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Supporting Information Imidazol(in)ium Hydrogen Carbonates as a Genuine Source of N- Heterocyclic Carbenes (NHCs): Applications to the Facile Preparation of NHC Metal Complexes and to NHC- Organocatalyzed Molecular and Macromolecular Syntheses Maréva Fèvre, 1,2 Julien Pinaud, 1,2 Alexandre Leteneur, 1,2 Yves Gnanou, 1,2 Joan Vignolle, 1,2 * Daniel Taton 1,2 * 1 Centre National de la Recherche Scientifique, Laboratoire de Chimie des Polymères Organiques, UMR 5629, 16 avenue Pey-Berland, F-33607 Pessac cedex, France 2 Université de Bordeaux, Laboratoire de Chimie des Polymères Organiques, UMR 5629, IPB-ENSCBP, F-33607 Pessac cedex, France Karinne Miqueu, 3 Jean-Marc Sotiropoulos 3 3 Université de Pau & des Pays de l Adour, IPREM, UMR CNRS 5254, 2 Avenue du Président P. Angot, 64053 PAU cedex 09, France S1

Contents 1 H NMR spectrum of 2a S3 13 C NMR spectrum of 2a S4 1 H NMR spectrum of 2b S5 13 C NMR spectrum of 2b S6 1 H NMR spectrum of 2c S7 13 C NMR spectrum of 2c S8 1 H NMR spectrum of 4a S9 13 C NMR spectrum of 4a S10 Molecular structure of 2a (short contacts) Molecular structure of 2a (dimer) Crystal data and structure refinement for 2a: DFT calculations S11 S12 S13 S14 S2

1 H NMR spectrum of 2a (MeOD): S3

13 C NMR spectrum of 2a (MeOD): S4

1 H NMR spectrum of 2b (MeOD): S5

13C NMR spectrum of 2b (MeOD): S6

1H NMR spectrum of 2c (MeOD): S7

13C NMR spectrum of 2c (MeOD): S8

S9

1H NMR spectrum of 4a (CDCl3): S10

13C NMR spectrum of 4a (CDCl3): S11

S12

Molecular structure of 2a (with short contacts in dashed line) with atoms depicted as thermal ellipsoids drawn at the 50% probability level: S13

Molecular structure of 2a (showing a dimer) with atoms depicted as thermal ellipsoids drawn at the 50% probability level: S14

Crystal data and structure refinement for 2a: Formula C10 H18 N2 O3 M 214.26 Crystal system monoclinic Space group P2(1)/c a/å 10.3706(17) b/å 9.6865(16) c/å 11.846(2) β/o 93.873(13) U/Å 3 1187.3(3) T /K 123(2) Z 4 ρ/g cm 1 1.199 Shape and color Colorless size (mm) 0.2x0.1x0.1 λ/ Å 1.54178 μ/mm -1 0.731 Unique data 2206 Absorption correction None transmission max/min unique data [Fo > 4σFo)] 1605 parameters/restraints 140 R1, wr2 0.0737, 0.1745 The crystal structures of compound 2a was solved using the charge flipping algorithm implemented in the SUPERFLIP software (L. Palatinus and G. Chapuis, J. Appl. Cryst., 2007, 40, 786-790). All structures were refined using SHELXL-97 (G. M. Sheldrick, Universität Göttingen, 1997). Full-matrix least-squares refinement was performed on F 2 for all unique reflections, minimizing w(fo 2 - Fc 2 )2, with anisotropic displacement parameters for nonhydrogen atoms. The positions of hydrogen atoms were located on a subsequent differential electron-density map. Hydrogen atoms were mostly spotted in Fourier differences but included in idealized positions and refined with a riding model, with Uiso constrained to 1.2 Ueq value of the parent atom (1.5 Ueq when CH3). The positions and isotropic displacement parameters S15

of the remaining hydrogen atoms were refined freely. S16

Computational Details: Calculations were performed with the Gaussian 03 program [S1] using the Density Functional Theory method. [S2] The various structures were fully optimized at B3LYP level. [S3] This functional is built with Becke s three parameter exchange functional [S3a] and the Lee-Yang-Parr correlation functional. [S3c] The 6-31G(d,p) basis set was used. [S4] All atoms were augmented with a single set of polarization functions. The second derivatives were analytically calculated in order to determine if a minimum or a transition state (one negative eigenvalue) existed for the resulting geometry. All total energies and Gibbs free energies have been zero-point energy (ZPE) and temperature corrected using unscaled density functional frequencies. The connection between the transition states and the corresponding minima was confirmed by IRC calculations. [S5] S17

Geometrical parameters for the compounds 2a, 2b and 2c C4 C2 C N2 H1 C1 C3 N1 O1 C4 N2 C2 C1 C O1 O3 H1 C5 O2 N1 C3 O2 H2 C5 O3 CN1 : 1.342 CN2 : 1.342 N1C1 : 1.385 C1C2 : 1.362 N2C2 : 1.366 CH1 : 1.136 H1O1 : 1.597 O1H2 : 0.968 O1C5 :1.268 C5O2 : 1.434 C5O3 : 1.227 N1C3 :1.490 N2C4 : 1.489 CO1 : 2.676 ΣN1 : 360.0 ΣN2 : 359.8 ΣC : 359.9 C4 C2 N2 C1 O1 C5 CN1 : 1.343 CN2 : 1.343 N1C1 : 1.393 C1C2 : 1.357 N2C2 : 1.392 CH1 : 1.085 H1O1 : 2.314 O2H2 : 0.967 O1C5 : 1.265 C5O2 : 1.439 C5O3 : 1.228 N1C3 :1.447 N2C4 : 1.446 CO1 : 2.529 CC5 : 3.211 ΣN1 : 360.0 ΣN2 : 360.0 ΣC : 359.9 N1 C H1 O3 O2 H2 C3 H2 CN1 : 1.406 CN2 : 1.405 N1C1 : 1.465 C1C2 : 1.538 N2C2 : 1.464 CH1 : 1.087 H1O1 : 2.094 O2H2 : 0.969 O1C5 : 1.324 C5O2 : 1.369 C5O3 : 1.210 N1C3 :1.431 N2C4 : 1.425 CO1 : 1.569 CC5 : 2.541 ΣN1 : 356.6 ΣN2 : 360.0 S18

Z-matrices: 2a : Sum of electronic and thermal Free Energies= -726.885285 ua C -0.22982900-0.48457400 0.23200900 C -2.00316700-1.70425300-0.33074500 C -0.92282500-2.53269900-0.27682600 H -3.03489600-1.91412600-0.55952800 H -0.83928600-3.59290400-0.45496400 H 0.34723400 0.46050300 0.48715100 N -1.54773800-0.43555300-0.01369400 N 0.16905100-1.75689700 0.07867200 C -2.33359900 0.82880900 0.05693000 C 1.57768700-2.23087600 0.16157300 H 1.49187100-3.31220700 0.31643300 C -3.31850500 0.77160900 1.22642700 H -3.83478400 1.73165000 1.31255300 H -4.07753600-0.00604800 1.08344000 H -2.79734400 0.58270100 2.16861300 C -3.01113800 1.10153500-1.28721500 H -3.76784400 0.34599400-1.52706200 H -3.51194600 2.07254900-1.24692500 H -2.27749100 1.13349600-2.09690500 H -1.57586300 1.59718700 0.24685600 C 2.29163100-1.59741800 1.35724900 H 1.73792800-1.76384100 2.28573600 H 3.27873300-2.05707400 1.46181000 H 2.43371800-0.52415400 1.20144700 C 2.29582800-1.94818500-1.16246000 H 3.30204500-2.37674600-1.13081500 H 1.76190700-2.39248000-2.00816800 H 2.38185800-0.86772500-1.31069400 C 1.58801800 2.46695400 0.02653400 O 0.57783600 2.03114900 0.65774700 O 1.91392400 3.60033000-0.31151100 O 2.48574700 1.40943700-0.33673500 H 3.20784800 1.87763800-0.78068300 2b : Sum of electronic and thermal Free Energies= -1188.863029 ua C 0.02299700-0.36748900 0.10286000 C -0.64184300-1.20481200 2.05485800 C 0.71466500-1.18820300 2.05290500 H -1.35011600-1.52409500 2.80119900 H 1.43302800-1.48908700 2.79730100 H 0.01983200 0.03936100-0.90281300 N -1.05900700-0.70601400 0.82362700 N 1.11527600-0.67994600 0.81957300 C -0.15694100 2.57442900-1.17028200 O -0.08037100 2.15848400 0.02230500 O -0.39949900 3.67891600-1.64785200 O 0.08536800 1.51586400-2.11516700 H -0.03100600 1.94230300-2.97559800 C 2.48558300-0.49386300 0.39450700 C 3.18729000 0.63763900 0.84324000 S19

