Janus nanoparticles capped with a hydrophobic and hydrophilic hemisphere of mercapto ligands can self‐assemble into hollow, emulsion‐like nanostructures in controlled media. As the nanoparticle emulsions are chiroptically active exhibiting a plasmonic circular dichroism absorption in the visible range, they can be exploited as a unique chiral nanoreactor by selective encapsulation of
The highly sensitive optical detection of oxygen including dissolved oxygen (DO) is of great interest in various applications. We devised a novel room‐temperature‐phosphorescence (RTP)‐based oxygen detection platform by constructing core–shell nanoparticles with water‐soluble polymethyloxazoline shells and oxygen‐permeable polystyrene cores crosslinked with metal‐free purely organic phosphors. The resulting nanoparticles show a very high sensitivity for DO with a limit of detection (LOD) of 60 n
- PAR ID:
- 10047038
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Angewandte Chemie
- Volume:
- 129
- Issue:
- 51
- ISSN:
- 0044-8249
- Page Range / eLocation ID:
- p. 16425-16429
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
more » « less
Abstract d ‐enantiomer into the water phase of the water‐in‐oil emulsions for directional functionalization of the nanoparticles and endow the resulting nanoparticles with select chirality. This is demonstrated in the present study with gold Janus nanoparticles functionalized with (hydrophobic) hexanethiolates and (hydrophilic) 3‐mercapto‐1,2‐propandiol, andd ,l ‐cysteine is used as the molecular probe. Experimental results demonstrate thatd ‐cysteine is the preferred enantiomers entrapped within the nanoparticle emulsions, where the ensuing ligand exchange reaction is initially confined to the hydrophilic face of the Janus nanoparticles. This suggests that with a deliberate control of the reaction time, chiral Janus nanoparticles can be readily prepared by ligand exchange reactions even with a racemic mixture of ligands. -
more » « less
Abstract Sensing of viral antigens has become a critical tool in combating infectious diseases. Current sensing techniques have a tradeoff between sensitivity and time of detection; with 10–30 min of detection time at a relatively low sensitivity and 6–12 h of detection at a high (picomolar) sensitivity. In this research, uniquely nanoengineered interfaces are demonstrated on 3D electrodes that enable the detection of spike antigens of SARS‐CoV‐2 and their variants in seconds at femtomolar concentrations with excellent specificity, thus, overcoming this tradeoff. The 3D electrodes, manufactured using a high‐resolution aerosol jet 3D nanoprinter, consist of a microelectrode array of sintered gold nanoparticles coated with graphene and antibodies specific to severe acute respiratory syndrome coronavirus‐2 (SARS‐CoV‐2) spike antigens. An impedance‐based sensing modality is employed to sense several pseudoviruses of SARS‐CoV‐2 variants of concern (VOCs). This device is sensitive to most of the pseudoviruses of SARS‐CoV‐2 VOCs. A high sensitivity of 100 f
m , along with a low limit‐of‐detection of 9.2 fm within a test range of 0.1–1000 pm , and a detection time of 43 s are shown. This work illustrates that effective nano‐bioengineering of interfaces can be used to create an ultrafast and ultrasensitive healthcare diagnostic tool for combating emerging infections. -
more » « less
Abstract Transition metal sulfides with a multi‐elemental nature represent a class of promising catalysts for oxygen evolution reaction (OER) owing to their good catalytic activity. However, their synthesis remains a challenge due to the thermodynamic immiscibility of the constituent multimetallic elements in a sulfide structure. Herein, for the first time the synthesis of high‐entropy metal sulfide (HEMS, i.e., (CrMnFeCoNi)S
x ) solid solution nanoparticles is reported. Computational and X‐ray photoelectron spectroscopy analysis suggest that the (CrMnFeCoNi)Sx exhibits a synergistic effect among metal atoms that leads to desired electronic states to enhance OER activity. The (CrMnFeCoNi)Sx nanoparticles show one of the best activities (low overpotential 295 mV at 100 mA cm−2in 1m KOH solution) and good durability (only slight polarization after 10 h by chronopotentiometry) compared with their unary, binary, ternary, and quaternary sulfide counterparts. This work opens up a new synthesis paradigm for high‐entropy compound nanoparticles for highly efficient electrocatalysis applications. -
more » « less
Abstract Using deep near-infrared Keck/MOSFIRE observations, we analyze the rest-optical spectra of eight star-forming galaxies in the COSMOS and GOODS-N fields. We reach integration times of ∼10 hr in the deepest bands, pushing the limits on current ground-based observational capabilities. The targets fall into two redshift bins, of five galaxies at
z ∼ 1.7 and three galaxies atz ∼ 2.5, and were selected as likely to yield significant auroral-line detections. Even with long integration times, detection of the auroral lines remains challenging. We stack the spectra together into subsets based on redshift, improving the signal-to-noise ratio on the [Oiii ]λ 4364 auroral emission line and, in turn, enabling a direct measurement of the oxygen abundance for each stack. We compare these measurements to commonly employed strong-line ratios alongside measurements from the literature. We find that the stacks fall within the distribution ofz > 1 literature measurements, but a larger sample size is needed to robustly constrain the relationships between strong-line ratios and oxygen abundance at high redshift. We additionally report detections of [Oi ]λ 6302 for nine individual galaxies and composite spectra of 21 targets in the MOSFIRE pointings. We plot their line ratios on the [Oiii ]λ 5008/Hβ versus [Oi ]λ 6302/Hα diagnostic diagram, comparing our targets to local galaxies and Hii regions. We find that the [Oi ]/Hα ratios in our sample of galaxies are consistent with being produced in gas ionized byα -enhanced massive stars, as has been previously inferred for rapidly forming galaxies at early cosmic times. -
more » « less
Abstract Metal–organic frameworks (MOFs) and MOF‐derived nanostructures are recently emerging as promising catalysts for electrocatalysis applications. Herein, 2D MOFs nanosheets decorated with Fe‐MOF nanoparticles are synthesized and evaluated as the catalysts for water oxidation catalysis in alkaline medium. A dramatic enhancement of the catalytic activity is demonstrated by introduction of electrochemically inert Fe‐MOF nanoparticles onto active 2D MOFs nanosheets. In the case of active Ni‐MOF nanosheets (Ni‐MOF@Fe‐MOF), the overpotential is 265 mV to reach a current density of 10 mA cm−2in 1
m KOH, which is lowered by ≈100 mV after hybridization due to the 2D nanosheet morphology and the synergistic effect between Ni active centers and Fe species. Similar performance improvement is also successfully demonstrated in the active NiCo‐MOF nanosheets. More importantly, the real catalytic active species in the hybrid Ni‐MOF@Fe‐MOF catalyst are unraveled. It is found that, NiO nanograins (≈5 nm) are formed in situ during oxygen evolution reaction (OER) process and act as OER active centers as well as building blocks of the porous nanosheet catalysts. These findings provide new insights into understanding MOF‐based catalysts for water oxidation catalysis, and also shed light on designing highly efficient MOF‐derived nanostructures for electrocatalysis.
