Electronic Supplementary information

Similar documents
Recyclable Heterogeneous Copper Oxide on Alumina Catalyzed Coupling of Phenols and Alcohols with Aryl halides under Ligand Free Conditions

4001 Transesterification of castor oil to ricinoleic acid methyl ester

Supporting Information. Pd-Catalyzed Intramolecular Aminoalkylation of Unactivated. Alkenes: Access to Diverse N-Heterocycles.

Synthesis, biological evaluations and molecular modelling of new. analogs of the anti-cancer agent

Synthesis of Biphenyl-Based Arsine Ligands by Suzuki-Miyaura Coupling and their Application to Pd-Catalyzed Arsination

SUPPORTING INFORMATION

Ambident Reactivites of Pyridone Anions. Table of Contents

Supporting Information

4025 Synthesis of 2-iodopropane from 2-propanol

The synthesis of the 2,3-difluorobutan-1,4-diol diastereomers

Heterogeneous Palladium-Catalysed Catellani Reaction in Biomass-Derived γ-valerolactone

First example of alkyl-aryl Negishi cross-coupling in flow: Mild, efficient and clean introduction of functionalized alkyl groups.

Supplementary Information

Metathesis Catalysts

Supporting Information

Supplementary information

SUPPLEMENTARY INFORMATION

Supplementary Data. Synthesis of chondroitin/dermatan sulfate-like oligosaccharides and

Supplementary Information for A library-screening approach to developing a fluorescent sensing array for the detection of metal ions

SUPPORTING INFORMATION

and Heparin Analogs that Interact with Mycobacterial Heparin-binding Hemagglutinin SUPPORTING INFORMATION

Sustainable Synthesis of Quinolines and Pyrimidines Catalyzed by Manganese PNP Pincer Complexes

Synthesis, characterization and antimicrobial activity of some 4-aryl-2,6-di(coumarin-3-yl)pyridines

Experiment 4 - A Small Scale Synthesis of Biodiesel

Synthesis of chiral 3-alkyl-3,4-dihydroisocoumarins by dynamic kinetic resolutions catalyzed by a Baeyer-Villiger monooxygenase.

Supplementary Information

Supporting Information

CHAPTER 3 EXPERIMENTAL METHODS AND ANALYSIS

Palladium-Catalyzed Cyclization: Regioselectivity and Structure of Arene-Fused C 60 Derivatives

Versatile Synthesis and Enlargement of Functionalized Distorted Heptagon-Containing Nanographenes

Synthesis of phenylacetaldehyde amidines and their intramolecular cyclization

A Strained Disilane-Promoted Carboxylation of Organic Halides with CO2 under Transition-Metal-Free Conditions

Supporting Information for jo051589t Synthesis of 2-Nitro and 2,2 -Dinitro-biphenyls by means of the Suzuki Cross-Coupling Reaction.

Supplementary Material

A Continuous Flow Microwave Reactor for Conducting. High Temperature and High Pressure Chemical Reactions

Petroleum Markers Synthesized from n-alkylbenzene and Aniline Derivatives

PREPARATION OF BIODIESEL AND SEPARATION OF HEMICELLULOSE FROM SOAP SKIMMINGS

Biodiesel. As fossil fuels become increasingly expensive to extract and produce, bio-diesel is

Self-Propelled Oil Droplets Consuming Fuel Surfactant

The preparation of biodiesel from rape seed oil or other suitable vegetable oils

SYNTHESIS AND LUMINESCENCE OF. SOLUBLE meso-unsubstituted TETRABENZO- AND TETRANAPHTHO [2,3]PORPHYRINS

Product: Isosorbide. Product: Isosorbide Flow Diagram

Bright prospects Solvents for spectroscopy Uvasol

SiliCycle MiniBlock XT

= (2) V = (3) Å 3 Z =4 Mo K radiation. Data collection. Refinement. R[F 2 >2(F 2 )] = wr(f 2 ) = S = reflections

Agilent 1200 Series Manual Injector

Heating Methods. Reflux and Distillation

Production of high quality biodiesel from desilked muga pupae (Antheraea assamensis)

Electronic Supporting Information

Determination of Iodine Value in Ethylic Biodiesel Samples by 1 H-NMR

International Journal of ChemTech Research CODEN (USA): IJCRGG ISSN: Vol.7, No.5, pp ,

Synthesis and Characterization of Fatty Acid Methyl Ester by In-Situ Transesterification in Capparis Deciduas Seed

Second Quarterly Report. For the Period 1 January 1991 to 31 March 1991

Gaseous fuel, production of H 2. Diesel fuel, furnace fuel, cracking

Composition of biodiesel from Gmelina arborea seed oil

Direct transesterification of lipids from Microalgae by acid catalyst

Used lubricating oils re-refining by solvent extraction

CLAVULANATE POTASSIUM (KALII CLAVULANAS) Revised draft proposed monograph for The International Pharmacopoeia. (February 2018)

Study on exhaust performances and preparation of a new curcas oil biodiesel

CM 4310, Green Engineering Fall 07 Homework #2 Mon. 03 Dec., ' Atom and Mass Efficiencies Problem 1 of Chapter 7, page 198.

