Transition metal-rich mesoporous silicas and their enhanced catalytic properties

Baowang Lu, Katsuya Kawamoto

Research output: Contribution to journalArticle

12 Citations (Scopus)

Abstract

A controllable and simple direct hydrothermal synthesis route was designed for synthesizing well-ordered mesoporous silica incorporating transition metals (M) (Ni, Cu, Zn, Co) with high metal loading. M-incorporated mesoporous silica could be obtained from a starting synthesis mixture with a Si/M mole ratio of 5 using transition metal-ammonia (NH3) complex ions [M(NH3)x]n+ as base. The Si/M mole ratio of 5 is the lowest value yet reported. XPS, UV-vis and H2-TPR analyses demonstrated that a chemical bond was formed between metal and silicon via oxygen and no bulk metal oxides existed in any of the M-MCM-41 samples; in other words, only tetrahedral coordinated metal species were detected. The formation of -O-M-O-Si-O- is completed via the reaction between hydrolyzate [M(OH)(NH3)x-1](n-1)+ from [M(NH3)x]n+ and ≡Si-OH (silanol sites) from a silica source (tetramethoxysilane (TMOS)). All the M-MCM-41 samples possessed remarkable physical properties and thermal stability. Ni-MCM-41, Cu-MCM-41 and CoMCM-41 catalysts exhibited excellent catalytic efficiency for carbon dioxide (CO2) hydrogenation, although Zn-MCM-41 catalyst did not. Ni-MCM-41 catalyst suited methanation, resulting in high CO2 conversion rate and methane selectivity, while Cu-MCM-41 catalyst favored the reverse water gas shift (RWGS) reaction and realized high CO2 conversion rate to carbon monoxide. A kinetic study was also carried out for methanation and RWGS reaction. Using Ni-MCM-41 catalyst for methanation, the rate equation could be expressed as r = kCCO2 0.68CH2 3.31, where C represents concentration. Using Cu-MCM-41 catalyst for RWGS reaction, the rate equation could be expressed as r = kCCO2 0.5CH2 1.1, where C represents concentration.

Original languageEnglish
Pages (from-to)4313-4321
Number of pages9
JournalCatalysis Science and Technology
Volume4
Issue number12
DOIs
Publication statusPublished - Dec 1 2014

Fingerprint

Multicarrier modulation
Silicon Dioxide
Transition metals
Silica
Methanation
Catalysts
Water gas shift
Metals
MCM-41
Catalyst selectivity
Chemical bonds
Hydrothermal synthesis
Methane
Silicon
Carbon Monoxide
Ammonia
Carbon Dioxide
Carbon monoxide
Oxides
Hydrogenation

ASJC Scopus subject areas

  • Catalysis

Cite this

Transition metal-rich mesoporous silicas and their enhanced catalytic properties. / Lu, Baowang; Kawamoto, Katsuya.

In: Catalysis Science and Technology, Vol. 4, No. 12, 01.12.2014, p. 4313-4321.

Research output: Contribution to journalArticle

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