Effect of Surface Cu0 Content of the Catalysts on CO2 Hydrogenation to C2+ Alcohols †

doi:10.7503/cjcu20200061

Abstract

Abstract:

Pyrolyzing metal organic framework(MOF) material Fe-MIL-88B loaded with Cu in air atmosphere, uniformly dispersed CuFe based catalysts with different Cu and Fe valence distribution were gained at different reduction temperatures. The structure of the catalysts were characterized by means of X-ray diffraction(XRD), X-ray photoelectron spectroscopy(XPS), H₂ temperature program reduction(H₂-TPR), N₂ adsorption-desorption(BET), scanning electron microscopy(SEM), and high resolution transmission electron microscopy(HRTEM). The catalytic performances of CO₂ hydrogenation to C₂₊ alcohols were investigated on a fixed-bed reactor. It was found that the higher the reduction temperature was, the more percentage of Cu and Fe with lower valence state was on the surface of the catalysts. When the reduction temperature was 350 ℃, Cu⁰/(Cu⁺+Cu⁰) was 73.9 %, and 0.4% Fe ⁰ appeared, the catalytic performance was the best, where the CO₂ conversion rate was 6.82%, the total alcohol selectivity was 39.4%, and the molar percentage of C₂₊ alcohol was 95.1%.

Key words: Fe-MIL-88B, CuFe Catalyst, Reduction temperature, C₂₊ Alcohol, CO₂ Hydrogenation

CLC Number:

O643.3

TrendMD:

ZHANG Weizhong,WEN Yueli,SONG Rongpeng,WANG Bin,ZHANG Qian,HUANG Wei. Effect of Surface Cu⁰ Content of the Catalysts on CO₂ Hydrogenation to C₂₊ Alcohols ^†[J]. Chem. J. Chinese Universities, 2020, 41(6): 1297.

