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Supporting Information for Solving the Density Functional Conundrum: Elimination of Systematic Errors to Derive Accurate Reaction Enthalpies of Complex rganic Reactions Arkajyoti Sengupta and Krishnan Raghavachari* Department of Chemistry, Indiana University, Bloomington, Indiana 47405 S1

Table of Contents Page No. Table S1 Table S2 Table S3 Table S4 Table S5 Table S6 Table S7 Computational Methods Calculated G4 reaction enthalpies of parent reactions (PR) R1 R25 and their corresponding CBH-1 and CBH-2 reaction schemes. Calculated deviations (in kcal mol -1 ) Dev-0 (G4 B3LYP) and CBH corrected deviations (Dev-1 and Dev-2 with CBH-1 and CBH-2 schemes respectively) in reaction energies of R1 R25 reactions obtained at B3LYP/6 311++G(3df,2p) level of theory. The mean absolute deviations (in kcal mol -1 ) MAD-0 and CBH corrected deviations (MAD-1 and MAD-2 with CBH-1 and CBH-2 corrections respectively) in reaction energies of R1 R25 reactions obtained at various DFT methods with 6 311++G(3df,2p) basis set. The mean absolute deviations (in kcal mol -1 ) MAD-0 and CBH corrected deviations (MAD-1 and MAD-2 with CBH-1 and CBH-2 corrections respectively) in reaction energies of R1 R25 reactions obtained at wave function-based methods with 6 311++G(3df,2p) basis set. The effect of basis set on mean absolute deviations of parent reactions and corrected deviations (in kcal mol -1 ) with M06-2X functional. CBH-1 and CBH 2 reaction schemes corresponding to the parent reactions R1 R25. Calculated deviations from G4 reaction energies of parent reactions (PR) and CBH-1 and CBH-2 reactions schemes of the reactions R1 R25. S3 S4 S5 S6 S7 S7 S8 S9 S10 S16 Table S8 Calculated Dev-0, Dev-1 and Dev-2 for reactions R1 R25. S17 S23 Cartesian coordinates of the reactants and products in the reactions R1 R25. The geoemtries were optimized at B3LYP/6-311+G(d,p). S24-S37 S2

Computational Methods Geometry optimizations of all species were carried out at B3LYP/6-311+G(d,p), and associated harmonic frequencies were scaled by a factor of 0.9854. Single point calculations were then performed with a range of density functionals including local density approximation (LDA) functional SVWN5, 1 pure GGA PBE, 2 meta-gga functional TPSS, 3 hybrid functionals B3LYP, 4,5 mpwpw91, 6 B3PW91, BMK, 7 TPPSh, 8 and PBE0 9 and M06-2X, 10 range-separated functionals: CAM-B3LYP 11 and ωb97xd, 12 and double hybrid functional B2PLYP. 13 As recommended, 14 we have used ultrafine grid for M06-2X calculations. Grimme s dispersion correction schemes with both zero and Becke-Johnson (BJ) damping were evaluated with B3LYP. Dispersion corrections with BJ damping were also applied on CAM-B3LYP, B2P-LYP and B2GP-PLYP. In addition to these DFT methods, error cancellation schemes were also assessed with wavefunction-based methods: HF, MP2, SCS-MP2 and CCSD(T). The DFT and WFT calculations were performed in conjunction with 6-311++G(3df,2p) basis-set using development version of Gaussian suite of programs. 15 CCSD(T) calculations were performed with a smaller 6-31+G(d,p) basis-set. Non-local and density dependent dispersion corrected revpbe NL and B3LYP NL methods were also evaluated with matching auxiliary basis sets def2-tzvp/c and def2-tzvp/jk using rca. 16 The quadrature grids for numerical integration of density functionals were increased to Grid6 in these calculations. For the NL approximation a larger grid (Vdwgrid4) was used as suggested by Calbo et al. 17 Calibration of the different methods were done against G4 for all the reactions except for R19, R20 and R22 wherein the G4 calculations were not tractable and hence CCSD(T)/cc-pVTZ with DLPN protocol were considered as the reference method. References (1) Vosko, S. H.; Wilk, L.; Nusair, M. Can. J. Phys. 1980, 58, 1200. (2) Perdew, J. P.; Burke, K.; Ernzerhof, M. Phys. Rev. Lett. 1996, 77, 3865. (3) Tao, J. M.; Perdew, J. P.; Staroverov, V. N.; Scuseria, G. E. Phys. Rev. Lett. 2003, 91. (4) Becke, A. D. J. Chem. Phys. 1997, 107, 8554. (5) Lee, C. T.; Yang, W. T.; Parr, R. G. Phys. Rev. B 1988, 37, 785. (6) Adamo, C.; Barone, V. J. Chem. Phys. 1998, 108, 664. (7) Boese, A. D.; Martin, J. M. L. The J. Chem. Phys. 2004, 121, 3405. (8) Staroverov, V. N.; Scuseria, G. E.; Tao, J. M.; Perdew, J. P. J. Chem. Phys. 2003, 119, 12129. (9) Adamo, C.; Barone, V. J. Chem. Phys. 1999, 110, 6158. (10) Zhao, Y.; Truhlar, D. Theor. Chem. Acc. 2008, 120, 215. (11) Yanai, T.; Tew, D. P.; Handy, N. C. Chem. Phys. Lett. 2004, 393, 51. (12) Chai, J. D.; Head-Gordon, M. Phys. Chem. Chem. Phys. 2008, 10, 6615. (13) Grimme, S. J. Chem. Phys. 2006, 124. S3

(14) Wheeler, S. E.; Houk, K. N. J. Chem. Theory Comput. 2010, 6, 395 404. (15) M. J. Frisch, G. W. Trucks, H. B. Schlegel, G. E. Scuseria, M. A. Robb, J. R. Cheeseman, G. Scalmani, V. Barone, B. Mennucci, G. A. Petersson, H. Nakatsuji, M. Caricato, X. Li, H. P. Hratchian, A. F. Izmaylov, J. Bloino, B. G. Janesko, F. Lipparini, G. Zheng, J. L. Sonnenberg, W. Liang, M. Hada, M. Ehara, K. Toyota, R. Fukuda, J. Hasegawa, M. Ishida, T. Nakajima, Y. Honda,. Kitao, H. Nakai, T. Vreven, J. A. Montgomery, Jr., J. E. Peralta, F. gliaro, M. Bearpark, J. J. Heyd, E. Brothers, K. N. Kudin, V. N. Staroverov, T. Keith, R. Kobayashi, J. Normand, K. Raghavachari, A. Rendell, J. C. Burant, S. S. Iyengar, J. Tomasi, M. Cossi, N. Rega, J. M. Millam, M. Klene, J. E. Knox, J. B. Cross, V. Bakken, C. Adamo, J. Jaramillo, R. Gomperts, R. E. Stratmann,. Yazyev, A. J. Austin, R. Cammi, C. Pomelli, J. W. chterski, R. L. Martin, K. Morokuma, V. G. Zakrzewski, G. A. Voth, P. Salvador, J. J. Dannenberg, S. Dapprich, P. V. Parandekar, N. J. Mayhall, A. D. Daniels,. Farkas, J. B. Foresman, J. V. rtiz, J. Cioslowski, and D. J. Fox, Gaussian, Inc., Wallingford CT, 2010. (16) Neese, F. WIREs: Comp. Mol. Sci. 2012, 2, 73. (17) Calbo, J.; rtí, E.; Sancho-García, J. C.; Aragó, J. J. Chem. Theory Comp. 2015, 11, 932. S4

Table S1. Calculated G4 reaction enthalpies of parent reactions (PR) R1 R25 and their corresponding CBH-1 and CBH-2 reaction schemes. Reaction PR CBH-1 CBH-2 R1 25.8 33.2 43.4 R2 30.2 43.0 58.6 R3 29.6 33.2 42.3 R4 31.8 33.2 42.3 R5 3.5 33.2 37.8 R6 0.3 10.8 27.7 R7 3.9 0.3 0.4 R8 18.8 16.9 16.7 R9 2.8 0.3 1.2 R10 29.7 7.7 13.1 R11 36.3 4.9 36.0 R12 19.0 33.2 39.0 R13 60.6 26.7 62.9 R14 22.6 7.8 23.2 R15 9.2 2.3 7.6 R16 14.3 8.9 21.6 R17 41.4 33.2 42.3 R18 9.6 5.9 16.8 R19 i 68.6 61.2 72.0 R20 i 15.6 16.6 23.1 R21 23.3 0.0 4.0 R22 i 0.5 12.3 17.8 R23 13.3 29.4 33.8 R24 16.7 22.5 16.2 R25 36.6 33.2 38.0 i The reaction enthalpies are calculated with CCSD(T)/cc-pVTZ instead of G4 method as discussed in Computational Methods. S5

Table S2. Calculated deviations (in kcal mol -1 ) Dev-0 (G4 B3LYP) and CBH corrected deviations (Dev-1 and Dev-2 with CBH-1 and CBH-2 schemes respectively) in reaction energies of R1 R25 reactions obtained at B3LYP/6 311++G(3df,2p) level of theory. Reaction Dev-0 Dev-1 Dev-2 R1 13.5 8.5 0.0 R2 11.1 8.1 1.4 R3 18.5 13.5 0.7 R4 18.7 13.7 0.8 R5 16.5 11.5 1.4 R6 12.7 9.7 1.0 R7 3.9 1.8 0.7 R8 8.7 4.1 0.7 R9 6.9 4.8 2.5 R10 6.2 2.7 0.5 R11 15.6 12.0 1.7 R12 28.1 23.1 1.5 R13 7.1 5.9 0.6 R14 1.9 3.8 1.5 R15 8.1 6.8 2.3 R16 3.0 2.3 1.3 R17 22.3 17.3 4.4 R18 3.2 2.6 3.2 R19 i 45.0 35.4 5.9 R20 i 9.6 7.1 0.6 R21 4.9 4.9 1.0 R22 i 15.2 12.0 2.9 R23 8.4 2.3 1.9 R24 6.1 4.2 0.0 R25 26.9 21.9 3.7 i The reaction enthalpies are calculated with CCSD(T)/cc-pVTZ instead of G4 method as discussed in Computational Methods. S6

Table S3. The mean absolute deviations (in kcal mol -1 ) MAD-0 and CBH corrected deviations (MAD-1 and MAD-2 with CBH-1 and CBH-2 respectively) in reaction energies of R1 R25 reactions obtained at various DFT methods with 6 311++G(3df,2p) basis set. Level of Theory MAD-0 MAD-1 MAD-2 LSDA SVWN5 10.0 6.9 3.6 GGA PBE 8.0 8.9 1.9 meta-gga TPSS 11.0 8.7 1.9 hybrid-gga B3LYP 12.9 9.6 1.7 CAM-B3LYP 7.1 7.9 1.9 B3PW91 7.6 8.7 1.6 MPW1PW91 5.5 8.4 1.4 PBE0 4.7 8.2 1.4 hybrid-meta-gga BMK 4.0 5.5 1.4 TPSSh 9.0 8.4 1.7 M06-2X 2.5 4.6 2.2 Dispersion corrected ωb97xd 2.2 4.8 1.6 B3LYP-D3 7.7 6.4 2.1 B3LYP-D3BJ 6.3 5.3 1.3 CAM-B3LYP-D3BJ 3.9 5.3 1.6 B97-D3BJ 8.5 5.4 1.6 B3LYP-NL 4.6 4.8 1.5 rev-pbe-nl 3.1 3.6 1.7 Double hybrid B2PLYP 6.9 5.6 1.1 B2PLYP-D3BJ 3.7 3.4 1.0 B2GPPLYP-D3BJ 8.3 1.5 1.6 MPW2PLYP 5.7 5.7 1.4 S7

Table S4. The mean absolute deviations (in kcal mol -1 ) MAD-0 and CBH corrected deviations (MAD-1 and MAD-2 with CBH-1 and CBH-2 schemes respectively) in reaction energies of R1 R25 reactions obtained at wave function-based methods with 6 311++G(3df,2p) basis set. Level of Theory MAD-0 MAD-1 MAD-2 HF 13.3 9.5 2.1 MP2 4.0 2.4 1.3 SCS-MP2 1.8 1.1 1.1 CCSD(T) i 0.9 0.6 0.5 i CCSD(T)/6-311++G(3df,2p) energies were obtained by extrapolation: CCSD(T)/6-311++G(3df,2p) = MP2/6-311++G(3df,2p) + CCSD(T)/6-31+G(d,p) MP2/6-31+G(d,p) Table S5. The effect of basis set on mean absolute deviations of parent reactions and corrected deviations (in kcal mol -1 ) with M06-2X functional. Level of Theory Dev-0 Dev-1 Dev-2 6-311++G(3df,2p) 2.5 4.6 2.2 aug-cc-pvdz 2.5 4.5 2.6 6-31G(d) 5.0 5.9 2.6 S8

