CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Sitao Wang,Zhijie Liu,Bolun Pang,Yuting Gao,Santu Luo,Qiaosong Li,Hailan Chen,Michael G Kong
Antibiotics are widely used to treat or prevent infectious diseases in human and veterinary medicine. Excessive residues in the aquatic environment lead to increasingly prominent antibiotic pollution; therefore, it is urgent to develop sustainable strategies for rapidly degrading antibiotics. In this study, a highly synergetic effect for norfloxacin (NOR) remediation is achieved by coupling underwater bubble plasma formation with a Fe (III)–S (IV) system due to the efficient utilization of reactive species in chain reactions. The degradation rate using synergetic approach can reach 76.4% within 50 min discharge, and further increases significantly to 94.4% after 5 h post-discharge. The effects of pulsed peak voltage and Fe (III)/S (IV) dosage on NOR removal are characterized. The existence of hydroxyl radicals ( • OH) and sulfate radicals (SO 4 •− ) are proved by electron spin resonance spectrometer (ESR) during degradation. Furthermore, radical scavenger experiments demonstrate that • OH and SO 4 •− play a crucial role in degradation. Underwater bubble plasma provides the oxic and acidic liquid environment for the Fe (III)–S (IV) system to accelerate the self-perpetuating chain reactions. These reactions not only introduce SO 4 •− and generate more • OH during plasma-on, but also induce their regeneration and further prolong the degradation process during plasma-off through plasma-generated effects. Finally, the degradation intermediates of NOR are identified, and a possible degradation pathway is proposed. The possible contribution weight of each approach on the degradation rate is speculated. These new findings offer promising applications for developing a technology with real potential for the treatment of organic compounds in industrial wastewater treatment.
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NANOTECHNOLOGY
·
2022
·Vol. 33
·期 13
·135502
·
IF 3.953
Hui Shu,Tingrun Lai,Jie Ren,Xiuxiu Cui,Xu Tian,Zhichao Yang,Xuechun Xiao,Yude Wang
The excessive use of imidacloprid in agricultural production leads to a large number of residues that seriously threaten human health. Therefore, the detection of imidacloprid has become very important. But how to quantitatively detect imidacloprid at ultra-low levels is the main challenges. In this work, trimetallic metal-organic frameworks Fe, Co, Ni-MOF (FCN-MOF) is in situ prepared on nickel foam (NF) and then used to make an electrochemical sensor in the detection of imidacloprid. FCN-MOF exhibits the characteristics of ultra-micro concentration detection for imidacloprid with high specific surface area and rich active metal centers. The high conductivity and 3D skeleton structure of the NF electrode enhance the contact site with imidacloprid and promote the transmission of electrons efficiently. All results show that the prepared electrochemical sensor has the advantages of ultra-low detection limits (0.1 pM), wide linear detection ranges (1–5 × 107 pM) and good sensitivity (132.91 μA pM‒1 cm‒2), as well as good reproducibility, excellent anti-interference ability, and fantastic stability. Meanwhile, the electrochemical sensor is used to determine imidacloprid in lettuce, tomato, and cucumber samples with excellent recovery (90%–102.7%). The novel electrochemical sensor is successfully applied to the ultra-micro detection of imidacloprid in vegetables, which provides a new way for the efficient monitoring of imidacloprid in agriculture.
