Conjugate extension carboxyl dipyridyl ligand and synthetic method and application for ruthenium dye thereof
A technology of carboxybipyridine and bipyridine, which is applied in the field of synthesis of conjugated extended carboxybipyridine ligands and ruthenium-based dyes, can solve the problems of narrow absorption range and poor use of sunlight in the long-wave region, and achieve the goal of using Sufficient, improve the molar extinction coefficient, the effect of good application prospects
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Embodiment 1
[0032] The synthesis method and conditions of ligand a: synthesize ligand a in ethanol with 2,2'-bipyridine-4,4'-dicarbaldehyde, malonic acid and tetrahydropyrrole;
[0033] Ligand a (4,4'-bis(2,2-dicarboxylic acid-1-vinyl)-2,2'-bipyridyl) synthetic route:
[0034]
[0035] The specific steps are: add 0.25g (2.4mmol) 2,2'-bipyridyl-4,4'-dicarbaldehyde, 0.75g (7.2mmol) malonic acid and 0.08g tetrahydropyrrole to the reaction tank filled with 30mL ethanol In the flask, stir for 0.5 hour to make it evenly mixed, then reflux at 95°C for 4 hours, let stand for 10 hours, vacuum filter, and wash with acetonitrile to obtain the final product.
[0036] Ligand a: 1H-NMR (298K, 200MHz, δin ppm) 7.7(m, 2H), 7.8~7.9(m, 2H), 8.1(s, 2H), 8.8(m, 2H), 9.1(s, 2H ),See figure 1 .
Embodiment 2
[0038] Ligand b synthesis method and conditions: 4,4'-dicarbaldehyde-2,2'-bipyridine, cyanoacetic acid and tetrahydropyrrole synthesize ligand b in acetonitrile;
[0039] Ligand b (4,4'-bis(2-cyano-1-acrylic acid)-2,2'-bipyridyl) synthetic route:
[0040]
[0041] The specific steps are: add 0.25g (2.4mmol) 2,2'-bipyridyl-4,4'-dicarbaldehyde, 0.61g (7.2mmol) cyanoacetic acid and 0.08g tetrahydropyrrole to the reaction tank filled with 30mL acetonitrile In the flask, stir for 0.5 hours to make it evenly mixed, then reflux at 105°C for 5 hours, let stand for 9 hours, vacuum filter, and wash with acetonitrile.
[0042] Ligand b: 1H-NMR (298K, 200MHz, δin ppm) 7.6~7.9(m, 4H), 8.3(m, 2H), 8.5~8.9(m, 2H), 12.7(s, 4H), see figure 2 .
Embodiment 3
[0044] Synthesis method of symmetrical ruthenium dye L121 based on ligand a: ligand a, RuCl 3 , NH 4 NCS synthesizes L121 in DMF;
[0045] L121 (ruthenium (bis(4,4'-bis(2,2-dicarboxylic acid-1-vinyl)-2,2'-bipyridine) (NCS) 2 )synthetic route:
[0046]
[0047] The specific steps are: add 0.058g (0.16mmol) ligand a, 0.017g (0.082mmol) RuCl 3 Added to 30mL DMF, stirred for 0.5 hours to mix, refluxed at 160°C for 4 hours, added 0.5g (6.57mmol) NH4 NCS, reflux at 130°C for 4 hours, and the entire reaction process was carried out in a nitrogen atmosphere. Let stand for 10 hours, vacuum filter, wash 3 times with water, and then 4 times with ether. Vacuum dry.
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