Table S6. CBH-1 and CBH 2 reaction schemes corresponding to the parent reactions R1 R25. Reaction CBH-1 CBH-2 Reactants Products Reactants Products R1 4 CH 4 + 2 CH 2 =CH 2 4 CH 3 CH 3 2 CH 3 CH=CH 2 + 4 CH 3 CH 3 2 CH 3 CH 2 CH 3 + 2 CH 3 CH(CH 3 ) 2 R2 4 CH 4 + CH CH 3 CH 3 CH 3 HC CH + 3 CH 3 CH 3 2 CH 3 CH(CH 3 ) 2 R3 4 CH 4 + 2 CH 2 =CH 2 4 CH 3 CH 3 4 CH 3 CH=CH 2 + 4 CH 3 CH 3 4 CH 3 CH(CH 3 ) 2 + 2 CH 2 =CH 2 R4 4 CH 4 + 2 CH 2 =CH 2 4 CH 3 CH 3 4 CH 3 CH=CH 2 + 4 CH 3 CH 3 4 CH 3 CH(CH 3 ) 2 + 2 CH 2 =CH 2 R5 4 CH 4 + 2 CH 2 =CH 2 4 CH 3 CH 3 CH 3 CH=CH 2 +3 CH 2 =CHH + 4 CH 3 CH 3 3 CH 3 CH(H)CH 3 + CH 3 CH(CH 3 ) 2 + 2 CH 2 =CH 2 3 CH R6 4 + CH 2 =CH 2 2 CH 2 =CHH + 2 CH 3 CH 3 + CH 3 CH 3 + CH 2 =CH 2 + 2 CH + HCH + H 2 3 CH 3 +2 CH 3 H 2 CH 3 H + CH 3 CH 2 CH 3 CH(H)CH 3 +CH 3 CH(H) 2 R7 CH 4 + HCH H 2 + CH 2 =CH 2 CH 3 CH + CH 2 =CH 2 + CH 3 CH 3 2 CH 3 CH=CH 2 + H 2 CH 3 C(=)CH 3 +4 CH 3 CH 3 CH 2 =C(CH 3 ) 2 + 3 CH 3 CH 2 CH 3 R8 3 CH 4 + HCH H 2 + 2 CH 3 CH 3 + CH 2 =CH 2 + H 2 CH 3 CH 2 CH 3 + CH 2 =CH 2 R9 CH 4 + HCH H 2 + CH 2 =CH 2 2 CH 2 =C(CH 3 ) 2 + H 2 + CH 3 C(=)CH 3 CH 3 CH=CH 2 + (CH 3 ) 2 C=NH 2 CH 3 C(=)CH 3 + CH 3 NHNH 2 + CH R10 3 CH 3 + 2 HCH CH 3 NH 2 + 2 H 2 + CH 2 =NNH 2 + NH 2 N(CH 3 ) 2 + CH + 2 NH 3 + CH 2 =CH 2 + CH 2 =NH 3 NH 2 + CH 3 CH 2 CH 3 + CH 3 CH 3 + 2 H 2 + H 2 C=NH + NH 2 NH 2 CH 2 =C(NH 2 )(CH 3 ) R11 4 CH 4 + 2 HCH + CH 2 =CH 2 + 2 H 2 4 CH 3 H + 2 CH 3 CH 3 2 CH 3 CH + 4 CH 3 H + 2 CH 3 CH 3 + CH 2 =CH 2 2 CH 3 CH 3 + CH 3 CH(H) 2 + CH 3 CH(H)CH 3 + CH 3 CH 2 H + CH 3 CH 2 CH 3 R12 2 CH 2 =CH 2 + 4 CH 4 4 CH 3 CH 3 4 CH 2 =C(CH 3 ) 2 + 4 CH 3 CH 3 4 C(CH 3 ) 4 + 2 CH 2 =CH 2 R13 6 CH 4 + HC CH + C 4 CH 3 CH 3 + HCH HC CH + C + 4 CH 3 CH 3 CH 3 C(=)CH 3 + 2 CH 3 CH(CH 3 ) 2 S9

Reaction CBH-1 CBH-2 Reactants Products Reactants Products R14 CH 4 + H 2 + HN= NH 2 H + CH 3 H HN= + CH 3 H + CH 3 CH 2 CH 3 CH 3 CH(H)CH 3 + CH 3 NH 2 R15 CH 4 + CH 2 =NH CH 3 NH 2 + CH 3 CH=NH CH 3 CH(CH 3 ) 2 + (CH 3 ) 2 NH + 2 CH 3 NH 2 + NH 3 CH 3 CH 3 + CH 3 CH 2 CH 3 CH 3 CH 2 NH 2 R16 HN C + 2 CH 4 CH 2 =NH + CH 3 CH 3 CH 3 CCl + CH 3 N C + CH 3 CH 3 + HN=CH 2 CH 3 N=CH 2 + CH 3 (Cl)C=NH + CH 3 C(=)CH 3 R17 4 CH 3 CH 3 4 CH 4 + 2 CH 2 =CH 2 4 CH 3 CH(CH 3 ) 2 +2 CH 2 =CH 2 4 CH 3 CH=CH 2 + 4 CH 3 CH 3 R18 2 CH 3 H CH 4 + HCH + H 2 CH 3 CH 3 + HCH CH 3 CH + CH 3 H R19 7 CH 3 CH 3 + H 2 CH 3 H + 3 CH 2 =CH 2 + 7 CH 4 CH 3 CH(H)CH 3 + CH 3 CH 2 CH 3 + 3 CH 2 =CH 2 + 4 C(CH 3 ) 4 + 6 CH 3 CH 3 + 2 CH 2 =C(CH 3 ) 2 + 3 CH 3 CH(CH 3 ) 2 + 2 CH 3 H 4 CH 3 CH=CH 2 + CH 3 CH 3 R20 2 CH 3 CH 3 2 CH 4 + CH 2 =CH 2 C(CH 3 ) 4 + CH 3 CH(CH 3 ) 2 CH 3 CH 3 +CH 2 =C(CH 3 ) 2 + CH 3 CH 2 CH 3 R21 CH 3 CH 3 CH 3 CH 3 2 C(CH 3 ) 4 + CH 3 CH 3 3 CH 3 CH(CH 3 ) 2 R22 2 CH 3 CH 3 + CH 2 =NH + CH 3 H 2 CH 4 + CH 2 =CH 2 + CH 3 NH 2 + HCH R23 6 CH 2 =CH 2 3 CH CH + 3 CH 3 CH 3 R24 CH 2 =CH 2 + CH 4 + 2 CH 3 H H 2 + 2 CH 3 CH 3 + HCH R25 4 CH 4 + 2 CH 2 =CH 2 4 CH 3 CH 3 (CH 3 ) 2 C=NH + CH 3 CH 2 CH 3 + (CH 3 ) 3 CF + (CH 3 ) 3 CH + CH 3 N=CH 2 + CH 3 NH 2 + CH 2 =CH 2 3 HC CH + 3 CH 3 CH 3 + 5 CH 2 =C=CH 2 CH 2 =C(H)CH 3 + CH 3 CH 2 H + 2 CH 3 CH=CH 2 + 2 CH 3 CH 3 + CH 3 CH 3 2 CH 2 =C(CH 3 ) 2 + 3 CH 3 CH=CH 2 + 5 CH 3 CH 3 CH 3 CH(F)CH 3 + CH 3 C(=)CH 3 + CH 3 CH=CH 2 + 2 CH 3 CH 3 + CH 2 =C(NH 2 )(CH 3 ) + (CH 3 ) 2 NH + H 2 C=NH 6 CH 2 =CH 2 + 5 CH CCH3 2 CH 3 CH(CH 3 ) 2 + CH 3 C(=)CH 3 + 2 CH 2 =CH 2 + 2CH 3 H 2 C(CH 3 ) 4 + 2 CH 3 CH(CH 3 ) 2 + CH 3 CH 2 CH 3 + 3 CH 2 =CH 2 S10

Table S7. Calculated Dev-0, Corr-1 and Corr-2 defined as deviations from G4 reaction energies of parent reactions (PR), CBH-1 and CBH-2 reactions schemes for the reactions R1 R25 R1 R2 R3 R4 PR CBH-1 CBH-2 PR CBH-1 CBH-2 PR CBH-1 CBH-2 PR CBH-1 CBH-2 SVWN5 12.6 20.4 18.0 15.0 21.7 22.2 8.9 20.4 14.8 8.8 20.4 14.8 PBE -4.4 2.9-4.6-1.0 4.8-0.3-9.8 2.9-9.0-9.9 2.9-9.0 TPSS -8.3-2.5-11.7-4.1 0.1-7.1-14.1-2.5-16.3-14.3-2.5-16.3 B3LYP -13.5-5.0-13.5-11.1-3.0-9.7-18.5-5.0-17.9-18.7-5.0-17.9 CAM-B3LYP -6.2 1.4-4.9-5.2 2.4-2.5-9.6 1.4-8.2-10.0 1.4-8.2 B3PW91-4.5 2.5-6.4-1.9 4.1-2.5-9.6 2.5-11.1-9.7 2.5-11.1 MPW1PW91-0.9 6.1-1.7 1.5 7.7 2.0-5.5 6.1-5.9-5.6 6.1-5.9 PBE0 1.6 8.7 1.6 3.7 10.1 5.1-2.9 8.7-2.3-3.0 8.7-2.3 BMK 1.0 5.0-0.3 2.0 5.9 1.7-2.0 5.0-2.8-2.1 5.0-2.8 TPSSh -5.7 0.2-8.7-2.0 2.5-4.5-11.1 0.2-13.1-11.2 0.2-13.1 M06-2X -0.7 4.3 1.8-2.0 3.5 1.7-2.5 4.3 0.5-2.6 4.3 0.5 ωb97xd 0.4 6.1 2.6 0.6 6.9 4.1-1.2 6.1 0.6-1.2 6.1 0.6 B3LYP-D3-9.3-2.0-6.1-8.4-0.2-3.4-11.9-2.0-8.3-11.8-2.0-8.3 B3LYP-D3BJ -7.4-1.2-5.4-5.6 0.9-1.9-9.2-1.2-7.9-9.2-1.2-7.9 CAM-B3LYP-D3BJ -3.3 3.0-0.9-2.6 4.1 1.3-4.6 3.0-3.3-4.7 3.0-3.3 B97-D3BJ -10.0-4.3-8.7-7.1-1.8-4.6-12.3-4.3-11.5-12.3-4.3-11.5 B3LYP-NL a -4.5 1.6-2.2-2.9 3.7 1.0-6.7 1.6-4.6-6.6 1.6-4.6 rev-pbe-nl a 2.6 5.9 2.4 5.2 7.9 5.9 0.1 5.9-0.1 0.3 5.9-0.1 B2PLYP -6.7-1.7-6.4-6.3-1.9-5.5-9.8-1.7-8.9-9.9-1.7-8.9 B2PLYP-D3-3.8 0.0-2.6-3.7-0.2-1.9-5.2 0.0-4.3-5.2 0.0-4.3 B2GPPLYP-D3-10.3-11.7-9.7-11.0-12.6-11.0-10.3-11.7-9.1-10.3-11.7-9.1 MPW2PLYP -5.1 0.4-3.9-4.8 0.4-2.8-8.0 0.4-6.2-8.1 0.4-6.2 HF -12.4-5.0-13.6-13.0-3.1-11.3-15.5-5.0-16.9-15.5-5.0-16.9 MP2 5.9 4.3 5.6 3.6 0.7 2.5 5.8 4.3 5.7 6.0 4.3 5.7 SCS-MP2 1.7 1.1 0.4-0.1-1.6-2.1 1.1 1.1 0.1 1.1 1.1 0.1 CCSD(T) 0.9 0.1 0.7 1.2 0.5 0.9 1.2 0.1 1.1 1.1 0.1 1.1 a with def2-tzvpp basis-set S11

