Research Progress of Ni-based Composite Catalysts for Methane Dry Reforming

doi:10.15541/jim20170585

Abstract

Abstract:

Methane Dry Reforming (DRM) catalysis converts the two greenhouse gases, CO₂ and CH₄ into syngas, which can be further utilized for liquid fuels production through Fischer-Tropsch synthesis. The DRM reaction is therefore of significance for both energy and environments. The key issue to promote industrialization of DRM reaction is to develop suitable catalysts. Nickel based composite catalysts have received extensive attention due to their outstanding catalytic activities comparable to those of precious metals and their bargain price. However, nickel based catalysts usually undergo severe deactivation due to the coke deposition and metal sintering during long-term reaction at high temperature, which seriously limit their industrial applications and development of the engineering of DRM. Many researches have been carried out to address this issue. In this review, the recent research progress in the activity, coke resistance, and sintering resistance of Ni-based composite catalysts are introduced from the aspect of catalyst components, structures, preparation methods, and simulations. The research trends of DRM catalysts are also predicted based on the recent research progress in single-atomic catalysis and the in-situ characterization techniques for catalysis.

Key words: methane dry reforming, Ni-based catalyst, coke resistance, metal sintering, research progress

CLC Number:

O643

ZHANG Peng, ZHANG Qing, LIU Jing, GAO Lian. Research Progress of Ni-based Composite Catalysts for Methane Dry Reforming[J]. Journal of Inorganic Materials, 2018, 33(9): 931-941.

Figures/Tables 12

Table 1 Main chemical reactions during methane dry reforming process[12,13]

Reaction	Reaction equation	△G	ΔH₂₉₈/(kJ·mol^-1)	Limit temperature/K
DRM	CH₄+CO₂→2H₂+2CO	61770-67.32T	247.3	913
RWGS	CO₂+H₂→CO+H₂O	-8545+7.84T	41.0	1093
Boudouard reaction	2CO→CO₂+C	-39810+40.87T	-171.0	973
Methane cracking	CH₄→C+2H₂	2190-26.45T	75.0	830

Fig. 1 Equilibrium constants of reactions as a function of tem- perature during DRM[14]

Fig. 2 Temperature programmed reduction (TPR) curves of NiO-γ-Al2O3 calcined at different temperatures for different durations[21]

Fig. 3 Methane conversion of the methane dry reforming catalysis on the hierarchical Cu-Ni/SiO2 catalysts with various Cu/Ni ratios and the control sample IM Ni/SiO2 at different temperatures[22]

Fig. 4 CO2-TPD profiles of the M-5NixCa(95-x)Al materials calcined at 600℃ with different Ca contents[36] (a) M-5Ni95Al; (b) M-5Ni1Ca94Al; (c) M-5Ni2Ca93Al; (d) M-5Ni3Ca92Al; (e) M-5Ni5Ca90Al; (f) M-5Ni8Ca87Al; (g) M-5Ni10Ca85Al

Fig. 5 Dry reforming performance and coke formed of different catalysts[55]

Fig. 6 TEM images of CuNi@SiO2 core-shell catalysts prepared in the typical synthesis route, a single silica shell contains one core particle[61]

Fig.7 Silica-coated catalysts with high coke resistance for DRM reaction[29]

Fig. 8 SEM images of the HT-NiMgAl (a) before calcination and (b) after reduction[62]

Fig. 9 Schematically representatives of electrode configurations of discharge phenomena applied for catalyst preparation[65](a) Glow discharge; (b) Microwave plasma; (c) Plasma spraying

Fig. 10 TEM images of Ni/SiO2 catalyst samples prepared by two methods (a, b) the conventional catalyst and (c, d) the novel catalyst prepared by plasma jet[69]

Fig. 11 Deactivation scheme to show schematically the phase transformation and coke formation[71]Ni(111) and Ni(211) stand for the clean nickel metal flat and stepped surfaces respectively, and Ni3C(001) and Ni3C(111) are the flat and stepped nickel carbide. Flat surfaces are marked in blue, while stepped surfaces are in red. Toxic coke is the more stable and high toxicity carbon atom which will result in the deactivation of the nickel catalyst. The corresponding overall reaction rates are marked below the different structures. The arrow with X means this step is not likely to occur, while arrow without X means this step could happen

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