NONEQUILIBRIUM NUCLEAR SPIN STATES OF ETHYLENE DURING ACETYLENE HYDROGENATION WITH PARAHYDROGEN OVER IMMOBILIZED IRIDIUM COMPLEXES

I. V. Skovpin; Сковпин И. В.; S. V. Sviyazov; Свиязов С. В.; D. B. Burueva; Буруева Д. Б.; L. M. Kovtunova; Ковтунова Л. М.; A. V. Nartova; Нартова А. В.; R. I. Kvon; Квон Р. И.; V. I. Bukhtiyarov; Бухтияров В. И.; I. V. Koptyug; Коптюг И. В.

doi:10.31857/S2686953522600933

NONEQUILIBRIUM NUCLEAR SPIN STATES OF ETHYLENE DURING ACETYLENE HYDROGENATION WITH PARAHYDROGEN OVER IMMOBILIZED IRIDIUM COMPLEXES

Autores: Skovpin I.V.¹, Sviyazov S.V.¹^,2, Burueva D.B.¹, Kovtunova L.M.¹^,3, Nartova A.V.³, Kvon R.I.³, Bukhtiyarov V.I.³, Koptyug I.V.¹
Afiliações:
1. International Tomography Center, Siberian Branch of the Russian Academy of Sciences
2. Novosibirsk State University
3. Boreskov Institute of Catalysis, Siberian Branch of the Russian Academy of Sciences
Edição: Volume 512, Nº 1 (2023)
Páginas: 120-129
Seção: PHYSICAL CHEMISTRY
URL: https://cardiosomatics.ru/2686-9535/article/view/651961
DOI: https://doi.org/10.31857/S2686953522600933
EDN: https://elibrary.ru/HPUROO
ID: 651961

Citar

Texto integral

Acesso aberto
Acesso é fechado

Acesso está concedido
Acesso é fechado

Acesso é pago ou somente para assinantes

Resumo
Sobre autores
Bibliografia
Arquivos suplementares
Estatísticas

Resumo

In this work rhodium and iridium immobilized complexes were prepared and characterized by X-ray photoelectron spectroscopy. For the first time, hyperpolarized ¹³C-ethylene was detected directly in the gas phase during acetylene hydrogenation with parahydrogen on immobilized iridium complexes. The line shape of polarized ¹³С‑ethylene unambiguously indicates that the hydrogen addition to the triple bond of acetylene on immobilized iridium complexes proceeds via syn-addition. It has been shown that the selective acetylene hydrogenation with parahydrogen over immobilized iridium complexes is an effective chemical method for enriching the nuclear spin isomers of ethylene.

Palavras-chave

hyperpolarization, parahydrogen, parahydrogen-induced polarization, NMR, heterogeneous catalysis, immobilized complexes, XPS, selective hydrogenation, ethylene

