Journal of Physical Chemistry C
·
2026
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IF 3.4
Jing-Jing Li,Can-Jun Zou,Wei Tang,Cheng-Yu Zhang,Jian-Hua Jia,Ping-Ping Fang
The detection of purine drugs has been a persistent concern among scientists in the biology and medicine fields over the past few decades. However, achieving both high sensitivity and selectivity in the detection of purine drugs sharing similar molecular structures remains a significant challenge. Herein, we achieve both high detection sensitivity and selectivity for purine drugs with similar structure on the Gold/Materials of Institut Lavoisier-101(Au/MIL-101) composite by surface-enhanced Raman scattering (SERS). In water solution, the detection sensitivity for adenine (Ade) is as low as 1 ng·mL–1. Importantly, in serum containing Ade, 6-mercaptopurine, and allopurinol, Ade can be selectively detected with a detection limit of 3 ng·mL–1, indicating excellent anti-interference capability and practical application potential. Such high detection sensitivity is attributed to the specific adsorption between the amino group of the Ade and the carboxyl groups of the Materials Institut Lavoisier-101(Cr) (MIL-101(Cr)). This work provides a strategy for detecting structurally similar drugs and illustrates the potential use of functionalized SERS substrates in pharmaceutical analysis and therapeutic drug monitoring.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Lipei Ren,Shuaifei Zhao,Milad Laghaei,Han Wang,Jiaqi Zhang,Weimin Gao,Joselito M. Razal,Weilin Xu,Lingxue Kong
Converting CO 2 into valuable chemicals through photocatalytic reduction is a promising method to achieve carbon neutrality. Nonetheless, the insufficient active sites of photocatalysts lead to low CO 2 reduction efficiency and product selectivity. Taking advantage of the synergistic effect of photocatalytic heterostructures is an effective way to overcome this shortcoming. Here, metal-organic frameworks (MIL-101(Cr))-titanium dioxide (TiO 2 ) staggered gap (type II) heterojunctions were deposited on different woven polyimide (PI) substrates (MIL-101-TiO 2 PI hybrid photocatalysts) via atomic layer deposition and hydrothermal reaction for CO 2 photoreduction. The immobilized photocatalysts on the PI substrates resolved the challenge of separating powdered photocatalysts from liquid products or reactants. The prepared MIL-101(Cr)-TiO 2 PI hybrid photocatalysts displayed synergistic photocatalytic reduction performance towards CO 2 by separating the photogenerated charge carriers. The charge transfer between the heterojunctions and the substrates extended the lifetime of the excited electrons and holes, thereby generating synergy effects and promoting the CO 2 reduction yield. The rougher surface and higher specific area of the PI felt enabled higher loadings of heterojunctions compared with other woven structures of the fabric and mat. As a result, MIL-101(Cr)-TiO 2 PI felts showed multiple reduction pathways over the heterostructures and enhanced photocatalytic performance, with the main product yields of 29.6, 9.2, and 0.8 μmol g −1 h −1 for CO, CH 4 and H 2 , respectively. Meanwhile, CO selectivity of the MIL-101(Cr)-TiO 2 PI felt reached as high as 75 %. This study provides significant insights into the role of the substrate in flexible and immobilized hybrid photocatalysts with synergistic performance to achieve enhanced CO 2 reduction yield.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2022
·
IF 3.656
Xiaxi Zhang,Fen Wei,Tao Bao,Sicen Wang
In this study, we report the adsorption removal of indomethacin sodium (IDM) by the mixed-linker Materials of Institute Lavoisier (MIL)-101(Cr)s. The MIL-101(Cr)s were synthesized by controlling the ratios of 1,4-benzene dicarboxylic acid (H 2 BDC) and 2-amino-1,4-benzene dicarboxylic acid (NH 2 –H 2 BDC). Then their adsorption performances toward IDM were investigated. Due to the increase in specific surface area and the contribution of enhanced multiple action mechanisms, MIL-101(20) was proved to have the optimal IDM absorption among all the mixed-ligand MIL-101(Cr)s. The adsorption kinetic data was found to accord with the pseudo-second-order kinetic model, and the rate constant ( k 2 ) was calculated as 0.0059 g mg −1 min −1 . The selected MIL-101(20) exhibited the maximum IDM adsorption capacity of approximately 641 mg g −1 (318 K), calculated from the Langmuir linear plots. The simulation results of the thermodynamic model suggest that the adsorption could be a spontaneous, endothermic process with increasing randomness. The adsorption mechanism analysis indicates that the synergistic effects of electrostatic interaction , hydrogen bond interaction, and π-π stacking could be responsible for efficient IDM adsorption. In addition, the adsorbent also presented good reproducibility over six successive adsorption/desorption cycles. Therefore, the mixed-ligand MIL-101(Cr) could be recommended as a promising adsorbent for the preferential removal of IDM from polluted wastewater.
