Conversion of dimethyl ether to light olefins on Rh-Mg/HZSM-5: role of Rh as a modifier

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Abstract

The influence of the second modifying metal (Rh) on the acid and catalytic properties of Mg/HZSM-5 in conversion of dimethyl ether to light olefins and the state of active components (Mg, Rh) on the zeolite surface are studied. It is shown that when it is introduced into Mg/HZSM-5, rhodium significantly increases stability of the catalyst operation while maintaining the selectivity for light olefins at the level of 75 wt. %. It is found that various oxocationic or oxide forms of magnesium are formed on the zeolite surface in the monometallic sample of Mg/HZSM-5, and introduction of rhodium contributes to stabilization of magnesium mainly in the form of Mg2+ cations while the strength of Lewis acid properties of magnesium cations decreases, which all together makes catalyst deactivation slow down.

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About the authors

T. I. Batova

A. V. Topchiev Institute of Petrochemical Synthesis, Russian Academy of Sciences

Author for correspondence.
Email: batova.ti@ips.ac.ru
Russian Federation, Moscow

T. K. Obukhova

A. V. Topchiev Institute of Petrochemical Synthesis, Russian Academy of Sciences

Email: batova.ti@ips.ac.ru
Russian Federation, Moscow

N. V. Kolesnichenko

A. V. Topchiev Institute of Petrochemical Synthesis, Russian Academy of Sciences

Email: batova.ti@ips.ac.ru
Russian Federation, Moscow

M. I. Shilina

M. V. Lomonosov Moscow State University

Email: batova.ti@ips.ac.ru
Russian Federation, Moscow

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Supplementary files

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2. Fig. 1. Effect of modifying Mg/HZ with rhodium on the stability of the catalyst (a) and the yield of target products in 4 h (b) in the conversion of DME to lower olefins; α is the conversion, C is the yield of lower olefins.

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3. Fig. 2. Temperature-programmed desorption curves of ammonia for Rh/HZ, Mg/HZ and Rh-Mg/HZ; v is the rate of ammonia desorption.

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4. Fig. 3. XANES (a) and EXAFS (b) spectra at the K-edge of Rh catalysts Rh/HZ and Rh-Mg/HZ.

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5. Fig. 4. IRDO spectra of adsorbed CO on Mg/HZ (a) and Rh-Mg/HZ (b) at equilibrium pressures of 5 (1), 10 Torr (2) and after evacuation to 0.05 Torr (3), k is the wave number.

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6. Fig. 5. Difference IRDO spectra of CO adsorbed on Mg/HZ and Rh-Mg/HZ at pressures of 5 (a) and 0.05 Torr (b). The spectra* were obtained by subtracting the spectra of the initial HZ zeolite from the spectra of these samples (Fig. 4, curves 1 and 3).

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