and low activation energy ( E a = 38.88 kJ mol −1 ). In addition, the Co leaching rate is low (<1 mg L –1 ) in the pH range of 5–11 and the total organic carbon (TOC) removal was reached 78.9% under the catalyst dosage was 50 mg L –1 . The DEP degradation pathways mainly involved ethyl formate elimination, ethoxy abstraction, carboxyl abstraction, decarboxylation, hydroxy abstraction, esterification and ring cleavage of DEP. Further, theoretical calculations confirm that Co nanoparticles (Co NPs) encapsulated with graphitized carbon shell derived from CO 2 reduce the work function (WF) of catalysts, enhance the length of bond O–O ( I O-O ) of PMS molecule, and facilitate the charge transfer from the catalysts to PMS molecule. This work provides a new insight into the utilization of CO 2 served as inorganic carbon sources and the design of heterogeneous catalysts.
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WATER RESEARCH
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2021
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IF 11.236
Jinxi Feng,Tiantian Zhang,Jingxiang Sun,Jinzhu Zhu,Wen Yan,Shuanghong Tian,Ya Xiong
Piezoelectric effect was firstly employed to improve dewatering efficiency of sludge. It was found that the piezoelectric effect could be driven directly by the pressure of pressure filtration process, without any additional energy. This piezo-dewatering process coupled piezoelectric effect with pressure filtration could efficiently remove moisture of sludge. Under 0.6 MPa for 2 h, moisture content (MC) and weight of sludge could be reduced to 63.9% and 3.2 g from 96.7% and 50 g by the piezo-dewatering process with 0.45 g t -BaTiO 3 . This piezo-dewatering efficiency was much higher than that of usual conditioning-pressure filtrations using CaO, FeCl 3 or polyacrylamide (PAM) as the conditioners. And the piezo-dewatering process assisted by PAM could further decrease MC and weight of the sludge to 54.9% and 2.1 g, correspondingly, which complied to the advanced dewatering requirement (MC < 60%). The favorable piezo-dewatering efficiency was contributed to the piezo-catalytic oxidation and the electric role of remnant piezo-field. The finding of this piezo-dewatering mechanism offered an inspiring look at developing the emerging dewatering technology.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Cong Pan,Libin Fu,Fenna Lide,Yaobin Ding,Chengjun Wang,Jia Huang,Shaobin Wang
Reduction of bromate (BrO 3 − ) by various technologies has been extensively investigated, while the fate of oxygen and bromine atoms in BrO 3 − in these processes has been largely ignored. In this study, reduction of BrO 3 − by Fe(II) ions was investigated under various conditions via electron spin resonance (ESR), laser flash photolysis (LFP), probe of phenol and quenching experiments. It was found that reduction of BrO 3 − by Fe(II) ions produced HO•, O 2 • − and reactive bromine species (eg., Br• and Br 2 • − ). HO• and O 2 • − were generated from release of one/two oxygen atoms in BrO 3 − and its reduction intermediates (BrO 2 − and BrO − ) at one time, while Br• and Br 2 • − were generated from activation of hypobromous acid by Fe(II) and reactions of HO• with formed Br − . Due to the formation of these reactive species, the tested ten organic pollutants with diverse structures can be efficiently degraded, which including carbamazepine (CBZ), ibuprofen, phenol, benzoic acid, paracetamol, bisphenol a, 4-chlorophenol, oxcarbazepine, diclofenac and sulfamethoxazole. CBZ degradation intermediates by BrO 3 − /Fe(II) system were specially identified by liquid chromatography (LC)-mass spectrometry (MS), and three pathways of hydroxylation/nitrosylation, ring contraction-amine cleavage and bromination for CBZ degradation were proposed accordingly. This study might shed new fundamental insights to bromate reduction and its implication for transformation of co-existed organic pollutants.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Yunjin Yao,Hongwei Hu,Hongyu Yin,Zhenshan Ma,Zhongming Tao,Yongjie Qiu,Shaobin Wang
FeS 2 -embedded in porous carbon (FeS 2 /C) was prepared by simultaneous sulfidation and carbonization of an iron-based metal–organic framework precursor, and subsequently immobilized in polyvinylidene fluoride membranes (FeS 2 /C@PVDF) for organics removal via peroxymonosulfate (PMS) activation. The composition , structure, and morphology of the FeS 2 /C@PVDF membrane were extensively characterized. Scanning electron microscopy images manifest that the FeS 2 /C nanoparticles with an average diameter of 40 nm are assembled on the external and internal membrane surface. The as-prepared FeS 2 /C@PVDF membrane exhibits excellent performances over a wide pH range of 1.53–9.50, exceeding carbon-free syn -FeS 2 @PVDF. The effective degradation could be improved by inner pyrite FeS 2 cores and thus enhanced the electron transfer between carbon shell and PMS. Electron paramagnetic resonance and quenching experiments elucidated that radical ( HO ∙ , SO 4 ∙ - ) and nonradical ( 1 O 2 ) species were the predominant reactive oxidants. In addition, FeS 2 /C@PVDF exhibited high stability with low Fe leaching (0.377 mg/L) owing to the effective protection of the outer carbon skeleton. Plentiful porosity of PVDF membranes not only affords a controlled size and confined uniform distribution of the immobilized FeS 2 /C nanoparticles, but also enables a persistent exposure of active sites and enhanced mass transfer efficiency. Our findings demonstrate a promise for utilizing the novel FeS 2 /C@PVDF membrane as an efficient catalyst for the environmental cleanup.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Kai Liu,Fangbai Li,Yan Pang,Liping Fang,Rosalie Hocking