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高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Wenbao Zuo,Weibin Chen,Jinxue Liu,Shuying Huang,Luping Chen,Qingna Liu,Nian Liu,Quanyi Jin,Yang Li,Peiyuan Wang,Xuan Zhu
Fe-based nanomaterials with Fenton reaction activity are promising for tumor-specific chemodynamic therapy (CDT). However, most of the nanomaterials suffer from low catalytic efficiency due to its insufficient active site exposure and the relatively high tumor intracellular pH, which greatly impede its clinical application. Herein, macrophage membrane-camouflaged carbonic anhydrase IX inhibitor (CAI)-loaded hollow mesoporous ferric oxide (HMFe) nanocatalysts are designed to remodel the tumor microenvironment with decreased intracellular pH for self-amplified CDT. The HMFe not only serves as a Fenton agent with high active-atom exposure to enhance CDT but also provides hollow cavity for CAI loading. Meanwhile, the macrophage membrane-camouflaging endows the nanocatalysts with immune evading capability and improves tumoritropic accumulation by recognizing tumor endothelium and cancer cells through α4/VCAM-1 interaction. Once internalized by tumor cells, the CAI could be specifically released, which can not only inhibit CA IX to induce intracellular H+ accumulation for accelerating the Fenton reaction but also could prevent tumor metastasis because of the insufficient H+ formation outside cells for tumor extracellular matrix degradation. In addition, the HMFe can be employed to highly efficient magnetic resonance imaging to real-time monitor the agents’ bio-distribution and treatment progress. Both in vitro and in vivo results well demonstrated that the nanocatalysts could realize self-amplified CDT and breast cancer metastasis inhibition via tumor microenvironment remodeling, which also provides a promising paradigm for improving CDT and antimetastatic treatment.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Zenglong Wu,Wenkai Song,Xiangwei Xu,Jiangnan Yuan,Weiyang Lv,Yuyuan Yao
Applicating co-catalyst into Fenton-like advanced oxidation processes to improve the performance for wastewater remediation has attracted widespread attention. Among them, developing highly active and green heterogeneous catalyst integrating homogeneous ferrous ions and inorganic co-catalyst is a great challenge. Herein, ascorbic acid additive was creatively introduced into the precursor composed of thiourea, sodium molybdate and ferric chloride to synthesize carbon intercalated molybdenum disulfide anchoring iron (C-MoS 2 @Fe) by a simple one-step hydrothermal method. C-MoS 2 @Fe exhibited an amazing apparent first-order constant as high as 0.739 min −1 about 10 times higher than that of the homogeneous Fe 2+ /MoS 2 system for the sulfamethoxazole (SMX) removal and achieved 68.7% removal of TOC in 6 min, which was attribute to the synergistic enhancement of high 1T phase (82.0%) and sulfur vacancies induced by the introduction of ascorbic acid. Notably, the C-MoS 2 @Fe was also capable of efficiently degrading multiple organic contaminants such as pharmaceuticals, phenolic compounds, and organic dyes. Compared with the homogeneous Fe 2+ /PMS system, the C-MoS 2 @Fe/PMS system expanded the effective pH range (2.0 ∼ 9.0) and the ultralow iron ions leaching (0.204 mg L -1 ) avoided the formation of iron containing sludge. The results of electron paramagnetic resonance (EPR), radical quenching and probe experiments indicated that •OH was the main active species with the contribution rate about 60.3%. Furthermore, possible degradation pathways were proposed based on the intermediate products of SMX investigated by LC-MS. This study provides novel insights for the development of highly active and green catalysts for wastewater remediation.
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Advanced Materials Interfaces
·
2022
·Vol. 9
·期 6
·2101510
·
IF 6.389
Jun Li,Tongtong Xu,Han Bai,Zhenyu Shen,Yanyan Huang,Wenwen Xing,Zhongxiang Zhou
Microwave absorption enhancements through atomic doping in traditional materials remain a significant challenge. Herein, the MAX phase materials of Fe-doped Ti 3 AlC 2 ( x Fe-Ti 3 AlC 2 , abbreviated as TFAC- x , x = 0, 0.2, 0.3, 0.4) are synthesized via solid-phase reaction method. The X-ray diffraction, Raman, and scanning electron microscopy confirm that the TFAC- x samples are of high quality with multiphase coexistence structure and abundant interfaces. Relying on the improved impedance matching originating from structural modulation, the synergistic effects of dielectric loss and magnetic loss, as well as the enhanced interfacial polarization and defect dipole polarization, both the microwave absorption intensity and bandwidth are greatly strengthened. Accordingly, the minimum reflection loss of TFAC-3 sample can achieve -33.3 dB and the absorption bandwidth could reach 3.9 GHz with the thickness of only 1.5 mm. Moreover, the investigated frequency can cover 86% through regulating their thickness from 1.5 to 5 mm, showing the excellent frequency modulation effect. The revealed improvements in both the microwave absorption performance and properties of TFAC- x may enlighten the designing of microwave absorption materials and have potentials for widespread applications.
