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DALTON TRANSACTIONS · 2014 ·Vol. 43 ·期 26 ·10057-10063 · IF 4.097

Fluorescent detection of TNT and 4-nitrophenol by BSA Au nanoclusters

Xin Yang,Junhai Wang,Dongyue Su,Qingdong Xia,Fang Chai,Chungang Wang,Fengyu Qu

Rapid and sensitive detection of 2,4,6-trinitrotoluene (TNT) and 4-nitrophenol (4-NP) has attracted considerable attention due to their wide applications as nitroaromatic explosive materials. A novel fluorescence method for TNT and 4-NP based on bovine serum albumin functionalized fluorescent gold nanoclusters (BSA Au-NCs) has been developed. The detection probe BSA Au-NCs can be used as a fluorescent probe for the sensitive and selective detection of TNT and 4-NP simultaneously. A good linearity of fluorescence detection using BSA Au-NCs as a fluorescent probe was observed for TNT and 4-NP concentrations in the range of 10−8–5 × 10−5 M and 10−9–5 × 10−5 M, with a detection limit of 10 nM and 1 nM, respectively. The high specificity of TNT and 4-NP with BSA Au-NCs interactions provided excellent selectivity towards detecting TNT and 4-NP over other relevant nitroaromatic compounds. This system can be applied to test strips to detect TNT and 4-NP with high sensitivity and selectivity. The vapour of TNT and 4-NP can be detected using BSA Au-NCs test paper within 1 min with a detection limit of 10 pM and 1 pM.

研究领域: 分析化学 · 环境科学 · 材料科学
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JOURNAL OF CATALYSIS · 2022 · IF 8.047

CuOx clusters decorated TiO2 for photocatalytic oxidation of nitrogen in air into nitric oxide under ambient conditions

Chaoxin Zhang,Yanmei Huang,Bohang Zhao,Yu Yu,Yifu Yu,Bin Zhang

Photocatalytic nitric oxide (NO) synthesis from air is an attractive way to supersede the conventional nitrogen fixation manufacturing technique accompanied by high energy requirements and greenhouse gas emission. The development of efficient photocatalysts for direct solar-driven N 2 oxidation to NO without external thermal assistance is highly challenged. Here, CuO x clusters decorated TiO 2 nanoflowers with various copper contents are constructed and used for solar-driven air reaction into NO under ambient conditions. When the copper content is 1 wt%, the sample shows the optimal performance with a yield rate of 35.0 mmol m −2  h −1 (7.7 μmol h −1 ) and an apparent quantum efficiency of 1.77% at 365 nm. A series of in situ and ex situ characterizations reveal Cu 2 O species and TiO 2 support form direct Z-scheme heterojunction over 1%Cu-TiO 2 . This heterojunction can promote the adsorption and activation of nitrogen and oxygen reactants, leading to the performance enhancement of NO photosynthesis from air. Also, we proposed a possible NO photosynthesis reaction pathway over 1%Cu-TiO 2 .

研究领域: 材料科学 · 环境科学 · 化学工程
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JOURNAL OF FLUORESCENCE · 2022 ·Vol. 32 ·期 5 ·1815-1823 · IF 2.525

A FRET Fluorescent Sensor for Ratiometric and Visual Detection of Sulfide Based on Carbon Dots and Silver Nanoclusters

Yang Jing,Huang Yan,Cui Hanyue,Li Li,Ding Yaping

In this work, the fluorescent sensor based on fluorescence resonance energy transfer (FRET) and electrostatic interaction (EI) was prepared for the ratiometric and visual detecting S 2– . The FRET fluorescent sensor consists of two fluorophores, with carbon dots (CDs) as energy donors and silver nanoclusters (Ag NCs) as acceptors. At 390 nm excitation, CDs and Ag NCs showed two well-separated peaks at 445 nm and 660 nm, separately. The existence of S 2– caused the red fluorescence at 660 nm to be quenched, whereas the blue fluorescence at 445 nm was restored, and the fluorescence color of the ratiometric sensor changed from pink to blue. It could be employed in ratiometric and visual detecting S 2– . The linear range of quantitative detection S 2– was 0.5–100 μM, and its detection limit was 0.35 μM. CDs-Ag NCs could be used for detecting S 2– in mineral water and tap water. The results showed that the FRET ratiometric fluorescent sensor exhibits good anti-interference and high selectivity for detecting S 2– in environmental water samples.