C 3.06613500-1.46896500-0.43115100 C 4.51600700 0.76760000 0.42637300 C 4.39621400-1.28396700-0.81756100 C 5.13494900-0.17152000-0.40389700 H 5.07803300 1.63655100 0.75872500 H 4.86394500-2.02881100-1.45635600 C -2.43401400-0.54349000 0.40510400 C -3.17409700 0.54019300 0.90827300 C -2.98055300-1.49361100-0.47183500 C -4.50513500 0.64735900 0.49167700 C -4.31451900-1.33228400-0.85492800 C -5.09043800-0.26679100-0.38897100 H -5.09586000 1.48013600 0.86420200 H -4.75567500-2.05878100-1.53263800 C 2.29338400-2.67830500-0.90227100 H 1.79177400-3.19221000-0.07563800 H 1.52060000-2.40440900-1.62975300 H 2.96086100-3.39412600-1.38745600 C 2.54345100 1.68527300 1.71496800 H 1.66902900 2.11803100 1.21091700 H 2.19982300 1.26471900 2.66753000 H 3.25824200 2.47950300 1.94245200 C 6.55985100 0.02586700-0.86252300 H 6.59899200 0.67238800-1.74762500 H 7.16738400 0.50193000-0.08722300 H 7.03087600-0.92420100-1.13013700 C -2.57007800 1.56827200 1.83045200 H -2.19357400 1.11604500 2.75544700 H -1.72616400 2.06883100 1.33627000 H -3.31938800 2.31350400 2.10701300 C -2.16920100-2.65313900-1.00037300 H -1.42600900-2.32384900-1.73602700 H -1.62769200-3.17238100-0.20294700 H -2.81793000-3.37981800-1.49488800 C -6.51876000-0.09142400-0.84567900 H -6.57114800 0.57637100-1.71415200 H -6.96674900-1.04514800-1.13894600 H -7.13865900 0.35024600-0.06001800 2c : Sum of electronic and thermal Free Energies= -1190.050223 ua C 0.04289200 0.06219000-0.13656100 H 0.06620600 0.73774500 0.71464600 N -1.08004000 0.14702800-0.97724700 N 1.15601400 0.16120800-0.98925100 C -0.18223300-1.51413000 1.84335300 O 0.04343900-1.34924700 0.54884000 O -0.17429300-2.58692900 2.40357400 O -0.43186200-0.34371700 2.50713900 H -0.57010000-0.61164200 3.42809400 C 2.50085300 0.20303400-0.50309700 C 3.32308400-0.94463200-0.47551900 C 3.00580600 1.44765400-0.06696200 C 4.63756400-0.81345500-0.01397600 C 4.32095900 1.52207900 0.39989100 C 5.15608500 0.40309000 0.43482000 H 5.26983100-1.69842800 0.00589400 H 4.70532100 2.48417400 0.73158600 S20

C -2.42413300 0.24280300-0.51331000 C -3.29470000-0.85955800-0.65776300 C -2.88646100 1.44087800 0.07039000 C -4.61800500-0.73219600-0.22522200 C -4.21519000 1.51554800 0.49886000 C -5.09887000 0.44270400 0.35902700 H -5.28751900-1.58227500-0.33741600 H -4.57038900 2.44249100 0.94418100 C 2.15689500 2.69593000-0.10317300 H 1.56955900 2.75152800-1.02357900 H 1.44508200 2.73047400 0.73097000 H 2.78135200 3.59044300-0.03132800 C 2.83468900-2.30494300-0.91712900 H 1.82392000-2.50128900-0.55387900 H 2.82757800-2.39949500-2.01023100 H 3.49490900-3.08676500-0.53249800 C 6.56676700 0.49959900 0.96569400 H 6.60134600 0.28168700 2.04052700 H 7.23152800-0.21392700 0.46958500 H 6.97963300 1.50295200 0.82464000 C -2.82311300-2.16347500-1.25520600 H -2.83024100-2.13526000-2.35267800 H -1.80503500-2.39550800-0.93478400 H -3.47864700-2.98416100-0.95218500 C -1.97603700 2.63191300 0.24798700 H -1.37454100 2.53981100 1.16141200 H -1.27970300 2.73671300-0.58827200 H -2.55519200 3.55528800 0.33411600 C -6.52333400 0.53803100 0.85256400 H -6.61261000 0.16370000 1.88012800 H -6.87901300 1.57265100 0.85190800 H -7.20293500-0.05475000 0.23285400 C -0.70187200 0.14496500-2.39123800 H -0.83178200 1.14372200-2.83498100 H -1.29892500-0.56229400-2.97507600 C 0.77784800-0.26403500-2.33922600 H 0.88673500-1.34534200-2.49545500 H 1.38657800 0.25527900-3.08433700 2 a : Sum of electronic and thermal Free Energies= -650.463170 ua C -0.00002100 0.08087500 0.00000300 C 0.67810600 2.21061000-0.00000800 C -0.67812700 2.21061300-0.00006500 H 1.38457000 3.02465700-0.00001900 H -1.38458600 3.02466300-0.00012200 N 1.08654400 0.88440800 0.00006600 N -1.08657600 0.88441000-0.00006400 C 2.51506000 0.45608400 0.00016500 C -2.51509900 0.45605400-0.00006900 H -3.06795100 1.40169800-0.00022600 C 2.85464700-0.30563800-1.28523200 H 3.91588400-0.57105600-1.27464000 H 2.25871200-1.21554200-1.37979300 H 2.66616700 0.31765200-2.16460700 C 2.85434400-0.30600100 1.28541600 H 2.25843500-1.21597000 1.37954100 H 3.91560400-0.57132100 1.27505400 S21

H 2.66556400 0.31700300 2.16494000 H 3.06786600 1.40175600 0.00037400 C -2.85456500-0.30570500 1.28533400 H -2.66616700 0.31763200 2.16469300 H -3.91576000-0.57129400 1.27476700 H -2.25847700-1.21551100 1.37990300 C -2.85446700-0.30601600-1.28530100 H -3.91570200-0.57145800-1.27478400 H -2.66588800 0.31705400-2.16481100 H -2.25849500-1.21592200-1.37955900 C 0.00004100-1.48911800-0.00006800 O -0.00022000-1.97299400 1.14378400 O 0.00033600-1.97279400-1.14400600 2 b : Sum of electronic and thermal Free Energies= -1112.452600 ua N 1.08534200 0.00001300 0.87408300 N -1.08533800 0.00001500 0.87409100 C 2.45812500-0.00042000 0.41794600 C 3.09138200-1.23195000 0.19865400 C 3.09091300 1.23162300 0.19355700 C 4.42928200-1.20283000-0.20557300 C 4.42757800 1.20199600-0.21103400 C 5.11566600-0.00101500-0.40397200 H 4.94033100-2.14521400-0.38473700 H 4.93750200 2.14419000-0.39525200 C -2.45812300 0.00043500 0.41796100 C -3.09090500-1.23161900 0.19358700 C -3.09139000 1.23195400 0.19866500 C -4.42756800-1.20200800-0.21099600 C -4.42929700 1.20281800-0.20555400 C -5.11566800 0.00100000-0.40394300 H -4.93748400-2.14420900-0.39520400 H -4.94035700 2.14519600-0.38471500 C 2.33623900 2.53193400 0.31570300 H 1.52875800 2.55826200-0.42552800 H 1.88439800 2.65546600 1.30627300 H 2.99960900 3.38165700 0.13940500 C 2.33816100-2.53272100 0.32473800 H 1.88593000-2.65379000 1.31541700 H 1.53109800-2.56214800-0.41682700 H 3.00246300-3.38229600 0.15129400 C 6.56911600 0.00189300-0.81337400 H 7.22376400 0.12889000 0.05781700 H 6.84938300-0.93632400-1.29987200 H 6.78714600 0.82166800-1.50435000 C -2.33621500-2.53192000 0.31574300 H -1.52873400-2.55824400-0.42548600 H -1.88437300-2.65544000 1.30631400 H -2.99957500-3.38165300 0.13945100 C -6.56911000-0.00195200-0.81337800 H -6.78684300-0.82106100-1.50524200 H -7.22373500-0.13012700 0.05765600 H -6.84968100 0.93668600-1.29888000 C -2.33818500 2.53273500 0.32473700 H -1.88594900 2.65381600 1.31541300 H -1.53112700 2.56216800-0.41683300 H -3.00249800 3.38230100 0.15129200 S22

