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Applied Nanoscience · 2020 ·Vol. 11 ·期 1 ·257-266 · IF 2.88

Rapid separation of nanodiamond particles by viscosity gradient centrifugation

Qu Jiaying,Mukerabigwi Jean Felix,Yang Nianshun,Huang Xueying,Sun Yuyang,Cai Xiaojuan,Cao Yu

The nanodiamond (ND) particles have several potential applications including tribology, drug delivery, bioimaging, etc. However, the severe colloidal aggregation tendency of ND particles strictly limits its exploitation. Moreover, due to NDs rich surface chemistry and relatively small size, it is still difficult to separate these large ND particles using conventional separation methods. Herein, we develop an efficient and straightforward strategy to separate the colloidal aminated nanodiamonds (ND-NH 2 ) into small size nanoparticles by viscosity gradient centrifugation method in a polyvinylpyrrolidone (PVP) aqueous solution. Prior to and after separation, the pristine ND and ND-NH 2 particles size and morphology were characterized by DLS (dynamic light scattering analyzer) and TEM (transmission electron microscopic), which show that ND particles with narrow size distribution and uniform morphology can be easily separated by the viscosity gradient of PVP aqueous solution. This simple, rapid and effective separation method could be extended to separate other functionalized NDs with different sizes.

CAS / MDL: 25249-54-1 9003-39-8
研究领域: 材料科学 · 纳米技术 · 化学工程
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ANALYST · 2019 ·Vol. 144 ·期 9 ·3072-3079 · IF 4.019

Nanogold hybrid silica gel and its 1-octadecanethiol self-assembled modified composite as a stationary phase for liquid chromatography

Yuhuan Wang,Ruyan Wang,Lei Wang,Licheng Wang,Yong Guo,Xiaojing Liang,Shuai Wang

Au nanoparticle-hybridized silica (Au@sil) spheres were synthesized in one step as a liquid chromatographic stationary phase for the first time. The hybridized stationary phase showed good separation performances in reversed-phase liquid chromatography (RPLC) and hydrophilic interaction liquid chromatography even without bonding with any organic groups. Compared with the bare silica stationary phase, the Au@sil stationary phase showed better separation performance under the same conditions in RPLC and HILIC modes. The effects of acetonitrile content, buffer concentration, and the pH of the mobile phase on analyte retention were further investigated. The results showed that the Au@sil stationary phase had a complex retention mechanism of electrostatic and partitioning interactions. By comparing Au solution (solAu) with different proportion volumes in silica sol, the optimum hybridized stationary phase was found to comprise 33 vol% solAu. Au@sil was further modified with 1-octadecanethiol by self-assembly and used to separate alkylbenzenes and polycyclic aromatic hydrocarbons by RPLC. The separation efficiency of the 1-octadecanethiol self-assembled modified Au@sil (C18-Au@sil) column was much better than that of Au@sil. Overall, the successful hybridization of Au nanoparticles provided a new method to prepare a stationary phase in a simple and environmentally friendly way.

研究领域: 分析化学 · 材料科学
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Efficient Ambient Electrocatalytic Ammonia Synthesis by Nanogold Triggered via Boron Clusters Combined with Carbon Nanotubes

Xue Zhao,Ziqiong Yang,Artem V. Kuklin,Glib V. Baryshnikov,Hans Ågren,Xiaohai Zhou,Haibo Zhang

Currently, the development of stable electrochemical nitrogen reduction reaction (ENRR) catalysts with high N2 conversion activity and low cost to instead of the traditional Haber-Bosch ammonia production process of high-energy consumption remains a great challenge for researchers. Here, we have immobilized reductive closo-[B12H11]− boron clusters on a carbon nanotubes (CNT) surface and have successfully prepared a novel Au-CNT catalyst with extraordinary ENRR activity after adding HAuCl4 to the CNT-[B12H11]− precursor. The excellent properties of ammonia yield (57.7 μg h–1 cm–2) and Faradaic efficiency (11.97%) make it possible to achieve using this Au-CNT catalyst in large-scale industrial production of ammonia. Furthermore, its outstanding cyclic stability and long-term tolerability performance make it one of the most cost-effective catalysts to date. Here, by means of density functional theory we disclose the associative mechanism of N2-to-NH3 conversion on the Au(111) surface, providing visual theoretical support for the experimental results.