R5 R6 R7 R8 PR CBH-1 CBH-2 PR CBH-1 CBH-2 PR CBH-1 CBH-2 PR CBH-1 CBH-2 SVWN5 3.7 20.4 8.0 12.3 21.8 15.0 1.2 0.9 1.2 7.3 11.1 9.9 PBE -10.3 2.9-12.5-5.5 3.0-8.5-2.8-2.0-2.5-3.9-0.5-4.3 TPSS -12.8-2.5-17.8-7.2-0.1-12.7-7.0-6.3-7.0-10.5-7.5-12.1 B3LYP -16.5-5.0-17.9-12.7-3.1-13.7-3.9-2.1-3.2-8.7-4.6-9.4 CAM-B3LYP -9.3 1.4-8.4-5.7 3.1-4.6-4.3-1.8-2.9-5.6-1.1-5.3 B3PW91-9.7 2.5-13.1-5.8 2.8-9.4-3.3-1.8-2.5-3.4-0.6-5.2 MPW1PW91-6.0 6.1-8.0-2.4 6.3-4.7-3.1-1.5-2.2-1.6 1.5-2.6 PBE0-4.0 8.7-4.9-0.3 8.5-1.7-2.8-1.3-1.9-0.3 3.1-0.7 BMK -5.7 5.0-6.2-3.5 3.9-4.6-5.6-3.7-4.5-4.5-1.2-4.7 TPSSh -10.2 0.2-14.3-5.2 2.2-9.7-6.6-5.5-6.3-8.4-5.4-9.9 M06-2X -4.6 4.3-1.8-0.5 6.6 2.0-2.4-0.9-1.1-1.9 1.3-0.2 ωb97xd -3.4 6.1-2.8-2.3 5.4-2.1-3.6-1.8-2.4-1.8 1.3-1.0 B3LYP-D3-10.8-2.0-9.4-8.7-0.5-7.1-2.8-1.9-2.7-6.7-2.9-5.7 B3LYP-D3BJ -8.5-1.2-9.4-7.0 0.0-7.0-2.0-1.6-2.0-4.5-2.2-4.5 CAM-B3LYP-D3BJ -5.1 3.0-4.1-2.8 4.4-1.4-3.1-1.6-2.3-3.4-0.1-2.8 B97-D3BJ -11.8-4.3-14.9-10.0-4.1-12.9-2.1-2.4-2.4-5.9-4.5-6.3 B3LYP-NL a -6.2 1.6-6.4-3.6 2.9-2.7-2.5-2.0-2.5-3.7-1.1-3.4 rev-pbe-nl a -1.2 5.9-5.3 1.3 4.9-2.6-2.6-3.0-3.0-0.7 0.0-1.3 B2PLYP -10.0-1.7-9.6-7.9-1.4-7.8-3.1-2.1-2.6-5.2-2.9-5.6 B2PLYP-D3-6.1 0.0-5.6-5.1-0.1-4.7-2.1-1.9-2.0-3.1-1.9-3.3 B2GPPLYP-D3-8.1-11.7-9.2-9.8-11.8-10.1-3.7-2.9-2.9-9.0-8.7-7.5 MPW2PLYP -8.1 0.4-6.7-6.0 0.9-4.7-3.0-1.8-2.5-4.4-1.6-4.2 HF -7.6-5.0-13.2-9.5-3.6-11.4-8.4-3.6-5.7-10.8-6.1-12.2 MP2-0.6 4.3 3.4 0.2 2.0 1.8-0.2-1.2-0.3 2.7 1.0 2.6 SCS-MP2-0.1 1.1-0.3-1.9-0.5-2.0-2.8-2.7-2.3-1.5-2.2-1.8 CCSD(T) 2.2 0.1 1.0 1.3 0.2 0.8-1.2-0.8-0.7-0.7-0.7-0.4 a with def2-tzvpp basis-set S12

R9 R10 R11 R12 PR CBH-1 CBH-2 PR CBH-1 CBH-2 PR CBH-1 CBH-2 PR CBH-1 CBH-2 SVWN5 1.8 0.9 1.6 0.0 0.2 8.7 28.3 33.5 33.9 4.1 20.4 10.1 PBE -4.4-2.0-3.1-4.1-3.6-1.4-6.1 4.6-3.7-18.3 2.9-17.1 TPSS -8.6-6.3-7.9-7.6-7.9-8.2-11.2 1.0-10.4-22.9-2.5-24.6 B3LYP -6.9-2.1-4.4-6.2-3.5-5.7-15.6-3.6-14.0-28.1-5.0-26.5 CAM-B3LYP -6.9-1.8-4.2-6.7-3.3-5.6-4.0 5.6-1.7-17.8 1.4-14.9 B3PW91-6.0-1.8-3.5-2.8-3.4-4.1-6.7 4.4-6.2-20.4 2.5-20.0 MPW1PW91-5.6-1.5-3.1-3.4-3.2-3.9-1.1 9.5 0.3-15.6 6.1-14.1 PBE0-4.9-1.3-2.6-3.3-2.9-2.8 2.7 12.8 4.7-12.1 8.7-9.9 BMK -8.0-3.7-5.6-6.8-6.6-7.5-2.6 5.4-1.1-6.0 5.0-8.7 TPSSh -8.4-5.5-7.2-6.8-7.1-8.1-7.4 4.4-6.7-20.1 0.2-21.2 M06-2X -3.3-0.9-1.5-4.2-1.1-1.2 4.7 11.1 7.9-3.8 4.3-2.1 ωb97xd -4.5-1.8-3.2-5.8-3.6-4.9 0.1 7.7 1.9-1.7 6.1-2.0 B3LYP-D3-4.5-1.9-3.7-8.1-3.5-4.4-8.8 0.0-6.1-14.0-2.0-12.5 B3LYP-D3BJ -2.7-1.6-2.4-6.1-3.0-2.8-7.4 0.6-5.4-13.1-1.2-12.8 CAM-B3LYP-D3BJ -4.3-1.6-3.1-6.4-3.1-4.2 0.2 7.4 2.4-9.5 3.0-8.2 B97-D3BJ -2.3-2.4-2.6-5.8-3.8-1.5-14.5-6.0-12.7-15.7-4.3-16.3 B3LYP-NL a -2.9-2.0-3.0-5.7-3.1-2.2-0.9 5.0 1.5-9.8 1.6-9.2 rev-pbe-nl a -1.6-3.0-2.9-3.9-4.7-0.3 2.3 6.9 3.8-2.3 5.9-4.4 B2PLYP -4.6-2.1-3.2-3.3-3.8-4.2-8.8-2.0-7.6-15.5-1.7-14.1 B2PLYP-D3-2.4-1.9-2.2-3.1-3.6-2.8-4.9-0.2-3.7-8.3 0.0-7.7 B2GPPLYP-D3-3.1-2.9-2.8-7.0-4.5-3.8-18.2-17.7-15.8-8.1-11.7-7.2 MPW2PLYP -4.4-1.8-3.0-4.2-3.5-4.1-5.4 1.6-3.4-13.5 0.4-11.0 HF -13.3-3.6-7.9-15.5-5.9-16.1-16.9-4.6-16.2-27.1-5.0-25.0 MP2 0.5-1.2 0.6 6.7-2.9 1.0 3.6 1.8 3.6 5.7 4.3 6.0 SCS-MP2-2.8-2.7-2.0-0.2-4.4-3.8-2.8-1.5-2.9-0.4 1.1-0.7 CCSD(T) -0.7-0.8-0.6-1.6-1.3-1.5 0.6 0.4 0.8 0.8 0.1 1.5 a with def2-tzvpp basis-set S13

R13 R14 R15 R16 PR CBH-1 CBH-2 PR CBH-1 CBH-2 PR CBH-1 CBH-2 PR CBH-1 CBH-2 SVWN5 39.7 39.8 44.5 15.8 14.7 16.2 10.2 12.1 10.9 15.9 13.8 18.3 PBE 8.9 12.4 8.6-0.1 2.8 1.2-4.0 1.8-2.1 3.8 4.6 4.7 TPSS -0.3 4.4-3.4-2.7 1.3-1.5-6.8-0.4-5.2-0.5 1.5-0.6 B3LYP -7.1-1.2-7.7-1.9 2.0-0.4-8.1-1.3-5.8-3.0-0.7-1.6 CAM-B3LYP -0.2 5.2 1.2 2.2 5.0 3.4-3.3 2.0-1.5-1.3 0.7 0.9 B3PW91 4.7 9.1 3.0-0.5 3.5 0.9-4.9 1.9-2.9 0.2 2.7 2.0 MPW1PW91 9.5 13.9 8.8 1.6 5.2 2.8-2.4 3.7-0.5 1.8 4.2 3.8 PBE0 13.3 17.6 13.4 2.8 5.9 3.9-0.7 4.8 1.0 3.4 5.4 5.5 BMK 3.4 7.1 3.3 3.8 6.2 4.4-2.1 2.1-0.7-3.4-1.2-2.1 TPSSh 2.1 7.0-0.5-1.3 2.6-0.2-5.3 0.9-3.7-0.4 2.0 0.2 M06-2X 0.6 5.1 3.8 4.9 6.3 5.2 1.4 3.6 2.2-1.1-0.1 0.5 ωb97xd 7.2 11.0 8.6 1.7 4.2 2.5 0.6 3.4 1.3 0.8 2.4 2.2 B3LYP-D3-1.3 2.7 0.1 0.8 2.9 1.6-3.3-0.1-2.5 0.2 0.4 0.5 B3LYP-D3BJ 1.7 4.4 2.4 1.1 3.1 1.8-2.7 0.3-2.0 1.2 1.1 1.4 CAM-B3LYP-D3BJ 4.2 7.6 6.0 3.8 5.4 4.4-0.4 2.7 0.3 0.9 1.4 2.4 B97-D3BJ -0.5 1.4-0.6-3.1-0.7-2.2-5.0-1.7-4.1 0.9 0.5 0.5 B3LYP-NL a 5.2 8.2 6.3 3.2 4.3 3.5-0.6 1.6-0.3 2.1 2.1 2.7 rev-pbe-nl a 15.5 15.8 14.7 1.3 2.3 1.6 0.7 2.4 0.8 6.1 5.3 6.0 B2PLYP -4.3-1.2-4.4-0.6 1.4 0.2-4.3-0.4-3.0-1.8-0.9-1.2 B2PLYP-D3-0.2 1.2 0.3 0.8 1.8 1.2-1.7 0.3-1.2 0.2-0.1 0.3 B2GPPLYP-D3-21.3-20.4-18.8-6.7-7.0-6.1-6.4-6.4-5.4-6.7-8.2-7.1 MPW2PLYP -1.6 1.9-0.8 1.1 2.8 1.8-2.9 0.8-1.6-0.9 0.0 0.0 HF -19.9-11.2-20.7-3.9 1.2-2.6-8.7-1.4-6.3-13.1-7.3-9.6 MP2 3.4 1.2 3.8 2.4 1.4 2.2 2.3 1.6 2.2 1.2 0.0 0.8 SCS-MP2-4.2-2.8-4.0-0.7-0.2-0.7-0.8 0.0-0.4-1.8-1.5-2.2 CCSD(T) -1.0 0.2 0.4 0.5 0.0 0.2 0.5 0.0 0.3 0.3-0.1-0.1 a with def2-tzvpp basis-set S14

