Journal of Materials Chemistry A
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2025
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IF 9.5
Yunxiang Zhang,Zhichao Mu,Chenliang Zhou,Hazem Abdelsalam,Xingmeng Zhou,Lin Shi,Zhili Chen,Yiran Liang,Zhongjie Wang,Qinfang Zhang
Bi-based Sillén–Aurivillius oxyhalides have attracted extensive attention from researchers owning to their wide range of light absorption, appropriate band structure, and excellent stability; however, their practical application is still limited by their rapid charge recombination. Herein, silver (Ag)-cluster-decorated novel Sillén–Aurivillius oxyhalides (bismuth iron titanium oxyhalide (Bi7Fe2Ti2O17Cl)) with abundant oxygen vacancies (OVs), were successfully synthesized to achieve efficient light absorption and interfacial charge separation. The optimal Ag/Bi7Fe2Ti2O17Cl composites showed excellent tetracycline hydrochloride (TCH) degradation and CO2 reduction efficiencies. The theoretical and experimental results demonstrate that the superior activity is primarily due to the increased magnetic moment of Bi7Fe2Ti2O17Cl induced by the interactions between Ag and O atoms, which strengthens the built-in electric field at the Schottky junction interface and promotes the transfer of photogenerated electrons from Ag clusters to oxyhalides, thus enhancing the generation of charge carriers in the semiconductor and inhibiting bulk recombination. Simultaneously, the synergistic effects of the thermodynamics and kinetics of photocatalytic CO2 reaction along with a lower Gibbs free energy are also responsible for the outstanding CO generation process. This work emphasizes the promising role of metal clusters as co-catalysts in the field of photocatalysis.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
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IF 15.7
Xu Guangyuan,Peng Xingjie,Wu Chuanqiang,Xi Shibo,Xiang Huixin,Feng Lei,Liu Zhendong,Duan Yi,Gan Lijin,Chen Si,Kong Yuan,Ma Yanzhe,Nie Fujing,Zhao Jie,Hai Xiao,Wei Wei,Zhou Meng,Wang Tianfu,Yao Chuanhao,Zhou Wu,Yan Huan
CO 2 electroreduction to CO promises to give an efficient strategy for CO 2 fixation and transformation. However, current reported active sites fail to deliver sufficient activity with high CO Faradic efficiency (FEco) over a wide range of potential. Here, we show a general synthetic protocol to fabricate a batch of highly pure and active NiN 2 catalysts with precise engineering of the uniform-large ( UL ) vacancy around the active sites, which is accomplished through the ‘pre-deposition + pyrolysis’ of various atomically precise Ni clusters (Ni n ) and in-situ etching of the support by the ‘nano bomb’ (sulfur-ligand in the clusters). The NiN 2 sites with UL vacancies could achieve a high turnover frequency (TOF) of 350000 h −1 with ~100% FEco in a wide potential range of 1500 mV. In-situ infrared spectra and theoretical calculations reveal that a highly pure NiN 2 site with UL vacancy contributes to this remarkable catalytic performance compared to the counterparts. This general synthetic strategy enables us to simultaneously engineer active sites and surrounding vacancies with the employment of atomically precise metal clusters, thereby enhancing catalytic performance for other specific reactions.
研究领域:
材料科学
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电化学
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催化反应
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DOI
PubMed
高影响因子
FUEL
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2024
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IF 6.7
Caijun Deng,Chaofan Qi,Zongping Xue,Kai Cui,Xiaomin Wu,Guohua Jing,Huawang Zhao
Hydrogen is a promising clean energy source, and formic acid serves as a significant hydrogen storage material. The electrocatalytic reduction of carbon dioxide (ECO 2 RR) is a promising approach to produce fromate. However, the challenge lies in developing high-performance electrocatalysts for the conversion of CO 2 to formate, due to the limited intrinsic activity, conductivity, and the low density of active sites. In this work, we have fabricated highly active and selective CH 3 COO(BiO) (BiOAc) nanosheets. These nanosheets undergo a transformation into Bi clusters-BiO 2 CO 3 during electrolysis, endowing the material with superior electrocatalytic capabilities for CO 2 reduction to formate, with a Faradaic selectivity of over 90 % across a wide potential window from −0.8 to −1.3 V. Additionally, this catalyst can sustain high current densities above 80 mA cm −2 at low applied potentials without compromising selectivity in a H type electron reactor. Both density functional theory (DFT) and in situ attenuated total reflection-infrared spectroscopy (in situ ATR-IR) findings indicate that the Bi 3+ with reduced density facilitate the activation of CO 2 to *CO 2 , while the charge density-enriched Bi 0 atoms in Bi cluster promote the capture of HCO 3 – and enhance subsequent proton-coupled electron transfer reactions. Collectively, these factors significantly reduce the energy barrier for *OCHO formation on BiOAc, thereby enhancing its catalytic activity and Faradaic efficiency for the electroreduction of CO 2 .
