Complete (1)H resonance assignment of beta-maltose from (1)H-(1)H DQ-SQ CRAMPS and (1)H (DQ-DUMBO)-(13)C SQ refocused INEPT 2D solid-state NMR spectra and first principles GIPAW calculations.
A disaccharide is a challenging case for high-resolution (1)H solid-state NMR because of the 24 distinct protons (14 aliphatic and 10 OH) having (1)H chemical shifts that all fall within a narrow range of approximately 3 to 7 ppm. High-resolution (1)H (500 MHz) double-quantum (DQ) combined rotation...
| Հիմնական հեղինակներ: | , , , , , , , , , , , |
|---|---|
| Ձևաչափ: | Journal article |
| Լեզու: | English |
| Հրապարակվել է: |
2010
|
| _version_ | 1826302781245358080 |
|---|---|
| author | Webber, A Elena, B Griffin, J Yates, JR Pham, T Mauri, F Pickard, C Gil, A Stein, R Lesage, A Emsley, L Brown, S |
| author_facet | Webber, A Elena, B Griffin, J Yates, JR Pham, T Mauri, F Pickard, C Gil, A Stein, R Lesage, A Emsley, L Brown, S |
| author_sort | Webber, A |
| collection | OXFORD |
| description | A disaccharide is a challenging case for high-resolution (1)H solid-state NMR because of the 24 distinct protons (14 aliphatic and 10 OH) having (1)H chemical shifts that all fall within a narrow range of approximately 3 to 7 ppm. High-resolution (1)H (500 MHz) double-quantum (DQ) combined rotation and multiple pulse sequence (CRAMPS) solid-state NMR spectra of beta-maltose monohydrate are presented. (1)H-(1)H DQ-SQ CRAMPS spectra are presented together with (1)H (DQ)-(13)C correlation spectra obtained with a new pulse sequence that correlates a high-resolution (1)H DQ dimension with a (13)C single quantum (SQ) dimension using the refocused INEPT pulse-sequence element to transfer magnetization via one-bond (13)C-(1)H J couplings. Compared to the observation of only a single broad peak in a (1)H DQ spectrum recorded at 30 kHz magic-angle spinning (MAS), the use of DUMBO (1)H homonuclear decoupling in the (1)H DQ CRAMPS experiment allows the resolution of distinct DQ correlation peaks which, in combination with first-principles chemical shift calculations based on the GIPAW (Gauge Including Projector Augmented Waves) plane-wave pseudopotential approach, enables the assignment of the (1)H resonances to the 24 distinct protons. We believe this to be the first experimental solid-state NMR determination of the hydroxyl OH (1)H chemical shifts for a simple sugar. Variable-temperature (1)H-(1)H DQ CRAMPS spectra reveal small increases in the (1)H chemical shifts of the OH resonances upon decreasing the temperature from 348 K to 248 K. |
| first_indexed | 2024-03-07T05:52:41Z |
| format | Journal article |
| id | oxford-uuid:e96e2318-6cc2-42c3-a5ed-47d58147f6c8 |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-03-07T05:52:41Z |
| publishDate | 2010 |
| record_format | dspace |
| spelling | oxford-uuid:e96e2318-6cc2-42c3-a5ed-47d58147f6c82022-03-27T10:54:18ZComplete (1)H resonance assignment of beta-maltose from (1)H-(1)H DQ-SQ CRAMPS and (1)H (DQ-DUMBO)-(13)C SQ refocused INEPT 2D solid-state NMR spectra and first principles GIPAW calculations.Journal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:e96e2318-6cc2-42c3-a5ed-47d58147f6c8EnglishSymplectic Elements at Oxford2010Webber, AElena, BGriffin, JYates, JRPham, TMauri, FPickard, CGil, AStein, RLesage, AEmsley, LBrown, SA disaccharide is a challenging case for high-resolution (1)H solid-state NMR because of the 24 distinct protons (14 aliphatic and 10 OH) having (1)H chemical shifts that all fall within a narrow range of approximately 3 to 7 ppm. High-resolution (1)H (500 MHz) double-quantum (DQ) combined rotation and multiple pulse sequence (CRAMPS) solid-state NMR spectra of beta-maltose monohydrate are presented. (1)H-(1)H DQ-SQ CRAMPS spectra are presented together with (1)H (DQ)-(13)C correlation spectra obtained with a new pulse sequence that correlates a high-resolution (1)H DQ dimension with a (13)C single quantum (SQ) dimension using the refocused INEPT pulse-sequence element to transfer magnetization via one-bond (13)C-(1)H J couplings. Compared to the observation of only a single broad peak in a (1)H DQ spectrum recorded at 30 kHz magic-angle spinning (MAS), the use of