The redox process of electron shuttles like cysteine on iron minerals under aerobic conditions may largely determine the fate of arsenic (As) in soils, while the interfacial processes and underlying mechanisms are barely explored. This work systematically investigates the interfacial oxidation processes of As(III) on goethite induced by cysteine. Results show that the addition of cysteine significantly enhances the oxidation efficiency (~ 40%) of As(III) (C 0 : 10 mg/L) by goethite at pH 7 under aerobic conditions, which is 19.5 times of that without cysteine. cysteine induces Fe(III) reduction on the surface of goethite, and the generation absorbed Fe(II) species play an important role in As(III) oxidation. In particular, the further complexation of Fe(II) with cysteine is thermodynamically favorable for electron transfer , leading to an enhanced As(III) oxidation efficiency. The oxidation efficiency of As(III) in the goethite/cysteine system increases by increasing cysteine concentration and decreases by elevating pH conditions. In addition, evidence indicates that •O 2 - radicals account for approximately 80% of total oxidized As(III). Meanwhile, only 16% of As(III) oxidation can be attributed to the formed •OH radicals. This work provides new insight into the role of organic electron shuttling compounds in determining As cycling in soils.
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Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Yue Gao,Fang Yang,Hongxian Jian,Kai Zhen,Peng Zhang,Xuejiao Tang,Zhen Fu,Wei Xu,Cuiping Wang,Hongwen Sun
To explore an effective liquid material for the degradation of polycyclic aromatic hydrocarbons (PAHs), sodium citrate (SC) was selected from four kinds of chelating agents for persulfate (PS) activation by transition metals to degrade pyrene in an aqueous system. PS activated by SC chelated ferrous ion (PS/Fe 2+ /SC) can catalyze pyrene degradation under neutral pH, and when the molar ratio of PS, SC, Fe 2+ and pyrene was 2000/2000/2000/1, the maximum degradation percentage reached 94.4% in 720 min through enhancing the PS consumption and oxidative capacity of the system. Furthermore, the pyrene degradation catalyzed by PS/Fe 2+ /SC was not influenced by pH in the range from 3.0 to 11.0, PS/Fe 2+ /SC system could effectively catalyze the pyrene degradation over a wide pH range. Additionally, the presence of 0.1 M of SO 4 2- and H 2 PO 4 - decreased the pyrene degradation using the PS/Fe 2+ /SC system, while 0.1 M of Cl - and NO 3 - had little effect on the pyrene degradation when PS/Fe 2+ /SC was used under neutral pH. Furthermore, pyrene degradation was attributed to the sulfate and hydroxyl radicals produced from PS/Fe 2+ /SC system, and these radicals were detected with strong signals of DMPO-SO 4 and DMPO-OH through electron paramagnetic resonance (EPR) spectroscopy. Finally, seven pyrene degradation products were identified by gas chromatography-mass spectrometer (GC-MS), and a possible pathway of pyrene degradation was proposed.
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WATER RESEARCH
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2021
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IF 11.236
Meng Li,Ce-Hui Mo,Xuan Luo,Ke-Ying He,Jian-Fang Yan,Qiong Wu,Peng-Fei Yu,Wei Han,Nai-Xian Feng,King Lun YEUNG,Shao-Qi Zhou
Perfluorooctane sulfonate (PFOS), normally present in groundwater and surface water, is an emerging environmental contaminants, but is extremely difficult to be degraded due to high energy of the C-F bond. Here, an electrocoagulation (EC) technique coupled with peroxymonosulfate (PMS) activation was used to deeply degrade PFOS. Results showed that approximately 100% PFOS was removed from the solution in the monopolar serial (MS) mode within 60 min and achieved a high kinetic rate of 0.074 min −1 , which was significantly higher than those of reported studies (Table S3). Energy consumption (2.06 kWh/kg) in the MS mode was significantly lower than that of Al (52.30 kWh/kg) and Zn (213.50 kWh/kg) electrodes, which further confirmed the potential application prospects of EC technique. The quenching experiments, electron spin response (ESR) analysis, and DFT calculations can verify that ·OH was the main radical from the reaction of Fe 2+ –OH reaction site with PMS. In addition, results from fluorine balance and TOC removal also indicated the complete mineralization and degradation of PFOS in the EC process. Quantum chemical calculations can confirm the PFOS degradation mechanism and key active sites for direct electron transfer and radical attack. After five cycle operations of PFOS degradation, the EC process was still effective in degrading PFOS with a removal efficiency above 98%. Thus, this work provided a novel alternative for the high-effective treatment of PFOS from contaminated environmental water bodies.