研究领域:
材料科学
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环境科学
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电化学
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DOI
高影响因子
MICROCHIMICA ACTA
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2020
·Vol. 187
·期 6
·1-9
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IF 6.232
Li Wanying,Qian Hui,Liu Rui,Zhao Xiaoli,Tang Zhi,Huang Xianhuai,Li Weihua,Chen Xiaoming,Xie Fazhi,Zou Wensheng,Qu Qishu
Based on a detailed study of the hydrolysis process of tetrabutyl orthotitanate (TBOT), TiO 2 nanoclusters were modified inside the pores of SiO 2 core-shell particles instead of the outside. The pore size distribution of SiO 2 core-shell spheres modified with TiO 2 (SiO 2 @ d SiO 2 @TiO 2 ) was analyzed by Barrett-Joyner-Halenda (BJH) method and density functional theory (DFT) method, respectively. The results of the DFT calculations demonstrate that the TiO 2 nanoclusters are always first formed in bulk solution and then enter the pores. By regulating the rate of hydrolysis of TBOT, almost all of the TiO 2 nanoclusters are modified into the pores and the structure of the original SiO 2 core-shell sphere is hardly affected. The morphology of the particles was characterized by scanning electron microscopy and transmission electron microscopy. The crystal phase of TiO 2 was measured by XRD. SiO 2 @ d SiO 2 @TiO 2 spheres functionalized with C18 were packed into a stainless steel column. The chemical stability of SiO 2 @ d SiO 2 @TiO 2 spheres under alkaline was tested by flushing of a mobile phase at pH 13 for 7 days. The efficiency of the column after the alkali solution treatment still reaches 98,430 plates m −1 , which is only about 1.6% lower than that before the alkali solution treatment. A series of basic and acidic analytes were also separated on the column.
TiO 2 nanocrystals were coated into the pore of core-shell silica spheres. The prepared particles were packed into the column and separation performance up to 98,430 plates per meter was achieved.
研究领域:
材料科学
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分析化学
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DOI
PubMed
高影响因子
Chem
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2024
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IF 19.1
Ying-Xue Yuan,Jia-Ni Zhang,Jun-Ru Wang,Kai Li,Shuang-Quan Zang
The construction of effective artificial chiral light-harvesting systems ( C -LHSs) is significantly important as it provides insights into the hierarchical levels of chirality evolution in natural systems. Herein, we devised pairs of chiral blue emitters, S -/ R -binaphthalene dioxygen- N -octadecamidephthalimide ( S -/ R -BPOA), which function as donors of chirality and light absorbers. S -/ R -BPOA co-assembled with enantiomers of atomically precise yellow-emitting subnanometer-scale Ag 6 clusters to fabricate C -LHSs. Within these hybrid C -LHSs, we successfully resolved enantioselective chirality/energy transfer that was dependent on the handedness of the components. This promoted the efficient circularly polarized energy transfer in chirality-compatible ensembles, resulting in a remarkable amplification of circularly polarized luminescence (CPL) in the ultrasmall silver cluster. The achieved dissymmetry factor ( g lum ) reached an impressive value of 1.54 × 10 −2 , and white-light CPL with chromaticity coordinates of (0.32, 0.33) was obtained. Furthermore, the customizable fluorescence and CPL in these C -LHSs bestow them with potential application possibilities in information storage and encryption.