Figures/Tables 9

References 36

[1]	Choi Y. H., Jang Y. J., Park H., Kim W. Y., Lee Y. H., Choi S. H., Lee J. S., Appl. Catal. B, 2017, 202, 605—610 doi: 10.1016/j.apcatb.2016.09.072 URL
[2]	Surisetty V. R., Dalai A. K., Kozinski J., Appl. Catal. A, 2011, 404(1/2), 1—11
[3]	Yu J., Mao D. S., Han L. P., Guo Q. S., Lu G. Z., J. Ind. Eng. Chem., 2013, 19(3), 806—812 doi: 10.1016/j.jiec.2012.10.021 URL
[4]	Claure M. T., Chai S. H., Dai S., Unocic K. A., Alamgir F. M., Agrawal P. K., Jones C. W., J. Catal., 2015, 324, 88—97 doi: 10.1016/j.jcat.2015.01.015 URL
[5]	Cheng S. Y., Gao Z. H., Kou J. W., Liu Y., Huang W., Energy Fuels, 2017, 31(8), 8572—8579 doi: 10.1021/acs.energyfuels.7b01307 URL
[6]	Xiao K., Qi X. Z., Bao Z. H., Wang X. X., Zhong L. S., Fang K. G., Lin M. G., Sun Y. H., Catal. Sci. Technol., 2013, 3(6), 1591—1602 doi: 10.1039/c3cy00063j URL
[7]	Xiao K., Bao Z. H., Qi X. Z., Wang X. X., Zhong L. S., Fang K. G., Lin M. G., Sun Y. H., J. Mol. Catal. A: Chem., 2013, 378, 319—325 doi: 10.1016/j.molcata.2013.07.006 URL
[8]	Cheng Y., Tavares S. R., Doherty C. M., Ying Y., Sarnello E., Maurin G., Zhao D., ACS Appl. Mater. Interfaces, 2018, 10(49), 43095—43103 doi: 10.1021/acsami.8b16386 URL
[9]	Chen Y. Z., Wang C., Wu Z. Y., Xiong Y., Xu Q., Yu S. H., Jiang H. L., Adv. Mater., 2015, 27(34), 5010—5016 doi: 10.1002/adma.201502315 URL
[10]	Bai Y. Z., Yi B. L., Li J., Jiang S. F., Zhang H. J., Shao Z. G., Song Y. J., Chin. J. Catal., 2016, 37(7), 1127—1133 doi: 10.1016/S1872-2067(15)61104-4 URL
[11]	Yin Y. Z., Hu B., Li X. L., Zhou X. H., Hong X. L., Liu G. L., Appl. Catal. B, 2018, 234, 143—152 doi: 10.1016/j.apcatb.2018.04.024 URL
[12]	Rungtaweevoranit B., Baek J., Araujo J. R., Archanjo B. S., Choi K. M., Yaghi O. M., Somorjai G. A., Nano Lett., 2016, 16(12), 7645—7649 doi: 10.1021/acs.nanolett.6b03637 URL
[13]	Zhang C., Liao P. Y., Wang H., Sun J., Gao P., Mater. Chem. Phys., 2018, 215, 211—220 doi: 10.1016/j.matchemphys.2018.05.028 URL
[14]	Ramirez A., Gevers L., Bavykina A., Ould-Chikh S., Gascon J., ACS Catal., 2018, 8(10), 9174—9182 doi: 10.1021/acscatal.8b02892 URL
[15]	Hu S., Liu M., Ding F. S., Song C. S., Zhang G. L., Guo X. W., J. CO₂ Util., 2016, 15, 89—95
[16]	Liu J. H., Zhang A. F., Liu M., Hu S., Ding F. S., Song C., Guo X.W., J. CO₂ Util., 2017, 21, 100—107
[17]	Liu R. W., Qin Z. Z., Ji H. B., Su T. M., Ind. Eng. Chem. Res., 2013, 52(47), 16648—16655 doi: 10.1021/ie401763g URL
[18]	Samiee L., Shoghi F., Vinu A., Appl. Surf. Sci., 2013, 265, 214—221 doi: 10.1016/j.apsusc.2012.10.173 URL
[19]	Kameoka S., Tanabe T., Tsai A. P., Catal. Lett., 2005, 100(1/2), 89—93 doi: 10.1007/s10562-004-3091-z URL
[20]	Faungnawakij K., Tanaka Y., Shimoda N., Fukunaga T., Kikuchi R., Eguchi K., Appl. Catal. B, 2007, 74(1/2), 144—151 doi: 10.1016/j.apcatb.2007.02.010 URL
[21]	Yamashita T., Hayes P., Appl. Surf. Sci., 2008, 254(8), 2441—2449 doi: 10.1016/j.apsusc.2007.09.063 URL
[22]	Lu W. S., Shen Y. H., Xie A. J., Zhang W. Q., J. Magn. Magn. Mater., 2010, 322(13), 1828—1833 doi: 10.1016/j.jmmm.2009.12.035 URL
[23]	Zhao B. R., Liu Y. J., Zhu Z. J., Guo H. Z., Ma X. X., J. CO₂ Util., 2018, 24, 34—39
[24]	Liu J. H., Zhang A. F., Jiang X., Liu M., Sun Y. W., Song C. S., Guo X. W., ACS Sustainable Chem. Eng., 2018, 6(8), 10182—10190 doi: 10.1021/acssuschemeng.8b01491 URL
[25]	Liu J., He P., Wang L., Liu H., Cao Y., Li H., Chin. J. Catal., 2018, 39(8), 1283—1293 doi: 10.1016/S1872-2067(18)63032-3 URL
[26]	Qi W., Ling Q., Ding D., Chen Y. Z., Shi C. W., Peng C., Wang Y., Zhang Q. H., Liu R., Hao S., Catal. Commun., 2018, 108, 68—72 doi: 10.1016/j.catcom.2018.01.009 URL
[27]	Gao W., Zhao Y. F., Liu J. M., Huang Q. W., He S., Li C. M., Zhao J. W., Min W., Catal. Sci. Technol., 2013, 3(5), 1324—1332 doi: 10.1039/c3cy00025g URL
[28]	Guo W., Gao W. G., Wang H., Tian J. J., Han C., Qin Z. Q. , Mater. Rev. 2013, 27(20), 47—50
	( 郭伟, 高文桂, 王华, 田俊杰, 韩冲, 覃志强 . 材料导报, 2013, 27(20) 47—50)
[29]	Chen Y., Choi S., Thompson L. T., J. Catal., 2016, 343, 147—156 doi: 10.1016/j.jcat.2016.01.016 URL
[30]	Zheng J. N., An K., Wang J. M., Li J., Liu Y. , J. Fuel Chem. Technol. 2019, 47(6), 697—708 doi: 10.1016/S1872-5813(19)30031-3 URL
	( 郑晋楠, 安康, 王嘉明, 李晶, 刘源 . 燃料化学学报, 2019, 47(6) 697—708) doi: 10.1016/S1872-5813(19)30031-3 URL
[31]	Yin L. H., Gao Z. H., Huang W. , Coal Conversion 2004, 27(2), 85—88
	( 阴丽华, 高志华, 黄伟 . 煤炭转化, 2004, 27(2) 85—88)
[32]	Li S. G., Guo H. J., Luo C. R., Zhang H. R., Xiong L., Chen X., Ma L. L., Catal. Let., 2013, 143(4), 345—355 doi: 10.1007/s10562-013-0977-7 URL
[33]	Li S., Wang X. N., Phys. Lett. B, 2002, 527(1/2), 85—91 doi: 10.1016/S0370-2693(02)01179-6 URL
[34]	Gupta M., Smith M. L., Spivey J. J., ACS Catal., 2011, 1(6), 641—656 doi: 10.1021/cs2001048 URL
[35]	Kiennemann A., Barama A., Boujana S., Bettahar M. M., Appl. Catal. A, 1993, 99(2), 175—194 doi: 10.1016/0926-860X(93)80098-B URL
[36]	Xiao K., Bao Z. H., Qi X. Z., Wang X.X., Zhong L. S., Lin M. G., Fang K. G., Sun Y. H., Catal. Commun., 2013, 40, 154—157 doi: 10.1016/j.catcom.2013.06.024 URL

Catalyst	Surface molar fraction(%)
Catalyst	Cu⁺	Cu⁰	Fe³⁺	Fe²⁺	Fe or Fe₃C
R-250	34.4	65.6	48.6	51.4	——
R-350	26.1	73.9	46.5	53.1	0.4
R-450	28.3	71.7	41.2	55.1	3.7

Catalyst	Surface molar fraction(%)
Catalyst	Cu⁺	Cu⁰	Fe³⁺	Fe²⁺	Fe or Fe₃C
R-250	34.4	65.6	48.6	51.4	——
R-350	26.1	73.9	46.5	53.1	0.4
R-450	28.3	71.7	41.2	55.1	3.7

Catalyst	C₁OH	C₂OH	C₃OH	C₄OH
R-N	5.48	62.8	16.1	15.6
R-250	3.71	56.6	16.7	23.0
R-350	4.94	61.5	22.3	11.3
R-450	5.80	59.3	13.0	21.9

Catalyst	C₁OH	C₂OH	C₃OH	C₄OH
R-N	5.48	62.8	16.1	15.6
R-250	3.71	56.6	16.7	23.0
R-350	4.94	61.5	22.3	11.3
R-450	5.80	59.3	13.0	21.9

Effect of Surface Cu⁰ Content of the Catalysts on CO₂ Hydrogenation to C₂₊ Alcohols ^†

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