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CHEMOSPHERE
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2021
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IF 7.086
Xiaoyu Jiao,Congcong He,Huan Yu,Jun He,Chengjun Wang
Polar stratospheric clouds (PSCs), of which the surface is a dynamic liquid water layer and might consist of aqueous HNO 3 and H 2 O 2 , is a well-known key meteorological condition contributing to the ozone hole in the polar stratosphere . PSCs has been considered to provide abundant surface for the heterogeneous reactions causing the formation of the Cl 2 and HOCl, which are further photolyzed into Cl and ClO radicals leading to the ozone destruction. Here we demonstrated that the sunlight drives the massive and stable production of OH radicals in aqueous HNO 3 and its main photo-induced byproduct HNO 2 . We also found that the photo-generated OH radicals in aqueous HNO 3 , HNO 2 and H 2 O 2 have the remarkable capability to react with the dissolved HCl , Cl − and Br − to form halogen radicals. In addition, we observed that the H 2 O 2 can react with dissolved HCl and Br − in darkness to form and release Cl 2 and Br 2 gases, which could further be photolyzed into reactive halogen radicals whenever sunlight is available. All these findings suggest that, except for the well-known heterogeneous reactions, photochemical reactions involving the aqueous HNO 3 and H 2 O 2 on and within PSCs surface might constitute another important halogen activation pathway for ozone destruction. This study may shed deeper insights into the mechanism of halogen radicals resulting in ozone depletion in polar stratosphere.
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Advanced Healthcare Materials
·
2021
·Vol. 11
·期 2
·2101926
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IF 9.933
Wenjie Feng,Wanrui Shi,Shuwei Liu,Huiwen Liu,Yi Liu,Pengfei Ge,Hao Zhang
Most of the antitumor chemotherapeutic drugs execute the therapeutic performance upon eliciting tumor cell apoptosis, which may cause chemoresistance of tumors. Design of novel drugs to eradicate apoptosis-resistant tumors via non-apoptotic cell death pathways is promising for improving the long-term chemotherapeutic efficacy. Herein, a Fe(III)-Shikonin metal-polyphenol-coordinated supramolecular nanomedicine for combined therapy of tumor via ferroptosis and necroptosis is designed. The construction of the nanomedicine based on the coordinated self-assembly between Fe 3+ and Shikonin not only overcomes the shortcomings of Shikonin including its low bioavailability and high toxicity toward normal tissues, but also integrates the theranostics functions of Fe ions. Under the exposure of the high concentration of glutathione (GSH) in tumor cells, the as-prepared nanomedicine will disassemble into Fe 2+ and Shikonin, followed by stimulating the tumor cell death through ferroptosis and necroptosis. In addition, benefiting from the stealth effect of polyethylene glycol (PEG) and the targeting ability of cyclo(Arg-Gly-Asp- d -Phe-Lys) (cRGD) to α v β 3 -integrin, NH 2 -PEG-cRGD-modified nanomedicine exhibits a GSH-responsive therapy toward 4T1 tumor in vivo and self-enhanced longitudinal relaxation (T 1 )-weighted imaging property. Since the self-assembly of natural Shikonin and human body-necessary Fe element is facile and feasible, the work may provide a promising supramolecular nanomedicine for next-generation chemotherapeutic applications.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2021
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IF 9.028
Liying Wu,Zhiqiang Sun,Yufei Zhen,Shishu Zhu,Chen Yang,Jing Lu,Yu Tian,Dan Zhong,Jun Ma
Ubiquitous oxygen vacancies (Vo) existing in metallic compounds can activate peroxymonosulfate (PMS) for water treatment. However, under environmental conditions, especially oxygenated surroundings, the interactions between Vo and PMS as well as the organics degradation mechanism are still ambiguous. In this study, we provide a novel insight into the PMS activation mechanism over Vo-containing Fe–Co layered double hydroxide (LDH). Experimental results show that Vo/PMS is capable of selective degradation of organics via a single-electron-transfer nonradical pathway. Moreover, O2 is firstly demonstrated as the most critical trigger in this system. Mechanistic studies reveal that, with abundant electrons confined in the vacant electron orbitals of Vo, O2 is thermodynamically enabled to capture electrons from Vo to form O2•– under the imprinting effect and start the activation process. Simultaneously, Vo becomes electron-deficient and withdraws the electrons from organics to sustain the electrostatic balance and achieve organics degradation (32% for Bisphenol A without PMS). Different from conventional PMS activation, under the collaboration of kinetics and thermodynamics, PMS is endowed with the ability to donate electrons to Vo as a reductant other than an oxidant to form 1O2. In this case, 1O2 and O2•– act as the indispensable intermediate species to accelerate the circulation of O2 (as high as 14.3 mg/L) in the micro area around Vo, and promote this nano-confinement electron-recycling process with 67% improvement of Bisphenol A degradation. This study provides a brand-new perspective for the nonradical mechanism of PMS activation over Vo-containing metallic compounds in natural environments.
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