Uncovering fast solid-acid proton conductors based on dynamics of polyanion groups and proton bonding strength,Energy & Environmental Science

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Uncovering fast solid-acid proton conductors based on dynamics of polyanion groups and proton bonding strength
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2024-06-19 , DOI: 10.1039/d4ee01219d
Pjotrs Žguns ₁ , Konstantin Klyukin _{1,

2} , Louis S. Wang ₃ , Grace Xiong ₃ , Ju Li _{1,

4} , Sossina M. Haile ₃ , Bilge Yildiz _{1,

4}

Affiliation

Achieving high proton conductivity in inorganic solids is key for advancing many electrochemical technologies, including low-energy nano-electronics and energy-efficient fuel cells and electrolyzers. A quantitative understanding of the physical traits of a material that regulate proton diffusion is necessary for accelerating the discovery of fast proton conductors. In this work, we have mapped the structural, chemical and dynamic properties of solid acids to the elementary steps of the Grotthuss mechanism of proton diffusion. Our approach combines ab initio molecular dynamics simulations, analysis of phonon spectra and atomic structure calculations. We have identified the donor–hydrogen bond lengths and the acidity of polyanion groups as key descriptors of local proton transfer and the vibrational frequencies of the cation framework as the key descriptor of lattice flexibility. The latter facilitates rotations of polyanion groups and long-range proton migration in solid acid proton conductors. The calculated lattice flexibility also correlates with the experimentally reported superprotonic transition temperatures. Using these descriptors, we have screened the Materials Project database and identified potential solid acid proton conductors with monovalent, divalent and trivalent cations, including Ag⁺, Sr²⁺, Ba²⁺ and Er³⁺ cations, which go beyond the traditionally considered monovalent alkali cations (Cs⁺, Rb⁺, K⁺, and NH₄⁺) in solid acids.

中文翻译：

基于聚阴离子基团动力学和质子键合强度揭示快速固体酸质子导体

在无机固体中实现高质子电导率是推进许多电化学技术的关键，包括低能纳米电子学和节能燃料电池和电解槽。定量了解调节质子扩散的材料的物理特性对于加速快速质子导体的发现是必要的。在这项工作中，我们将固体酸的结构、化学和动力学性质映射到质子扩散的格罗萨斯机制的基本步骤。我们的方法结合了从头算分子动力学模拟、声子光谱分析和原子结构计算。我们已经确定供体氢键长度和聚阴离子基团的酸度作为局部质子转移的关键描述符，以及阳离子框架的振动频率作为晶格柔性的关键描述符。后者促进聚阴离子基团的旋转和固体酸质子导体中的长程质子迁移。计算出的晶格柔性也与实验报告的超质子转变温度相关。使用这些描述符，我们筛选了材料项目数据库，并确定了具有一价、二价和三价阳离子的潜在固体酸质子导体，包括 Ag ⁺ 、 Sr ²⁺ 、 Ba ²⁺ 阳离子，超出了传统上认为的一价碱金属阳离子（Cs ⁺ 、 Rb ⁺ 、 K ⁺ ，和 NH ₄ ⁺ ）在固体酸中。

更新日期：2024-06-19

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