TALANTA
·
2022
·
IF 6.556
Hao Feng,Fan Wang,Junhua Li,Qian Wu,Ying Cui,Lingzhi He,Xing Liu,Zeng Liu,Dong Qian,Haixia Tong
Lack of highly efficient, inexpensive, and easily available catalysts severely limits the practical applicability of electrochemically sensing assay towards 5-hydroxytryptamine (5-HT). Herein, four kinds of Fe–Co bimetallic Prussian blue analogues (FeCo–PBAs) with different molar ratios of Fe to Co were prepared using a simple coprecipitation method. Interestingly, Fe(III) in K 3 [Fe(CN) 6 ] can be reduced to Fe(II) by adding trisodium citrate dehydrate, which could offer a new clue to synthesize PBAs with Fe(II) core ions. With the optimizational FeCo-PBA synthesized at a 0.5/1 M ratio of Fe to Co as an electrocatalyst , the constructed sensor shows excellent comprehensive performance for the 5-HT assay with a high sensitivity of 0.856 μA μM −1 and an ultralow detection limit of 8.4 nM. Under the optimum conditions, linearity was obtained in the ranges of 0.1–10.0 μM and 10.0–200.0 μM and preferable recoveries ranged from 97.8% to 103.0% with relative standard deviation (RSD) < 4.0%. The integrated properties of FeCo-PBA can be comparable to previously reported electrocatalysts for the 5-HT assay including noble metal-based and expensive carbon (graphene and carbon nanotubes)-based electrocatalysts. The proposed sensor also exhibits outstanding selectivity, reproducibility, and practicality for real sample analyses. This work is the first report on the PBA-based sensor for the 5-HT assay, verifying the practicability of this high-performance sensor for the 5-HT assay.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Feng-Di Tu,Zi-Yun Wu,Pan Guo,Li-Xiao Shen,Zi-Yu Zhang,Yun-Kun Dai,Miao Ma,Jing Liu,Bin Xu,Yun-Long Zhang,Lei Zhao,Zhen-Bo Wang
Platinum group metal (PGM)-free catalysts represented by nitrogen and iron co-doped carbon (Fe-N-C) catalysts are desirable and critical for metal-air batteries , but challenges still exist in performance and stability. Here, cerium oxides (CeO x ) are incorporated into a two-dimensional Fe-N-C catalyst (FeNC-Ce-950) via a host-guest strategy. The Ce 4+ /Ce 3+ redox system creates a large number of oxygen vacancies for rapid O 2 adsorption to accelerate the kinetics of oxygen reduction reaction (ORR). Consequently, the as-synthesized FeNC-Ce-950 catalyst exhibits a half-wave potential ( E 1/2 ) of 0.921 V and negligible decay (<2 mV for Δ E 1/2 ) after 5,000 accelerated durability cycles, significantly outperforming most of ORR catalysts reported in recent years and precious metal counterparts. When applied in a zinc-air battery, it demonstrates a peak power density of 175 mW cm −2 and a specific capacity of 757 mAh g Zn −1 . This study also provides a reference for the exploration of Fe-N-C catalysts decorated with variable valence metal oxides .
