Identifying hydroxylated copper dimers in SSZ-13 via UV-vis-NIR spectroscopy
Identifying hydroxylated copper dimers in SSZ-13 via UV-vis-NIR spectroscopy
复制标题
通过紫外-可见-近红外光谱鉴定 SSZ-13 中的羟基化铜二聚体
DOI：
10.1039/d2cy00353h
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发表时间：
2022
影响因子：
5
通讯作者：
Mavrikakis, Manos
中科院分区：
文献类型：
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作者：
Göltl, Florian;Bhandari, Saurabh;Lebrón-Rodríguez, Edgard A.;Gold, Jake I.;Zones, Stacey I.;Hermans, Ive;Dumesic, James A.;Mavrikakis, Manos
铜交换沸石是一种很有前途的甲烷选择性转化为甲醇的材料。它们的活性归因于小的cu -氧和cu -羟基簇的存在，但各种沸石结构中活性中心的性质仍在争论中。在这篇论文中，我们结合时间依赖的密度泛函理论和自旋轨道耦合来预测SSZ-13中各种Cu单体和二聚体的光谱。我们进一步将理论结果与实验结果进行比较，发现Cu-羟基二聚体和Cu单体的存在可能解释实验观察到的UV-vis-NIR光谱。
Cu-Exchanged zeolites are promising materials for the selective conversion of methane to methanol. Their activity is attributed to the presence of small Cu-oxo and Cu-hydroxy clusters, but the nature of active centers in various zeolite structures is still under debate. In this contribution, we combine time dependent density functional theory with spin–orbit coupling to predict the optical spectra of various Cu monomers and dimers in SSZ-13. We furthermore compare theoretical results to experimental measurements and find that the presence of Cu-hydroxy dimers and Cu monomers could potentially explain the experimentally observed UV-vis-NIR spectra.