Analytical Methods
·
2024
·Vol. 16
·期 38
·6529-6537
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IF 2.7
Na Li,Baokun Tang,Tao Zhu
Carbendazim (CBZ) is widely used for crop protection and its residues threaten human health and the environment. Therefore, developing an effective electrocatalyst is important for the extremely sensitive detection of CBZ. Lattice-strain engineering is an effective strategy to change its electronic structure and ultimately optimize the catalytic performance of materials, which can be used as a modification method to improve the detection performance of electrochemical sensors. Herein, a NiFeLDH@HsGY-NH2/MWCNTs heterojunction with strain effect is prepared by the electrostatic self-assembly method. The structure, morphology, composition, crystallinity and electrochemical performance of NiFeLDH@HsGY-NH2/MWCNTs are analyzed using various instrumental techniques, in which geometric phase analysis (GPA) and X-ray diffraction (XRD) images confirm the lattice-strain generated in NiFeLDH@HsGY-NH2/MWCNTs. The results indicate that the prepared electrochemical sensor exhibited an excellent response for carbendazim (CBZ) in the linear range of 0.05–50.00 μM with a detection limit of 10.00 nM (S/N = 3) under the optimal detection conditions. By analyzing the reasons for the improvement of the catalytic performance of the composite material, it is found that the composite of MWCNTs not only improves the conductivity of NiFeLDH but also regulates the electronic structure of metal atoms through double effects. This study provides new insights into the design of efficient and low-cost catalysts to facilitate electrochemical sensor applications.
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TALANTA
·
2024
·
IF 5.6
Shengyuan Zhang,Haiyan Li,Dezhi Yang,Yaling Yang
In the present research, Fe-based metal-organic frameworks (MIL-101(Fe)–NH 2 ) nanoparticles were synthesized by simple solvothermal methods and used to assay Cr(Ⅵ). The MIL-101(Fe)–NH 2 performs dual functions: the 2-aminoterephthalic acid (NH 2 -BDC) ligand endows a strong fluorescence emission, and the Fe metal nodes are able to facilitate the oxidation of 3,3′,5,5′- tetramethylbenzidine (TMB) directly, resulting in the generation of oxidized-TMB (ox-TMB). Our research results showed that reducing agents such as ascorbic acid (AA) can collapse the structures of MIL-101(Fe)–NH 2 because of the reduction of Fe 3+ by AA, resulting in release of NH 2 -BDC. In the presence of Cr(Ⅵ), the fluorescence intensity of the MIL-101(Fe)–NH 2 + AA system will be decreased due to the competitive reduction of Fe 3+ and Cr(Ⅵ). Nevertheless, Cr(Ⅵ) can significantly accelerate the oxidation of TMB by MIL-101(Fe)–NH 2 as it boosts the electron transfer rate between Fe 3+ and Fe 2+ . Therefore, a fluorescent/colorimetric dual-mode platform was developed for the detection of Cr(Ⅵ) with an extensive linear range (7.5–750 μg/L and 13.3–1000 μg/L) as well as a remarkably low detection limit (0.99 μg/L and 1.98 μg/L). This MOF with the ability to release ligands not only provides inspiration for the design of new luminescent materials, but also offers a novel and reliable solution for the detection of Cr(Ⅵ).
