Catalysis Science & Technology
·
2021
·Vol. 11
·期 19
·6507-6515
·
IF 6.119
PanPan Xu,Liuxue Zhang,Xu Jia,Hao Wen,Xiulian Wang,Suqing Yang,Juxian Hui
Compared to the current commercial three-step production process involving low phenol yield, low atomic efficiency, and the formation of explosive intermediates, the direct oxidation of aromatic hydrocarbon to more desirable and important chemical industry intermediate such as phenol offers a more attractive and challenging pathway. Here, we report the selective photocatalytic hydroxylation of benzene to phenol using NH2-MIL-88/PMo10V2-3 as the catalyst and H2O2 as a mild oxidant. Heteropoly acid (PMo10V2) was immobilized to metal–organic frameworks (NH2-MIL-88), where PA anions play an essential role in anchoring NH3+ cations to form stable heterogeneous photocatalysts. The reaction offered a high selectivity of 99% with a yield of 24% for phenol under optimum reaction conditions. Comprehensive characterizations and experiments disclosed a multistep reaction mechanism in which high dispersion of PMo10V2, the production of hydroxyl radical(˙OH) and the formation of V5+/V4+ redox pairs are responsible for the activity of the reaction in the presence of electrons (e−). The recycling experiments were essential in confirming the reusability of the catalyst, and FT-IR characterization analysis also proved the integrity of NH2-MIL-88/PMo10V2-3 after three cycles. This work provides potential applications in the green and highly efficient photocatalytic synthesis of other organic compounds and other environmental applications.
研究领域:
化学
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环境科学
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材料科学
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DOI
高影响因子
Analytical Methods
·
2021
·Vol. 13
·期 48
·5830-5837
·
IF 2.896
Shouhui Chen,Jingguo Yu,Zhen Chen,Zhenzhong Huang,Yonghai Song
The presence of Cd2+, Pb2+, Cu2+ and Hg2+ in drinking-water can be harmful to human health, even if their concentration is fairly low. Hence, it is significant to detect these heavy metal ions in sewage to evaluate the quality of water. Herein, amino-functionalized metal–organic frameworks (NH2-MIL-88(Fe)) embedded with graphitic carbon nitride (g-C3N4) nanosheets and acid-functionalized carbon nanotubes were prepared via a one-pot synthesis. The composite can be directly modified on the surface of glass carbon electrodes without the assistance of Nafion or other binders. The modified glass carbon electrodes can be used to simultaneously detect Cd2+, Pb2+, Cu2+ and Hg2+ in water via square wave stripping voltammetry. The doping of g-C3N4 in the composite, rich in N-containing functional groups, participates in the adsorption of metal ions on the surface of the electrodes. The porous composite provides accommodation room for metals generated by electro-reduction. The detection limit for Cd2+, Pb2+, Cu2+ and Hg2+ is 39.6 nM, 7.6 nM, 11.9 nM, and 9.6 nM, respectively. And the sensitivity for Cd2+, Pb2+, Cu2+ and Hg2+ is 0.0789 mA μM−1 cm−2, 0.4122 mA μM−1 cm−2, 0.2616 mA μM−1 cm−2, and 0.3251 mA μM−1 cm−2, respectively. This work not only enriches the functional design of Fe-MOF materials, but also develops a method for the determination of metal ions using the adsorption sites in g-C3N4.
