Nature Communications
·
2021
·Vol. 12
·期 1
·1-8
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IF 14.919
Lei Yuting,Zhang Guihua,Zhang Qinglan,Yu Ling,Li Hua,Yu Haili,He Yi
Zeolitic imidazolate frameworks (ZIFs) are very useful as high-capacity iodine (I 2 ) adsorbents. The adsorption performance is usually probed by measuring a statistical average property over an entire sample consisting of a large number of ZIF particles, leaving the interparticle heterogeneity information among individuals. Here we report a dark-field microscopy (DFM) method to visualize gaseous I 2 adsorption on single ZIF-90 particles in situ and in real time. The adsorption of I 2 is found to alter the scattering spectrum of ZIF-90 particles, inducing a distinct color change from bluewhite to yellow. According to correlating the adsorption amount of gaseous I 2 with the change of B value from DFM images, we quantitatively image the adsorption process and estimate the related kinetic parameters at the single particle level. Single particle measurements clarify the large particle-to-particle heterogeneity in adsorption reactivity and significant adsorption activity improvement of ZIF-90 after introduction of linker defects, which provides a microscopic understanding of the structure-activity relationship. We further demonstrate the capacity of this strategy for studying gaseous I 2 adsorption on single ZIF-91 particle as a derivative of ZIF-90 to illustrate the generality.
研究领域:
材料科学
·
化学
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DOI
PubMed
高影响因子
Journal of the American Chemical Society
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2024
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IF 14.4
Xuannuo Yi,Shasha Liu,Taotao Zhao,Xiangke Guo,Kai Zhou,Weiping Ding,Wei Wang
Zeolites are essential solid acid catalysts in various chemical processes. Temperature-programmed desorption (TPD) is one of the most established techniques used to characterize the acidity of zeolites by measuring the desorption kinetics of probes from bulk samples. However, conventional TPD can hardly deliver the intrinsic acid properties of zeolites because the apparent desorption kinetics are inevitably mixed with mass transfer and thermal conduction due to the large sample amount (∼0.1 g). Herein, we developed an optical microscopy approach to measure the TPD spectra of single zeolite nanoparticles, termed oTPD, by in situ monitoring of the reduced scattering intensity of individuals as a result of the desorption of probe molecules during heating. A significantly reduced sample amount contributed to the oTPD spectrum, revealing an intrinsic desorption temperature of ∼300 °C lower than the apparent value and also a greatly narrowed peak width from ∼150 to ∼15 °C. Correlating oTPD and micro-Raman spectra of the very same individuals further uncovered a linear dependence between the acidity and the content of silicon islands. This study provided unprecedented capabilities for measuring the intrinsic acid properties and the desorption kinetics of single zeolite nanoparticles, with implications for better understanding the structure–acidity relationship and for designing better zeolite catalysts.
研究领域:
化学工程
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催化科学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Jingrui Liu,Yimin Xuan,Liang Teng,Qibin Zhu,Xianglei Liu,Yulong Ding
The calcium-based thermochemical energy storage is one of the most promising technologies in the field of solar energy utilization and energy storage. However, the pore-scale spectral absorption and heat and mass transfer processes of calcium-based particles in thermochemical energy storage remain unclear. In this work, the spectral absorption, flow heat transfer and chemical reaction coupling processes are investigated from the perspective of a single modified calcium-based particle. Among them, the spectral absorption properties are studied by Finite-Difference Time-Domain method and Monte Carlo ray tracing method, respectively. At the same time, the flow heat transfer and chemical reaction inside the particles are predicted based on the lattice Boltzmann method. The conversion and storage from solar to chemical energy are realized by simulations and experiments. The results show that the structure and morphology, particle size and solar irradiation flux are the main factors affecting the calcination of single particle calcium carbonate. This method reveals the intrinsic relationship between microscopic spectral absorption and thermal mass transport of single particle, and provides a theoretical basis for the co-design and optimization of photothermal systems at the particle scale.