Bibliografia

Bos A.N.R., Westerterp K.R. // Chem. Eng. Process. Process Intensif. 1993. V. 32. P. 1–7. https://doi.org/10.1016/0255-2701(93)87001-B
Zhivonitko V.V., Kovtunov K.V., Chapovsky P.L., Kop-tyug I.V. // Angew. Chem. Int. Ed. 2013. V. 52. P. 13251–13255. https://doi.org/10.1002/anie.201307389
Chapovsky P.L., Zhivonitko V.V., Koptyug I.V. // J. Phys. Chem. A. 2013. V. 117. P. 9673–9683. https://doi.org/10.1021/jp312322f
Гельмуханов Ф.Х., Шалагин А.М. // Письма в ЖЭТФ. 1979. V. 29. P. 773–776.
Sun Z.-D., Takagi K., Matsushima F. // Science. 2005. V. 310. P. 1938–1941. https://doi.org/10.1126/science.1120037
Eills J., Budker D., Cavagnero S., Chekmenev E.Y., Elliott S.J., Jannin S., Lesage A., Matysik J., Meersmann T., Prisner T., Reimer J.A., Yang H., Koptyug I.V. // Chem. Rev. 2023. V. 123. P. 1417–1551. https://doi.org/10.1021/acs.chemrev.2c00534
Ковтунов К.В., Буруева Д.Б., Свиязов С.В., Сальников О.Г., Гудсон Б.М., Чекменев Э.Ю., Коптюг И.В. // Изв. АН. Сер. Хим. 2021. V. 12. P. 2382–2389.
Покочуева Е.В., Святова А.И., Буруева Д.Б., Коптюг И.В. // Изв. АН. Сер. Хим. 2023. V. 1. P. 1–19.
Duckett S.B., Mewis R.E. // Acc. Chem. Res. 2012. V. 45 P. 1247–1257. https://doi.org/10.1021/ar2003094
Koptyug I.V., Kovtunov K.V., Burt S.R., Anwar M.S., Hilty C., Han S.-I., Pines A., Sagdeev R.Z. // J. Am. Chem. Soc. 2007. V. 129. P. 5580–5586. https://doi.org/10.1021/ja068653o
Kovtunov K.V., Beck I.E., Bukhtiyarov V.I., Koptyug I.V. // Angew. Chem. Int. Ed. 2008. V. 47. P. 1492–1495. https://doi.org/10.1002/anie.200704881
Kovtunov K.V., Zhivonitko V.V., Skovpin I.V., Barskiy D.A., Koptyug I.V. // Top. Curr. Chem. 2013. V. 338. P. 123–180. https://doi.org/10.1007/128_2012_371
Pokochueva E.V., Burueva D.B., Kovtunova L.M., Bukhtiyarov A.V., Gladky A.Yu., Kovtunov K.V., Koptyug I.V., Bukhtiyarov V.I. // Faraday Discuss. 2021. V. 229. P. 161–175. https://doi.org/10.1039/C9FD00138G
Burueva D.B., Kovtunov K.V., Bukhtiyarov A.V., Barskiy D.A., Prosvirin I.P., Mashkovsky I.S., Baeva G.N., Bukhtiyarov V.I., Stakheev A.Yu., Koptyug I.V. // Chem. Eur. J. 2018. V. 24. P. 2547–2553. https://doi.org/10.1002/chem.201705644
Zhao E.W., Maligal-Ganesh R., Xiao C., Goh T.-W., Qi Z., Pei Y., Hagelin-Weaver H.E., Huang W., Bowers C.R. // Angew. Chem. Int. Ed. 2017. V. 56. P. 3925–3929. https://doi.org/10.1002/anie.201701314
Corma A., Salnikov O.G., Barskiy D.A., Kovtunov K.V., Koptyug I.V. // Chem. Eur. J. 2015. V. 21. P. 7012–7015. https://doi.org/10.1002/chem.201406664
Skovpin I.V., Zhivonitko V.V., Koptyug I.V. // Appl. Magn. Reson. 2011. V. 41. P. 393–410. https://doi.org/10.1007/s00723-011-0255-z
Skovpin I.V., Zhivonitko V.V., Kaptein R., Koptyug I.V. // Appl. Magn. Reson. 2013. V. 44. P. 289–300. https://doi.org/10.1007/s00723-012-0419-5
Skovpin I.V., Zhivonitko V.V., Prosvirin I.P., Khabibulin D.F., Koptyug I.V. // Z. Phys. Chem. 2017. V. 231. P. 575–592. https://doi.org/10.1515/zpch-2016-0824
Skovpin I.V., Kovtunova L.M., Nartova A.V., Kvon R.I., Bukhtiyarov V.I., Koptyug I.V. // Catal. Sci. Technol. 2022. V. 12. P. 3247–3253. https://doi.org/10.1039/D1CY02258J
Crabtree R.H., Morris G.E. // J. Organomet. Chem. 1977. V. 135. P. 395–403. https://doi.org/10.1016/S0022-328X(00)88091-2
Yamada T., Matsuo T., Ogawa A., Ichikawa T., Kobayashi Y., Masuda H., Miyamoto R., Bai H., Meguro K., Sawama Y., Monguchi Y., Sajiki H. // Org. Process Res. Dev. 2018. V. 23. P. 462–469. https://doi.org/10.1021/acs.oprd.8b00291
Huang L., Ang T.P., Wang Z., Tan J., Chen J., Wong P.K. // Inorg. Chem. 2011. V. 50. P. 2094–2111. https://doi.org/10.1021/ic100824e
Crudden C.M., Sateesh M., Lewis R. // J. Am. Chem. Soc. 2005. V. 127. P. 10045–10050. https://doi.org/10.1021/ja0430954
Holsboer F., Beck W., Bartunik H.D. // J. Chem. Soc., Dalt. Trans. 1973. P. 1828–1829. https://doi.org/10.1039/DT9730001828
Fernando N.K., Cairns A.B., Murray C.A., Thompson A.L., Dickerson J.L., Garman E.F., Ahmed N., Ratcliff L.E., Regoutz A. // J. Phys. Chem. A. 2021. V. 125. P. 7473–7488. https://doi.org/10.1021/acs.jpca.1c05759
Bowers C.R., Weitekamp D.P. // J. Am. Chem. Soc. 1987. V. 109. P. 5541–5542. https://doi.org/10.1021/ja00252a049
Salnikov O.G., Kovtunov K.V., Barskiy D.A., Khudorozhkov A.K., Inozemtseva E.A., Prosvirin I.P., Bukhtiya-rov V.I., Koptyug I.V. // ACS Catal. 2014. V. 4. P. 2022–2028. https://doi.org/10.1021/cs500426a
Giordano G., Crabtree R.H., Heintz R.M., Forster D., Morris D.E. Di-μ-chloro-bis(η4-1,5-cyclooctadlene) dirhodium (I). In: Inorganic syntheses. V. 19. Shri-ver D.F. (Ed.). John Wiley & Sons, 1979. P. 218–220. https://doi.org/10.1002/9780470132500.ch50
Moulder J.F., Stickle W.F., Sobol P.E., Bomben K.D. Handbook of X-ray photoelectron spectroscopy. 2nd edn. Perkin-Elmer Corp., Eden Priarie, MN, USA, 1992.
XPSPEAK, свободно распространяемое программное обеспечение для анализа спектров РФЭС // http://xpspeak.software.informer.com/4.1/ (ссылка активна на 27.12.2022).
Квон Р.И., Нартова АВ., Ковтунова Л.М., Бухтияров В.И. // Журн. структ. хим. 2023. V. 64. P. 106142. https://doi.org/10.26902/JSC_id106142