Zhang Yaru, Yang Xiaoli, Yang Xiaofeng, Duan Hongmin, Qi Haifeng, Su Yang, Liang Binglian, Tao Huabing, Liu Bin, Chen De, Su Xiong, Huang Yanqiang, Zhang Tao
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.
University of Chinese Academy of Sciences, Beijing, 100049, China.
Nat Commun. 2020 Jun 24;11(1):3185. doi: 10.1038/s41467-020-17044-4.
The activity of Fischer-Tropsch synthesis (FTS) on metal-based nanocatalysts can be greatly promoted by the support of reducible oxides, while the role of support remains elusive. Herein, by varying the reduction condition to regulate the TiO overlayer on Ru nanocatalysts, the reactivity of Ru/TiO nanocatalysts can be differentially modulated. The activity in FTS shows a volcano-like trend with increasing reduction temperature from 200 to 600 °C. Such a variation of activity is characterized to be related to the activation of CO on the TiO overlayer at Ru/TiO interfaces. Further theoretical calculations suggest that the formation of reduced TiO occurs facilely on the Ru surface, and it involves in the catalytic mechanism of FTS to facilitate the CO bond cleavage kinetically. This study provides a deep insight on the mechanism of TiO overlayer in FTS, and offers an effective approach to tuning catalytic reactivity of metal nanocatalysts on reducible oxides.
费托合成（FTS）在金属基纳米催化剂上的活性可通过可还原氧化物载体得到极大促进，然而载体的作用仍不明确。在此，通过改变还原条件来调控Ru纳米催化剂上的TiO覆盖层，Ru/TiO纳米催化剂的反应活性可得到不同程度的调节。费托合成中的活性随还原温度从200℃升高到600℃呈现出类似火山的趋势。这种活性变化的特征是与Ru/TiO界面处TiO覆盖层上CO的活化有关。进一步的理论计算表明，还原态TiO在Ru表面容易形成，并且它参与费托合成的催化机制，从动力学上促进CO键的断裂。本研究深入洞察了费托合成中TiO覆盖层的机制，并提供了一种有效方法来调节金属纳米催化剂在可还原氧化物上的催化反应活性。
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