C -0.00000600-0.00000100-1.47421700 O -0.00149400 1.14729000-1.95370200 O 0.00148000-1.14729800-1.95368500 C -0.00000100 0.00001100 0.07538300 C 0.67809900 0.00004100 2.20798800 H 1.39188600 0.00005300 3.01539300 C -0.67808600 0.00000300 2.20799300 H -1.39186700-0.00000800 3.01540200 2 c : Sum of electronic and thermal Free Energies= -1113.638777 ua N 1.10220500-0.00033900 0.86101400 N -1.10220400 0.00037500 0.86101900 C 2.45743000-0.00059100 0.37486700 C 3.09832200-1.22949100 0.15041000 C 3.09786000 1.22895000 0.14601600 C 4.43194100-1.20205700-0.26760200 C 4.43025400 1.20119400-0.27233000 C 5.11723800-0.00098900-0.47270300 H 4.94110900-2.14466000-0.45209000 H 4.93826400 2.14370700-0.46130400 C -2.45743200 0.00061200 0.37487900 C -3.09786400-1.22894800 0.14604900 C -3.09832700 1.22949400 0.15040800 C -4.43024500-1.20120500-0.27230000 C -4.43195900 1.20204500-0.26760000 C -5.11724000 0.00098100-0.47269600 H -4.93826000-2.14372100-0.46125000 H -4.94113200 2.14464500-0.45208300 C 2.34957100 2.53267700 0.27571300 H 1.52031900 2.55429300-0.44044000 H 1.92974000 2.67357800 1.27879000 H 3.00949000 3.37915100 0.07157500 C 2.35149200-2.53369300 0.28357600 H 1.93148600-2.67246200 1.28686600 H 1.52248900-2.55802100-0.43277200 H 3.01230100-3.38003400 0.08179700 C 6.56670600 0.00194400-0.89630200 H 7.23044300 0.12937700-0.03198900 H 6.84236100-0.93646300-1.38522600 H 6.77805300 0.82134100-1.58991400 C -2.34955600-2.53266100 0.27576200 H -1.52033400-2.55428700-0.44042400 H -1.92968300-2.67352500 1.27882600 H -3.00947100-3.37915200 0.07167600 C -6.56669500-0.00201400-0.89633900 H -6.77767300-0.82062800-1.59099500 H -7.23041100-0.13083300-0.03221700 H -6.84272200 0.93688600-1.38410100 C -2.35152300 2.53371300 0.28355500 H -1.93150900 2.67250100 1.28683900 H -1.52252500 2.55805100-0.43280000 H -3.01235400 3.38003500 0.08177300 C 0.00000300-0.00000700-1.43646300 O -0.00141100 1.14793300-1.91273300 O 0.00141700-1.14796000-1.91270200 C -0.00000100 0.00001200 0.11213700 C 0.77348800 0.00136400 2.30341100 S23

H 1.19473000 0.88926600 2.78436100 H 1.19792000-0.88330100 2.78739200 C -0.77347400-0.00131600 2.30341900 H -1.19471300-0.88921300 2.78437800 H -1.19790100 0.88335600 2.78739000 6a : Sum of electronic and thermal Free Energies= -461.878682 ua C 0.41489900 0.00014000 0.00000000 C -1.78460200-0.00042500 0.67869000 C -1.78460200-0.00042500-0.67869000 H -2.60164500-0.00072500 1.38423000 H -2.60164500-0.00072500-1.38423000 N -0.44711300-0.00005100 1.06250900 N -0.44711300-0.00005100-1.06250900 C 0.01885600-0.00004200 2.46105600 C 0.01885600-0.00004200-2.46105600 H -0.88769800-0.00038400-3.07810000 C 0.81990500 1.27209100 2.75486600 H 1.15661800 1.28155500 3.79658600 H 1.69202900 1.31764200 2.09775600 H 0.21244400 2.16516100 2.57940100 C 0.82071500-1.27169600 2.75470300 H 1.69288800-1.31665900 2.09762400 H 1.15740200-1.28108300 3.79643800 H 0.21380500-2.16513600 2.57915100 H -0.88769800-0.00038400 3.07810000 C 0.82071500-1.27169600-2.75470300 H 0.21380500-2.16513600-2.57915100 H 1.15740200-1.28108300-3.79643800 H 1.69288800-1.31665900-2.09762400 C 0.81990500 1.27209100-2.75486600 H 1.15661800 1.28155500-3.79658600 H 0.21244400 2.16516100-2.57940100 H 1.69202900 1.31764200-2.09775600 6b : Sum of electronic and thermal Free Energies= -923.865006 ua C 0.00005300 0.00059800-0.27905500 C -0.67690700 0.00667400 1.93455800 C 0.67692000-0.01158800 1.93455700 H -1.38597300 0.02029500 2.74763100 H 1.38598900-0.02727700 2.74759300 N -1.06405600 0.01168100 0.59106100 N 1.06408800-0.01288200 0.59104900 C 2.43468400-0.02850500 0.15762800 C 2.98052300-1.22136100-0.34527900 C 3.19448000 1.14863700 0.24263500 C 4.31850100-1.21436500-0.74863000 C 4.53108000 1.10382700-0.16819200 C 5.11327600-0.06678700-0.66072300 H 4.74944800-2.13135700-1.14410700 H 5.12647500 2.01213600-0.11120100 C -2.43462600 0.02823600 0.15762600 C -2.97998400 1.22171800-0.34437500 C -3.19495900-1.14864400 0.24169100 C -4.31794700 1.21557100-0.74777400 S24

C -4.53155000-1.10293100-0.16908600 C -5.11324300 0.06828700-0.66074800 H -4.74849300 2.13305900-1.14253900 H -5.12731200-2.01104200-0.11278700 C -2.58629200-2.44100800 0.73079300 H -1.65396100-2.65907000 0.20060600 H -2.34191800-2.40348900 1.79830400 H -3.27498500-3.27527300 0.57578400 C -2.14253600 2.47102500-0.46318500 H -1.75889200 2.78982700 0.51277500 H -1.27338100 2.29129500-1.10293800 H -2.72812500 3.29285000-0.88289800 C -6.56609700 0.10164500-1.07321000 H -7.20017600 0.48358500-0.26324300 H -6.72131400 0.75303000-1.93881900 H -6.93216800-0.89644800-1.33049200 C 2.14345300-2.47081300-0.46519600 H 1.76002800-2.79073500 0.51047900 H 1.27416700-2.29073500-1.10469100 H 2.72920800-3.29204700-0.88583200 C 6.56615900-0.09924400-1.07316300 H 7.20035900-0.48160300-0.26348200 H 6.72165100-0.74989300-1.93927700 H 6.93185700 0.89919300-1.32961600 C 2.58511400 2.44024000 0.73284300 H 1.65354600 2.65907900 0.20162000 H 2.33913400 2.40097000 1.79992000 H 3.27399100 3.27478000 0.58015100 6c : Sum of electronic and thermal Free Energies= -925.047214 ua C -0.00000600-0.00006000-0.22035600 N -1.07680200-0.06311200 0.59795500 N 1.07679600 0.06324000 0.59793500 C 2.42916500 0.00137700 0.13201700 C 2.90686700-1.17684800-0.47617700 C 3.27019300 1.11593900 0.29851900 C 4.23644200-1.21525200-0.90242500 C 4.59725200 1.02685300-0.13748900 C 5.10238900-0.12924300-0.73467700 H 4.60596400-2.12090200-1.37853100 H 5.24632300 1.89159900-0.01762500 C -2.42917300-0.00134700 0.13202200 C -2.90692400 1.17679400-0.47629400 C -3.27014400-1.11592700 0.29864700 C -4.23650400 1.21509900-0.90253700 C -4.59720700-1.02695000-0.13737300 C -5.10239700 0.12906400-0.73467600 H -4.60607000 2.12068300-1.37873400 H -5.24624100-1.89170900-0.01741200 C -2.76266200-2.40052500 0.90909100 H -1.73580600-2.60783400 0.59628500 H -2.76895700-2.36458300 2.00619800 H -3.39173300-3.24424000 0.61292300 C -2.00534000 2.36940700-0.68381800 H -1.60540200 2.74238000 0.26664900 H -1.14549300 2.10140200-1.30468900 H -2.54920400 3.18799500-1.16246000 S25

