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β-oxopropylcarbamate 6 can be obtained via tautomerization.
In the case of a primary amine, further intramolecular nucleo-
philic attack followed by dehydration affords the oxazolidinone
4.
Notes and references
1 (a) P. H. Abelson, Science, 2000, 289, 1293; (b) D. W. Keith,
Science, 2009, 325, 1654–1655; (c) C. Federsel, R. Jackstell
and M. Beller, Angew. Chem., Int. Ed., 2010, 49, 6254–6257;
(d) A.-H. Liu, R. Ma, C. Song, Z.-Z. Yang, A. Yu, Y. Cai,
L.-N. He, Y.-N. Zhao, B. Yu and Q.-W. Song, Angew. Chem.,
Int. Ed., 2012, 51, 11306–11310.
Conclusions
In summary, we have described a sustainable and cost-com-
petitive catalytic process promoted by the Ag2WO4/Ph3P system
for efficient chemical fixation of CO2 to produce α-alkylidene
cyclic carbonates, α-alkylidene cyclic carbamates, and β-oxo-
propylcarbamates under mild conditions, respectively. The
scope of the reaction is broad, with a variety of propargylic
alcohols undergoing carboxylative cyclization. Moreover, the
three-component reactions of propargylic alcohols, amines
and CO2 are also well performed with this protocol. In
addition, this procedure can eliminate the need for large quan-
tities of caustic base and flammable organic solvents, yielding
the strategy to prepare value-added α-alkylidene cyclic carbon-
ates, α-alkylidene cyclic carbamates, and β-oxopropylcarba-
mates from both environmental and economical points of
view. Importantly, the catalytic system is not sensitive to air
and minor moisture, which may enhance the possibility of fix-
ation of CO2. Such findings may be of great interest for devel-
oping alternative access to chemical fixation of CO2 with the
preparation of the CO2-based products under mild conditions.
2 (a) D. J. Darensbourg, Chem. Rev., 2007, 107, 2388–2410;
(b) J. Louie, Curr. Org. Chem., 2005, 9, 605–623;
(c) S. N. Riduan and Y. Zhang, Dalton Trans., 2010, 39,
3347–3357; (d) X. Yin and J. R. Moss, Coord. Chem. Rev.,
1999, 181, 27–60; (e) Z.-Z. Yang, Y.-N. Zhao and L.-N. He,
RSC Adv., 2011, 1, 545–567; (f) L.-N. He, J.-Q. Wang and
J.-L. Wang, Pure Appl. Chem., 2009, 81, 2069–2080.
3 For reviews on chemical fixation of CO2, see:
(a) T. Sakakura, J.-C. Choi and H. Yasuda, Chem. Rev., 2007,
107, 2365–2387; (b) M. Cokoja, C. Bruckmeier, B. Rieger,
W. A. Herrmann and F. E. Kühn, Angew. Chem., Int. Ed.,
2011, 50, 8510–8537; (c) K. Huang, C.-L. Sun and Z.-J. Shi,
Chem. Soc. Rev., 2011, 40, 2435–2452; (d) Y. Tsuji and
T. Fujihara, Chem. Commun., 2012, 48, 9956–9964;
(e) W.-Z. Zhang and X.-B. Lu, Chin. J. Catal., 2012, 33, 745–
756; (f) Z.-Z. Yang, L.-N. He, J. Gao, A.-H. Liu and B. Yu,
Energy Environ. Sci., 2012, 5, 6602–6639.
4 (a) G. Centi, E. A. Quadrelli and S. Perathoner, Energy
Environ. Sci., 2013, 6, 1711–1731; (b) P. Markewitz,
W. Kuckshinrichs, W. Leitner, J. Linssen, P. Zapp,
R. Bongartz, A. Schreiber and T. E. Muller, Energy Environ.
Sci., 2012, 5, 7281–7305.
5 A few reports on the transformation of α-alkylidene cyclic
carbonates, see: (a) Y. Inoue, K. Matsushita, I. F. Yen and
S. Imaizumi, Chem. Lett., 1991, 20, 1377–1378; (b) K. Ohe,
H. Matsuda, T. Ishihara, S. Ogoshi, N. Chatani and
S. Murai, J. Org. Chem., 1993, 58, 1173–1177; (c) K. Ohe,
H. Matsuda, T. Morimoto, S. Ogoshi, N. Chatani and
S. Murai, J. Am. Chem. Soc., 1994, 116, 4125–4126;
(d) M. Yoshida and M. Ihara, Angew. Chem., Int. Ed., 2001,
40, 616–619.
Experimental section
General procedure for the synthesis of α-alkylidene cyclic car-
bonates 2a: Ag2WO4 (23.2 mg, 1 mol%), PPh3 (26.2 mg, 2 mol%),
and propargylic alcohols (5 mmol) were added to
a
Schlenk tube equipped with a magnetic stir bar. A CO2 balloon
was consecutively introduced. Then the mixture was stirred at
25 °C for the desired time. Upon completion, the mixture was
diluted with n-hexane (3 × 5 mL). The organic phase was col-
lected and then purified by column chromatography on silica
gel using petroleum ether–ethyl acetate as an eluent to give the
desired products. The solid residue in the tube was Ag2WO4,
which could be used directly in the next run. 2a was obtained
as a colourless oil. 1H NMR (CDCl3, 400 MHz) δ 4.75 (d, J = 4.0
Hz, 1H), 4.31 (d, J = 4.0 Hz, 1H), 1.59 (s, 6H) ppm. 13C NMR
6 C. Bruneau and P. H. Dixneuf, J. Mol. Catal., 1992, 74,
97–107.
7 K. Iritani, N. Yanagihara and K. Utimoto, J. Org. Chem.,
1986, 51, 5499–5501.
8 Y. Inoue, J. Ishikawa, M. Taniguchi and H. Hashimoto,
Bull. Chem. Soc. Jpn., 1987, 60, 1204–1206.
(CDCl3, 100.6 MHz)
δ 158.6 (CvO), 151.2, 85.2, 84.6,
27.5 ppm. MS (EI, 70 eV) m/z (%) = 128.10 (2.81), 85.10 (6.49),
84.10 (100), 83.10 (3.54), 69.10 (48.16).
9 (a) H.-S. Kim, J.-W. Kim, S.-C. Kwon, S.-C. Shim and
T.-J. Kim, J. Organomet. Chem., 1997, 545–546, 337–344;
(b) H.-F. Jiang, A.-Z. Wang, H.-L. Liu and C.-R. Qi,
Eur. J. Org. Chem., 2008, 2309–2312.
10 (a) S. Kikuchi, S. Yoshida, Y. Sugawara, W. Yamada,
K. Sekine, I. Iwakura, T. Ikeno, T. Yamada and
H.-M. Cheng, Bull. Chem. Soc. Jpn., 2011, 84, 698–717;
(b) W. Yamada, Y. Sugawara, H. M. Cheng, T. Ikeno and
T. Yamada, Eur. J. Org. Chem., 2007, 2604–2607.
Acknowledgements
We are grateful to the National Natural Science Foundation of
China (no. 21172125 and 21376123), Specialized Research
Fund for the Doctoral Program of Higher Education
(20130031110013), and Tianjin Co-Innovation Center of 11 T.-J. Kim, K.-H. Kwon, S.-C. Kwon, J.-O. Baeg, S.-C. Shim
Chemical Science and Engineering.
and D.-H. Lee, J. Organomet. Chem., 1990, 389, 205–217.
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