SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Sheng Liang,Jinling Wang,Zhizhi Shen,Wei Yan,Lichao Nengzi,Chunhua Feng,Xin Lei,Li Yu,Junqing Hu
The strategy to mineralize dissolved organics for the decontamination of landfill leachate concentrate (LLC) is expensive. Because mineralization requires high stoichiometric ratio of oxidants (e.g., •OH) or electron transfer (i.e., energy) to the pollutant molecules. Whereas, transferring the dissolved organic pollutants into separable insoluble matters is an energy-saving strategy. Herein, we developed a dual-anode Fe 2+ /HClO system for removing dissolved organic pollutants in LLC through insolubilization based on oxidative coupling. In this system, the majority of dissolved organic pollutants were transferred into insoluble substances, which could be removed easily. As a result, 89.8 % of the dissolved organic carbon (DOC) in LLC was fast removed in 3 h with a low specific energy consumption (SEC, 4.0 kWh kg −1 COD and 17.6 kWh kg −1 DOC), and the formation of toxic by-products can be well controlled to total organic chlorine (TOCl) < 0.1 mg/L. The formation of insoluble substances was attributed to the oxidative coupling of organic small molecules into the macromolecular ones. This was evidenced by the generation of insoluble compounds with the larger molecular mass, and the formation of coupling or polymerization products of the model pollutant (guaiacol). The predominant mechanism was proposed that Fe(IV) was generated in the dual-anode Fe 2+ /HClO system, and Fe(IV) oxidized pollutants to produce organic radicals, then the organic radicals coupled and polymerized to form larger molecules and insoluble compounds. This work offers a novel electrochemical method for efficient removal of organic pollutants in LLC with minimal toxic by-products generated, and revealed the significance of oxidative coupling process in the electrochemical Fe 2+ /HClO system.
研究领域:
环境科学
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电化学工程
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2018
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IF 5.667
Jing Chen,Yunjing Gao,Qin Ma,Xiaoyan Hu,Yali Xu,Xiaoquan Lu
In the present work, the classical synthesis method of 5,10,15,20-(4-sulphonatophenyl) porphyrin (TPPS 4 ) was improved. The synthesis process became more environmentally friendly, and the yield was increased by 10%. We constructed a sensitive fluorescent sensor for detection hydrogen peroxide (H 2 O 2 ) and glucose (C 6 H 12 O 6 ) by using the hyperfluorescence of TPPS 4 . The TPPS 4 -Fe 3+ complex system of the sensor could generate electron transfer process (ET) in the process of hydrogen peroxide (H 2 O 2 ) and glucose oxidation, which quenched the TPPS 4 fluorescence. The system had a linear range of 0–42 μM for hydrogen peroxide, and the minimum detectable limit (LOD) was 1.24 nM (S/N = 3). Compared with other detection methods, the proposed method had the advantages of higher sensitivity, lower detection limit and more simple operation.