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Lan Liang,Guanyi Chen,Jianhui Zhao,Penghui Shao,Ning Li,Mengting He,Qinglong Fu,Beibei Yan,Li-an Hou
The peroxymonosulfate (PMS) process may be hindered severely due to natural organic matter (NOM) conversion in the treatment of emerging pollutants from river water, becoming a critical engineering and technical issue. In this study, a Fe(II)-induced river water (RW)/PMS catalytic system was constructed for investigating molecular transformation of NOM and related influence mechanism to sulfamethoxazole (SMX) degradation. Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS) analysis indicated that NOM molecules containing no more than one heteroatom in river may be attacked by hydroxyl radicals ( OH) and then polymerized, converting into molecules with two or three heteroatoms during PMS oxidation. Based on the correlation analysis, CHONP-NOM, CHOSP-NOM and CHONSP-NOM showed a significant inhibition against SMX degradation, while CHONS-NOM exhibited a moderate inhibitory effect. Besides, more condensed aromatic structures, carbohydrates and tannins were generated via reactive species ( OH and sulfate radicals (SO 4 − )) oxidation, radical addition and polymerization reactions. Notably, condensed aromatic structures, carbohydrates and tannins presented weak, modest and strong inhibition to SMX degradation, respectively. Based on the current results, the inhibition of target pollutants degradation would be mitigated via regulation of NOM molecules in a Fe(II)-induced PMS activation system, providing valuable information to reduce NOM impact. In addition, this study paves the way to achieve efficient removal of emerging pollutants from river water.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yin Li,Jiahui Hu,Yubin Zou,Lin Lin,Hebin Liang,Huaxin Lei,Bing Li,Xiao-yan Li
High-valent iron–oxo species (Fe V =O) generated through peroxide activation by Fe-based catalysts can realize the selective and efficient degradation of organic pollutants in water treatment. However, the rapid and efficient generation of Fe V =O for the selective degradation of pollutants over a wide pH range with high stability is challenging. In this study, a N, P, and S co-doped Fe-single atom (SA) catalyst (Fe SA -NPS@C) with FeN 4 active center was synthesized as a highly efficient catalyst for the peroxymonosulfate (PMS)-based oxidation. The Fe SA -NPS@C catalyst exhibited an excellent catalytic performance at low dosages of both the catalyst and PMS for the degradation of pollutants over a wide pH range with high stability. For the degradation of ofloxacin (OFX), the rate constant pertaining to PMS with Fe SA -NPS@C was 1.68 min −1 , considerably higher than those obtained using the N -doped and N and P co-doped Fe-SA catalysts. The degradation pathway of OFX revealed that the electrostatic effect was of significance in its degradation by Fe V N 4 =O with Fe V N 4 =O being the dominant reactive species. Density functional theory calculations revealed that the heteroatom doping effectively altered the electronic structure of the FeN 4 site of Fe SA -NPS@C, which strengthen its coordination with PMS, promote the electron transfer to PMS, and facilitate the interaction between Fe V N 4 = O and OFX, and thus significantly enhanced its catalytic activity. These findings provide new insights into the oxidation mechanism of Fe V =O in heterogeneous systems and the catalytic ability enhancement through heteroatom doping.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Ying Cai,Jinhong Fan,Zhigang Liu
This study constructed a FeS-based Fenton-like process to explore the degradation of TTC in the presence of copper ions . The acidic condition of pH 3 was more favorable to the H 2 O 2 decomposition and TTC degradation , and it was slightly enhanced by Cu(II). The production of •OH from H 2 O 2 was revealed through radical scavenging and benzoic acid probe experiments, and the ratio of H 2 O 2 decomposition to •OH production was about 1–1.5, which is comparatively consistent with the theoretical ratio. FeS-based Fenton process was proved to be a homogenous system, the slow release of Fe(II) source and the autocatalytic cycle of Fe(III) to Fe(II) resulting from the reductive species of TTC and dissolved S(-II) improved the production of •OH and the degradation of TTC, which was proved by comparing TTC degradation, TOC removal, H 2 O 2 decomposition and Fe(II) concentration with different iron sources (FeS, Fe(II) and Fe(III)) and external addition of dissolved S(-II). The possible degradation pathways of TTC were subsequently inferred according to the detected products by LC-MS. Understanding these autocatalytic processes is essential to reveal the transformation of redox-active substances in environments and may have potential significance in applying FeS-based Fenton-like process for the treatment of wastewater containing reductive organic matters.
