Alkane-alkene coupling via tandem alkane-dehydrogenation/alkene-dimerization catalyzed by pincer iridium catalyst heterogenized on solid supports
IPC분류정보
국가/구분
United States(US) Patent
등록
국제특허분류(IPC7판)
C07C-002/36
C07C-005/42
B01J-031/24
출원번호
US-0664333
(2017-07-31)
등록번호
US-10017430
(2018-07-10)
발명자
/ 주소
Mironov, Oleg
Saxton, Robert J.
Goldman, Alan S.
Kumar, Akshai
출원인 / 주소
Chevron U.S.A. Inc.
대리인 / 주소
Hayworth, Melissa M.
인용정보
피인용 횟수 :
0인용 특허 :
15
초록▼
Disclosed herein are processes for tandem alkene dehydrogenation/alkene dimerization using an iridium pincer complex catalyst on a support comprising magnesium silicates (e.g., Florisil®). The reaction process comprises providing an iridium pincer complex bound to a solid support comprising magnesiu
Disclosed herein are processes for tandem alkene dehydrogenation/alkene dimerization using an iridium pincer complex catalyst on a support comprising magnesium silicates (e.g., Florisil®). The reaction process comprises providing an iridium pincer complex bound to a solid support comprising magnesium silicates; providing a gaseous alkane feedstock comprising at least one alkane; and contacting the gaseous alkane feedstock with the iridium pincer complex bound to the solid support in the presence of a hydrogen acceptor to form dimerized alkenes. The processes disclosed herein can accomplish facile, low-temperature tandem transfer dehydrogenation of alkanes and dimerization of alkenes with unprecedented TONs at a reasonable rate of conversion.
대표청구항▼
1. A process for preparing dimerized alkenes in a tandem dehydrogenation/alkene dimerization reaction comprising: providing an iridium pincer complex bound to a solid support comprising magnesium silicates;providing a gaseous alkane feedstock comprising at least one alkane;contacting the gaseous alk
1. A process for preparing dimerized alkenes in a tandem dehydrogenation/alkene dimerization reaction comprising: providing an iridium pincer complex bound to a solid support comprising magnesium silicates;providing a gaseous alkane feedstock comprising at least one alkane;contacting the gaseous alkane feedstock with the iridium pincer complex bound to the solid support in the presence of a hydrogen acceptor to form the dimerized alkenes; andrecovering the dimerized alkenes as recovered dimerized alkenes. 2. The process of claim 1, wherein the at least one alkane of the gaseous alkane feedstock comprises 4 or 5 carbons. 3. The process of claim 1, wherein the recovered dimerized alkenes comprise C7+ dimerized alkenes. 4. The process of claim 3, wherein the recovered dimerized alkenes comprise C7-19 dimerized alkenes. 5. The process of claim 1, wherein the hydrogen acceptor comprises ethylene, propene or mixtures thereof. 6. The process of claim 1, wherein the iridium pincer complex is (p-OMiPr4PCP)Ir(C2H4) bound to the solid support comprising magnesium silicate, where M is K or the solid support. 7. The process of claim 1, wherein the process has a TON for C7+ products of at least 100 at 10 minutes. 8. The process of claim 1, wherein the process has a TON for C7+ products of at least 185 at 40 minutes. 9. The process of claim 1, wherein the process is run for four cycles with a same iridium pincer complex bound to the solid support. 10. The process of claim 9, wherein the process has a TON for olefins in a fourth cycle of at least 40 at 10 minutes. 11. The process of claim 9, wherein the process has turnover frequency rates (TOF) of at least 4260, 960, 300, and 240 TOh−1 in a first, a second, a third, and the fourth cycle respectively. 12. The process of claim 1, wherein the process has a TON for C8 of at least 65 after 10 minutes and of at least 125 after 40 minutes. 13. The process of claim 1, wherein the iridium pincer complex has a Formula wherein M is K or the solid support; “n” is an integer from 0 to 4; and each L is independently H, alkyl, or alkene. 14. The process of claim 13, wherein L is ethylene. 15. The process of claim 1, wherein the iridium pincer complex is selected from the group consisting of: and mixtures thereof. 16. The process of claim 1, wherein the iridium pincer complex is (p-OM-iPr4PCP)Ir(C2H4) or (p-OM-iPr4PCP)Ir(C3H6), where M is K or the solid support. 17. The process of claim 1, wherein the contacting is performed at a reaction temperature of less than 300° C. 18. The process of claim 17, wherein the reaction temperature is 160° C.-260° C. 19. The process of claim 1, wherein the contacting is performed for up to 24 hours. 20. The process of claim 1, wherein the contacting is performed for 10-100 minutes.
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이 특허에 인용된 특허 (15)
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