Activation and Control of Electron-Transfer Reactions by Noncovalent Bond
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- なごみ ひがき
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1
2 2 + 4e hν 2 2 1
3 2
4 20 J. Am. Chem. oc. Angew. Chem. Int. Ed. umber of Papers Year : J. Am. Chem. oc. (Trost, B. M.; tanford University, UA) 3
5 π 1/2 k ET = V 2 ( G 0 ET + λ) 2 exp (1) λ k B T h 4 λk B T 4
6 (a) (b) mall λ Long-lived C tate * e D A G 0 C Charge eparation (C) e D A k C λ small λ large fast C hν G 0 CR Charge Recombination (CR) 1 lo g(k E T/s ) k CR slow CR D A G 0 C G 0 CR G 0 ET / ev λ π 0 5
7 l ogk e t, M s G 0 et, ev 6
8 Me Me Me 2 C M Me Et Me Me Me M Me Me 2 C Et Me Me Me Et M Me Me Me 2 C M = Zn (5, ZnCh C 60 ) M = Zn (1, ZnCh C 60 ) = 2 (3, 2 Ch C 60 ) M = Zn (2, ZnPor C 60 ) = 2 (4, 2 Por C 60 ) CR Me Me Me Me 2 C Me Et M Me l ogk 6 C 4 E Tor k BE T,s M = 2 (6, 2 BCh C 60 ) G 0 ET or G 0 BET, ev
9 (a) Me Me Me Me 2 C Zn Me exyl Et τ = 230 µs (298 K) Me Angew. Chem., Int. Ed., 2004, 45, 853 (b) Zn = C τ = 0.77 µs (298 K) JAC, 2001,, 2607 Me (c) Zn τ = 330 µs (278 K) Me (d) Zn ZnPQ AuPQ + τ = 10 µs (298 K) Au rg. Lett. 2003, 5, 2719 JAC, 2003, 125,
10 (a) (3) (2) (1) Fe C Zn C C C 3 (4) τ = 0.38 s Fc-ZnP- 2 P-C 60 = 3,5-di-t-butylphenyl (b) hν hν hν e e Fe C Zn Zn Zn C C 3 τ = 0.53 s Fc-(ZnP) 3 -C 60 9
11 1 * Fc- ZnP - 2 P-C 60 (2.04 ev) k E Fc-ZnP- 1 2 P * -C 60 (1.89 ev) k ET(C1) Fc-ZnP- 2 P + -C 60 (1.63 ev) k ET(C1) Fc-ZnP P-C 60 hν k ET(CR1) (1.34 ev) k ET(C2) Fc + -ZnP- 2 P-C 60 hν k ET(CR2) (1.11 ev) k ET(CR3) 0.4 s Fc-ZnP- 2 P-C 60 10
12 (C 2 ) n n = 3, 6, 10 Zn hν k CR = ~10 6 s 1 Control of a tructural caffold Control of Redox Reactivity of Quinone µ 11
13 12
14 λ λ Ph + Me λ = 0.34 ev Ph Me (AcrPh + ) (AcrPh ) EXP. 5 G G 1.00 g = C IM. J. Am. Chem. oc. 2001,123, 8459 msl = 0.22 G λ 13
15 14
16 Ph-Q Me 3 Ph-AQ Ph-AQ aph-aq An-AQ aph- 1 (AQ) * (2.85 ev) hυ 0.34 ps aph- 3 (AQ) * 1.7 ps (2.45 ev) 71 s at 263 K in Frozen DM aph + -AQ (1.97 ev) aph-aq 15
17 Bz C 2 BA 0.57 V BA + ZnP-C 60 h ZnP + -C V 0.67 V ZnP P-C V 0.67 V V + V V C (Cl 4 ) 2 + C 6 13 = C = V 2+ nv 2+ Au n BA + V + Au n 2 PC 11 AuMPC BA + BA V 2+ 2 PC 11 AuMPC/V 2+ hν BA 2 P + C 11 AuMPC 1 11AuMPC/V 2+ 2 P * C V + 16
