Carbonyl Groups Modified Graphite Sheets Catalyze Oxidative Dehydrogenation of Propane to Propene

doi:10.15541/jim20190040

Abstract

Abstract:

Using earth abundant graphite sheets as raw material, carbonyl groups modified graphite sheets were prepared via a simple gaseous-phase oxidation strategy. As-prepared carbonyl groups modified graphite sheets catalyzed oxidative dehydrogenation of propane (ODHP) to propene with high target product selectivity: the product contains 73.9% propene and 13% ethene when the propane conversion is 12.4%. Its high target product selectivity was much better than carbon nanotube that treated by gaseous-phase oxidation, and could compare favorably with the state-of-the-art hexagonal boron nitride catalysts. After 48 h stability test at 505 ℃, there was no obvious variation in the propane conversion and olefins selectivity, demonstrating the remarkable stability of the carbonyl groups modified graphite sheets catalysts. The characterization results revealed that gaseous-phase oxidation didn’t destroy the structure of graphite sheets and inherit the nature of high thermal stability against oxidation. The content of carbonyl groups increased significantly after gaseous-phase oxidation treatment. As active sites, carbonyl groups could abstract the hydrogen atoms from propane and form hydroxyl groups. Hydroxyl groups could react with oxygen atom and regenerate to carbonyl group. The high target product selectivity can be attributed to the controllable reaction style on catalyst surface. Furthermore, graphite sheets are rich in resource and low cost. As a catalyst, it would promote the industrialization of ODHP.

Key words: carbonyl group, graphite sheet, oxidative dehydrogenation, propane, propene

CLC Number:

O643

CAO Lei, DAI Peng-Cheng, LIU Dan-Dan, GU Xin, LI Liang-Jun, ZHAO Xue-Bo. Carbonyl Groups Modified Graphite Sheets Catalyze Oxidative Dehydrogenation of Propane to Propene[J]. Journal of Inorganic Materials, 2019, 34(11): 1187-1192.

Figures/Tables 9

Fig. 1 TGA curve of carbonyl groups graphite sheets tested at high purity air

Fig. 2 Catalytic performance of ODHP over the carbonyl groups graphite sheets as a function of reaction temperature (a), and olefins yield as a function of propane conversion (b)

Fig. 3 Stability (a) and carbon balance during the catalytic test (b) of carbonyl groups graphite sheets for ODHP over 48 h

Fig. 4 SEM images of carbonyl groups graphite sheets before (fresh) and after (spent) ODHP test (a, b) Fresh; (c, d) Spent

Fig. 5 XRD patterns of carbonyl groups graphite sheets before (fresh) and after (spent) ODHP test

Fig. 6 TEM images of carbonyl groups graphite sheets after ODHP stability test

Fig. 7 N2 adsorption/desorption isotherms (a) and DFT pore size distribution (b) of carbonyl groups graphite sheets before (fresh) and after (spent) ODHP test

Fig. 8 FT-IR spectra of the carbonyl groups graphite sheets before (fresh) and after (spent) ODHP test

Fig. 9 XPS spectra (a) and fitting curves of O1s spectra (b) of carbonyl groups graphite sheets before (fresh) and after (spent) ODHP test

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