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JOURNAL OF MATERIALS SCIENCE
·
2022
·Vol. 57
·期 1
·526-537
·
IF 4.682
Xu Lin-Wei,Qian She-Liang,Dong Bao-Xia,Feng Li-Gang,Li Zong-Wei
Molecular complexes with active metal centers exhibit high activity and selectivity for electrochemical CO 2 reduction reaction (CO 2 RR), which represents a promising method for transforming greenhouse gas into valuable chemicals and feedstock. Using metal–organic frameworks (MOFs) to load the active molecular complexes then employing the combination with the carbonic conducting material may exhibit a beneficial effect for CO 2 RR. Herein, we obtained a composite catalyst named PCN-222(Fe)/CNTs, which was in situ synthesized through the solvothermal method that loads iron porphyrin-centered PCN-222(Fe) molecules onto CNTs. The catalyst PCN-222(Fe)/CNTs exhibits excellent electrocatalytic performance for CO 2 RR with a FE CO of 95.5% (m(Fe-TCPP):m(CNTs) = 1:30, written as PCN-222(Fe)/CNTs-30) and an overpotential ( η ) of 494 mV. In addition, the turnover frequency (TOF) is high as 448.76 h −1 (3.011 site −1 s −1 ) and the hydrogen evolution reaction (HER) is indistinctive. After long-term electrocatalysis of 10 h at −0.6 V vs. RHE, PCN-222(Fe)/CNTs-30 remained its high catalytic performance with average FE CO = 90%. This work provides a solid foundation for further research in the high-efficiency transformation of CO 2 to CO. Graphical abstract
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Journal of Water Process Engineering
·
2023
·
IF 7
Lilan Huang,Haimei Chen,Jin Han,Haojie Chen,Jian Pan,Zihan Zhao,Zhichao Dong,Hailin Cong
Printing and dying wastewater has a pervasive problem afflicting people worldwide due to negative impacts on ecosystems and humans. Herein, Fe/Cu bimetallic catalyst/polyethersulfone (4A-Fe@Cu/PES) mixed matrix membrane (APMMM) with macropore and high porosity were developed as catalytic membrane reactor for reduction of congo red (CR) in flow-through reaction. The forced flow of the reactants through the membrane improved the mass transfer and intensified the contact between reactants and immobilized catalysts, allowing for efficient adsorption and catalysis. Furthermore, the CR adsorption by 4A-Fe@Cu would form catalytic microzones in the membrane, which was conducive to further improving the catalytic efficiency. As a result, the apparent activation energy of dynamic catalysis (21.1 kJ/mol) was significantly decreased compared with that of static catalysis (93.7 kJ/mol). Therefore, the dynamic processes exhibited more excellent adsorption and catalytic efficiency. In cross-flow circulation mode, the maximum CR adsorption capacity of APMMM-18 (doping amount of 4A-Fe@Cu is 18.0 wt%) was 199.5 mg/g 4A-Fe@Cu with a catalyst/CR mass ratio of 1/1.5 and initial CR concentration of 50 mg/L. For catalysis, the APMMM-18 could remove 99.8 % CR after 5 h with a catalyst/CR mass ratio of 1/1.5 and 1.9 mM of H 2 O 2 at pH 8. The catalytic membranes showed much higher performances than 4A-Fe@Cu particles even under lower H 2 O 2 conditions. The intrinsic CR adsorption and degradation ratio of one layer of APMMM-18 under dead-end filtration was also investigated. The combination of the Fenton catalyst with the membrane process accomplished the effective removal of CR.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
