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Dynamic Phase Transition of Iron Oxycarbide Facilitated by Pt Nanoparticles for Promoting the Reverse Water Gas Shift Reaction
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-11-18 , DOI: 10.1021/acscatal.1c03772 Hanming Chen 1 , Zhiying Zhao 1 , Genyuan Wang 1 , Zhiping Zheng 1 , Jiayu Chen 1 , Qin Kuang 1 , Zhaoxiong Xie 1, 2
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-11-18 , DOI: 10.1021/acscatal.1c03772 Hanming Chen 1 , Zhiying Zhao 1 , Genyuan Wang 1 , Zhiping Zheng 1 , Jiayu Chen 1 , Qin Kuang 1 , Zhaoxiong Xie 1, 2
Affiliation
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The catalytic activation of CO2 is a crucial process in CO2 recycling for both fundamental research and industrial applications. Fe-based catalysts have been demonstrated to be highly active for the reverse water gas shift (RWGS) reaction. However, the structural complexity and dynamic reduction/oxidation/carburization of iron-based catalysts mean that it is challenging to understand the mechanism of these catalysts and further improve their reaction activity. Herein, we report a highly efficient Pt/Fe3O4 catalyst for the RWGS reaction, in which the content of Pt is only 0.017 wt %. The CO2 conversion rate reaches 46.9 × 10–5 molCO2/(gcat s) with a CO selectivity of up to 99.7% at reaction conditions of 500 °C and atmospheric pressure. Structure–performance investigations reveal that the reduction process of Fe-based supports can be enhanced by the in situ formation of Pt nanoparticles, which significantly promote the dynamic phase transition of Fe3O4 to Fe3C via carburization and thus considerably improve CO2 activation. The synergistic interaction of Pt with Fe-oxycarbide improves catalytic activity and ensures long-term catalytic stability. This simple strategy by improving the reduction process of Fe-based catalysts to promote carburization provides an alternative way to manipulate the activity and selectivity of Fe-based catalysts in CO2 hydrogenation.
中文翻译：
铂纳米粒子促进碳氧化铁的动态相变促进反向水煤气变换反应
对于基础研究和工业应用，CO 2的催化活化是 CO 2回收的关键过程。铁基催化剂已被证明对逆水煤气变换 (RWGS) 反应具有高活性。然而，铁基催化剂的结构复杂性和动态还原/氧化/渗碳意味着理解这些催化剂的机理并进一步提高它们的反应活性具有挑战性。在此，我们报道了一种用于 RWGS 反应的高效 Pt/Fe 3 O 4催化剂，其中 Pt 的含量仅为 0.017 wt%。CO 2转化率达到 46.9 × 10 –5 mol CO 2 /(gcat s) 在 500 °C 和大气压的反应条件下具有高达 99.7% 的 CO 选择性。结构-性能研究表明，原位形成 Pt 纳米粒子可以增强 Fe 基载体的还原过程，这显着促进了 Fe 3 O 4通过渗碳向 Fe 3 C的动态相变，从而显着改善了 CO 2激活。Pt 与 Fe-碳氧化物的协同相互作用提高了催化活性并确保了长期的催化稳定性。这种通过改进铁基催化剂的还原过程来促进渗碳的简单策略提供了一种替代方法来控制铁基催化剂在 CO 2加氢中的活性和选择性。
更新日期：2021-12-03
中文翻译：
铂纳米粒子促进碳氧化铁的动态相变促进反向水煤气变换反应
对于基础研究和工业应用，CO 2的催化活化是 CO 2回收的关键过程。铁基催化剂已被证明对逆水煤气变换 (RWGS) 反应具有高活性。然而，铁基催化剂的结构复杂性和动态还原/氧化/渗碳意味着理解这些催化剂的机理并进一步提高它们的反应活性具有挑战性。在此，我们报道了一种用于 RWGS 反应的高效 Pt/Fe 3 O 4催化剂，其中 Pt 的含量仅为 0.017 wt%。CO 2转化率达到 46.9 × 10 –5 mol CO 2 /(gcat s) 在 500 °C 和大气压的反应条件下具有高达 99.7% 的 CO 选择性。结构-性能研究表明，原位形成 Pt 纳米粒子可以增强 Fe 基载体的还原过程，这显着促进了 Fe 3 O 4通过渗碳向 Fe 3 C的动态相变，从而显着改善了 CO 2激活。Pt 与 Fe-碳氧化物的协同相互作用提高了催化活性并确保了长期的催化稳定性。这种通过改进铁基催化剂的还原过程来促进渗碳的简单策略提供了一种替代方法来控制铁基催化剂在 CO 2加氢中的活性和选择性。
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