Computationally designed metal-free hydrogen activation site: Reaching the reactivity of metal - Ligand bifunctional hydrogenation catalysts

Inorganic Chemistry

Volumn 49, Issue 1, 2010, Pages 295-301

  Lu, Gang ^a   Li, Haixia ^a   Zhao, Lili ^a   Huang, Fang ^a   Wang, Zhi Xiang ^a  

^a UNIVERSITY OF CHINESE ACADEMY OF SCIENCES   (China)

Author keywords

[No Author keywords available]

Indexed keywords

EID: 73349130040     PISSN: 00201669     EISSN: None     Source Type: Journal    
DOI: 10.1021/ic902039g     Document Type: Article

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83. Our distortion energy is defined as the energy difference between a free molecule and the corresponding frozen moiety in the transition state. For 1, this is different from the approach proposed in ref 10c, the reported value (2.4 kcal/mol) is the difference between interaction energy of 1 and that of the frozen 1 moiety in the transition state. The authors used two set of reference monomers to calculate the two interaction energies. In our cases, 10-13 are not pairs (unlike 1, the acidic and basic centers are incorporated in the same molecule), we thus calculated the distortion energies as defined. Our value of 1 (6.2 kcal/mol) can be obtained via the same approach of ref 10c but using the same reference monomers.
84. (a) Hedberg, C.; Kallstrom, K.; Arvidsson, P. I; Brandt, P.; Andersson, P. G. J. Am. Chem. Soc. 2005, 127, 15083.
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86. For the Ru-containing model 14, the calculations were performed using the M05-2X functional in combination with the basis sets of 6-311++G for H, C, N, P and aug-cc-pVTZ for Ru.
87. Using the mPWlPW91 functional in combination with the SDD basis set for Ru and 6-311++G for H, N, C, and P, De Iuliis et al. predicted the activation free energy of model 14 to be 16.6 kcal/mol (see ref 11f); Hedberg et al. reported an activation free energy of 17.8 kcal/mol at. B3LYP+/ LACVP //B3LYP/LACVP level (see ref 20a); Chen et al. predicted the barrier to be 22.0 kcal/mol using B3LYP functional with 6-31+G for H, N, C, P and LANL2DZ for Ru (see ref 20b).