CATKINAS软件包与相关体系动力学模拟

多相催化在现代化工中有着不可或缺的作用，尤其是在能源转化和环境领域，其中催化剂扮演着关键角色。现如今，高效催化剂的科学设计已成为研究人员的重要目标，但也是挑战难题。相比于传统实验上相对低效的试错法，近二十多年来密度泛函理论(DFT)和微观动力学分析的发展，可以促使研究人员从理论上评估催化剂的活性及变化规律，进而有助于催化剂的科学筛选和整体设计。第一性原理计算可以从微观层面计算得到每一步基元反应的反应能垒和焓变，以及中间物种的吸附能。基于平均场近似的微观动力学则在微观化学基元反应和宏观催化剂反应 活性之间扮演了桥梁作用。通过微观动力学分析，可以得到反应的宏观性质(覆盖度、反应速率等)以及决速因素等，进而来描述催化剂的活性趋势。然而，由于微动力学方程组的复杂性(基元反应多、中间物种多、反应级数不同)和基元反应速率常数之间数量级的差异等引发的刚性问题(stiff problem)，一般很难快速求解。为了克服现有的求解稳态微观动力学方程组求解方法的不足，我们开发了灵敏度监督联锁算法（SSIA）、粒子群优化与修正牛顿法耦合系统（PNEWCS）和可逆性迭代法（RIM）等功能强大的自研稳态求解器；最后以求解算法为核心，我们开发了一个大规模催化反应微动力学模拟与分析软件CATKINAS程序(A large-scale catalytic microkinetic analysis software)，可以实现不同反应温度、压力下反应网络的高效稳定的活性模拟与评估；同时针对能源转化和环境领域密切相关的催化体系，比如合成氨、NO消除、CO2还原等，通过DFT计算获得基元反应的能垒和焓变的数据，利用CATKINAS进行了活性评估和动力学模拟（微动力学求解和反应动力学演化）以及催化分析（活性/选择性，敏感度，物种分布图，活性趋势图，反应坐标/网络图等），从而为实验上能源/环境相关的催化剂优化提供理论指导，数据量1.1GB。

Heterogeneous catalysis plays an indispensable role in modern chemical industry, especially in the fields of energy conversion and environmental protection, where catalysts act as pivotal components. Currently, the rational design of high-performance catalysts has become a core goal for researchers, yet it remains a significant challenge. Compared with the relatively inefficient trial-and-error method in traditional experiments, the development of density functional theory (DFT) and microkinetic analysis over the past two decades has enabled researchers to theoretically evaluate the activity and variation rules of catalysts, thereby facilitating the rational screening and overall design of catalysts. First-principles calculations can obtain the reaction energy barriers, enthalpy changes of each elementary reaction, as well as the adsorption energies of intermediate species at the microscopic level. Microkinetics based on the mean-field approximation acts as a bridge between microscopic elementary chemical reactions and macroscopic catalytic reaction activity. Through microkinetic analysis, one can acquire the macroscopic properties of the reaction (such as surface coverage, reaction rates, etc.) and rate-determining factors, thus describing the activity trends of catalysts. However, due to the complexity of microkinetic differential equations (including a large number of elementary reactions, diverse intermediate species, and varying reaction orders) and the stiff problem caused by orders-of-magnitude differences among elementary reaction rate constants, it is generally difficult to solve them rapidly. To address the limitations of existing solvers for steady-state microkinetic differential equations, we developed several powerful in-house steady-state solvers, including the Sensitivity Supervised Interlocking Algorithm (SSIA), the Particle Swarm Optimization coupled with Modified Newton Method system (PNEWCS), and the Reversibility Iteration Method (RIM). Finally, centered on these solvers, we developed a large-scale catalytic reaction microkinetic simulation and analysis software named CATKINAS, which can efficiently and stably simulate and evaluate reaction networks under different reaction temperatures and pressures. Meanwhile, for catalytic systems closely related to energy conversion and environmental protection, such as ammonia synthesis, NO abatement, CO₂ reduction, etc., we obtained data on energy barriers and enthalpy changes of elementary reactions via DFT calculations, and conducted activity evaluation, kinetic simulation (including microkinetic solving and reaction kinetic evolution), and catalytic analysis (such as activity/selectivity, sensitivity analysis, species distribution plots, activity trend plots, reaction coordinate/network diagrams, etc.) using CATKINAS, thereby providing theoretical guidance for the experimental optimization of catalysts related to energy and environmental applications. The total dataset size is 1.1 GB.

搜集汇总

背景与挑战

背景概述

该数据集包含CATKINAS软件包及相关催化体系的动力学模拟数据，用于大规模催化反应的微动力学分析与评估。它基于自研稳态求解器，能够高效模拟不同温度、压力下的反应网络，并应用于合成氨、NO消除等能源环境领域的催化剂活性评估，为实验优化提供理论指导。数据量约为1.23GB，包含7150个文件，属于化学学科范畴。