Pyrolysis of Metal–Organic Frameworks to Fe3O4@Fe5C2 Core–Shell Nanoparticles for Fischer–Tropsch Synthesis

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• 作者：Bing An ; Kang Cheng ; Cheng Wang ; Ye Wang ; Wenbin Lin
• 刊名：ACS Catalysis
• 出版年：2016
• 出版时间：June 3, 2016
• 年：2016
• 卷：6
• 期：6
• 页码：3610-3618
• 全文大小：653K
• 年卷期：0
• ISSN：2155-5435

文摘

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 μmol_CO g_Fe^–1 s^–1 under the conditions of 300 °C, 2 MPa, and H₂/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.