研究领域:
生物化学
·
分析化学
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高影响因子
Materials Today Communications
·
2023
·
IF 3.8
Siyuan Zhang,Xinjian Cheng
Developing water-soluble fluorescent probes has important scientific and practical significance. In this work, coumarin derivatives bearing -OH were obtained through the classical Knoevenagel reaction firstly. Secondly, -C C- on allyl bromide was introduced into coumarin by Williamson ether formation method. Thirdly, hydrazine hydrate was added to the coumarin derivatives, a polymerizable small molecular coumarin fluorophore containing probe was obtained successfully. And, the -COOH on di-thioester underwent an esterification reaction with –OH groups on β-cyclodextrin(β-CD) to prepare oligomer based reversible addition-fragmentation chain transfer(RAFT) reagents. Finally, three copolymer probes β-CD-PMAA-Coumarin, β-CD-PMAm-Coumarin, and β-CD-PHEMA-Coumarin were prepared via RAFT polymerization , in which C C-coumarin was used as the functional monomer and methacrylamide(MAm)/methacrylic acid (MAA)/hydroxyethyl methacrylate (HEMA) as the main monomers. The MALDI-TOF mass tests showed that the macromolecular level probes were successfully prepared. These polymer probes have molecular weights up to 5.4 kDa and have narrow molecular weight distributions (PDI≤1.31). With the assistance of water-soluble long-chained PMAm/PMAA/PHEMA and hydrophilic β-CD, the coumarin containing macromolecular fluorescent probes could be dissolved in water readily. These water soluble polymer fluorescent probes could recognize Fe 3+ /Fe 2+ and Cu 2+ ions with high sensitivity. The detection limit of Fe 3+ could be as low as 0.34 μM. This study successfully developed a promising technique for producing highly selective, fully water-soluble fluorescent macromolecular probes.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2025
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IF 7.7
Xiaotong Wang,Tongtong Ye,Shaohui Geng,Shuna Ren,Xuming Zhao,Lihua Chen
A dual-signal strategy was developed based on a coordination reaction between iron(II) ions (Fe 2+ ) and potassium hexacyanoferrate(III) (K 3 [Fe(CN) 6 ]) to distinguish between brucella vaccine and wild strain. Utilizing metal-organic frameworks (MOFs), MOF Al (aluminum) @Fe 2+ @P 1 and MOF Fe @P 2 were synthesized and affixed to a hyaluronic acid (HA)-doped electrode. Hairpin probe 1 (P 1 ) has a common sequence (P 1 ') recognizing a fragment (T 1 ) in vaccines and wild strains. In contrast, hairpin probe 2 (P 2 ) has a differential sequence (P 2 ') only targeting a specific fragment (T 2 ) in the wild strain. Experimental findings indicated that activation of T 1 led to the dissociation of P 1 from MOF Al @Fe 2+ @P 1 , which released Fe 2+ into a buffer containing trace Fe 2+ . Following this, the addition of hydrogen peroxide (H 2 O 2 ) and K 3 [Fe(CN) 6 ] resulted in the formation of KFe[Fe(CN) 6 ] (PB). In contrast, specific activation of T 2 caused the detachment of P 2 from MOF Fe , thereby exposing its catalytic site. In H 2 O 2 , this catalytic site facilitated the conversion of trace Fe 2+ in buffer to Fe 3+ , with no PB generated after the addition of K 3 [Fe(CN) 6 ]. Simultaneous activation of T 1 and T 2 promoted the oxidation of Fe 2+ released from MOF Al by the exposed catalytic site of MOF Fe . The ratio of K 3 [Fe(CN) 6 ] to PB exhibited dynamic changes. Specifically, the ratio below 2.37 ± 0.05 indicated a Brucella-positive sample, whereas a ratio under 0.9 ± 0.02 suggested a sample derived from the vaccine. The scarcity of dual-signal sensors employing coordination reactions underscores the significance of this approach. Moreover, it addressed the challenges associated with brucella detection, demonstrating robust analytical performance.