DUMBO (1)H homonuclear decoupling in the (1)H DQ CRAMPS experiment allows the resolution of distinct DQ correlation peaks which, in combination with first-principles chemical shift calculations based on the GIPAW (Gauge Including Projector Augmented Waves) plane-wave pseudopotential approach, enables the assignment of the (1)H resonances to the 24 distinct protons. We believe this to be the first experimental solid-state NMR determination of the hydroxyl OH (1)H chemical shifts for a simple sugar. Variable-temperature (1)H-(1)H DQ CRAMPS spectra reveal small increases in the (1)H chemical shifts of the OH resonances upon decreasing the temperature from 348 K to 248 K. |
| spellingShingle | Webber, A Elena, B Griffin, J Yates, JR Pham, T Mauri, F Pickard, C Gil, A Stein, R Lesage, A Emsley, L Brown, S Complete (1)H resonance assignment of beta-maltose from (1)H-(1)H DQ-SQ CRAMPS and (1)H (DQ-DUMBO)-(13)C SQ refocused INEPT 2D solid-state NMR spectra and first principles GIPAW calculations. |
| title | Complete (1)H resonance assignment of beta-maltose from (1)H-(1)H DQ-SQ CRAMPS and (1)H (DQ-DUMBO)-(13)C SQ refocused INEPT 2D solid-state NMR spectra and first principles GIPAW calculations. |
| title_full | Complete (1)H resonance assignment of beta-maltose from (1)H-(1)H DQ-SQ CRAMPS and (1)H (DQ-DUMBO)-(13)C SQ refocused INEPT 2D solid-state NMR spectra and first principles GIPAW calculations. |
| title_fullStr | Complete (1)H resonance assignment of beta-maltose from (1)H-(1)H DQ-SQ CRAMPS and (1)H (DQ-DUMBO)-(13)C SQ refocused INEPT 2D solid-state NMR spectra and first principles GIPAW calculations. |
| title_full_unstemmed | Complete (1)H resonance assignment of beta-maltose from (1)H-(1)H DQ-SQ CRAMPS and (1)H (DQ-DUMBO)-(13)C SQ refocused INEPT 2D solid-state NMR spectra and first principles GIPAW calculations. |
| title_short | Complete (1)H resonance assignment of beta-maltose from (1)H-(1)H DQ-SQ CRAMPS and (1)H (DQ-DUMBO)-(13)C SQ refocused INEPT 2D solid-state NMR spectra and first principles GIPAW calculations. |
| title_sort | complete 1 h resonance assignment of beta maltose from 1 h 1 h dq sq cramps and 1 h dq dumbo 13 c sq refocused inept 2d solid state nmr spectra and first principles gipaw calculations |
| work_keys_str_mv | AT webbera complete1hresonanceassignmentofbetamaltosefrom1h1hdqsqcrampsand1hdqdumbo13csqrefocusedinept2dsolidstatenmrspectraandfirstprinciplesgipawcalculations AT elenab complete1hresonanceassignmentofbetamaltosefrom1h1hdqsqcrampsand1hdqdumbo13csqrefocusedinept2dsolidstatenmrspectraandfirstprinciplesgipawcalculations AT griffinj complete1hresonanceassignmentofbetamaltosefrom1h1hdqsqcrampsand1hdqdumbo13csqrefocusedinept2dsolidstatenmrspectraandfirstprinciplesgipawcalculations AT yatesjr complete1hresonanceassignmentofbetamaltosefrom1h1hdqsqcrampsand1hdqdumbo13csqrefocusedinept2dsolidstatenmrspectraandfirstprinciplesgipawcalculations AT phamt complete1hresonanceassignmentofbetamaltosefrom1h1hdqsqcrampsand1hdqdumbo13csqrefocusedinept2dsolidstatenmrspectraandfirstprinciplesgipawcalculations AT maurif complete1hresonanceassignmentofbetamaltosefrom1h1hdqsqcrampsand1hdqdumbo13csqrefocusedinept2dsolidstatenmrspectraandfirstprinciplesgipawcalculations AT pickardc complete1hresonanceassignmentofbetamaltosefrom1h1hdqsqcrampsand1hdqdumbo13csqrefocusedinept2dsolidstatenmrspectraandfirstprinciplesgipawcalculations AT gila complete1hresonanceassignmentofbetamaltosefrom1h1hdqsqcrampsand1hdqdumbo13csqrefocusedinept2dsolidstatenmrspectraandfirstprinciplesgipawcalculations AT steinr complete1hresonanceassignmentofbetamaltosefrom1h1hdqsqcrampsand1hdqdumbo13csqrefocusedinept2dsolidstatenmrspectraandfirstprinciplesgipawcalculations AT lesagea complete1hresonanceassignmentofbetamaltosefrom1h1hdqsqcrampsand1hdqdumbo13csqrefocusedinept2dsolidstatenmrspectraandfirstprinciplesgipawcalculations AT emsleyl complete1hresonanceassignmentofbetamaltosefrom1h1hdqsqcrampsand1hdqdumbo13csqrefocusedinept2dsolidstatenmrspectraandfirstprinciplesgipawcalculations AT browns complete1hresonanceassignmentofbetamaltosefrom1h1hdqsqcrampsand1hdqdumbo13csqrefocusedinept2dsolidstatenmrspectraandfirstprinciplesgipawcalculations |