18 2 2 hν Acr -Mes Acr + -Mes Acr + -Mes
19 TE e - e - n 2 TE: ptically Transparent Electrode e - e - e - e - hν e - e - I - / I 3 - Mes-Acr V Mes + -Acr + /(Mes-Acr + ) * Pt -0.2 V - C 60 /C V Mes-Acr + /Mes-Acr CB 0 V VB hν 1.8 V C * - 60 /C 60 Enhanced Photocurrent by upramolecular Charge eparation hν 2.0 V Mes + -Acr + /Mes-Acr V I - 3 /I - n 2 vs E 18
20 e - n 2 e - e - hν TE e - I - / I 3 - e - Pt Acridinium Dye C 60 Ti 2 anoparticle TE: ptically Transparent Electrode 19
21 D 4 P 4 = 2 P-ref D 8 P 8 D 16 P 16 η 20
22 18 a IPCE, % 12 6 b d c Wavelength, nm 21
23 Primary Molecule econdary rganization C (C 2 ) n (n = 5, 11, 15) Toluene C 60 Au Tertiary rganization C11 2 PC15MPC (n=15) 2 PC11MPC (n=11) 2 PC5MPC (n=5) 300 nm C11 Quaternary rganization Au MeC/Tol = 3/1 ( 2 PCnMPC+C 60 ) m η 22
24 e - Pt e TE I - / I 3 - TE: ptically Transparent Electrode e - - Porphyrin C 60 Gold anoparticle e - hν 23
25 λ D 2 D + 2 D 2 D + 2 M n+ M n+ D + 2 D 2 M n+ D + 2 D + 2 M n+ 24
26 hν + Lewis acid hν f Lewis acid Me Me (2) 25
27 g = M n+ Fc Q ET Fc Q Fc + Q /M n+ First Example 6 G Fc + Q /c 3+ Fe + Fc-Q Angew. Chem. Int. Ed. 2002, 41, 620. (C 2 ) 5 ² msl = 0.35 G a(c) = 2.57 G c 3+ a(1) = 1.80 G 1.73 G 0.60 G 0.20 G 0.10 G a(3) = 0.70 G a(2) = 0.09 G a(2) = 0.04 G 26
28 c 3+ Ir(ppy) Q -nc [Ir(ppy) 3 ] + + -Q Q (a) Exp. (Q) 298 K (c) 203 K g = Exp. (n = 2, 3) g = (b) im. 5 G (d) 5 G im. c 3+ a(2c 3+ ) = 1.12 G c 3+ a(8) = 1.12 G Η msl = 0.90 G a(2c 3+ ) = 1.50 G a(c 3+ ) = 0.75 G c 3+ c 3+ c 3+ a(8) = 1.50 G Η msl = 0.75 G 27
29 Fc-Q Fe Fe Fc-Q Me + +M n+ Fe + +M n+ Fe Me M n+ M n+ Fc-(Me)Q 28
30 no alt hυ hυ in DM P* Q 2 P + Q /( 4 + ) 2 in C 2 Cl 2 4 PF 6 no alt Bu 4PF 6 2 P P + + Q Q tabilization tabilization 2 P* Q 2 P + + Q + /Bu 4 29
31 π ππ 30
32 µ µ 1 ZnP*-Im 431 nm hν 2.5 ns (2.12 ev) 0.29 ns ZnP + -Im Š (1.33 ev) Zn ZnP-Im c 3+ nc µs ZnP + -Im Š /c 3+ (0.80 ev) ZnP-Im [c 3+ ] = 1 mm 14 µs 31
33 Fc- 1 AQ* Fc- 1 AQ* Y(Tf) 3 < 500 fs < 500 fs Fe Fc-AQ hυ Fc + -AQ hυ Fc + -AQ Y(Tf) 3 Y(Tf) 3 12 ps 83 µs Fc-AQ Fc-AQ Y(Tf) 3 µ µ 32
34 µµ 33
35 Cu(II)-Zn(II) 2 2 Cu(I)-Zn(II) Cu(I)-Zn(II)
36
