CHEMOSPHERE
·
2020
·
IF 5.778
Jing Wang,Lidong Kou,Liang Zhao,Wenjie Duan
The use of waste sludge as a precursor of catalysts for environmental applications has been encouraged during the past few years. In this study, a series of magnetic Fe,N-codoped carbon catalysts (UBC- x ) were successfully prepared by a facile one-pot pyrolysis method using Fe-rich sludge and N-rich urea as the raw materials. By carefully controlling the mass ratio of urea/dry sludge ( x = 0–3), a significant amount of N (1–10 mass%) were incorporated, and the UBC- x catalysts, especially UBC-0.5 and UBC-0.75, could be imparted with high catalytic activity , convenient magnetic separation and high recycle stability. Phenolic contaminants like phenol and bisphenol A (BPA) could be nearly completely removed through peroxymonosulfate (PMS)-induced degradation by using UBC- x as the catalysts under a wide pH range (2–11) and with the co-existence of water constituents (chloride Cl − and sodium humate NaH, 0–50 mM). Among the several reactive oxidative species (ROS), singlet oxygen ( 1 O 2 ) was deemed as the main reactive species responsible for BPA degradation. Both Fe and N active sites contributed to the high catalytic activity of UBC- x , and their coordination made the catalysts rather stable with no significant Fe leaching under a wide pH range. Therefore, after an easy magnetic separation, the UBC- x could be recycled and reused efficiently in another BPA removal cycle. The as-synthesized magnetic Fe,N-codoped carbon catalysts provided a new route for sludge reutilization and showed potential applications in wastewater treatment .
研究领域:
环境科学
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催化
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废水处理
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材料科学
✓ 已验证
DOI
高影响因子
Science Advances
·
2022
·Vol. 8
·期 40
·
IF 14.957
Jingzhong Qin,Bo Han,Xixi Liu,Wen Dai,Yanxin Wang,Huihui Luo,Xiaomei Lu,Jiabao Nie,Chensheng Xian,Zehui Zhang
The cleavage and functionalization of recalcitrant carbon─carbon bonds is highly challenging but represents a very powerful tool for value-added transformation of feedstock chemicals. Here, an enzyme-mimic iron single-atom catalyst (SAC) bearing iron (III) nitride (FeN 3 ) motifs was prepared and found to be robust for cleavage and cyanation of carbon–carbon bonds in secondary alcohols and ketones. High nitrile yields are obtained with a wide variety of functional groups. The prepared FeN 3 -SAC exhibits high enzyme-like activity and is capable of generating a dioxygen-to-superoxide radical at room temperature, while the commonly reported FeN 4 -SAC bearing FeN 4 motifs was inactive. Density functional theory (DFT) calculation reveals that the activation energy of dioxygen activation and the activation energy of the rate-determining step of nitrile formation are lower over FeN 3 -SAC than FeN 4 -SAC. In addition, DFT calculation also explains the catalyst’s high selectivity for nitriles.
研究领域:
催化化学
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有机化学
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材料科学
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理论化学
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可持续化学
✓ 已验证
DOI
高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2016
·
IF 3.926
Qingxiang Zhou,Man Lei,Jing Li,Kuifu Zhao,Yongli Liu
Magnetic Fe@MgAl-layered double hydroxides (MgAl-LDHs) composite was firstly synthesized by coating MgAl-layered double hydroxides on the surface of the dispersed nanoscale zero valent irons with co-precipitation method and characterized by transmission electron microscopy and X-ray diffraction techniques. The synthesized Fe@MgAl-LDHs nanoparticles were investigated for magnetic solid phase extraction (MSPE) of 1-naphthol and 2-naphthol from the water samples. The elutent containing 1-naphthol and 2-naphthol was analyzed by high performance liquid chromatography with variable wavelength detection (HPLC–UV). Under optimal conditions, there is good linear relationship between the concentration and the peak area in the range of 0.5–200 μg L −1 with the correlation coefficients ( r 2 ) above 0.998 for 1-naphthol and 2-naphthol. The limits of detection were 0.22 μg L −1 and 0.19 μg L −1 for 1-naphthol and 2-naphthol, respectively, and precisions were both below 2.5% ( n = 6). The real water analysis demonstrated that the spiked recoveries were in the range of 79.2–80.9% ( n = 3). All these results indicated that the developed MSPE–HPLC–UV method was proved to be an efficient tool for the analysis of naphthols.