R17 R18 R19 R20 PR CBH-1 CBH-2 PR CBH-1 CBH-2 PR CBH-1 CBH-2 PR CBH-1 CBH-2 SVWN5-7.5-20.4-14.8-3.6-11.6-2.0-18.7-30.3-17.2-5.9-10.2-7.7 PBE 13.7-2.9 9.0 3.2-1.5-1.1 28.7-3.4 23.7 5.2-1.5 5.3 TPSS 19.3 2.5 16.3 3.9-1.1 2.6 40.4 8.0 38.5 8.2 1.2 9.2 B3LYP 22.3 5.0 17.9 3.2 0.6 0.0 45.0 9.6 39.1 9.6 2.5 10.2 CAM-B3LYP 12.5-1.4 8.2 0.2-2.5 0.0 26.0-0.3 22.3 4.3-0.7 5.1 B3PW91 13.2-2.5 11.1 0.9-1.6-1.1 28.6-2.7 27.7 5.0-1.2 6.6 MPW1PW91 9.0-6.1 5.9-0.4-3.2-1.1 20.2-8.3 18.9 2.9-3.1 4.0 PBE0 6.3-8.7 2.3-0.9-4.2-1.3 14.6-12.4 12.4 1.5-4.3 2.1 BMK 5.3-5.0 2.8 0.0-1.5 0.2 8.7-6.1 12.4 0.7-2.5 2.3 TPSSh 15.9-0.2 13.1 2.3-2.1 2.1 33.9 3.5 32.8 6.5-0.1 7.6 M06-2X 3.6-4.3-0.5-1.1-4.5 1.0 3.5-4.9 3.6-0.5-2.2 0.1 ωb97xd 2.3-6.1-0.6 1.1-2.3-0.7-0.7-8.7 2.5-2.0-3.1 0.0 B3LYP-D3 13.2 2.0 8.3 3.4-0.5 0.3 21.4 4.6 19.4 5.1 1.0 4.8 B3LYP-D3BJ 10.9 1.2 7.9 3.2-0.6 0.1 15.7 3.3 18.4 3.8 0.6 4.5 CAM-B3LYP-D3BJ 6.2-3.0 3.3 0.1-2.9 0.0 9.7-2.9 12.0 1.0-1.5 2.3 B97-D3BJ 14.2 4.3 11.5 6.5 2.0-0.1 22.3 7.7 23.2 5.6 2.1 6.1 B3LYP-NL 7.0-1.6 4.6 1.1-2.1 0.4 8.6-0.8 14.2 1.6-0.8 2.9 rev-pbe-nl 0.2-5.9 0.1 2.1-1.9-0.2-3.7-7.9 5.8-1.9-3.0 0.3 B2PLYP 12.0 1.7 8.9 2.4 0.6-0.1 21.4 3.7 20.5 4.3 0.8 5.2 B2PLYP-D3 6.4 0.0 4.3 2.3 0.1 0.0 7.3 0.9 10.7 1.4 0.0 2.5 B2GPPLYP-D3 11.6 11.7 9.1 7.2 6.0 1.6 14.7 18.9 13.5 3.5 5.8 4.3 MPW2PLYP 10.3-0.4 6.2 1.4-0.7 0.0 18.0 0.5 16.1 3.4-0.2 3.8 HF 19.5 5.0 16.9-1.3 1.1 1.0 43.7 10.1 38.4 8.7 2.5 10.3 MP2-5.9-4.3-5.7 0.3 0.2-0.5-19.4-7.0-10.7-5.2-2.2-3.2 SCS-MP2-0.2-1.1-0.1 1.1 1.0 0.7-5.7-1.0 0.7-2.1-0.5 0.1 CCSD(T) -0.7-0.1-1.1 0.5-0.1 0.6 -i- -i- -i- -i- -i- -ia with def2-tzvpp basis-set -i- Calculations with the large basis-set could not be performed due to their size. S15

R21 R22 R23 R24 PR CBH-1 CBH-2 PR CBH-1 CBH-2 PR CBH-1 CBH-2 PR CBH-1 CBH-2 SVWN5 0.7 0.0 0.7-0.2-9.6-4.2-13.9-4.0-20.0-6.4-1.4-7.2 PBE 5.3 0.0 3.1 11.7-0.4 8.6-13.3-5.5-16.7-4.7-0.1-5.5 TPSS 7.0 0.0 3.6 14.2 2.2 11.6-12.4-7.6-13.1-6.7-2.3-7.2 B3LYP 4.9 0.0 3.9 15.2 3.2 12.3-8.4-6.1-10.3-6.1-1.9-6.1 CAM-B3LYP 3.3 0.0 3.0 8.8 0.1 7.0-2.8-3.2-7.2-4.9-1.8-4.9 B3PW91 5.0 0.0 3.6 11.0-0.2 9.7-8.4-4.8-11.3-4.8-0.3-5.3 MPW1PW91 4.4 0.0 3.3 8.3-1.9 7.1-7.4-4.7-10.1-4.3-0.1-4.7 PBE0 4.1 0.0 3.0 6.7-3.2 5.3-7.5-4.5-10.6-3.9 0.1-4.3 BMK 4.8 0.0 2.8 6.9-0.6 5.8-4.2-2.7-8.6-0.6 1.0-1.9 TPSSh 6.6 0.0 3.5 12.2 0.9 10.1-10.2-7.0-11.1-6.2-2.0-6.5 M06-2X 1.5 0.0 1.0 2.2-2.1 1.4-1.2 2.6-6.9-3.0-2.3-3.8 ωb97xd 2.8 0.0 1.1 3.4-1.5 3.8-2.7-2.4-8.0-0.3 0.8-0.9 B3LYP-D3 2.4 0.0 2.0 9.7 1.7 7.1-8.4-5.3-10.9-3.4-1.5-3.2 B3LYP-D3BJ 1.7 0.0 1.8 9.0 1.4 7.0-8.6-6.5-10.5-3.2-1.2-3.4 CAM-B3LYP-D3BJ 1.7 0.0 2.0 5.1-0.7 4.4-2.9-3.3-7.4-3.4-1.4-3.5 B97-D3BJ 1.9 0.0 1.7 12.5 3.2 9.6-13.0-7.5-14.3-2.1-0.2-2.9 B3LYP-NL 1.3 0.0 1.9 6.1-0.2 4.9-8.6-6.3-10.9-4.3-1.3-4.5 rev-pbe-nl 2.2 0.0 1.3 3.6-1.8 3.7-13.3-5.9-16.8-2.1 1.0-3.3 B2PLYP 2.7 0.0 2.1 9.4 1.9 7.0-2.2 0.6-3.4-2.6-0.2-2.9 B2PLYP-D3 1.1 0.0 1.1 6.3 1.1 4.5-2.3 0.4-3.6-1.3 0.1-1.7 B2GPPLYP-D3 1.4 0.0-0.5 5.4 6.6 4.3-1.9 2.7-5.7 1.0 0.1 0.8 MPW2PLYP 2.3 0.0 2.0 8.1 0.8 5.5-1.7 0.0-3.1-2.8-0.4-2.9 HF 3.6 0.0 4.6 10.4 3.9 12.2 7.2-5.9 7.2-3.1-1.5-2.8 MP2-0.9 0.0-0.9-1.5-0.6-1.5 8.8 10.9 5.4 2.4 2.3 1.5 SCS-MP2 0.4 0.0 0.2-0.3 0.9 1.2 8.9 8.0 5.9 2.0 1.6 1.0 CCSD(T) 0.2 0.0-0.2 -i- -i- -i- -0.7-1.2-0.2 0.5-0.1 0.4 S16

R25 PR CBH-1 CBH-2 SVWN5 6.3 20.4 11.0 PBE -17.8 2.9-14.3 TPSS -22.8-2.5-21.4 B3LYP -26.9-5.0-23.2 CAM-B3LYP -16.4 1.4-12.3 B3PW91-17.8 2.5-16.7 MPW1PW91-13.3 6.1-11.0 PBE0-10.2 8.7-7.2 BMK -7.1 5.0-6.4 TPSSh -19.4 0.2-18.2 M06-2X -4.3 4.3-1.1 ωb97xd -2.8 6.1-1.0 B3LYP-D3-15.2-2.0-10.9 B3LYP-D3BJ -12.8-1.2-11.0 CAM-B3LYP-D3BJ -8.9 3.0-6.2 B97-D3BJ -16.1-4.3-14.7 B3LYP-NL -8.9 1.6-7.4 rev-pbe-nl -1.9 5.9-3.1 B2PLYP -14.7-1.7-12.1 B2PLYP-D3-8.0 0.0-6.5 B2GPPLYP-D3-11.3-11.7-8.0 MPW2PLYP -12.8 0.4-9.2 HF -25.0-5.0-21.1 MP2 4.9 4.3 5.5 SCS-MP2-0.5 1.1-0.5 CCSD(T) -0.7 0.1 1.4 S17

Table S8. Calculated Dev-0, Dev-1 and Dev-2 for reactions R1 R25. Dev-1= Dev-0 Corr-1. Dev-2= Dev-0 Corr-2. PR=Parent Reaction R1 R2 R3 R4 Dev-0 Dev-1 Dev-2 Dev-0 Dev-1 Dev-2 Dev-0 Dev-1 Dev-2 Dev-0 Dev-1 Dev-2 SVWN5 12.6-7.8-5.4 15.0-6.7-7.2 8.9-11.5-5.9 8.8-11.5-5.9 PBE -4.4-7.3 0.2-1.0-5.8-0.7-9.8-12.7-0.8-9.9-12.9-0.9 TPSS -8.3-5.9 3.4-4.1-4.2 3.1-14.1-11.7 2.2-14.3-11.8 2.0 B3LYP -13.5-8.5 0.0-11.1-8.1-1.4-18.5-13.5-0.7-18.7-13.7-0.8 CAM-B3LYP -6.2-7.6-1.3-5.2-7.6-2.7-9.6-11.0-1.5-10.0-11.3-1.8 B3PW91-4.5-7.0 1.9-1.9-5.9 0.6-9.6-12.0 1.5-9.7-12.2 1.4 MPW1PW91-0.9-7.0 0.8 1.5-6.3-0.5-5.5-11.6 0.5-5.6-11.7 0.3 PBE0 1.6-7.1-0.1 3.7-6.5-1.4-2.9-11.6-0.6-3.0-11.7-0.7 BMK 1.0-4.0 1.3 2.0-3.8 0.3-2.0-6.9 0.8-2.1-7.0 0.7 TPSSh -5.7-5.9 3.0-2.0-4.6 2.4-11.1-11.3 2.0-11.2-11.4 2.0 M06-2X -0.7-5.1-2.6-2.0-5.4-3.7-2.5-6.8-3.0-2.6-7.0-3.1 ωb97xd 0.4-5.7-2.2 0.6-6.4-3.5-1.2-7.3-1.8-1.2-7.3-1.8 B3LYP-D3-9.3-7.4-3.3-8.4-8.2-4.9-11.9-9.9-3.6-11.8-9.9-3.5 B3LYP-D3BJ -7.4-6.2-2.0-5.6-6.5-3.7-9.2-8.0-1.3-9.2-7.9-1.3 CAM-B3LYP-D3BJ -3.3-6.2-2.3-2.6-6.7-3.9-4.6-7.6-1.3-4.7-7.7-1.5 B97-D3BJ -10.0-5.7-1.3-7.1-5.3-2.6-12.3-8.1-0.8-12.3-8.0-0.8 B3LYP-NL -4.5-6.1-2.3-2.9-6.6-3.9-6.7-8.3-2.2-6.6-8.2-2.0 rev-pbe-nl 2.6-3.4 0.2 5.2-2.7-0.7 0.1-5.8 0.2 0.3-5.6 0.5 B2PLYP -6.7-5.0-0.3-6.3-4.4-0.8-9.8-8.1-0.8-9.9-8.2-1.0 B2PLYP-D3-3.8-3.8-1.2-3.7-3.5-1.8-5.2-5.2-0.9-5.2-5.2-0.9 B2GPPLYP-D3-10.3 1.4-0.6-11.0 1.6 0.1-10.3 1.4-1.2-10.3 1.4-1.2 MPW2PLYP -5.1-5.5-1.2-4.8-5.2-2.0-8.0-8.4-1.8-8.1-8.5-1.9 HF -12.4-7.4 1.2-13.0-9.9-1.7-15.5-10.5 1.3-15.5-10.5 1.3 MP2 5.9 1.6 0.3 3.6 3.0 1.1 5.8 1.5 0.1 6.0 1.7 0.3 SCS-MP2 1.7 0.7 1.3-0.1 1.5 2.0 1.1 0.0 1.0 1.1 0.1 1.0 CCSD(T) 0.9 0.8 0.2 1.2 0.8 0.3 1.2 1.1 0.1 1.1 1.1 0.0 S18