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Wenhao Gu,Jinxian Feng,Xingshuai Lv,Weng Fai Ip,Hui Pan
Photocatalytic CO 2 reduction has been considered as an efficient way for the carbon nuetrality. In this work, a series of (Cu, Mn) co-incorporated metal-orgnaic frameworks (MOFs) (NH 2 -MIL-125(Ti) (NML)) with different Cu 2+ /Ti 4+ and Mn 2+ /Ti 4+ molar ratios are systematically investigated to improve the efficiency for photocatalytic CO 2 reduction. The optimized sample (1 M−5C−−NML) shows a highest yield of HCOOH (116.74 μmol . g −1. h −1 ) (3.71 times higher than that of NML), and a superior apparent quantum efficiency (AQE) (6.74 % at 405 nm). The improved performance is attributed to the formed oxygen vacancy and intermediate energy level as introduced by the co-incorporation, which facilitate the charge separation and enhance the visible-light-harvesting of NML. It shows that the density of oxygen vacancies increases with the increasing amount of Cu, resulting in enhanced charge separation. However, the increasing amount of Mn leads to the short-range Mn-Mn interaction, the concentration quenching effect as well as the inhibited photocatalytic performance. This work shows that the co-incorporated MOFs can be used as an advanced photocatalyst.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Meipeng Jian,Xiaoqin Yang,Congxin Huang,Chaochun Tang,Xiwang Zhang,Ruiping Liu,Haiyan Li
Flexible metal–organic frameworks (MOFs) with the gate opening feature can optimize the removal efficiency on the adsorption behavior by accommodating to the specific target molecules. In this study, a flexible MOF denoted as NH 2 -MIL-53(Al) was investigated to remove Hg(II) from water, in which the adsorption capacities of large-pore NH 2 -MIL-53(Al) (NH 2 -MIL-53(Al)-LP) for Hg(II) reached 433.20 mg/g, which is about 4 times higher than narrow-pore NH 2 -MIL-53(Al) (112.75 mg/g). Further, the kinetic experiment also revealed that nearly 90 % Hg(II) can be captured within 60 min for NH 2 -MIL-53(Al)-LP. Advanced characterizations and density functional theory calculations demonstrated that the strong coordination of the amino and oxygen centers on NH 2 -MIL-53(Al)-LP to Hg(II). Importantly, molecular dynamic simulation verified the gate opening effect of NH 2 -MIL-53(Al)-LP, as the faster diffusivity of Hg(II) ions in NH 2 -MIL-53(Al)-LP was observed. This work provides another opportunity in designing the pore geometry of porous materials for water remediation.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Ruyi Cui,Yong Zhou,Xingyi Xu,Hengxin Fang,Wenlong Wang,Sanmei Wang,Pengbo Lyu,Lizhong Sun,Biao Wang,Changqing Sun
Ammonia borane (AB) is a highly promising hydrogen carrier with significant potential for safe and efficient hydrogen storage and transportation. However, its high chemical stability poses considerable challenges for hydrogen release, emphasizing the importance of highly efficient catalysts. In this study, we present Ru nanocatalysts supported on UiO-66-NH 2 -derived carbon nitride (Ru/CN) as high-performance catalysts for AB hydrolysis. A facile pyrolysis-impregnation method was employed to synthesize highly dispersed Ru nanoparticles with tunable sizes, while retaining the octahedral morphology of the MOF-derived support. Detailed characterizations revealed tunable Ru nanoparticle sizes achieved by simply adjusting the Ru loading. Among the catalysts, the 2.5Ru/CN, featuring Ru nanoparticles with an average size of 2.2 nm, achieved an impressive turnover frequency of 493 mol H 2 (mol Ru −1 ·min −1 ) at 30 °C, demonstrating exceptional catalytic activity. Density functional theory (DFT) calculations confirmed that the optimized Ru cluster size enhances key catalytic steps, including H 2 O dissociation, AB activation, and H 2 desorption. This study highlights the critical role of fine-tuning nanoparticle sizes and provides valuable insights into the rational design of advanced catalysts for more efficient hydrogen production.
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Analytical Methods
·
2025
·
IF 2.6
Xinxing Jiang,Jihong Fu,Shuxian Ren,WenXia Xue
Substrate materials with high sensitivity and good reproducibility are highly desirable for the practical applications of surface-enhanced Raman scattering (SERS) techniques. In this study, a novel Ni-based metal-organic frameworks loaded gold nanoparticles (Ni-BDC-NH2/Au NPs) SERS substrate was successfully synthesized via electrostatic self-assembly method. The enhancement of the SERS signal is achieved owing to the synergy between chemical enhancement (CM) effect of Ni-BDC-NH2 and the electromagnetic enhancement (EM) of Au NPs, and the enriching of the analyte near the SERS “hot spots” through the strong adsorption capacity of the Ni-BDC-NH2. The Ni-BDC-NH2/Au NPs exhibited a high enhancement factor (EF) of 1.10×107 and a low detection limit of 5×10-9 mol/L. Besides, the substrate material showed exceptional stability up to 45 days at room temperature. The Ni-BDC-NH2/Au NPs was used to detect methylene blue (MB) that displayed a wide linearity (5×10-7-5×10-5 mol/L) and high recoveries (86.82-104.46%). These indicate that the Ni-BDC-NH2/Au NPs hybrid substrate has great potential for the detection of environmental pollution in practical applications.