C -6.54477900 0.21434400-1.17536900 H -7.16076000 0.72494300-0.42439000 H -6.64526000 0.77567300-2.10964000 H -6.97572100-0.77914200-1.32955000 C 2.00524700-2.36945900-0.68356200 H 1.60523600-2.74225400 0.26694400 H 1.14544500-2.10152800-1.30452700 H 2.54911300-3.18814700-1.16203200 C 6.54476900-0.21463000-1.17535300 H 7.16081000-0.72478200-0.42411700 H 6.64528000-0.77643400-2.10933300 H 6.97562600 0.77881200-1.33005600 C 2.76279800 2.40064600 0.90881000 H 1.73582100 2.60779400 0.59629800 H 2.76948700 2.36498600 2.00592500 H 3.39169400 3.24434100 0.61220900 C -0.76331800 0.07192000 2.04766000 H -1.26329400-0.69829700 2.64046000 H -1.09459800 1.05132100 2.41570200 C 0.76331300-0.07140600 2.04767800 H 1.26328900 0.69896800 2.64027000 H 1.09459600-1.05071000 2.41597600 6a +CO2 +H2O : Sum of electronic and thermal Free Energies= -726.876331 ua C 0.00000400-0.32084200 0.35062900 C -0.67764100-2.49005900 0.08124100 C 0.67765200-2.49005100 0.08118700 H -1.38157300-3.30375500-0.00328200 H 1.38158500-3.30374100-0.00338300 N -1.06810200-1.16640900 0.24980700 N 1.06811100-1.16640800 0.24980200 C -2.49019100-0.76253500 0.24221600 C 2.49020000-0.76253000 0.24220400 H 3.01663700-1.53941400 0.81108100 C -3.02527400-0.75837700-1.19646700 H -4.09110300-0.50942600-1.20472100 H -2.48935200-0.01545300-1.79540100 H -2.89996000-1.73422600-1.67557500 C -2.72124300 0.57731100 0.93939100 H -2.33072200 1.40730700 0.34561400 H -3.79856200 0.72729600 1.06185400 H -2.23815700 0.62510200 1.91690000 H -3.01662300-1.53942000 0.81109800 C 2.72125200 0.57731900 0.93937400 H 2.23817100 0.62511300 1.91688500 H 3.79857200 0.72730900 1.06183000 H 2.33072500 1.40730900 0.34559400 C 3.02527300-0.75837300-1.19648300 H 4.09110100-0.50942100-1.20474400 H 2.89995500-1.73422200-1.67559000 H 2.48934700-0.01544900-1.79541400 C -0.00001600 2.31369000-1.33470400 O -0.00006200 1.62854900-2.28261200 O 0.00002700 3.05209900-0.42732400 O 0.00000700 1.64741800 2.55467500 H 0.00000600 1.09129300 1.74054000 S26

H 0.00001600 2.54565900 2.20000400 6b +CO2 +H2O : Sum of electronic and thermal Free Energies= -1188.867601 ua C 0.00199100 0.16310400-0.15446000 C 0.68344400 0.41943500-2.33397900 C -0.67167300 0.42039000-2.33630600 H 1.39645300 0.52048700-3.13698000 H -1.38173800 0.52256700-3.14177200 N 1.07179700 0.26184200-1.00356300 N -1.06476400 0.26315000-1.00723700 C -0.02009100-1.88529900 2.36970300 O -0.02043300-2.74711700 1.57880600 O -0.02028600-1.07051000 3.20743000 C -2.44440200 0.18983400-0.59358700 C -3.11391900-1.04203300-0.69566400 C -3.08875100 1.34808900-0.12937100 C -4.45818000-1.09329300-0.31692100 C -4.43547400 1.24135800 0.23709900 C -5.13564800 0.03548300 0.15496900 H -4.98738000-2.04034400-0.39289500 H -4.94803100 2.13095000 0.59530700 C 2.45020900 0.18660400-0.58614400 C 3.09462200 1.34344900-0.11868800 C 3.11597000-1.04804600-0.67924600 C 4.43853900 1.23321900 0.25707300 C 4.45747300-1.10274600-0.29144600 C 5.13721000 0.02641500 0.17635600 H 4.94923400 2.12026400 0.62410600 H 4.98195300-2.05339200-0.35426500 C -2.40782000-2.28407700-1.18479700 H -1.99630200-2.15161800-2.19101800 H -1.57034400-2.54474000-0.53014200 H -3.09624300-3.13234700-1.21180500 C -6.57994900-0.05436900 0.58807900 H -7.12963100-0.79563600 0.00012600 H -6.65855100-0.35224800 1.64108100 H -7.08978700 0.90784000 0.48415700 C -2.36468100 2.66511000 0.00082000 H -1.68182500 2.64607300 0.85878700 H -1.76649200 2.88893200-0.88803900 H -3.07855900 3.48051800 0.14468700 C 2.40637100-2.29093900-1.16108300 H 1.56878800-2.54656500-0.50455000 H 1.99421000-2.16220400-2.16751300 H 3.09278800-3.14093600-1.18476200 C 6.59677900-0.05250100 0.55742900 H 6.84887900-1.03174500 0.97553000 H 7.24287100 0.10350900-0.31559700 H 6.85911000 0.70994200 1.29648200 C 2.37163200 2.66103500 0.01208000 H 1.77622600 2.88681900-0.87814000 H 1.68630100 2.64165000 0.86805700 H 3.08604400 3.47543100 0.15898900 O -0.00220200 1.84979300 2.22522100 H -0.00066900 1.13629700 1.54194500 H -0.00506500 1.36689700 3.06067400 S27

6c +CO2 +H2O : Sum of electronic and thermal Free Energies= -1189.045332 ua C 0.00775400-0.00043900-0.18086300 N 1.09082600 0.15933200-0.97072800 N -1.07083700 0.15299000-0.97823900 C -0.08937400-0.86510300 2.46478300 O -0.08276300-2.00258900 2.18939400 O -0.10536100 0.20840900 2.93926000 C -2.43248100 0.01605000-0.54871600 C -2.99256000-1.27116700-0.44087300 C -3.19922000 1.16467900-0.27917500 C -4.32941200-1.38784200-0.04917400 C -4.53410000 0.99585100 0.10598800 C -5.11888500-0.26724400 0.22507600 H -4.76371300-2.38105100 0.04168300 H -5.12991500 1.87962800 0.32307900 C 2.45006100 0.00695900-0.53762600 C 3.24338300 1.14941500-0.31775500 C 2.98403200-1.28606200-0.38585900 C 4.57628400 0.96695600 0.06467500 C 4.32169200-1.41586000 0.00215300 C 5.13409300-0.30345300 0.23436200 H 5.19338700 1.84585000 0.23789500 H 4.73800100-2.41375400 0.12063800 C -2.17140600-2.50775500-0.71666900 H -1.66363700-2.45255600-1.68552500 H -1.39606400-2.64203300 0.04354000 H -2.80482400-3.39877300-0.71915700 C -6.57079100-0.41960500 0.61372700 H -7.20975000-0.52887000-0.27162700 H -6.72795700-1.30621200 1.23585600 H -6.92995700 0.45176000 1.16888900 C -2.60570600 2.54964200-0.37254000 H -1.72393100 2.65752100 0.26838900 H -2.29178300 2.79038800-1.39520300 H -3.34360100 3.30069900-0.07652400 C 2.13946100-2.51643200-0.61523500 H 1.37975200-2.62027700 0.16526900 H 1.61026500-2.47709400-1.57317300 H 2.75986900-3.41659000-0.60978200 C 6.56796300-0.46620100 0.68127200 H 6.97334800-1.43704800 0.38161000 H 7.20986100 0.31412200 0.26069400 H 6.65268200-0.40042300 1.77327100 C 2.68187000 2.54319800-0.46411600 H 2.34502000 2.74372000-1.48800900 H 1.82536600 2.70593700 0.19803200 H 3.44632600 3.28740200-0.22407300 O 0.09511000 2.91750100 1.68909000 H 0.03635200 2.03943100 2.09587700 H -0.17765000 3.52662700 2.38622600 C -0.75474700 0.41131400-2.40851900 H -1.15791400 1.37768200-2.72776900 H -1.19727200-0.36360800-3.04389800 C 0.78168400 0.38062800-2.40909100 S28

