SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Xindan Fan,Qintie Lin,Kehuan Xu,Junli Zheng,Jian Sun,Hengyi Fu,Yuxin Liu,Yongjie Ma,Jin He
Considering that high concentrations of ciprofloxacin (CIP) are generally ecotoxic and persistent in water bodies, the refractory degradability has not been addressed in depth. In this study, an N-doped modified graphitized iron-based carbon nanomaterial (0.8 N@FeCS) was prepared by hydrothermal synthesis for the rapid degradation of ciprofloxacin by activated peroxydisulfate. More importantly, the N-doped nitrogen configuration in the iron-based carbon material is pyridine nitrogen, pyrrole nitrogen and graphite nitrogen. The nitrogen modification imparts a new twist to the CIP degradation system: a shift from a common free radical reaction to a nonradical process ( 1 O 2 and electron transfer pathways). The degradation intermediates were identified by LC-MS analysis and density functional theory (DFT), it is suggested that the possible CIP degradation pathway. In conclusion, the process of catalytic activation results in removal of CIP, and this study provides a new perspective for the removal of antibiotics from aqueous solutions.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Yujing Tan,Kaiwen Chen,Jianyi Zhu,Fengze Sun,Hui Peng,Tianyi Zhan,Jianxiong Lyu
Metal organic frameworks hold great promise as heterogeneous catalysts in sulfate radical (SO 4 ∙- ) based advanced oxidation. However, the aggregation of powdered MOF crystals and the complicated recovery procedure largely hinder their large-scale practical applications. It is important to develop eco-friendly and adaptable substrate-immobilized metal organic frameworks. Based on the hierarchical pore structure of the rattan, gravity-driven metal organic frameworks loaded rattan-based catalytic filter was designed to degrade organic pollutants by activating PMS at high liquid fluxes. Inspired by the water transportation of rattan, ZIF-67 was in-situ grown uniformly on the rattan channels inner surface using the continuous flow method. The intrinsically aligned microchannels in the vascular bundles of rattan acted as reaction compartments for the immobilization and stabilization of ZIF-67. Furthermore, the rattan-based catalytic filter exhibited excellent gravity-driven catalytic activity (up to 100 % treatment efficiency for a water flux of 10173.6 L·m −2 ·h −1 ), recyclability, and stability of organic pollutant degradation. After ten cycles, the TOC removal of ZIF-67@rattan was 69.34 %, maintaining a stable mineralisation capacity for pollutants. The inhibitory effect of the micro-channel promoted the interaction between active groups and contaminants, increasing the degradation efficiency and improving the stability of the composite. The design of a gravity-driven rattan-based catalytic filter for wastewater treatment provides an effective strategy for developing renewable and continuous catalytic systems.
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Food Science and Human Wellness
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2023
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IF 7
Jie Ding,Chunyan Zhu,Pengfei Jiang,Libo Qi,Na Sun,Songyi Lin
Enzymatic hydrolysis, isolation, and purification might make a great deal of difference in antioxidant activity and antigenicity of peptide components. This study aimed to isolate and purify antioxidant peptide components from Antarctic krill and evaluate their allergenicity of them. Electron paramagnetic resonance (EPR) spectroscopy results indicated 3 10 kDa Antarctic krill hydrolysates (AKHs) had higher DPPH and · OH radical scavenging rates. And the second component (N2-2) purified 3 10 kDa hydrolysate showed better ability to scavenge DPPH and · OH radicals ( P < 0.05), which were (47.43 ± 2.18)% and (34.33 ± 1.25)%, respectively. Additionally, indirect-ELISA results revealed that N2-1 had a weaker ability to bind specific IgE and that N2-2 had a lower binding capability to specific IgG1 ( P < 0.05). And N2-2 had a higher EC 50 value of (5.29 ± 0.95) ng/mL ( P < 0.05) in cell degranulation assay, which was about 13.80 times that of Antarctic krill. Therefore, N2-2 might be the potential source of the antioxidant peptides with lower allergenicity.