研究领域:
材料科学
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光学
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化学
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DOI
高影响因子
TALANTA
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2024
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IF 5.6
Na Li,Qing-Hong Long,Xin-Yuan Li,Can Dong,Tian-Sheng Zhao,Xi Mai,Yong-Sen Zhao,Zhong-Feng Gao,Qin Wei,Fan Xia
Understanding charge transport in metal ion-mediated glutathione-stabilized gold nanoclusters (GSH-Au NCs) has proved difficult due to the presence of various competitive mechanisms, such as electron transfer (ET) and aggregation induction effect (AIE). In this paper, we present a dual-channel fluorescence (FL) and second-order Rayleigh scattering (SRS) sensing method for high-throughput classification of metal ions, relying on the competition between ET and AIE using GSH-Au NCs. The SRS signals show significant enhancement when Pb 2+ , Ag + , Al 3+ , Cu 2+ , Fe 3+ , and Hg 2+ are present, as a result of the aggregation of GSH-Au NCs. Notably, the fluorescence signal exhibits the opposite trend. The FL intensities of GSH-Au NCs are enhanced by Pb 2+ , Ag + , and Al 3+ through the AIE mechanism, while they are quenched by Cu 2+ , Fe 3+ , and Hg 2+ , which is dominated by the ET mechanism. By employing principal component analysis and hierarchical cluster analysis, these signals are transformed into unique fingerprints and Euclidean distances, respectively, enabling successful distinction of six metal ions and their mixtures with a low detection limit of 30 nM. This new strategy has successfully addressed interference from impurities in the testing of real water samples, demonstrating its strong ability to detect multiple metal ions. Impressively, we have achieved molecular cryptosteganography, which involves encoding, storing, and concealing information by transforming the selective response of GSH-Au NCs to binary strings. This research is anticipated to advance utilization of nanomaterials in logic sensing and information safety, bridging the gap between molecular sensors and information systems.
研究领域:
分析化学
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纳米科学
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信息加密
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DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
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IF 5.4
Yu Chen,Huan Chen,Haihua Wang,Xia Xin,Wenbing Kang
Silver nanoclusters (NCs) possess precise and tunable structures characterized by their unique properties, yet a single component often underperforms in practical applications. In this work, a series of stable and highly effective antibacterial gels were prepared by incorporating fluoropolymer (perfluoro-2, 5-dimethyl-3, 6-dioxactyl glycol acrylate-co-acrylic acid, FAA) into aqueous solutions of (NH 4 ) 6 [Ag 6 (mna) 6 ] (Ag 6 -NCs). It can be quickly gelated within a few seconds to achieve the rapid transformation of one-dimensional into three-dimensional structures. These gels are formed through the layering of nanowires, and their mechanical properties can be tailored by adjusting the FAA concentration. The assembly process of Ag 6 -NCs/FAA hydrogels was investigated by comparing it with various poly carboxylic acids, neutralized FAA, and aqueous AgNO 3 solutions under identical experimental conditions. This assembly results from various interactions, including hydrophobic interactions, van der Waals forces and hydrogen bonds. Furthermore, the hydrogel system demonstrated improved antibacterial activity due to the presence of Ag ions and fluorine atoms. The functional composite of materials, achieved through heterogeneous assembly, promoted the design of metal NC materials and furthered the development of macro manufacturing technology.
