INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2021
·Vol. 22
·期 15
·8250
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IF 5.924
Shanmeiyu Zhang,Yanyan Zhang,Chongchong Wu,Hui Yang,Qiqi Zhang,Fuyi Wang,Jingyi Wang,Ian Gates,Jinben Wang
Although small water clusters (SWCs) are important in many research fields, efficient methods of preparing SWCs are still rarely reported, which is mainly due to the lack of related materials and understanding of the molecular interaction mechanisms. In this study, a series of functional molecules were added in water to obtain small water cluster systems. The decreasing rate of the half-peak width in a sodium dodecyl sulfate (SDS)–water system reaches ≈20% at 0.05 mM from17O nuclear magnetic resonance (NMR) results. Based on density functional theory (DFT) and molecular dynamics (MD) simulation calculation, it can be concluded that functional molecules with stronger negative electrostatic potential (ESP) and higher hydrophilicity have a stronger ability to destroy big water clusters. Notably, the concentrations of our selected molecule systems are one to two magnitudes lower than that of previous reports. This study provides a promising way to optimize aqueous systems in various fields such as oilfield development, protein stability, and metal anti-corrosion.Keywords:water cluster;functional molecule;molecular interaction
研究领域:
化学
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材料科学
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DOI
PubMed
高影响因子
Science China-Chemistry
·
2020
·Vol. 63
·期 12
·1777-1784
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IF 6.356
Ma Xiaoshuang,Ma Guanyu,Qin Lubing,Chen Guangxu,Chen Shaowei,Tang Zhenghua
Despite the recent progress on controllable synthesis of alkynyl-protected Au nanoclusters, the effective synthetic means are very limited and the cluster formation process still remains puzzling. Here, we develop a novel synchronous nucleation and passivation strategy to fabricate Au 36 (PA) 24 (PA=phenylacetylenyl) nanoclusters with high yield. In Au 36 (PA) 24 formation process, Au 22 (PA) 18 as key intermediate was identified. Meanwhile, Au 22 (PA) 18 can be synthesized under a low amount of reductant, and by employing more reductants, Au 22 (PA) 18 can turn into Au 36 (PA) 24 eventually. Moreover, the structure evolution from Au 22 (PA) 18 to Au 36 (PA) 24 is proposed, where four Au 13 cuboctahedra can yield one Au 28 kernel. Finally, the ratiocination is verified by the good accordance between the predicted intermediate/product ratio and the experimental value. This study not only offers a novel synthetic strategy, but also sheds light on understanding the structural evolution process of alkynyl-protected Au nanoclusters at atomic level.
研究领域:
材料科学
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纳米技术
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化学
✓ 已验证
产品关联
DOI
高影响因子
Exploration
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2024
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IF 0
Yunshan Gao,Jie Xu,Shaohua Qu,Yixiao Li,Gleb B. Sukhorukov,Li Shang
Silver nanoclusters (AgNCs) have shown broad application prospects in catalysis, sensing, and biological fields. However, the limited stability of AgNCs has become the main challenge restricting their practical application in complex environments. Herein, a mussel-inspired, dopamine-assisted self-assembly approach is reported to fabricate 3D AgNC aerogels (PDA/AgNCs), which possess significantly enhanced structural stability and synergistic functional properties. The prepared AgNC aerogels display a hierarchical network structure with an ultrafine ligament size of 10.3 ± 1.2 nm and a high specific surface area of 50.7 m 2 g −1 . The gelation mechanism is elucidated by in-depth characterization and time-lapse monitoring of the gelation process vis spectroscopic and microscopic approaches. Owing to the distinct features of aerogels and the synergistic effect of AgNCs and PDA, the fabricated aerogels can not only efficiently decolorize dyes with a faster kinetic than individual AgNCs, but also exhibit remarkable broad-spectrum antimicrobial activity. Consequently, a conceptual water-treatment device is established by depositing PDA/AgNC aerogels on the cotton substrate, which shows good performance in both catalytic dye degradation and bacterial killing in the flowing system. This mussel-inspired self-assembly strategy has great potential in developing robust AgNC-based functional materials, which also provides a new guideline for designing sophisticated materials with integrated functions and synergistic properties.