研究领域: 分析化学 · 环境科学
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS · 2023 ·Vol. 26 ·期 4 ·3263-3273 · IF 3.3

Fine-tuned local coordination environment of Pt–N in nanocarbons for efficient propane dehydrogenation

Ziwei Zhai,Bofeng Zhang,Yutong Wang,Guozhu Liu

Based on the disturbance of electronic density, nitrogen-doped nanocarbons show promising properties to anchor metal clusters. However, precisely regulating the coordination mode between N species and the active site remains challenging. Herein, we rationally designed three N types (graphitic N, pyridinic N and pyrrolic N) in nanocarbons to anchor Pt clusters for the benchmark propane dehydrogenation. The specific activity of the pyridinic-N-doped catalyst was 147.54 molC3H6 molPt−1 h−1 at 550 °C, which was 1.3 times higher than those of graphitic- and pyrrolic-N-doped catalysts. Unlike the regular tetrahedron Pt cluster in the graphitic-N catalyst or the distorted three-layered Pt cluster in the pyrrolic-N catalyst, the Pt cluster in the pyridinic-N catalyst was an inverted tetrahedron, which increased the contact degree without geometric repulsion towards C–H bond scission. The geometric parameters of detached H and C atoms in the methylene group for the pyridinic N catalyst was decreased to strengthen the C–H bond scission. After CH3CHCH3* adsorption, the Bader charge of the Pt active site also became highly positive, which tailored the d-band center closer to the Fermi level and provided more vacant orbitals for C–H bond breakage. Therefore, pyridinic N in nanocarbons is promising to anchor small-sized Pt for alkane dehydrogenation in terms of geometric and electronic effects.

CAS / MDL: 18497-13-7
研究领域: 催化化学 · 材料科学
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TALANTA · 2023 · IF 6.1

Simultaneous detection of patulin and ochratoxin A based on enhanced dual-color AuNCs modified aptamers in apple juice

Pengfei Ma,Hualin Guo,Ke Li,Yin Zhang,Huiqing Guo,Zhouping Wang

Patulin (PAT) and ochratoxin A (OTA) are the two main mycotoxins present in apples. Herein, a sensitive aptasensor for simultaneous detection of PAT and ochratoxin OTA was developed. Dual-color gold nanoclusters (AuNCs) with enhanced fluorescence properties were synthesized and employed as fluorescence amplifiers. Two separated fluorescence peaks at 650 nm and 530 nm were monitored simultaneously by employing single excitation (405 nm), corresponding to the aptamer probes of Cys@BSA-AuNCs-Apt PAT and Arg@ATT-AuNCs-Apt OTA , respectively. The fluorescent aptasensor demonstrated satisfying specificity, storage ability and accuracy. Under the optimal experimental conditions, the linear detection range for PAT and OTA was 0.10–50 ng/mL, with the limit of detection of 0.09 ng/mL and 0.06 ng/mL, respectively. Most importantly, practicability of the constructed aptasensor were confirmed by conducting the determination of PAT and OTA in apple juice sample, indicating the great potential of the aptasensor in practical detection applications.

研究领域: 食品科学 · 分析化学 · 生物技术
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Journal of Materials Chemistry A · 2020 ·Vol. 8 ·期 36 ·18755-18766 · IF 11.301

Pt decorated hierarchical Sb2WO6 microspheres as a surface functionalized photocatalyst for the visible-light-driven reduction of nitrobenzene to aniline

Yingzhang Shi,Huan Wang,Zhiwen Wang,Taikang Wu,Yujie Song,Binbin Guo,Ling Wu

Optimizing the structure of semiconductor materials and introducing functional metal clusters have emerged as an effective strategy to improve the photocatalytic performances of catalysts through the synergistic effect between metals and supports. In this work, Pt nanocluster decorated hierarchical Sb2WO6 microspheres which are assembled from ultra-thin nanosheets with only 3.3 nm thickness (Pt/SWO-NS) jointly achieve an efficient photocatalytic reduction of nitrobenzene to aniline and show 10 times higher activity than Pt decorated bulk Sb2WO6 (Pt/SWO-bulk). More importantly, the respective roles of SWO-NS and Pt nanoclusters are deeply studied. SWO-NS with a unique 2D structure, abundant unsaturated surface sites and good visible light response would be favorable for stabilizing Pt nanoclusters, adsorbing and activating more nitrobenzene molecules and providing abundant photo-generated electrons. Meanwhile, Pt nanoclusters serve as electron enrichment centers to decompose HCOONH4 to produce rich ·CO2− and active H for reducing the activated nitrobenzene molecules. In addition, on combining coordination chemistry, a possible synergistic mechanism for hierarchical Sb2WO6 microspheres and Pt nanoclusters is proposed to elucidate the efficient reduction of nitrobenzene to aniline. We believe that this work would provide an effective strategy to optimize catalytic performance by the design of applicable nanocomposites with synergistic effects.