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Frontiers in Bioengineering and Biotechnology
·
2022
·
IF 6.064
Xie Dan,Wang Ruimeng,Fu Jinghao,Zhao Zhongxing,Li Min
Surface-enhanced Raman scattering (SERS) is an important and powerful analytical technique in chemical and biochemical analyses. Metal–organic frameworks (MOFs) can effectively capture volatile organic compounds (VOCs) with high adsorption capacity and fast kinetics, and the local surface plasmon resonance characteristics of gold nanoparticles can quickly and effectively distinguish different VOCs by SERS. Combining both, we designed a novel SERS substrate based on embedding gold nanoparticles (AuNPs) within MIL-101(Cr) for the recognition of various VOCs in the gaseous phase. Occupying of AuNPs inside MIL-101(Cr) increased the micropore-specific surface area of AuNPs@MIL-101(Cr), which enabled AuNPs@MIL-101(Cr) to absorb more toluene molecules and consequently realized its high detection sensitivity. The detection limits for toluene, 4-ethylbenzaldehyde, and formaldehyde were down to 6, 5, and 75, ppm respectively. Moreover, this substrate could be used for detecting different VOCs simultaneously. Finally, we discussed the enhancement of AuNPs outside and inside MIL-101(Cr) on the Raman signal.
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CATALYSIS LETTERS
·
2021
·Vol. 151
·期 9
·2560-2569
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IF 3.186
Han Jishu,Wang Ying,Liu Ying,Bai Jiayu,Zhao Ruiyang,Wang Lei
In this paper, novel CdSe/NH 2 -MIL-101(Cr) nanocomposites for photocatalytic hydrogen production were synthesized. When the prepared NH 2 -MIL-101(Cr) MOFs were modified with CdSe QDs, the photocatalytic hydrogen production amount was significantly increased and reached to 17,664 μmol g −1 in 7 h. The formation of CdSe/NH 2 -MIL-101(Cr) nanocomposites enhanced the light absorption intensity, broadened the visible light absorption range, promoted the transfer of photogenerated electrons and inhibited the recombination of photogenerated electron–hole pairs, then effectively improved the photocatalytic hydrogen production performance. In addition, the CdSe/NH 2 -MIL-101(Cr) nanocomposites exhibited high cycle stability, which was beneficial to the practical application in photocatalytic hydrogen production. Graphic Abstract
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Molecular Catalysis
·
2022
·
IF 5.089
Rongzhao Li,Chengtao Zhang,Shuo Li,Yupeng Du
Propane dehydrogenation is commonly operated at temperatures exceeding 600 °C due to thermodynamic requirements. However, high temperature accelerates the deactivation of catalysts because of the coke deposition. Therefore, it is quite necessary to develop catalysts with high catalytic activity and improved anti-coking ability. To this end, an Al-doped Cr 2 O 3 catalyst derived from MIL-101(Cr/Al) is prepared in this work. The preparation conditions, including the carbonization temperature of MIL-101 and the proportion of Cr/Al, are optimized via experimental studies. Meanwhile, the adsorption and dehydrogenation behaviors of propane on the catalyst are investigated using Density Functional Theory (DFT) methods. Findings indicate that the optimum carbonization temperature and Cr/Al proportion are 900 °C and 6:4, respectively. Under the reaction condition of P = 0.1 MPa, T = 580 °C and GHSV = 800 h −1 , the propane conversion and propylene selectivity on the Cr 6 /Al 4 catalyst are 19.5% and 92.0%, respectively. The activity stability of the Al-doped Cr 2 O 3 is elongated significantly due to the lower desorption energy of propene and higher energy barrier for the coke formation on the catalyst. In sum, the present work completed via experiments and DFT calculations will lead to a better understanding of the Al-doped Cr 2 O 3 catalyst and guide the rational design of anti-coking catalysts for propane dehydrogenation.