研究领域:
材料科学
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化学
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环境科学
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DOI
APPLIED BIOCHEMISTRY AND BIOTECHNOLOGY
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2025
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IF 3.3
Zhang Xiuju,Nie Xiaowei,Yu Wenxiao,Du Guanchao,Liu Shaoming,Song Yewen
MicroRNA (miRNA) has emerged as a potential diagnostic marker for malignancies, such as prostate cancer; yet, few analytical approaches have been established for the simple and effective identification and quantification of miRNA. We depict here a fluorescent dumbbell probe utilizing DNA-silver nanoclusters (DNA-AgNCs) to facilitate the simple and label-free quantification of miRNA. The fluorescent probe was methodically engineered using a double-flapped dumbbell structure, wherein the 5′ flap was synthesized using DNA-AgNCs, and the 3′ flap was extended by a G-rich sequence. The DNA scaffold rigidifies the DNA-AgNCs and the G-rich sequence, bringing them into close contact, which leads to enhanced fluorescence due to the activation of DNA-AgNCs by the G-rich sequence. Upon the introduction of miRNA, the 5′ flap of the probe unfolds, liberating the G-rich sequence from the probe, disrupting the closeness between DNA-AgNCs and the G-rich region, and resulting in decreased fluorescence. The proposed method, by incorporating target recycling and polymerase/endonuclease-assisted cycles, enables sensitive detection of miRNA with a detection limit of 4.2 fM and demonstrates high specificity for monitoring target miRNA in clinical samples, offering a robust platform for miRNA monitoring and disease diagnosis. Graphical
研究领域:
生物化学
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分子生物学
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医学诊断
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DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
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2018
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IF 6.042
Jian-Yu Yang,Ting Yang,Xiao-Yan Wang,Ming-Li Chen,Yong-Liang Yu,Jian-Hua Wang
Fluorescent nanoparticles are widely used for sensing biologically significant species. However, there are only rare reports of the discrimination or speciation of metal species. In this work, we report for the first time the speciation of mercury (Hg2+) and methylmercury (CH3Hg+) by taking advantage of the fluorescence feature of folic-acid-capped gold nanoclusters (FA-AuNCs). FA-Au NCs exhibit an average size of 2.08 ± 0.15 nm and a maximum emission at λex/λem = 280/440 nm with a quantum yield of 27.3%. It is interesting that Hg2+ causes a significant quench of the fluorescence of FA-Au NCs, whereas CH3Hg+ leads to a remarkable fluorescence enhancement. On the basis of this discriminative fluorescent response between Hg2+ and CH3Hg+, a novel nanosensor for the speciation of CH3Hg+ and Hg2+ was developed, providing limits of detection (LODs) of 28 nM for Hg2+ and 25 nM for CH3Hg+ within 100–1000 nM. This sensing system is highly selective to mercury. Its practical applications were further demonstrated by the analysis of CH3Hg+ and the speciation of mercury (CH3Hg+ and Hg2+) in environmental water and fish samples.
研究领域:
环境科学
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分析化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Cheng-wang Shi,Xiao-dong Li,Xu-feng Zhang,Mei-shuai Zou
Thermosetting epoxy resins with high strength , high toughness, and recyclability are strongly sought after, but due to crosslinked structure, balancing strength and toughness and achieving degradation and reprocessing of resins is a challenge. Enhancing strength without compromising toughness during designing recyclable epoxy resin is a challenging task. Herein, a solution is demonstrated where isofluorodioxanone diisocyanate (IPDI), Poly (propylene glycol) bis(2-aminopropyl ether) (D230), and naturally occurring vanillin synthesized a novel imine-functionalized epoxy monomer (IDV-EP), and cured with diamino-diphenylmethane (DDM), 2-(4-aminophenyl)-1H-benzimidazol-5-amine (APBIA) and 4, 4-diamino benzoyl triphenylamine (DABA), respectively, for the purpose of building different contents of the sacrificial hydrogen-bonding clusters (SHBC) in topological network structures. As the hydrogen-bonding (H-bonding) binding energy of the crosslinked network increases, the strength and toughness of the resin were increased concurrently, SHBC was demonstrated to be a feasible method to achieve the strength-toughness trade-off of thermosets, in which IDV-EP-DABA illustrated a tensile strength of 90 MPa, an elongation at break of 16.5%, as well as toughness of 9.73 MJ/m 3 , which was higher than that of the ordinary bisphenol A-type epoxy thermosetting resin (DGEBA/DDM) by 1.8, 3.7 as well as 6.7 times, respectively. Furthermore, the covalent adaptive networks (CANs) formed by imine bonds provide the resins with effective capabilities for swift degradation (rapid degradation in acid/solvent, room temperature and static conditions) and reprocessing (only a slight decrease in the mechanical properties after hot pressed at 180°C/10 MPa for 15 minutes) , showcasing promising prospects for sustainable utilization.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
ADVANCED MATERIALS
·
2024
·Vol. 36
·期 30
·2401694
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IF 27.4
Yin Zhu,Yanxu Chen,Yafei Feng,Xiangmin Meng,Jing Xia,Genqiang Zhang
Hydrazine oxidation-assisted water splitting is a critical technology to tackle the high energy consumption in large-scale H 2 production. Ru-based electrocatalysts hold promise for synergetic hydrogen reduction (HER) and hydrazine oxidation (HzOR) catalysis but are hindered by excessive superficial adsorption of reactant intermediate. Herein, this work designs Ru cluster anchoring on NiFe-LDH (denoted as Ru c /NiFe-LDH), which effectively enhances the intermediate adsorption capacity of Ru by constructing Ru─O─Ni/Fe bridges. Notably, it achieves an industrial current density of 1 A cm −2 at an unprecedentedly low voltage of 0.43 V, saving 3.94 kWh m −3 H2 in energy, and exhibits remarkable stability over 120 h at a high current density of 5 A cm −2 . Advanced characterizations and theoretical calculation reveal that the presence of Ru─O─Ni/Fe bridges widens the d-band width (W d ) of the Ru cluster, leading to a lower d-band center and higher electron occupation on antibonding orbitals, thereby facilitating moderate adsorption energy and enhanced catalytic activity of Ru.