Biofuel Synthesis Acid and Spectroscopic Characterization by 1 H and 13 C NMR

Effect of Mesh Size Variations on Glycerin Adsorption by Silica from Rice Husk Ash in Biodiesel Purification

How to Use the Chemical Compatibility Chart. Vials and Closures >> Chemical Compatibility Chart

Isomerizable (E/Z)-Alkynyl-O-Methyl Oximes Employing TMSCl-NCS in Chlorinative Cyclization for the Direct Synthesis of 4-Chloroisoxazoles

BIODIESEL PRODUCTION FROM JATROPHA CURCAS OIL

Supplementary Material

DRAFT PROPOSAL FOR THE INTERNATIONAL PHARMACOPOEIA: CARBAMAZEPINUM - CARBAMAZEPINE

The Pennsylvania State University. The Graduate School. Eberly College of Science THE UNDERFUNCTIONALIZATION OF ALCOHOLS BY HETEROGENEOUS CATALYSTS

Supplementary Information

ASTM Methods that are feasible with Metrohm instruments

A Study of Alternative Catalysts and Analysis Methods for Biodiesel Production

Report No. 35 BUTADIENE. March A private report by the PROCESS ECONOMICS PROGRAM STANFORD RESEARCH INSTITUTE I PARK, CALIFORNIA

KF-loaded mesoporous Mg-Fe bi-metal oxides: high performance transesterification catalysts for biodiesel production

COOLANTS. Tx COOLANTS PRODUCT GUIDE

TEST REPORT: CHM12-01-LSM

SUPPORTING INFORMATION

SUPPORTING INFORMATION

SCOPE OF ACCREDITATION TO ISO/IEC 17025:2005

Центр Фотохимии Российской Академии Наук Сборник публикаций 2001

SAMPLING CONTAINERS & HOLDING TIMES. Parameters Method Holding Time 8 Minimum Volume Water Sampling Water Soil Water Soil Container Preservative 9

Supplementary Figure 1: Supplementary Figure 2: XRD patterns of charged and discharged graphite

Agilent 1260 Infinity Manual Injector

Reliable. Efficient. Economical. Distillation Technology ENGINEERING - EQUIPMENT - TURNKEY SYSTEMS

Investigation of Emission Properties and Performance Characteristics of Biodiesel from Chicken Waste

CHEMISTRY 135. Biodiesel Production and Analysis

Research Article Preparation, Characterization and Cross-linking of Chitosan by Microwave Assisted Synthesis

Alkaline Catalytic Transesterification for Palm Oil Biodiesel and Characterisation of Palm Oil Biodiesel

Beverage Grade Carbon Dioxide

Multifunctional multivalency: a focused library of polymeric cholera toxin antagonists

Biodiesel Production and Analysis

Flash Chromatography Column Guide Medicinal Chemistry Natural Products Proteins & Peptides

BIODIESEL Using renewable resources Introduction: Reference: Background information:

SENSORS AND SYSTEMS FOR HUMIDITY AND TEMPERATURE MEASUREMENTS RELIABILITY REPORT. HS1100 / HS1101 Relative Humidity Capacitive Sensors

Available online at WSN 58 (2016) EISSN

LEVONORGESTRELUM LEVONORGESTREL (May 2015)

DRAFT PROPOSAL FOR THE INTERNATIONAL PHARMACOPOEIA: CARBAMAZEPINUM - CARBAMAZEPINE

Biodiesel from soybean oil in supercritical methanol with co-solvent

In-situ upgrading of whole biomass to biofuel. precursors with low average molecular weight and. acidity by the use of zeolites mixture

Smog Chamber Studies on SOA Formation from Gasoline Exhaust and Pure Precursors

Synthesis of Dibenzosultams by Transition-Metal Free Photoinduced Intramolecular Arylation of N-aryl-2-halobenzenesulfonamides

Transcription:

Electronic Supplementary information C-H Functionalization of Tertiary Amines by Cross Dehydrogenative Coupling Reactions: Solvent-Free Synthesis of α-amino Nitriles and β-nitro Amines under Aerobic Condition Kaliyamoorthy Alagiri, and Kandikere Ramaiah Prabhu* Department of rganic Chemistry, Indian Institute of Science, Bangalore 560 012, Karnataka, India. Contents 1 Typical experimental procedure the preparation of N-aryl tetrahydroisoquinoline Page no SI 2 - SI 3 2 Characterization data for N-Aryl Tetrahydroisoquinoline SI 3 SI 5 3 Typical experimental procedure for the synthesis of α-amino nitrile SI - 5 4 References SI 5 5 1 H and 13 C NMR spectra SI 6 SI 41

