Pahari Swagata, Roy Sudip
National Chemical Laboratory, Pune, India.
Phys Chem Chem Phys. 2015 Nov 11;17(45):30551-9. doi: 10.1039/c5cp05735c.
We performed first principles molecular dynamics simulations to elucidate the mechanism and role of 1,2,3-triazole in proton transport while it is mixed with phosphoric acid (PA) and a phosphoric acid imidazole mixture. PA doped imidazole based polymer acts as an efficient polyelectrolyte membrane for fuel cells. The conductivity of this membrane increases when triazole is added to the system. For the first time we performed ab initio molecular dynamics simulations of complex mixtures of PA, imidazole and triazole. We have quantitatively estimated the structural diffusion and vehicular motion of protons. We found that upon the addition of triazole in PA and the PA imidazole mixture, the structural diffusion of protons increases significantly. The mechanism of proton transport is different when triazole is added to the mixture. We have also identified two different paths for structural diffusion (constructive and non-constructive) that contribute to long and short range proton transport.
我们进行了第一性原理分子动力学模拟，以阐明1,2,3 - 三唑在与磷酸（PA）及磷酸咪唑混合物混合时在质子传输中的机制和作用。PA掺杂的咪唑基聚合物用作燃料电池的高效聚电解质膜。当向该体系中添加三唑时，该膜的电导率会增加。我们首次对PA、咪唑和三唑的复杂混合物进行了从头算分子动力学模拟。我们定量估计了质子的结构扩散和载流子运动。我们发现，在PA和PA - 咪唑混合物中添加三唑后，质子的结构扩散显著增加。当三唑添加到混合物中时，质子传输的机制有所不同。我们还确定了结构扩散的两条不同路径（建设性和非建设性），它们分别有助于长程和短程质子传输。