研究领域: 材料科学 · 化学 · 纳米技术 · 催化 · 环境科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2022 · IF 24.319

Nitrogen doped carbon-distributed and nitrogen-stabilized ultrafine FeM (M = Pd, Pt, Au) nanoclusters for doxorubicin detoxification

Haoyang Fu,Meirong Li,Qianyu Xu,Guoliang Chen,Yunjie Zou,Weixian Zhang,Shuzhou Li,Lan Ling

Downsizing supported metal of Fe 0 -based materials in dealing with ever-growing pharmaceutical contamination issues are highly desired but still challenging. Herein, we develop a modular design protocol to synthesize a family of ultrafine alloy nanoclusters embedded in a nitrogen-enriched carbon framework (NEC@FeM (M=Pd, Pt, Au)). Engineering the fine structure of nitrogen-enriched carbon and interfacial interaction with bimetallic nanoclusters largely suppresses bimetallic overgrowth, eventually producing supported ultrafine (< 4 nm), highly dispersed, well-alloyed nanoclusters. The alloying Fe 0 with M for ultrafine nanoclusters optimize the electron flow, chemical stability, and catalytic property, resulting in the obtained NEC@FeM exhibiting excellent doxorubicin (DOX) degradation performance. Density functional theory calculation combined with experimental results attribute the outstanding DOX degradation ability of NEC@FePd originally to the synergistic effect of enhanced DOX affinity and efficient electrons transfer from Fe to DOX. This work provides a paradigm for the design of ultrafine Fe 0 -based nanocluster with application in pollution control.

CAS / MDL: 527-31-1
研究领域: 材料科学 · 环境科学 · 纳米技术 · 药物化学
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SENSORS AND ACTUATORS B-CHEMICAL · 2018 · IF 5.667

Multifunctional fluorescent sensors for independent detection of multiple metal ions based on Ag nanoclusters

Na Xiao,Jiang Xue Dong,Shi Gang Liu,Na Li,Yu Zhu Fan,Yan Jun Ju,Nian Bing Li,Hong Qun Luo

Selective and sensitive detection of multiple metal ions is significant for biological researches and environmental monitoring, because the abnormal metal ions levels have potential damage to the human body and environment. In this study, a fluorescent sensing platform based on Ag nanoclusters has been established for independent detection of Hg 2+ , Cu 2+ , and Fe 3+ ions in a solution. The interference of the fluorescence induced by coexistent metal ions was removed by altering buffers with different pH and using different masking agents. Moreover, the detection mechanism is discussed in detail, which provides a valuable reference for the detection of heavy metal ions with metal nanomaterials. This sensor exhibits a high selectivity and sensitivity, and the linear ranges for Hg 2+ , Cu 2+ , and Fe 3+ detection are 0.05-9, 0.05-18, and 0.1–18 μM with the corresponding detection limits of 12, 27, and 50 nM, respectively. Furthermore, this method was successfully used for analyzing the three metal ions in environmental and biological samples.

研究领域: 分析化学 · 环境科学 · 生物传感
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Methods and Applications in Fluorescence · 2019 ·Vol. 7 ·期 3 ·034004 · IF 2.94

Turn-on fluorescence detection of cysteine with glutathione protected silver nanoclusters

Nan Cao,Huangmei Zhou,Hao Tan,Ruijuan Qi,Jinquan Chen,Sanjun Zhang,Jianhua Xu

In this work, we report a sensitive and selective turn-on fluorescence detection of cysteine with glutathione protected silver nanoclusters (GSH-Ag NCs). The glutathione stabilized silver nanoclusters were synthesized by the boiling water method. When excited at 380 nm, the GSH-Ag NCs exhibited a weak emission at about 680 nm, which could be enhanced by cysteine. The proposed method allows evaluation of cysteine in the range of 2–3000 μM with a detection limit of 0.51 μM. The recoveries were found to be 95.07%-101.38% when detecting cysteine contents in fetal bovine serum samples. In addition, we also discussed the possible mechanism for the fluorescence enhancement of GSH-Ag NCs by addition of cysteine. It might be the formation of cysteine and glutathione co-capped Ag NCs. This work reported a fluorimetric method for the assay of cysteine and provided a strategy for the synthesis of dual ligand-protected Ag nanoclusters.

