SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA. SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, CA 94305, USA.
SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA.
Science. 2014 Jul 11;345(6193):197-200. doi: 10.1126/science.1253486.
We introduce a general method for estimating the uncertainty in calculated materials properties based on density functional theory calculations. We illustrate the approach for a calculation of the catalytic rate of ammonia synthesis over a range of transition-metal catalysts. The correlation between errors in density functional theory calculations is shown to play an important role in reducing the predicted error on calculated rates. Uncertainties depend strongly on reaction conditions and catalyst material, and the relative rates between different catalysts are considerably better described than the absolute rates. We introduce an approach for incorporating uncertainty when searching for improved catalysts by evaluating the probability that a given catalyst is better than a known standard.
我们介绍了一种基于密度泛函理论计算来估算计算材料性质不确定性的一般方法。我们通过一系列过渡金属催化剂上氨合成催化速率的计算来说明该方法。研究表明，密度泛函理论计算中的误差相关性在降低计算速率的预测误差方面起着重要作用。不确定性强烈依赖于反应条件和催化剂材料，不同催化剂之间的相对速率比绝对速率描述得要好得多。我们通过评估给定催化剂优于已知标准的概率，引入了一种在寻找改进的催化剂时纳入不确定性的方法。
