SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yi Ren,Naiwen Li,Jun Li,Weiming Zhang,Chao Liu,Bo Lai
Iron based Fenton-like processes have been widely investigated, while how to regulate active species generation still is a problem of concern. In this study, MILs(Al) with various carboxyl group amounts were used as research tools, loading iron for Fenton-like oxidation, to investigate the effect of free carboxyl group on surface or free HO generation. Active species identification indicates that surface and free HO were main active species for carbamazepine removal. Moreover, it was concluded that contribution of free HO for the decontamination was positively correlated with carboxyl group amounts on MILs(Al). With free carboxyl group amounts increasing from 3.07 to 5.09 mmol/g on MILs(Al)-Fe, concentration of free HO for carbamazepine removal increased from 47.4% to 62.5%. The mechanisms of carboxyl group amounts impact the chemical state of HO was proposed as steric hindrance effect and charge density near iron sites. The destruction of carbamazepine was proposed in different systems by intermediates determination, and the results indicate that the existing form of HO mainly influenced the efficiency of pollutant degradation, rather than oxidation mechanisms of it. Various pollutants degradation in different MILs(Al)-Fe catalyzed Fenton-like systems were investigated as well, to understand the superiority of different HO for decontamination. MILs(Al)-Fe with various carboxyl group amounts catalyzed Fenton-like processes could remove 34.2%–73.0% carbamazepine, 56.7%–93.8% sulfamethoxazole, 36.4%–75.6% bisphenol S and 43.8–79.7% salicylic acid. This study understood the regulation of active species by carboxyl group in MILs(Al)-Fe/H 2 O 2 systems, and sheds new light on active species precise regulation in Fenton-like systems.
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Journal of Materials Chemistry B
·
2023
·Vol. 11
·期 18
·4020-4027
·
IF 7
Min Feng,Xiaofang Chen,Yuhang Liu,Yan Zhao,Pran Gopal Karmaker,Jia Liu,Ya Wang,Xiupei Yang
Single-atom catalysts with atomically dispersed sites have been widely used as nanozymes for colorimetric sensing because their tunable M–Nx active centers are similar to those of natural enzymes. However, their low metal atom loading leads to insufficient catalytic activity and affects the sensitivity of colorimetric sensing, which limits their further applications. Herein, multi-walled carbon nanotubes (MWCNs) are selected as carriers to reduce the aggregation of ZIF-8 and improve the electron transfer efficiency of nanomaterials. Meanwhile, MWCN/FeZn-NC single-atom nanozymes with excellent peroxidase-like activity were prepared by pyrolysis on ZIF-8 doped with a second metal Fe. Based on the excellent peroxidase activity of MWCN/FeZn-NCs, a dual-functional colorimetric sensing platform for Cr(VI) and 8-hydroxyquinoline was established. The detection limits of the dual-function platform are 40 nM for Cr(VI) and 55 nM for 8-hydroxyquinoline. This work provides a highly sensitive and selective strategy for the detection of Cr(VI) and 8-hydroxyquinoline in hair care products, which has great application prospects in the field of pollutant detection and control.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Chao Zhang,Mengxiang Ye,Huaimeng Li,Zhenzhen Liu,Zhen Fu,Haimin Zhang,Guozhong Wang,Yunxia Zhang
Heterogeneous electro-Fenton is a promising technology for the degradation of organic contaminants. To ensure its effectiveness, it is in urgent demand to design cathode materials with the integrated capability of sufficient H 2 O 2 generation and subsequent activation into reactive oxygen species (ROS) together with catalytic stability. Herein, a composite constituted by Fe/Fe 3 C nanoparticles embedded into N-doped porous carbon (NPC), designated as Fe/Fe 3 C@NPC, was successfully fabricated from Fe 3+ -loaded poly(imine dioxime) (PIDO) membrane via the thermal treatment in N 2 atmosphere and employed as the heterogeneous electro-Fenton catalyst to degrade bisphenol A (BPA). By optimizing the pyrolysis temperature and loading level of iron species, the catalyst obtained at 800 °C (i.e. Fe/Fe 3 C@NPC-800) achieved almost 100% of BPA removal efficiency within 120 min via the electro-Fenton system, accompanied by 69.2% of the total organic carbon (TOC) removal rate. Furthermore, the proposed composite catalyst also exhibited satisfactory reusability and stability, as reflected by low decrease in removal efficiency after six successive degradation tests and limited iron leaching (<0.5 mg/L). This work might provide valuable instruction for the rational design of highly efficient and stable heterogeneous electro-Fenton catalysts for organic pollutant control.
