INORGANIC CHEMISTRY
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2024
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IF 4.3
Xudong Wu,Kaifu Yu,Yizhou He,Xin Cao,Tao Chen,Wenkun Zhu
The phenomenon of rapid migration of photogenerated charges in natural photosynthetic systems has motivated the design of efficient photocatalysts capable of fast charge separation and efficient reaction kinetics for photocatalytically assisted enrichment and separation of uranium U(VI) in uranium wastewater. In this study, we developed a biomimetic photocatalytic system MnOx/NH2-UiO-66-rGO (M/UiO-rGO) with spatially separated dual cocatalysts. Among them, rGO functions to capture electrons and participates in reduction reactions, while MnOx captures holes and participates in oxidation reactions. The M/UiO-rGO catalyst exhibits excellent performance in photocatalytic reduction of uranium (reaching 91.8% in 1 h), and even under natural light conditions, it exhibits excellent uranium removal ability (80.4%). Using multispectral coupling technology, we further confirmed that enriched uranium undergoes a continuous and complex reaction process of “capture-reduction-free radical oxidation–nucleation–crystallization”. This work presents a viable strategy for designing biomimetic photocatalysts with efficient charge separation and rapid reaction kinetics for environmental purification purposes.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2024
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IF 8
Li Gong,Yijiao Zhang,Renlong Liu,Zuohua Liu,Siwei Jin,Li Zhang,Tengda Zhao,Huanbao Fa,Wei Yin
Due to the toxicity and corrosiveness of the ammonia gas, low-cost, portable, and accurate methods of ammonia detection are of great importance in environmental testing and disease diagnosis. In this study, flower-like UIO-66-NH 2 @MoS 2 composite modified screen-printed electrodes (SPEs) were prepared by hydrothermal treatment using ionic liquids [BMIM][BF 4 ] as electrolytes. The UIO-66-NH 2 @MoS 2 /SPEs were then combined with a miniature electrochemical workstation to construct a novel electrochemical ammonia sensor. The experimental results showed that UIO-66-NH 2 @MoS 2 had excellent adsorption capacity for ammonia, exhibiting good linearity in the range of 5–500 ppm with a low limit of detection (2.1 ppm) and a fast response time for 100 ppm ammonia (13 s). This sensor also possessed excellent stability, reproducibility, and anti-interference ability. The synthesized UIO-66-NH 2 @MoS 2 nanocomposite was demonstrated to be an excellent candidate for the construction of high-performance ammonia sensors for various applications.
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MICROCHEMICAL JOURNAL
·
2024
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IF 4.9
Li Gong,Siwei Jin,Renlong Liu,Zuohua Liu,Yijiao Zhang,Li Zhang,Tengda Zhao,Huanbao Fa,Wei Yin
Achieving the real-time, low-cost, portable and accurate NH 3 detection is of great importance in industry owing to the toxicity of NH 3 . In this paper, Pt NPs@MIL-101-NH 2 composites modified screen-printed electrodes (SPEs) were prepared by solvothermal method and ionic liquids [BMIM][BF 4 ] were used as electrolytes. Finally, the prepared Pt NPs@MIL-101-NH 2 /SPEs were combined with a miniature electrochemical workstation to construct a novel electrochemical NH 3 sensor. The experimental results showed that Pt NPs@MIL-101-NH 2 has excellent adsorption capacity for NH 3 , and the sensor has good linearity in the range of 0.7–600 ppm with low limit of detection (0.58 ppm) and fast response time for 10 ppm NH 3 (8.0 s). Furthermore, this sensor also possesses excellent stability, reproducibility, anti-interference and accuracy. The synthesized Pt NPs@MIL-101-NH 2 nanocomposite was proved to be an excellent candidate for constructing high-performance NH 3 sensor for industry.