研究领域:
环境科学
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分析化学
✓ 已验证
DOI
高影响因子
ACS Applied Nano Materials
·
2021
·
IF 5.097
Ruya Guo,Li Xue,Gaozhe Cai,Wuzhen Qi,Yuanjie Liu,Jianhan Lin
Early screening of Salmonella is of utmost importance to minimize the incidence of related foodborne diseases. Here, we reported an immunosensor to fast detect Salmonella using Fe-MIL-88NH2 metal–organic framework (Fe-MOF) nanocubes to load platinum nanoparticles (PtNPs) for signal amplification and smartphone thermal imaging to monitor the temperature change. The Fe-MOF nanocubes decorated with PtNPs (Fe-MOF/PtNPs) were prepared as peroxidase mimics to catalyze hydrogen peroxide (H2O2) to produce O2. The immune magnetic nanoparticles (MNPs), the target bacteria, and the immune Fe-MOF/PtNPs were first mixed by the three-dimensional (3D) chaotic micromixer and conjugated in the microfluidic chip to form MNP–bacteria–Fe-MOF/PtNPs sandwich complexes. After magnetic separation and washing, H2O2 was injected and decomposed by Fe-MOF/PtNPs on the sandwich complexes to generate O2 in a sealed chamber. The increase in the pressure pushed the preloaded water to react with calcium oxide powder, resulting in the generation of heat, which was measured using the smartphone-based thermal sensor to determine the bacteria. The microfluidic immunosensor could detect Salmonella as low as 93 CFU/mL within 1 h.
研究领域:
生物传感器
·
纳米技术
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微流控技术
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食品安全
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生物医学工程
✓ 已验证
DOI
高影响因子
RSC Advances
·
2023
·Vol. 13
·期 20
·13902-13910
·
IF 3.9
Jing Tian,Weixin Qian,Haitao Zhang,Hongfang Ma,Weiyong Ying
In this paper, catalysts with different aluminum contents were prepared by a co-precipitation method using LDHs (layered double hydroxides) as the precursors through the adjustment of Cu2+ : Fe2+, and the catalysts were named LDO catalysts. The effect of aluminum on CO2 hydrogenation to methanol was investigated by evaluating the characterization. With the addition of Al, Ar physisorption results showed an increase in BET-specific surface area, TEM demonstrated a decrease in catalyst particle diameter, XRD showed that Cu and Fe existed in the catalyst mainly in the form of CuFe2O4 and CuO, XPS demonstrated a decrease in electron cloud density and an increase in base sites and oxygen vacancies, and CO2-TPD and H2-TPD results indicated that Al promoted the dissociation and adsorption of CO2 and H2. When the reaction temperature was 230 °C, the pressure was 4 MPa, H2/CO2 = 2.5 and the space velocity was 2000 ml (h gcat)−1, the best conversion (14.87%) and the highest methanol selectivity (39.53%) of the catalyst were obtained at 30% aluminum content.
研究领域:
催化
·
化学工程
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
FUEL
·
2025
·
IF 7.5
Lina Dai,Qiang Li,Xianglan Dong,Enqi Zhang,Yufeng Hu,Xin Guo,Yanduo Liu
Photocatalysis exhibits great potential for applications in solving energy and environmental problems, and has received widespread attention. This article constructs a new type of Mn-Fe Prussian blue analogues S-scheme mechanism photocatalytic material. The material is composed of oxidized photocatalysts (Ag 2 MoO 4 ) and reduced photocatalysts (Mn-Fe PBAs). The composite photocatalyst constructed in this way shows advantages such as a wide spectral response range, high charge carrier separation efficiency, and strong oxidation–reduction ability, which can significantly enhance photocatalytic efficiency. By studying the construction method and CO 2 reduction performance of the photocatalyst, the structure-performance relationship can be clarified. The CO production rate is 43.3 μmol/g/h, and the selectivity can reach 94.9 %, which is far superior to the current mainstream photocatalytic system. The electron transfer kinetics and S-scheme charge separation mechanism between the Mn-Fe PBAs and Ag 2 MoO 4 interfaces are explained by steady-state surface photovoltage spectroscopy (SS-SPS) and near ambient pressure XPS (NAP-XPS). In-situ DRIFTS techniques are used to monitor the changes of transition intermediates, and combined with theoretical calculations, the activation mechanism of CO 2 by the Mn-Fe catalytic site is deeply revealed at the atomic level. This study provides new theoretical guidance and profound insights for the construction of Prussian blue analogues photocatalysts.