ESI - 2 Typical experimental procedure for the Preparation of Nitroolefin H CH 3 N 2 AcH N 2 Heliotropin (5 g, 33.3 mmol) and ammonium acetate (2.56 g, 33.3 mmol) were taken into the RB flask. Nitromethane (8.9 ml, 166.5 mmol) and glacial acetic (10 ml) acid were added at room temperature. The reaction mixture was refluxed for 1.5h, and then reaction mixture was cooled in an ice bath, filtered through sintered crucible and washed successively with water, hexane and 1% ethanol in hexane. The crude mixture was concentrated under vacuo. Typical experimental procedure for the reduction of nitroolefin N 2 LiAlH 4 NH 2 The crude nitroolefin (2 g, 10.3 mmol) in dry THF (10 ml) was added drop wise to a stirred solution of LiAlH 4 (0.98 g, 25.9 mmol) in THF (20 ml). The reaction mixture was refluxed for 4h and then cooled in ice bath, quenched with saturated solution of Na 2 S 4 until effervescence ceases completely. Then filtered through sintered crucible and washed successively with ethyl acetate and concentrated under vacuo. Typical experimental procedure for the preparation of [1, 3]dioxolo[7, 8-g]- 1, 2, 3, 4- tetrahydroisoquinoline NH 2 (CH 2 )n HCH NH The amine (1.35 g, 8.18 mmol) obtained in previous step was added to formic acid (3.5 ml) at 0 o C and stirred for 10 min at same temperature until complete dissolution of amine. Then paraformaldehyde (0.25 g, 8.18 mmol) was added and stirred at 50 o C for 24h, added saturated

ESI - 3 NaH solution and extracted with DCM. The combined organic layer was dried over Na 2 S 4 and concentrated under reduced pressure. Then purified by column chromatography on silica gel using MeH/ CHCl 3. Typical experimental procedure for the preparation of N-phenyl Tetrahydroisoquinoline. CuI K 3 P 4 NH PhI Ethylene glycol N Ph Copper (I) iodide (0.21g, 1.13 mmol) and potassium phosphate (4.8 g, 22.6 mmol) were taken into the RB flask filled with nitrogen. 2-Propanol (10 ml), ethylene glycol (1.24 ml, 22.6 mmol), 1,2,3,4-tetrahydro-isoquinoline (2 g, 11.3 mmol) and iodobenzene (1.26 ml, 11.3 mmol) were added successively at room temperature. The reaction mixture was heated at 90 C for 24 h and then allowed to cool to room temperature. The solvent was removed under vacuo, added water (20 ml) and extracted with dichloromethane (3x 30 ml). The organic layer was dried over sodium sulfate. The solvent was concentrated under reduced pressure and purified by column chromatography on silica gel (hexane/ethyl acetate=95:5), to give the desired product 4a with 30% isolated yields. Characterization data for N-Aryl Tetrahydroisoquinoline 1, 2, 3, 4-Tetrahydro-2-phenylisoquinoline (1a) 1 1a N Ph Pale yellow solid; Yield - 60%; mp: 44-46 C (lit. 1 45 C); R f (20% EtAc/Hexane) 0.7; Prepared as shown in general experimental procedure. IR (KBr, cm -1 ): 2824, 1599, 1505, 1388, 1238, 1156, 1034, 934, 873, 749; 1 H NMR (400 MHz, CDCl 3 ): δ 7.27 (2H, t, J = 7.9Hz), 7.15 (4H, d, J = 3.8Hz), 6.97 (2H, d, J = 8.1Hz), 6.81 (1H, t, J = 7.2Hz), 4.39 (2H, s), 3.54 (2H, t, J = 5.8Hz), 2.96 (2H, t, J = 5.7Hz); 13 C NMR (100MHz, CDCl 3 ): 150.5, 134.8, 134.4, 129.1, 128.4, 126.4, 126.2, 125.9, 118.6, 115.0, 50.6, 46.4, 29.0; HRESI-MS (m/z): Calculated for C 15 H 15 N (M + H): 210.1283, found (M + H): 210.1286.

