Bimetallic Ni-Fe catalysts derived from layered double hydroxides for CO methanation from syngas

doi:10.1007/s11705-017-1664-9

Front. Chem. Sci. Eng.

2017, Vol. 11

Issue (4) : 613-623 https://doi.org/10.1007/s11705-017-1664-9

RESEARCH ARTICLE

Bimetallic Ni-Fe catalysts derived from layered double hydroxides for CO methanation from syngas

Honggui Tang^1,², Shuangshuang Li^1,², Dandan Gong^1,², Yi Guan^1,², Yuan Liu^1,²(

)

¹. Department of Catalysis Science and Technology, School of Chemical Engineering, Tianjin University, Tianjin 300072, China
². Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), School of Chemical Engineering, Tianjin University, Tianjin 300072, China

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Abstract

Carbon deposition and sintering of active components such as nano particles are great challenges for Ni-based catalysts for CO methanation to generate synthetic natural gas from syngas. Facing the challenges, bimetallic catalysts with different Fe content derived from layered double hydroxide containing Ni, Fe, Mg, Al elements were prepared by co-precipitation method. Nanoparticles of Ni-Fe alloy were supported on mixed oxides of aluminium and magnesium after calcination and reduction. The catalysts were characterized by Brunner-Emmett-Teller (BET), X-ray diffraction, hydrogen temperature programmed reduction, inductively coupled plasma, X-ray photoelectron spectroscopy, transmission electron microscopy and thermogravimetric techniques, and their catalytic activity for CO methanation was investigated. The results show that the Ni-Fe alloy catalysts exhibit better catalytic performance than monometallic catalysts except for the Ni4Fe-red catalyst. The Ni2Fe-red catalyst shows the highest CO conversion (100% at 260–350 °C), as well as the highest CH₄ selectivity (over 95% at 280–350 °C), owing to the formation of Ni-Fe alloy. In stability test, the Ni2Fe-red catalyst exhibits great improvement in both anti-sintering and resistance to carbon formation compared with the Ni0Fe-red catalyst. The strong interaction between Ni and Fe element in alloy and surface distribution of Fe element not only inhibits the sintering of nanoparticles but restrains the formation of Ni clusters.

Keywords methanation layered double hydroxide bimetal Ni-Fe alloy sintering carbon deposition

Corresponding Author(s): Yuan Liu

Just Accepted Date: 19 June 2017 Online First Date: 14 September 2017 Issue Date: 06 November 2017

Cite this article:

Honggui Tang,Shuangshuang Li,Dandan Gong, et al. Bimetallic Ni-Fe catalysts derived from layered double hydroxides for CO methanation from syngas[J]. Front. Chem. Sci. Eng., 2017, 11(4): 613-623.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-017-1664-9
https://academic.hep.com.cn/fcse/EN/Y2017/V11/I4/613

Fig.1 XRD patterns of NixFeLDHs with x of (a) 0, (b) 1, (c) 2 and (d) 4

Tab.1 Cell parameters for the NixFeLHDs (x = 0, 1, 2, 4) precursors

Fig.2 Textural properties of the NixFe-CLDHs (a) N₂ adsorption-desorption isotherm, and (b) the pore size distribution

Fig.3 The XRD patterns of the NixFe-CLDHs with x of (a) 0, (b) 1, (c) 2 and (d) 4

Fig.4 H₂-TPR profiles of NixFe-CLDHs with x of (a) 0, (b) 1, (c) 2 and (d) 4

Tab.2 Physicochemical property of the NixFe-CLDHs (x= 0, 1, 2, 4) catalysts

Fig.5 The XRD patterns of the NixFe-red catalysts with x of (a) 0, (b) 1, (c) 2 and (d) 4

Tab.3 Physicochemical properties of NixFe-red catalysts after reduction and reaction

Fig.6 TEM images of the reduced catalysts with x of (a) 0, (b) 1, (c) 2 and (d) 4; STEM images and the corresponding EDS line scanning profiles for Ni and Fe elements of Ni2Fe-red catalyst of (e) and (f); (g), (h) and (i) EDX mapping of Ni and Fe

Fig.7 Ni 2p XPS spectra of the catalysts (a) Ni0Fe-red, (b) Ni2Fe-red, (c) Ni0Fe-used, and (d) Ni2Fe-used

Tab.4 XPS results for the reduced and used catalysts

Fig.8 Catalytic performance for CO methanation reaction over NixFe-red catalysts (x = 0, 1, 2, 4) at 30000 mL?g⁻¹?h⁻¹, 0.1 MPa and H₂/CO/N₂ = 3:1:1

Fig.9 The stability of (a) Ni0Fe-red and (b) Ni2Fe-red catalysts for CO methanation at 600 °C, 0.1 MPa, and 30000 mL?g⁻¹?h⁻¹

Fig.10 XRD patterns of (a) Ni0Fe-red and (b) Ni2Fe-red after stability test under the reaction conditions as listed in Fig. 9

Fig.11 TEM images of the catalysts after stability test (a) Ni0Fe-used and (b) Ni2Fe-used

Fig.12 TG profiles of the reduced and used catalysts after stability test in air

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