Functional mesoporous carbons have attracted significant scientific and technological interest owning to their fascinating and excellent properties. However, controlled synthesis of functional mesoporous carbons with large tunable pore sizes, small particle size, well-designed functionalities, and uniform morphology is still a great challenge. Herein, we report a versatile nanoemulsion assembly approach to prepare Ndoped mesoporous carbon nanospheres with high uniformity and large tunable pore sizes (5−37 nm). We show that the organic molecules (e.g., 1,3,5-trimethylbenzene, TMB) not only play an important role in the evolution of pore sizes but also significantly affect the interfacial interaction between soft templates and carbon precursors. As a result, a welldefined Pluronic F127/TMB/dopamine nanoemulsion can be facilely obtained in the ethanol/water system, which directs the polymerization of dopamine into highly uniform polymer nanospheres and their derived N-doped carbon nanospheres with diversely novel structures such as smooth, golf ball, multichambered, and dendritic nanospheres. The resultant uniform dendritic mesoporous carbon nanospheres show an ultralarge pore size (∼37 nm), small particle size (∼128 nm), high surface area (∼635 m 2 g −1 ), and abundant N content (∼6.8 wt %), which deliver high current density and excellent durability toward oxygen reduction reaction in alkaline solution.
The reduction of ammonia (NH3) emissions is urgently needed due to its role in aerosol nucleation and growth causing haze formation during its conversion into ammonium (NH4(+)). However, the relative contributions of individual NH3 sources are unclear, and debate remains over whether agricultural emissions dominate atmospheric NH3 in urban areas. Based on the chemical and isotopic measurements of size-resolved aerosols in urban Beijing, China, we find that the natural abundance of (15)N (expressed using δ(15)N values) of NH4(+) in fine particles varies with the development of haze episodes, ranging from -37.1‰ to -21.7‰ during clean/dusty days (relative humidity: ∼ 40%), to -13.1‰ to +5.8‰ during hazy days (relative humidity: 70-90%). After accounting for the isotope exchange between NH3 gas and aerosol NH4(+), the δ(15)N value of the initial NH3 during hazy days is found to be -14.5‰ to -1.6‰, which indicates fossil fuel-based emissions. These emissions contribute 90% of the total NH3 during hazy days in urban Beijing. This work demonstrates the analysis of δ(15)N values of aerosol NH4(+) to be a promising new tool for partitioning atmospheric NH3 sources, providing policy makers with insights into NH3 emissions and secondary aerosols for regulation in urban environments.
The
low-efficiency cellular uptake property of current nanoparticles
greatly restricts their application in the biomedical field. Herein,
we demonstrate that novel virus-like mesoporous silica nanoparticles
can easily be synthesized, showing greatly superior cellular uptake
property. The unique virus-like mesoporous silica nanoparticles with
a spiky tubular rough surface have been successfully synthesized
via a novel single-micelle epitaxial growth approach in a low-concentration-surfactant
oil/water biphase system. The virus-like nanoparticles’ rough
surface morphology results mainly from the mesoporous silica nanotubes
spontaneously grown via an epitaxial growth process. The obtained
nanoparticles show uniform particle size and excellent monodispersity.
The structural parameters of the nanoparticles can be well tuned with
controllable core diameter (∼60–160 nm), tubular length
(∼6–70 nm), and outer diameter (∼6–10
nm). Thanks to the biomimetic morphology, the virus-like nanoparticles
show greatly superior cellular uptake property (invading living cells
in large quantities within few minutes, <5 min), unique internalization
pathways, and extended blood circulation duration (t1/2 = 2.16 h), which is much longer than that of conventional
mesoporous silica nanoparticles (0.45 h). Furthermore, our epitaxial
growth strategy can be applied to fabricate various virus-like mesoporous
core–shell structures, paving the way toward designed synthesis
of virus-like nanocomposites for biomedicine applications.
The limited availability of ammonia (NH) measurements is currently a barrier to understanding the vital role of NH in secondary aerosol formation during haze pollution events and prevents a full assessment of the atmospheric deposition of reactive nitrogen. The observational gaps motivated us to design this study to investigate the spatial distributions and seasonal variations in atmospheric NH on a national scale in China. On the basis of a 1-year observational campaign at 53 sites with uniform protocols, we confirm that abundant concentrations of NH [1 to 23.9 μg m] were identified in typical agricultural regions, especially over the North China Plain (NCP). The spatial pattern of the NH surface concentration was generally similar to those of the satellite column concentrations as well as a bottom-up agriculture NH emission inventory. However, the observed NH concentrations at urban and desert sites were comparable with those from agricultural sites and 2-3 times those of mountainous/forest/grassland/waterbody sites. We also found that NH deposition fluxes at urban sites account for only half of the emissions in the NCP, suggesting the transport of urban NH emissions to downwind areas. This finding provides policy makers with insights into the potential mitigation of nonagricultural NH sources in developed regions.
Like surfactants with tunable hydrocarbon chain length, Janus nanoparticles also possess the ability to stabilize emulsions. The volume ratio between the hydrophilic and hydrophobic domains in a single Janus nanoparticle is very important for the stabilization of emulsions, which is still a great challenge. Herein, dual-mesoporous FeO@mC&mSiO Janus nanoparticles with spatial isolation of hydrophobic carbon and hydrophilic silica at the single-particle level have successfully been synthesized for the first time by using a novel surface-charge-mediated selective encapsulation approach. The obtained dual-mesoporous FeO@mC&mSiO Janus nanoparticles are made up of a pure one-dimensional mesoporous SiO nanorod with tunable length (50-400 nm), ∼100 nm wide and ∼2.7 nm mesopores and a closely connected mesoporous FeO@mC magnetic nanosphere (∼150 nm diameter, ∼10 nm mesopores). As a magnetic "solid amphiphilic surfactant", the hydrophilic/hydrophobic ratio can be precisely adjusted by varying the volume ratio between silica and carbon domains, endowing the Janus nanoparticles surfactant-like emulsion stabilization ability and recyclability under a magnetic field. Owing to the total spatial separation of carbon and silica, the Janus nanoparticles with an optimized hydrophilic/hydrophobic ratio show spectacular emulsion stabilizing ability, which is crucial for improving the biphasic catalysis efficiency. By selectively anchoring catalytic active sites into different domains, the fabricated Janus nanoparticles show outstanding performances in biphasic reduction of 4-nitroanisole with 100% conversion efficiency and 700 h high turnover frequency for biphasic cascade synthesis of cinnamic acid.
The greatest challenge for lithium−sulfur (Li−S) batteries application is the development of cathode hosts to address the low conductivity, huge volume change, and shuttling effect of sulfur or lithium polysulfides (LiPs). Herein, we demonstrate a composite host to circumvent these problems by confining sub-nanometric manganous oxide clusters (MOCs) in nitrogen doped mesoporous carbon nanosheets. The atomic structure of MOCs is well-characterized and optimized via the extended X-ray absorption fine structure analysis and density functional theory (DFT) calculations. Benefiting from the unique design, the assembled Li−S battery displays remarkable electrochemical performances including a high reversible capacity (990 mAh g −1 after 100 cycles at 0.2 A g −1 ) and a superior cycle life (60% retention over 250 cycles at 2 A g −1 ). Both the experimental results and DFT calculations demonstrate that the well-dispersed MOCs could significantly promote the chemisorption of LiPs, thus greatly improving the capacity and rate performance.
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