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首页> 外文期刊>The Journal of Chemical Physics >A thermodynamic correction to the theory of competitive chemisorption of ions at surface sites with nonelectrostatic physisorption
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A thermodynamic correction to the theory of competitive chemisorption of ions at surface sites with nonelectrostatic physisorption

机译：具有非电诱诱导物地区表面位点竞争性化学理论的热力学校正

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摘要

We resolve a thermodynamic inconsistency in previous theoretical descriptions of the free energy of chemisorption (charge regulation) under conditions where nonelectrostatic physisorption is included, as applied to surface forces and particle-particle interactions. We clarify the role of nonelectrostatic ion physisorption energies and show that a term previously thought to represent physisorbed ion concentrations (activities) should instead be interpreted as a "partial ion activity" based solely on the electrostatic physisorption energy and bulk concentration, or alternatively on the nonelectrostatic physisorption energy and surface concentration. Second, the chemisorption energy must be understood as the change in chemical potential after subtracting the electrostatic energy, not subtracting the physisorption energy. Consequently, a previously reported specific ion nonelectrostatic physisorption contribution to the chemisorption free energy is annulled. We also report a correction to the calculation of surface charge. The distinction in "partial ion activity" evaluated from bulk concentration or from surface concentration opens a way to study nonequilibrium forces where chemisorption is in equilibrium with physisorbed ions but not in equilibrium with bulk ions, e.g., by a jump in ion concentrations. Published under license by AIP Publishing.
机译：在包括非电诱导物理吸附的条件下，在将存在于非电解理物质的条件下，解决了在包括的条件下，解决了在包括表面力和颗粒颗粒相互作用的条件下解决了热力学不一致。我们阐明了非电解离子理由能量的作用，并表明先前认为代表物质离子浓度（活性）的术语应仅基于静电地理能量和体积浓度来解释为“部分离子活性”，或者非电诱惑性能和表面浓度。其次，化学吸收能量必须被理解为减去静电能后的化学潜力的变化，而不是减去物理化能量。因此，将取消先前报道的特定离子非电诱变物理学对化学吸收的贡献。我们还报告了对表面电荷计算的校正。从批量浓度或表面浓度评价的“部分离子活性”的区别开启了一种缺乏研究的方法，其中化学吸附是与物理吸收离子的平衡，但不能与体离子的平衡，例如，通过离子浓度的跳跃。通过AIP发布在许可证下发布。

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