研究领域:
能源科学
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材料科学
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DOI
高影响因子
INTERNATIONAL JOURNAL OF ENVIRONMENTAL ANALYTICAL CHEMISTRY
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2022
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IF 2.731
Quan Zeng,Ting Xu,Qinshu Kang,Shengqing Li
The existence of inorganic elements in natural water is heterogeneous due to the suspended micro colloidal and nanoparticles. In this work, the signals of Fe, Cu, Cd, Pb content in natural water samples collected from a city lake were examined using the single-particle inductively coupled plasma mass spectrometry (ICP-MS) under the time resolved detection mode. Total numbers, data distributions and central values of the detected signals were obtained based on statistical analysis using the Excel and the Origin software. Both fractionation filtration (0.22, 0.45 and 3.0 µm membranes) and centrifugation (2000, 4000, 6000 and 8000 rpm rotating speed) have a significant effect on the detection of metals coexisted in the natural colloidal particles (NCPs) in water. Notable number of single-particle signals still presents in the lake water samples even after the pretreatment of 0.22 µm filtration or 8000 rpm centrifugation, which reveals the ubiquitous existence of micro aggregates or colloids in natural water. Sampling with online dilution is proved to be a direct, simple and effective method for the implementation of time resolved analysis of metallic micro NCPs in lake water by ICP-MS, especially for elements with high dissolved concentration. The results enhance the knowledge of how-to evaluation of the quantity and chemical stability of metal-containing aggregates, colloids and nanoparticles that may exist in natural water.
研究领域:
环境科学
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分析化学
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产品关联
DOI
高影响因子
ANALYTICAL CHEMISTRY
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2024
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IF 6.7
Zhi-Gang Wang,Yusi Hu,Hao-Yang Liu,Hai-Yan Wen,Bao-Ping Qi,Shu-Lin Liu
Electrochemiluminescence (ECL) imaging, a rapidly evolving technology, has attracted significant attention in the field of cellular imaging. However, its primary limitation lies in its inability to analyze the motion behaviors of individual particles in live cellular environments. In this study, we leveraged the exceptional ECL properties of quantum dots (QDs) and the excellent electrochemical properties of carbon dots (CDs) to develop a high-brightness ECL nanoprobe (CDs-QDs) for real-time ECL imaging between living cells. This nanoprobe has excellent signal-to-noise ratio imaging capabilities for the single-particle tracking (SPT) of biomolecules. Our finding elucidated the enhanced ECL mechanism of CDs-QDs in the presence of reactive oxygen species through photoluminescence, electrochemistry, and ECL techniques. We further tracked the movement of single particles on membrane nanotubes between live cells and confirmed that the ECL-based SPT technique using CD-QD nanoparticles is an effective approach for monitoring the transport behaviors of biomolecules on membrane nanotubes between live cells. This opens a promising avenue for the advancement of ECL-based single-particle detection and the dynamic quantitative imaging of biomolecules.
研究领域:
细胞生物学
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分析化学
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DOI
PubMed
高影响因子
ACS Nano
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2024
·
IF 15.8
Bei Li,Min Lv,Yujia Zhang,Xueqin Gong,Zaizhu Lou,Zeyan Wang,Yuanyuan Liu,Peng Wang,Hefeng Cheng,Ying Dai,Baibiao Huang,Zhaoke Zheng
Piezoelectric-assisted photocatalysis has a huge potential in solving the energy shortage and environmental pollution problems, and imaging their detailed charge-transfer process can provide in-depth understanding for the development of high-active piezo-photocatalysts; however, it is still challenging. Herein, topotactic heterostructures of TiO2@BaTiO3 (TO@BTO-S) were constructed by the epitaxial growth of ferroelectric BaTiO3 mesocrystals on TiO2-{001} facets, resulting in a ferroelectric photocatalyst with a polarization orientation on the surface. Notably, the photoinduced charge transfer in ferroelectric TiO2@BaTiO3 was accurately monitored and directly visualized at the single-particle level by the advanced photoluminescence (PL) imaging microscopy systems. The longer PL lifetime of TO@BTO-S demonstrated the efficient charge separation caused by a built-in electric field, which is constructed by the polarization orientation of BaTiO3 mesocrystals. Therefore, the TO@BTO-S heterostructure exhibits efficient piezoelectric-assisted photocatalytic pure water splitting, which is 290 times higher than photocatalysis. This work revealed time/spatial-resolved photoinduced charge transfer in piezoelectric assistance photocatalysts at the single-particle level and demonstrated the great role of polarization orientation in promoting charge transfer for photocatalysis.
