Manipulating the reaction path of the CO2 hydrogenation reaction in molecular sieves

We demonstrate that the kinetics of the Sabatier reaction catalysed by sorption catalysts depends on the nanostructure of the catalyst–sorbent system. The catalysts are prepared by ion exchange of a nickel nitrate solution in two zeolites with different pore sizes. Besides their different pore sizes — which enables or hinders the adsorption of the reactants, intermediates and products in the inner of the crystallites — the catalyst systems have slightly different size distributions of the Ni-particles. By studying various catalysts with different Ni-contents we can attribute different catalytic activity and in particular the shape selectivity of the zeolite support. Therefore we focus on the microstructural characterization of the catalyst. We observe that the selectivity for methane is greatly enhanced if the pore size of the support is larger than 5 A, while pore sizes of less than 3 A reduce the overall conversion rate and the selectivity for methane. Thus, Ni on 3A zeolites can be used as low temperature catalysts for the reversed water-gas shift reaction to produce carbon monoxide.

[1]  Wim G. Haije,et al.  Sorption enhanced methanation for substitute natural gas production: Experimental results and thermodynamic considerations , 2014 .

[2]  S. Malčić,et al.  Ion-exchange equilibria of synthetic 4A zeolite with Ni2+, Co2+, Cd2+ and Zn2+ ions , 1971 .

[3]  S. T. Sie Past, Present and Future Role of Microporous Catalysts in the Petroleum Industry , 1994 .

[4]  J. Yates,et al.  IRAS study of the adsorption of CO on Ni(111): Interrelation between various bonding modes of chemisorbed CO , 1988 .

[5]  Guangwen Xu,et al.  Effect of nickel nanoparticle size in Ni/α-Al2O3 on CO methanation reaction for the production of synthetic natural gas , 2013 .

[6]  C. Louis,et al.  Sintering of Ni/SiO2 catalysts prepared by impregnation and deposition-precipitation during CO hydrogenation , 1997 .

[7]  R. V. Hardeveld,et al.  Influence of Metal Particle Size in Nickel-on-Aerosil Catalysts on Surface Site Distribution, Catalytic Activity, and Selectivity , 1972 .

[8]  Berend Smit,et al.  Towards a molecular understanding of shape selectivity , 2008, Nature.

[9]  H. Gesser,et al.  Pressure dependence of methane encapsulation in type 3A zeolites , 1984 .

[10]  M. D. Amiridis,et al.  Formation and Thermal Stability of Ni+ Cationic Sites in Ni−ZSM-5 , 2007 .

[11]  Jens K Nørskov,et al.  Modeling CO2 reduction on Pt(111). , 2013, Physical chemistry chemical physics : PCCP.

[12]  J. Nørskov,et al.  Towards the computational design of solid catalysts. , 2009, Nature chemistry.

[13]  T. Nenoff,et al.  Internal surface modification of MFI-type zeolite membranes for high selectivity and high flux for hydrogen. , 2009, Langmuir : the ACS journal of surfaces and colloids.

[14]  Andreas Züttel,et al.  Sorption enhanced CO2 methanation. , 2013, Physical chemistry chemical physics : PCCP.

[15]  V. Kazansky,et al.  First observation of the broad-range DRIFT spectra of carbon dioxide adsorbed on NaX zeolite , 1999 .

[16]  Jeffrey Raymond Hufton,et al.  Sorption-enhanced reaction process , 1996 .

[17]  E. Iglesia,et al.  The catalytic diversity of zeolites: confinement and solvation effects within voids of molecular dimensions. , 2013, Chemical communications.

[18]  Enrico Drioli,et al.  Energy and mass intensities in hydrogen upgrading by a membrane reactor , 2014 .

[19]  Guangwen Xu,et al.  A thermodynamic analysis of methanation reactions of carbon oxides for the production of synthetic natural gas , 2012 .

[20]  W. A. Jong,et al.  Kinetics of the methanation of CO and CO2 on a nickel catalyst , 1973 .

[21]  Junhang Dong,et al.  On-stream modification of MFI zeolite membranes for enhancing hydrogen separation at high temperature , 2008 .

[22]  Hans Geerlings,et al.  Efficient production of solar fuel using existing large scale production technologies. , 2011, Environmental science & technology.

[23]  John L. Falconer,et al.  Spillover in Heterogeneous Catalysis , 1995 .

[24]  G. Busca,et al.  Adsorption of CO on LTA zeolite adsorbents: An IR investigation , 2008 .

[25]  Eric G. Derouane,et al.  A novel effect of shape selectivity: Molecular traffic control in zeolite ZSM-5 , 1980 .

[26]  T. Degnan,et al.  The implications of the fundamentals of shape selectivity for the development of catalysts for the petroleum and petrochemical industries , 2003 .

[27]  N. Tsubaki,et al.  Core-shell catalysts and bimodal catalysts for Fischer-Tropsch synthesis , 2013 .