ࡱ> `abcdefNE7 5bjbjUU  7|7|&lZZZ$~PLf~9*(&(NN;%U% a%s8u8u8u8u8u8u8$:  =8Zi% $0;%i%i%8w.N;z9w.w.w.i%NZs8w.i%s8w.w.O5^ZO5 @N~L+^O5O5$909O5=w.=O5w.~~ Supplementary Information For MacDonald [2 + 2]-Type Condensation with Vicinal Diketones: Synthesis and Properties of Novel Spiro-Tricyclic Porphodimethenes Michael Harmjanz, Ivana Bo~idarevi, Michael J. Scott* Department of Chemistry, University of Florida P.O. Box 117200, Gainesville, FL 32611-7200 Experimental Details General procedures. NMR spectra were recorded on a Varian Mercury or VXR 300 MHz spectrometer at 299.95 for the proton channel. UV-vis spectra were recorded with a Varian Cary 50 spectrophotometer. The University of Florida Mass Spectrometry Services measured all mass spectral data while Complete Analysis Laboratories Inc., Parsippany, New Jersey, performed elemental analyses. Fluorescence measurements were preformed with SPEX F-112 spectrophotometer. A solution of Ru(bpy)3Cl2 (f= 0.0379) in water was used as a standard for quantum yield measurements. Aceanthrenequinone and phenanthrenequione were used as received while pyrene-4,5-dione was prepared as described in reference 8. Chromatography. Absorption column chromatography was performed using neutral alumina (Aldrich, Brockmann I ~158 mash, 58) or chromatographic silica gel (Fisher, 200- 425 mesh) . Synthesis of 1 and 2: A sample of aceanthrenequinone (500 mg, 2.15 mmol) and 569 mg (2.15 mmol) of 5-mesityldipyrromethane were dissolved in 200 mL of CH2Cl2 and 0.3 ml (3.9 mmol) of TFA was added. After 1 h of stirring at room temperature, a 490 mg portion of DDQ (2.16 mmol) was added to the greenish-blue solution, and the mixture stirred for an additional hour. The volume was reduced by 90 % and the dark solution was loaded onto an alumina column (CH2Cl2 : Hexanes 5 : 1). The column was eluted until no more porphodimethene was detected. The solvents were removed and the isomers were separated by silica chromatography (benzene). 1: Yield: 187 mg (18%) UV-vis [CHCl3, (max(log ()] 452(4.92) nm. Fluorescence spectrum (CHCl3): exc = 448nm, em= 615nm, f= 1.02x10-4. mp 358C (dec). 1H NMR (300 MHz, CDCl3): ( = 13.91 (s, 2H, NH), 9.56 (d, 2H, J = 8.6 Hz), 8.77 (s, 2H), 8.16 (d, 2H, J = 8.3 Hz), 8.12 (d, 2H, J = 8.6 Hz), 7.92 (d, 2H, J = 6.6 Hz), 7.78 (dd, 4H, J1 = J2 = 7.7 Hz), 7.63 (dd, 2H, J1 = J2 = 7.2 Hz), 6.85 (s, 2 H), 6.77 (s, 2H), 6.15 (d, 4H, J = 4.3 Hz), 5.93 (d, 4H, J = 4.3 Hz) 2.26 (s, 6H), 2.20 (s, 6H), 1.98 (s, 6H). HRMS (FAB) calcd. for MH+ (C68H49N4O2): 953.3856 Found 953.3855. 2: Yield: 40 mg (4%). UV-vis [CHCl3, (max(log ()] 448(4.94) nm. Fluorescence spectrum (CHCl3): exc = 452nm, em= 688nm, f= 1.13x10-4. mp 398C (dec). 