研究领域:
材料科学
·
环境科学
·
物理化学
·
纳米技术
·
催化
·
能量转换
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Wenyu He,Jinhui Wei,Ting Huang,Enren Zhang
For practical applications of microbial fuel cells (MFCs), 5H-dibenz [b,f] azepine-5-carboxamide (Carbamazepine, CBZ) was used as the organic precursor for the synthesis of catalysts composed of Fe–N–C complexes (named as Fe-CBZ-Cats) through a sacrificial support method. Characterizations by SEM, XPS and TEM-EDS elemental mapping show that the synthesized Fe-CBZ-Cats have porous structure and uniformly dispersed Fe/N/C complex centers which could play key roles in effective ORR . Linear scanning voltammetry (LSV) measurements show that the synthesized Fe-CBZ-Cats exhibits ORR activity comparable to commercial Pt/C catalysts under the same catalyst loading (2 mg cm −2 ). The maximum power density produced by cathode-limiting MFCs with Fe-CBZ-Cats air cathodes was 431 ± 23 μW cm −2 , higher than those in the control MFCs with Pt/C air cathodes (403 ± 13 μW cm −2 ) and activated carbon air cathodes (296 ± 24 μW cm −2 ). In addition, the toxicity tolerance of the synthesized Fe-CBZ-Cats is much higher than Pt/C.
研究领域:
环境科学
·
电化学
·
生物工程
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Zhujun Huang,Zhan Lai,Dongying Zhu,Haiyan Wang,Chenxi Zhao,Guihua Ruan,Fuyou Du
The electrospun graphene oxide/MIL-101(Fe)/poly(acrylonitrile- co -maleic acid) nanofibers (E-spun GO/MIL-101(Fe)/PANCMA NFs) were fabricated by a facile electrospinning method and used as integrated photocatalytic adsorbents (IPAs) to remove dye pollutant from water samples. Compared with E-spun GO/PANCMA and E-spun MIL-101(Fe)/PANCMA NFs, the fabricated E-spun GO/MIL-101(Fe)/PANCMA NFs exhibited higher adsorption ability and excellent photocatalytic activity towards a model pollutant Rhodamine B (RhB). Under the optimized conditions, the as-prepared IPAs achieved almost complete adsorption of RhB within 15 min with the maximum adsorption capacity of 10.46 mg/g. Under visible-light irradiation, 93.7% of RhB in 20 mL water sample was degraded within 20 min, and the degradation kinetics of RhB fitted well with the first-order kinetic model. In addition, LC-MS analysis of the RhB degradation products confirmed the degradation pathways, and the generated •OH radicals played important roles in the degradation process. Importantly, the E-spun GO/MIL-101(Fe)/PANCMA NFs exhibited good reusability and could be reused for consecutive 20 cycles, which make them promising candidate materials in the field of industrial applications and environmental remediation.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yuchen Li,Zhen Chen,Guoxiong Zhan,Bingling Yuan,Lidong Wang,Junhua Li
Catalytic amine-based solvent regeneration with solid acid is a feasible option for reducing energy consumption of CO 2 capture, but facing crucial challenges on designing material structures and understanding reaction mechanisms. Herein, we cover the nanoscale NiFe 2 O 4 cluster with covalent organic frameworks (COFs), to prepare solid acid catalysts. The pristine chemical bonds of Ni(Fe)-O and Ni(Fe)-Ni(Fe) are substituted by Ni(Fe)-N and Ni(Fe)-N-Ni(Fe) by targeting the anchoring of NiFe 2 O 4 cluster over COFs. The created coordination state stimulates the production of Brønsted acid sites. The obtained nanomaterials achieve a considerable improvement in CO 2 desorption of up to 290.1 mmol/(min·g) at 88 °C for spent monoethanolamine (MEA) solvent, representing a substantial increase of 540% relative to traditional thermal desorption. Consequently, the energy consumption of MEA generation is reduced by approximately 58%. Intermediate species (HCO 3− , CO 3 2− , and RNHCOO − ) and reaction pathways are established by combining operando Raman spectroscopy and ex situ 13 C NMR spectrum measurements. Theoretical calculations are performed to clarify the transformation mechanism of the acid sites around Ni/Fe atoms and its intrinsic role in the adsorption equilibrium of solvent regeneration.