研究领域: 材料科学 · 化学工程 · 理论化学
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ANALYST · 2021 ·Vol. 146 ·期 13 ·4384-4390 · IF 4.616

Determination of selenium and copper in water and food by hierarchical dendritic nano-gold modified glassy carbon electrodes

Haofan Wang,Yin Guo,Hongcheng Pan

The sensitive determination of selenium and copper is of importance for environmental monitoring and food safety. A stripping voltammetric determination of selenium and copper in water and selenium-rich foods was developed using hierarchical dendritic gold nanostructure (AuHD) modified glassy carbon electrodes (GCE). The AuHD thin films were electrodeposited potentiostatically onto the GCE from a solution containing 25 mM HAuCl4 and 0.1 M Na2SO4 at −0.6 V for 20 min. Scanning electron microscopy (SEM) and energy-dispersive X-ray spectroscopy (EDX) studies showed that the electrodeposited gold thin film shows a nanoforest-like morphology with a thickness of about 30–40 μm and a hierarchical dendritic structure with primary-, secondary-, and higher-order branches. Se(IV) and Cu(II) in a 0.1 M H2SO4 solution were determined by square-wave anodic stripping voltammetry using the AuHDs/GCE as the working electrode. Prior to anodic stripping, Se(IV) and Cu(II) were accumulated onto the working electrode surface at −0.2 V for 300 s. The stripping peak currents of Se(IV) at 0.81 V and Cu(II) at 0.31 V were positively correlated with the concentrations of Se(IV) and Cu(II) in a range of 50–700 nM. The limits of detection (3σ) for Se(IV) and Cu(II) were 1.4 nM and 3.7 nM, respectively. The accuracy of the method was verified by analysing certified water standard reference materials, and the results showed that the method has good accuracy and high precision. The method was used to determine selenium and copper in tap water, selenium-rich rice and selenium-rich eggs. The results were compared with those obtained by using inductively coupled plasma-mass spectrometry (ICP-MS) and found to be consistent with those of ICP-MS. The proposed method had the advantages of simplicity, rapidity, good reproducibility, and high sensitivity and it can be used for the analysis of real samples.

研究领域: 环境科学 · 食品科学 · 分析化学
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DIAMOND AND RELATED MATERIALS · 2024 · IF 4.3

Microcontact printing fabrication of diamond MEMS cantilevers on silicon substrate

Biao Yan,Zhixin Zhao,Xiaojuan Wu,Haoran Li,Duo Liu

Diamond shows great potentials as an ultimate material candidate for application in microelectromechanical systems (MEMS). In this work, we report microcontact printing (μCP) transfer as a facile technique to fabricate diamond MEMS cantilever arrays. We started from the Deryaguin–Landau–Verwey–Overbeek (DLVO) principles and formulated a colloidal “ink” that contains nanodiamonds (NDs) seeds well dispersed in polymethyl methacrylate/acetone. The NDs seeds were then transfer printed onto a silicon (100) substrate by using a flexible polydimethylsiloxane (PDMS) stamp with predefined pattern. The densely packed NDs pattern (∼10 9  cm −2 ) enables facile and selected-area growth of diamond with microwave plasma chemical vapor deposition (MPCVD) technique. A diamond film with minimal graphite contaminants and low residual stresses was obtained after growth at 1118 K for 3 h. The diamond cantilevers were released from the substrate by wet chemical etching using KOH (40 % wt.) and isopropyl alcohol (10 % vol.). An examination of the vibrational kinetics indicates that the diamond film has a high Young's modulus (∼795 GPa) and the cantilevers exhibit consistently distributed resonant frequencies and high quality factors in ambient air. The method opens the door for large-scale, cost-effective production of uniform diamond MEMS devices for sensor and quantum applications.