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ACS ES&T Water
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2023
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IF 5.3
Shaopeng Zhang,Bingnan Song,Runhua Wang,Zhengshuo Zhan,Michel Saakes,Renata D. van der Weijden,Cees J. N. Buisman,Yang Lei
Hypophosphite (P(I)) is ubiquitous in some waste streams. It may contribute to the eutrophication of water bodies, yet conventional methods are ineffective in treating P(I)-laden wastewater. Here, we propose a novel CaO2/ultraviolet (UV) system that can simultaneously remove P(I) and recover Ca-phosphate. This system lies in the simultaneous release of OH–, Ca2+, and H2O2, with the last being activated and producing reactive oxygen species (ROS) under UV irradiation. Subsequently, the generated ROS converts P(I) to phosphite and phosphate, forming Ca-phosphate with the released Ca2+ at pH 11.0. Beyond activating H2O2, UV light also promotes the dissolution of CaO2 powders. The system removes 97.0% of 1.0 mM P(I) in 6 h with dosing 2.0 mM CaO2. The presence of 5.0 mM HCO3– drops P(I) removal from 97.0 to 14.1% by competing with P(V) toward Ca2+. Nitrate and humic acid show similar effects by adsorbing UV light or quenching ROS. However, we may overcome the adverse effects with an enhanced CaO2 dose. For example, with 10 mM CaO2, the CaO2/UV system removed more than 78% of non-ortho P from actual electroless rinse water. These results confirmed that CaO2/UV is an exciting all-in-one system for treating P(I)-laden wastewater and recovering valuable P products.
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CHEMOSPHERE
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2023
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IF 8.8
Jie Li,Hua Yin,Haoyu Luo,Yingchao Li,Xufa Rong,Zhi Dang
Polychlorinated biphenyls (PCBs) degradation by peroxymonosulfate (PMS) activation through •OH and SO 4 •– radical oxidation process was the effective technology in the last decades; however, there were few research focusing on removing PCBs by O 2 •– and 1 O 2 induced by PMS activation. In this work, 90.86% of 2,4,4-trichlorodiphenyl (PCB 28) was degraded by 0.3 g/L Fe 3 C@Fe-800 activated 0.5 mM PMS system under the synergistic action of O 2 •– and 1 O 2 . The structures of Fe 3 C@Fe-800 were identified by Scanning electron microscope (SEM), High resolution-transmission electron microscopy (HR-TEM), X-ray photoelectron spectroscopy (XPS), Brunauer-Emmett-Teller (BET), Raman spectra and Fourier transform infrared (FT-IR) spectra. Electron paramagnetic resonance (EPR) measurements and quenching tests verified that O 2 •– and 1 O 2 were the primary reactive species in Fe 3 C@Fe-800/PMS/PCB 28 ternary reaction system. Density functional theory (DFT), Linear sweep voltammetry (LSV), and chronoamperometry test revealed that electron-deficient Fe atoms on Fe 3 C were the main active sites in Fe 3 C@Fe-800 for PMS activation to generate 1 O 2 . Unlike the reported •OH and SO 4 •– mediated degradation induced by the iron-based catalyst, both O 2 •– and 1 O 2 contributed to PCB 28 degradation： nucleophilic dichlorination reaction by O 2 •- and then ring-open oxidation process by 1 O 2 . Fe 3 C@Fe-800/PMS system had excellent catalytic performance under different reaction conditions and possessed desirable inorganic salt and natural organic matter resistance. This work elucidated the important role of Fe 3 C in PMS activation to generate O 2 •- and 1 O 2 for PCB 28 decontamination by nonradical way and provided a clue to design rationally catalysts in polychlorinated biphenyl pollution remediation.
