Synthesis of hollow nanocubes and macroporous monoliths of silicalite-1 by alkaline treatment

Chengyi Dai, Anfeng Zhang, Lingling Li, Keke Hou, Fanshu Ding, Jie Li, Dengyou Mu, Chunshan Song, Min Liu, Xinwen Guo

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Abstract

A simple strategy involving desilication and recrystallization of silicalite-1 in tetrapropylammonium hydroxide (TPAOH) solution was successfully developed to prepare hollow zeolite nanocubes and three-dimensionally macroporous zeolite monoliths. Large voids were introduced to silicalite-1 crystals by controlled silicon leaching with OH- and thin intact shells were formed by the recrystallization of silicon with TPA+. The size of nanocubes could be easily controlled from ∼150 nm to ∼600 nm by simply adjusting the size of parent silicalite-1. Apart from template function to increase the yield of hollow silicalite-1, TPA+ adsorbed on the zeolite protects the parent crystal surface where the recrystallization occurred. The size of the mesopores and/or macropores in the hollow zeolite shell can be controlled by varying the amount of competitive Na+ adsorbent added to the TPAOH solution. Furthermore, three-dimensional macroporous zeolite monoliths can be formed when an electrolyte, such as NaCl, was added to the TPAOH solution. When the sample was used as the support for iron-based catalyst for hydrogenation of CO2 to hydrocarbons, both the conversion of CO2 and the selectivity of C5 + higher hydrocarbons were improved.

Original languageEnglish (US)
Pages (from-to)4197-4205
Number of pages9
JournalChemistry of Materials
Volume25
Issue number21
DOIs
StatePublished - Nov 12 2013

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All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Chemical Engineering(all)
  • Materials Chemistry

Cite this

Dai, C., Zhang, A., Li, L., Hou, K., Ding, F., Li, J., Mu, D., Song, C., Liu, M., & Guo, X. (2013). Synthesis of hollow nanocubes and macroporous monoliths of silicalite-1 by alkaline treatment. Chemistry of Materials, 25(21), 4197-4205. https://doi.org/10.1021/cm401739e