Materials Chemistry Frontiers
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2024
·Vol. 9
·期 4
·608-617
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IF 6
Tao Hu,Zixuan Wu,Wei Lv,Yan Gao,Qingguang Zeng,Yayun Zhou,Xinxin Han
Broadband near-infrared (NIR) phosphors are essential for assembling portable NIR light sources. However, the development of efficient and stable broadband NIR phosphors remains a major challenge. This work designed an ultra-high efficient NIR-emitting Cs2KSc0.83Ga0.1F6:0.07Cr3+ phosphor by substituting Sc3+ with a Ga3+ ion. This cationic substitution strategy enables the internal quantum efficiency of NIR emission to reach a staggering high of 98.56%, almost 100%, along with excellent thermal quenching resistance (I423K = 62.4%). The Ga3+ → Sc3+ replacement lowers the local site symmetry and overcomes the parity selection rule, rendering the electronic transitions with much larger oscillator strength and thus improved optical properties. The NIR phosphor conversion light emitting diode (pc-LED) based on Cs2KSc0.83Ga0.1F6:0.07Cr3+ demonstrated a premium photoelectric conversion efficiency of 31.46% at 40 mA. The potential of the pc-LED as a light source for night vision and anti-counterfeiting has also been demonstrated. These results highlight the phosphor's performance improvement via a cationic substitution strategy and demonstrate the practical application potential of the broadband Cr3+-based NIR phosphor in the design of high-efficiency devices.
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ANALYTICA CHIMICA ACTA
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2021
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IF 6.558
Jiabi Xu,Yanyan Xing,Yutong Liu,Mingzhe Liu,Xiaohong Hou
In recent decades, artificial nanozymes with excellent stability, low cost and availability have been gradually explored to avoid the limits of natural enzymes such as poor stability, high cost and difficult preparation. Herein, for the first time, we investigated the capability of nanoscale Fe 3 O 4 @MIL-100(Fe) as a nanozyme, which was quickly synthesized in situ by a microwave-assisted method within 20 min using Fe 3 O 4 as the metal precursor. The obtained Fe 3 O 4 @MIL-100(Fe) showed satisfactory intrinsic dual enzyme mimetic activities, including peroxidase (POD)- and catalase (CAT)-like activities. Moreover, a simple and effective colorimetric biosensor was fabricated to detect glutathione (GSH) based on its POD-like activity. The proposed measurement had a linear range of 1–45 μM and a limit of detection (LOD) of 0.26 μM (3.3 δ/S). It was proved that the established colorimetric sensing system could be successfully applied to detect GSH in actual biological samples. Importantly, the outstanding reusability and stability made it extremely valuable as a catalyst. The present work implied that Fe 3 O 4 @MIL-100(Fe) synthesized in situ by the microwave-assisted method was a very promising candidate for biocatalyst and biosensing.