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FOOD CHEMISTRY
·
2024
·
IF 8.5
Xiaoyu Du,Gan Wu,Xilin Dou,Zhaoyang Ding,Jing Xie
Food prone to spoilage has a huge food safety hazard, threatening people’s health, so early detection of food spoilage is a continuous and urgent need. Herein, we developed a dual-mode response sensor, alizarin complexone@UiO-66-NH 2 , which can accurately detect pH. The sensor demonstrated significant changes in color from pale yellow to deep pink, while the fluorescence shifted from light blue to blue violet. Moreover, both UV absorption and fluorescence intensity showed a linear correlation with pH raging from 4.5 to 7.5. These results indicate that the sensor effectively responds to pH, making it suitable for detecting the freshness of perishable food. To put this into practice, we integrated the sensor with cellulose-based filter paper to determine the freshness of shrimp and beef, which was proved to be effective in assessing freshness. In the future, it can be combined with intelligent colorimetric and fluorescence instruments to achieve visual detection.
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Analytical Methods
·
2020
·Vol. 12
·期 41
·4967-4976
·
IF 2.596
Xin Yao,Jinhui Shen,Qingyan Liu,Huanbao Fa,Mei Yang,Changjun Hou
In this work, we designed and synthesized a nanocomposite comprising an amine-functionalized metal organic framework (UiO-66-NH2), a multiwalled carbon nanotube@reduced graphene oxide nanoribbon (MWCNT@rGONR) and a covalent organic framework (COF) synthesized using melamine and cyanuric acidmonomers via polycondensation (represented by MCA). The UiO-66-NH2/MCA/MWCNT@rGONR nanocomposite was used as a sensitive platform for an electrochemical aptasensor to detect kanamycin (kana). Owing to the rich chemical functionality, amino-rich structure and excellent electrochemical activity, the cDNA strands with terminal amino groups can not only anchor over the UiO-66-NH2/MCA/MWCNT@rGONR surface but also penetrate into the interior of porous UiO-66-NH2/MCA/MWCNT@rGONR networks. The characterization of the UiO-66-NH2/MCA/MWCNT@rGONR nanocomposite was performed by scanning electronic microscopy (SEM), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FT-IR) spectroscopy and X-ray diffraction (XRD). Furthermore, cyclic voltammetry (CV) and square wave voltammetry (SWV) were employed for the electrochemical performance study of this biosensor. The results indicated that the UiO-66-NH2/MCA/MWCNT@rGONR nanocomposite exhibited high bioaffinity toward the aptamer and the lowest limit of detection at 13 nM (S/N = 3) within a linearity of the kana concentration of 25–900 nM. In addition, it possessed great repeatability, stability and selectivity and obtained satisfactory recovery results in the real analysis of fish meat and milk, indicating the great potential for analytical measurements in food safety.