1H NMR (300 MHz, CDCl3): ( = 14.05 (s, 2H, N-H), 9.35(d, 2H, J = 8.1 Hz), 8.80 (d, 2H, J = 6.3 Hz), 8.72 (s, 2H), 8.14 (d, 2H, J = 8.7 Hz), 8.06 (d, 2H, J = 8.7 Hz), 7.94 (dd, 2H, J1 = 6.6, J2 = 8.4 Hz), 7.78 (dd, 2H, J1 = J2 = 7.1 Hz), 7.59 (dd, 2H, J1 = J2 = 7.1 Hz), 6.81 (s, 4H), 6.19 (s, 8H), 2.26 (s, 6H), 2.05 (s, 12H). Anal calcd. for C68H48N4O2 C, 85.69; H, 5.08; N, 5.88. Found C, 85.48; H, 4.97; N, 5.65. HRMS (FAB) calcd. for MH+ (C68H49N4O2): 953.3856. Found: 953.3814. Synthesis of 3: 394 mg (1.89 mmol) of phenanthrenequinone and 500 mg (1.89 mmol) 5-mesityldipyrromethane were reacted as described for 1 and 2. After 2.5 h, a portion of DDQ (428 mg, 1.89 mmol) was added. After column chromatography (neutral alumina, CH2Cl2), 3 was isolated as the only isomer. Yield: 93 mg (11%). UV-vis [CHCl3, (max(log ()] 432(4.89) nm. Fluorescence spectrum (CHCl3): exc = 433nm, em= 624nm, f= 1.41x10-3. mp 396C (dec). 1H NMR (300 MHz, CDCl3): ( = 13.23 (s, 2H, N-H), 8.23 (dd, 2H, J1 = 1.5, J2 = 7.8 Hz), 8.11 (dd, 4H, J1 = J2 = 7.7 Hz), 7.96 (dd, 2H, J1 = 1.7, J2 = 7.6 Hz), 7.74 7.68 (m, 2H), 7.54 7.42 (m, 6H), 6.79 (s, 4H), 6.12 (d, 4H, J = 4.2 Hz), 5.65 (d, 4H, J = 4.2 Hz), 2.26 (s, 6H), 2.04 (s, 12H). HRMS (FAB) calcd. for MH+ (C64H49N4O2): 905.3855. Found: 905.3872. Synthesis of 3a: A sample of the porphodimethene 3 (84 mg, 0.093 mmol) was reacted with 85 mg (2.25 mmol) of NaBH4 according to the literature procedure described in reference 3b. After stirring for one hour at room temperature another portion of NaBH4 (25 mg, 0.66 mmol) was added and the reaction mixture was stirred for an additional 3 h. Acidic work up as described in reference 3b yields 3a as a microcrsytalline solid. Yield: 83 mg (98 %). UV/Vis [CHCl3, (max] 423, 519, 553, 592 nm. 1H NMR (300 MHz, CDCl3): ( = 8.74 (bs, 2H), 8.68 (bs, 2H), 8.54 (bs, 4H), 8.25(d, 2H, J = 7.4 Hz), 7.84 7.70 (m, 4H), 7.61 (d, 2H, J = 8.4 Hz), 6.97 (d, 2H, J = 7.7 Hz), 6.67 (d, 2H, J = 7.6), 6.34 (dd, 2H, J1 = J2 = 7.6 Hz), 6.18 (dd, 2H, J1 = J2 = 7.5 Hz), 4.50 (bs, 2H), 4.32 (bs, 2H), 2.60(s, 6H), 2.71 (bs, 12H), 0.714 (bs, 2H), -2.98(s, 2H). HRMS (FAB) calcd. For MH+ (C64H55N4O2): 911.4325. Found: 911.4326. Synthesis of 4: A sample of Pyrene-4,5-dione (2.000 g, 8.62 mmol) and 2.276 g (8.62 mmol) 5-mesityldipyrromethane were dissolved in 930 ml of CH2Cl2. TFA (1.19 ml, 14.61 mmol) was added and the reaction mixture was stirred for 50 minutes at room temperature. 1.909 g of DDQ was added and the mixture was stirred for another 20 minutes. The volume was reduced by 90% and the mixture was loaded onto alumina column and eluated with CH2Cl2. The first orange fraction was collected. The solvent was then evaporated and the residue redissolved in a minimal amount of o-dichlorobenzene and placed on a silica column. Separation has been achieved with benzene as an eluant. 4 was isolated as the second orange fraction. Removal of the solvent yielded 4 as an orange solid (0.041g, 1%). UV/Vis [o-dichlorobenzene, (max(log ()] 442(4.97), 504(3.88). Fluorescence spectrum (o-dichlorobenzene): exc= 442nm, em= 624nm, f= 8.70x10-3. mp 240C (dec). 