R5 R6 R7 R8 Dev-0 Dev-1 Dev-2 Dev-0 Dev-1 Dev-2 Dev-0 Dev-1 Dev-2 Dev-0 Dev-1 Dev-2 SVWN5 3.7-16.7-4.4 12.3-9.5-2.7 1.2 0.3 0.0 7.3-3.8-2.6 PBE -10.3-13.2 2.3-5.5-8.5 3.1-2.8-0.8-0.3-3.9-3.4 0.3 TPSS -12.8-10.3 5.0-7.2-7.1 5.5-7.0-0.7 0.0-10.5-2.9 1.6 B3LYP -16.5-11.5 1.4-12.7-9.7 1.0-3.9-1.8-0.7-8.7-4.1 0.7 CAM-B3LYP -9.3-10.7-0.9-5.7-8.9-1.1-4.3-2.5-1.3-5.6-4.5-0.3 B3PW91-9.7-12.2 3.4-5.8-8.6 3.6-3.3-1.5-0.8-3.4-2.8 1.9 MPW1PW91-6.0-12.1 2.0-2.4-8.7 2.2-3.1-1.6-0.9-1.6-3.1 1.1 PBE0-4.0-12.7 0.9-0.3-8.9 1.4-2.8-1.5-0.9-0.3-3.4 0.4 BMK -5.7-10.7 0.4-3.5-7.4 1.1-5.6-1.9-1.1-4.5-3.3 0.2 TPSSh -10.2-10.4 4.2-5.2-7.4 4.5-6.6-1.0-0.3-8.4-3.0 1.5 M06-2X -4.6-8.9-2.8-0.5-7.1-2.6-2.4-1.5-1.3-1.9-3.2-1.6 ωb97xd -3.4-9.5-0.6-2.3-7.6-0.2-3.6-1.9-1.2-1.8-3.1-0.8 B3LYP-D3-10.8-8.8-1.4-8.7-8.1-1.6-2.8-0.9-0.1-6.7-3.9-1.0 B3LYP-D3BJ -8.5-7.3 0.9-7.0-7.0 0.1-2.0-0.4 0.0-4.5-2.3 0.0 CAM-B3LYP-D3BJ -5.1-8.1-1.0-2.8-7.3-1.4-3.1-1.5-0.8-3.4-3.3-0.6 B97-D3BJ -11.8-7.5 3.1-10.0-5.9 2.9-2.1 0.3 0.4-5.9-1.4 0.4 B3LYP-NL -6.2-7.8 0.2-3.6-6.5-0.9-2.5-0.5 0.1-3.7-2.6-0.3 rev-pbe-nl -1.2-7.1 4.2 1.3-3.6 4.0-2.6 0.4 0.4-0.7-0.6 0.7 B2PLYP -10.0-8.3-0.4-7.9-6.4-0.1-3.1-1.0-0.4-5.2-2.3 0.4 B2PLYP-D3-6.1-6.1-0.5-5.1-5.0-0.5-2.1-0.2-0.1-3.1-1.2 0.2 B2GPPLYP-D3-8.1 3.6 1.0-9.8 2.0 0.3-3.7-0.8-0.8-9.0-0.2-1.5 MPW2PLYP -8.1-8.5-1.5-6.0-6.9-1.3-3.0-1.1-0.5-4.4-2.8-0.2 HF -7.6-2.6 5.6-9.5-5.9 1.9-8.4-4.8-2.7-10.8-4.7 1.4 MP2-0.6-4.9-4.0 0.2-1.8-1.6-0.2 1.0 0.2 2.7 1.7 0.2 SCS-MP2-0.1-1.2 0.2-1.9-1.4 0.0-2.8-0.1-0.5-1.5 0.7 0.3 CCSD(T) 2.2 2.1 1.2 1.3 1.1 0.6-1.2-0.4-0.5-0.7 0.0-0.3 S19

R9 R10 R11 R12 Dev-0 Dev-1 Dev-2 Dev-0 Dev-1 Dev-2 Dev-0 Dev-1 Dev-2 Dev-0 Dev-1 Dev-2 SVWN5 1.8 1.0 0.3 0.0-0.2-8.7 28.3-5.2-5.6 4.1-16.3-6.0 PBE -4.4-2.4-1.3-4.1-0.5-2.7-6.1-10.6-2.4-18.3-21.3-1.2 TPSS -8.6-2.3-0.7-7.6 0.3 0.6-11.2-12.2-0.7-22.9-20.5 1.7 B3LYP -6.9-4.8-2.5-6.2-2.7-0.5-15.6-12.0-1.7-28.1-23.1-1.5 CAM-B3LYP -6.9-5.0-2.7-6.7-3.4-1.1-4.0-9.6-2.3-17.8-19.2-2.9 B3PW91-6.0-4.2-2.5-2.8 0.6 1.2-6.7-11.1-0.5-20.4-22.9-0.4 MPW1PW91-5.6-4.0-2.5-3.4-0.2 0.5-1.1-10.6-1.4-15.6-21.8-1.6 PBE0-4.9-3.6-2.3-3.3-0.4-0.4 2.7-10.2-2.0-12.1-20.8-2.2 BMK -8.0-4.3-2.5-6.8-0.2 0.7-2.6-8.0-1.5-6.0-10.9 2.7 TPSSh -8.4-2.8-1.2-6.8 0.3 1.3-7.4-11.8-0.7-20.1-20.3 1.1 M06-2X -3.3-2.4-1.8-4.2-3.1-3.0 4.7-6.4-3.1-3.8-8.1-1.7 ωb97xd -4.5-2.7-1.3-5.8-2.2-0.9 0.1-7.6-1.9-1.7-7.8 0.3 B3LYP-D3-4.5-2.6-0.8-8.1-4.5-3.6-8.8-8.8-2.7-14.0-12.0-1.5 B3LYP-D3BJ -2.7-1.1-0.2-6.1-3.1-3.4-7.4-8.1-2.0-13.1-11.9-0.3 CAM-B3LYP-D3BJ -4.3-2.7-1.2-6.4-3.3-2.2 0.2-7.2-2.3-9.5-12.5-1.4 B97-D3BJ -2.3 0.1 0.3-5.8-2.0-4.3-14.5-8.5-1.8-15.7-11.4 0.6 B3LYP-NL -2.9-0.9 0.1-5.7-2.6-3.5-0.9-5.9-2.5-9.8-11.4-0.6 rev-pbe-nl -1.6 1.4 1.2-3.9 0.7-3.6 2.3-4.6-1.6-2.3-8.2 2.1 B2PLYP -4.6-2.5-1.4-3.3 0.6 0.9-8.8-6.8-1.2-15.5-13.9-1.5 B2PLYP-D3-2.4-0.6-0.2-3.1 0.5-0.3-4.9-4.8-1.2-8.3-8.3-0.7 B2GPPLYP-D3-3.1-0.2-0.3-7.0-2.5-3.2-18.2-0.5-2.4-8.1 3.6-1.0 MPW2PLYP -4.4-2.6-1.4-4.2-0.6 0.0-5.4-7.0-2.0-13.5-13.9-2.6 HF -13.3-9.7-5.4-15.5-9.5 0.6-16.9-12.4-0.7-27.1-22.0-2.0 MP2 0.5 1.7-0.1 6.7 9.6 5.7 3.6 1.8 0.0 5.7 1.4-0.3 SCS-MP2-2.8-0.1-0.9-0.2 4.2 3.6-2.8-1.3 0.1-0.4-1.5 0.3 CCSD(T) -0.7 0.1-0.1-1.6-0.3-0.2 0.6 0.2-0.2 0.8 0.7-0.7 S20

R13 R14 R15 R16 Dev-0 Dev-1 Dev-2 Dev-0 Dev-1 Dev-2 Dev-0 Dev-1 Dev-2 Dev-0 Dev-1 Dev-2 SVWN5 39.7-0.1-4.8 15.8 1.1-0.4 10.2-1.9-0.7 15.9 2.1-2.4 PBE 8.9-3.5 0.3-0.1-2.9-1.3-4.0-5.8-1.9 3.8-0.9-1.0 TPSS -0.3-4.7 3.1-2.7-4.0-1.2-6.8-6.4-1.7-0.5-2.0 0.1 B3LYP -7.1-5.9 0.6-1.9-3.8-1.5-8.1-6.8-2.3-3.0-2.3-1.3 CAM-B3LYP -0.2-5.4-1.4 2.2-2.8-1.2-3.3-5.3-1.8-1.3-2.0-2.2 B3PW91 4.7-4.4 1.8-0.5-4.0-1.3-4.9-6.7-2.0 0.2-2.5-1.8 MPW1PW91 9.5-4.4 0.7 1.6-3.5-1.2-2.4-6.1-1.9 1.8-2.4-2.1 PBE0 13.3-4.3-0.1 2.8-3.1-1.1-0.7-5.5-1.7 3.4-2.1-2.1 BMK 3.4-3.7 0.1 3.8-2.4-0.6-2.1-4.2-1.4-3.4-2.3-1.3 TPSSh 2.1-4.9 2.6-1.3-3.9-1.1-5.3-6.3-1.6-0.4-2.4-0.6 M06-2X 0.6-4.5-3.2 4.9-1.4-0.4 1.4-2.2-0.9-1.1-1.0-1.6 ωb97xd 7.2-3.7-1.4 1.7-2.5-0.8 0.6-2.8-0.7 0.8-1.6-1.4 B3LYP-D3-1.3-4.1-1.5 0.8-2.1-0.8-3.3-3.2-0.8 0.2-0.2-0.3 B3LYP-D3BJ 1.7-2.7-0.7 1.1-2.0-0.7-2.7-3.0-0.7 1.2 0.1-0.2 CAM-B3LYP-D3BJ 4.2-3.4-1.9 3.8-1.6-0.7-0.4-3.1-0.7 0.9-0.5-1.5 B97-D3BJ -0.5-1.9 0.2-3.1-2.4-1.0-5.0-3.2-0.9 0.9 0.5 0.4 B3LYP-NL 5.2-2.9-1.0 3.2-1.1-0.4-0.6-2.2-0.3 2.1 0.0-0.7 rev-pbe-nl 15.5-0.3 0.8 1.3-1.0-0.4 0.7-1.7-0.1 6.1 0.8 0.2 B2PLYP -4.3-3.1 0.1-0.6-1.9-0.8-4.3-3.9-1.3-1.8-0.9-0.6 B2PLYP-D3-0.2-1.4-0.5 0.8-1.0-0.4-1.7-2.0-0.6 0.2 0.3-0.1 B2GPPLYP-D3-21.3-0.9-2.5-6.7 0.3-0.7-6.4-0.1-1.0-6.7 1.5 0.4 MPW2PLYP -1.6-3.5-0.8 1.1-1.7-0.7-2.9-3.6-1.3-0.9-0.9-1.0 HF -19.9-8.8 0.7-3.9-5.1-1.4-8.7-7.3-2.4-13.1-5.8-3.5 MP2 3.4 2.2-0.4 2.4 1.0 0.2 2.3 0.7 0.0 1.2 1.3 0.4 SCS-MP2-4.2-1.4-0.2-0.7-0.5 0.0-0.8-0.8-0.4-1.8-0.3 0.4 CCSD(T) -1.0-1.2-1.4 0.5 0.5 0.3 0.5 0.5 0.2 0.3 0.4 0.4 S21