研究领域:
环境科学
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材料科学
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分析化学
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DOI
PubMed
高影响因子
RENEWABLE ENERGY
·
2025
·
IF 9.1
Jingchuan Guo,Yan Gao,Xuankai Cao,Linxuan Li,Xin Yu,Shidan Chi,Haoyu Liu,Guohong Tian,Xudong Zhao
The technology of using electricity generated from renewable energy sources such as wind and solar power for water electrolysis to produce hydrogen has achieved high efficiency, high purity, and environmental friendliness. However, its further development is constrained by the high overpotential of the oxygen evolution reaction (OER) and the high cost of precious metal catalysts. The methanol oxidation reaction (MOR) as an alternative to OER can significantly reduce overall energy consumption and accelerate the hydrogen evolution reaction. This study innovatively utilizes the metal-organic framework (MOF) of NH₂-MIL-88(Fe) to introduce Ni doping, preparing a series of Fe x Ni y -MOF and their bimetallic carbon derivatives (Fe x Ni y /C) through solvothermal synthesis and high-temperature carbonization. Results show that FeNi₂/C exhibited excellent performance in OER, with a Tafel slope of 38.69 mV·dec⁻ 1 and an overpotential of 335 mV at 10 mA cm⁻ 2 , comparable to RuO₂. In MOR, the overpotential was 193 mV, reduced by approximately 140 mV compared to OER, with outstanding stability. The catalytic mechanism was analyzed using ion chromatography, revealing the key role of Ni doping in enhancing catalytic activity and stability. This study provides new strategies for improving the electrocatalytic hydrogen production efficiency of renewable energy and reducing the production cost of hydrogen energy.
研究领域:
材料科学
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能源化学
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催化化学
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DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2017
·
IF 3.012
Shuo Duan,Yuming Huang
A novel electrochemical sensor was developed for the sensitive and selective detection of Cu 2 + , Pb 2 + and Cd 2 + , which was based on NH 2 -MIL-88(Fe)-rGO composite modified glass carbon electrode (NH 2 -MIL-88(Fe)-rGO/GCE). The NH 2 -MIL-88(Fe)-rGO composite was facilely prepared by a one-step method and characterized by SEM, XRD, Raman spectrum and electrochemical methods. The stepwise GCE modified process was investigated by cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). The electrochemical behaviors of Cu 2 + , Pb 2 + and Cd 2 + ions on the NH 2 -MIL-88(Fe)-rGO/GCE were explored by differential pulse anodic stripping voltammetry (DPASV). It was found that NH 2 -MIL-88(Fe)-rGO was capable of adsorbing Cu 2 + , Pb 2 + and Cd 2 + ions from aqueous solutions and the NH 2 -MIL-88(Fe)-rGO/GCE could enhance the electrochemical responses of Cu 2 + , Pb 2 + and Cd 2 + effectively. Important operational parameters such as electrolyte pH and deposition time were investigated and optimized for the determination of trace Cu 2 + , Pb 2 + and Cd 2 + ions. Under the optimum conditions, the proposed electrochemical sensor had a linear range of 0.005––0.3 μM for Cd 2 + , 0.01–0.3 μM for Pb 2 + and 0.005–0.05 μM for Cu 2 + , respectively. The limits of detection (LODs) are 4.9 nM for Cd 2 + , 10 nM for Pb 2 + and 3.6 nM for Cu 2 + , respectively. The proposed method has been successfully applied to determine three metal ions in water samples. The developed sensor promises simple preparation, fast operation, good sensitivity and excellent reusability, showing great potential for monitoring of water quality.