研究领域:
生物化学
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医学检测
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分析化学
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NEW JOURNAL OF CHEMISTRY
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2023
·Vol. 47
·期 41
·19202-19209
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IF 3.3
Xinlei Zhang,Peng Liu,Yuchi Zhang,Bohan Li,Yan Xu
Almost all types of proteins in biology are composed of L-amino acids, and very few contain D-amino acids. Therefore, chiral recognition, especially for the detection of L-amino acids, is of great importance. In this work, luminescent zinc-doped carbon dots (Zn-CDs) were successfully synthesized through a one-step hydrothermal method using [Zn(EDA)3]Cl2 (EDA = ethylenediamine) complex as a precursor, exhibiting superior water stability, low cytotoxicity and good photobleaching stability. It can be used as an “on–off–on” fluorescence probe in aqueous solution to sequentially detect Fe2+ ions and enantiomeric L-Lysine (L-Lys) molecules with the corresponding limit of detection (LOD) of 0.092 and 0.204 μM, respectively. Also, the sequential on–off–on fluorescent changes of Zn-CDs upon the addition of Fe2+ and L-Lys can be applied in living cell imaging, as observed by the contrast of images in confocal microscopy. In addition, two distinct multi-input molecular logic gates, involving distinguishing the effect of L-Lys and D-Lys on the fluorescence of Zn-CDs, and the regulation of fluorescence quenching and recovery of Zn-CDs by Fe2+ ions and L-Lys are established. The Zn-CDs also exhibits a linearly temperature-dependent fluorescence performance with high temperature sensitivity (Sr) of 1.10% °C−1 in 10–90 °C, demonstrating its great potential for biological temperature sensing applications. This work provides a new strategy for exploring novel metal-doped carbon dots with outstanding biocompatibility and multifunctionality in biological applications.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xi Chen,Yunfeng Chen,Songrong Li,Cheng Xue,Dongfang Liu,Wenli Huang
Phthalic acid esters (PAEs) pose serious health risks to humans and are difficult to remove by conventional sewage treatment processes. Herein, Fe 2 Mo 3 O 8 /MoO 2 /Mo 2 N composite (FMON) derived from bimetallic organic framework was used to activate peroxymonosulfate (PMS) for dibutyl phthalate (DBP) degradation. FMON exhibited an excellent catalytic effect with DBP removal efficiency of 92.4 % within 60 min. Mo 2 N showed a superior ability in promoting Fe 3+ /Fe 2+ redox cycle. The reduction efficiencies of Fe 3+ by Mo 2 N/MoO 2 composite and MoO 2 were 67 %–94 % and 11 %–23 %, respectively, in the homogeneous comparative experiment. Moreover, the ratio of Fe 2+ /Fe 3+ in FMON increased significantly after the catalytic reaction. Fe element doping also enhanced the reuse stability and reduced the metal ion leaching of the catalyst. The degradation of DBP was mediated by a variety of reactive species, of which SO 4 − , OH and O 2 − were dominant. Fe element, Mo element and O vacancies were confirmed to exert significant contributions as active sites in the catalytic process. Three degradation pathways of DBP were obtained by DFT calculation and HPLC-MS analysis. And the toxicity of DBP degradation products was significantly reduced based on the assessment result of Toxicity Estimation Software Tool (T.E.S.T.). This study explored a novel Fe/Mo bimetallic catalyst with friendly Fe 3+ /Fe 2+ cycling for environmental catalysis and provided new ideas for the treatment of PAEs wastewater.
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ANALYTICAL CHEMISTRY
·
2023
·
IF 7.4
Mingxia Sun,Hongjie Song,Haiyi Liu,Yingying Su,Xiaobo Xie,Yi Lv