R17 R18 R19 R20 Dev-0 Dev-1 Dev-2 Dev-0 Dev-1 Dev-2 Dev-0 Dev-1 Dev-2 Dev-0 Dev-1 Dev-2 SVWN5-7.5 12.9 7.3-3.6 8.0-1.6-18.7 11.6-1.5-5.9 4.3 1.7 PBE 13.7 16.7 4.7 3.2 4.7 4.3 28.7 32.1 5.1 5.2 6.7-0.1 TPSS 19.3 16.9 3.0 3.9 5.0 1.4 40.4 32.4 1.8 8.2 7.0-1.0 B3LYP 22.3 17.3 4.4 3.2 2.6 3.2 45.0 35.4 5.9 9.6 7.1-0.6 CAM-B3LYP 12.5 13.9 4.4 0.2 2.6 0.2 26.0 26.3 3.7 4.3 4.9-0.8 B3PW91 13.2 15.7 2.1 0.9 2.5 2.0 28.6 31.3 0.9 5.0 6.2-1.7 MPW1PW91 9.0 15.2 3.1-0.4 2.8 0.7 20.2 28.6 1.3 2.9 6.0-1.0 PBE0 6.3 15.0 3.9-0.9 3.3 0.4 14.6 27.0 2.2 1.5 5.8-0.6 BMK 5.3 10.3 2.5 0.0 1.4-0.2 8.7 14.7-3.8 0.7 3.1-1.7 TPSSh 15.9 16.1 2.8 2.3 4.4 0.2 33.9 30.4 1.1 6.5 6.6-1.1 M06-2X 3.6 7.9 4.1-1.1 3.3-2.1 3.5 8.5-0.1-0.5 1.6-0.6 ωb97xd 2.3 8.4 2.9 1.1 3.4 1.8-0.7 8.0-3.2-2.0 1.1-2.0 B3LYP-D3 13.2 11.3 4.9 3.4 3.9 3.1 21.4 16.9 2.1 5.1 4.2 0.3 B3LYP-D3BJ 10.9 9.7 3.0 3.2 3.8 3.1 15.7 12.4-2.7 3.8 3.2-0.7 CAM-B3LYP-D3BJ 6.2 9.2 2.9 0.1 3.0 0.0 9.7 12.7-2.3 1.0 2.5-1.3 B97-D3BJ 14.2 10.0 2.8 6.5 4.6 6.6 22.3 14.6-0.9 5.6 3.5-0.6 B3LYP-NL 7.0 8.6 2.4 1.1 3.2 0.7 8.6 9.3-5.6 1.6 2.4-1.3 rev-pbe-nl 0.2 6.2 0.1 2.1 4.1 2.4-3.7 4.3-9.5-1.9 1.1-2.2 B2PLYP 12.0 10.3 3.1 2.4 1.8 2.4 21.4 17.7 0.9 4.3 3.4-0.9 B2PLYP-D3 6.4 6.4 2.1 2.3 2.3 2.3 7.3 6.4-3.4 1.4 1.4-1.1 B2GPPLYP-D3 11.6 0.0 2.6 7.2 1.3 5.7 14.7-4.2 1.2 3.5-2.3-0.8 MPW2PLYP 10.3 10.7 4.1 1.4 2.1 1.5 18.0 17.5 1.9 3.4 3.6-0.3 HF 19.5 14.4 2.6-1.3-2.3-2.2 43.7 33.6 5.3 8.7 6.2-1.6 MP2-5.9-1.6-0.2 0.3 0.2 0.9-19.4-12.4-8.7-5.2-3.1-2.0 SCS-MP2-0.2 0.9-0.1 1.1 0.1 0.4-5.7-4.7-6.4-2.1-1.5-2.1 CCSD(T) -0.7-0.6 0.4 0.5 0.6-0.1 -i- -i- -i- -i- -i- -i- -i- Calculations with the large basis-set could not be performed due to their large size. S22

R21 R22 R23 R24 Dev-0 Dev-1 Dev-2 Dev-0 Dev-1 Dev-2 Dev-0 Dev-1 Dev-2 Dev-0 Dev-1 Dev-2 SVWN5 0.7 0.7 0.0-0.2 9.3 4.0-13.9-9.9 6.1-6.4-5.0 0.8 PBE 5.3 5.3 2.1 11.7 12.1 3.1-13.3-7.8 3.4-4.7-4.7 0.7 TPSS 7.0 7.0 3.4 14.2 12.0 2.6-12.4-4.8 0.7-6.7-4.4 0.5 B3LYP 4.9 4.9 1.0 15.2 12.0 2.9-8.4-2.3 1.9-6.1-4.2 0.0 CAM-B3LYP 3.3 3.3 0.3 8.8 8.7 1.8-2.8 0.4 4.4-4.9-3.1 0.0 B3PW91 5.0 5.0 1.4 11.0 11.2 1.4-8.4-3.6 2.8-4.8-4.4 0.5 MPW1PW91 4.4 4.4 1.2 8.3 10.3 1.2-7.4-2.7 2.7-4.3-4.2 0.4 PBE0 4.1 4.1 1.1 6.7 9.9 1.5-7.5-3.0 3.1-3.9-4.0 0.5 BMK 4.8 4.8 2.0 6.9 7.5 1.1-4.2-1.5 4.4-0.6-1.6 1.3 TPSSh 6.6 6.6 3.1 12.2 11.3 2.1-10.2-3.2 0.9-6.2-4.2 0.3 M06-2X 1.5 1.5 0.4 2.2 4.4 0.8-1.2-3.8 5.7-3.0-0.7 0.8 ωb97xd 2.8 2.8 1.6 3.4 4.9-0.5-2.7-0.2 5.4-0.3-1.1 0.6 B3LYP-D3 2.4 2.4 0.4 9.7 7.9 2.5-8.4-3.1 2.5-3.4-2.0-0.2 B3LYP-D3BJ 1.7 1.7-0.2 9.0 7.7 2.1-8.6-2.1 1.9-3.2-2.0 0.2 CAM-B3LYP-D3BJ 1.7 1.7-0.3 5.1 5.7 0.7-2.9 0.4 4.5-3.4-2.0 0.1 B97-D3BJ 1.9 1.9 0.2 12.5 9.3 2.9-13.0-5.4 1.4-2.1-2.0 0.8 B3LYP-NL 1.3 1.3-0.6 6.1 6.3 1.2-8.6-2.3 2.3-4.3-3.0 0.2 rev-pbe-nl 2.2 2.2 0.9 3.6 5.4-0.1-13.3-7.4 3.5-2.1-3.2 1.1 B2PLYP 2.7 2.7 0.5 9.4 7.5 2.5-2.2-2.8 1.3-2.6-2.4 0.3 B2PLYP-D3 1.1 1.1 0.0 6.3 5.2 1.8-2.3-2.7 1.3-1.3-1.4 0.3 B2GPPLYP-D3 1.4 1.4 1.9 5.4-1.2 1.1-1.9-4.6 3.9 1.0 0.9 0.2 MPW2PLYP 2.3 2.3 0.3 8.1 7.3 2.6-1.7-1.7 1.4-2.8-2.3 0.2 HF 3.6 3.6-1.1 10.4 6.5-1.8 7.2 13.0 0.0-3.1-1.6-0.3 MP2-0.9-0.9 0.0-1.5-1.0-0.1 8.8-2.1 3.4 2.4 0.1 1.0 SCS-MP2 0.4 0.4 0.2-0.3-1.2-1.5 8.9 0.9 3.0 2.0 0.4 0.9 CCSD(T) 0.2 0.2 0.4 -i- -i- -i- -0.7 0.6-0.4 0.5 0.6 0.1 -i- Calculations with the large basis-set could not be performed due to their large size. S23

R25 Dev-0 Dev-1 Dev-2 SVWN5 6.3-14.1-4.7 PBE -17.8-20.8-3.5 TPSS -22.8-20.3-1.3 B3LYP -26.9-21.9-3.7 CAM-B3LYP -16.4-17.8-4.2 B3PW91-17.8-20.3-1.1 MPW1PW91-13.3-19.4-2.2 PBE0-10.2-18.9-3.0 BMK -7.1-12.0-0.7 TPSSh -19.4-19.6-1.3 M06-2X -4.3-8.6-3.1 ωb97xd -2.8-9.0-1.8 B3LYP-D3-15.2-13.2-4.3 B3LYP-D3BJ -12.8-11.6-1.8 CAM-B3LYP-D3BJ -8.9-11.9-2.7 B97-D3BJ -16.1-11.8-1.4 B3LYP-NL -8.9-10.5-1.5 rev-pbe-nl -1.9-7.8 1.2 B2PLYP -14.7-13.0-2.6 B2PLYP-D3-8.0-8.0-1.5 B2GPPLYP-D3-11.3 0.3-3.4 MPW2PLYP -12.8-13.3-3.6 HF -25.0-20.0-4.0 MP2 4.9 0.6-0.6 SCS-MP2-0.5-1.6-0.1 CCSD(T) -0.7-0.7-2.0 S24

Cartesian coordinates of the reactants and products in the reactions R1 R25. The geoemtries were optimized at B3LYP/6-311+G(d,p). 6 0.00000 1.17952 0.28186 6 0.00000 0.73415-0.99031 6 0.00000-0.73415-0.99031 6 0.00000-1.17952 0.28186 1 0.00000 2.2109 0.60733 1 0.00000 1.34815-1.88191 1 0.00000-1.34815-1.88191 1 0.00000-2.2109 0.60733 6 0.00000 0.00000 1.21567 1 0.87642 0.00000 1.87824 1-0.87642 0.00000 1.87824 6 1.27668 0.66971-0.50872 6 0.08714 1.12852 0.32299 6 0.08884-1.1279 0.32417 6 1.2779-0.66881-0.50773 1 1.91952 1.32448-1.08435 1 1.92134-1.32337-1.08291 6 0.0411 0.00096 1.38078 1-0.87682 0.0007 1.97672 1 0.91054 0.00208 2.04117 6-1.19139 0.77928-0.51663 6-1.18987-0.78155-0.5162 1-2.08408-1.17818-0.02794 1-1.14377-1.20681-1.52028 1 0.11988 2.1555 0.68622 1 0.12303-2.15429 0.6889 1-2.08644 1.17472-0.02863 1-1.14562 1.20394-1.52082 C 2 H 4 C 2 H 2 6 0.00000 0.00000 0.66439 1 0.00000 0.92285 1.23517 6 0.00000 0.00000-0.66439 1 0.00000 0.92285-1.23517 1 0.00000-0.92285 1.23517 1 0.00000-0.92285-1.23517 6 0.00000 0.00000 0.59977 6 0.00000 0.00000-0.59977 1 0.00000 0.00000 1.66299 1 0.00000 0.00000-1.66299 6 0.662226-0.429355 0.000667 1 0.611935-1.119565 0.866310 6-0.530543 0.523228 0.000401 1-0.483991 1.162743 0.890516 1-0.482849 1.163434-0.889127 1 0.612312-1.118029-0.866503 8-1.702742-0.289140-0.000513 1-2.481180 0.274889-0.000082 8 1.881951 0.173302-0.000427 6 0.25527 0.26376 0.00011 6-0.77347 1.17301-0.00033 6-1.98016 0.4198 0.00025 6-1.59866-0.89128 0.00002 1-0.66884 2.24695-0.0005 1-2.99156 0.79303 0.00049 1-2.14956-1.81743 0.00007 8-0.25325-1.00473-0.00023 6 1.69594 0.46419 0.0003 8 2.53286-0.41231-0.00002 1 1.97955 1.53688-0.00018 H N 6 0.00000 0.66606-1.25657 6 0.00000-0.66606-1.25657 6-0.00009 1.2643 0.66699 6-0.00009 1.2643-0.66699 S25

1 0.00000 1.35753-2.08616 1 0.00000-1.35753-2.08616 8 0.00000 0.00000 0.97136 6 0.00000 1.13126 0.1591 8 0.00000 2.23833 0.5982 6 0.00000-1.13126 0.1591 8 0.00000-2.23833 0.5982 6-1.25172 0.66907 1.30473 6-1.37904 1.1328-0.13926 6-1.3802-1.1316-0.14011 6-1.25239-0.66917 1.30421 1-1.08662 1.32439 2.14985 1-1.08799-1.32528 2.14886 6-2.2693 0.00125-0.71215 1-2.33373 0.00168-1.80417 1-3.27227 0.00166-0.2828 6-0.02521 0.77117-0.86865 6-0.02583-0.77052-0.86919 1 0.00269-1.22014-1.86307 1-1.69489 2.16185-0.29494 1-1.69686-2.16023-0.29677 1 0.00332 1.22147-1.86224 6 1.23564 1.15314-0.12221 8 1.66491 2.23562 0.129 6 1.23434-1.1541-0.12252 8 1.66233-2.23701 0.12886 8 1.90384-0.00081 0.27916 1-0.00029 2.0995 1.35209 1-0.00029 2.0995-1.35209 6-0.00009-0.1576 1.15511 8-0.00008-0.55875 2.29263 6-0.00009-0.1576-1.15511 8-0.00008-0.55875-2.29263 7 0.00043-0.94127 0.00000 1 0.00102-1.95054 0.00000 6 1.26219-0.66902 1.30901 6 1.3863-1.13277-0.13531 6 1.38653 1.13231-0.13592 6 1.26223 0.66927 1.30869 1 1.10015-1.32468 2.15465 1 1.10024 1.32542 2.15397 6 2.27636-0.00053-0.70789 1 2.33879-0.00087-1.80017 1 3.28042-0.00053-0.28052 6 0.03288-0.7758-0.8625 6 0.03316 0.77563-0.86264 1 0.01627 1.2151-1.86187 1 1.70594-2.16104-0.28959 1 1.70679 2.16038-0.29041 1 0.01611-1.21539-1.86167 6-1.23901-1.1777-0.1302 8-1.63911-2.29038 0.11493 6-1.23866 1.17797-0.13025 8-1.63818 2.29085 0.11489 7-1.89405 0.00022 0.22428 1-2.75988 0.00009 0.74913 NH 6-0.32803 0.68956 0.00000 8 0.32803 1.6982 0.00000 1-1.43545 0.68063 0.00000 6 0.32803-0.68956 0.00000 8-0.32803-1.6982 0.00000 1 1.43545-0.68063 0.00000 6 0.00000 0.00000 0.18488 8 0.00000 0.00000 1.39645 6 0.00000 1.2906-0.61289 1 0.94793 1.38875-1.15278 1-0.7953 1.28352-1.36439 1-0.12443 2.14263 0.05406 6 0.00000-1.2906-0.61289 1-0.94793-1.38875-1.15278 1 0.79530-1.28352-1.36439 1 0.12443-2.14263 0.05406 6 0.64157 1.47363 0.038 6 1.17798-0.04101-0.00009 S26