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JOURNAL OF NANOBIOTECHNOLOGY
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2022
·Vol. 20
·期 1
·1-12
·
IF 9.429
Hong Liping,Pan Mingfei,Yang Xiao,Xie Xiaoqian,Liu Kaixin,Yang Jingying,Wang Shan,Wang Shuo
In this study, a thermo-sensitive molecularly imprinted fluorescence sensor was developed for the specific detection of β-Lactoglobulin (β-LG) allergen in milk products. The metal–organic frameworks (MIL-100) with a high specific surface area was coated on the surface of upconversion micro-particles (UCMPs). As the core, an imprinted polymer layer allowing for swelling and shrinking with response to temperature was prepared, which exhibited high adsorption and mass transfer capabilities for β-LG allergen. The fluorescence intensity of UCMPs@MIL-100@MIP decreased linearly with the concentration of β-LG in the range of 0.1–0.8 mg mL−1, and the limit of detection was 0.043 mg mL−1. The imprinting factor reached 3.415, which indicated that excellent specificity of the UCMPs@MIL-100@MIP for β-LG allergen. In the analysis of β-LG allergen in actual milk samples, the proposed UCMPs@MIL-100@MIP fluorescence sensor produced reliable and accurate results (recovery: 86.0–98.4%, RSD: 2.8–6.8%), closely related to the results of standard HPLC method (correlation coefficient: 0.9949), indicating that its feasibility in the detection of β-LG allergen.Graphical Abstract
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CARBON
·
2022
·
IF 11.307
Bin Li,Biao Ma,Mengying Wei,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Qing Xia,Wenchao Peng
Recycle of the spent lithium-ion batteries (LIBs) can reuse the toxic heavy metals for the synthesis of useful materials. In this study, the cobalt metal is obtained by recycling the cathodes of spent LIBs, which is then used as cobalt source for the synthesis of highly porous Co-NC composites. Attributing to the addition of EDTA-2Na and NaNO 3 as chelate agent and activation agent respectively, very large surface areas (>3700 m 2 /g) and highly porous structure can be achieved. These composites can activate peroxymonosulfate (PMS) effectively for the degradation of bisphenol A (BPA) in aqueous solution. The optimized Co-NC/PMS system also shows good performance in a wide pH range and great tolerance to different inorganic ions and NOMs. Radical scavenging experiments and EPR results prove that 1 O 2 is the only functional reactive oxidation species (ROS) for BPA degradation. A generation route of PMS – *OH – *O – 1 O 2 for 1 O 2 is also simulated and proved by DFT calculation. This work provides a novel way to synthesize effective catalysts for PMS activation from the environmental wastes.
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ANALYTICAL CHEMISTRY
·
2019
·
IF 6.35
Yongjie Wang,Jing Chen,Yingyan Jiang,Xian Wang,Wei Wang
The past decade has witnessed theoretical and experimental debates on the extraordinary long lifetime and low contact angle of surface nanobubbles. While several kinds of imaging techniques have provided promising evidence on the lifetime and gaseous nature of single surface nanobubble, each of them suffered from its own limitations before a consensus can be reached. In the present work, we employ a recently developed surface plasmon resonance microscopy (SPRM) to nonintrusively visualize single sub-100-nm surface nanobubble without labeling for the first time. The quantitative dependence between optical signal and nanobubble volume allows for resolving the dissolution kinetics, which is a key for understanding the lifetime. A superlocalization method is further introduced to monitor the trajectory of its mass center during dissolution, which uncovers the stick–slip behavior in the early stage and the migration behavior in the late stage. The label-free, nonintrusive, quantitative and sensitive features of SPRM and the potential compatibility with atomic force microscopy shed new light on the long-standing puzzle behind surface nanobubbles.
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RSC Advances
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2019
·Vol. 9
·期 41
·23711-23717
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IF 3.049
Shu-Hui Huo,Chen-Xu Liu,Peng-Xin Zhou,Jing Yu,Lei Bai,Zhen-Gang Han,Xiao-Quan Lu
Development of novel porous materials for efficient adsorption and removal of environmental pollutants from aqueous solution is of great importance and interest in environmental science and chemistry. Herein, we reported a facile synthesis of recyclable magnetic carbonaceous porous composite derived from iron-based metal–organic framework MIL-100(Fe) for superior adsorption and removal of malachite green (MG) from aqueous solution. Because of large surface area and high porosity, the synthesized magnetic carbonaceous porous material presented a superior adsorption capacity of 2090 mg g−1 for MG. The adsorption of MG on magnetic carbonaceous porous composite is endothermic and spontaneous. The prepared magnetic carbonaceous porous composite could be separated easily and rapidly from the solution matrix by an external magnet. The rapid adsorption, large adsorption capacity and good reusability make it attractive for practical use in the adsorption and removal of dyes from aqueous solutions.