研究领域:
材料科学
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电化学
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能源技术
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DOI
PubMed
高影响因子
Theranostics
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2022
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IF 11.6
Bohan Yin,Qin Zhang,Xinyue Xia,Chuanqi Li,Willis Kwun Hei Ho,Jiaxiang Yan,Yingying Huang,Honglian Wu,Pui Wang,Changqing Yi,Jianhua Hao,Jianfang Wang,Honglin Chen,Siu Hong Dexter Wong,Mo Yang
Background: CRISPR-Cas12a has been integrated with nanomaterial-based optical techniques, such as surface-enhanced Raman scattering (SERS), to formulate a powerful amplification-free nucleic acid detection system. However, nanomaterials impose steric hindrance to limit the accessibility of CRISPR-Cas12a to the narrow gaps (SERS hot spots) among nanoparticles (NPs) for producing a significant change in signals after nucleic acid detection. Methods: To overcome this restriction, we specifically design chimeric DNA/RNA hairpins (displacers) that can be destabilized by activated CRISPR-Cas12a in the presence of target DNA, liberating excessive RNA that can disintegrate a core-satellite nanocluster via toehold-mediated strand displacement for orchestrating a promising “on-off” nucleic acid biosensor. The core-satellite nanocluster comprises a large gold nanoparticle (AuNP) core surrounded by small AuNPs with Raman tags via DNA hybridization as an ultrabright Raman reporter, and its disassembly leads to a drastic decrease of SERS intensity as signal readouts. We further introduce a magnetic core to the large AuNPs that can facilitate their separation from the disassembled nanostructures to suppress the background for improving detection sensitivity. Results: As a proof-of-concept study, our findings showed that the application of displacers was more effective in decreasing the SERS intensity of the system and attained a better limit of detection (LOD, 10 aM) than that by directly using activated CRISPR-Cas12a, with high selectivity and stability for nucleic acid detection. Introducing magnetic-responsive functionality to our system further improves the LOD to 1 aM. Conclusion: Our work not only offers a platform to sensitively and selectively probe nucleic acids without pre-amplification but also provides new insights into the design of the CRISPR-Cas12a/SERS integrated system to resolve the steric hindrance of nanomaterials for constructing biosensors.
研究领域:
生物技术
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分析化学
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分子生物学
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DOI
PubMed
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
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2020
·
IF 2.726
Yanling Shi,Song Ye,Huazhen Liao,Junfang Liu,Deping Wang
Faujasite (FAU) type zeolite is built from sodalite cages that joined by oxygen bridges between the hexagonal faces, and is characteristic of high cation exchange capacity and thermal stability. In this research, the FAU-NaX zeolite with Na/Si/Al molar ratio of 4.08:1.4:1.0 was prepared with template-free hydrothermal method and then confirmed with XRD analysis , based on which a series of Ag + or/and Eu 3+ loaded zeolites were obtained through the ion-exchange procedure. The PL spectra measurement indicated that after heat treatment at optimized temperatures between 400-600 °C, the Ag + loaded zeolites showed strong green visible emission centered around 540–550 nm, which is due to the formation of Ag 3 n+ clusters. Furthermore, efficient energy transfer from silver-clusters to Eu 3+ can be achieved in the Ag + /Eu 3+ loaded zeolites, and the energy transfer efficiency that evaluated with silver-clusters lifetimes are 23.9%, 44.6%, 67.4% and 73.6%, respectively, in ZX-2Eu30Ag, ZX-5Eu30Ag, ZX-10Eu30Ag and ZX-20Eu30Ag. Besides, the XPS measurements implied that the loading of Eu 3+ resulted in a further reduction of silver-clusters, which can also promote the formation of silver-clusters without heat treatment. This new class of metal-clusters and rare earth (RE) ions co-actived phosphors may offer interesting perspective applications in optoelectronics and lighting.