6 0.259 0.37622 1.01976 6 1.53028-0.56487-0.36858 6 1.45512 0.88062-0.839 1 0.22715 2.47165 0.01818 1 1.87574 1.27-1.7548 6-0.67183-0.63055 0.22798 1-0.07089 0.63696 2.01977 1 2.33889-1.21348-0.68676 1-1.02131-1.40902 0.91033 8 0.24653-1.17936-0.7212 6-1.85793 0.01826-0.45682 8-2.91388 0.19775 0.09717 1-1.68466 0.32402-1.5077 8 1.44208-0.44338 1.03314 6-2.01632-0.10202 0.00001 6-0.80518-0.65954-0.00001 1-2.11924 0.97798 0.00009 1-0.68964-1.73981-0.00005 6 0.44394 0.16614-0.00006 8 0.41189 1.38104 0.00000 6 1.7498-0.6007 0.00000 1 1.8053-1.24966 0.8805 1 1.80462-1.25127-0.87935 1 2.59065 0.09104-0.00086 1-2.92031-0.69984 0.00004 6 1.85736 1.154-0.00003 6 3.24509 0.84183 0.00012 6 3.32744-0.51975 0.00021 1 1.41289 2.13653-0.00012 1 4.07329 1.53236 0.00018 1 4.15369-1.21076 0.00034 8 2.09157-1.07034 0.00006 6-0.20325-0.42545-0.00027 6-1.26518 0.40426-0.00041 1-0.39994-1.49451-0.00032 1-1.13748 1.48259-0.00035 6-2.64934-0.12579-0.00065 8-2.89107-1.32114 0.00027 6-3.76028 0.90696 0.00042 1-3.67724 1.55291 0.88081 1-3.67906 1.55252-0.88043 1-4.72915 0.40998 0.00150 Me 6-1.14564 0.01755 0.05459 8-0.97534-0.85028 0.87109 8-2.34634 0.34628-0.45971 6-3.47224-0.40961 0.03158 1-4.33885-0.00443-0.48547 1-3.34671-1.46845-0.19734 1-3.57223-0.28275 1.11007 6-0.0654 0.9051-0.5419 1-0.08757 0.79314-1.62809 1-0.29565 1.9439-0.30058 6 1.30588 0.56738 0.0052 8 1.8544 1.16226 0.89768 8 1.83703-0.48321-0.64394 6 3.11376-0.94446-0.16016 1 3.85913-0.15235-0.24099 1 3.02926-1.25797 0.88081 1 3.37648-1.78727-0.79515 Me Me Me 6 1.02713 1.21174-0.14517 6-0.33479 1.7184 0.34087 6-1.4762 0.88985-0.25637 6 0.09832-1.09249 0.05989 6 1.1744-0.28653-0.01831 1-2.45217 1.17948 0.13785 1-0.37145 1.64643 1.43371 1-0.45728 2.7758 0.08976 1 1.17827 1.48393-1.20043 1 1.83771 1.70354 0.4037 1 0.20878-2.16794 0.16085 6 1.40946 0.12823-0.01118 8 2.36541 0.86289-0.12278 8 1.53281-1.21814 0.0624 6 2.87337-1.73527 0.01709 1 2.77058-2.81367 0.11523 1 3.34898-1.47897-0.93066 1 3.46628-1.32914 0.83761 6-0.9778-0.61489 0.36086 8-1.33957-0.95878 1.4592 8-1.39751-1.19646-0.7797 6-2.26587-2.33562-0.62301 S27

1-1.51545 1.03461-1.34495 6-1.2897-0.60226-0.01776 8-2.24051-1.36178 0.06755 6 2.57586-0.82445-0.00114 1 3.12437-0.44149 0.86705 1 2.59513-1.91479 0.0287 1 3.12612-0.49094-0.88861 CH 3 NHNH 2 1-1.76269-3.11791-0.05322 1-3.18364-2.05007-0.10696 1-2.48325-2.67493-1.63331 6-0.02216 0.51786 0.0798 6-0.48119 1.78217-0.03825 6 0.37856 2.99118-0.28939 1 1.35784 2.74472-0.68672 1-0.14094 3.67749-0.96473 1 0.5282 3.52959 0.65464 6-1.9494 2.09642 0.08464 1-2.33051 2.46162-0.87558 1-2.55591 1.24867 0.39957 1-2.09382 2.90596 0.80785 CH 3 CH 7-1.24592-0.14936 0.05405 1-1.13817-0.92151 0.71488 1-1.5228-0.53693-0.84161 7-0.02785 0.56799-0.12055 1-0.02508 1.3182 0.56011 6 1.18004-0.24038-0.00217 1 1.24221-0.93346-0.84604 1 2.05399 0.41578-0.03900 1 1.22596-0.83023 0.93022 6 0.00000 0.46024 0.00000 1-0.49888 1.45438 0.00000 6-0.93145-0.7206 0.00000 1-1.58426-0.66984 0.8785 1-1.58426-0.66984-0.8785 1-0.37435-1.65737 0.00000 8 1.20381 0.3881 0.00000 N N 6 0.00000 1.24549 0.09788 8 1.04174 1.73271-0.28011 6 0.00000 0.00000 0.99659 1-0.89746-0.03148 1.61567 1 0.89746 0.03148 1.61567 6 0.00000-1.24549 0.09788 8-1.04174-1.73271-0.28011 6 1.35338-1.78201-0.30095 1 1.98702-0.97055-0.67122 1 1.85254-2.19748 0.58115 1 1.24348-2.55907-1.05611 6-1.35338 1.78201-0.30095 1-1.98702 0.97055-0.67122 1-1.85254 2.19748 0.58115 1-1.24348 2.55907-1.05611 6-1.39144 0.06896 0.00299 6-0.54609 1.20441 0.0111 6 0.74463 0.70712-0.00483 7 0.62299-0.65003-0.02791 1-0.83373 2.24432 0.02079 6 1.67811-1.64348 0.01923 1 2.47821-1.38488-0.67735 1 2.09703-1.73478 1.02647 1 1.24297-2.59728-0.27174 7-0.67365-1.05149-0.01555 6-2.88809 0.01709 0.00535 1-3.30512 0.50057-0.88344 1-3.22300-1.02097 0.02026 1-3.30239 0.52616 0.88082 6 2.06447 1.40831-0.00181 1 2.66929 1.13994 0.87067 1 2.65344 1.17572-0.89533 1 1.90837 2.48735 0.02081 H 3 C 6 1.16448-0.30884 0.31722 6 0.00000 1.1166 0.09578 S28

6 0.14754 1.80546 0.12662 6-1.17954 1.13913-0.23267 6-1.20992-0.28374 0.33583 1 1.15559-0.19387 1.41701 1 0.19926 1.99631 1.21025 1 0.28121 2.7558-0.39175 1-2.0156 1.72413 0.16519 1-1.28348 1.09219-1.32139 1-1.21225-0.22419 1.43735 8 1.24509 0.97967-0.26134 8-0.02051-0.97979-0.06696 6-2.39849-1.1066-0.12768 1-2.35784-2.11068 0.30015 1-3.33446-0.6338 0.18264 1-2.39812-1.19682-1.21692 6 2.3506-1.12061-0.14704 1 3.27797-0.62592 0.14661 1 2.31757-2.11652 0.29781 1 2.3255-1.21455-1.23422 6 1.1166 0.00000-0.09578 6 0.00000-1.1166 0.09578 6-1.1166 0.00000-0.09578 6 0.00000-1.75969 1.49499 1-0.88088-2.39669 1.61924 1 0.88088-2.39669 1.61924 1 0.00000-1.0417 2.31429 6 0.00000-2.28017-0.90735 1 0.88044-2.91318-0.75508 1-0.88044-2.91318-0.75508 1 0.00000-1.96379-1.9496 6-2.28017 0.00000 0.90735 1-2.91318 0.88044 0.75508 1-2.91318-0.88044 0.75508 1-1.96379 0.00000 1.9496 6-1.75969 0.00000-1.49499 1-2.39669-0.88088-1.61924 1-2.39669 0.88088-1.61924 1-1.0417 0.00000-2.31429 6 0.00000 1.75969 1.49499 1 0.88088 2.39669 1.61924 1-0.88088 2.39669 1.61924 1 0.00000 1.0417 2.31429 6 0.00000 2.28017-0.90735 1-0.88044 2.91318-0.75508 1 0.88044 2.91318-0.75508 1 0.00000 1.96379-1.9496 6 2.28017 0.00000 0.90735 1 2.91318-0.88044 0.75508 1 2.91318 0.88044 0.75508 1 1.96379 0.00000 1.9496 6 1.75969 0.00000-1.49499 1 2.39669 0.88088-1.61924 1 2.39669-0.88088-1.61924 1 1.0417 0.00000-2.31429 6 0.67329 0.00002 0.00000 6-0.67329 0.00002-0.00002 6 1.52569 1.24973-0.00763 1 2.14216 1.29858 0.8984 1 2.22344 1.22583-0.85329 1 0.96045 2.1768-0.07472 6-1.52569 1.24973 0.00763 1-2.14223 1.29855-0.89835 1-2.22336 1.22586 0.85336 1-0.96044 2.17681 0.07464 6 1.52563-1.24974 0.00763 1 2.14205-1.29866-0.89843 1 2.22341-1.22584 0.85327 1 0.96034-2.17677 0.07479 6-1.52563-1.24973-0.00763 1-0.96035-2.17676-0.07505 6-0.32415 0.58235 0.00004 1-1.41414 0.572-0.00023 6 0.32415 1.93626 0.00001 1 0.02557 2.51893 0.87884 1 1.41422 1.85818 0.00000 6 0.32415-0.58235 0.00004 1 1.41414-0.57200-0.00023 6-0.32415-1.93626 0.00001 1-1.41422-1.85818 0.00000 1-0.02561-2.51882-0.87886 1-0.02557-2.51893 0.87884 1 0.02561 2.51882-0.87886 S29

1-2.14185-1.29878 0.89856 1-2.22361-1.22572-0.8531 F 3 C Cl NCH 3 6-0.12565 0.65185 0.56134 6 1.14353-0.25074 0.48752 6 0.58051-1.61083 0.14074 6-0.7262-1.59646-0.14818 1 1.21434-2.4915 0.10579 1-1.33803-2.43306-0.45929 6-0.07031 2.04373-0.06862 1 0.19627 2.0001-1.12699 1-1.05302 2.51342 0.00548 1 0.65531 2.68351 0.44006 6 2.21913 0.17564-0.52866 1 1.81425 0.22969-1.54238 1 2.63657 1.15252-0.27458 1 3.04117-0.54582-0.53655 6-1.25611-0.22225-0.01326 8-2.37462 0.15938-0.28610 1-0.38631 0.77132 1.62109 1 1.62709-0.30083 1.47087 9 0.95802-0.91386-1.08947 17-1.88493-0.44411-0.00001 8-0.55829 1.81545 0.00019 6-0.48234 0.63932 0.0001 6 0.86751-0.13892-0.00011 9 0.95778-0.91518 1.08876 9 1.88411 0.72058 0.00057 NH 2 6 0.8236-1.59342 0.00000 6 0.15638-1.04142 1.26605 6 0.15638 0.50100 1.28511 6 0.15638 0.50100-1.28511 6 0.15638-1.04142-1.26605 1-0.40891 0.90164 2.12833 1-0.87889-1.39936 1.31617 1 0.65879-1.41798 2.16194 1 1.88779-1.32412 0.00000 1 0.77899-2.68692 0.00000 1-0.40891 0.90164-2.12833 1 1.19122 0.85837-1.37749 1-0.87889-1.39936-1.31617 1 0.65879-1.41798-2.16194 1 1.19122 0.85837 1.37749 6-0.40986 1.08583 0.00000 8-1.25335 1.95703 0.00000 CH 3 CH=NH 6-1.94678-1.15404 0.1487 6-2.34459 0.29715-0.14843 6-1.32572 1.29411 0.44288 6 0.50402-0.49816 0.25697 6-0.52708-1.46506-0.34548 1-1.54217 2.32446 0.15585 1-2.40051 0.44584-1.233 1-3.34073 0.51197 0.24894 1-2.00805-1.3362 1.22896 1-2.65586-1.84118-0.32224 1 0.54594-0.63095 1.34893 1-0.48122-1.38093-1.437 1-0.23482-2.48703-0.0911 1-1.35707 1.23464 1.53875 6 0.08385 0.95332-0.00695 8 0.81575 1.74841-0.55466 8 1.76259-0.80744-0.30069 7 2.80005-0.12854 0.44266 1 3.59766-0.74824 0.31949 1 2.98761 0.71564-0.09959 MeHN S30