37 C 2 Ph C 2 + M n+ Electron Transfer C 2 Ph C 2 (a) M n+ M n+ BA + Q 2M n+ (b) M n+ C 2 M n+ C 2 Ph C 2 Ph M n+ M n+ C 2 M n+ + C 2 M n+ C Ph BA Q M n+ BA + + M n+ g = C 2 Ph keto form tautomerization 2 C 2 Ph enol form C 2 Ph g = D D C 2 Ph 40 G msl = 1.8 G a (2) = 1.0 G a (4) = 53.0 G a (5) = 7.6 G a (6) = 1.8 G a (1) = 8.0 G a (C2Ph) = 7.4 G 40 G msl = 1.8 G a (2) = 1.0 G a (D4) = 8.1 G a (5) = 7.6 G a (6) = 1.8 G a (1) = 8.0 G a (C 2 Ph) = 7.4 G 36
38 C2 C 2 Ph BA e - C2 C 2 Ph Keto Form + + Ru(bpy) 3+ 3 C 2 C 2 + C 2 Ph Ru(bpy) 2+* C 2 Ph BA 3 BA + hν BA + 3 C C 2 Ph Pr i 2 + c 3+ ET without c 3+ 3 C 5 6 g = C 2 Ph Pr i 2 5G K 3 C C 2 Ph msl = 0.21 G c 3+ Pr i 2 k et Fe(Cp * ) 2 Fe(Cp * ) 2 + g = G 3 C c 3+ C 2 Ph 3 C C 2 Ph Pr i 2 c 3+ Pr i 2 a (C 3 ) = 1.03 G a (2) = 0.90 G a (5) = 0.82 G a (6) = 1.11 G a (C 2 Ph) = 2.31 G a (1) = 2.63 G a (c) = 1.24 G 37
39 Bn 2 C C 2 + Bn [(BA) 2 ] Me (Acr + ) Bn + 2 C + Acr C 2 Bn DA Cleavage Bn C BA + Bn (BA + ) C 2 38
40 (a) g // = G g = (b) (BA) 2 + Acr + + Fe 4 Form II Form III Form I Cat. 4 Fe 4 Fe Fe(C 5 4 Me) Catalyst p Co Co p DPA DPB DPX DPD 39
41 2Fe(C 5 5 ) Co(III) + Fe(C5 5) 2 2Fe(C 5 5 ) Co(III) + k et(1) Fe(C 5 5 ) 2 + Fe(C 5 Me 5 ) 2 Co(III) + 2 Co(IV) Co(II) Co(III) + r.d.s - bond cleavage Co(III) Co(III) + Fe(C 5 5 ) 2 Fe(C 5 4 Me) 2 r.d.s Co(III) + Co(III) + + Co(III) + 2 Fe(C 5 5 ) 2 Co(II) Fe(C 5 5 )
42 R R Cat. Me Me Dehydrogenation p Co Co R Me xygenation 41
43 42
44 43
45 44
46 45
47 46
48 47
49 48
50 49
51 µ 50
52 µ 51
53 µ 52
54 µη η µ µ µ 53
55 γ µ 54
56 π 55
57 α 56
58 57
59 π 58
60 π π 59
61 α α π 60
62 é 61
63 62
64 γ 63
65 64
66 µ 65
67 ü ü 66
68 67
69 π é 68
70 69
71 µ 70
72 µ 71
73 γ 72
74 73
75 74
76 75
77 76
78 π 77
79 78
80 79
81 π π 80
82 81
83 82
84 π π 83
85 84
86 85
87 π 86
88 µ 87
89 88
90 α 89
91 π 90
92 91
93 92
94 93
95 ü 94
96 95
97 96
98 π 97
99 98
100 99
101 100
102 101
103 102
104 I 103
105 ü 104
106 105
107 106
物理化学I-第12回(13).ppt
I- 12-1 11 11.1 2Mg(s) + O 2 (g) 2MgO(s) [Mg 2+ O 2 ] Zn(s) + Cu 2+ (aq) Zn 2+ (aq) + Cu(s) - 2Mg(s) 2Mg 2+ (s) + 4e +) O 2 (g) + 4e 2O 2 (s) 2Mg(s) + O 2 (g) 2MgO(s) Zn(s) Zn 2+ (aq) + 2e +) Cu 2+ (aq)
006 11 8 0 3 1 5 1.1..................... 5 1......................... 6 1.3.................... 6 1.4.................. 8 1.5................... 8 1.6................... 10 1.6.1......................