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NANOTECHNOLOGY
·
2022
·Vol. 34
·期 8
·085401
·
IF 3.953
Hongna Jia,Yao Wang,Shuya Zhao,Haipeng Wang,Na Ju,Xinyue Zhang,Hong Li,Zejun Sun,Hong-bin Sun
Carbon materials derived from metal-organic frameworks have attracted increasing attention as anodes for energy storage. In this study, Fe, Ni-doped ZIF-8 is carbonized at high temperature to obtain bimetallic Fe and Ni modified tension -relaxed carbon (FeNi@trC). Fe and Ni have opposite structural modification effects when the metal ions are doped into the ZIF-8 dodecahedron. The obtained carbon material maintains the regular dodecahedron morphology, which means the relaxation of tension and strong thermal stability during annealing. Moreover, the presence of nickel enhances the carbonization degree and electrochemical stability of FeNi@trC, while the calcination of the tensive ZIF-8 precursor offers more defect sites. The discharge capacities of FeNi@trC materials are stable at 182.9 mAh·g−1 and 567.9 mAh·g−1 for sodium-ion batterie (SIB) and lithium-ion batterie (LIB) at 0.05 A·g−1. Compared with the current density of 0.05 A·g−1, the discharge capacity of SIB and LIB attenuates by 29.4% and 55.9% at 1 A·g−1, respectively, and the FeNi@trC shows good performance stability in the following cycles.
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Science China-Materials
·
2023
·Vol. 66
·期 5
·1779-1792
·
IF 8.1
Yang Jia,Wang Mengxiao,Chen Tao,Yu Xiang,Qin Gang,Fang Xiaohan,Su Xiaoxiang,Chen Qiang
Supercapacitors exhibiting toughness, self-healing, and high specific capacitance have practical significance for use in flexible and wearable electronic equipment. To meet these requirements, a novel multifunctional gel polymer electrolyte (GPE) consisting of polyvinyl alcohol (PVA)-sodium alginate (SA)-K 3 [Fe(CN)] 6 -Na 2 SO 4 was prepared. In this GPE, K 3 [Fe(CN)] 6 plays three crucial roles by serving as a carrier donor, ionic crosslinking agent and redox-active mediator. Consequently, the usual conflict between the conductivity and mechanical properties of GPEs is alleviated to some extent. In addition, the electrode specific capacitance and the energy density of the assembled supercapacitor are obviously improved because of the pseudocapacitance generated from the redox reaction of K 3 [Fe(CN)] 6 . Based on this GPE, the supercapacitor exhibits outstanding bending and stretching stabilities, significant self-healing, and anti-freezing properties. Therefore, the prepared GPE and supercapacitor are promising for application in flexible and wearable electronic equipment with complex service conditions.
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PLASMA CHEMISTRY AND PLASMA PROCESSING
·
2022
·Vol. 43
·期 2
·491-511
·
IF 3.337
Huang Shaoyong,Huang Quanjia,Gan Jiaming,Li Ting,Wang Lei
In this study, Fe-rich sludge was pretreated by dielectric barrier discharge (DBD) and used as a Fenton catalyst for the degradation of 2,4-dichlorophenoxyacetic acid (2,4-D) in aqueous solution, where hydrogen peroxide was in situ supplied from a glow discharge plasma (GDP) in contact with the solution. Synergistic mechanism of the two plasmas during 2,4-D degradation was explored. The Fe-rich sludge pretreated by H 2 -DBD could significantly accelerate the 2,4-D degradation as it converted Fe(III) in the sludge to the active Fe(II). 2,4-D can be completely removed in the presence of H 2 -DBD pretreated Fe-rich sludge with 25 min of GDP at pH 0 3.0 and catalyst dosage of 1.0 g/L. Quenching experimental studies showed that both ·OH (oxidative degradation) and ·H (reductive dechlorination) were responsible for 2,4-D degradation. Reducing radicals (such as ·R and·H) formed during GDP can continuously reduce the Fe 3+ back to Fe 2+ , which further promoted the degradation and dechlorination of 2,4-D. The results of three consecutive experiments indicated the stability and reusability of catalyst. This study provides a potential method for the recycle of Fe-rich sludge as a novel and cost-effective catalyst for 2,4-D removal from aqueous environments, which is significant for the terminal disposal of Fe-rich sludge. Graphical Abstract
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Nano-Micro Letters
·
2023
·Vol. 15
·期 1
·1-17
·
IF 26.6
Chen Shengmei,Liang Xiongyi,Hu Sixia,Li Xinliang,Zhang Guobin,Wang Shuyun,Ma Longtao,Wu Chi-Man Lawrence,Zhi Chunyi,Zapien Juan Antonio
The strong interaction between Ti 3 C 2 S x and FeN 4 species induces the central metal Fe(II) in FeN 4 species with intermediate spin state transferred to high spin state, in which the latter is favorable to initiate the reduction of oxygen.