研究领域:
分析化学
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环境科学
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材料科学
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DOI
高影响因子
MICROCHIMICA ACTA
·
2022
·Vol. 189
·期 11
·1-10
·
IF 6.408
Fan Ru,Tian Jinrong,Wang Huili,Wang Xuedong,Zhou Peipei
By employing NH 2 -MIL-88 as a template, we synthesized the intermediate Fe@CN under high-temperature calcination and further fabricated the FeS 2 @CN nanocomposites in the presence of sulfur powder. Under varying temperatures (300–600 °C) and Fe@CN-to-S ratios (1:3–6), FeS 2 @CN 500-5 nanocomposites had the highest peroxidase-mimetic activity. Under optimized conditions (incubation temperature 40 °C; solution pH 4.0 and nanocomposite concentration 10 μg/mL; 652-nm absorption), the Michaelis-Menten constant ( K m ) of FeS 2 @CN was much lower than that of horseradish peroxidase (HRP), therefore demonstrating that it had a higher affinity for both chromogenic substrates than conventional HRP. The limits of detection for H 2 O 2 and glucose were 0.15 and 0.30 μmol/L, respectively, and the recoveries for glucose were 91.8–103% with RSDs <5.2%. The novelty of this study lies in (1) the FeS 2 @CN was confirmed to possess stronger enzyme-mimetic activity than its precursors (NH 2 -MIL-88 and Fe@CN); (2) the enhanced activity resulted from the unsaturated sites of N and S doping and the plentiful defects on the porous carbon surface; and (3) free radical trapping experiments evidenced that •OH played a major role in the catalytic reaction, while h + and •O 2 − simultaneously participated in the catalytic process. These convincing performance metrics lead us to postulate that the FeS 2 @CN-based colorimetric biosensor provides a promising approach for several real-world applications, such as point-of-care diagnosis and workplace health evaluations. Graphical abstract
研究领域:
生物化学
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分析化学
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材料科学
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DOI
PubMed
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
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2021
·
IF 3.498
Cong Huang,Bo Cai,Lihua Zhang,Chenrui Zhang,Hui Pan
Two metal-organic framework materials (NH 2 -MIL-101 and NH 2 -MIL-88(b))were loaded on cellulose aerogel (CA) by in situ growing method and the resulting composite aerogels were used for dye adsorption. The characterization of resulting composite aerogels by SEM、XRD and FTIR confirmed that the two MOF materials grown in situ on cellulose aerogels still remained their pristine structure and crystal form . Both NH 2 -MIL-101@CA and NH 2 -MIL-88(b)@CA demonstrated excellent adsorption capacity for Congo red dye. The maximum adsorption capacity of NH 2 -MIL-101@CA and NH 2 -MIL-88(b)@CA were 223.4 mg g −1 and 280.3 mg g −1 , respectively. The adsorption kinetics and isotherm suggests that the adsorption process follows the pseudo-second-order model and the Langmuir isotherm model. The recovered aerogels showed comparable adsorption performance with fresh prepared aerogels even after five cycles.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2026
·
IF 4
Aihong Tang,Yujuan Cao,Manli Guo,Bixia Lin
One-step synthesis of magnetic nitrogen-doped porous carbon (MNPC). • The addition of urea promotes the graphitization degree of MNPC. • MNPC serves as an MSPE adsorbent with excellent reusability. • Good analytical performance for chloramphenicol in honey is obtained. Magnetic porous carbon (MPC) materials derived from metal-organic frameworks (MOFs) inherit the high porosity and tunable pore structure of MOFs and also endow the materials with magnetic response, demonstrating great potential for magnetic solid-phase extraction (MSPE). However, MPCs obtained directly by carbonizing MOFs suffer from issues such as easy pore collapse and a single surface chemical functionality, which necessitate modification methods to improve their performance. The nitrogen-doping strategy offers unique advantages in charge distribution, the creation of active sites, alterations in surface chemical properties, and enhanced structural stability. Therefore, a magnetic nitrogen-doped porous carbon (MNPC) derived from NH 2 -MIL-88(Fe) was developed as an MSPE adsorbent, combined with liquid chromatography, for sensitive determination of trace amounts of chloramphenicol in honey samples. The developed method exhibits a good linear relationship in the range of 0.05-50 μg·L -1 , with R 2 of 0.9999, LOD (S/N=3) of 0.005 μg·L -1 , and LOQ (S/N=10) of 0.02μg·L -1 . The spiked recovery rate ranged from 93.5% to 99.2%, and the RSD ranged from 1.3% to 10.7%. Therefore, this method has significant potential for routine monitoring of chloramphenicol residues in food safety supervision.