Sulfur dioxide (SO2) as one kind of air pollution not only causes extreme environmental pollution but also negatively affects human health. Chemiluminescence (CL) methods applied for sulfite analysis with high selectivity based on activating sulfite with oxidants are always implemented in acid media with a high background rise. In this work, we proposed to develop a mild CL system of Fe2+-SO32– to detect sulfite under neutral conditions and provide in situ CL spectral data for deeply studying the CL mechanism of Fe2+-SO32–. Herein, we first synthesized one type of water-soluble supramolecular nanosheets, APDI NSs, which had a strong oxidation potential (+2.9 V) due to a π-conjugated system for activation of sulfite to enhance the generation of SO3̇– and other active radicals, and strong a CL signal from the APDI NSs-Fe2+-SO32– system was generated. By studying the CL mechanism under acidic and neutral conditions, a new CL reaction pathway (path-1) and a key intermediate, S2O42–, from the reaction of Fe2+ and SO32– were found. The CL signal was emitted by SO2* after oxidation of S2O42– by strong oxidants like SO4•– and further amplified by APDI NSs through the CL resonance energy transfer (CRET) process. Based on the APDI NSs-Fe2+-SO32– system under neutral conditions, a CL method for detecting SO32– was established. The detection limit was 2.7 × 10–8 M (S/N = 3), and the recovery rates in spiked water samples were in the range of 87%–101%. This study strengthens the understanding of the CL reaction process of the Fe2+-SO32– system and provides a mild sulfite sensing platform for environmental samples.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Yun Ji,Zhelin Song,Yu Xu,Yanlin Zhang
In this work, typical refractory pollutant Rhodamine B (RhB) was effectively degraded by Cu-Fe LDHs/Bi 2 WO 6 composite in the photo-Fenton process. The hydrothermal synthesis of Cu-Fe LDHs/Bi 2 WO 6 composite with ethylene glycol as reductant created the multivalent coexistence of the same metal element to achieve a self-circle redox reaction between metals. The photo-Fenton process by Cu-Fe LDHs/Bi 2 WO 6 incredibly eliminated the limitation of strong acidic pH value applied in the Fenton process. ∙OH generated by Cu-Fe LDHs/Bi 2 WO 6 was 5 times that of Cu-Fe LDHs during the photo-Fenton process. The complete degradation of RhB in the photo-Fenton process under the optimal conditions of initial pH= 6, 5 mmol/L of H 2 O 2 , and 1 g/L of Cu-Fe LDHs/Bi 2 WO 6 dosage was far more than 46% of RhB degradation in the photocatalytic process and 76% of RhB degradation in the Fenton process. Cu-Fe LDHs/Bi 2 WO 6 composite exhibited the excellent redox ability, electron transfer ability and reusability during the photo-Fenton process. The acceleration of Fe 3+ /Fe 2+ cycles in the Cu-Fe LDHs/Bi 2 WO 6 /H 2 O 2 /Vis system was mainly ascribable to the combination of efficient transfer of photogenerated electrons and self-circle redox of Fe 3+ /Cu + . It is expected for the promising application of multivalent bimetallic photo-Fenton catalysts and rendering enlightenments for photo-Fenton catalytic oxidation reaction.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Xiaodong Ma,Tiantong Rao,Mingchen Zhao,Zhiwei Jia,Gengbo Ren,Jingyang Liu,Haiwei Guo,Zhineng Wu,Haijiao Xie
In-situ generation of iron catalysts in electro-Fenton (EF) process deserves more attention like in-situ generation of H 2 O 2 . In this work, a novel induced zero-valent iron (ZVI) electrode, which was composed of a graphite plate with good conductivity, ZVI powders and a small magnet, was for the first time designed through magnetic assembly. Fe 2+ could be slowly generated in-situ from induced ZVI electrode and effectively trigger EF oxidation of chlorobenzenes (CB) under neutral pH. Compared to the in-situ rapid release of Fe 2+ from sacrificial anodes and traditional one-time external dosing of Fe 2+ in EF, in-situ slow release of Fe 2+ from induced ZVI electrode was the most effective way to activate electrogenerated H 2 O 2 under neutral pH. Induced ZVI electrode had obvious advantages in terms of effective active areas, corrosion potentials and current responses. The optimum conditions including pH of 7.0, current of 29.9 mA, ZVI of 0.10 g and electrolysis time of 35.25 min were obtained by the response surface methodology (RSM) model with the maximum removal efficiency of 99.12%. The uniformed weak positive charge on the ZVI powders induced by the electric field was the dominant contribution to the in-situ slow release of Fe 2+ from the induced electrode. And, the impact of magnetic field on the CB removal and the release of iron ions was negligible. The degradation mechanism was revealed through the Fukui function based on the density functional theory (DFT) and by-products analysis. The evolution of acute toxicity to zebrafish in EF was further clarified. Besides, this induced ZVI electrode could be easily reused and has satisfactory stability. In briefly, this work provided a novel idea for the in-situ slow release of Fe 2+ in EF process.