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TALANTA
·
2024
·
IF 5.6
Kexin Xu,Jinhui Zhu,Tong Zhang,Guodong Sui
Wastewater-based epidemiology (WBE) is a powerful tool for early warning of infectious disease outbreaks. Hence, a rapid and portable pathogen monitoring system is urgent needed for on-site detection. In this work, we first reported synthesis of an artificial modulated wide-spectrum bacteria capture nanoparticle (Arg-CSP@UiO@Fe 3 O 4 ). Arginine-modified phosphorylated chitosan (Arg-CSP) coating could provide strongly positive charged guanidinium group for pathogen interaction by electrostatic attraction, and UiO-66-NH 2 layer could help Arg-CSP graft onto Fe 3 O 4 magnetic particles. The capture efficiency of Arg-CSP@UiO@Fe 3 O 4 reached 92.2 % and 97.3 % for Escherichia coli ( E.coli ) and Staphylococcus epidermidis ( S.epidermidis )within 40 min, in 10 mL sample. To prevent pathogen degradation in sewage, a portable nucleic acid extraction-free method was also developed. UiO-66-NH 2 could disintegrate in buffer with high concentration of PO 4 3− for bacterium desorption, and then nucleic acid of the bacteria was released by heating. The DNA template concentration obtained by this method was 779.28 times higher than that of the direct thermal lysis product and 8.63 times higher than that of the commercial kit. Afterwards, multiple detection of bacteria was realized by loop-mediated isothermal amplification (LAMP). Artificial regulated pathogen desorption could prevent non-specific adsorption of nucleic acid by nanoparticles. The detection limit of Arg-CSP@UiO@Fe 3 O 4 -LAMP method was 80 cfu/mL for E.coli and 300 cfu/mL for S.epidermidis . The accuracy and reliability of the method was validated by spiked sewage samples. In conclusion, this bio-monitoring system was able to detect multiple bacteria in environment conveniently and have good potential to become an alternative solution for rapid on-site pathogen detection.
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APPLIED SURFACE SCIENCE
·
2017
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IF 3.387
Xipeng Li,Changwei Zhao,Mei Yang,Bin Yang,Deyin Hou,Tao Wang
Reduced graphene oxide-NH 2 (R-GO-NH 2 ), a kind of amino graphene oxide, was embedded into the polyamide (PA) layer of nanofiltration (NF) composite hollow fiber membranes via interfacial polymerization to enhance the permeate flux and antifouling properties of NF membranes under low pressure conditions. In addition, it could mitigate the poor compatibility issue between graphene oxide materials and PA layer. To evaluate the influence of R-GO-NH 2 on the performance of the NF composite hollow fiber membrane, SEM, AFM, FTIR, XPS and Zeta potentials were used to characterize the membranes. The results indicated that the compatibility and interactions between R-GO-NH 2 and PA layer were enhanced, which was mainly due to the polymerization reaction between amino groups of R-GO-NH 2 and acyl chloride groups of TMC. Therefore, salts rejection of the current membranes was improved significantly, and the modified membranes with 50 mg/L R-GO-NH 2 demonstrated highest performance in terms of the rejections, which were 26.9%, 98.5%, 98.1%, and 96.1%, for NaCl, Na 2 SO 4 , MgSO 4 , and CaCl 2 respectively. It was found that with the R-GO-NH 2 contents rasing from 0 to 50 mg/L, pure water flux increased from 30.44 ± 1.71 to 38.57 ± 2.01 L/(m 2 .h) at 2 bar. What’s more, the membrane demonstrated improved antifouling properties.
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RSC Advances
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2016
·Vol. 6
·期 32
·27039-27046
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IF 3.289
Honglin Yao,Qianqian Ding,Hongjian Zhou,Zhenfu Zhao,Gang Liu,Guozhong Wang
In this study, mesoporous amino-group functionalised iron/silica hollow spheres (Fe/SiO2–NH2 HSs) were successfully developed as a magnetic absorbent for the highly effective removal of Cr(VI) ions. The Fe/SiO2–NH2 HSs were synthesized using monodispersed silica colloids as a chemical template, followed by a one-pot hydrothermal treatment, hydrogen reduction and surface modification with an amino silane coupling agent. The Fe/SiO2–NH2 HSs have a diameter of ca. 950 nm and a shell thickness of ca. 60 nm, and the surfaces were composed of Fe and SiO2 units with amino functional groups. Meanwhile, the ferromagnetic property endowed them with easy recyclability for practical applications. The Fe/SiO2–NH2 HSs exhibited significantly improved ability to remove pollutant Cr(VI) and methyl orange. The removal percentage of Cr(VI) (8 mg L−1) could reach 98.3% in just 5 min using Fe/SiO2–NH2 HSs; however, only 10% of Cr(VI) were removed using the unmodified samples. XPS analysis suggested that the removal of Cr(VI) was attributed to the adsorption and reduction synergistic process of the Fe/SiO2–NH2 HSs. During the process, an electrostatic attraction occurred between the positively charged amino-groups and the negatively charged pollutant species in the aqueous solution, and adsorbed Cr(VI) ions were reduced to Cr(III) species by the iron of Fe/SiO2–NH2 HSs.
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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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