1H NMR (300 MHz, o-dichlorobenzene-d4):  13.71 (s, 2H), 8.01 (d, 2H J= 7.49 Hz), 7.71 (d, 2H J= 7.79 Hz) , 7.44  7.37 (m, 4H) 7.54 (d, 2H, J= 8.99 Hz), 7.43 (d, 2H J= 8.39 Hz), 7.38 (d , 2H J= 7.49 Hz), 7.26 (dd, 2H J1 = J2= 7.49 Hz), 6.47 (s, 2H), 6.37 (s, 2H), 5.91 (bs, 4H), 5.39 (d, 4H J = 4.20 Hz), 1.93 (s, 6H), 1.65 (s, 6H), 1.46 (s, 6H). HRMS (FAB) calcd. for MH+ (C68H49O2N4): 953.3855. Found 953.3833. 5: The anti isomer 5 was collected as the first fraction from the silica column in the reaction procedure described for 4. Yield: (0.178 g, 4 %). UV-vis [o-dichlorobenzene, (max(log ()] 440(4.94), 497(3.98). Fluorescence spectrum (o-dichlorobenzene): exc= 440nm, em=592 nm, f= 7.94x10-4. mp 320C (dec). 1H NMR (300 MHz, o-dichlorobenzene-d4):  13.82 (s, 2H), 8.53 (d, 2H J = 7.49 Hz), 8.33 (d, 2H J=7.49 Hz), 7.76 (d, 2H J= 8.08 Hz), 7.66 (d, 2H J1= J2*= 7.79 Hz), 7.55 (d, 2H, J = 7.79 Hz), 7.48 (d, 2H 8.99 Hz), 7.42 7.34 (m, 4H), 6.40 (s, 4H), 5.95 (d, 4H J = 3.90 Hz), 5.71 (d, 4H, J = 4.20 Hz), 1.91 (s, 6H), 1.54 (s, 12H). HRMS (FAB) calcd. for MH+ (C68H49O2N4): 953.3855. Found 953.3869. Xray-Crystallography Unit cell dimensions and intensity data (Table 1) for all the structures were obtained on a Siemens CCD SMART diffractometer at 100C, with monochromatic Mo-Ka X-rays (l = 0.71073 ). The data collections nominally covered over a hemisphere of reciprocal space, by a combination of three sets of exposures; each set had a different ( angle for the crystal and each exposure covered 0.3( in (. The crystal to detector distance was 5.0 cm. The data sets were corrected empirically for absorption using SADABS (Blessing, R. H. Acta Cryst., Sect. A , 1995, 51, 33). All the structures were solved using the Bruker SHELXTL software package for the PC, using the direct methods option of SHELXS. The space groups for all of the structures were determined from an examination of the systematic absences in the data, and the successful solution and refinement of the structures confirmed these assignments. All hydrogen atoms were assigned idealized locations and were given a thermal parameter equivalent to 1.2 or 1.5 times the thermal parameter of the carbon atom to which it was attached. For the methyl groups, where the location of the hydrogen atoms was uncertain, the AFIX 137 card was used to allow the hydrogen atoms to rotate to the maximum area of residual density, while fixing their geometry. In both 1 and 3a the crystal contained severely disordered solvate molecules and in instances where a suitable model could not be constructed for the solvates, their contribution to the diffraction was removed (squeezed) from the data by the Platon for Windows software program. The final residuals are given in Table 1. The asymmetric unit of 1 contained six chloroform solvate molecules. Two of these solvates were severely disordered and there contribution to the diffraction was removed from the structure with Platon. Four cholorbenzenes crystallized with 5 in the solid-state, one of which was disordered in two orientations. The two chloroforms in the asymmetric unit of 3a were disordered and they were