Journal
ACS CATALYSIS
Volume 6, Issue 6, Pages 3610-3618Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.6b00464
Keywords
pyrolysis; metal-organic frameworks; Fischer-Tropsch synthesis; iron oxide@iron carbide nanoparticles; core-shell; weak interaction
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Funding
- National Natural Science Foundation of P.R China [21471126, 21503174, 21433008, 91545203]
- National Thousand Talents Program of the P.R of China
- 985 Program of Chemistry and Chemical Engineering disciplines of Xiamen University
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We prepared highly active catalysts for Fischer Tropsch (FT) synthesis through the pyrolysis of iron-containing metal organic frameworks (MOFs). The Fe time yields of the nitrogen-doped catalyst were as high as 720 pmolco gFe(-1) s(-1) under the conditions of 300 degrees C, 2 MPa, and H-2/CO = 1, which is a value that surpasses that of most FT catalysts reported in the literature. The pyrolysis of the MOFs yielded nanoparticles with a unique iron oxide@iron carbide core shell structure dispersed on carbon supports. Such a structure is favorable for FT synthesis and has never been reported previously. Our strategy resolved the problem that the strong metal support interactions that are usually required to stabilize dispersed particles in calcination compromise the catalytic activity, because of the difficulty of reducing metal oxides. Moreover, we found full coverage of carbonates on the particle surfaces, which likely result from decarboxylation of the MOFs and further stabilize the particles before decomposing to CO2, leaving an active surface rich with dangling bonds for catalytic turnover.
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