ESI - 4 1, 2, 3, 4-Tetrahydro-2- (4-methoxyphenyl)isoquinoline (1b) 1 1b N PMP Pale yellow solid; Yield - 50%; mp: 93-95 C (lit. 1 95 C); R f (20% EtAc/Hexane) 0.7; Prepared as shown in general experimental procedure. IR (KBr, cm -1 ): 3456, 1584, 1510, 1459, 1384, 1273, 1242, 1151, 1036, 823, 755; 1 H NMR (400 MHz, CDCl 3 ): δ 7.11 7.18 (4H, m), 6.98 (2H, d, J = 8.8Hz), 6.86 (2H, d, J = 8.8Hz), 4.29 (2H, s), 3.77 (3H, s), 3.43 (2H, t, J = 5.8Hz), 2.98 (2H, t, J = 5.7Hz); 13 C NMR (100MHz, CDCl 3 ): 153.4, 145.2, 134.5, 134.4, 128.6, 126.4, 126.2, 125.8, 118.0, 114.5, 55.5, 52.6, 48.4, 29.0; HRESI-MS (m/z): Calculated for C 16 H 17 N (M + H): 240.1388, found (M + H): 240.1387. 6, 7-dimethoxy-2-phenyl-1, 2, 3, 4-tetrahydroisoquinoline (1c) 2 1c N Ph Pale yellow solid; Yield - 30%; mp: 91-93 C; R f (20% EtAc/Hexane) 0.7; Prepared as shown in general experimental procedure. IR (KBr, cm -1 ): 3446, 1601, 1519, 1466, 1384, 1271, 1238, 1116, 1025, 861, 761; 1 H NMR (400 MHz, CDCl 3 ): δ 7.28 (2H, t, J = 7.8Hz), 6.98 (2H, d, J = 8.2Hz), 6.82 (1H, t, J = 7.2Hz), 6.64 (2H, d, J = 4.2Hz), 4.33(2H, s), 3.87 (3H, s), 3.86 (3H,s), 3.54 (2H, t, J = 5.8Hz), 2.89 (2H, t, J = 5.7Hz); 13 C NMR (100MHz, CDCl 3 ): 150.5, 147.5, 147.4, 129.1, 126.6, 126.1, 118.7, 115.3, 111.2, 109.3, 55.94, 55.90, 50.4, 46.7, 28.5; HRESI- MS (m/z): Calculated for C 17 H 19 N 2 (M + Na): 292.1313, found (M + Na): 292.1314. [1,3]dioxolo[7, 8-g]-2-phenyl-1, 2, 3, 4-tetrahydroisoquinoline (1d) 1d N Ph Pale yellow solid; Yield - 30%; mp: 65-66 C R f (20% EtAc/Hexane) 0.7; Prepared as shown in general experimental procedure. IR (KBr, cm -1 ): 2807, 1583, 1508, 1460, 1385, 1273, 1241,

ESI - 5 1207, 1190, 1036, 823, 755; 1 H NMR (400 MHz, CDCl 3 ): δ 7.27 (2H, t, J = 7.8Hz), 6.95 (2H, d, J = 8.1Hz), 6.82 (1H, t, J = 7.2Hz), 6.61 (2H, s), 5.90 (2H, s), 4.29 (2H, s), 3.51 (2H, t, J = 5.8Hz), 2.86 (2H, t, J = 5.7Hz); 13 C NMR (100MHz, CDCl 3 ): 150.3, 146.1, 145.9, 129.1, 127.8, 127.2, 118.7, 115.2, 108.3, 106.4, 100.6, 50.7, 46.6, 28.9; HRESI-MS (m/z): Calculated for C 16 H 15 N 2 (M + H): 254.1181, found (M + H): 254.1185. Typical experimental procedure for the synthesis of α-amino nitrile To the 10 mol% of Mo 2 (acac) 2 (0.05 mmol) and N-phenyltetrahydroisoquinoline (0.5 mmol) was added TMSCN (1.0 mmol). The reaction mixture was stirred at 80 o C under oxygen atmosphere (oxygen balloon) for 17 h. The reaction mixture was cooled to room temperature, added saturated NaHC 3 solution and extracted with DCM (3 X 10 ml). The combined organic layer was dried over Na 2 S 4 and concentrated under reduced pressure. The crude product was purified by column chromatography on silica gel using Hexane / Ethyl acetate (95 : 5) and furnished pale yellow solid (78%, NMR conversion = 96%). References 1) M. Jerome, H. Philippe, T. Christophe,G. R. Sylviane, -P. H. Henri, Synth. Commun., 2001, 31, 987 992. 2) A. Sud, D. Sureshkumar, M. Klussmann, Chem. Commun. 2009, 3169

ESI - 6 1.99 2.04 1.95 2.00 2.04 2.01 2.03 10.0 9.5 9.0 8.5 8.0 7.5 7.0 6.5 6.0 5.5 5.0 4.5 4.0 3.5 3.0 2.5 2.0 1.5 1.0 0.5 0.0 CDCl 3 400MHz 1 HNMR 1d N 7.3009 7.2815 7.2621 6.9848 6.9646 6.8563 6.8382 6.8200 6.6109 5.9030 4.2967 3.5296 3.5152 3.5007 2.8842 2.8700 2.8558-0.0002-0.5-1.0

