Effect of calcination atmospheres on the catalytic performance of nano-CeO2 in direct synthesis of DMC from methanol and CO2

Zixiang Cui; Jie Fan; Huijuan Duan; Junfeng Zhang; Yongqiang Xue; Yisheng Tan

Korean Journal of Chemical Engineering, Vol.34, No.1, 29-36, January, 2017

DOI10.1007/s11814-016-0212-5 Export Citation

Effect of calcination atmospheres on the catalytic performance of nano-CeO2 in direct synthesis of DMC from methanol and CO2

Zixiang Cui, Jie Fan, Huijuan Duan, Junfeng Zhang¹, Yongqiang Xue^†, and Yisheng Tan^{1, †}

Department of Applied Chemistry, Taiyuan University of Technology, Taiyuan 030024, China
¹State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China

E-mail:,

Nano-CeO2 was prepared through the calcination of Ce(OH)3 precursor in different atmospheres (H2, Ar, air, O2), which was prepared by a hydrothermal method, and then used as catalysts in the direct synthesis of dimethyl carbonate (DMC) from methanol and CO2. The results indicated that the catalyst calcined in O2 (CeO2-O2) showed an optimum catalytic performance, and the yield of DMC reached to 1.304mmol/mmolcat. In addition, reaction temperature and weight of catalyst were optimized. Based on characterizations of the catalysts, the ratio of Ce(IV)/Ce(III) and Lewis acid-base property of nano-CeO2 catalyst could be adjusted through different calcination atmosphere treatment. It was determined that the higher activity of CeO2-O2 catalyst is mainly attributed to its higher ratio of Ce(IV)/Ce(III) as well as abundant and moderate intensity Lewis acid base sites.

Keywords:Nano-CeO2;Calcination Temperature;Valence State;Methanol;CO2;DMC

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[Referenced By]

[1] Ono Y, Pure Appl. Chem., 68(2), 367 (1996)

[2] Kumar P, Srivastava VC, Mishra IM, Korean J. Chem. Eng., 32(9), 1774 (2015)

[3] Qin X, Zhao W, Han B, Liu B, Lian P, Wu S, Korean J. Chem. Eng., 32(6), 1 (2015)

[4] Larsen JW, Energy Fuels, 11(1), 1 (1997)

[5] Delledonne D, Rivetti F, Romano U, Appl. Catal. A: Gen., 221(1), 241 (2001)

[6] Ono Y, Appl. Catal. A: Gen., 155(2), 133 (1997)

[7] Fu Y, Baba T, Ono Y, Appl. Catal. A: Gen., 166(2), 419 (1998)

[8] Choi JC, He LN, Yasuda H, Sakakura T, Green Chem., 4(3), 230 (2002)

[9] Ballivet-Tkatchenko D, Chambrey S, Keiski R, Ligabue R, Plasseraud L, Richard P, Turunen H, Catal. Today, 115(1), 80 (2006)

[10] Nam JK, Choi MJ, Cho DH, Suh JK, Kim SB, J. Mol. Catal. A-Chem., 370, 7 (2013)

[11] Bian J, Wei XW, Jin YR, Wang L, Luan DC, Guan ZP, Chem. Eng. J., 165(2), 686 (2010)

[12] Han MS, Lee BG, Suh I, Kim HS, Ahn BS, Hong SI, J. Mol. Catal. A-Chem., 170(1), 225 (2001)

[13] Wang H, Shi S, Wang Y, Li CS, Sun J, J. Shanghai University, 14, 281 (2010)

[14] Wang SP, Zhou JJ, Zhao SY, Zhao YJ, Ma XB, Chin. Chem. Lett., 26(9), 1096 (2015)

[15] Aresta M, Dibenedetto A, Pastore C, Angelini A, Aresta B, Papai I, J. Catal., 269(1), 44 (2010)

[16] Zhang M, Xiao M, Wang S, Han D, Lu Y, Meng Y, J. Clean Prod., 103, 847 (2014)

[17] Chen L, Wang S, Zhou J, Shen Y, Zhao Y, Ma X, RSC Adv., 4(59), 30968 (2014)

[18] Wang S, Zhao L, Wang W, Zhao Y, Zhang G, Ma X, Gong J, Nanoscale, 5(12), 5582 (2013)

[19] Aresta M, Dibenedetto A, Pastore C, Cuocci C, Aresta B, Cometa S, De Giglio E, Catal. Today, 137(1), 125 (2008)

[20] Wang W, Direct Synthesis of Dimethyl Carbonate from CO2 and Methanol over CeO2 Catalyst, Tianjin University (2011).

[21] Bansode A, Urakawa A, Acs Catal., 4(11), 3877 (2014)

[22] Bauchspiess KR, Boksch W, Holland-Moritz E, Launois H, Pott R, Wohlleben D, North-Holland Publications, Amsterdam, (1981).

[23] Fujimori A, Phys. Rev. B, 28(4), 2281 (1983)

[24] Kotani A, Mizuta H, Jo T, Solid State Commun., 53(9), 805 (1985)

[25] Yoshida Y, Arai Y, Kado S, Kunimori K, Tomishige K, Catal. Today, 115(1), 95 (2006)

[26] Tomishige K, Furusawa Y, Ikeda Y, Asadullah M, Fujimoto K, Catal. Lett., 76(1-2), 71 (2001)

[27] Romeo M, Bak K, El Fallah J, Le Normand F, Hilaire L, Surf. Interface Anal., 20(6), 508 (1993)

[28] Pfau A, Schierbaum KD, Surf. Sci., 321, 71 (1994)

[29] Larachi F, Pierre J, Adnot A, Bernis A, Appl. Surf. Sci., 195, 234 (2002)

[30] Mullins DR, Overbury SH, Huntley DR, Surf. Sci., 409, 307 (1998)

[31] Hou XL, Xu HF, Dong JH, Sun X, DianHuaxue, 12(1), 89 (2006)

[32] Ovari L, Calderon SK, Lykhach Y, Libuda J, Erdohelyi A, Papp C, Kiss J, Steinruck HP, J. Catal., 307, 132 (2013)

[33] Trudeau ML, Tschope A, Ying JY, Surf. Interface Anal., 23(4), 219 (1995)

[34] Hong ST, Park HS, Lim JS, Lee YW, Anpo M, Kim JD, Res. Chem. Intermed., 32(8), 737 (2006)

[35] Lee HJ, Park S, Song IK, Jung JC, Catal. Lett., 141(4), 531 (2011)

[36] La KW, Jung JC, Kim H, Baeck SH, Song IK, J. Mol. Catal. A-Chem., 269(1), 41 (2007)

[37] Lee HJ, Joe W, Song IK, Korean J. Chem. Eng., 29(3), 317 (2012)

[38] Ikeda Y, Asadullah M, Fujimoto K, Tomishige K, J. Phys. Chem. B, 105(43), 10653 (2001)

[39] Jung KT, Shul YG, Bell AT, Kim HJ, J. Korean Ind. Eng. Chem., 12(7), 814 (2001)