Adsorption of water and methanol on zeolite Bro/nsted acid sites: An ab initio, embedded cluster study including electron correlation
Adsorption of water and methanol on zeolite Bro/nsted acid sites: An ab initio, embedded cluster study including electron correlation
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水和甲醇在沸石布朗/恩斯台德酸性位点上的吸附：从头算、嵌入簇研究，包括电子关联
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发表时间：
1996
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影响因子：
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通讯作者：
P. Sherwood
中科院分区：
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作者：
S. P. Greatbanks;I. H. Hillier;N. Burton;P. Sherwood
嵌入式簇模型，采用一个点电荷场，以正确地考虑周围的晶格的静电效应，被用来研究水和甲醇在沸石Bro/nsted酸网站的吸附。点电荷场和电子相关的影响（在二阶Mo/ller-Plesset（MP2）和密度泛函理论（DFT）水平上研究）反映在预测的底物结构，结合能和1H NMR位移。两者都导致增强的底物结合，以产生与实验的良好一致性，以及质子转移到底物的程度增加，在甲醇的情况下效果特别明显。有一个建议，从测量的1H NMR位移的比较，这种效果是有点高估了这里使用的模型。
An embedded cluster model, employing a point charge field to correctly account for the electrostatic effect of the surrounding lattice, is used to study the adsorption of water and methanol at zeolite Bro/nsted acid sites. The effects of both the point charge field and electron correlation (studied at the second order Mo/ller–Plesset (MP2) and density functional theory (DFT) levels) are reflected in the predicted substrate structures, binding energies and 1H NMR shifts. Both result in enhanced substrate binding to yield good agreement with experiment, and an increased degree of proton transfer to the substrate, an effect particularly evident in the case of methanol. There is a suggestion from a comparison with measured 1H NMR shifts that this effect is somewhat overestimated by the model used here.