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Nanomaterials
·
2023
·Vol. 13
·期 14
·2072
·
IF 5.3
Xu Zhang,Bo Tian,Zhiheng Ma,He Wang,Zhixuan Cheng,Jiaqiang Xu
As a volatile air pollutant, formaldehyde can enter people’s living environment through interior decoration, furniture and paint, causing serious harm to human health. Therefore, it is necessary to develop a sensor for the real-time detection of formaldehyde in low concentrations. According to the chemical interaction between amino groups and formaldehyde, a MIL-101(Cr) aminated-material-based formaldehyde cantilever sensor was prepared, of which ethylenediamine- functionalized MIL-101(Cr) named ED-MIL-101(Cr)) showed the best gas sensing performance. Using quasi-in situ infrared spectroscopy, ED-MIL-101(Cr) was found bound to formaldehyde through a Schiff base. The adsorption enthalpy of formaldehyde-bound ED-MIL-101(Cr) was −52.6 kJ/mol, which corresponds to weak chemical adsorption, so the material showed good selectivity. In addition, ED-MIL-101(Cr) has the most active sites, so its response value to formaldehyde is larger and it takes longer to reach saturation adsorption than bare MIL-101(Cr). Through the research on the gas sensing performance of functionalized MIL-101(Cr) material, we found that it has a strong application potential in the field of formaldehyde monitoring, and the material performance can be quantitatively and accurately evaluated through combining calculation and experimentation for understanding the gas sensing mechanism.
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ANALYTICAL CHEMISTRY
·
2023
·
IF 7.4
Yu-Fei Li,Can-Jun Zou,Xing-Biao Liu,Feng Gan,Ping-Ping Fang
The detection of pharmaceuticals has been a matter of concern among scientists and health researchers in the past few decades. However, it is still difficult to realize the sensitivity and selectivity detection of pharmaceuticals with similar structures. Herein, the pharmaceutical molecules of 2-mercaptobenzimidazole (MBI) and 2-mercaptobenzothiazole (MBT) with so similar structures can be selectively detected by surface-enhanced Raman spectroscopy (SERS) taking advantage of the fingerprint identification on Au/MIL-101(Cr), with sensitive detection limits of 0.5 ng·mL–1 for MBI and 1 ng·mL–1 for MBT. MBI is selectively enriched by Au/MIL-101(Cr) from the mixture solution and detected by SERS below 30 ng·mL–1. MBI can also be selectively detected in the serum samples with a detection limit of 10 ng·mL–1. Density functional theory calculations combined with the SERS experiments explained that the high sensitivity and selectivity are caused by the intrinsic differences in Raman intensity and different adsorption energies from the pharmaceutical molecules adsorbed on Au/MIL-101(Cr), respectively. This study provides an effective way to enrich and detect pharmaceutical molecules with similar structures.
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INORGANICA CHIMICA ACTA
·
2017
·
IF 2.002
Tian Zhao,Ling Yang,Peiyong Feng,Irina Gruber,Christoph Janiak,Yuejun Liu
MIL-101(Cr), one of the best investigated and widely used metal–organic frameworks, has been easily synthesized with particle diameters in the range from 387(28) nm to 90(10) nm by using acetic acid as a modulator . The particle size of MIL-101(Cr) decreased with increasing acetic acid concentration. The decrease of size in high concentration of acetic acid may be explained with the efficient suppression of the framework extension. In a selected condition, MIL-101(Cr) possessing an average diameter of about 90 nm can be prepared easily and reproducibly in gram-scale, with high BET-surface areas (3200–3500 m 2 /g) and fairly good yield (60–75%).
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Small
·
2022
·Vol. 19
·期 10
·2205619
·
IF 15.153
Fei Yu,Xiaochen Zhang,Peng Liu,Bingbing Chen,Jie Ma
Metal-organic frameworks (MOF) have attracted extensive attention due to their ultra-high specific surface area and tunable structure, the mechanism of direct utilization for capacitive deionization (CDI) defluorination remains undefined. Here, MIL-101(Cr) with ultra-high specific surface area, high water stability, and open metal sites (OMSs) is prepared by a hydrothermal method for defluorination of CDI. Carbon black is used as a “chain” to connect F-stored in the holes of MIL-101(Cr) (Cr-MOF)as “blocks” to enhance the conductivity and ion storage capacity of MIL-101(Cr)/carbon black electrodes (Cr-MOF electrodes). This simple construction method avoids the process complexity of in situ synthesis and performs better. These easily constructed “blockchain-like” Cr-MOF electrodes exhibit excellent defluorination capacity (39.84 mg NaF g electrodes −1 ), low energy consumption (1.2 kWh kg NaF −1 ), and good stability. The coupling of the electrochemical redox reaction of Cr 3+ /Cr 4+ with confined water is investigated using in situ and ex situ analysis methods combined with density functional theory (DFT), resulting in an unprecedented defluorination mechanism for Cr-MOF electrodes. This study opens up new ideas for the application of MOF in CDI, clarifies the removal mechanism of MOF, and lays a foundation for further promoting the application of raw materials with poor conductivity in the field of CDI.