ESI - 7 190 180 170 160 150 140 130 120 110 100 90 80 70 60 50 40 30 20 10 CDCl 3 100MHz 13 CNMR 1d N 150.1163 146.1437 145.9813 129.1837 127.7042 127.0459 119.0269 115.3891 108.3719 106.4193 100.7076 77.3175 76.9999 76.6822 50.8600 46.7882 28.8099

ESI - 8 2.13 2.86 1.15 2.04 1.03 1.04 1.04 1.04 10 9 8 7 6 5 4 3 2 1 0 CDCl 3 400MHz 1 HNMR N Ph 3a CN 7.3759 7.3709 7.3574 7.3544 7.3493 7.3407 7.3359 7.3263 7.3096 7.3041 7.2969 7.2863 7.2844 7.2798 7.2754 7.2637 7.2363 7.2181 7.0894 7.0698 7.0273 7.0090 6.9907 5.5044 3.7932 3.7907 3.7857 3.7830 3.7784 3.7758 3.7708 3.7682 3.7622 3.7596 3.7547 3.7520 3.7474 3.7448 3.7399 3.7374 3.5133 3.5030 3.4865 3.4823 3.4763 3.4721 3.4555 3.4453 3.1916 3.1767 3.1649 3.1505 3.1359 3.1242 3.1093 2.9885 2.9797 2.9709 2.9477 2.9390 2.9301 0.0001

ESI - 9 200 180 160 140 120 100 80 60 40 20 0 CDCl 3 100MHz 13 CNMR N Ph 3a CN 148.35 134.59 129.58 129.54 129.32 128.72 127.03 126.82 121.85 117.71 117.56 77.32 77.00 76.68 53.17 44.16 28.50

ESI - 10 4.21 2.05 2.05 3.08 1.06 1.08 1.07 1.04 10 9 8 7 6 5 4 3 2 1 CDCl 3 400MHz 1 HNMR N PMP CN 3b 7.2866 7.2763 7.2549 7.2443 7.2254 7.2072 7.0903 7.0681 6.9214 6.8992 5.3574 3.7889 3.5958 3.5802 3.5655 3.5504 3.4617 3.4519 3.4324 3.4230 3.4033 3.3936 3.1953 3.1795 3.1674 3.1534 3.1385 3.1266 3.1108 2.9405 2.8996-0.0001

ESI - 11 200 180 160 140 120 100 80 60 40 20 0 CDCl 3 100MHz 13 CNMR N PMP CN 3b 155.64 142.54 134.30 129.66 129.42 128.61 127.03 126.65 120.93 117.56 114.75 77.32 77.00 76.68 55.51 55.49 44.86 28.65

ESI - 12 2.07 2.05 1.01 1.03 1.04 6.20 1.10 1.04 1.05 1.07 10 9 8 7 6 5 4 3 2 1 CDCl 3 400MHz 1 HNMR N Ph 3c CN 7.3704 7.3513 7.3309 7.0865 7.0856 7.0656 7.0068 6.7478 6.6794 5.4427 3.8780 3.7868 3.7781 3.7720 3.7615 3.7556 3.7468 3.7410 3.4713 3.4612 3.4428 3.4328 3.4124 3.4024 3.1166 3.1018 3.0890 3.0757 3.0616 3.0488 3.0340 2.8707 2.8627 2.8546 2.8305 2.8228 2.8145-0.0000

ESI - 13 200 180 160 140 120 100 80 60 40 20 0 CDCl 3 100MHz 13 CNMR N Ph 3c CN 149.35 148.39 148.04 129.49 126.84 121.86 121.07 117.83 117.67 111.51 109.31 77.32 77.00 76.68 56.03 55.90 53.00 44.15 28.04

ESI - 14 2.02 3.03 0.98 1.01 2.05 1.02 1.02 1.02 1.03 10 9 8 7 6 5 4 3 2 1 CDCl 3 400MHz 1 HNMR N Ph 3d CN 7.3724 7.3531 7.3332 7.0691 7.0490 7.0277 7.0093 6.9910 6.7252 6.6586 5.9623 5.3850 3.7462 3.7393 3.7323 3.7222 3.7156 3.7083 3.7020 3.4613 3.4511 3.4331 3.4233 3.4034 3.3934 3.0899 3.0752 3.0631 3.0492 3.0348 3.0228 3.0081 2.8581 2.8503 2.8253 2.8177 0.0001