·
IF 5.2
Ximin Chen,Yingqing Zhan,Wei Yang,Ao Sun,Hongshan Jia,Junlei Tang,Bing Lin
The complicated oily wastewater containing hazardous organics post a great challenge to the membrane separation technology . Herein, a multilayer porous multifunctional MXene/MOF composite membrane with high permeability and photocatalytic degradation performance was prepared by embedding rod-shaped MIL-53(Fe) into layered MXene nanosheets and self-assembling them onto porous polyacrylonitrile fibrous mat. It was found that the embedment of rod-like MIL-53(Fe) with rough nanostructures could effectively avoid the dense physical stacking of MXene nanosheets and regulate the layer spacing, which was conducive to the enhancement of water channel and permeability of membrane. Moreover, the hydrophilic modification of TA could render the super-wetting feature (WCA=0°, UOCA>150°) and enhance the oil resistance of the membrane. Thence, the composite membrane exhibited favorable separation flux (904.3 ∼ 1226.5 L·m −2 ·h −1 ) and retention rate (99.06 ∼ 99.62%) for different O/W emulsions. In addition, the coupling of rod-like MIL-53(Fe) and MXene nanosheets endowed the composite membrane with efficient photocatalytic performance, which could degrade various dyes contained in oily wastewater (CV: 62.4%, MeB : 99.0%, CR: 79.5%, MO: 84.1%). Overall, this study opens up a new way for the preparation of super-wetting and multi-functional fibrous composite membrane, showing the broad application prospects in the purification of multi-component oily wastewater.
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ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Zhiwen Xu,Guangyu Chen,Fei Yang,Juhee Jang,Guimei Liu,Fei Xiao,Yan Sun,Xiaoyi Qiu,Weiwei Chen,Dong Su,Meng Gu,Minhua Shao
The development of inexpensive and high-performance bifunctional electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is of crucial significance for rechargeable metal-air batteries , but remains challenging. Herein, we report an ingenious bifunctional oxygen electrocatalyst integrating ZIF-derived carbon-anchored Fe/Ni single atoms, FeNi alloy nanoparticles , and graphene support (denoted as Fe/Ni-NC||FeNi@G). Synergizing highly active Fe single atoms for the ORR and highly efficient FeNi alloy nanoparticles for the OER, the as-constructed Fe/Ni-NC||FeNi@G catalyst exhibits outstanding bifunctionality; the potential gap between the OER potential at 10 mA cm –2 and the ORR half-wave potential is only 0.618 V, outperforming the benchmark Pt/C + Ir/C catalyst and most transition metal-based bifunctional catalysts reported in the literature. More importantly, the Fe/Ni-NC||FeNi@G-driven zinc-air battery (ZAB) delivers a maximum power density of ∼200 mW cm –2 , a specific capacity of 876 mAh g –1 , and excellent cycling stability with negligible voltage decay up to 500 hours (3000 cycles). This work provides an effective approach to designing highly efficient non-noble metal multifunctional catalysts for practical applications in rechargeable metal-air batteries.
