Chemistry 125: Lecture 61 March 25, 2011 NMR Spectroscopy This Higher-Order Effects Dynamics Proton Decoupling For copyright notice see final page of this file Spin-Spin Splitting: Other Nuclei & Higher-Order Effects J 13 C-H 99% of sample is C12 Coupling electron must be on the C13 nucleus. Amplify 30x (instrumental artifact) 126 Hz Hybridization and J coupling (Hz) C C C (-CH2-) C C (-CH2-) C C ( C-H) ( CH2) C C sp3 Three Populations 2 sp sp Why does CH4 give a single unsplit peak instead of a quartet? 7.700 7.647 1.270 0.053 Chem 220 15.7 Hz NMR Problem 7 7.673 Unsymmetrical Doublets 381 Hz mess! Bo (T) d (Hz) / J (Hz) 7.05 (3002.89 MHz) 0.86 0.29 0.06 24.4 10.0 3.0 0.5 0.2 6.429 6.377 0.052 15.6 Hz 6.403 Cinnamic Acid 8 7.5 100 200 Change to Frequency Scale 07 dHz (ppm) -100 6.5 -200 6 Energy of Nuclear Spin States in Bo O “Higher-Order” Effects J/4 1/√2( p* O C O C p C d J/4 J also mixes with toward ) & 1/√2( This influences Suppose the spins the intensity of interact favorably the transitions. as magnetic when antiparallel. 5 to see the J/4 Enlarge by ~10perpendicular d/2 ppm energy difference to and Bo blue as or between red environments J ) non-magnetic . C=O analogy J/4 d chemical shift J Rf light loses its “handle” on the flanking peaks as d becomes small compared to J J 3 d 1 0.6 By increasing d (Hz) a strong magnet reduces asymmetry and gives “ideal” pattern. Note: d is measured in Hz (not ppm) between the weighted average positions of the lines in the two doublets 0.2 Dynamics (the NMR Time Scale / Decoupling) e.g. J&F Sec. 15.9 pp. 746-749 Sec. 15.6e p. 739 DMSO H+ HOCH2CH3 CDCl3 2.00 average of many HOCH2CH 3 HOCH2CH3 1.00 2.00 1.14 2.00 + CDCl3 H H+ DMSO CDCl3 CDCl3 H+ H-bond structures 3.05 on (dependent concentration, solvent, & temperature) 3.03 OH CH3CH 2 spin-spin splitting? average for H exchange among many molecules, (fast with H+ slow in DMSO) spectra courtesy of P. Lichtor 0.96 ROH chemical 3.04 shift? R O HH H O R H O HH R d- d+ CD3 O H O S R CD3 Form A Form A Why doesn’t (This particular sample IR show OH is a solid, but no averaging is observed in solution averaging? spectra either.) 110 x 1010 Hz 102 x 1010 Hz Difference ~ 1011 Hz How long does it take to measure frequency precisely? light field 20 Hz But a 1 sec pulse samples full range of phases. 21 Hz No netwith interaction Match a short with pulselight. of 20pulse Hz light is nearly as 1 sec light distinguishes 20good. Hz from 21 Hz. 22 Hz 0.5 sec (1/) is long enough to sample the full range, favorable and unfavorable. 1 second What if a proton changes frequency faster than 1/? 20 Hz 21 Hz Very good match with the 21Hz average frequency single, sharp peak. 22 Hz 20 Hz 22 Hz 1 second 20 Hz 22 Hz 22 20Hz Hz When do Peaks Average? When atoms don’t stay put long enough to tell the difference in frequency. e.g. If two peaks differ by 100 Hz, you must count for ~0.01 sec to tell them apart. These IR peaks differ by 1011 Hz. Exchange of position is not that fast. The NMR Time Scale Single, sharp peak at room temperature, even for C6H12 Handy way to measure fast rates and small barriers Cyclohexane-d11 d11 to avoid complications from spin-spin splitting -49 D -57 Coalesce with lifetime ~ 4 -60 Barrier 10.5 kcal/mole -63 D -68 -89 (°C) = 29 Hz (0.48 ppm at 60 MHz) F. A. Bovey (1965) a b c Almost anyplace (d 1-6) depending on concentration and temperature (averaged H-bonding) Probably no splitting (broad singlet) because of rapid OH proton exchange among different molecules Slightly deshielded by two oxygen atoms on neighboring carbon d 1-2 (a real analogue is at d 1.3) 1:1 doublet from single H on neighboring carbon (J about 7 Hz) Deshielded by two oxygen atoms on the same carbon d 4-5 (a real analogue is at d 4.7) 1:3:3:1 quartet from three H atoms on neighboring carbon (J about 7 Hz) d e f Slightly deshielded by oxygen atom on neighboring carbon d 1 (a real analogue is at d 1.1) Deshielded by oxygen atom on the same carbon (but less than c) d 4 (a real analogue is at d 3.8) Slightly deshielded by oxygen atom on neighboring carbon. d 1 (a real analogue is at d 1.1) different from d (diastereotopic) 1:1 doublet from single H on neighboring C (J about 7 Hz) Seven line multiplet from 6 H atoms on neighboring carbons (J about 7 Hz) 1:1 doublet from single H on neighboring carbon (J about 7 Hz) Proton Decoupling 25 MHz 100 MHz (in frame rotating at 100 MHz) 13C C13 NMR spectrum irradiate H (100 MHz) and pulse (25MHz) to observe C13 H H NMR spectrum or or J ~ 125 Hz H up H average H down Decoupling Power determines the rate of this precession. C13 up C12 C13 down End of Lecture 61 March 25, 2011 Copyright © J. M. McBride 2010. Some rights reserved. Except for cited third-party materials, and those used by visiting speakers, all content is licensed under a Creative Commons License (Attribution-NonCommercial-ShareAlike 3.0). Use of this content constitutes your acceptance of the noted license and the terms and conditions of use. Materials from Wikimedia Commons are denoted by the symbol . Third party materials may be subject to additional intellectual property notices, information, or restrictions. The following attribution may be used when reusing material that is not identified as third-party content: J. M. McBride, Chem 125. License: Creative Commons BY-NC-SA 3.0