ANALYTICA CHIMICA ACTA
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2023
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IF 6.2
DanDan Yang,Jingqi Chen,Yuting Huang,Ganghui Chen,Xueliang Liu,Xuan Wang,Like Yang,Zhaohui Li,Jie Hu,Qi Zhou,Jia Ge,Yu Yang
The development of cost-effective and easy-to-use strategies for the detection of ascorbic acid (AA) and acid phosphatase (ACP) is in high demand but challenging. Thus, we report a novel colorimetric platform based on Fe–N/C single atom nanozyme with efficient oxidase mimicking activity for their highly sensitive detection . The designed Fe–N/C single atom nanozyme can directly oxidize 3,3′,5,5′-tetramethylbenzidine (TMB) to produce a blue oxidation product (oxTMB) in the absence of H 2 O 2 . In addition, L-ascorbic acid 2-phosphate can be hydrolyzed to ascorbic acid in the presence of ACP, which inhibits the oxidation reaction and results in a significant bleaching of the blue color. Based on these phenomena, a novel colorimetric assay with high catalytic activity was developed for the determination of ascorbic acid and acid phosphatase with detection limits of 0.092 μM and 0.048 U/L, respectively. Notably, this strategy was successfully applied to the determination of ACP in human serum samples and evaluate ACP inhibitors, indicating its potential as a valuable tool for clinical diagnosis and research.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Shiyu Zhang,Mengru Li,Jingwen Wang,Ruonan Zhang,Xiaoyu Ma,Haisheng Tao
Metal-organic frameworks with high porosity have received much attention in environmental pollutant treatment. This study presented a simple single-pot solvent thermal method for the preparation of a bimetal-organic framework MIL-53(Fe,Ni), further used for activated peroxydisulfate to degrade rhodamine B (RhB). The morphology and structure of the sample were characterized by scanning electron microscopy, transmission electron microscopy , x-ray diffraction, photoelectron spectroscopy , fourier transform infrared spectroscopy , and thermogravimetric analysis . The results showed that MIL-53(Fe,Ni) was successfully synthesized by the simple reaction, with high thermal stability and high specific surface area. The effects of pH value, co-existing ions, temperature, humic acid and different real water samples on RhB degradation were systematically investigated. Under optimized conditions, 93.9% of RhB was degraded within 180 min, together with excellent reusability. Quenching experiments and electron paramagnetic resonance showed that both free radicals (∙OH, SO 4 ∙- and O 2 ∙- ) and non-free radicals ( 1 O 2 and direct charge transfer) were responsible for the RhB degradation. In addition, the identification of intermediates by high-resolution mass spectrometer and reaction site prediction calculations (electrostatic potential, Fukui function and molecular orbit analysis), proposing a possible degradation pathway of RhB. The work highlights the broad applications of bimetal-organic frameworks in advanced oxidation processes .
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MOLECULES
·
2023
·Vol. 28
·期 8
·3445
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IF 4.6
Lei Zhang,Heng Liu,Jiaqi Zhu,Xueling Liu,Likun Li,Yanjun Huang,Benquan Fu,Guozhi Fan,Yi Wang
A novel pyridine-modified chitosan (PYCS) adsorbent was prepared in a multistep procedure including the successive grafting of 2-(chloromethyl) pyridine hydrochloride and crosslinking with glutaraldehyde. Then, the as-prepared materials were used as adsorbents for the removal of metal ions from acidic wastewater. Batch adsorption experiments were carried out to study the impact of various factors such as solution pH value, contact time, temperature, and Fe (III) concentration. The results showed that the absorbent exhibited a high capacity of Fe (III) and the maximum adsorption capacity was up to 66.20 mg/g under optimal experimental conditions (the adsorption time = 12 h, pH = 2.5, and T = 303 K). Adsorption kinetics and isotherm data were accurately described by the pseudo-second-order kinetic model and Sips model, respectively. Thermodynamic studies confirmed that the adsorption was a spontaneous endothermic process. Moreover, the adsorption mechanism was investigated using Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). The results revealed the pyridine group forms a stable chelate with iron (III) ions. Therefore, this acid-resistant adsorbent exhibited excellent adsorption performance for heavy metal ions from acidic wastewater compared to the conventional adsorbents, helping realize direct decontamination and secondary utilization.Keywords:acidic wastewater;heavy metal ions;pyridine-modified chitosan adsorbent;adsorption mechanism