研究领域:
材料科学
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环境科学
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DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2023
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IF 11.4
Qingsheng Bai,Qingcun Li,Jingfu Liu
The potential risk of various silver-containing nanoparticles (AgCNPs) in soils is related to the concentration, size, and speciation, but their determination remains a great challenge. Herein, we developed an effective method for determining the particle number, size, and species of dominant AgCNPs in soils, including nanoparticles of silver (Ag NPs), silver chloride (AgCl NPs), and silver sulfide (Ag2S NPs). By ultrasonication wand-assisted tetrasodium pyrophosphate extraction, these AgCNPs were extracted efficiently from soils. Then, multistep selective dissolution of Ag NPs, AgCl NPs, and whole Ag NPs/AgCl NPs/Ag2S NPs was achieved by 1% (v/v) H2O2, 5% (v/v) NH3·H2O, and 10 mM thiourea in 2% (v/v) acetic acid, respectively. Finally, the particle number concentration and size distribution of AgCNPs in the extracts and the remaining AgCNP particle number concentration after each dissolution were determined by single-particle inductively coupled plasma mass spectroscopy for speciation of the dominant AgCNPs. AgCNPs were detected in all five soil samples with the concentrations of 0.23–8.00 × 107 particles/g and sizes of 16–110 nm. Ag2S NPs were the main form of AgCNPs in the examined soils with the percentage range of 53.98–69.19%, followed by AgCl NPs (11.42–23.31%) and Ag NPs (7.78–16.19%). Our method offers a new approach for evaluating the occurrence and potential risk of AgCNPs in environmental soils.
研究领域:
环境科学
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分析化学
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PubMed
高影响因子
LAB ON A CHIP
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2025
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IF 5.4
Chunhua He,Huasheng Zhuo,Canfeng Yang,Jianxin Wang,Xian Jiang,Fan Li,Chengxu Lin,Hai Yang,Tuying Yong,Xiangliang Yang,Zhiyong Liu,Yan Ma,Lei Nie,Guanglan Liao,Tielin Shi
Target particle encapsulation is crucial in droplet microfluidics for high-throughput applications like single-cell sequencing and drug screening. However, it faces limitations, with encapsulation rates of only 10% to 30% due to suspension density and the inherent functionality of the chip being restricted by the Poisson distribution. This leads to reagent waste and reduced effectiveness in applications requiring ultra-high multiplexing or extensive particle analysis, due to the massive empty droplets. Here we propose a droplet microfluidic system integrating surface acoustic wave (SAW) and sheath flow control. Suspensions of varying concentrations within the channel are initially pre-focused by sheath fluid, and then acoustically focused into a linear arrangement by SAW. Spacing between particles can be regulated by modulating the sheath fluid, ensuring sequential encapsulation of cells or beads in individual droplets. Thermal shock generated by the SAW, particle and droplet frequency, and particle encapsulation ratio are all elaborately evaluated. The results demonstrate that our system reaches an exciting single-bead packing efficiency of up to 78%, and achieves a packing rate of more than 60% for both high and low concentrations of solutions for polystyrene microspheres, magnetic beads and H22 cells, 6 times higher than the theoretical upper limit of the conventional method and 1.8 times higher than the Poisson distribution. More importantly, our system is designed to be free of structural and parametric constraints, which is quite important in future practical application. Thus, our on-chip particle focusing control method and droplet microfluidic system provide great potential in biological applications needing a high single-particle encapsulation ratio in limited partitions, such as ultra-high multiplex digital biomolecular detection, single-cell analysis, drug screening, and single exosome detection.
研究领域:
生物技术
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医学工程
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分子生物学
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DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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IF 7.963
Wen-Jing Wei,Lei Li,Yu-Pei Gao,Qiang Wang,Yao-Yu Zhou,Xin Liu,Yuan Yang
Plants can absorb and accumulate engineered nanomaterials (ENMs) through water and soil, providing a potential way for nanoparticles to be enriched in humans through the food chain. In this paper, a combination of enzymatic digestion method and SP-ICP-MS analysis was used to quantitatively characterize the enriched AuNPs in mustard and lettuce plants. The results showed that Macerozyme R-10 enzyme can extract AuNPs from plants without obvious aggregation/dissolution. Both mustard and lettuce plants can absorb and enrich the complete AuNPs to the above-ground organs, and the particle number concentrations detected are 1.24 × 10 7 particles L −1 and 4.39 × 10 7 particles L −1 , respectively. With different exposure level of AuNPs(0.5 mg L −1 ,), a particle number concentration of 2.32 × 10 7 particles L −1 was detected in the stems of lettuce plants, while the mustard failed to transport AuNPs to the above-ground organs. The transport efficiency of Au ions by plants is higher than that of AuNPs, and the plants have stronger bioavailability for ions.