ESI - 15 200 180 160 140 120 100 80 60 40 20 0 CDCl 3 100MHz 13 CNMR N Ph 3d CN 148.24 148.10 146.63 129.53 128.31 122.14 121.88 117.67 117.54 108.84 106.65 101.32 77.32 77.00 76.68 53.23 44.11 28.49

ESI - 16 1.92 0.96 1.91 2.00 2.97 10 9 8 7 6 5 4 3 2 1 CDCl 3 400MHz 1 HNMR 3e N CN 7.3298 7.3108 7.3094 7.2897 6.9367 6.9183 6.9000 6.8765 6.8557 4.1577 2.9992-0.0002

ESI - 17 200 180 160 140 120 100 80 60 40 20 0 CDCl 3 100MHz 13 CNMR 3e N CN 147.75 129.43 120.16 115.45 114.85 77.32 77.00 76.69 42.24 39.21

ESI - 18 1.93 1.95 2.00 2.99 3.00 10 9 8 7 6 5 4 3 2 1 CDCl 3,400MHz, 1 HNMR 3f N CN 7.1179 7.0975 6.7935 6.7720 4.0990 2.9392 2.2770-0.0000

ESI - 19 220 200 180 160 140 120 100 80 60 40 20 0 CDCl 3 100MHz 13 CNMR 3f N CN 145.60 129.89 129.74 115.44 115.31 77.32 77.00 76.68 42.70 39.36 20.30

ESI - 20 2.00 2.02 1.04 1.07 4.26 10 9 8 7 6 5 4 3 2 1 0 CDCl 3,400MHz, 1 HNMR 3g CN N 7.3159 7.2955 7.2767 6.8477 6.8295 6.8111 6.7011 6.6807 4.4358 4.4179 3.4787 3.4709 3.4566 3.4511 3.4378 3.4321 3.3893 3.3690 3.3498 3.3296 2.4380 2.4174 2.4109 2.4013 2.3732 2.3331 2.3147 2.3070 2.2889 2.2718 2.2561 2.2377 2.2327 2.2225 2.2134 2.2037 2.1914 2.1783 2.1603-0.0001

ESI - 21 200 180 160 140 120 100 80 60 40 20 0 CDCl 3 100MHz 13 CNMR 3g CN N 145.1047 129.3253 119.1931 118.0512 112.5860 77.3186 77.0006 76.6821 48.9457 47.3286 31.3837 23.8004-20

ESI - 22 1.96 1.98 1.08 3.48 1.10 1.01 1.15 1.01 1.01 10 9 8 7 6 5 4 3 2 1 N Ph 4 CDCl 3,400MHz, 1 HNMR 7.9925 7.9896 7.9693 7.4781 7.4735 7.4606 7.4402 7.4170 7.4044 7.3993 7.3930 7.3810 7.2896 7.2828 7.2747 7.2702 7.2587 7.2539 7.2486 7.2437 7.2325 7.2177 7.0949 7.0637 7.0453 5.0677 5.0296 4.5919 4.5538 4.1675 4.1563 4.1436 4.1397 4.1324 4.1285 4.1161 4.1042 3.8084 3.7946 3.7855 3.7689 3.7527 3.7295 3.6827 3.6717 3.6576 3.6431 3.6323 3.6294 2.8649 2.8535 2.8423 2.8226 2.8114-0.0001

ESI - 23 200 180 160 140 120 100 80 60 40 20 0 N Ph 4 CDCl 3,100MHz, 13 CNMR 154.05 131.23 130.04 129.08 128.90 128.53 127.43 126.68 126.26 120.52 77.32 77.00 76.68 71.45 65.54 28.45 26.25

ESI - 24 5.43 1.03 2.15 1.09 1.01 2.12 1.06 1.09 10 9 8 7 6 5 4 3 2 1 7.2702 7.2493 7.2307 7.2236 7.2038 7.1929 7.1748 7.1622 7.1449 7.1093 7.0911 6.9680 6.9467 6.8441 6.8258 6.8077 5.5423 5.5243 5.5064 4.8489 4.8294 4.8193 4.7999 4.5438 4.5272 4.5141 4.4977 3.6622 3.6486 3.6297 3.6159 3.6062 3.6032 3.5954 3.5850 3.5737 3.5626 3.5524 3.5408 3.0881 3.0738 3.0666 3.0482 3.0330 3.0256 3.0113 2.7851 2.7729 2.7606 2.7444 2.7321 2.7198-0.0001

ESI - 25 200 180 160 140 120 100 80 60 40 20 0 148.37 135.21 132.85 129.43 129.12 128.03 126.92 126.61 119.35 115.04 78.68 77.31 77.00 76.68 58.11 41.97 26.35