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Journal of Cleaner Production
·
2023
·
IF 11.1
Yang Yang,Wenqing Zhen,Tingting Zhao,Maoquan Wu,Shouchun Ma,Liyan Zhao,Jie Wu,Li Liu,Jiaxu Zhang,Tongjie Yao
Fenton/photo-Fenton reaction was limited by slow Fe 3+ /Fe 2+ cycle, low H 2 O 2 activation efficiency, and narrow applicable pH range. Here, Fe atoms doped MoS 2 (Fe–MoS 2 ) with abundant of low-valence Mo δ+ (0 < δ < 4) was prepared. Benefiting from the powerful reduction capacity of Mo δ+ , the rate-limiting step of Fe 3+ reduction was significantly accelerated. Nearly 100% of H 2 O 2 utilization efficiency was realized. Importantly, 90% of H 2 O 2 was effectively activated to be • OH. As a result, tetracycline degradation rate in photo-Fenton reaction catalyzed by Fe–MoS 2 was 5.8 and 4.2 times higher than those of MoS 2 and Fe–MoS 2 -Hyd (prepared by hydrothermal reaction). In comparison with MoS 2 and Fe–MoS 2 -Hyd whose efficient work range were limited in acidic condition, Fe–MoS 2 was a pH-universal catalyst (pH = 2.6–14.0) by taking advantage of the exposed Mo δ+ and photoinduced electrons, largely improving the environmental tolerance. This work simultaneously addressed three bottlenecks in Fenton/photo-Fenton reaction, and provided a new strategy for the preparation of catalysts with powerful catalytic performance and high environmental adaptability.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Xiaoyan Bai,Haichuan Sun,Jian Sun,Zhihua Zhu
It is urgent to remove polycyclic aromatic hydrocarbons (PAHs) from textile dyeing sludge (TDS) before its final deposal due to their recalcitrant nature and generation of toxic byproducts during TDS treatment . In this study, an electrochemical Fe 2+ -activated peroxymonosulfate (PMS) oxidation process for removing 16 priority PAHs from real TDS was firstly investigated. The results showed that the removal efficiency of the ∑16PAHs in TDS was positively correlated to the concentration of Fe 2+ released from sacrificial iron anode and the concentration of electroregenerated Fe 2+ in the cathode by the reduction of Fe 3+ within the applied voltage range of 3–7 V, but a higher voltage of 10 V did not lead to further improvement in ∑16PAHs removal due to the radical scavenging reaction resulted from the excessive accumulation of Fe 2+ . 64.7% and 16.1% of the ∑16PAHs were removed in the anodic and cathodic chamber under the optimum reaction conditions of 400 mg/g PMS/VSS, pH 3 and applied voltage 7 V, respectively. low-ring PAHs were preferentially degraded compared to high-ring PAHs. The O ⋅ H played a major role while SO 4 ⋅ — had a minor role in PAHs degradation in TDS. The intracellular PAHs released from cracked sludge cells were found to undergo further degradation under free radical attack.
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高影响因子
FOOD CONTROL
·
2026
·
IF 6.3
Yaping Zhong,Kayi Shao,Ruixia Zhang,Linlong Zhang,Dong Wang
Food safety is a key public concern, making the detection of harmful substances in food increasingly urgent. Herein, a multifunctional fluorescence sensing platform was designed utilizing glutathione-derived N, S-co-doped carbon quantum dots (N, S-CDs), capable of sensitively monitoring nitrite (NO 2 - ) and hydrogen sulfide (H 2 S) in both food and living biological cells. The detection relies on Fe 3+ -induced fluorescence quenching of N, S-CDs through inner filter effect and static quenching, combined with the redox reactions of NO 2 - with Fe 2+ and H 2 S with Fe 3+ . The linear ranges and limits of detection (LOD) were as follows: NO 2 - , 1-1000 μM and 0.164 μM; H 2 S, 25-425 μM and 0.114 μM. Thanks to its ideal biocompatibility, N, S-CDs enabled visualization of NO 2 - and H 2 S in living cells. Meanwhile, N, S-CDs paper-based fluorescent sensor was constructed to detect NO 2 - in pickled meat and H 2 S in spoiled meat, demonstrating great potential for biological tracking and portable sensor development.
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