研究领域:
植物学
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环境科学
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纳米毒理学
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DOI
PubMed
高影响因子
MICROCHEMICAL JOURNAL
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2022
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IF 5.304
Xiang Yuan,Huiling Zhang,Xiang Yuan,Guojiang Mao,Lin Wei
In this work, we demonstrate a simple and label-free single particle detection (SPD) method for the quantification of melamine (Mel) based MnO 2 -modified gold nanoparticles (Au@MnO 2 NPs). Without Mel, MnO 2 shell of Au@MnO 2 NPs are able to be directly decomposed by gallic acid. In the existence of Mel, the decomposition process is restrained due to the strong hydrogen bonding between Mel and gallic acid. The selective etching of MnO 2 shell on AuNPs surface results in evident color change from single Au@MnO 2 NPs. Through quantitatively enumerating the number of color coded particles, trace amounts of Mel can be accurately detected. A linear range from 0.02 to 1 μM (R 2 = 0.98) and a limit of detection of 16.7 nM are acquired. In milk sample, satisfactory recovery was acquired. Therefore, the SPD method is expected to be used for the detection of various chemical contaminants in food.
研究领域:
分析化学
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食品安全
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产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2024
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IF 10.8
Xiangwei Tian,Qingqing Yang,Yuqian Zhao,Dandan Cao,Yanwei Liu,Yingying Guo,Wenbin Cui,Ligang Hu,Yongguang Yin,Yong Cai,Guibin Jiang
Dust released from widely established plastic sports courts and synthetic turf poses potential environmental and health risks. Herein, we systematically investigate the metal(loid) characteristics, potential sources, and health risks of 162 dust samples from 17 campuses in Beijing, using complementary analytical techniques. Bulk analysis revealed higher levels of Zn, Pb, Cu, Sb, Cd, and Cr than background values, suggesting excessive anthropogenic contamination. Pb and Cr in plastic basketball court and track dust and Zn and Sb in synthetic turf dust were higher than those in other sports facilities. Multielement single-particle inductively coupled plasma time-of-flight mass spectrometry (spICP-TOF-MS) revealed more Fe-, Al-, Si-, Ti-, and Pb-containing particles in the dust. At least 92% toxic Pb-containing particles were composed of multiple elements. The significant correlations between Pb and Cr contents on individual dust particles support their common potential source from inorganic pigments (crocoite, PbCrO4). Pb, Sb, As, and Cr in the dust pose higher health risks through intake. The risks were estimated to be approximately 3–5 times higher for children than for adults. Additionally, highly toxic Cr(VI) and As(III) species were observed in the sweat and gastric juice leachate of dust, highlighting severe threats of the metal(loid)s to human health.
研究领域:
环境科学
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公共卫生
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分析化学
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产品关联
DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
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2024
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IF 6.7
Jing Shang,Siyu Jiang,Pei Zhang,Jinsong Fan,Kun Li
Dark-field microscopy (DFM) imaging based on plasmonic metal nanoparticles has garnered significant attention. Here, we exploit the susceptibility of MnO2 to reduction to modulate the local dielectric environment of an Au nanoparticle core through the etching/antietching effects of specific targets on the encapsulated MnO2 shell. The presence of d-penicillamine promotes MnO2 etching, while the chelation of d-penicillamine with Cu2+ effectively inhibits this etching. By recording the Cu2+-induced color shift of scattered light from orange to bright green at the single-particle level and performing the statistical analysis of the green-to-red (G/R) values in DFM images, we achieved quantitative determination of Cu2+ with a wide linear range (0.1–10 μM) and a low limit of detection (4.55 nM). With the facile and reliable Cu2+ assay in real-world samples exemplifying the practicality of the single-particle nanoplasmonic imaging method, this work may inspire future DFM-based investigations of nanoshell etching inhibition processes.
研究领域:
分析化学
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纳米生物学
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产品关联
DOI
PubMed
高影响因子
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