研究领域:
材料科学
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生物学
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化学工程
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DOI
高影响因子
ACS Catalysis
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2025
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IF 13.1
Shengpeng Mo,Shuangde Li,Jiangjing Zhou,Xin Zhao,Huimin Zhao,Xiaobin Zhou,Yinming Fan,Zongqiang Zhu,Bing Li,Qinglin Xie,Wenzhe Si,Yunfa Chen,Daiqi Ye,Junhua Li
A concentrated solar reaction device has been designed for the solar-driven photothermal CO2 reverse water–gas shift reaction, in which solar-to-chemical conversion efficiency would be up to 26% via a concentrated solar panel. Meanwhile, a special photothermal Ni–C–In catalyst (Ni/C–In2O3) with interstitial C, the In3Ni2 intermetallic compound, and disordered Ni clusters has been synthesized. As a result, the SO2-tolerant Ni/C–In2O3 catalyst exhibits an outstanding solar-driven photothermal catalytic performance (near thermodynamic limitation) with 100% CO selectivity and a 20.96 mmol gcat–1 h–1 CO production rate for solar-driven CO2 hydrogenation under concentrated solar irradiation (around 1521.9 mW/cm2) even sunlight without external heating. The incorporation of interstitial C and exposed Ni clusters in the Ni–C–In intermetallic catalyst could strengthen intensive solar light absorption. Moreover, quasi in situ XPS and DFT theoretical calculation results validate that asymmetric interaction between interstitial C and the Ni-cluster not only effectually regulates the electronic structure of the Ni–C–In intermetallic catalyst but also greatly optimizes the activation of H2 and CO2 molecules and the energy barriers of key reaction dynamics (HCOO* formation and dehydrogenation) in the RWGS reaction. Accordingly, this study provides a promising strategy for the electronic structure modification of photothermal functional catalysts with C modification to boost CO2 hydrogenation, putting forward an important step toward practical solar-to-fuel production with concentrated natural sunlight.
研究领域:
材料科学
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催化化学
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能源科学
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DOI
高影响因子
ACS Sensors
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2024
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IF 8.2
Rongrong Huang,Peipei Wan,Shengjie Hu,Chenyang Zhang,Wenjun Miao
MicroRNAs (miRNAs) in dermal interstitial fluid (ISF) have recently been recognized as clinically promising biomarkers for the diagnosis and prognosis of cancer. However, the detection poses significant challenges, primarily due to the low abundance of miRNAs and the limitations of current sampling techniques. To address this issue, we develop novel porous microneedles (PMNs) array-based sensor composed of poly(vinyl alcohol) porous hydrogel and DNA-templated silver nanoclusters (AgNCs) to facilitate the enrichment and highly sensitive detection of ISF miRNA. Leveraging the capillary action facilitated by its unique porous structure and the swelling properties of the hydrogel, the PMNs array can efficiently extract 2.7 ± 0.3 mg of ISF within 5 min. Additionally, the interconnected pores within the PMNs array contribute to an increased specific surface area, thereby offering a convenient platform for the decoration of DNA-templated AgNCs. The immobilized large amount of AgNCs effectively capture the target miRNA from the extracted ISF, resulting in miRNA-induced fluorescence quenching of AgNCs. Subsequently, the introduction of the duplex-specific nuclease leads to the cleavage of DNA in DNA-RNA heteroduplexes, which release miRNA to interact with other AgNCs. This process of target recycling triggers a further reduction in fluorescence intensity, thereby enabling sensitive detection of the low-abundant miRNA down to 1.6 pM. Both in vitro and in vivo experiments validate the efficacy of the AgNCs immobilized PMNs array for the detection of miRNA biomarkers in ISF within minutes. These results indicate that the proposed PMNs array-based sensor holds great potential for the development of noninvasive personalized diagnostic strategies.
研究领域:
生物医学工程
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分子诊断
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纳米技术
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产品关联
DOI
PubMed
高影响因子
ANALYTICA CHIMICA ACTA
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2024
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IF 5.7
Lingjun Cheng,Yuanyuan Yang,Shaobin Lin,Canping Su,Mingming You,Yating Liu,Qingfei He,Jiaming Chen,Zhenyu Lin,Guolin Hong
Background Gold nanoclusters (AuNCs) obtained by electroreduction have excellent electrochemiluminescence (ECL) properties, and its ECL intensity is regulated by the valence state. In addition, their ECL signals can be rapidly quenched by reactive oxygen species (ROS). Based on this observation, a sensitive ROS biosensor was designed based on valence regulation of AuNCs. Excessive ROS in seminal plasma can lead to male infertility, and the short half-life and instability of ROS pose a challenge for their detection. Since valence regulation can be done quickly and is very sensitive, this ECL biosensor holds promise to address this issue. Results The ECL mechanism of AuNCs and the quenching mechanism of AuNCs by ROS were explored, mainly because ROS change the valence state of AuNCs. The ECL signals of the biosensor have a linear relationship with logarithm of the target concentration in the range of 1.0 × 10 −8 to 1.0 × 10 −3 M and 1.0 × 10 −3 to 1.0 × 10 −1 M, with a detection limit of 0.75 × 10 −10 M (S/N = 3). The biosensor enables rapid one-step detection of ROS and has the advantage of being stable and reusable. More notably, the results of 57 real samples showed that the biosensor can be used to accurately assess the concentration of seminal plasma ROS, guiding the monitoring of sperm quality and the diagnosis of male infertility. Significance Compared with the traditional strategy of applying AuNCs only as a luminescent body, this strategy of regulating the valence state of AuNCs to achieve sensitive and rapid detection broadens the application of AuNCs in the field of analysis. Compared with other ROS detection strategies, the one-step immediate detection method effectively avoids the inaccuracy caused by the short half-life and natural dissipation of ROS, and is expected to improve the accuracy and efficiency of clinical diagnosis.