研究领域: 材料科学 · 微机电系统 · 表面化学
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Catalysts · 2020 ·Vol. 10 ·期 9 ·1037 · IF 3.52

Facile Fabrication of Rhodium/Nanodiamond Hybrid as Advanced Catalyst toward Hydrogen Production from Ammonia–Borane

Zhaoyu Wen,Jie Wu,Guangyin Fan

Hydrogen generation through ammonia–borane (AB) hydrolysis has been regarded as one of the most promising pathways to tap renewable green energy. The design and synthesis of highly effective catalysts toward hydrogen production from aqueous AB is of paramount significance. Here, the facile synthesis of Rh nanoparticles (NPs) immobilized on nanodiamond (nano-DA) and concomitant AB hydrolysis to produce hydrogen was successfully achieved. The in situ generated Rh/nano-DA exhibited excellent catalytic activity toward AB hydrolysis, with a high turnover frequency (TOF) value of 729.4 min−1at 25 °C and a low activation energy of 25.6 kJ mol−1. Moreover, the catalyst could be reused four times. The unique properties of DA with abundant oxygen-containing groups enable the homogeneous distribution of small and surface-clean Rh NPs on the nano-DA surface, which can supply abundant accessible active sites for hydrogen evolution from AB hydrolysis. This study demonstrated that nano-DA can be applied as an ideal matrix to deposit efficient Rh nanocatalyst toward hydrogen evolution reaction.Keywords:nanodiamond;ammonia–borane;hydrogen evolution;rhodium nanoparticles

CAS / MDL: 64-17-5
研究领域: 材料科学 · 催化化学
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ACS Applied Materials & Interfaces · 2019 · IF 8.456

Ultra-Wear-Resistant MXene-Based Composite Coating via in Situ Formed Nanostructured Tribofilm

Xuan Yin,Jie Jin,Xinchun Chen,Andreas Rosenkranz,Jianbin Luo

Newly emerging two-dimensional (2D) materials of MXenes possess lots of merits, which provide potential solutions for the lubrication issues in harsh conditions. Here, preliminary efforts were devoted to developing an MXene-based 2D composite coating and its antiwear interfacial performance in ambient environments. Macroscale and atomic-scale characterizations were utilized to explore the lubrication behaviors of the composite coating to clarify the influence of the coating composition and tribo-test parameters in the establishment of ultra-wear-resistant sliding interfaces. The results highlighted a unique lubrication mechanism for the 2D MXene composite coating. They suggested that the MXene/nanodiamond coating exhibited almost no wear when rubbed against a polytetrafluoroethylene (PTFE) ball. A nanostructured tribofilm with unprecedented bonding features was in situ formed along the sliding interface. The ultra-wear resistance highly depended on the combined effects of shielding and self-lubrication of PTFE, layer shearing of MXenes, and self-rolling of nanodiamond. These discoveries clearly enrich the 2D material-based lubrication theories and offer technical guidance for designing and exploiting high-performance ultra-wear-resistant materials.

