Computational studies of nonequilibrium processes in electrochemical materials science and catalysis

该奖项支持电化学材料科学和多相催化中非平衡现象的计算和理论研究的研究和教育。 这些研究涉及特定实验系统的建模，对此类系统重要的基本非平衡现象的调查，以及计算和理论方法的进一步发展。将与实验组合作研究的特定实验现象是（i）验证PI计算机模拟建议的加速锂离子电池充电的新方法，和（ii）在单晶金表面的电化学脉冲电位研究中的岛生长和溶解。 研究中的特殊非平衡现象包括电化学表面改性和多相催化反应中的横向扩散效应。 PI将使用大规模计算机模拟来模拟各种感兴趣的系统。将采用连续和离散模型。 计算方法包括动力学蒙特卡罗和分子动力学模拟，模型参数从基于密度泛函理论的量子力学计算获得。 模拟数据将通过几种理论方法进行分析，包括有限尺寸标度理论，随机过程理论和统计学。在更广泛的意义上，支持的研究有助于理解与一般非平衡过程相关的问题。更具体地说，它预计将导致实现在电极-电解质界面的非平衡过程的更好的理解。 因此，它可能在支持未来开发新的基于电化学的环境清理，纳米材料，化学品和药物制造，腐蚀防护以及可再生能源技术（包括可充电电池和燃料电池）方面具有广泛的影响。通过该奖项开发的基础知识和仿真算法适用于许多科学和技术领域，包括材料科学，化学，生物学，甚至通信网络和电网的设计和分析。 从教育的角度来看，这种计算密集型研究非常适合让初级和高级学徒参与发现过程。这些活动将促进各级教育，同时包括妇女和少数民族，让本科生、研究生和博士后研究员参与，他们将指导K-12学生。研究成果将通过在各种专业期刊上发表文章、在科学会议上发表演讲、向公众发表演讲以及通过万维网进行传播。非技术性总结该奖项支持在纳米尺度上材料和原子结构生长的理论和计算研究和教育，大约是一千万分之一英寸 形成本研究重点的“电化学”现象和过程是在金属或半导体（称为“电极”）与离子导体（称为“电解质”）的界面处发生的化学反应，例如在电池内部发生的化学反应。 在过去的三十年中，实验技术已经变得可用，使电化学方法能够制造高科技材料和设计催化剂，这些催化剂从纳米长度尺度上的特定结构中获得其功能。这些方法正迅速成为传统方法的成本效益高的替代方法。 这些令人印象深刻的实验发展与计算机技术和计算方法的惊人进步相匹配。PI将使用大规模计算机模拟方法来研究纳米长度尺度的结构如何在浸入化学溶液中的电极材料表面生长，电流流过电极。从更广泛的意义上说，所支持的研究有助于理解与远离平衡状态的过程有关的问题。更具体地说，它预计将导致实现在电极-电解质界面的平衡过程的改善的理解。 因此，它可能在支持未来开发新的基于电化学的环境清理，纳米材料，化学品和药物制造，腐蚀防护以及可再生能源技术（包括可充电电池和燃料电池）方面具有广泛的影响。通过该奖项开发的基础知识和仿真算法适用于许多科学和技术领域，包括材料科学，化学，生物学，甚至通信网络和电网的设计和分析。 从教育的角度来看，这种计算密集型研究非常适合让初级和高级学徒参与发现过程。这些活动将促进各级教育，同时包括妇女和少数民族，让本科生、研究生和博士后研究员参与，他们将指导K-12学生。研究结果将通过各种专业期刊上的文章、科学会议上的谈话、向公众介绍以及通过万维网进行传播。

TECHNICAL SUMMARYThis award supports research and education in computational and theoretical studies of nonequilibrium phenomena in electrochemical materials science and heterogeneous catalysis. These studies are concerned with modeling of specific experimental systems, with investigation of fundamental nonequilibrium phenomena of importance to such systems, and with further development of computational and theoretical methods.The particular experimental phenomena that will be investigated in collaboration with experimental groups are (i) validation of a new method to accelerate the charging of Li-ion batteries suggested by the PI's computer simulations, and (ii) island growth and dissolution in electrochemical pulsed-potential studies of single-crystal gold surfaces. The particular nonequilibrium phenomena under investigation include the effects of lateral diffusion during electrochemical surface modification and in heterogeneous catalytic reactions. The PI will use large scale computer simulation to model various systems of interest. Both continuous and discrete models will be employed. Computational methods include kinetic Monte Carlo and Molecular Dynamics simulations with model parameters obtained from quantum mechanical calculations based on density functional theory. The simulation data will be analyzed by several theoretical methods including finite-size scaling theory, theory of stochastic processes, and statistics.In a broader sense, the supported research contributes to understanding issues related to nonequilibrium processes in general. More specifically, it is expected to lead to achieving an improved understanding of nonequilibrium processes at electrode-electrolyte interfaces. As such, it could have broad implications in supporting the future development of new, electrochemistry-based processes for environmental cleanup, manufacturing of nanomaterials, chemicals, and pharmaceuticals, and corrosion protection, as well as renewable-energy technologies including rechargeable batteries and fuel cells. The fundamental knowledge and simulation algorithms developed through this award are applicable in many scientific and technological fields, including materials science, chemistry, biology, and even to the design and analysis of communications networks and power grids. From an educational perspective, this computationally intensive research is ideal for involving both beginning and advanced apprentices in the discovery process. The activities will contribute to education at all levels while including women and minorities by involving undergraduate and graduate students and postdoctoral fellows, who will mentor K-12 students. The results of the research will be communicated through articles in a wide spectrum of professional journals, through talks at scientific meetings, and through presentations for the general public, as well as through the World Wide Web.NONTECHNICAL SUMMARYThis award supports theoretical and computational research and education on the growth of materials and structures of atoms at the length scale of a nanometer, that is approximately one ten-millionth of an inch. The "electrochemical" phenomena and processes that form the focus of this research are chemical reactions that occur at the interface of a metal or a semiconductor, called the "electrode", with an ionic conductor, called the "electrolyte", such as those that take place inside a battery. During the last three decades, experimental techniques have become available that enable electrochemical methods to manufacture high-tech materials and designer catalysts that derive their functionality from the particular structures on the nanometer length scale. Such methods are rapidly becoming cost-effective alternatives to traditional methods. These impressive experimental developments are matched by spectacular progress in computer technology and computational methods. The PI will use large scale computer simulation methods to study how structures at the nanometer length scale grow on the surface of electrode materials immersed in a chemical solution with an electric current flowing through the electrodes. In a broader sense, the supported research contributes to understanding issues related to processes that are far from the state of balance understood as equilibrium. More specifically, it is expected to lead to achieving an improved understanding of out-of-equilibrium processes at electrode-electrolyte interfaces. As such, it could have broad implications in supporting the future development of new, electrochemistry-based processes for environmental cleanup, manufacturing of nanomaterials, chemicals, and pharmaceuticals, and corrosion protection, as well as renewable-energy technologies including rechargeable batteries and fuel cells. The fundamental knowledge and simulation algorithms developed through this award are applicable in many scientific and technological fields, including materials science, chemistry, biology, and even to the design and analysis of communications networks and power grids. From an educational perspective, this computationally intensive research is ideal for involving both beginning and advanced apprentices in the discovery process. The activities will contribute to education at all levels while including women and minorities by involving undergraduate and graduate students and postdoctoral fellows, who will mentor K-12 students. The results of the research will be communicated through articles in a wide spectrum of professional journals, through talks at scientific meetings, and through presentations for the general public, as well as through the World Wide Web.