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DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 40
·19161-19167
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IF 3.925
Peng Miao,Weixing Chen,Kailei Li,Weifeng Zhao,Jie Kong
Design of microwave absorbents with hierarchical interfacial structures has become an effective method to scatter microwaves. Metal/carbon composites derived from metal–organic frameworks (MOFs) have attracted considerable attention due to their tunable chemical composition and microstructure. We describe the facile synthesis of a Co/CoO/FeO/C nanocomplex employing Co(OH)2 on NH2-MIL-88B as the “sacrificial template” through one-step pyrolysis. The as-prepared flaky-like Co/CoO/FeO/C nanocomplex showed an effective absorption width of 4.7 GHz at 1.86 mm and a minimum reflection loss of −45.5 dB at 2.01 mm. Our study can aid design of a microstructural strategy for preparing high-performance microwave absorbents.
研究领域:
材料科学
·
电磁学
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DOI
高影响因子
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.
研究领域:
分析化学
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环境科学
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食品科学
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产品关联
DOI
PubMed
高影响因子
MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Lili Yuan,Yongkang Yan,Yiyue Tang,Xueer Huang,Jiajing Liao,Jianmei Zou,Jinfang Nie,Lang Zhang,Shan Liao,Yun Zhang
This study initially reports a distance-based quantitative assay of pyrophosphate ion (PPi) based on analyte-triggered decomposition of metal–organic framework (MOF) in microfluidic paper-based analytical devices (µPADs). The µPADs were created using a mini-cutter machine and a home-use hot-pressing machine for loading one type of MOF of NH 2 -MIL-88 (Fe) prepared with Fe 3+ and fluorescent ligand of 2-aminoterephthalic acid (NH 2 -BDC). Upon sample introduction, the PPi could compete with NH 2 -BDC to bind Fe 3+ , leading to disintegration of the MOF and releasing of the fluorescent ligand in paper channel. The length (distance) of the NH 2 -BDC’s flow trace, when irradiated by a money tester pen, is proportional to the PPi level. The results show that the developed method only requires a ruler to linearly quantify PPi in a concentration range of 0–1000 μM, with a limit estimated to be ∼0.25 μM. Furthermore, recovery of PPi in orange juice and human urine was between 95.72 and 108.11 %, further validating its high detection accuracy. The fabrication method for µPADs offers many attractive advantages kike simplicity, batch production capability and low cost. Moreover, to our knowledge, this may be the first report of a portable quantitative MOF-based PPi assay with distance-based readout in µPADs.
研究领域:
分析化学
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生物医学工程
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材料科学
✓ 已验证
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DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Wenjie Yang,Dong Li,Lili Chen,Shuang You,Lihua Chen
A novel fluorometric strategy for the simultaneous identification of SARS-CoV-2 and SARS-CoV was successfully established based on a hybridization-induced signal on–off-on mechanism. Here, one part of the probe (P1) of SARS-CoV-2 (P = P1/P2) is partially related to SARS-CoV, while the other part (P2) is completely irrelevant to SARS-CoV. They as smart gatekeepers were anchored on NH 2 -MIL-88(Fe) ( [email protected] /P2) to turn off its catalytic performance. Only the specific SARS-CoV-2 genetic target can strongly restore the peroxidase-like activity of [email protected] /P2. In the presence of o-phenylenediamine, SARS-CoV-2 can be efficiently detected with high sensitivity, accuracy, and reliability. This strategy demonstrated excellent analytical characteristics with a linear range (10 -9 M ∼ 10 -6 M) under the limit of detection of 0.11 nM not only in buffer but also in 10 % serum, which partly shows its practicability. Most importantly, with the help of the auxiliary test of [email protected] and [email protected] , SARS-CoV-2 and SARS-CoV can be efficiently quantified and distinguished. This novel strategy has provided a breakthrough in the development of such identification. In the whole process, only a simple one-step experiment was involved. This circumvents the trouble of pretreatment experiments in traditional methods, including complex enzymatic mixtures, specialized experimental equipment, many primers optimization as well as reverse transcriptase. Additionally, this novel strategy is rapid, low-cost, and easy-to-use tools.
研究领域:
分析化学
·
病毒学
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分子生物学
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生物技术
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产品关联
DOI
PubMed
高影响因子