We introduce Plasmene- in analogy to graphene-as free-standing, one-particle-thick, superlattice sheets of nanoparticles ("meta-atoms") from the "plasmonic periodic table", which has implications in many important research disciplines. Here, we report on a general bottom-up self-assembly approach to fabricate giant plasmene nanosheets (i.e., plasmene with nanoscale thickness but with macroscopic lateral dimensions) as thin as ∼40 nm and as wide as ∼3 mm, corresponding to an aspect ratio of ∼75,000. In conjunction with top-down lithography, such robust giant nanosheets could be milled into one-dimensional nanoribbons and folded into three-dimensional origami. Both experimental and theoretical studies reveal that our giant plasmene nanosheets are analogues of graphene from the plasmonic nanoparticle family, simultaneously possessing unique structural features and plasmon propagation functionalities.
Because of their unique photoluminescence and magnetic properties, nanodiamonds (NDs) are promising for biomedical imaging and therapeutical applications. However, these biomedical applications will hardly be realized unless the potential hazards of NDs to humans and other biological systems are ascertained. Previous studies performed in our group and others have demonstrated the excellent biocompatibility of NDs in a variety of cell lines without noticeable cytotoxicity. In the present paper, we report the first genotoxicity study on NDs. Our results showed that incubation of embryonic stem cells with NDs led to slightly increased expression of DNA repair proteins, such as p53 and MOGG-1. Oxidized nanodiamonds (O-NDs) were demonstrated to cause more DNA damage than the pristine/raw NDs (R-NDs), showing the surface chemistry specific genotoxicity. However, the DNA damages caused by either the O-NDs or the R-NDs are much less severe than those caused by multiwalled carbon nanotubes (MWNTs) observed in our previous study. These findings should have important implications for future applications of NDs in biological applications.
Ultralow-density metal aerogel monoliths were successfully fabricated from copper nanowires. Their conductivity, mechanical strength and surface wetting properties were finely tunable.
We systematically investigated the size- and shape-dependent SERS activities of plasmonic core-shell nanoparticles towards detection of the pesticide thiram. Monodisperse Au@Ag nanocubes (NCs) and Au@Ag nanocuboids (NBs) were synthesized and their Ag shell thickness was precisely adjusted from ∼1 nm to ∼16 nm. All these nanoparticles were used as SERS substrates for thiram detection, and the Raman intensities with three different lasers (514 nm, 633 nm and 782 nm) were recorded and compared. Our results clearly show that: (1) the excitation wavelength discriminated particle shapes regardless of particle sizes, and the maximized Raman enhancement was observed when the excitation wavelength approaches the SERS peak (provided there is significant local electric field confinement on the plasmonic nanostructures at that wavelength); (2) at the optimized laser wavelength, the maximum Raman enhancement was achieved at a certain threshold of particle size (or silver coating thickness). By exciting particles at their optimized sizes with the corresponding optimized laser wavelengths, we achieved a detection limit of roughly around 100 pM and 80 pM for NCs and NBs, respectively.
The rational design of photocatalysts for efficient nitrogen (N 2 ) fixation at ambient conditions is important for revolutionizing ammonia production and quite challenging because the great difficulty lies in the adsorption and activation of the inert N 2 . Inspired by a biological molecule, chlorophyll, featuring a porphyrin structure as the photosensitizer and enzyme nitrogenase featuring an iron (Fe) atom as a favorable binding site for N 2 via π-backbonding, here we developed a porphyrin-based metal−organic framework (PMOF) with Fe as the active center as an artificial photocatalyst for N 2 reduction reaction (NRR) under ambient conditions. The PMOF features aluminum (Al) as metal node imparting high stability and Fe incorporated and atomically dispersed by residing at each porphyrin ring promoting the adsorption and the activation of N 2 , termed Al-PMOF(Fe). Compared with the pristine Al-PMOF, Al-PMOF(Fe) exhibits a substantial enhancement in NH 3 yield (635 μg g −1 cat. ) and production rate (127 μg h −1 g −1 cat. ) of 82% and 50%, respectively, on par with the best-performing MOF-based NRR catalysts. Three cycles of photocatalytic NRR experimental results corroborate a stable photocatalytic activity of Al-PMOF(Fe). The combined experimental and theoretical results reveal that the Fe−N site in Al-PMOF(Fe) is the active photocatalytic center that can mitigate the difficulty of the rate-determining step in photocatalytic NRR. The possible reaction pathways of NRR on Al-PMOF(Fe) were established. Our study of porphyrin-based MOF for the photocatalytic NRR will provide insight into the rational design of catalysts for artificial photosynthesis.
Gold-coated horizontally aligned carbon nanotube (Au-HA-CNT) substrates were fabricated for surface-enhanced Raman spectroscopy (SERS). The Au-HA-CNT substrates, which are granular in nature, are easy-to-prepare with large SERS-active area. Enhancement factors (EFs) of ∼10(7) were achieved using the Au-HA-CNTs as substrates for rhodamine 6G (R6G) molecules. Maximum enhancement was found when the polarization direction (E-field) of the incident laser beam was parallel to the aligned direction of the HA-CNTs. Simulations using the finite-difference time-domain (FDTD) method were carried out for the granular Au-HA-CNT samples. Enhancement mechanisms and determination of EFs were analyzed. Biological samples, including (13)C- and deuterium (D)-labeled fatty acids and Coccomyxa sp. c-169 microalgae cells, were also measured using this SERS substrate. The limits of detection (LODs) of D- and (13)C-labeled fatty acids on the SERS substrate were measured to be around 10 nM and 20 nM, respectively. Significantly enhanced Raman signals from the microalgae cells were acquired using the SERS substrate.
We report an efficient electrocatalyst utilizing non‐noble metals consisting of Cu and Sn supported on nitrogen‐doped graphene (NG) for reduction of CO2 over a wide potential range. The CuSn alloy nanoparticles (NPs) on NG were prepared through a hydrothermal method followed by pyrolysis under nitrogen atmosphere to achieve a uniform dispersion of the alloy NPs. The CuSn NP (Cu/Sn ratio of 0.175) decorated NG catalyst performed electrocatalytic reduction of CO2 into C1 products at a Faradaic efficiency (FE) of nearly 93 % at an overpotential of −1.0 V vs. RHE, considerably higher than that of the Cu and Sn counterparts, i. e., 32 % and 58 %, respectively. The enhanced catalytic activity could be attributed to the collaboration between the CuSn alloy and Sn metal. The first‐principles density functional theory (DFT) simulation results indicate that the CuSn bimetal alloy nanoparticles enable more H atoms to participate in the electrocatalytic reduction of CO2 and exhibit an improved CO2 capture performance. In addition, the CuSn alloy having a lower barrier than that of Sn metal can accelerate the CO2 reduction process. This study presents the strategy that utilizes low‐cost non‐noble metals as highly efficient electrocatalysts for aqueous reduction of CO2.
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