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APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING
·
2025
·Vol. 131
·期 6
·1-12
·
IF 2.8
Cai Hongxin,Yu Hang,Liu Yuanyuan,Yan Lingling,Chen Liang,Hu Qiang,Wang Lingli,Li Bin
A series of FeCl 3 doped MIL-101(Cr)/silicon nanoporous pillar array (FeCl 3 /MIL-101(Cr)/Si-NPA) humidity sensors were prepared by growing FeCl 3 doped MIL-101(Cr) on Si-NPA via a facile spin-coating method. Systematically evaluation of capacitive sensing performance demonstrated that FeCl 3 incorporation significantly enhanced humidity sensitivity. This improvement can be attributed to the increased hydrophilicity of the MIL-101(Cr)/Si-NPA composite membranes induced by FeCl 3 , as confirmed by the water contact angle test results. Notably, the 8 wt.% FeCl 3 /MIL-101(Cr)/Si-NPA humidity sensor exhibited the best comprehensive sensing properties, with excellent linearity (R 2 = 0.991) in the 11–75% relative humidity (RH) range. The capacitance of the humidity sensor increased by nearly three orders of magnitude from 11% RH to 75% RH at 300 Hz. Additionally, the humidity sensor displayed fast response (46 s) and recovery (6 s) times, as well as excellent reproducibility. The sensing mechanism was explored through the analysis of complex impedance curves. These finding indicate that the 8 wt.% FeCl 3 /MIL-101(Cr)/Si-NPA sensor holds considerable promise for humidity sensing applications.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Yandi Li,Bo Wang,Shuangjiang Li,Zhiyong Xu,Wenbo Zhao
A series of MCl 2 @MIL-101(Cr) composites were fabricated via vacuum wet impregnation. • CaCl 2 @MIL-101(Cr)-0.35 exhibits ultrahigh NH 3 uptake of 28.9 mmol/g at 298 K and 100 kPa. • Composite shows excellent NH 3 /N 2 selectivity and cycling stability. • Adsorption rate is extremely fast and follows pseudo-second-order kinetic. • Synergistic effect between chemical and physical adsorption was proved. Ammonia (NH 3 ) is a vital chemical raw material and promising carbon-free energy carrier, its efficient capture is essential for both industrial production and energy development. However, achieving high capacity, high selectivity and high stability in NH 3 capture adsorbents still remains a challenge. Herein, a series of metal chloride@MIL-101(Cr) composite adsorbents (M = Ca, Co, Ni) were fabricated via a vacuum wet impregnation method. Structural characterization confirmed that metal chlorides were highly dispersed within the MIL-101(Cr) pores as an amorphous phase without damaging the MOF framework. The optimal CaCl 2 @MIL-101(Cr)-0.35 achieved an ultrahigh NH 3 adsorption capacity of 28.9 mmol/g at 298 K and 100 kPa, which is 3.6 times that of pure MIL-101(Cr). The extremely high NH 3 adsorption capacity is attributed to strong coordination bonds between Ca 2+ and NH 3 , and synergistically enhanced by N–H···Cl − and N–H···O hydrogen bonds involving the Cl − as well as the framework carboxylate oxygen atoms, respectively. It also demonstrated estimated high NH 3 /N 2 selectivity (>6000 at low pressure) and good short-term cycling stability, retaining over 95% of its initial capacity after 10 adsorption-desorption cycles. The adsorption kinetics were rapid, and the process was best described by the pseudo-second-order model, indicating a chemisorption-dominated mechanism. This “confinement loading” strategy effectively combines the physisorption advantages of MOFs host and chemisorption merits of metal chlorides guests, achieving synergistic enhancement of NH 3 adsorption performance. The prepared composite material exhibits shows potential for further evaluation in industrial ammonia separation and capture.
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