研究领域: 材料科学 · 摩擦学 · 表面工程
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Materials · 2024 ·Vol. 17 ·期 22 ·5593 · IF 3.1

Deposition of Diamond Coatings on Ultrathin Microdrills for PCB Board Drilling

Shuangqing Zhou,Stephan Handschuh-Wang,Tao Wang

The drilling of State-of-the-Art printed circuit boards (PCBs) often leads to shortened tool lifetime and low drilling accuracy due to improved strength of the PCB composites with nanofillers and higher thickness-to-hole diameter ratio. Diamond coatings have been employed to improve the tool lifetime and drilling accuracy, but the coated microdrills are brittle and suffer from coating delamination. To date, it is still difficult to deposit diamonds on ultrathin microdrills with diameters lower than 0.2 mm. To avoid tool failure, the pretreatment was optimized to afford sufficient fracture strength and enough removal of cobalt. Further, the adhesion of the diamond coating was improved by employing an interlayer comprising SiC/microcrystalline diamond, which mitigates stress accumulation at the interface. By these means, microdrills with diameters of 0.8 and 0.125 mm were coated with adherent diamonds. In this context, the composite coating with the diamond/SiC interlayer and a nanodiamond top layer featured enhanced adhesion compared to single nano- or microdiamond coatings on the WC-Co microdrills. The composite diamond-coated WC-Co microdrills featured improved wear resistance, resistance to delamination of the diamond coating, and improved performance for drilling PCBs compared to micro- and nanodiamond-coated microdrills without interlayer. In addition, a higher hole quality was achieved when the diamond-coated microdrills were used. These results signify that the composite/nanodiamond coating features the highest bonding strength and best drilling performance.

CAS / MDL: 25155-30-0 13943-58-3
研究领域: 材料科学 · 机械工程
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Journal of Materials Chemistry A · 2024 ·Vol. 12 ·期 16 ·9817-9829 · IF 10.7

SERS sensing chip based on Ti3C2/nano-Au@MA for ultrasensitive amine gas detection

Liwei Hou,Xinyue Xu,Xiaoli Wang,Li Wang,Fengchun Tian,Yi Xu

In this paper, we propose a composite nano-microstructure comprising Ti3C2 and nanogold as a surface-enhanced Raman spectroscopy (SERS)-active substrate for the highly sensitive sensing of amine gases. The adsorption performance of Ti3C2 was tested by a quartz crystal microbalance (QCM) sensor. Excellent adsorption ability of Ti3C2 was observed for aniline, phenylenediamine, and diethylamine, with adsorption amounts exceeding 2210, 1740, and 970 ng cm−2, respectively. The synergistic effect of the electromagnetic properties of Ti3C2 and nano-Au in the Ti3C2/nano-Au composite nanostructures was verified by finite-difference time-domain simulation. Partial chemical enhancement between Ti3C2 and aniline was verified by photocurrent tests. To achieve assay specificity, mercaptoacetaldehyde (MA) was adopted as a recognition probe. The Schiff base reaction between aldehyde groups and amino groups produces the –CN– bond, with the Raman characteristic peak at 1635 cm−1, enabling precise amine identification with the SERS chip. To obtain the Ti3C2/nano-Au@MA SERS sensing chip, nano Au was deposited on an indium tin oxide substrate using the chronoamperometric method, followed by nano-Au aldolization modification through Au-SH interactions and the spin-coating of a Ti3C2 film layer. Due to the high affinity of Ti3C2 for amine molecules and the low SERS background signal of MA and Ti3C2, the SERS spectra could be used for ultra-sensitive detection of amines. Three amine gases, i.e. aniline, p-phenylenediamine, and diethylamine, were detected quantitatively using the intensity ratiometric method on the functionalized Ti3C2/nano-Au@MA SERS sensor chip. The detection limits were 1, 1, and 20 parts per billion, respectively. By identifying the characteristic fingerprint peaks and comparing the relative intensity of the –CN– characteristic peak, quantitative analysis of the components of aniline and p-phenylenediamine mixed gas was accomplished. These findings demonstrate that the Ti3C2/nano-Au@MA SERS sensor chip offers a promising approach for the detection of amine gas molecules and holds potential for applications in environmental monitoring, disease diagnosis, and chemical analysis.

