论文标题
外部电场下的三维活动火山图
Three Dimensional Activity Volcano Plot under External Electric Field
论文作者
论文摘要
外部电场（EEF）会影响氧化还原系统以外的广泛催化过程。针对特定操作条件的EEFS下的催化剂的计算设计基本上需要对复杂的物理化学系统对集体参数（例如EEF强度/方向/温度）的响应进行准确的预测。在这里，我们开发了一种基于第一原理的多尺度方法，该方法可以使异质催化的有效依赖EEF依赖性动力学建模。以甲醇的蒸汽重整为例，我们发现甲醇转化率对温度和EEF表现出强烈的非线性反应，并且在温度下定义的最佳场和恒定碳浓度线 - EEEF参数空间是催化剂设计的强大指标。在深层神经网络的协助下，我们在EEFS下建立了三维活动的火山图，用于成千上万的金属合金。
An external electric field (EEF) can impact a broad range of catalytic processes beyond redox systems. Computational design of catalysts under EEFs targeting specific operation conditions essentially requires accurate predictions of the response of a complex physicochemical system to collective parameters such as EEF strength/direction and temperature. Here, we develop a first-principles-based multiscale approach that enables efficient EEF-dependent kinetic modeling of heterogeneous catalysis. Taking steam reforming of methanol as an example, we find that the methanol conversion rate exhibits strong nonlinear response to temperature and EEF, and the optimal field line and constant carbon concentration line defined in the temperature--EEF parameter space serve as powerful metrics for catalyst design. Assisted with a deep neural network, we establish a three-dimensional activity volcano plot under EEFs for thousands of metallic alloys.