LLG-R8.Nisus.pdf
d M d t = γ M H + α M d M d t M γ [ 1/ ( Oe sec) ] α γ γ = gµ B h g g µ B h / π γ g = γ = 1.76 10 [ 7 1/ ( Oe sec) ] α α = λ γ λ λ λ α γ α α H α = γ H ω ω H α α H K K H K / M 1 1 > 0 α 1 M > 0 γ α γ =
. ev=,604k m 3 Debye ɛ 0 kt e λ D = n e n e Ze 4 ln Λ ν ei = 5.6π / ɛ 0 m/ e kt e /3 ν ei v e H + +e H ev Saha x x = 3/ πme kt g i g e n
003...............................3 Debye................. 3.4................ 3 3 3 3. Larmor Cyclotron... 3 3................ 4 3.3.......... 4 3.3............ 4 3.3...... 4 3.3.3............ 5 3.4.........
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1 1 1.1 64 A6, 1) B1, 1) 65 C A, 1) B, ) C 66 + 1 = 0 A1, 1) B, 0) P 67 A, ) B1, ) C4, 0) 1) ABC G ) A B C P 64 A 1, 1) B, ) AB AB = 1) + 1) A 1, 1) 1 B, ) 1 65 66 65 C0, k) 66 1 p, p) 1 1 A B AB A 67
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36 th ICh - - 5 - - : - 3 ( ) - 169 - -, - - - - - - - G D L U C K final 1 1 1.01 2 e 4.00 3 Li 6.94 4 Be 9.01 5 B 10.81 6 C 12.01 7 N 14.01 8 16.00 9 F 19.00 10 Ne 20.18 11 Na 22.99 12 Mg 24.31 Periodic
ω 0 m(ẍ + γẋ + ω0x) 2 = ee (2.118) e iωt x = e 1 m ω0 2 E(ω). (2.119) ω2 iωγ Z N P(ω) = χ(ω)e = exzn (2.120) ϵ = ϵ 0 (1 + χ) ϵ(ω) ϵ 0 = 1 +
2.6 2.6.1 ω 0 m(ẍ + γẋ + ω0x) 2 = ee (2.118) e iωt x = e 1 m ω0 2 E(ω). (2.119) ω2 iωγ Z N P(ω) = χ(ω)e = exzn (2.120) ϵ = ϵ 0 (1 + χ) ϵ(ω) ϵ 0 = 1 + Ne2 m j f j ω 2 j ω2 iωγ j (2.121) Z ω ω j γ j f j
m(ẍ + γẋ + ω 0 x) = ee (2.118) e iωt P(ω) = χ(ω)e = ex = e2 E(ω) m ω0 2 ω2 iωγ (2.119) Z N ϵ(ω) ϵ 0 = 1 + Ne2 m j f j ω 2 j ω2 iωγ j (2.120)
2.6 2.6.1 mẍ + γẋ + ω 0 x) = ee 2.118) e iωt Pω) = χω)e = ex = e2 Eω) m ω0 2 ω2 iωγ 2.119) Z N ϵω) ϵ 0 = 1 + Ne2 m j f j ω 2 j ω2 iωγ j 2.120) Z ω ω j γ j f j f j f j sum j f j = Z 2.120 ω ω j, γ ϵω) ϵ
= hυ = h c λ υ λ (ev) = 1240 λ W=NE = Nhc λ W= N 2 10-16 λ / / Φe = dqe dt J/s Φ = km Φe(λ)v(λ)dλ THBV3_0101JA Qe = Φedt (W s) Q = Φdt lm s Ee = dφe ds E = dφ ds Φ Φ THBV3_0102JA Me = dφe ds M = dφ ds
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医系の統計入門第 2 版 サンプルページ この本の定価 判型などは, 以下の URL からご覧いただけます. http://www.morikita.co.jp/books/mid/009192 このサンプルページの内容は, 第 2 版 1 刷発行時のものです. i 2 t 1. 2. 3 2 3. 6 4. 7 5. n 2 ν 6. 2 7. 2003 ii 2 2013 10 iii 1987
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ダイアライザー性能評価表
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