squeezed from the structure. Table 1: Summary of X-ray structural data. 16CHCl354C6H4Cl23a2CHCl3FormulaC74H54Cl18N4O2C92H64Cl8N4O2C66H56Cl6N4O2Fomula weight1669.311541.071149.85Crystal systemTriclinicMonoclinicTriclinicSpace groupP EMBED Equation.3 P21/nP EMBED Equation.3 Z241temp, K173(2)173(2)173(2)Dcalc/g cm-31.4581.350 1.337a 13.807(4)20.934(6)9.647(4)b 16.793(4)16.421(4) 12.991(6)c 18.384(5)22.497(8)13.047(6)a, deg68.960(4)66.728(8)(, deg80.192(4)101.358(15)78.609(8)g, deg73.496(4)72.660(8)V 33803.1(16)7582(4)1427.8(11)(, mm-10.6960.3520.351Uniq. data coll./obs.13272/618411196/71813964/2860R10.07550.09660.0893wR20.18700.23950.2467        S- PAGE 1 S- PAGE 10  EMBED ChemDraw.Document.4.5   EMBED ChemDraw.Document.4.5   EMBED Photoshop.Image.5 \s   EMBED ChemDraw.Document.4.5   EMBED ChemDraw.Document.4.5   EMBED ChemDraw.Document.4.5   EMBED Word.Document.8 \s  X TV?DMNcuw ' f g i j L M o p r s v { | Կ jeB*CJph jlB*CJphB*CJH*ph B*CJph5B*CJphCJH*5B*\phf 6CJ]5\CJH*OJQJCJOJPJQJ CJOJQJ56CJOJPJQJ\]5CJOJPJQJ\5CJOJQJ\2  DFHJLTVXVX?@ABC$a$dxdd$a$445CDEFGHIJKLMc  L FG#&&$dha$$dha$$dha$$a$$(<>PTxz :; "68JNrt56:; jeCJ jlCJCJH*CJ5B*CJph jdB*CJphB*CJH*phB*CJH*ph B*CJphL,8:>@FH>@HPdh|~&'BCGHcdmn!"$%&'(FGU jdB*CJph jeCJ jlCJCJH*CJ5CJ5B*CJH*ph B*CJphB*CJH*phMUVxyBC12FGJK $%)*bcefmo    5H*\5B*\ph je5\ jl5\5B*\phf 5H*\5\ jdH* jlH*5 5B*phH D!F!J!L!""Z"["_"`"""""""""""##0#1############2$8$L$P$d$f$x$|$~$$$$$$$$%%%%%&&&&&&&&&&&&߾߰ľ߾ B*H*ph B*H*phH* jeH* jl 5H*\ 5H*\ 56\]5\ B*ph5B*H*\ph5B*\ph5B*H*\phE&&.d0e000000 $$Ifa$$`a$$a$ &&'((((\)^)))))^*n*******----..//$0&000000000000000000000000000000000000000000000000#1$1.1/1816]H*\ 5mH sH 6mH sH mH sH  jw j jfOJQJ65\R000000jaaaa $$Ifa$$$Ifl  h\~ Hl(# $  t30  #4 la00001 1jaaaa $$Ifa$$$Ifl  h\~ Hl(# $  t30  #4 la 1 11$1/191:1F1_1e1~11jaaaajaaaaj$ $$Ifa$$$Ifl  h\~ Hl(# $  t30  #4 la 8191F1G1H1[1\1]1^1_1a1b1d1e1f1g1z1{1|1}111111111122`2b222222222$3&3*3.3l3n3v3z3!4%4<4=4>4U4W4k4m4o4p4r4s444444jCJUmHnHujUmHnHu jm jb6]6OJQJ]H*H* jEHU 6H*] jEHUjn1; UVmHnHu jU6]B11111111111XxX$$Ifl  h\~ Hl(# $  t30  #4 la $$Ifa$ $$Ifa$ 111111111111aa$$Ifl  h\~ Hl(# $  t30  #4 la $$Ifa$ 11222"262J2^2`2n22aat$$Ifl  h\~ Hl(# $  t30  #4 la $$Ifa$ 2222222222 33aat$$Ifl  h\~ Hl(# $  t30  #4 la $$Ifa$ 3"3$3.3D3T3j3l3|3333aal$$Ifl  h\~ Hl(# $  t30  #4 la $$Ifa$ 3333344 444 4jaaaajdXaaa $$Ifa$ $$Ifa$$$Ifl  h\~ Hl(# $  t30  #4 la 4!4%4,434:4;4<4?4@4A4jhaaaaj____ $$Ifa$$$Ifl  h\~ Hl(# $  t30  #4 la A4B4C4D4E4F4G4H4I4J4K4L4M4N4O4P4Q4R4S4T4U4X4Y4Z4[4\4]4^4_4$dha$_4`4a4b4c4d4e4f4g4h4i4j4k4n4o4q4r4t4u4v4w4x4y4z4{4|4}4~44$dha$444444444444444444444445595:5]5$ a$$dha$444444444444444444444444444455555555657585:5;5Y5Z5[5\5^5_5}5~555555þ jOUjݒ> UV j!Uj!> CJUVaJ jzUjR> CJUVaJ j;Uj > UV ji UjȞ> UV jUj > CJUVaJ jU0JmHnHu j0JU0J4]5^5555555$dha$55555 jU j Ujj> CJUVaJ 1h/ =!"#$%'&P1h0= /!"#$%`!ZrtzbQSlq_?~,h (xڽ\ xT>;m$a @LX$P!@ؗ"P6KmTPQQZ_}l}P[i Gokks;ޙa+^39s݅(,1ywR'GÇ+PשCUͧV*廒*c*?0ɛN+Rg}ܠիk7Mљaț?"/'? 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