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BIOSENSORS & BIOELECTRONICS
·
2024
·
IF 10.7
Yajun Gao,Suhui Xu,Ge Guo,Yajie Li,Wenyuan Zhou,Huaxiang Li,Zhenquan Yang
Herein, novel nanozyme mimics MoO 3 /MIL-125-NH 2 were reported and conjugated with bacteriophages as a new electrochemical probe for high sensitivity and specific electrochemical detection of staphylococcus aureus . The excellent peroxidase-like activity of MoO 3 /MIL-125-NH 2 composites was attributed to the integration of MIL-125-NH 2 with MoO 3 , which can boost the generation of superoxide radicals (O• 2 – ) and thus promote the oxidation of TMB in the presence of H 2 O 2 . In this work, two bacteriophages named SapYZU04 and SapYZU10 were isolated from sewage samples by using staphylococcus aureus YZUsa12 as the host. In comparison, MoO 3 /MIL-125-NH 2 @SapYZU04 was selected as a recognition agent. The DPV current declined linearly with staphylococcus aureus YZUsa12 concentration in the range of 10 1 −10 8 CFU mL −1 , with a low detection limit of 16 CFU mL −1 (S/N = 3). 20 strains including 13 host strains and 7 non-host strains were used to evaluate the selectivity of the proposed sensor. Regardless of the differences in the degrees of lytic performance for phage SapYZU04, all selected host strains can be screened with merely the same DPV current. Host spectrum-oriented bacteriophage sensing is of great importance for the practical application of bacteriophage-based biosensors in the future.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Chunhua Li,Luqian Bao,Yubo Shi,Zhehang Tian,Yixin Ji,Mengyao Cui,Zhilei Zhao,Xianyou Wang
A hollow heterojunction of W-Zr-MOF-NH 2 @TpTt-COF (WZT) was fabricated by combining etched W-Zr-MOF-NH 2 with TpTt-COF. WZT, synthesized through acid etching and hydrothermal methods, showed better tetracycline degradation than pure W-Zr-MOF-NH 2 and pure TpTt-COF due to its larger specific surface area and more active sites. The surface of WZT contains abundant oxygen vacancies (OVs) that capture electrons, promoting the separation of photogenerated e - -h + pairs and increasing WZT’s photocatalytic activity. WZT (1:1, mass) showed 87% degradation of tetracycline under 300 W Xenon lamp irradiation. The results of cycling experiments demonstrated the high stability and reusability of WZT (1:1), making it feasible for production. The excellent photocatalytic degradation of tetracycline by WZT (1:1) originates from the formation of heterojunctions and the presence of surface OVs, which reduces the strong photogenerated e - -h + complexation efficiency. Possible photocatalytic degradation mechanisms are proposed while demonstrating the formation of Z-scheme heterojunction in WZT, which aligned with the experimental results of electron spin resonance (ESR). The tetracycline oxidative decomposition process involves the participation of •OH, 1 O 2 , • O 2 - , e - , and h + as proven by ESR and radical trapping experiments. This work proposes a research idea to prepare high-performance photocatalysts with MOF@COF type, featuring OVs-rich and Z-scheme heterojunctions.
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CRYSTENGCOMM
·
2024
·Vol. 26
·期 38
·5431-5439
·
IF 2.6
Ting-Ting Xu,De-Sheng Wei,Shuang-Bao Li,Yu-Teng Zhang,Nan Lv
Although the fundamental configuration (tetrahedron-type and capsule-type) of Zr-MOCs is well understood, the synthesis of amino-functionalized Zr-based capsule (denoted as ZrC-1-NH2) based on 2-aminoterephthalic acid remains a considerable challenge. Fortunately, we obtained single crystals under solvothermal conditions and further achieved the rapid synthesis of ZrC-1-NH2 with pure phase and high yield using a microwave-assisted solvothermal method. In addition, ZrC-1-NH2 was utilized as a photocatalyst to perform the degradation of tetracycline (TC) in water. The degradation efficiency of 92.3% was achieved at the optimal conditions, and the main active free radical was determined as ·O2− according to the trapping agent experiment and EPR results. Furthermore, the possible degradation pathway of TC was proposed.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
·
2024
·
IF 4.1
Lingtao Liu,Lijian Wang,Jingxin Tan,Cong Yu,Junjie Bian,Xinbo Wang
Photocatalytic selective oxidation of furfural is a green, gentle way of preparing furoic acid. Photocatalytic oxidation effectively avoids the problems of difficult separation and high energy consumption in subsequent work-ups caused by the use of homogeneous oxidants. The photocatalytic process suffers from uncontrollable reactive oxygen species, resulting in low selectivity of the target product and excessive oxidation. Therefore, the K x -C 3 N 4 /UiO-66-NH 2 -Y catalyst was prepared by the mass proportion of UiO-66-NH 2 and K x -C 3 N 4 to form a heterogeneous structure, and the band gap width was adjusted to effectively avoid the formation of non-target strong reactive oxygen species ( OH). The results showed that: the aqueous 0.1 mM Na 2 CO 3 solution had an inhibitory effect on the non– target reactive oxygen species at room temperature; when the reaction time was 5 h and K 0.1 -C 3 N 4 /UiO-66-NH 2 -20, the furoic acid had the highest yield of 70.7, the target reactive oxygen species was confirmed by free radical capture experiments as O 2 – , and it was postulated that the reaction mechanism for the preparation of furoic acid by selective oxidation of furfural.
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