ESI - 26 2.37 2.12 2.18 2.02 1.02 1.01 3.08 1.96 1.08 1.04 10 9 8 7 6 5 4 3 2 1 0 CDCl 3,400MHz, 1 HNMR 6b N 2 PMP N 7.2486 7.2352 7.2204 7.2180 7.2030 7.1664 7.1434 7.1251 6.9218 6.8993 6.8201 6.7975 5.4006 5.3855 5.3796 5.3647 4.8425 4.8211 4.8127 4.7913 4.5732 4.5587 4.5434 4.5289 3.7420 3.5699 3.5658 3.5596 3.5480 3.0475 3.0303 3.0248 3.0067 2.9839 2.9664 2.7197 2.7098 2.6999 2.6785 2.6685 2.6586-0.0001-1

ESI - 27 200 180 160 140 120 100 80 60 40 20 0 153.96 143.03 135.41 132.86 129.43 127.87 126.89 126.59 118.84 114.68 78.93 77.32 77.00 76.68 58.89 55.56 43.12 25.77

ESI - 28 2.22 2.02 0.98 1.04 6.24 1.09 1.02 1.09 1.03 10 9 8 7 6 5 4 3 2 1 7.2784 7.2582 7.2395 6.9782 6.9573 6.8604 6.8422 6.8240 6.6434 6.6017 5.4750 5.4569 5.4392 4.8694 4.8493 4.8399 4.8199 4.5837 4.5679 4.5543 4.5384 3.8519 3.8442 3.8308 3.7010 3.6883 3.6754 3.6681 3.6553 3.6428 3.6022 3.5910 3.5785 3.5677 3.5581 3.5454 3.5341 3.0307 3.0171 3.0074 2.9914 2.9766 2.9669 2.9530 2.6995 2.6883 2.6769 2.6592 2.6479 2.6366-0.0004

ESI - 29 200 180 160 140 120 100 80 60 40 20 0 CDCl 3 100MHz 13 CNMR N Ph 6c N 2 148.76 148.57 147.71 129.41 127.40 124.55 119.54 115.51 111.72 109.63 78.76 77.32 77.00 76.68 57.95 56.04 55.88 42.04 25.79

ESI - 30 2.16 1.99 1.02 1.97 2.02 2.07 1.08 1.04 10 9 8 7 6 5 4 3 2 1 7.2794 7.2581 7.2399 6.9537 6.9330 6.8593 6.8410 6.8228 6.6174 6.5879 6.5720 5.9127 5.8805 5.8752 5.4206 5.4026 5.3848 4.8367 4.8173 4.8071 4.7877 4.5276 4.5111 4.4980 4.4815 3.6256 3.6118 3.5932 3.5788 3.5660 3.5570 3.5452 3.5341 3.5244 3.5126 2.9890 2.9743 2.9683 2.9491 2.9337 2.9275 2.9128 2.6892 2.6769 2.6643 2.6487 2.6363 2.6239 0.0000

ESI - 31 200 180 160 140 120 100 80 60 40 20 0 148.38 147.43 146.33 129.44 128.78 125.67 119.46 115.18 108.95 106.92 101.09 78.71 77.32 77.00 76.68 58.14 42.15 26.39

ESI - 32 6.02 2.43 0.61 0.39 0.63 1.44 1.05 1.04 1.17 2.24 10 9 8 7 6 5 4 3 2 1 7.2883 7.2679 7.2486 7.2385 7.2276 7.2089 7.1912 7.1661 7.1474 7.1202 7.1038 7.0851 7.0122 6.9928 6.9723 6.8344 6.8175 6.8045 6.7867 5.2592 5.2359 5.2142 5.0738 5.0569 5.0381 5.0205 5.0034 4.8983 4.8782 4.8599 3.8586 3.8443 3.8390 3.8249 3.8112 3.8060 3.7912 3.6093 3.5946 3.5862 3.5694 3.5624 3.5535 3.5375 3.5214 3.5058 3.0801 3.0632 3.0394 3.0221 3.0043 2.9337 2.9194 2.9041 2.8796 2.8650 2.8418 2.8265 1.6970 1.6799 1.5488 1.5361 1.5195

ESI - 33 200 180 160 140 120 100 80 60 40 20 0 149.113 148.833 135.575 134.741 133.771 131.979 129.389 129.269 129.064 128.675 128.309 128.162 127.210 126.555 126.086 119.281 118.741 115.374 114.442 88.911 85.394 77.318 77.000 76.682 62.698 61.111 43.506 42.625 26.703 26.342 17.384 16.347

