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.
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