CAREER: First Principles Studies of Interfacial Phenomena: Applications to Catalysis and Electrochemistry

Perla Balbuena教授将开发分子建模方法来研究金属、碳金属、合金和电解质的晶体和界面结构和性质。特别感兴趣的性质是离子扩散系数，离子电导率，溶剂化结构，吸附热和反应。这一结果将影响化学和电化学原理及其应用。它将主要涉及工业产品，如吸附剂、催化剂、电池和燃料电池；在它们的应用中涉及的基本物理化学现象；以及由此衍生的应用过程。研究的第一个目标是石墨中锂嵌入的建模。预期的结果是预测和验证开路电压和差分容量与组成的依赖关系，以及从超密相LiC2到LiC6转变的条件。第二个目标是确定锂离子和高氯酸盐离子的扩散动力学，以及高氯酸锂离子对在碳酸乙烯和碳酸丙烯电解质中的结合。为了实现这一目标，PI将研究石墨电极的降解机制，特别是Li2CO3钝化层的形成。她还将模拟溶剂化物质插入石墨的过程。第三个目标是研究甲烷在Ni和Ni/Cu上裂解生成氢和碳，以及氢在碳中的储存的相关现象。这些研究将涉及结构模型的发展，从头算和半经验量子力学计算，以及分子动力学模拟，用于具有实际重要性的化学和电化学系统。所开发的方法可能会对化学工程学生的培训以及过程和产品设计的实践产生影响。PI正在开发新的入门课程，并修改现有课程，以提高工程专业学生从第一性原理预测微观性质的能力。

Professor Perla Balbuena will develop molecular modeling methods to study the crystalline and interfacial structure and properties of metals, carbon-metal, alloys and electrolytes. The properties of particular interest are ionic diffusion coefficients, ionic conductivities, solvation structures, heats of adsorption and reaction. The outcome will impact chemical and electrochemical principles and applications. It will pertain mostly to industrial products such as adsorbents, catalysts, batteries, and fuel cells; the fundamental physicochemical phenomena involved in their utilization; and the applied processes derived from them. The first objective of the research is the modeling of Li intercalation in graphite. The expected result is prediction and validation of the dependence of open-circuit voltage and differential capacity with respect to composition, and the conditions for the transition from the super dense phase LiC2 to LiC6. The second objective is the determination of diffusion dynamics of Li and perchlorate ions, and of ion-pair association of Li perchlorate, in ethylene carbonate and propylene carbonate electrolytes. Following that objective, the PI will investigate the mechanism of degradation of graphite electrodes, in particular the formation of a presumed Li2CO3 passivation layer. She will also model the intercalation of solvated species into graphite. The third objective is the study of methane cracking over Ni and Ni/Cu to produce hydrogen and carbon, and the related phenomenon of hydrogen storage in carbon. These investigations will involve the development of structural models, ab initio and semiempirical quantum mechanical calculations, and molecular dynamics simulations, for chemical and electrochemical systems of practical importance. The methodology to be developed will likely have impact in the training of chemical engineering students as well as the practice of process and product design. The PI is developing new introductory courses and modifying the existing ones to raise the engineering students' capability to predict microscopic properties from first principles.