Covalent organic frameworks (COFs)
represent a new class of porous
crystalline polymers with a diversity of applications. However, synthesis
of uniform spherical COFs poses a great challenge. Here, we present
size-controllable synthesis of uniform spherical COFs from nanometer
to micrometer scale by a facile approach at room temperature. The
as-prepared spherical COFs with different sizes exhibited ultrahigh
surface area, good crystallinity, and chemical/thermal stability.
Multifarious microscopic and spectroscopic techniques were performed
to understand the formation mechanism and influencing factors of the
spherical COFs. Moreover, the general applicability for room-temperature
synthesis of the spherical COFs was demonstrated by varying different
building blocks. Spherical COFs, because of the advantageous nature
of their surface area, hydrophobicity, and mesoporous microenvironment,
serve as an attractive restricted-access adsorption material for highly
selective and efficient enrichment of hydrophobic peptides and size
exclusion of macromolecular proteins simultaneously. On this basis,
the spherical COFs were successfully applied to the specific capture
of ultratrace C-peptide from human serum and urine samples. This research
provides a new strategy for room-temperature controllable synthesis
of uniform spherical COFs with different sizes and extends the application
of COFs as an attractive sample-enrichment probe for clinical analysis.
Three types of nitrogen‐doped hollow carbon spheres with different pore sized porous shells are prepared to investigate the performance of sulfur confinement. The reason that why no sulfur is observed in previous research is determined and it is successfully demonstrated that the sulfur/polysulfide will overflow the porous carbon during the lithiation process.
The poor understanding of HONO sources in the daytime highlights the importance of the heterogeneous photochemical reaction of NO2 with aerosol or soil surfaces. The conversion of NO2 to HONO on humic acid (HA) under simulated sunlight was investigated using a flow tube reactor at ambient pressure. The uptake coefficient (γ) of NO2 linearly increased with irradiation intensity and HA mass in the range of 0-2.0 μg/cm(2), while it decreased with the NO2 concentration. The HONO yield was found to be independent of irradiation intensity, HA mass, and NO2 concentration. The temperature (278-308 K) had little influence on both γ and HONO yield. Additionally, γ increased continuously with relative humidity (RH, 7-70%), and a maximum HONO yield was observed at 40% RH. The heterogeneous photochemical reaction of NO2 with HA was explained by the Langmuir-Hinshelwood mechanism.
Batteries using lithium (Li) metal as the anode are considered
promising energy storage systems because of their high specific energy
densities. The crucial bottlenecks for Li metal anode are Li dendrites
growth and side reactions with electrolyte inducing safety concern,
low Coulombic efficiency (CE), and short cycle life. Vinylene carbonate
(VC), as an effective electrolyte additive in Li-ion batteries, has
been noticed to significantly enhance the CE, whereas the origin of
such an additive remains unclear. Here we use cryogenic transmission
electron microscopy imaging combing with energy dispersive X-ray spectroscopy
elemental and electron energy loss spectroscopy electronic structure
analyses to reveal the role of the VC additive. We discovered that
the electrochemically deposited Li metal (EDLi) in the VC-containing
electrolyte is slightly oxidized with the solid electrolyte interphase
(SEI) being a nanoscale mosaic-like structure comprised of organic
species, Li2O and Li2CO3, whereas
the EDLi formed in the VC-free electrolyte is featured by a combination
of fully oxidized Li with Li2O SEI layer and pure Li metal
with multilayer nanostructured SEI. These results highlight the possible
tuning of crucial structural and chemical features of EDLi and SEI
through additives and consequently direct correlation with electrochemical
performance, providing valuable guidelines to rational selection,
design, and synthesis of additives for new battery chemistries.
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