Theoretical analysis of cooperative effects of small molecule activation by frustrated Lewis pairs.
Theoretical analysis of cooperative effects of small molecule activation by frustrated Lewis pairs.
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受挫路易斯对小分子活化协同效应的理论分析。
DOI：
10.1039/c2dt30562c
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发表时间：
2012
影响因子：
4
通讯作者：
S. Grimme
中科院分区：
文献类型：
--
作者：
Christian Mück‐Lichtenfeld;S. Grimme
用色散校正DFT （TPSS-D3）计算了小分子(H(2), Br（2)和CO(2)）与硼/磷受挫刘易斯对（FLPs）的激活反应的能量谱。我们通过分析三元体系和反应物对的相互作用能，研究了反应的协同性质。对总相互作用能的非加性贡献增加了活化反应的驱动力，即使在过程的早期阶段也是如此。我们提出了多体变形密度Δρ(mb)的等值面表示，作为一种定性工具来可视化复杂化学系统中的合作，非加性效应。
The energy profiles of the activation reaction of small molecules (H(2), Br(2) and CO(2)) with boron/phosphorus frustrated Lewis pairs (FLPs) have been calculated with dispersion corrected DFT (TPSS-D3). We have investigated the cooperative nature of the reactions by analyzing interaction energies in the ternary system and for reactant pairs. The non-additive contributions to the total interaction energy add to the driving force of the activation reaction, even at early stages of the process. We propose the isosurface representation of the many-body deformation density Δρ(mb) as a qualitative tool to visualize cooperative, non-additive effects in complex chemical systems.