研究领域:
环境科学
·
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2024
·Vol. 27
·期 24
·e202400196
·
IF 2.2
Wenkang Mao,Jinjing Ju,Dan Li,Daishe Wu,Feigao Xu
Graphical Synopsis: A pyrrolic N-rich g-C 3 N 4 (PN-g-C 3 N 4 ) framework is synthesized with transition metal M (M=Fe, Co, Ni, Cu, Cr, and Mn) atomic sites coordinated onto it. M/PN-g-C 3 N 4 are constructed for peroxodisulfate activation. The synergy between photocatalysis and Fe/PN-g-C 3 N 4 catalyst results in increased generation and separation of charge carriers, along with the cyclic transformation of the Fe 3+ /Fe 2+ couple. Photocatalysis is an efficient technology for the degradation of pollutants. However, there is still much room for improvement in its degradation efficiency. In this study, a pyrrolic N-rich g-C 3 N 4 (PN-g-C 3 N 4 ) framework was synthesized with transition metal M (M=Fe, Co, Ni, Cu, Cr, and Mn) atomic sites coordinated onto it. Then, a series of single atomic metals M anchored to PN-g-C 3 N 4 (M/PN-g-C 3 N 4 ) are constructed for peroxodisulfate activation. Their order of catalytic activity follows Fe>Cr>Ni>Cu≈Co>Mn, in particular the degradation rates of the TCH for Fe-PN-g-C 3 N 4 are 3.74 times higher than that of undoped PN-g-C 3 N 4 . These carefully regulated pyrrolic N-rich Fe sites demonstrate outstanding performance in degrading organic pollutant. As an exemplary model, the Fe/PN-g-C 3 N 4 catalyst efficiently drives the catalytic oxidation of TCH through Fenton-like reaction under visible light, showcasing exceptional cycle stability and a broad effective pH range of 3.0–11.0. The synergy between photocatalysis and Fe doped catalysis results in increased generation and separation of charge carriers, along with the cyclic transformation of the Fe 3+ /Fe 2+ couple. This combination significantly enhances the Fenton-like performance, making it a highly effective process for pollutant degradation.
研究领域:
环境科学
·
催化
·
材料科学
·
化学工程
·
水处理技术
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Limeng Yang,Wendou Chen,Cuihong Sheng,Hailiang Wu,Ningtao Mao,Hui Zhang
Peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) are encouraging methods for wastewater treatments, but the recycling of used PMS activators in powder form from the wastewater treatment system is still problematic. In this paper, we designed a novel and highly effective carbocatalyst for PMS activation, which was achieved by pyrolyzing the hybrids of metal–organic framework MIL-101(Fe) and dicyandiamide immobilized on the surface of carbon cloth (CC), and a facile route for the preparation of fibrous catalysts was developed. The resultant CC loaded with Fe/N-codoped carbocatalyst exhibited desirable reusability and good stability for the degradation of organic dyes. The mechanism of the novel Fe/N-codoped carbocatalyst for PMS activation including the specific roles of N species and Fe-N binding was investigated. It was demonstrated in electrochemical impedance spectroscopy (EIS) results that the CC facilitated the electron transport of the carbocatalyst in AOPs. It was shown in the radical quenching and electron paramagnetic resonance (EPR) experiments that both the radical and non-radical pathways were accountable for the degradation of contaminants, and the non-radical path was principal. It was also evident in the X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) results that pyridinic N and graphitic N were the main active species for PMS activation.
研究领域:
环境科学
·
催化
·
水处理
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2022
·
IF 4.598
Wei-Chang Chen,Xiao-Shuang Guo,Ze-Yu Liu,Chuan-Qing Huang,Jian-Shan Ye,Hai-Yang Liu,Xin-Yan Xiao
Fe-based nanoparticles encapsulated in carbon can effectively promote the ORR activity of the neighboring Fe–N x and prevent the dissolution of metal nanoparticles to ensure the long-term durability of catalysts. Herein, we employed a facile two step pyrolysis strategy to construct “plane-active sites” structure, namely FeO y nanoparticles embedded in carbon were loaded on two dimensional (2D) porous carbon with exposed abundant Fe–N x active sites (FeOy@C/Fe-N x /C). The optimized FeO y @C/Fe-N x /C catalyst with low Tafel slope (48 mV dec −1 ) and nearly-four-electron selectivity (3.91–3.97) showed excellent performance towards ORR with a more positive shift of 15 mV of half-wave potential (E 1/2 = 0.856 V) than that of commercial Pt/C (E 1/2 = 0.841 V) in alkaline solution, and also had a superior long-term stability and methanol resistance as compared with commercial Pt/C. The excellent electrochemical performance of FeO y @C/Fe-N x /C can be attributed to FeO y @C structure, exposed abundant Fe–N x active sites and two dimensional porous carbon with a large specific surface area.
研究领域:
材料科学
·
电化学
·
纳米技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）