Computational studies of nonequilibrium processes in electrochemical materials science and catalysis

技术总结该奖项支持在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方面的研究和教育。这些研究涉及特定实验系统的建模，对这些系统重要的基本非平衡现象的研究，以及计算和理论方法的进一步发展。将与实验小组合作研究的特殊实验现象是：(I)由PI的计算机模拟提出的加速锂离子电池充电的新方法的验证；(Ii)单晶金表面电化学脉冲电位研究中的岛生长和溶解。所研究的特殊非平衡现象包括电化学表面修饰和多相催化反应中的侧扩散效应。PI将使用大规模计算机模拟来对各种感兴趣的系统进行建模。将采用连续和离散两种模型。计算方法包括用基于密度泛函理论的量子力学计算得到的模型参数进行动力学蒙特卡罗模拟和分子动力学模拟。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。从更广泛的意义上说，支持的研究有助于从总体上理解与非平衡过程相关的问题。更具体地说，这将有助于更好地理解电极-电解液界面的非平衡过程。因此，它可能会对支持未来环境清理、纳米材料、化学品和药品制造、腐蚀保护以及可再生能源技术(包括充电电池和燃料电池)的基于电化学的新工艺的发展产生广泛影响。通过该奖项开发的基础知识和模拟算法适用于许多科学和技术领域，包括材料科学、化学、生物，甚至适用于通信网络和电网的设计和分析。从教育的角度来看，这种计算密集的研究是让初学者和高级学徒参与发现过程的理想选择。这些活动将有助于各级教育，同时包括妇女和少数群体，让本科生和研究生以及博士后研究员参与，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、科学会议上的演讲和面向公众的演讲以及通过万维网进行交流。非技术总结该奖项支持在纳米尺度上生长材料和原子结构的理论和计算研究和教育，这一尺度大约为1000万英寸。形成这项研究重点的“电化学”现象和过程是指在金属或半导体(称为“电极”)与离子导体(称为“电解液”)的界面上发生的化学反应，例如发生在电池内部的化学反应。在过去的三十年里，实验技术已经成为可能，使电化学方法能够制造高科技材料和设计催化剂，这些催化剂从纳米级的特定结构中获得功能。这些方法正在迅速成为传统方法的具有成本效益的替代品。与这些令人印象深刻的实验发展相匹配的是计算机技术和计算方法的惊人进步。PI将使用大规模的计算机模拟方法来研究在电流流过电极的化学溶液中浸泡的电极材料表面如何生长纳米尺度的结构。在更广泛的意义上，得到支持的研究有助于理解与过程相关的问题，这些过程远远不是被理解为均衡的平衡状态。更具体地说，这将有助于更好地理解电极-电解液界面的非平衡过程。因此，它可能会对支持未来环境清理、纳米材料、化学品和药品制造、腐蚀保护以及可再生能源技术(包括充电电池和燃料电池)的基于电化学的新工艺的发展产生广泛影响。通过该奖项开发的基础知识和模拟算法适用于许多科学和技术领域，包括材料科学、化学、生物，甚至适用于通信网络和电网的设计和分析。从教育的角度来看，这种计算密集的研究是让初学者和高级学徒参与发现过程的理想选择。这些活动将有助于各级教育，同时包括妇女和少数群体，让本科生和研究生以及博士后研究员参与，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的文章、在科学会议上的演讲、面向公众的演讲以及通过万维网进行交流。

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.