ESI - 34 4.37 2.25 2.14 1.63 0.42 3.95 1.38 1.11 1.01 2.01 10 9 8 7 6 5 4 3 2 1 7.2458 7.2391 7.2212 7.2007 7.1799 7.1516 7.1348 7.1116 7.0931 6.9222 6.9003 6.8275 6.7894 6.7669 5.0683 5.0474 5.0312 5.0090 4.9907 4.9747 4.9695 4.9537 4.8920 4.8749 4.8572 4.8392 4.8209 4.8129 4.7913 4.5728 4.5583 3.7442 3.7238 3.5213 3.5081 3.4972 3.4863 3.4741 3.4612 3.0127 2.9982 2.9897 2.9713 2.9560 2.9484 2.9336 2.8417 2.8289 2.8160 2.7878 2.7524 2.7391 1.6761 1.6592 1.5318 1.5170-0.0002

ESI - 35 200 180 160 140 120 100 80 60 40 20 0 153.77 153.53 143.47 135.79 135.00 133.64 132.02 129.23 128.93 128.35 127.98 127.94 127.16 126.48 126.00 118.85 118.82 118.20 114.67 114.54 88.78 85.73 77.32 77.00 76.68 63.43 62.14 55.57 55.51 44.98 43.97 26.22 25.99 17.06 16.54

ESI - 36 2.02 1.90 0.96 0.98 0.58 0.32 0.90 0.58 0.33 6.30 1.34 0.99 0.91 1.77 10 9 8 7 6 5 4 3 2 1 0 CDCl 3,400MHz, 1 HNMR N 2 6g Ph N 7.2785 7.2557 7.2482 7.2342 7.2148 7.0053 6.9837 6.9619 6.8324 6.8143 6.7961 6.6339 6.6249 6.5628 6.4940 5.1664 5.1464 5.1374 5.1145 5.0689 5.0523 5.0340 5.0166 4.9057 4.8885 4.8844 4.8667 3.8649 3.8471 3.8421 3.8319 3.8160 3.8000 3.7815 3.7684 3.7611 3.7472 3.6305 3.6089 3.5945 3.5793 3.5602 3.5460 3.5391 3.5325 3.5198 3.5108 3.4984 3.4871 3.4782 2.9961 2.9791 2.9567 2.9381 2.9188 2.8200 2.8064 2.7928 2.7790 2.7653 2.7515 2.7381 2.7249 2.6976 1.6975 1.6806 1.5376 1.5211 0.0000

ESI - 37 200 180 160 140 120 100 80 60 40 20 0 CDCl 3 100MHz 13 CNMR N Ph 6g N 2 149.25 148.87 148.80 148.60 147.32 147.06 129.32 129.23 127.81 126.78 125.50 123.50 119.36 118.95 115.61 115.03 111.53 111.48 111.13 110.17 88.90 85.31 77.32 77.00 76.68 62.44 60.90 56.00 55.89 55.79 55.76 43.28 42.56 25.89 25.79 17.47 16.15

ESI - 38 2.25 1.87 1.04 0.94 0.62 2.00 0.91 0.57 0.36 0.58 1.39 1.06 0.97 1.10 2.63 10 9 8 7 6 5 4 3 2 1 7.2863 7.2662 7.2510 7.2487 7.2267 7.2077 6.9680 6.9477 6.8421 6.8318 6.8242 6.8136 6.7955 6.6110 6.5785 5.9280 5.9174 5.9153 5.8979 5.1296 5.1052 5.0826 5.0414 5.0250 5.0085 4.9883 4.8722 4.8552 4.8507 4.8333 3.8018 3.7877 3.7813 3.7678 3.7546 3.7483 3.7340 3.5690 3.5542 3.5378 3.5207 3.5045 3.4859 2.9717 2.9556 2.9308 2.9145 2.8961 2.8150 2.8005 2.7859 2.7800 2.7594 2.7440 1.6852 1.6682 1.5682 1.5515 1.5352-0.0001

ESI - 39 200 180 160 140 120 100 80 60 40 20 0 149.14 148.88 147.51 147.41 146.14 145.89 129.39 129.27 129.16 128.36 126.74 124.77 119.44 118.88 115.59 114.63 108.93 108.74 108.27 107.61 101.07 101.01 88.98 85.53 77.32 77.00 76.68 62.76 61.11 43.63 42.65 26.69 26.37 17.49 16.47

ESI - 40 2.05 2.04 2.00 2.03 3.02 3.39 10 9 8 7 6 5 4 3 2 1 CDCl 3,400MHz, 1 HNMR 6i N 2 N 7.0876 7.0669 6.6761 6.6551 4.5656 4.5497 4.5339 3.9739 3.9580 3.9422 2.9439 2.2632-0.0001

ESI - 41 200 180 160 140 120 100 80 60 40 20 0 CDCl 3 100MHz 13 CNMR 6i N 2 N 145.83 129.99 127.49 113.18 77.31 77.00 76.68 72.59 50.98 38.96 20.20