评估用于氮物种多相催化的交换关联泛函
Assessing exchange-correlation functionals for heterogeneous catalysis of nitrogen species
AI总结：
针对含氮化合物多相催化领域交换关联泛函评估不足的问题，研究评估了GGA到RPA的多种泛函在氮物种形成能、催化剂晶格常数及中间体吸附能计算中的表现，发现泛函和范德华校正影响显著，需根据具体反应和材料选择泛函。
摘要：
人们对氨、硝酸盐和尿素的可持续合成日益增长的兴趣，推动了利用多相催化剂实现含氮化合物间催化转化的研究增多。密度泛函理论（DFT）常被用于从分子尺度深入理解这些反应，但针对最适合含氮化合物多相催化的交换关联泛函，相关评估仍相对较少。本文中，我们评估了从广义梯度近似（GGA）到无规相近似（RPA）的一系列泛函，评估维度包括气相氮物种的形成能、几类常见催化剂（金属、氧化物、金属有机框架（MOFs））代表性固体的晶格常数，以及多种含氮中间体在这些材料上的吸附能。结果表明，交换关联泛函和范德华校正的选择会产生惊人的巨大影响，且提升理论水平并不总能提高含氮化合物相关计算的准确性。这表明泛函的选择需基于所研究的特定反应和材料进行仔细评估。
英文摘要：
Increasing interest in sustainable synthesis of ammonia, nitrates, and urea has led to an increase in studies of catalytic conversion between nitrogen-containing compounds using heterogeneous catalysts. Density functional theory (DFT) is commonly employed to obtain molecular-scale insight into these reactions, but there have been relatively few assessments of the exchange-correlation functionals that are best suited for heterogeneous catalysis of nitrogen compounds. Here, we assess a range of functionals ranging from the generalized gradient approximation (GGA) to the random phase approximation (RPA) for the formation energies of gas-phase nitrogen species, the lattice constants of representative solids from several common classes of catalysts (metals, oxides, and metal-organic frameworks (MOFs)), and the adsorption energies of a range of nitrogen-containing intermediates on these materials. The results reveal that the choice of exchange-correlation functional and van der Waals correction can have a surprisingly large effect and that increasing the level of theory does not always improve the accuracy for nitrogen-containing compounds. This suggests that the selection of functionals should be carefully evaluated on the basis of the specific reaction and material being studied.
机构、总结、中文摘要均由AI分析而来，可能存在错误，请以论文正文为准。
