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1.
Article in English | MEDLINE | ID: mdl-35682431

ABSTRACT

New particle formation (NPF) contributes significantly to atmospheric particle number concentrations and cloud condensation nuclei (CCN). In sulfur-rich environments, field measurements have shown that sulfuric acid dimer formation is likely the critical step in NPF. We investigated the dimer formation process based upon the measured sulfuric acid monomer and dimer concentrations, along with previously reported amine concentrations in a sulfur-rich atmosphere (Atlanta, USA). The average sulfuric acid concentration was in the range of 1.7 × 107-1.4 × 108 cm-3 and the corresponding neutral dimer concentrations were 4.1 × 105-5.0 × 106 cm-3 and 2.6 × 105-2.7 × 106 cm-3 after sub-collision and collision ion-induced clustering (IIC) corrections, respectively. Two previously proposed acid-base mechanisms (namely AA and AB) were employed to respectively estimate the evaporation rates of the dimers and the acid-amine complexes. The results show evaporation rates of 0.1-1.3 s-1 for the dimers based on the simultaneously measured average concentrations of the total amines, much higher than those (1.2-13.1 s-1) for the acid-amine complexes. This indicates that the mechanism for dimer formation is likely AA through the formation of more volatile dimers in the initial step of the cluster formation.


Subject(s)
Atmosphere , Sulfuric Acids , Amines , Sulfur
2.
Nanoscale ; 11(36): 17084-17092, 2019 Sep 19.
Article in English | MEDLINE | ID: mdl-31506661

ABSTRACT

Developing economic, effective and stable bifunctional electrocatalysts to achieve sustainable hydrogen production is highly desired. Herein, C-coated CoP hollow microporous nanocages (C-CoP-1/12) are synthesized by calcination of a Prussian blue analog precursor and subsequent phosphorization treatment. Under alkaline condition, the C-CoP-1/12 exhibit splendid electrocatalytic performance with a low overpotential of 173 mV for hydrogen evolution reaction (HER) and 333 mV for oxygen evolution reaction (OER) at a current density of 10 mA cm-2. The C-CoP-1/12 show high electrocatalytic performance for overall water splitting at a low potential of only 1.650 V for the driving current density of 10 mA cm-2, and they exhibit remarkable stability for at least 24 h. The engineering of phosphating is the critical step for the synthesis of pure-phase CoP with hollow nanoarchitecture. Compared with Co2P, CoP possesses lower water dissociation barrier and favorable ΔGH* value according to theoretical calculations, resulting in superior electrocatalytic performance. Such impressive water splitting performance is mainly attributed to the collective effects of metal phosphide with unique electronic structure, the shortened electron transport paths, and the conductive C coating. This strategy is believed to provide a basis for the development of electrode materials with highly efficient electrocatalytic water-splitting capability.

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