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Incorporating nitrogen atoms into cobalt nanosheets as a strategy to boost catalytic activity toward CO 2 hydrogenation
Nature Energy ( IF 56.7 ) Pub Date : 2017-10-09 , DOI: 10.1038/s41560-017-0015-x
Liangbing Wang , Wenbo Zhang , Xusheng Zheng , Yizhen Chen , Wenlong Wu , Jianxiang Qiu , Xiangchen Zhao , Xiao Zhao , Yizhou Dai , Jie Zeng

Hydrogenation of CO2 into fuels and useful chemicals could help to reduce reliance on fossil fuels. Although great progress has been made over the past decades to improve the activity of catalysts for CO2 hydrogenation, more efficient catalysts, especially those based on non-noble metals, are desired. Here we incorporate N atoms into Co nanosheets to boost the catalytic activity toward CO2 hydrogenation. For the hydrogenation of CO2, Co4N nanosheets exhibited a turnover frequency of 25.6 h−1 in a slurry reactor under 32 bar pressure at 150 °C, which was 64 times that of Co nanosheets. The activation energy for Co4N nanosheets was 43.3 kJ mol−1, less than half of that for Co nanosheets. Mechanistic studies revealed that Co4N nanosheets were reconstructed into Co4NH x , wherein the amido-hydrogen atoms directly interacted with the CO2 to form HCOO* intermediates. In addition, the adsorbed H2O* activated amido-hydrogen atoms via the interaction of hydrogen bonds.



中文翻译:

将氮原子掺入钴纳米片中作为提高对CO 2加氢的催化活性的策略

将CO 2加氢为燃料和有用的化学物质可以帮助减少对化石燃料的依赖。尽管在过去的几十年中已经在改善用于CO 2加氢的催化剂的活性方面取得了很大的进步,但是仍需要更有效的催化剂,尤其是那些基于非贵金属的催化剂。在这里,我们将N原子结合到Co纳米片中,以增强对CO 2氢化的催化活性。对于CO 2的氢化,在淤浆反应器中在150℃的32巴压力下,Co 4 N纳米片表现出25.6h -1的周转频率,这是Co纳米片的64倍。Co 4 N纳米片的活化能为43.3 kJ mol -1,不到钴纳米片的一半。机理研究表明,Co 4 N纳米片被重建为Co 4 NH x,其中酰胺氢原子直接与CO 2相互作用形成HCOO *中间体。此外,被吸附的H 2 O *通过氢键的相互作用活化了酰胺氢原子。

更新日期:2017-10-11
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