6 1.20566-0.14096 0.00000 1 1.75366 0.21509-0.87921 1 1.18782-1.2312-0.0003 1 1.75333 0.21456 0.87961 6-0.18892 0.40487-0.00004 1-0.26935 1.50176 0.00008 7-1.2078-0.35371 0.00001 1-2.07127 0.19229-0.00002 C 2 Me H 6 0.36588 0.1278-0.19250 6 1.18521-1.08787 0.33462 6 0.34954-2.34732 0.36956 6-0.93386-2.43295 0.02197 6-1.76175-1.24088-0.37247 6-1.13838 0.04601 0.19890 6-1.96117 1.27486-0.22724 6-3.23006-1.38151 0.06932 6 2.4982-1.33565-0.48092 6 3.35358-2.45683 0.13531 6 3.37107-0.07983-0.63541 6 0.91987 1.43345 0.35547 8 1.18738 1.64218 1.51510 8 1.03867 2.37946-0.60493 6 1.51106 3.6669-0.16705 1 0.42681 0.1653-1.28503 1 1.48764-0.85366 1.36476 1 0.85679-3.24979 0.69311 1-1.43122-3.40017 0.04816 1-1.89257 1.39793-1.31607 1-1.54661 2.18653 0.21279 1-3.26539-1.50569 1.15946 1-3.65561-2.2943-0.36255 1 2.19172-1.65729-1.48561 H 6 2.08855-1.4474-0.0528 6 0.55715-1.45131 0.01208 6-0.00924-0.22381 0.76724 6 2.1024 1.08665 0.07657 6 2.6177-0.15347-0.68069 1 0.13511-1.46041-0.99708 1 0.19935-2.36051 0.50609 1 2.50337-1.55779 0.95788 1 2.43694-2.31173-0.62700 1 2.39368 2.0185-0.41128 1 2.52797 1.09059 1.08913 1 2.29200-0.0954-1.72595 1 3.71165-0.14579-0.69341 1 0.35645-0.28272 1.80452 6 0.58941 1.0696 0.21322 8-0.09277 2.02529-0.10058 6-1.54233-0.19939 0.82169 1-1.86674 0.61533 1.49105 1-1.88084-1.13654 1.27855 7-2.14819-0.10259-0.50377 1-1.92373 0.81076-0.88494 6-3.59557-0.28484-0.48684 1-4.12541 0.39951 0.19832 1-3.99399-0.13488-1.49292 1-3.83475-1.30932-0.18479 C 2 Me 6 7.45622 0.21196 1.20331 6 6.96797 0.00573-0.23403 6 7.49976 1.11462-1.16413 6 5.47062-0.12057-0.37652 6 4.55301-0.05854 0.59697 6 3.10209-0.21102 0.42108 6 2.50008-1.00349-0.47505 6 1.01924-1.15696-0.69675 6 0.1004-0.32065 0.19743 6-1.38519-0.53924-0.11082 6-3.76380 0.04982 0.52191 6-4.64856 0.97293 0.13192 6-6.07996 0.71863-0.1304 8-6.85986 1.57482-0.48658 8-6.44319-0.57152 0.06658 6-7.82739-0.87544-0.17367 6-2.31192 0.30785 0.78239 1 8.54854 0.24995 1.2312 1 7.08211 1.15368 1.61757 1 7.13383-0.59925 1.86134 1 7.39461-0.94222-0.59651 1 7.12767 2.0944-0.84920 1 7.18206 0.95326-2.19824 1 8.59316 1.14502-1.14942 S31

1 2.85022-3.42472 0.13897 1 3.62769-2.21374 1.16791 1 4.28117-2.57775-0.43114 1 3.66143 0.32177 0.34086 1 2.87456 0.71242-1.19744 1 4.2889-0.32988-1.1753 1 1.53445 4.2874-1.06039 1 2.50864 3.57969 0.26605 1 0.83556 4.09076 0.57748 1-1.17984-0.02776 1.29408 1-1.76391-1.15727-1.47196 6-3.43408 1.13858 0.1867 6-4.06004-0.15903-0.33992 1-4.00161 2.00508-0.16821 1-3.50001 1.1517 1.28219 1-4.11982-0.11436-1.43524 1-5.08779-0.25969 0.02386 H H H H H 6-1.21719-1.2242-0.30397 6-1.67238 0.15609 0.19347 6-0.65078 1.21507-0.19871 6 0.73105 0.80497 0.29375 6 1.08537-0.59744-0.22284 8 0.07232-1.51899 0.20479 8-2.91813 0.53361-0.37734 8-0.93986 2.48888 0.37094 8 1.73276 1.71737-0.15083 6 2.42604-1.1132 0.30513 8 3.52841-0.47341-0.31369 1-3.55875-0.16402-0.1946 1-1.82046 2.75522 0.08232 1 3.39416 0.48125-0.24324 1 1.43899 2.60918 0.07265 8-2.09621-2.23357 0.10507 1-1.91081-2.42736 1.03328 1-1.21879-1.24631-1.40151 1-1.74602 0.11844 1.29042 1-0.62935 1.29589-1.29473 1 0.71555 0.77689 1.39227 1 1.13096-0.57903-1.3208 1 2.45493-1.00229 1.3985 1 2.5026-2.17664 0.07306 1 5.12505-0.26183-1.40035 1 4.87681 0.14407 1.61522 1 2.48916 0.36526 1.11047 1 3.12476-1.62131-1.11824 1 0.80459-0.92453-1.74991 1 0.76064-2.21998-0.58769 1 0.34178 0.74219 0.07836 1 0.28956-0.56484 1.24958 1-1.58452-0.29883-1.16142 1-1.63387-1.60025 0.01485 1-4.109-0.97263 0.65638 1-4.35853 2.00732-0.02044 1-7.93183-1.93818 0.03507 1-8.46854-0.29005 0.48713 1-8.09297-0.66038-1.20987 1-2.08913 1.37155 0.64968 1-2.09688 0.06737 1.83263 CH H H H H H H H H CH 2 H 6 2.89392-1.1088-0.36555 8 3.84526-1.10951 0.36404 6 1.94825 0.06611-0.5791 8 2.38396 1.17312 0.17353 6 0.50807-0.34035-0.18078 1 0.29833-1.33955-0.57981 6-0.54606 0.62754-0.75074 8-0.20289 1.98816-0.45354 6-1.97978 0.35901-0.25927 1-2.64893 1.02324-0.8138 6-2.47897-1.07233-0.44883 8-3.85779-1.17364-0.13405 1 2.61905-2.00566-0.96506 1 1.95966 0.2726-1.66234 1 1.75769 1.89026-0.01605 8 0.42021-0.42966 1.24446 1-0.52794 0.53162-1.84239 1-0.73194 2.24948 0.31492 8-2.1167 0.76307 1.11049 1-1.8897-1.76465 0.16828 1-2.37733-1.37592-1.4947 1-3.98515-0.77577 0.73601 1 1.11709 0.13725 1.60996 1-1.43982 0.27777 1.61131 H S32

6 1.87341-0.51153-0.04288 6 3.36772-0.61044 0.35695 6 4.06894 0.73787-0.03013 6 3.33272 1.909 0.6304 6 1.89782 2.00104 0.10359 1 3.32349 1.78545 1.71658 1 3.83998 2.8569 0.43827 1 1.29222 2.6037 0.78891 1 1.8951 2.558-0.84495 1 3.87625 0.83003-1.10998 6 5.63402 0.80211 0.08393 6 4.07363-1.74643-0.42954 6 5.59511-1.74778-0.25669 6 6.20824-0.42393-0.68559 1 5.97092-0.27391-1.75084 1 3.84025-1.63575-1.49596 1 3.68063-2.72006-0.12553 1 5.87847-1.96093 0.77819 1 6.03807-2.54312-0.86318 6 1.2269 0.66586-0.12316 6 1.15176-1.83857-0.25073 6-0.36507-1.79406-0.57178 1 1.30189-2.44449 0.65169 1 1.64827-2.4027-1.04611 1-0.51769-1.83461-1.65314 1-0.82587-2.69914-0.17127 8 7.62854-0.56449-0.54575 1 8.06117 0.17636-0.98025 6 3.41004-0.94989 1.87128 1 3.05842-0.11997 2.48605 1 2.75799-1.80245 2.07807 1 4.40657-1.22441 2.21592 6 6.12711 2.07613-0.64257 1 5.72435 2.14176-1.65848 1 5.84769 2.98645-0.109 1 7.21997 2.08946-0.71103 6 6.17041 0.85891 1.52853 1 5.67981 1.65659 2.09225 1 6.03102-0.07163 2.07616 1 7.2425 1.06571 1.52308 6-1.02948-0.53149-0.01318 6-0.23039 0.70192-0.57931 6-1.11745 1.87889-0.11428 6-2.5673 1.35097-0.28887 1-0.93926 2.78852-0.69328 1-0.92483 2.12791 0.93133 6-2.48809-0.20416-0.47259 1-3.17429 1.6033 0.58539 1-3.05649 1.82087-1.14475 1-2.54866-0.43302-1.54356 6-0.97353-0.57254 1.53414 1 0.05316-0.56041 1.89971 1-1.4956 0.26862 1.99437 1-1.44724-1.48559 1.90347 6-11.49556-1.74734-0.27361 6-12.96933-1.61557-0.59743 6-10.66537-0.52587-0.2364 6-9.39528-0.33103 0.55482 6-8.37988 0.54331-0.21185 6-7.07378 0.76807 0.52291 6-5.93779 0.23852 0.04763 6-4.54293 0.34204 0.59963 6-3.58484 1.06919-0.37685 6-2.13921 1.10555 0.07549 6-1.20316 0.42985-0.6059 6 0.27404 0.33673-0.34205 6 1.11946 0.92201-1.50055 6 2.5953 0.70917-1.30814 6 3.56314 1.62316-1.14926 6 5.0014 1.18407-0.9616 6 5.56122 1.42531 0.46352 6 7.00833 1.03293 0.57844 6 7.55712 0.04671 1.30193 6 9.05316-0.19144 1.25337 6 9.46499-1.48674 0.50887 6 10.94919-1.72314 0.55613 6 11.8291-1.72947-0.45413 6 13.29622-1.97922-0.2002 6-11.12757-2.99931 0.49255 6-7.16917 1.60848 1.77329 6-1.8657 1.93803 1.30494 6 11.48019-1.50213-1.9037 1-11.46427-3.88242-0.05907 1-13.16083-0.7119-1.17875 1-10.05199-3.08662 0.63959 1-11.61742-3.00974 1.47133 1-13.3084-2.47628-1.18216 1-13.56621-1.57462 0.3191 1-11.18728 0.40797-0.45759 1-7.76751 1.11003 2.54416 1-6.19672 1.83494 2.2096 1-7.66898 2.55965 1.55588 1-0.80266 2.042 1.52052 1-2.28451 2.94384 1.18453 1-2.34118 1.50534 2.19221 1 5.46631 2.48969 0.71045 1 5.09363 0.11915-1.19343 1 2.89846-0.33818-1.29115 1 0.808 0.43282-2.43321 1 0.55223 0.83524 0.58907 1-1.53547-0.12225-1.48556 1-3.64566 0.58288-1.35536 1-6.01192-0.33793-0.87464 1 13.64553-2.86054-0.75151 1 13.50384-2.13732 0.86001 1 13.9038-1.13404-0.54528 1 12.04317-0.65049-2.30346 1 10.42038-1.31014-2.06849 S33