研究领域:
材料科学
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光学
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2015
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IF 4.529
Jian Rong Zhang,Ai Lian Zeng,Hong Qun Luo,Nian Bing Li
In this work, a simple and sensitive Cr(VI) sensor is proposed based on fluorescent polyethyleneimine-stabilized Ag nanoclusters, which allows the determination over a wide concentration range of 0.1 nM–3.0 μM and with a detection limit as low as 0.04 nΜ and a good selectivity. The quenching mechanism was discussed in terms of the absorption and fluorescence spectra, suggesting that Cr(VI) is connected to Ag nanoclusters by hydrogen bond between the oxygen atom at the vertex of tetrahedron structure of Cr(VI) and the amino nitrogen of polyethyleneimine that surrounded Ag nanoclusters and electron transfer from Ag nanoclusters to highly electron-deficient Cr(VI) results in fluorescence quenching. Despite the failure to quench the fluorescence efficiently, Cr(III) can also be measured using the proposed Ag nanoclusters by being oxidized to Cr(VI) in alkaline solution (pH ∼9) containing H 2 O 2 . Therefore, our approach could be used to detect Cr(VI), Cr(III) and the total chromium level in aqueous solution. In addition, Cr(VI) analysis in real water samples were satisfactory, indicating this method could be practically promising for chromium measurements.
研究领域:
分析化学
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环境科学
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产品关联
DOI
PubMed
高影响因子
RENEWABLE ENERGY
·
2022
·
IF 8.634
Siteng Rong,Hongzi Tan,Zhaobin Pang,Zhiyuan Zong,Rongrong Zhao,Zhihe Li,Zhe-Ning Chen,Ning-Ning Zhang,Weiming Yi,Hongyou Cui
Lignin could be depolymerized into large amount of phenolic compounds via fast pyrolysis . The upgrade of phenolic compounds via hydrodeoxygenation (HDO) involves multiple reaction pathways. It is challenging to selectively remove the oxygen-containing groups while keeping the aromatic rings intact. In this work, hierarchical Nb 2 O 5 (H–Nb 2 O 5 ) microspheres with abundant oxygen vacancies were synthesized to anchor the Pd clusters, which is featured with strong metal-support interaction via the electron transfer between Pd species and Nb species. For phenol HDO reaction, the oxygen vacancies were prone to interact with the phenolic hydroxy groups, resulting in phenol molecule adsorbed in a “nonplanar” manner, greatly weakening the C Ar -O bonds and averting the ring hydrogenation. Besides, the activated hydrogen atoms on Pd clusters could migrate to the vicinity of oxygen vacancies via spillover, promoting the cleavage of C Ar -O bond to obtain benzene. Current work provides a deep insight into the synergetic catalytic mechanism of Pd/H–Nb 2 O 5 catalyst for phenol HDO reaction, and also sheds light on the design and synthesis of high-efficient catalysts in other heterogeneous catalysis fields.
研究领域:
催化化学
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材料科学
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能源化学
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产品关联
DOI
高影响因子
ENVIRONMENTAL MICROBIOLOGY
·
2022
·Vol. 24
·期 12
·6307-6319
·
IF 5.476
Chao-Fan Yin,Ying Xu,Tao Li,Ning-Yi Zhou
Alkane constitutes major fractions of crude oils, and its microbial aerobic degradation dominantly follows the terminal oxidation and the sub-terminal pathways. However, the latter one received much less attention, especially since the related genes were yet to be fully defined. Here, we isolated a bacterium designated Acinetobacter sp. strain NyZ410, capable of growing on alkanes with a range of chain lengths and derived sub-terminal oxidation products. From its genome, a s econdary a lcohol d egradation gene cluster ( sad ) was identified to be likely involved in converting the aliphatic secondary alcohols (the sub-terminal oxidation products of alkanes) to the corresponding primary alcohols by removing two-carbon unit. On this cluster, sadC encoded an alcohol dehydrogenase converting the aliphatic secondary alcohols to the corresponding ketones; sadD encoded a Baeyer–Villiger monooxygenase catalysing the conversion of the aliphatic ketones to the corresponding esters; SadA and SadB are two esterases hydrolyzing aliphatic esters to the primary alcohols and acetic acids. Bioinformatics analyses indicated that the sad cluster was widely distributed in the genomes of probable alkane degraders, apparently coexisting (64%) with the signature enzymes AlkM and AlmA for alkane terminal oxidation in 350 bacterial genomes. It suggests that the alkane sub-terminal oxidation may be more ubiquitous than previously thought.
研究领域:
微生物学
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环境科学
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分子生物学
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）