H 1.19068400-0.43617000-3.01472800 H 1.22368000 1.31568800-2.76561300 2 a +H2O : Sum of electronic and thermal Free Energies= -726.883230 ua C -0.00001100-0.25554000 0.08238700 C 0.67815700-1.59825900-1.56105800 C -0.67813500-1.59827500-1.56106400 H 1.38456500-2.10649500-2.19663300 H -1.38452700-2.10652500-2.19664500 N 1.08678400-0.76170200-0.53482100 N -1.08678600-0.76173000-0.53482700 C 2.51714100-0.49043500-0.21178700 C -2.51713600-0.49041100-0.21183800 H -3.05845800-1.01472600-1.00628000 C 2.88895500-1.11371600 1.13744100 H 3.94669000-0.92486100 1.34354800 H 2.28881200-0.68562200 1.94375200 H 2.72915100-2.19621900 1.12651300 C 2.84311800 1.00328900-0.31404300 H 2.43317200 1.56233700 0.52890200 H 3.93049700 1.12519900-0.31861600 H 2.42381600 1.43186000-1.22776100 H 3.05846200-1.01482000-1.00618300 C -2.84303100 1.00334700-0.31402700 H -2.42301800 1.43209200-1.22733900 H -3.93040300 1.12527800-0.31940700 H -2.43371500 1.56221100 0.52934600 C -2.88902700-1.11373900 1.13734500 H -3.94670600-0.92465300 1.34352800 H -2.72947700-2.19628000 1.12631200 H -2.28874400-0.68585000 1.94366100 C -0.00003200 0.71381700 1.30058500 O -0.00002900 0.13530300 2.39536100 O -0.00004800 1.92740200 0.98748400 O 0.00011700 2.24846400-1.76160800 H 0.00008400 2.24706500-0.77604900 H -0.00049800 3.18421000-1.99666200 2 b +H2O : Sum of electronic and thermal Free Energies= -1188.873535 ua C 0.00021200-0.12351100 0.07966600 C -0.68010600 0.00372600 2.20709900 C 0.67516200 0.00401600 2.20881000 H -1.39522000 0.04910300 3.01181700 H 1.38821600 0.04979400 3.01533500 N -1.08796400-0.07570800 0.87787800 N 1.08632000-0.07522300 0.88060800 C 0.00257800-0.31280600-1.46509200 O 0.00978900-1.50752100-1.80208200 O -0.00337100 0.74098800-2.12947400 C 2.47133900-0.12216600 0.45394000 C 3.04391100-1.37471100 0.17578900 C 3.19598500 1.07916700 0.38194800 C 4.38584900-1.39511800-0.21336300 C 4.53590400 0.99345600-0.00986000 C 5.14435000-0.22569300-0.32091900 H 4.84718600-2.35363700-0.43660000 S29

H 5.11615000 1.91032400-0.07428700 C -2.47225100-0.12205800 0.44873100 C -3.19526300 1.07980900 0.37342900 C -3.04349400-1.37377600 0.16304600 C -4.53307900 0.99559800-0.02642600 C -4.38290000-1.39254700-0.23420300 C -5.14208300-0.22296200-0.33756100 H -5.11015800 1.91376300-0.09954500 H -4.84126500-2.34961400-0.46965000 C 2.25246900-2.65411800 0.28393500 H 1.79423400-2.76214400 1.27389600 H 1.44821800-2.66713700-0.45961200 H 2.89956900-3.51854300 0.11850900 C 6.58134800-0.27770100-0.78129600 H 7.06692100-1.20890500-0.47501600 H 6.64260000-0.22320300-1.87508100 H 7.16157700 0.55829400-0.38032500 C 2.57774400 2.41710600 0.70420200 H 1.80446400 2.70356800-0.02005700 H 2.10614500 2.42117100 1.69306400 H 3.34565100 3.19479700 0.70318900 C -2.25132700-2.65324700 0.26591200 H -1.44597300-2.66340100-0.47648100 H -1.79424100-2.76503600 1.25598000 H -2.89797000-3.51723400 0.09643100 C -6.59525800-0.28089800-0.74410500 H -6.77338900-1.07462900-1.47552400 H -7.23868200-0.48516500 0.12074700 H -6.92597500 0.66522000-1.18135100 C -2.57620400 2.41770600 0.69418100 H -2.10613800 2.42258800 1.68375900 H -1.80147700 2.70260800-0.02909600 H -3.34342400 3.19607200 0.69111000 O 0.00455600 3.25767900-1.17663400 H 0.00226100 2.34167700-1.54999200 H 0.00511300 3.83137600-1.95228600 2 c +H2O : Sum of electronic and thermal Free Energies= -1190.058126 ua C 0.00030300-0.04068800 0.11480700 N -1.10435800 0.00480000 0.86199300 N 1.10491700 0.00513100 0.86200600 C 0.00029400-0.18773000-1.43419100 O 0.00834800-1.37106200-1.80466700 O -0.00803700 0.88930200-2.05964700 C 2.46900600-0.10546600 0.40338700 C 2.99580400-1.38525800 0.14796300 C 3.25219500 1.05820100 0.29305400 C 4.33072500-1.47373500-0.25583700 C 4.58203000 0.90823300-0.11301400 C 5.13702200-0.34158600-0.40041300 H 4.74786900-2.45621400-0.46210500 H 5.19854100 1.79859400-0.20813900 C -2.46828400-0.10729900 0.40321900 C -3.25395900 1.05558200 0.29809800 C -2.99259800-1.38670500 0.14256800 C -4.58333200 0.90499300-0.10799400 C -4.32778600-1.47586600-0.26138300 S30