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JOURNAL OF CHROMATOGRAPHY A
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2012
·
IF 4.531
Yan-Yan Fu,Cheng-Xiong Yang,Xiu-Ping Yan
Metal-organic framework MIL-100(Fe) was explored as a novel stationary phase for both normal-phase and reverse-phase high performance liquid chromatography. Two groups of analytes (benzene, toluene, ethylbenzene, naphthalene and 1-chloronaphthalene; aniline, acetanilide, 2-nitroaniline and 1-naphthylamine) were used to test the separation performance of MIL-100(Fe) in the reverse-phase mode, while the isomers of chloroaniline or toluidine were employed to evaluate its performance in the normal-phase mode. The MIL-100(Fe) packed column gave a baseline separation of all the tested analytes with good precision. The separation was controlled by negative enthalpy change and entropy change in the reverse-phase mode, but positive enthalpy change and entropy change in the normal-phase mode. The relative standard deviations of retention time, peak area, peak height, and half peak width for eleven replicate separations of the tested analytes were 0.2–0.7%, 0.5–3.6%, 0.6–2.3% and 0.8–1.7%, respectively. The mesoporous cages, accessible windows, excellent chemical and solvent stability, metal active sites and aromatic pore walls make MIL-100(Fe) a good candidate as a novel stationary phase for both normal-phase and reverse-phase high performance liquid chromatography.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
·
IF 20.2
Jianxin Zhu,Haiyang Liu,Haijun Chen,Xiuyi Hua,Deming Dong,Dapeng Liang,Zhiyong Guo,Na Zheng
Low degradation efficiency and significant transition metal leaching are two challenges in persulfate activation systems based on metal-organic frameworks (MOFs) for organic pollutant degradation. Here, the challenges were solved by designing and synthesizing a micron-sized core-shell material, γ-Al 2 O 3 -C-MIL-100(Fe) (γACM), by coating the γ-Al 2 O 3 core with carbon (γ-Al 2 O 3 -C) and futher modifying with MIL-100(Fe). Testing γACM with sulfamethazine (SMZ) demonstrated its outstanding peroxydisulfate (PDS) activation, achieving 92.5 % SMZ removal within 20 min at a low oxidant/pollutant ratio. Fe leaching from γACM was effectively inhibited, with only 3.59 % Fe lost after three recycles. The system showed adaptability across a wide pH range, and usability in sewage effluent, indicating promise for practical application. The hydrophobicity of γ-Al 2 O 3 -C, the coordinatively unsaturated sites in MIL-100(Fe), and the strong bounding of MIL-100(Fe) on γ-Al 2 O 3 -C ensured the effective SMZ gather, PDS activation, and Fe stability respectively, which led to the excellent performances of γACM.
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Journal of Materials Chemistry A
·
2024
·
IF 10.7
Yuanzhe Zhao,Xiuheng Wang
Singlet oxygen (1O2) is an excellent active species for eliminating organic pollutants in single-atom catalyst (SAC) catalyzed peroxymonosulfate (PMS)-based Fenton-like systems. However, it is difficult to achieve high efficiency and selectivity in 1O2 generation as a result of the lack of effective SACs. In this work, a Co SAC (Co–N–C) containing highly uniform Co–N4 active sites with an ultralow-level Co loading of 0.34 wt% is fabricated, delivering boosted performance in tetracycline degradation with an extremely rapid rate of 0.573 min, which outperforms most advanced catalysts in reported studies. A vibrating-sample magnetometer is used to preliminarily determine the atomically dispersed Co sites in Co–N–C according to the obvious paramagnetic characteristics of Co–N–C, and this is in good agreement with the test results obtained by using an aberration-corrected high-angle annular dark-field scanning transmission electron microscope and synchrotron radiation facility. Electron spin resonance and free radical quenching experiments prove that Co–N–C facilitates PMS activation with the 1O2 generation of almost 100%. Mechanism analyses suggest that the Co–N4 site strengthens the adsorption of the terminal O of PMS, realizing enhanced electron transfer from Co–N–C to PMS, promoting the simultaneous and spontaneous cleavage of O–O and O–H bonds to produce O*, followed by a reaction with another O* to generate 1O2.
