Abstract:N-Heterocyclic carbenes (NHCs) are becoming increasingly popular ligand frameworks for nanocrystal surfaces; however, as of yet the nature of the NHC-nanocrystal interface remains unexplored across different material types. Here we report a facile synthetic route to NHC-stabilized metal and metal chalcogenide nanocrystals. It was observed that NHC-Ag nanocrystals are colloidally stable, but much less so than the corresponding NHC-AgE analogues. Comprehensive NMR studies suggest a dynamic NHC-nanocrystal interf… Show more
“…1 H NMR spectroscopy was performed on a Bruker Avance III 400 MHz instrument. Spectra were collected at 25 °C using a standard proton pulse (zg), 32 scans, and 30 s delay between scans to complete relaxation between pulses . NC/ligand samples were dried under vacuum, resuspended in 700 μL CDCl 3 , and transferred to J.…”
The marriage of colloidal semiconductor nanocrystals and functional organic molecules has brought unique opportunities in emerging photonic and optoelectronic applications. Traditional semiconductor nanocrystals have been widely demonstrated to initiate efficient triplet energy transfer at the nanocrystal−acene interface. Herein, we report that unlike conventional semiconductor nanocrystals, lead halide perovskite nanocrystals promote an efficient Dexter-like singlet energy transfer to surface-anchored pentacene molecules rather than triplet energy transfer. Subsequently, molecular pentacene triplets are efficiently generated via singlet fission on the nanocrystal surface. Our demonstrated strategy not only unveils the obscure energy dynamics between perovskite nanocrystal and acenes, but also brings important perspectives of utilizing singlet fission throughout the solar spectrum.
“…1 H NMR spectroscopy was performed on a Bruker Avance III 400 MHz instrument. Spectra were collected at 25 °C using a standard proton pulse (zg), 32 scans, and 30 s delay between scans to complete relaxation between pulses . NC/ligand samples were dried under vacuum, resuspended in 700 μL CDCl 3 , and transferred to J.…”
The marriage of colloidal semiconductor nanocrystals and functional organic molecules has brought unique opportunities in emerging photonic and optoelectronic applications. Traditional semiconductor nanocrystals have been widely demonstrated to initiate efficient triplet energy transfer at the nanocrystal−acene interface. Herein, we report that unlike conventional semiconductor nanocrystals, lead halide perovskite nanocrystals promote an efficient Dexter-like singlet energy transfer to surface-anchored pentacene molecules rather than triplet energy transfer. Subsequently, molecular pentacene triplets are efficiently generated via singlet fission on the nanocrystal surface. Our demonstrated strategy not only unveils the obscure energy dynamics between perovskite nanocrystal and acenes, but also brings important perspectives of utilizing singlet fission throughout the solar spectrum.
“…XPS was utilized to study the NHC-AuNPs, as it has already been proven to be a powerful tool in the characterization of NHC-coated AuNPs whereby the C 1s and N 1s signals are used to evidence the presence of the NHC ligand on AuNPs. 10,16,[19][20][21][22][23] In addition to the C 1s and N 1s signals, we also utilized information arising from the Au 4f peaks to investigate Au oxidation states.…”
NHC-AuNPs prepared via chlorido(1,3-dimethyl-N-Boc-O-methylhistidin-2-ylidene)gold(i), an NHC–Au(i) complex, affords AuNPs containing not just Au(0), but also Au(i).
“…Moreover, a spectroscopic investigation of the spatial orientation and coordination mode of NHC moieties on different metallic surfaces will provide useful insights to modulate the reactivity of the organic/inorganic interface towards CO 2 RR. [458][459][460][461][462]…”
An overview of the main strategies for the rational design of transition metal-based catalysts for the electrochemical conversion of CO2, ranging from molecular systems to single-atom and nanostructured catalysts.
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