研究领域: 分析化学 · 生物医学
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Nature Synthesis · 2023 ·Vol. 2 ·期 5 ·423-429 · IF 0

Carbon-free sandwich compounds based on arsenic and antimony with icosahedral metal cores

Yue Xu-Hui,Chen Wei-Xing,Yang Tao,Muñoz-Castro Alvaro,Frenking Gernot,Sun Zhong-Ming

Traditionally, a metallocene complex comprises a metal centre sandwiched between two aromatic organic ligands and such complexes have been extensively investigated. Carbon-free analogues of metallocene with homoleptic As 5 or Sb 5 ligands, however, have remained experimentally elusive, especially analogues of higher nuclearity. Here we report the synthesis and characterization of sandwich-type clusters [Pn@M 12 Pn 10 (Pn 5 ) 2 ] 4–/5– (Pn = As, Sb; M = Co, Fe), where the endohedral icosahedral cluster [Pn@M 12 ] can be regarded as a spherical-like three-dimensional coordination centre surrounded by a Pn 10 ring and two Pn 5 pentagonal caps. Quantum chemical calculations reveal that the [Pn@M 12 ] has orbitals that mimic 1S, 1P and 1D electronic shells, which can interact with the outer (Pn 5 ) 2 ring layer. These interactions occur because the frontier orbitals are dominated by the ( n  − 1) d block orbitals of the metal atoms. The π 1 -As 5 orbitals interact with 1S and part of the 1P shell of the central core, while the π 2 - and π 3 -As 5 orbitals interact with the symmetry-allowed part of the 1P and 1D shells. The characteristics of this orbital interaction are analogous to those of mononuclear metallocenes.

研究领域: 无机化学 · 材料科学 · 理论化学
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RSC Advances · 2021 ·Vol. 11 ·期 53 ·33202-33207 · IF 3.361

Fluorescent PEI@Pd nanoclusters: facile synthesis and application

Wen Wen,Zhongping Li,Xu Wang,Xiaoyan Du,Guangming Wen,Li Li

Metal nanoclusters (NCs) have recently emerged as a novel class of luminescent nanomaterials and held significant potential in analytical chemistry. In this work, novel polyethyleneimine stabilized palladium nanoclusters (PEI–Pd NCs) were synthesized by chemical reduction at 60 °C for 6 h, and used as a fluorescent nanosensor for the detection of oxytetracycline (OTC). The spectral characteristics, surface structure and morphology of the Pd NCs were studied. The selectivity and stability of the nanosensor were also investigated. The experimental results showed that the Pd NCs had good biocompatibility, stability and photobleaching resistance in aqueous solution. The fluorescence quenching effect showed a good linear relationship with the degree of fluorescence quenching of Pd NCs and OTC in the range of 25–440 nM, with a correlation coefficient of 0.99. The limit of detection (LOD) of the proposed nanosensor for OTC was calculated to be 22 nM. The mechanism of determination was thought to be an inner filter effect (IFE) between OTC and Pd NCs. Based on this, we have established a new nanosensing analysis method for detecting OTC.

研究领域: 分析化学 · 纳米材料科学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2024 · IF 8.1

Self-assembled formation of platinum single atoms and nanoclusters stabilized on MXene as an efficient catalyst for boosting electrocatalytic hydrogen evolution

Xin Sun,Jun Wang,Jing Yu,Yifu Jing,Jingyuan Liu,Manish Singh,Peter D. Lund,Muhammad Imran Asghar

Atomic isolated and dispersed single atom catalyst is ideal for high-performance industrial catalyst. However, the contribution from small amounts of nanoclusters coexisting with single atoms to the catalytic reaction activity is often neglected. In this work, a MXene-supported uniformly dispersed Pt single atoms and nanoclusters (Pt 1 +Pt n /MXene) were obtained by self-assembly through an impregnation method. The catalyst exhibits high electrochemical performance in the hydrogen evolution reaction with an overpotential of only 61.3 mV and a Tafel slope of 32.5 mV dec −1  at a current density of 10 mA cm −2 in an acidic environment. The XAFS analysis and further DFT calculation indicate that the synergistic effect between single atoms and nanoclusters can facilitate adsorption of H* and promote the HER reaction. This work provides an efficient method for integrating multiple active sites in noble metal catalysts.

研究领域: 材料科学 · 催化化学 · 能源科学
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