This strong interaction induces a remarkable Fe 3 d electron delocalization with d band center upshift, boosting oxygen-containing groups adsorption on FeN 4 species and oxygen reduction reaction kinetics.
The resulting FeN 4 –Ti 3 C 2 S x with FeN 4 moieties in high spin state exhibits high half-wave potential of 0.89 V vs. RHE and high limiting current density of 6.5 mA cm −2 , enabling wearable zinc–air battery showing a good discharge performance with a maximum power density of 133.6 mW cm −2 .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Chen Wang,Zewei Hu,Wei Lou,Mingjie Huang,Wei Xiang,Tao Zhou,Juan Mao,Xiaohui Wu
This study has demonstrated that the Fenton fluidized bed (FFB) technology could successfully immobilize As ions on the iron-crystallized (IC) carriers, with simultaneous crystallization of ferric and mineralization of organic pollutants. It was found that rapid fluidized immobilization of aqueous As(V) on the IC carriers was through surface favorable bidentate complexion, while the adsorptive removal of As(III) was rather slow. Adding Fe 3+ caused competitive complexion and inhibited the As(V) immobilization. However, effective oxidative crystallization of Fe(II) and As(III) in FFB would take place. With the simultaneous generation of As(V) and Fe(III) by rapid •OH oxidation, two different crystalline precursors would be formed on the IC carriers, leading to efficient co-crystallization of As(V)/Fe(III). Recursive Fe(III) crystallization in the FFB continuously provided essential surface hydroxyl groups for capturing As(V), inducing layer-by-layer co-crystallized immobilization As(V)/Fe(III). The long-term continuous-flow treatment of a practical As(III)-containing industrial organic wastewater exhibited effective/stable co-crystallizations of As(V)/Fe(III), as well as COD removal. The FFB technology is expected to be a good option in treating complex industrial wastewater containing heavy metal and recalcitrant organic pollutants.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Xiaoyu He,Xutao Gao,Xiao Chen,Shen Hu,Fangchang Tan,Yujie Xiong,Ran Long,Min Liu,Edmund C.M. Tse,Fei Wei,Hong Yang,Jungang Hou,Chunshan Song,Xinwen Guo
Increasing CO 2 conversion efficiency over metal-organic framework (MOF) based photocatalysts is of great significance to promote the carbon capture and utilization. In this work, a dual-benefit design strategy is deployed in the synthesis of a new two-dimensional Fe/Ti-BPDC MOF photocatalyst with atomically dispersed Fe sites. This catalyst demonstrated an excellent catalytic performance in the visible-light-driven CO 2 conversion to HCOOH, achieving a high yield of 703.9 μmol g -1 h -1 at a selectivity greater than 99.7%. This is attributed to the ‘dual-optimization’ achieved by this catalyst to sustain the supply of photogenerated electrons and to effectively activate CO 2 . Specifically, the Fe/Ti-BPDC catalyst provides a high proportion of effective photogenerated electrons for the CO 2 photocatalysis process via a unique electron transfer mechanism. Meanwhile, the strong O/Fe affinity between CO 2 and atomically dispersed Fe active sites not only enables a fast CO 2 activation, but also dictates the intermediate reaction pathways towards high HCOOH selectivity.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Youpu Zhao,Qing Sun,Jian Zhang,Jiawei Sheng
In this study, natural porous diatomite was utilized as a conciliatory carrier for the fabrication of Fe/N/C nano-clusters with assistance of binary molten salt of NaCl-ZnCl 2 under different annealing temperature and used to removal of norfloxacin (NFA). The sample Fe/D m900 (prepared at 900 °C) exhibited a high surface area and great catalytic performance for antibiotics in the presence of PMS. Over 97% NFA can be decomposed within 5 min and the final degradation rate reached 98%. Meaningfully, high-efficiency Fe/D m900 -PMS system was nearly impervious to pH values and inorganic cations in aqueous solution and could be a likely candidate for degradation of multiple contaminants in pharmaceutical outlet water. Furthermore, the other impacting variables such as catalyst dosage, PMS dosage, NFA concentration and initial pH were moreover explored towards debasement, and conceivable degradation pathways of NFA were presented through LC-MS. This work builds up a compelling procedure to synthesize super-dispersed Fe clusters, which may be amplified to other transition metal-based catalyst via molten salt.