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LANGMUIR
·
2023
·
IF 3.9
Jie Ying,Zhen-Zhao He,Jiang-Bo Chen,Yu-Xuan Xiao,Xiao-Yu Yang
Many attempts have been made to enhance the relatively poor electrochemical activity of Ni3S2 for the oxygen evolution reaction (OER) by elevating the d-band center. Unfortunately, only limited success has been encountered thus far. Owning to the lower electronegativity and one less 3d electron relative to Ni, Fe shows great potentials in upshifting the overall d-band center of Ni3S2 when incorporating into its crystal structures. Herein, to enhance the intrinsic activity by elevating the d-band center, Ni3S2 nanosheets incorporated with suitable Fe content have been fabricated by a facile one-step solvothermal method. The obtained Fe-incorporated Ni3S2 catalyst exhibits an outstanding OER performance in alkaline media, only requiring 244 mV overpotential (with a reduction of 210 mV compared to Ni3S2) at 50 mA cm–2 in 1 M KOH and without obvious degradation after sustaining for a 60 h test at a voltage above 1.5 V. Ultraviolet photoemission spectroscopy and density functional theory calculations consistently demonstrate that the superior performance of Fe-incorporated Ni3S2 is attributed to the upshift of the d-band center on neutralizing the electron densities of Ni, which optimize greatly the adsorption energy of the intermediate (OOH*) in the rate-determining Volmer step.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Haiying Li,Shishuai Sun,Wen Cui,Xiaolan Li,Chuanjia Kou,Zhihui Xu,Zhihui Zhang
Reasonably regulating the dimensionality and interface of an electrode material can effectively improve its surface chemical reactivity, charge transfer rate, and ion transport performance, which is crucial to solving several problems with supercapacitors , including low energy density and poor cycle stability. The multidimensional hybrid morphology of Co-Fe carbonate hydroxide (CH) coupled with Co-Mn layered double hydroxide (LDH) is generated directly on the nickel foam substrate by a two-stage process. The prepared multidimensional hybrid materials with pore morphology with the synergistic effect of 1D nanorods , 2D nanosheets , and 3D “porous coral” not only ensure sufficient contact between the electrolyte and electrode material but also enhance the charge transfer and ion diffusion of the electrolyte. The strong coupling effect of Co, Fe, and Mn metals between the heterojunction surface can produce various ionic valence states and high conductivities, resulting in increased redox activity, which thus improves the electrochemical performance. The results of the electrochemical performance test show that when the current density is 10 mA cm −2 , the high area-specific capacitance of 7.33 F cm −2 is two times (3.85 F cm −2 ) that of a Co-Fe CH electrode and five times that of a Co CH electrode. The quasi-solid state asymmetric supercapacitor with a Co-Fe-Mn positive electrode and an active carbon negative electrode displays an energy density of 0.723 mWh cm −2 at a power density of 8.53 mW cm −2 . After 5500 cycles, the apparatus exhibits 101.72 % of the initial capacitance, which can effectively drive small electrical appliances. The results indicate that the supercapacitor exhibits excellent cycle stability and application potential in energy storage.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Jing Wei,Zhigang Zheng,Lin Zhao,Zhaoguo Qiu,Dechang Zeng
Fe-based metallic glasses (Fe MGs ) are popular reductants for the restoration of wastewater containing various pollutants, but it still suffers from surface passivation and a narrow applicable pH range. In this work, pyrite, an abundant iron sulfide , was used to enhance the reactivity of Fe MGs for the removal of azo dye . Synergetic effects between pyrite and Fe MGs improved the removal of Orange II when using an Fe MGs /pyrite mixture, where the reaction rate constant k obs was 0.218 min −1 , which was higher than when using Fe MGs alone (0.114 min −1 ). Orange II was removed at pH 0 ranging from 5.0 to 10.0 in the presence of pyrite, while it was inefficiently removed by Fe MGs alone (10 g/L) at pH 0 10.0. Mechanistic investigations showed that the synergistic effect between Fe MGs and pyrite enhanced the surface corrosion of Fe MGs and accelerated the Fe 3+ /Fe 2+ redox cycle to generate more sorbed Fe 2+ , which was the dominant reactive species during Orange II removal. This study proposes an approach for enhancing the removal of dye wastewater by using Fe MGs to treat mine waste.