C -5.13615200-0.34494500-0.40070000 H -5.20159800 1.79464500-0.19887200 H -4.74305800-2.45815100-0.47206300 C 2.15728700-2.63217200 0.28347200 H 1.68763400-2.70461600 1.27179200 H 1.35929300-2.63294000-0.46612000 H 2.77257400-3.52430400 0.14465500 C 6.56481300-0.46430100-0.87589800 H 7.00632800-1.41914900-0.57584200 H 6.61822500-0.41045500-1.97018800 H 7.19033000 0.34092100-0.47968800 C 2.70477000 2.43167200 0.59403800 H 1.85837000 2.70164800-0.04782000 H 2.36090800 2.51524700 1.63217600 H 3.48497700 3.18462100 0.45541900 C -2.15236300-2.63308400 0.27292000 H -1.35454000-2.63065700-0.47686300 H -1.68227500-2.70863900 1.26079600 H -2.76672800-3.52537700 0.13113900 C -6.56429700-0.46675200-0.87537100 H -6.62776800-0.33246900-1.96216000 H -6.98084000-1.45115500-0.64371600 H -7.20558600 0.29204200-0.41695900 C -2.70832400 2.42863400 0.60422800 H -2.35962400 2.50724700 1.64111800 H -1.86560300 2.70365000-0.04029200 H -3.49086900 3.18053700 0.47332100 O -0.00589600 3.38184700-1.03595300 H -0.00753300 2.48206500-1.44450800 H -0.00524300 3.98525300-1.78883200 C 0.77210500 0.06467300 2.30370900 H 1.18895300 0.97146800 2.74900200 H 1.20179400-0.80029200 2.81758300 C -0.77158700 0.05765400 2.30396800 H -1.19299600-0.81517400 2.81160700 H -1.19682000 0.95711500 2.75593900 TS6a 2a : Sum of electronic and thermal Free Energies= -726.869427 ua C -0.46850000-0.30967300 0.18738300 C -0.49325700-2.51221800-0.27592400 C -1.77167400-2.05841700-0.36897100 H -0.08907900-3.50020900-0.42375000 H -2.68679900-2.57517900-0.61170800 H -0.10403900 0.94588000 0.40321100 N 0.29029400-1.41950500 0.06715800 N -1.73495600-0.70350300-0.08103900 C 1.76322100-1.43045900 0.23376900 C -2.90357700 0.21012600-0.11258200 H -3.75617300-0.43604600-0.34877700 C 2.44627400-1.78351200-1.08916400 H 3.53155700-1.74014400-0.96144500 H 2.18665000-2.79354000-1.42558100 H 2.16864900-1.06182500-1.85985400 C 2.16441200-2.35204400 1.38847800 H 1.93119200-3.40032700 1.17146900 H 3.24264700-2.28069200 1.55696700 S31

H 1.65421000-2.07040800 2.31404600 H 2.01681600-0.39703900 0.47378400 C -2.73088900 1.25882000-1.21652300 H -2.57584500 0.78348100-2.18946800 H -3.63018900 1.87957000-1.27680700 H -1.87382600 1.90088800-0.99221000 C -3.12264700 0.84861800 1.26195200 H -4.04555000 1.43596600 1.25254100 H -3.20379700 0.09043000 2.04630800 H -2.29413200 1.52104900 1.49920300 C 1.93108500 2.48253400-0.17008900 O 2.13987500 1.59061800-0.94411200 O 2.29135100 3.45112500 0.42603400 O 0.14652600 2.18687900 0.41258100 H 0.13162700 2.60756900 1.28323900 TS6b 2b : Sum of electronic and thermal Free Energies= -1188.851004 ua C 0.08361300-0.36687600 0.05064100 C -0.53427200-1.79348700 1.69848500 C 0.82188900-1.74787600 1.68762800 H -1.22452200-2.34004000 2.32079700 H 1.55642900-2.24396400 2.30145300 H 0.09552800 0.63195100-0.91388200 N -0.96750200-0.93905500 0.68794300 N 1.18085800-0.86942600 0.66913100 C -0.61827200 2.99359600-1.00654900 O -0.30118900 3.05800100 0.15869800 O -1.25566000 3.48322200-1.89844000 O 0.19891800 1.56964900-1.66565600 H -0.24666300 1.41847700-2.51129700 C 2.54417400-0.53479800 0.32394900 C 3.10967500 0.63840500 0.84894400 C 3.25694000-1.40450900-0.51532400 C 4.43671800 0.91905400 0.50925400 C 4.58041500-1.07545900-0.82156400 C 5.18599800 0.08153500-0.32259800 H 4.89359100 1.82212500 0.90612500 H 5.14786800-1.73809400-1.47025600 C -2.35542100-0.69766600 0.36521900 C -3.04645400 0.31616200 1.04801600 C -2.96812400-1.50014100-0.61030300 C -4.39238200 0.51057500 0.72028200 C -4.31390600-1.26078200-0.89994000 C -5.04092500-0.25817700-0.25004600 H -4.94410100 1.29222200 1.23605900 H -4.80380700-1.87273200-1.65330800 C 2.62139300-2.64872300-1.08845100 H 2.30371600-3.34737200-0.30661100 H 1.73096300-2.40440000-1.67760600 H 3.32311700-3.17368700-1.74058600 C 2.32160200 1.57543900 1.72897200 H 1.54616800 2.10076100 1.15879400 H 1.82015100 1.03954200 2.54203000 H 2.98113000 2.32361100 2.17555900 C 6.60648900 0.43531400-0.69360600 H 6.62729900 1.17838000-1.49997300 S32

H 7.14628600 0.86570300 0.15550700 H 7.16089600-0.44116400-1.04039600 C -2.36976600 1.18969100 2.07515700 H -1.80341500 0.60038700 2.80352200 H -1.66950400 1.88204900 1.59347400 H -3.11020500 1.77963100 2.62069000 C -2.20661800-2.58568700-1.33316500 H -1.36873500-2.17361200-1.90581500 H -1.78589500-3.32088200-0.63841000 H -2.86072500-3.11641600-2.02860200 C -6.48339000 0.00760200-0.60852300 H -6.55613200 0.77381500-1.38989200 H -6.97581300-0.89285100-0.98686300 H -7.04991400 0.36979100 0.25428300 TS6c 2c : Sum of electronic and thermal Free Energies= -1190.033890 ua C 0.10343300-0.38436700 0.08949600 H 0.09266600 0.62065500-0.87084400 N -0.96263600-0.91777300 0.69372200 N 1.21774000-0.88945300 0.62907100 C -0.73774800 2.94150700-0.92334000 O -0.42271300 2.99444500 0.24283800 O -1.39876100 3.41633100-1.80534100 O 0.15529700 1.57359100-1.61341500 H -0.28394600 1.41626900-2.46129700 C 2.55891300-0.50393700 0.27859400 C 3.09831700 0.68174400 0.80762700 C 3.30651600-1.34287000-0.56648600 C 4.41546300 1.00757500 0.46751300 C 4.61796600-0.97235400-0.87417100 C 5.18955400 0.19995200-0.36973100 H 4.84416400 1.92279100 0.86824600 H 5.20373000-1.61276500-1.52943200 C -2.33360400-0.67042700 0.33540800 C -3.07522200 0.27287500 1.06778300 C -2.90847400-1.40359800-0.71801700 C -4.41675700 0.46256300 0.72016200 C -4.25119000-1.17354900-1.02806500 C -5.02157700-0.24366500-0.32266400 H -4.99980800 1.19236500 1.27622200 H -4.70456500-1.73383400-1.84238600 C 2.71650200-2.60687400-1.14560300 H 2.55980700-3.37763100-0.38075900 H 1.74617300-2.41857500-1.61519400 H 3.38153700-3.03137500-1.90152400 C 2.28821000 1.59470600 1.69392500 H 1.49349600 2.10006900 1.13284200 H 1.80695700 1.04733500 2.51220000 H 2.92835500 2.36059700 2.13908000 C 6.59626900 0.59903100-0.74719200 H 6.60033800 1.20295800-1.66291900 H 7.06690800 1.19748900 0.03817700 H 7.22605100-0.27625200-0.93224200 C -2.44726200 1.09739600 2.16455300 H -1.89816700 0.48208300 2.88531300 H -1.74209400 1.82183600 1.74186300 S33