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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
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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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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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JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Rongsheng Ning,Heliang Pang,Zhongsen Yan,Zhenyu Lu,Qiankun Wang,Zengling Wu,Wenxin Dai,Lingshan Liu,Zhongsheng Li,Gongduan Fan,Xianzhi Fu
The development of high efficient photocatalysts for antibiotics contamination in water remains a severe challenge. In this study, a novel step-scheme (S-scheme) photocatalytic heterojunction nanocomposites were fabricated from integrating AgCl nanoparticles on the MIL-100(Fe) octahedron surface through facile multi-stage stirring strategy. The S-scheme heterojunction structure in AgCl/MIL-100(Fe) (AM) nanocomposite provided a more rational utilization of electrons (e - ) and holes (h + ), accelerated the carrier transport at the junction interface, and enhanced the overall photocatalytic performance of nanomaterials . The visible-light-driven photocatalysts were used to degrade sulfamethazine (SMZ) which attained a high removal efficiency (99.9%). The reaction mechanisms of SMZ degradation in the AM photocatalytic system were explored by electron spin resonance (ESR) and active species capture experiments, which superoxide radical (•O 2 - ), hydroxyl radical (•OH), and h + performed as major roles. More importantly, the SMZ degradation pathway and toxicity assessment were proposed. There were four main pathways of SMZ degradation, including the processes of oxidation , hydroxylation, denitrification, and desulfonation. The toxicity of the final products in each pathway was lower than that of the parent according to the toxicity evaluation results. Therefore, this work might provide new insights into the environmentally-friendly photocatalytic processes of S-scheme AM nanocomposites for the efficient degradation of antibiotics pollutants.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2022
·
IF 4.598
Xiaoyue Liu,Hongtao Xie,Jian Mao
The porous electrodes derived from Prussian blue analogs (PBAs) show high specific capacity and superior energy densities in supercapacitors due to their tunable chemical compositions, open three-dimensional network framework and large surface area. In this work, La-Fe PBA with different morphologies is prepared at mild conditions via controlling the composition of mixed solvent and the structural evolution of the La-Fe PBA is further explored. The solubility of K 3 [Fe(CN) 6 ] and the influence of ethanol on the crystal growth is used to control the synthesis of La-Fe PBA. Four different morphologies of La-Fe PBA, such as chamfered hexagonal bipyramid microcrystals, hexagonal flakes, erythrocyte-like microstructure and small flakes, are successfully synthesized by changing the ethanol/water ratio of mixed solvent. The porous LaFeO 3 with the same shape is obtained by calcining the La-Fe PBA at 500 °C, which is subsequently employed as electrodes for battery-type supercapacitor. The erythrocyte-like LaFeO 3 shows remarkable specific capacity (330 C g −1 ) at 1 A g −1 , energy density (23.8 Wh kg −1 ) and power density (400 W kg −1 ) at 1 A g −1 . This work could provide a porous material for high-performance supercapacitors as well as an exciting strategy to develop and design materials with specific morphology.
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Journal of Materials Chemistry C
·
2022
·Vol. 10
·期 16
·6252-6262
·
IF 8.067
Zhaoju Yu,Qikun Zhu,Fen Li,Ting Chen,Hanzi Du
In the present work, novel single-source-precursors for CNTs/Fe3Si/Fe/SiOCN ceramic nanocomposites were synthesized by the reaction of poly(methylvinyl) silazane (HTT 1800) with ferric acetylacetonate [Fe(acac)3] and carboxylic functionalized carbon nanotubes (CNTs-COOH), which were characterized by means of Fourier transform infrared spectra. The microstructure, phase evolution, electromagnetic properties and electromagnetic microwave absorbing (EMA) performance of the as-prepared ceramics were investigated in detail. The results reveal that the introduced CNTs and the in situ formed nanocrystallites, including α-Fe, Fe3Si, α-Si3N4, β-Si3N4, Si2N2O, and SiC, are dispersed in an amorphous SiOCN matrix after annealing at 900–1500 °C. The obtained ceramic powders mixed with paraffin wax possess a very low minimum reflection coefficient of −65.3 dB and a broad effective absorption bandwidth of 6 GHz (12–18 GHz) with a thickness of 1.6 mm, indicating outstanding EMA performance. This is due to (i) the increase in interfacial polarization caused by the formation of multiple hetero-interfaces and (ii) the synergistic effect of magnetic and dielectric losses. Therefore, the multicomponent CNTs/Fe3Si/Fe/SiOCN ceramic nanocomposites have promising potential for thin and high-performance EMA materials applied in a harsh environment.
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