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TALANTA
·
2023
·
IF 6.1
Qingying Wang,Lianfang Chen,Xiaoyan Cui,Jie Zhang,Yaohui Wang,Xiupei Yang
Herein, a covalent organic framework (COF) was grown on a magnetic metal-organic framework (MOF) by a solvothermal method for the efficient extraction of bisphenols (BPs). The magnetic solid-phase extraction (MSPE) of four bisphenols (bisphenol A, bisphenol B , bisphenol AF and bisphenol C) was carried out without adjusting the pH and salt concentration. When 30 mg Fe 3 O 4 @NH 2 -MIL-88(Fe)@TpPa was used to adsorb for 25 min, 6 mL methanol was used to elute for 20 min, and the extract was detected by high-performance liquid chromatography (HPLC). The proposed method has a low detection limit of 0.011–0.036 ng mL −1 , a wide linear range of 0.05–100 ng mL −1 , and a correlation coefficient (R 2 ) of 0.9980–0.9998. The intra-day and inter-day precisions are 0.74–2.54% and 1.68–3.72%, respectively. Bisphenol A was determined by applying the proposed method to the determination of actual milk samples. The standard addition experiment showed that the relative recovery of the four bisphenols was 85.70–119.7%. Pseudosecond-order, first-order, Langmuir and Freundlich models were applied to explore the adsorption characteristics of Fe 3 O 4 @NH 2 -MIL-88(Fe)@TpPa. In general, the established Fe 3 O 4 @NH 2 -MIL-88(Fe)@TpPa-MSPE-HPLC-UV method exhibits attractive sensitivity, simple manipulation, and excellent reusability, and it has excellent prospects for the detection of trace BPs in complex milk matrices.
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CHEMOSPHERE
·
2023
·
IF 8.8
Gangya Cheng,Chen Yuan,Wansheng Ruan,Ben Ma,Xinyu Zhang,Xinjing Yuan,Zhihui Li,Dan Wang,Fei Teng
In this work, Fe-based metal-organic frameworks (Fe-MOFs) are prepared by a simple solvothermal method, in which acetic acid/N, N-dimethylformamide (HAc/DMF) mixture solvents are employed to regulate the particle morphology, exposed facets and ligand defects. At HAc/DMF = 0/50, 5/45 and 8/42 (volume ratio), the irregular particles (MIL-53(Fe)), elongated icosahedrons (5H-MIL-101(Fe)) and icosahedrons (8H-MIL-101(Fe)) are obtained, respectively. Under visible light irradiation (λ > 420 nm) and the addition of sodium persulfate (PS), 5H-MIL-101(Fe) shows the highest degradation activity for tetracycline (TC). Specifically, 80% of TC has been removed by 5H-MIL-101(Fe) within 25 min, and the degradation kinetics rate is 3.03 times higher than that over MIL-53(Fe). The improvement of catalytic activity is mainly attributed to the active facets exposed and ligand defects of 5H-MIL-101(Fe). Density functional theory (DFT) calculation further confirms that the active facets exposed and ligand defects of 5H-MIL-101(Fe) favor the adsorption and activation of PS, benefiting the generation of •SO 4 − . Besides, a probable degradation pathway of TC is proposed based on trapping experiments and liquid chromatography-mass spectrometry (LC-MS) test. Furthermore, the toxicities of intermediates are predicted by the quantitative structure-activity relationship (QSAR) mathematical model. This work demonstrates that visible light enhanced PS activation (Vis-PSA) can more effectively degrade organic pollutants, and this work also provides a simple strategy to precisely regulate ligand defects and actively exposed facets of Fe-MOFs to enhance the adsorption and activation of PS.
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