研究领域: 材料科学 · 分析化学 · 环境科学
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DALTON TRANSACTIONS · 2019 ·Vol. 48 ·期 22 ·7910-7917 · IF 4.052

A self-calibrated luminescent thermometer based on nanodiamond-Eu/Tb hybrid materials

Xue-Ying Wu,Qi Zhao,Dong-Xue Zhang,Ya-Chuan Liang,Kui-Kui Zhang,Qian Liu,Lin Dong,Chong-Xin Shan

Luminescent hybrid materials based on nanodiamonds (NDs) and rare earth ions have been successfully synthesized by covalently modifying NDs with pyromellitic acid (PMA) which is capable of coordinating to Eu3+ and Tb3+ ions. With NDs acting as a host matrix, the PMA and rare earth ions serve as an organic sensitizer and activator, respectively, yielding a highly bright hybrid composite. Interestingly, for the co-doped hybrid composites ND-PMA-Eu/Tb, the intensity ratio of the two emissions, 5D4 → 7F5 transition (Tb3+) to 5D0 → 7F2 transition (Eu3+), is linearly related to temperature in the range from 77 K to 277 K. Therefore, the hybrid could be developed as a self-calibrated ratiometric luminescent thermometer due to its temperature-dependent luminescence performance.

研究领域: 材料科学 · 光学
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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Synergy of nitrogen vacancies and nanodiamond decoration in g-C3N4 for boosting CO2 photoreduction

Xinran Li,Shuohan Li,Jian Xu,Lanxin Wang,Kaiwei Liang,Huihui Zhang,Xuelian Yu,Zhongwei Liu

Photoconversion of CO 2 into fuel is critical for realizing a net-zero emission future, but it remains an open challenge due to the unsatisfactory light absorption and photogenerated carriers’ separation efficiency of catalysts. In this work, upon in situ thermal polymerization method, the nanodiamond (ND) are homogeneously and solidly modified on the defective graphitic carbon nitride (g-C 3 N 4 ) surface. Under visible light irradiation, the ND/g-C 3 N 4 (NH) exhibits excellent CO 2 photocatalytic performance with a CO yield of 10.98 μmol/h (18.6 times higher than bulk g-C 3 N 4 ), predominant performance in the selectivity of CO and cyclic stability. The improved CO 2 photoreduction ability was sourced from the synergetic effect of nitrogen vacancies engineering and ND decoration, which also significantly improved visible light absorption capacity and facilitated electron transport pathways, and promoted the separation and transfer of charge carriers efficiently.

CAS / MDL: 108-78-1
研究领域: 材料科学 · 环境科学 · 化学工程
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ANALYTICAL CHEMISTRY · 2020 · IF 6.785

Linker-Eliminated Nano Metal–Organic Framework Fluorescent Probe for Highly Selective and Sensitive Phosphate Ratiometric Detection in Water and Body Fluids

Yu Ma,Yingqiu Zhang,Xiangyuan Li,Peng Yang,Jie-Yu Yue,Yu Jiang,Bo Tang

Phosphate is an important anion in both the aquatic environment and biological systems. The search for a selective and sensitive phosphate ratiometric fluorescent probe to quantify the phosphate level in water samples and body fluids is of great significance for the protection of the ecological environment and human health. Here, a porphyrin-based nano metal–organic framework (NMOF), PCN-224, was successfully exploited as a simple but highly sensitive and selective single-component ratiometric fluorescent probe with accurate composition and measurable structure for the quantitative determination of phosphate, based on the interesting double-emission fluorescence of the porphyrin ligand itself. Compared with other zirconium-based NMOF probes for phosphate, the reduced number of connections for ZrO clusters with the ligand in PCN-224 obtained by a linker-elimination strategy simultaneously provides more active recognition sites for phosphate, which effectively improves the sensitivity of the zirconium-based NMOF probes. The detection limit of the probe is only 54 nM. Additionally, the accuracy of the ratiometric detection based on this probe was further proved by the detection of phosphate in human serum and drinking water.

研究领域: 环境科学 · 分析化学 · 生物化学
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