Graphene Supported Nickel Catalyst for Methanation of Carbon Dioxide†

doi:10.7503/cjcu20170348

Abstract

Abstract:

Graphene oxide(GO) was prepared from purified natural graphite via the modified Hummers method, and hydrazine hydrate reduced graphene oxide supported nickel catalysts were prepared via impregnation method. The influence of different supports of Ni-based catalysts for the carbon dioxide methanation reaction was investigated. Using reduced graphene oxide(RGO), carbon nanotubes(CNTs) and activated carbon(AC) as supports, nickel catalysts with different morphologies were formed. The prepared samples were characterized by FTIR, BET, H₂-TPR, XRD and TEM techniques and applied in carbon dioxide methanation. The results reveal that Ni/RGO has a relative large specific surface area(316 m²/g). The particle size of nickel on Ni/RGO(5.3 nm) is smaller than that on Ni/CNTs(8.9 nm) and Ni/AC(11.6 nm). Ni/RGO shows better catalytic activity and selectivity of carbon dioxide methanation reaction than that on Ni/CNTs and Ni/AC. Ni/RGO catalyst has a remarkable stability.

Key words: Graphene, Carbon nanotubes, Activated carbon, CO2 methanation, Ni catalyst

CLC Number:

O643.3

TrendMD:

ZHANG Rongbin, TONG Sai, YANG Jinmei, TANG Xiannong, HUANG Chuanqing, WANG Xuewen, FENG Gang, CAI Jianxin. Graphene Supported Nickel Catalyst for Methanation of Carbon Dioxide^†[J]. Chem. J. Chinese Universities, 2017, 38(12): 2255.

Figures/Tables 9

Fig.1 FTIR spectra of the supports a. GO; b. CNTs; c. AC; d. RGO.

Fig.2 N2 adsorption-desorption isotherms of the CNTs (A), RGO (B) and AC (C)

Table 1 Specific surface area, interlayer distance and NiO crystallite size of the samples

Sample	S_BET/(m²·g^-1)	2θ/(°)	Interlayer distance^a/nm	Crystallite size/nm
Sample	S_BET/(m²·g^-1)	2θ/(°)	Interlayer distance^a/nm	NiO^b	Ni^c
GO	60	11	0.81
RGO	463	24	0.37
Ni/RGO	316	24.9	0.35	4.1	5.3
CNTs	334	26
Ni/CNTs	149	26		4.0	8.9
AC	868.6	23.7
Ni/AC	739	24.8		6.1	11.6

Fig.3 XRD patterns of pure supports(A), fresh catalysts(B) and after reduction catalysts(C)

Fig.4 TEM images of RGO(A), Ni/RGO(B), Ni/CNTs(C) and Ni/AC(D), the SEM image of RGO(E) and the particle diameter distribution of Ni/RGO(F), Ni/CNTs(G) and Ni/AC(H)

Fig.5 H2-TPR profiles of Ni/AC(a), Ni/CNTs(b) and Ni/RGO(c)

Fig.6 Effects of reaction temperature on CO2 conversion(A), CH4 selectivity(B),CH4 yield(C) over Ni/AC(a), Ni/CNTs(b) and Ni/RGO(c)

Table 2 Comparison of catalytic performance of Ni/AC, Ni/CNTs and Ni/RGO in methanation reaction

Sample	$X C O 2$ (%)	Ni particle size^a/nm	TO $F C O 2 b$ /s^-1	Ni dispersion^c(%)
Ni/RGO	23.7	5.3	0.0659	18.9
Ni/CNTs	13.5	8.9	0.0630	11.2
Ni/AC	7.8	11.6	0.0474	8.6

Table 2 Comparison of catalytic performance of Ni/AC, Ni/CNTs and Ni/RGO in methanation reaction

Sample	$X C O 2$ (%)	Ni particle size^a/nm	TO $F C O 2 b$ /s^-1	Ni dispersion^c(%)
Ni/RGO	23.7	5.3	0.0659	18.9
Ni/CNTs	13.5	8.9	0.0630	11.2
Ni/AC	7.8	11.6	0.0474	8.6

Fig.7 Stable testing of Ni/AC(a), Ni/CNTs(b)and Ni/RGO(c)Reaction conditions: 50 mg catalyst, 400 ℃, 30 mL/min.

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