储氢的密度泛函：用Ab Initio基准定义H2Bind275测试集并评估55个泛函
Density Functionals for Hydrogen Storage: Defining the H2Bind275 Test Set with Ab Initio Benchmarks and Assessment of 55 Functionals
摘要：
高效和高容量的存储材料对于氢基经济是不可或缺的。计算机工具可以加速发现具有最佳氢吸附性能的新吸附材料的过程。密度泛函理论很有可能成为高通量筛选潜在材料的一个非常有用的工具。在这项工作中，我们已经确定了密度泛函近似，提供了良好的性能，氢结合的应用程序后，双管齐下的方法。首先，我们编制了一个数据集（H2 Bind 275），全面代表了氢结合问题，捕获贮氢材料中遇到的结合位点的化学和机械多样性。我们还计算了参考相互作用能为这个数据集使用耦合集群理论。其次，我们评估了55个密度泛函近似预测H $_2$相互作用能的性能，并确定了两个混合密度泛函（$ω$ B 97 X-V和$ω$ B 97 M-V），两个双混合密度泛函（DSD-PBEPBE-D3（BJ）和PBE 0-DH）和一个半局域密度泛函（B 97 M-V）作为最佳性能。我们已经推荐了经验色散修正系统欠约束密度泛函，如revPBE，BLYP和B3 LYP的性能改善，在可以忽略不计的额外成本。我们还推荐使用def 2-TZVPP基组，因为它代表了精度和成本之间的良好折衷，将有限基组误差限制在1 kJ/mol以下。
英文摘要：
Efficient and high capacity storage materials are indispensable for a hydrogen-based economy. In silico tools can accelerate the process of discovery of new adsorbent materials with optimal hydrogen adsorption enthalpies. Density functional theory is well-poised to become a very useful tool for enabling high-throughput screening of potential materials. In this work, we have identified density functional approximations that provide good performance for hydrogen binding applications following a two-pronged approach. First, we have compiled a dataset (H2Bind275) that comprehensively represents the hydrogen binding problem capturing the chemical and mechanistic diversity in the binding sites encountered in hydrogen storage materials. We have also computed reference interaction energies for this dataset using coupled cluster theory. Secondly, we have assessed the performance of 55 density functional approximations for predicting H$_2$ interaction energies and have identified two hybrid density functionals ($ω$B97X-V and $ω$B97M-V), two double hybrid density functionals (DSD-PBEPBE-D3(BJ) and PBE0-DH), and one semi-local density functional (B97M-V) as the best performing ones. We have recommended the addition of empirical dispersion corrections to systematically underbinding density functionals like revPBE, BLYP, and B3LYP for improvements in performance at negligible additional cost. We have also recommended the usage of the def2-TZVPP basis set as it represents a good compromise between accuracy and cost, limiting the finite basis set errors to less than 1kJ/mol.
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