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ACS Applied Materials & Interfaces
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2023
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IF 9.5
Chu Dai,Ziyang Sheng,Xike Tian,Yulun Nie
In this work, a novel strategy for Fenton activity improvement of Cu2X was reported, in which the local electron density of Cu sites was regulated via manipulation of simple chalcogen elements (O, S, and Se). Among them, Cu2Se catalysts show excellent catalytic activity to activate H2O2 for the complete removal of ofloxacin (10 mg/L) at an initial pH of 6.5 within 120 min. Radical scavenger experiments and electron spin resonance spectroscopy confirm that •OH radicals are the primary oxygen reactive species to drive ofloxacin degradation. In addition, density functional theory calculations further proved that electrons would migrate from X and accumulate on Cu active sites in the order Se > S > O. Compared with Cu2O and Cu2S, the highly concentrated electron density of Cu atoms in Cu2Se not only decreased the activation energy of the Fenton-like reaction but also boosted the Cu2+/Cu+ cycle with the generation of more •OH radicals (18–66 μm) and the maintenance of high stability of catalysts, leading to excellent catalytic activity and application potential. We believe this work will lay the foundation for designing excellent Fenton catalysts for practical applications since developing a heterogeneous Fenton system with the highest oxidation efficiency has always been the long-term goal in this field.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Xiaoxiang Cheng,Jinchuan Lian,Bin Liu,Xuewu Zhu,Yan Jin,Lijie Zhang,Fengxun Tan,Daoji Wu,Heng Liang
To alleviate severe algal-source membrane fouling in the ultrafiltration (UF) process, calcium sulfite (CaSO 3 ) integrated with ferrate (Fe(VI)) was proposed. With the integrated pre-treatment, the maximum removal rate of algae cells was improved to 91.19 %, and numerous larger flocs with great settleability were generated. The fluorescent organic components were effectively eliminated, as well as the dissolved organic matter decreased by 38.20 %. During the Fe(VI)/CaSO 3 process, oxidation played a fateful role in fouling alleviation and promoted the in-situ coagulation efficiency. Compared with single Fe(VI) treatment, the oxidation capacity was strengthened through the formation of a series of reactive intermediates (involving Fe(V), Fe(IV), SO 3 •− , SO 5 •− , SO 4 •− and • OH), which were easy to be quenched by the cell-coated extracellular organic matter. Moreover, the consumption of all the oxidants was also remarkably accelerated, thereby the cell integrity was well-kept, and the intercellular organic matter (IOM) was not released. The IOM which already existed in water could also be eliminated, as well as the effluent safety was well guaranteed. During UF, the terminal J/J 0 was elevated to 0.87 at most from 0.10, and the fouling resistances were strikingly reduced. The algal foulants deposition was effectively decreased, and the contact angle of the fouled membrane was closer to the virgin membrane. The dominant fouling mechanism was also converted to intermediate and standard blocking without forming the cake layer.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Minghao Xu,Jiaojiao Yang,Bin Lu,Rufen Chen,Sen Wang,Hui Liu
In this study, the NiCo 4 -LDH with abundant surface oxygen vacancies (SOVs) was synthesized by a simple solvent thermal method, and was used to activate peroxymonosulfate (PMS) through heterogenous catalysis for ciprofloxacin (CIP) degradation. The OV-rich NiCo 4 -LDH/PMS system exhibited excellent CIP removal efficiency and rapid kinetics, as 95.0 % of the CIP was degraded within 10 min and the COD removal rate was 71.2 %. SO 4 •− , • OH, O 2 •− and 1 O 2 were involved in the degradation of CIP, with O 2 •− contributing the most, followed by SO 4 •− , • OH and 1 O 2 . Ethanol, as solvent, could modulate the intrinsic electron properties and produce abundant OVs on the surface of NiCo 4 -LDH, which enhanced the generation of O 2 •− . This study shed new light on the skillful design and application of heterogeneous catalysts for environmental remediation.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Long Cheng,Jiale Bai,Mingyu Wei,Shuaiqi Zhao,Aihua Xu,Xiaoxia Li
Transition metal oxides and carbon can activate peroxymonosulfate (PMS) to decompose organic contaminants. The combination of two materials can facilitate the adsorption of oxidants and pollutants on the catalyst and improve electron transfer efficiency. In this study, carbon nanoparticles-MnO 2 composites (IC-MnO 2 ) were synthesized by coating carbon ink on α-MnO 2 and applied in PMS activation for acid orange 7 (AO7) degradation. The results showed that carbon nanoparticles were uniformly loaded on the α-MnO 2 surface. Complete degradation of AO7 (20 mg/L) can be achieved in 15 min in the IC-MnO 2 /PMS system with a first-order kinetic rate constant of 0.22 min −1 . Electrochemical analysis , quenching experiments, electron paramagnetic resonance , PMS decomposition, and removal of various contaminants demonstrated that AO7 could be efficiently degraded via a direct electron transfer pathway. A galvanic oxidation system containing the salt bridge and two separate cells was further established to confirm the electron transfer mechanism of the catalytic system. The study expands MnO 2 applications by compositing nanocarbon materials in advanced oxidation processes and sheds light on the direct electron transfer mechanism.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Lu Yang,Zhao Wang,HaiJiang Gong,Shili Gai,RuiFang Shen
Chemodynamic therapy (CDT), an emerging oncology treatment, has received considerable attention owing to its high selectivity, less aggressiveness, and endogenous stimulation. However, the complex intra-tumor environment limits the therapeutic effect. In this study, Cu + was directly doped into the structure of the UiO-66 matrix using an in situ one-pot oil bath method. The as-formed UiO-66/Cu possessed a large surface area, making it feasible to modify folic acid (FA) and carry more chemotherapeutic agents like tirapazamine (TPZ), thus forming UiO-66/Cu-FA-TPZ nanoplatforms. For CDT, the nanoplatform catalyzed the cyclic generation of the highly oxidizing hydroxyl radical (·OH) from H 2 O 2 . Particularly, low-frequency ultrasound enhanced the curative effect. Notably, in a tumor, a severe hypoxic environment and ultrasound can activate more TPZ for safe and efficient chemotherapy, achieving synergistic and hypoxia-activated tumor treatment with a low risk of side effects. Moreover, the nanoplatform exhibits computed tomography imaging functions for combined diagnosis and treatment. Our designed nanoplatform overcomes the dilemma of insufficient efficacy from conventional therapy attributed to a hypoxic environment, expecting to guide the design of future treatment regimens for hypoxic tumors.