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Environmental Science-Nano
·
2023
·Vol. 10
·期 5
·1284-1296
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IF 7.3
Yuxuan Lin,Weihua Qin,Yuwei Lu,Mingye Ren,Pan Gao,Feng Xiao,Shaoxia Yang
Improving the performance of single-atom catalysts (SACs) is still challenging in Fenton-like reactions for degrading refractory organic pollutants. Here, we designed P and N co-doped Fe SACs to regulate the electronic structure of Fe active sites and enhance the reaction kinetics of peroxymonosulfate (PMS) activation. The obtained heteroatom-doped Fe SACs for the first time exhibited an ultra-low activation energy (ca. 3.7 kJ mol−1) and excellent degradation efficiency for bisphenol A (BPA) in a wide pH range (4.3–9.2). The superior reaction kinetics of the Fe SACs were attributed to enriching the electron density of atomic Fe and then forming dual electron-rich/-deficient sites, which accelerated the electron transformation to generate reactive oxygen species (ROS). In this study the heteroatom-doped Fe SACs with rapid reaction kinetics are achieved, and provides an idea to design SACs with superior performance in heterogeneous Fenton-like reactions.
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Frontiers in Chemistry
·
2023
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IF 5.5
Chang Yongliang,Wu Xiawei,Lu Shengwei,Du Jiahao,Long Yixiu,Zhu Yefei,Qin Huanlong
Inflammatory bowel disease (IBD) is an idiopathic chronic inflammatory bowel disease characterized by inflammation, intestinal barrier injury, and imbalance of gut microbiota. Excess accumulation of reactive oxygen species (ROS) is closely correlated with the development and reoccurrence of IBD. Previous researches demonstrate that procyanidin, as a natural antioxidant, exhibits strong ability of eliminating ROS, thus showing good therapeutic effects in the inflammation-related diseases. Non-etheless, its poor stability and solubility always limits the therapeutic outcomes. Here, we typically designed an antioxidant coordination polymer nanoparticle using the engineering of procyanidin (Pc) and free iron (Fe), named Pc-Fe nanozyme, for effectively scavenging ROS and further inhibiting inflammation while altering the gut microbiome for the treatment of colitis. Furthermore, in vitro experiments uncover that Pc-Fe nanoparticles exert strong multi biomimic activities, including peroxidase, and glutathione peroxidase, for the scavenging of ROS and protecting cells from oxidative injury. In addition, the colon accumulation of Pc-Fe nanozyme effectively protects the intestinal mucosa from oxidative damage while significantly downregulates pro-inflammatory factors, repairs the intestinal barriers and alternates gut microbiome after orally administrated in sodium dextran sulfate (DSS) induced colitis mice. The results collectively illustrate that the multienzyme mimicking Pc-Fe nanozyme owns high potential for treating IBD through scavenging ROS, inhibiting inflammation, repairing gut barriers and alternating gut microbiome, which further promising its clinical translation on IBD treatment and other ROS induced intestinal diseases.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Xiang-Yu Wang,Meng Zhu,Qing-Nan Bian,Ben-Shuai Guo,Wei-Qing Kong,Chong-Bin Wang,Yuan-Yuan Feng
Hydrogen, carrying a high energy density and emitting zero greenhouse gases when in use, is particularly promising as an alternative for traditional fossil fuels. Electrochemical water splitting is an economical technology for producing sustainable and high-purity hydrogen gas. However, the intrinsically sluggish kinetics of the anode oxygen evolution reaction (OER) always decreases the efficiency of hydrogen production; the development of highly active and durable electrocatalysts with improved OER kinetics is thus desirable and crucial. Herein, Fe-based metal–organic framework (MOF)-Ni3S2 heterostructure nanocomposites are synthesized on a nickel foam (NF) substrate. The self-supporting Fe MOF-Ni3S2/NF catalyst shows excellent catalytic activities for OER. In alkaline media (1.0 M KOH), only 243 mV of overpotential is needed to reach the current density of 100 mA·cm–2. Even at the commercially viable high current densities of 500 and 1000 mA·cm–2, ultralow overpotentials of 283 and 309 mV are required, respectively. The catalytic activity of Fe MOF-Ni3S2/NF far exceeds that of the noble metal catalysts (e.g., RuO2) and most non-noble metal OER catalysts reported in the literature. In addition, the Fe MOF-Ni3S2/NF nanocomposite exhibits ultrahigh long-term stability at high current densities, with almost no activity attenuation in the chronopotentiometry test conducted at 100 mA·cm–2 and a negligible attenuation (23 mV) at 500 mA·cm–2 for 20 h. Our findings provide insights into designing and preparing cost-effective, highly active, and durable electrocatalysts for OER at high current densities.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Jiakang Wan,Ling Wang,Wentao Xu,Zehai Xu,Junsheng Yuan,Guoliang Zhang
