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Frontiers of Chemical Science and Engineering

ISSN 2095-0179

ISSN 2095-0187(Online)

CN 11-5981/TQ

Postal Subscription Code 80-969

2018 Impact Factor: 2.809

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Front. Chem. Sci. Eng.    2022, Vol. 16 Issue (10) : 1505-1513    https://doi.org/10.1007/s11705-022-2164-0
RESEARCH ARTICLE
Catalytic hydrogenation of insoluble organic matter of CS2/Acetone from coal over mesoporous HZSM-5 supported Ni and Ru
Reyila Abuduwayiti1, Feng-Yun Ma1(), Xing Fan1,2()
1. Key Laboratory of Coal Clean Conversion & Chemical Engineering Process of Xinjiang Uygur Autonomous Region, Xinjiang University, Urumqi 830046, China
2. College of Chemical and Biological Engineering, Shandong University of Science and Technology, Qingdao 266590, China
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Abstract

Four supported catalysts, nickel and ruthenium on a HZSM-5 support, were prepared by equal volume impregnation and in-situ decomposition of carbonyl nickel. The properties of catalysts were investigated by catalytic hydro-conversion of 2,2′-dinaphthyl ether as the model compound and extraction residue of Naomaohu lignite as the sample under an initial H2 pressure of 5 MPa and temperature at 150 °C. According to the catalytic hydro-conversion results of the model compound, Ni−Ru/HZSM-5 exhibited the best catalytic performance. It not only activated H2 into H···H, but also further heterolytically split H···H into immobile H‒ attached on the acidic centers of Ni−Ru/HZSM-5 and relatively mobile H+. Catalytic hydro-conversion of the extraction residue from Naomaohu lignite was further examined over the optimized catalyst, Ni−Ru/HZSM-5. Detailed molecular compositions of products from the extraction residue with and without hydrogenation were characterized by Fourier transform infrared spectroscopy and gas chromatography/mass spectrometry. The analytical results showed that the oxygen-containing functional groups in products of hydrogenated extraction residue were obviously reduced after the catalytic treatment. The relative content of oxygenates in the product with catalytic treatment was 18.57% lower than that in the product without catalytic treatment.

Keywords HZSM-5      Ni-based catalyst      catalytic hydrogenation      coal      model compound     
Corresponding Author(s): Feng-Yun Ma,Xing Fan   
About author:

Tongcan Cui and Yizhe Hou contributed equally to this work.
Online First Date: 23 June 2022    Issue Date: 17 October 2022
 Cite this article:   
Reyila Abuduwayiti,Feng-Yun Ma,Xing Fan. Catalytic hydrogenation of insoluble organic matter of CS2/Acetone from coal over mesoporous HZSM-5 supported Ni and Ru[J]. Front. Chem. Sci. Eng., 2022, 16(10): 1505-1513.
 URL:  
https://academic.hep.com.cn/fcse/EN/10.1007/s11705-022-2164-0
https://academic.hep.com.cn/fcse/EN/Y2022/V16/I10/1505
Proximate analysis Petro-graphical analysis Ultimate analysis (daf) H/C O/C
Mad Ad Vdaf FCdaf Vitrinite Inertinite Exinite R0max/% C H Odiff N St,d
10.36 9.45 52.46 47.54 66.7 2.9 29.4 0.29 74.65 5.96 17.77 1.27 0.35 0.96 0.18
Tab.1  The proximate, petro-graphical and ultimate analyses of Naomaohu lignite a)
Fig.1  XRD patterns of HZSM-5, Ni/HZSM-5, NTC/HZSM-5, Ni−Ru/HZSM-5 and NTC−Ru/HZSM-5. Ni (PDF#04-0850) and Ru (PDF#06-0663) are the standard XRD patterns of nickel and ruthenium.
Fig.2  SEM images and EDS of (a) HZSM-5, (b) Ni/HZSM-5, (c) NTC/HZSM-5, (d) Ni−Ru/HZSM-5 and (e) NTC−Ru/HZSM-5.
Sample SBET/(m2?g?1) Smicro/(m2?g?1) Smeso/(m2?g?1) Vtotal/(cm3?g?1) Vmicro/(cm3?g?1) Vmeso/(cm3?g?1)
HZSM-5 398 215 183 0.360 0.101 0.259
Ni/HZSM-5 365 193 172 0.332 0.086 0.246
NTC/HZSM-5 233 107 126 0.247 0.053 0.194
Ni−Ru/HZSM-5 379 195 184 0.349 0.095 0.254
NTC−Ru/HZSM-5 390 205 185 0.352 0.098 0.254
Tab.2  The textural parameters of support and catalysts
Fig.3  (a) N2 adsorption/desorption isotherms and (b) pore size distributions of HZSM-5, Ni/HZSM-5, NTC/HZSM-5, Ni−Ru/HZSM-5 and NTC−Ru/HZSM-5.
Fig.4  Curve fitting for the X-ray photoelectron spectra of (a–d) Ni 2p and (e–f) Ru 3d of Ni/HZSM-5, NTC/HZSM-5, Ni−Ru/HZSM-5 and NTC−Ru/HZSM-5.
Fig.5  NH3-TPD profiles of HZSM-5, Ni/HZSM-5, NTC/HZSM-5, Ni−Ru/HZSM-5 and NTC−Ru/HZSM-5.
No. Catalyst Conversion/% Selectivity/mol%
PAHs
1 Ni−Ru/HZSM-5 100 47.0 8.0 10.0 6.0 29.0
2 NTC−Ru/HZSM-5 100 18.8 0.6 2.5 0.9 77.2
3 Ni/HZSM-5 58.6 25.7 0.7 3.4 1.3 27.5
4 NTC/HZSM-5 100 18.7 1.3 2.9 1.7 75.4
Tab.3  The selectivity of products from the CHC of DNE over catalysts a)
FGs Range of wavenumber/cm?1 Region
?N–H and –OH tensile vibration 3200–3600 I
C–H stretching vibration in aromatic ring 3000–3100
C–H stretching vibration in aliphatic groups 3000–2800 II
Aliphatic C=O stretching vibration 1770–1730 III
Aromatic ring C=O stretching vibration 1721–1695
Aromatic ring C=C stretching vibration 1635–1547
C–H deformation vibration of aliphatic 1530–1410
C–O–C stretching vibration of phenol aldehydes 1310–1180
C–OH in phenols 1180–1100
Isolated hydrogen in aromatic rings 900–880 IV
Two adjacent aromatic ring hydrogen 850–810
Three adjacent aromatic ring hydrogen 780–760
Four adjacent aromatic ring hydrogen 750–730
Five adjacent aromatic ring hydrogen 710–680
Tab.4  Functional groups assignment of FTIR absorption peaks
Fig.6  FTIR spectra of RNCHC and RCHC.
Fig.7  Distribution of group components in RNCHC and RCHC.
  Scheme1 Possible reaction pathways for the CHC of residues over Ni−Ru/HZSM-5.
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