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Cobalt nanocrystals on carbon nanotubes in the Fischer-Tropsch synthesis: impact of support oxidation
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2020-01-30 , DOI: 10.1016/j.apcata.2020.117441
T.W. van Deelen , H. Yoshida , R. Oord , J. Zečević , B.M. Weckhuysen , K.P. de Jong

The effect of oxidation of a carbon nanotube (CNT) support on the structure and catalytic performance in the Fischer-Tropsch (FT) synthesis of pre-synthesized cobalt nanocrystals (NC) has been investigated. 6 nm CoO-NC were prepared using colloidal techniques and impregnated on pristine and surface-oxidized CNT. The CoO-NC on pristine CNT were reduced completely to Co, while ∼50 % CoO reduction was observed on oxidized CNT (oxCNT), indicating a stronger Co-support interaction on oxCNT. In FT, the turnover frequency (TOF) after 100 h was exceptionally high on pristine CNT (150·10-3 s-1) against 63·10-3 s-1 on oxCNT. In the initial stage of FT, the TOF was 35 % lower on oxCNT than on pristine CNT, which matched with 32 % lower crystallinity of cobalt determined using in situ XRD. Furthermore, deactivation was observed mainly on oxCNT. These results demonstrate the large impact of the support on the structure and performance of nanocrystal-based catalysts.



中文翻译:

费-托合成中碳纳米管上的钴纳米晶体:载体氧化的影响

研究了碳纳米管(CNT)载体的氧化对费-托(FT)合成预合成钴纳米晶体(NC)的结构和催化性能的影响。使用胶体技术制备了6 nm CoO-NC,并浸渍在原始的和表面氧化的CNT上。原始CNT上的CoO-NC完全还原为Co,而在氧化的CNT(oxCNT)上观察到〜50%CoO还原,表明oxCNT上的Co-载体相互作用更强。在FT中,原始CNT(150·10 -3 s -1)相对于63·10 -3 s -1在100 h后的转换频率(TOF)异常高。在oxCNT上。在FT的初始阶段,oxCNT的TOF比原始CNT的TOF低35%,这与使用原位XRD测定的钴的结晶度低32%相匹配。此外,主要在oxCNT上观察到失活。这些结果证明了载体对纳米晶体基催化剂的结构和性能的巨大影响。

更新日期:2020-01-31
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