H -3.21386900 1.64863800 2.71474900 C -2.10323300-2.40239600-1.51599200 H -1.27976600-1.91818400-2.05219800 H -1.65874700-3.17814700-0.88225500 H -2.73399700-2.90130400-2.25550400 C -6.46047300 0.01466400-0.70060100 H -6.52907700 0.80219300-1.46093800 H -6.93395800-0.88041800-1.11480700 H -7.04789200 0.34356400 0.16145800 C -0.59622000-1.92022800 1.72535500 H -0.93892300-2.91485500 1.41996100 H -1.06853100-1.67791100 2.68092200 C 0.93982600-1.80407600 1.76483400 H 1.30703100-1.36085500 2.69658500 H 1.44454900-2.76311400 1.62214900 TS6a 2 a : Sum of electronic and thermal Free Energies= -650.453381 ua C -0.00009500-0.16157700 0.00010600 C 0.67825900-2.33469400-0.00079400 C -0.67758800-2.33493700-0.00137800 H 1.38470300-3.14991500-0.00097300 H -1.38371800-3.15042400-0.00215100 N 1.07119300-1.00123000 0.00010500 N -1.07106300-1.00163000-0.00086800 C 2.48889300-0.57230000 0.00123900 C -2.48887200-0.57297300-0.00059100 H -3.06125800-1.50756900-0.00209700 C 2.82524800 0.19898200 1.28144300 H 3.88755100 0.46223800 1.28682100 H 2.23721700 1.11572100 1.35846100 H 2.61846200-0.41077100 2.16604500 C 2.82796900 0.19730500-1.27926000 H 2.24044400 1.11417600-1.35876000 H 3.89036600 0.46025300-1.28282000 H 2.62288900-0.41355200-2.16350200 H 3.06132200-1.50687200 0.00243200 C -2.82597800 0.19961200-1.27980500 H -2.62077800-0.40956300-2.16517200 H -3.88795300 0.46417900-1.28382400 H -2.23673400 1.11559300-1.35636000 C -2.82671500 0.19577800 1.28075600 H -3.88908200 0.45879700 1.28563800 H -2.62062300-0.41557800 2.16441600 H -2.23888900 1.11248600 1.35987500 C -0.00046400 2.06572300-0.00051400 O -0.00237100 2.33761400 1.15915900 O 0.00127600 2.33680100-1.16039700 TS6b 2 b : Sum of electronic and thermal Free Energies= -1112.444411 ua C 0.00000700 0.01156500-0.07344300 C -0.67769100 0.17201600-2.24839700 C 0.67771600 0.17200600-2.24839400 H -1.38989100 0.22986700-3.05627000 H 1.38992100 0.22983700-3.05626400 N -1.07033700 0.07335800-0.91137900 S34

N 1.07035600 0.07334200-0.91137400 C -0.00005800-0.21382100 2.12609300 O -0.00008500 0.91266300 2.50640000 O -0.00005500-1.39721400 2.25735200 C 2.44348000 0.04155800-0.47273600 C 3.09512000 1.25335600-0.19414800 C 3.08218100-1.19907400-0.32668400 C 4.43410800 1.19838900 0.20203400 C 4.42235300-1.19988800 0.07299100 C 5.11731100-0.01516300 0.33234500 H 4.95203400 2.12835100 0.42407400 H 4.93087200-2.15337300 0.19255700 C -2.44346400 0.04159400-0.47274500 C -3.08226400-1.19902000-0.32697300 C -3.09500300 1.25338000-0.19387400 C -4.42243700-1.19982200 0.07269600 C -4.43399600 1.19842700 0.20229500 C -5.11729900-0.01509800 0.33232100 H -4.93103000-2.15329400 0.19204600 H -4.95184800 2.12838000 0.42454800 C 2.36125100 2.57000100-0.26686400 H 1.87948900 2.71934800-1.23871000 H 1.57428400 2.60876200 0.49436500 H 3.04523000 3.40441800-0.09445700 C 6.57389800-0.04109600 0.73078000 H 7.22501200 0.09270100-0.14214700 H 6.80937600 0.76160700 1.43602200 H 6.84446200-0.99268000 1.19691600 C 2.33709000-2.49367600-0.54135800 H 1.55822800-2.61383800 0.21962600 H 1.84482300-2.52683300-1.51882700 H 3.01657100-3.34671700-0.47400900 C -2.36102900 2.56998400-0.26628000 H -1.57419800 2.60857900 0.49509800 H -1.87908600 2.71942700-1.23802000 H -3.04498100 3.40442500-0.09387700 C -6.57388900-0.04100800 0.73074600 H -6.80932200 0.76160400 1.43610600 H -7.22499100 0.09295300-0.14216300 H -6.84450900-0.99264500 1.19674200 C -2.33726200-2.49362900-0.54191200 H -1.84506200-2.52666000-1.51941900 H -1.55835600-2.61395700 0.21900000 H -3.01678400-3.34664500-0.47465200 TS6c 2 c : Sum of electronic and thermal Free Energies= -1113.627965 ua C 0.00339200 0.01595400-0.11406700 N -1.08053500 0.04152800-0.90416800 N 1.08788700 0.08068300-0.90164600 C -0.02211600-0.13285000 2.13334400 O -0.02698700 1.01017500 2.45558700 O -0.02457600-1.30987200 2.29746700 C 2.44466400 0.03233200-0.43558800 C 3.14209800 1.23532200-0.23338700 C 3.05188800-1.21358100-0.19857000 C 4.47666400 1.16753300 0.17791300 C 4.38735800-1.23067100 0.21376400 S35

C 5.12007400-0.05379100 0.39717600 H 5.02228400 2.09384300 0.34169900 H 4.86358300-2.18965200 0.40439700 C -2.43792600 0.02722800-0.43752700 C -3.11491200-1.20011900-0.33801300 C -3.06568600 1.23841900-0.09809200 C -4.45134700-1.18910700 0.07248300 C -4.40256900 1.19913400 0.30832800 C -5.11602000-0.00080700 0.38914200 H -4.98132600-2.13491800 0.15667500 H -4.89523400 2.13058300 0.57756800 C 2.45535700 2.56948200-0.39824500 H 2.05431600 2.70914800-1.40843500 H 1.61526700 2.65783700 0.29850500 H 3.15023200 3.38952800-0.20092300 C 6.57209000-0.10365500 0.81007500 H 7.22651900-0.24508300-0.05923300 H 6.87986300 0.82300200 1.30277700 H 6.76424000-0.93319800 1.49732400 C 2.27151100-2.49921700-0.32790400 H 1.48660200-2.54713400 0.43444000 H 1.78283400-2.59050600-1.30399200 H 2.92687400-3.36438300-0.19971000 C -2.30377600 2.54140100-0.11049200 H -1.51616300 2.52851800 0.65054800 H -1.82105600 2.73116500-1.07533500 H -2.97009800 3.38147800 0.10099300 C -6.57034000-0.00937700 0.79674700 H -6.78803100 0.78418500 1.51782700 H -7.22515400 0.15037300-0.06914100 H -6.85420000-0.96465300 1.24758300 C -2.40299000-2.50391300-0.60604300 H -1.95638600-2.53662600-1.60600100 H -1.59263100-2.65105300 0.11579200 H -3.09307300-3.34708600-0.52147100 C -0.76583800 0.16637600-2.35239800 H -1.15741200 1.11052800-2.74673400 H -1.22317500-0.65028300-2.91933200 C 0.77308300 0.11190200-2.35529400 H 1.16432600-0.78554200-2.84711100 H 1.23007500 0.98405700-2.83255500 TS6a 2 a + H2O : Sum of electronic and thermal Free Energies= -726.867347 ua C 0.00004000-0.25225000-0.06551600 C -0.67762000-2.34474900 0.52620800 C 0.67800600-2.34465000 0.52623100 H -1.38347200-3.12593600 0.76110200 H 1.38396700-3.12573300 0.76114600 N -1.07024300-1.06176500 0.16642000 N 1.07044600-1.06160500 0.16645900 C -2.49040000-0.66488900 0.03835500 C 2.49056900-0.66457000 0.03839800 H 3.04786100-1.48093300 0.51167600 C -2.89605700-0.58703000-1.43766000 H -3.95743300-0.33328500-1.52345600 H -2.31179800 0.17619200-1.95812000 H -2.73070300-1.54446200-1.94114200 S36