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WATER RESEARCH
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2022
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IF 13.4
Chaozhi Kuang,Guoshen Zeng,Yangjian Zhou,Yaoyao Wu,Dexuan Li,Yingfei Wang,Chuanhao Li
Conventional electrocatalytic degradation of pollutants involves either cathodic reduction or anodic oxidation process, which caused the low energy utilization efficiency. In this study, we successfully couple the anodic activation of sulfates with the cathodic H 2 O 2 production/activation to boost the generation of sulfate radical (SO 4 ·− ) and hydroxyl radical (·OH) for the efficient degradation of emerging contaminants. The electrocatalysis reactor is composed of a modified-graphite-felt (GF) cathode, in-situ prepared by the carbonization of polyaniline (PANI) electrodeposited on a GF substrate, and a boron-doped diamond (BDD) anode. In the presence of sulfates, the electrocatalysis system shows superior activities towards the degradation of pharmaceutical and personal care products (PPCPs), with the optimal performance of completely degrading the representative pollutant carbamazepine (CBZ, 0.2 mg L −1 ) within 150 s. Radicals quenching experiments indicated that ·OH and SO 4 ·− act as the main reactive oxygen species for CBZ decomposition. Results from the electron paramagnetic resonance (EPR) and chronoamperometry studies verified that the sulfate ions were oxidized to SO 4 ·− radicals at the anode, while the dissolve oxygen molecules were reduced to H 2 O 2 molecules which were further activated to produce ·OH radicals at the cathode. It was also found that during the catalytic reactions SO 4 ·− radicals could spontaneously convert into peroxydisulfate (PDS) which were subsequently reduced back to SO 4 ·− at the cathodes. The quasi-steady-state concentrations of ·OH and SO 4 ·− were estimated to be 0.51×10 −12 M and 0.56×10 −12 M, respectively. This study provides insight into the synergistic generation of ·OH/SO 4 ·− from the integrated electrochemical anode oxidation of sulfate and cathode reduction of dissolved oxygen, which indicates a potential practical approach to efficiently degrade the emerging organic water contaminants.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2022
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IF 11.357
Dashi Lei,Chunli Gou,Chunli Wang,Juanqin Xue,Zhongshen Zhang,Weizhen Liu,Zhang Lin,Jing Zhang
The reduced chromite ore processing residue (rCOPR) deposited in environments is susceptible to surrounding factors and causes reoccurrence of Cr(VI). However, the impact of natural sunlight on the stability of rCOPR is still unexplored. Herein, we investigated the dissolution and transformation behaviors of Cr(III)–Fe(III) hydroxide, a typical Cr(III)-containing component in rCOPR, under visible light. At acidic conditions, the release rate of Cr(III) under illumination markedly increased, up to 7 times higher than that in the dark, yet no Cr(VI) was produced. While at basic conditions, only Cr(VI) was obtained by photo-oxidation, with an oxidation rate of ∼7 times higher than that by δ-MnO2 under dark conditions at pH 10, but no reactive oxygen species was generated. X-ray absorption near-edge structure and density functional theory analyses reveal that coexisting Fe in the solid plays a critical role in the pH-dependent release and transformation of Cr(III), where photogenerated Fe(II) accelerates Cr(III) produced at acidic conditions. Meanwhile, at basic conditions, the production of intermediate Cr(III)–Fe(III) clusters by light leads to the oxidation of Cr(III) into Cr(VI) through the nonradical “metal-to-metal charge transfer” mechanism. Our study provides a new insight into Cr(VI) reoccurrence in rCOPR and helps in predicting its environmental risk in nature.
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