研究领域:
分析化学
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生殖医学
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产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Luo Nan,Lu Bing-Qiang,Deng Yu-Wei,Zeng Hua,Zhang Yu,Zhan Jing-Yu,Xu Xiao-Chen,Cao Gui-Zhi,Wen Jin,Zhang Zhiyuan,Feng Xi-Ping,Jiang Xinquan,Chen Feng,Chen Xi
Remineralization is a common strategy for the repair of early demineralized tooth enamels, but the harsh dynamic oral environment often hampers its efficacy. Rapid remineralization is expected to address this challenge, however, the stabilizers of remineralization materials often resist their transformation required for repair. Here, by dissolving the ions of calcium and phosphate in glycerol-dominant solvents, we obtain the calcium phosphate clusters (1–2 nm), which are stabilized by glycerol (with high viscosity and affinity to clusters), but can perform a fast enamel repair via the water-triggered transformation in both static and dynamic environments. Upon the in vitro and in vivo (female Sprague-Dawley rats) studies, the clusters swiftly enter the nano-/micro-sized enamel defect sites, then form a compact hydroxyapatite repair layer within a short time (30 min, much faster than the conventional materials), and significantly recovers mechanical properties. This material is promising for large-scale preparation and applications in dental remineralization.
研究领域:
牙医学
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材料科学
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生物医学工程
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产品关联
DOI
PubMed
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
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2024
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IF 3.9
Jinglin Shen,Fengjie Zhou,You Yu,Ensheng Zhang,Wei Qi,Yongjie Zhang
Graphical The Gold nanoclusters (DPT-AuNCs) could self-assembles into two distinct aggregation structures in MeOH/water mixed solvent, exhibiting pathway complexity with different photoluminescent property. DPT-AuNCs firstly assembles into non-luminescent nanofibers (kinetically controlled), which further transforms into strongly luminescent microflowers (thermodynamically controlled). Modulating the assembly pathway is an indispensable strategy for optimizing the performance of optical materials. However, implementing this strategy is nontrivial for metal nanocluster building blocks, due to the limited functional modification of nanoclusters and complexity of their emission mechanism. In this report, we demonstrate that a gold nanocluster modified by 4,6-diamino-2-pyrimidinethiol (DPT-AuNCs) self-assembles into two distinct aggregation structures in methanol (MeOH)/water mixed solvent, thus exhibiting pathway complexity. Kinetic studies show that DPT-AuNCs firstly assembles into non-luminescent nanofibers (kinetically controlled), which further transforms into strongly luminescent microflowers (thermodynamically controlled). In-depth analysis of the assembly mechanism reveals that the transformation of aggregation structures involves the disassembly of nanofibers and a subsequent nucleation-growth process. Temperature-dependent photoluminescence (PL) spectroscopy and infrared (IR) measurements reveal that inter-cluster hydrogen bonding bridged by solvent molecules and C−H⋅⋅⋅π interaction are the key factors for emission enhancement. The photoluminescent property of DPT-AuNCs can be controlled by varying the cosolvent in water, enabling DPT-AuNCs to distinguish different kind of alcohols, particularly the isomerism n-propanol (NPA) and isopropanol (IPA). Additionally, the addition of seeds effectively regulate the assembly kinetics of DPT-AuNCs. This study advances our understanding of assembly pathways and improves the luminescent performance of nanoclusters (NCs).
研究领域:
材料科学
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光学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）