C -2.79212700 0.62271400 0.81042700 H -2.37355800 1.49788900 0.30907400 H -3.87624600 0.75815400 0.87730900 H -2.37070000 0.58702300 1.81798100 H -3.04762900-1.48138400 0.51147700 C 2.79217100 0.62321500 0.81020200 H 2.37049300 0.58796100 1.81766600 H 3.87628500 0.75857500 0.87736800 H 2.37384500 1.49822500 0.30838400 C 2.89632400-0.58687900-1.43759100 H 3.95787800-0.33384300-1.52329700 H 2.73034200-1.54414500-1.94117500 H 2.31268300 0.17684300-1.95800300 C -0.00024800 1.85631000-1.07098000 O -0.00053600 1.54760100-2.21357100 O -0.00005200 2.59245600-0.13694700 O -0.00023100 1.36913800 2.69431400 H -0.00004000 1.50830000 1.73399000 H -0.00058700 2.26726200 3.04904600 TS6b 2 b + H2O : Sum of electronic and thermal Free Energies= -1188.857596 ua C 0.00068900-0.06913900-0.11930100 C 0.68111500 0.05474600-2.30245000 C -0.67345200 0.05555600-2.30437900 H 1.39452200 0.09829100-3.11009300 H -1.38451200 0.09996500-3.11404500 N 1.07233600-0.02111900-0.96493600 N -1.06844200-0.01983000-0.96795200 C -0.01148900-0.65732600 2.19136800 O -0.01761900-1.83467100 2.09205300 O -0.00795800 0.40151600 2.72401500 C -2.44883300-0.06249000-0.55022500 C -3.04741400-1.31223200-0.31725900 C -3.16310100 1.14079100-0.42257800 C -4.39027200-1.33279000 0.07116600 C -4.50490600 1.06210200-0.03420200 C -5.13366300-0.15887700 0.22456500 H -4.86596200-2.29340200 0.25374300 H -5.07150700 1.98463400 0.06734400 C 2.45183100-0.06372700-0.54423100 C 3.16610100 1.13921700-0.41723700 C 3.04716500-1.31309200-0.29897000 C 4.50568900 1.06102500-0.02002900 C 4.38703400-1.33301200 0.09849200 C 5.13288100-0.15921600 0.24377500 H 5.07054700 1.98392800 0.08708200 H 4.85817300-2.29272700 0.29722500 C -2.27571600-2.60012300-0.47461500 H -1.77779900-2.65646100-1.44828700 H -1.49943400-2.68870000 0.29139100 H -2.94371100-3.46051100-0.38601200 C -6.57367700-0.20839300 0.67763200 H -7.06663400-1.12739200 0.34685600 H -6.64349100-0.17804300 1.77208600 H -7.14448900 0.64158800 0.29229300 C -2.51891900 2.48104600-0.68062000 H -1.76123000 2.71863500 0.07548900 S37

H -2.01827400 2.51027900-1.65391800 H -3.27288900 3.27262300-0.66817500 C 2.27262600-2.60044700-0.44672000 H 1.49387700-2.68113300 0.31760800 H 1.77725600-2.66349800-1.42128700 H 2.93839800-3.46162500-0.34944600 C 6.58842300-0.21365700 0.64401300 H 6.77769800-1.02368700 1.35494400 H 7.23218400-0.39000400-0.22680500 H 6.91198700 0.72426800 1.10416000 C 2.52305700 2.47960100-0.67750600 H 2.02316900 2.50765000-1.65120000 H 1.76503900 2.71892100 0.07772800 H 3.27766300 3.27059100-0.66591400 O 0.00174900 3.02426800 1.50070600 H 0.00072700 2.09219000 1.77682500 H 0.00104200 3.51398200 2.33230800 TS6c 2 c + H2O : Sum of electronic and thermal Free Energies= -1190.041075 ua C 0.00027500-0.01480600-0.14241600 N 1.08979100 0.09477700-0.91843000 N -1.08702000 0.09516800-0.92146400 C -0.00530500-0.46342800 2.06239800 O -0.01271200-1.65142700 2.09657500 O 0.00039200 0.61150300 2.58257500 C -2.44965400-0.04675000-0.48481800 C -2.97184200-1.33823100-0.28297400 C -3.25063800 1.09959400-0.32312200 C -4.30940600-1.46003600 0.10580500 C -4.58294500 0.92153300 0.06426900 C -5.13009200-0.34435500 0.28971100 H -4.71854400-2.45497800 0.26506600 H -5.20827200 1.80160400 0.19512100 C 2.45150200-0.04690300-0.47895500 C 3.25090900 1.09986100-0.31277800 C 2.97211500-1.33793500-0.27032500 C 4.58090200 0.92255800 0.08283300 C 4.30724300-1.45892000 0.12700900 C 5.12858800-0.34319700 0.30763400 H 5.20321500 1.80326300 0.22367200 H 4.71313200-2.45319600 0.29818000 C -2.12164900-2.57282100-0.46275700 H -1.57973500-2.56262200-1.41456700 H -1.37638200-2.65231800 0.33437100 H -2.74244800-3.47219600-0.44081000 C -6.56229400-0.50101100 0.74291400 H -6.98824600-1.45008100 0.40406700 H -6.63324300-0.48538700 1.83762500 H -7.19317000 0.30925200 0.36547200 C -2.70931500 2.49126900-0.54566300 H -1.83458100 2.70169000 0.07901400 H -2.40965500 2.65049100-1.58866300 H -3.47709500 3.23538300-0.31677000 C 2.12097200-2.57259000-0.44549000 H 1.37224100-2.64699700 0.34883700 H 1.58301500-2.56703400-1.39959600 H 2.74063200-3.47252900-0.41618800 S38

C 6.57691300-0.50199800 0.70587800 H 6.72788900-1.39529700 1.31908400 H 7.22190200-0.60033400-0.17639500 H 6.93257000 0.36318200 1.27305400 C 2.70820100 2.49149100-0.53207800 H 2.41209400 2.65361900-1.57564500 H 1.83078700 2.69884700 0.08987100 H 3.47414700 3.23593400-0.29816100 O -0.00593600 3.15854200 1.33726800 H -0.00478800 2.27476200 1.74791400 H -0.00250600 3.76860900 2.08484400 C -0.76601300 0.25590100-2.36446600 H -1.18791300 1.18739300-2.75170400 H -1.19208800-0.57371500-2.93838100 C 0.77277700 0.25583300-2.36229900 H 1.20043400-0.57368200-2.93515100 H 1.19579600 1.18743700-2.74811800 References : [S1] M. J. Frisch, G. W. Trucks, H. B. Schlegel, G. E. Scuseria, M. A. Robb, J. R. Cheeseman, J. A. Montgomery, Jr. T. Vreven, K. N. Kudin, J. C. Burant, J. M. Millam, S. S. Iyengar, J. Tomasi, V. Barone, B. Mennucci, M. Cossi, G. Scalmani, N. Rega, G. A. Petersson, H. Nakatsuji, M. Hada, M. Ehara, K. Toyota, R. Fukuda, J. Hasegawa, M. Ishida, T. Nakajima, Y. Honda, O. Kitao, H. Nakai, M. X. Klene, X. Li, J. E. Knox, H. P. Hratchian, J. B. Cross, C. Adamo, J. Jaramillo, R. Gomperts, R. E. Stratmann, O. Yazyev, A. J. Austin, R. Cammi, C. Pomelli, J. W. Ochterski, P. Y. Ayala, K. Morokuma, G. A. Voth, P. Salvador, J. J. Dannenberg, V. G. Zakrzewski, S. Dapprich, A. D. Daniels, M. C. Strain, O. Farkas, D. K. Malick, A. D. Rabuck, K. Raghavachari, J. B. Foresman, J. V. Ortiz, Q. Cui, A. G. Baboul, S. Clifford, J. Cioslowski, B. B. Stefanov, G. Liu, A. Liashenko, P. Piskorz, I. Komaromi, R. L. Martin, D. J. Fox, T. Keith, M. A. Al-Laham, C. Y. Peng, A. Nanayakkara, M. Challacombe, P. M. W. Gill, B. Johnson, W. Chen, M. W. Wong, C. Gonzalez, J. A. Pople, Gaussian 03, Revision D-02, Gaussian, Inc., Pittsburgh PA, 2003. [S2] [S3] [S4] [S5] R. G. Parr, W. Yang, Functional Theory of Atoms and Molecules, R. Breslow, J. B. Goodenough, Eds., Oxford University Press: New York, 1989. a) A. D. Becke, Phys. Rev. 1988, A38, 3098-3100; b) A. D. Becke, J. Chem. Phys. 1993, 98, 5648-5652; c) C. Lee, W. Yang, R. G. Parr, Phys. Rev. 1988, B37, 785-789. P. C. Hariharan, J. A. Pople, Theor. Chim. Acta 1973, 28, 213-222. a) C. Gonzalez, H. B. Schlegel. J. Chem. Phys. 1989, 90, 2154-2161; b) C. Gonzalez, H. B. Schlegel. J. Phys. Chem. 1990, 94, 5523-5527. S39