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Advanced Science
·
2023
·Vol. 10
·期 22
·2301869
·
IF 15.1
Zhiyong Jiang,Xiaodi Zhu,Zhiyu Wang,Wei Liu,Wensheng Yan,Kevin Sivula,Jun Bao
The structural properties of octahedral sites (B Oh ) in spinel oxides (AB 2 O 4 ) play vital roles in the electrochemical performance of oxygen-related reactions. However, the precise manipulation of AB 2 O 4 remains challenging due to the complexity of their crystal structure. Here, a simple and versatile molten-salt-mediated strategy is reported to introduce Ni 2+ in B oh sites intentionally on the surface of zinc ferrite (ZnFe 2 O 4 , ZFO) to promote the active sites for photoelectrochemical (PEC) water splitting. The as-created photoanode (ZFO-MSNi) shows a remarkable cathodic shift of ≈ 450 mV (turn-on voltage of ≈ 0.6 V RHE ) as well as three times the 1-sun photocurrent density at 1.23 V RHE for PEC water oxidation in comparison with bare ZFO. A comprehensive structural characterization clearly reveals the local structure of the introduced Ni 2+ in ZFO-MSNi. Fewer surface trapping states are observed while the precisely introduced Ni 2+ and associated neighboring Fe (3- σ )+ (0< σ <1) sites unite in an edge-sharing octahedral configuration to function as Ni Fe dual active sites for PEC water oxidation. Moreover, open circuit potential measurements and rapid-scan voltammetry investigation give further insight into the enhanced PEC performance. Overall, this work displays a versatile strategy to regulate the surface active sites of photoelectrodes for increasing performance in PEC solar energy conversion systems.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Jiajun Wen,Zhongwu Li,Changsheng Jin,Jia Chen,Changqing Cai
Dissolved organic matter (DOM) or iron/manganese (hydro)oxides were important factors in the migration of Cd in sediments of wetlands. DOM and Fe oxides simultaneously affect the longitudinal and transverse migration of Cd in wetlands sediments of plants was still unclear. In this study, a 14-day rhizobox experiment was conducted and the result showed that the rhizosphere effect of Cd migration was only limited to the upper layer of sediments (− 2 to − 4 cm). Fe with fulvic acid (FA) simultaneously existed can precipitate Cd(II) from supernatant to sediments downward. Fe oxides at sediment concentration could effectively prevent Cd(II) from migrating to root surface (0.21 vs 0.02 at%). While Fe oxides with FA together at sediment concentration could effectively promoted the migration of Cd(II) to root surface (0.07 vs 0.08 at%). The formation of organo-metallic complexes of Fe in the presence of FA profoundly proved this finding (increased by ~33.0%). And the polysaccharides and aromatics in organic matter were the chief functional groups participating in the incorporation of Cd and Fe oxides. The findings reveal the migration rules of Cd(II) in sediments by FA and Fe oxides and give an insight into the mechanisms of Cd(II) migration to the root surface around wetland plants.
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高影响因子
RARE METALS
·
2021
·Vol. 41
·期 4
·1265-1275
·
IF 4.003
Tian Kang-Hui,Duan Chan-Qin,Ma Qun,Li Xing-Long,Wang Zhi-Yuan,Sun Hong-Yu,Luo Shao-Hua,Wang Dan,Liu Yan-Guo
High entropy oxides (HEOs), as a new type of single-phase multielement solid solution materials, have shown many attractive features and promising application prospect in the energy storage field. Herein, six-element HEOs (CoNiZnFeMnLi) 3 O 4 and (CoNiZnCrMnLi) 3 O 4 with spinel structure are successfully prepared by conventional solid-phase method and present outstanding lithium storage performances due to the synergy effect of various electrochemically active elements and the entropy stabilization. By contrast, (CoNiZnFeMnLi) 3 O 4 delivers higher initial discharge specific capacity of 1104.3 mAh·g −1 , better cycle stability (84% capacity retention after 100 cycles at 100 mA·g −1 ) and rate performance (293 mAh·g −1 at 2000 mA·g −1 ) in the half-cell. Moreover, the full-cell assembled with (CoNiZnFeMnLi) 3 O 4 and LiCoO 2 provides a reversible specific capacity of 260.2 mAh·g −1 after 100 cycles at 500 mA·g −1 . Ex situ X-ray diffraction reveals the electrochemical reaction mechanism of HEOs (CoNiZnFeMnLi) 3 O 4 , and the amorphous phase and the large amount of oxygen vacancies were obtained after the initial discharge process, which are responsible for the excellent cycle and rate performance. This research puts forward fresh insights for the development of advanced energy storage materials for high-performance batteries. Graphical Abstract
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危险品化学品经营许可证（带存储）