Design and synthesis of high-efficiency and stable heterogeneous catalysts for the electro-Fenton process remain challenging. In this study, a co-doped Ce and N metal–organic framework MIL-101(Fe) heterogeneous catalyst (Ce/N-MIL-101(Fe) was synthesized by a facile one-step solvothermal method. Polyvinyl pyrrolidone played dual roles during the fabrication process, which not only acted as a nitrogen source for doping but also prevented MIL-101(Fe) molecules from aggregating and reinforcing the formation crystal with a complete polyhedral crystal shape. The introduction of Ce significantly enhanced the density of active sites and promoted the Fe3+/Fe2+ cycle of the reaction system. Owing to the specific structure and properties, the rate of electron transfer in the catalytic process was significantly promoted. The synthesized Ce/N-MIL-101(Fe) catalyst exhibited a high degradation rate for dyes (>98%) with competitive stability and reusability. Moreover, compared with common electro-Fenton catalysts usually operated in a limited pH range of 3.0–6.0, the working pH range of Ce/N-MIL-101(Fe) was widened up to 10.0. The design concept for producing abundant active sites with co-doping into frameworks can be extended to more heterogeneous electro-Fenton catalysts constituted by other porous materials.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2019
·
IF 4.084
Jianshuo Zhang,Kun Hou,Qianqian Yao,Chuxin Wu,Meihua Huang,Lunhui Guan
Transition metal phosphides represent a class of promising electrocatalysts for electrochemical water oxidization and other energy conversion reactions. In this work, we report a novel seal strategy, followed by a second step phosphorization treatment, produces Ni-Fe-P heterostructure directly grown on nickel foam that shows highly catalytic activity for electrochemical water oxidation . The as-prepared catalyst exhibits an excellent electrocatalytic activity , manifested by a current density of 20 mA cm −2 with a very low overpotential (260 mV) for oxygen evolution reaction along with an extremely small Tafel slope of 27 mV decade −1 and a very excellent durability of 120 h in alkaline solution. The excellent performance with exceptional durability owe much to the synergistic effect between the Ni-Fe-P heterostructure and the outer oxidized layer. Remarkably, a current density of 10 mA cm −2 was reached at a low cell voltage of 1.63 V when the original electrode and surface oxidized electrode are used as cathode and anode , respectively.
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CARBON
·
2019
·
IF 7.466
Yu-Jiao Zhang,Jin Qu,Qiu-Yu Ji,Ting-Ting Zhang,Wei Chang,Shu-Meng Hao,Zhong-Zhen Yu
The loss and sluggish kinetics of intermediate polysulfides in electrochemical processes seriously reduce electrochemical activity of sulfur in lithium-sulfur batteries (LSBs). Herein, we design and synthesize freestanding graphitized carbon interlayers decorated with Fe/Fe 3 C nanocatalysts by thermal treatment of cellulose paper with adsorbed ferric nitrate at 1000 °C, during which the freestanding carbon network derives from the cellulose paper while the Fe results from the reduction of Fe 3+ with a carbothermal reduction process; simultaneously, the in situ formed Fe boosts graphitization of carbon to enhance electrical conductivity of the interlayer, and the carbon network effectively helps confine and accommodate Fe/Fe 3 C nanoparticles . Therefore, the well dispersed Fe/Fe 3 C nanoparticles catalytically accelerate electrochemical conversion of polysulfides, while the enhanced conductive network of carbon benefits the electron transfer during the electrocatalytic process. The cell with an optimal carbon/Fe/Fe 3 C interlayer delivers excellent cyclability and rate performances. At current densities of 0.2C and 2C, the specific capacities are close to 1000 and 735 mA h g −1 , respectively. Even after 200 cycles at 1C, the reversible specific capacity is still 772 mA h g −1 . Such a synergistic catalytic interlayer with an enhanced conversion kinetic towards polysulfides provides a new approach for improving electrochemical performances of LSBs.
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