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Xianlong Lu,Lili Wang,Xueyang Zhao,Binbin Pan,Zhendong Li,Xiangfei Du,Shihan Zhang,Fan Dong,Bangwei Deng
Copper (Cu)-based catalysts show significant potential for producing high value-added C 2+ products in electrocatalytic CO 2 /CO reduction reactions (CO (2) RR). However, the structural reconfiguration during operation poses substantial challenges in identifying the intrinsic catalytic active site, especially under similar mass transport conditions. Herein, three typical and commercial Cu-based catalysts (Cu, CuO, and Cu 2 O) are chosen as representatives to elucidate the structure-activity relationship of CORR in the membrane electrode assembly electrolyzer. Notably, only the Cu catalyst demonstrates the most suppression of hydrogen evolution reaction, thus achieving the highest FE of 86.7% for C 2+ products at a current density of 500 mA cm –2 and maintaining a stable electrolysis over 110 h at a current of 200 mA cm –2 . The influence of chemical valence state of Cu, electrochemical surface area, and local pH were firstly investigated and ruled out for the significant FE differences. Finally, based on the structure analysis from high resolution transmission electron microscope, OH – adsorption, in situ infrared spectroscopy and density functional theory calculations, it is suggested that the asymmetric C-C coupling ( via *CHO and *CO) is the most probable reaction pathway for forming C 2+ products, with Cu (100)-dominant grain boundaries (GBs) being the most favorable active sites. These findings provide deeper insights into the synergistic relationship between crystal facets and GBs in electrocatalytic systems.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2021
·
IF 7.46
Qiaojuan Zhang,Mengyu Liao,Keren Xiao,Kangyuan Zhuang,Weilian Zheng,Zhiyi Yao
Perfluorooctane sulfonate (PFOS) is the most typical compound as emerging persistent organic pollutants (POPs). It is very significant to monitor PFOS concentration in environmental samples. In this paper, a novel fluorescence probe based on a cationic perylene diimide derivative (PDI-Pyr) toward PFOS detection was designed and synthesized. The sensing properties were investigated systematically by spectroscopic techniques. The detection limit in the method was calculated to be 28 nmol/L. It was found that the formation of PDI-Pyr/PFOScomplex through electrostatic and hydrophobic interactions accounted for the mechanism of the fluorescent assay. This method could be further applied in real tap water samples and environmental samples such as soil extract. To the best of our knowledge, this work is the first report of PDI-based fluorescent sensor for PFOS determination.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Hailin Tian,Tirusew Araya,Ruiping Li,Yanfen Fang,Yingping Huang
Microcystin-LR (MC-LR), which is produced from cyanobacteria, is the common microcystin with a serious threat to aquatic life and human beings. And the efficient removal method of MC-LR is urgent needed. In this work, the MIL-100/MIL-53 (Fe) photocatalysts, which were successfully prepared by the electrostatic interaction with each other, were applied for the photocatalytic degradation of MC-LR. The structure and optical properties of the MIL-100/MIL-53 (Fe) photocatalysts were characterized by using SEM, XRD, XPS, FT-IR and UV–vis DRS. The very low dosage of the MIL-100/MIL-53 (Fe) photocatalysts achieved the degradation of MC-LR, and the optimized loading was the 50% MIL-100/MIL-53 (Fe) photocatalyst. Compared to MIL-100 (Fe) and MIL-53 (Fe), the MC-LR degradation was up to 96.5% after 3 h under visible light illumination with the 50% MIL-100/MIL-53 (Fe) photocatalyst due to the pore-effect adsorption and the effective separation of photogenerated carriers. The effect of coordinate immobilized layers between MIL-100 (Fe) and MIL-53 (Fe) contributed to the stable and efficient removal of MC-LR for the 50% MIL-100/MIL-53 (Fe) photocatalyst. The MC-LR photocatalytic mechanism and degradation pathway, which the photogenerated holes (h + ) were the main active species, were proposed by radical capture experiments and LC-MS analysis.
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