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Facet-dependent catalytic activities of Pd/rGO: exploring dehydrogenation mechanism of dodecahydro-N-ethylcarbazole
Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2020-01-21 , DOI: 10.1016/j.apcatb.2020.118658
Bin Wang , You-Tao Chen , Tie-Yan Chang , Zhao Jiang , Zheng-Qing Huang , Si-Yao Wang , Chun-Ran Chang , Yu-Sheng Chen , Jin-Jia Wei , Sen Yang , Tao Fang

Facet structure plays an important role in many reactions. Generally, dehydrogenation reactions with only C-H bond cleavage are often considered as structure insensitive reactions and therefore, there is no report on facet effect in reactions of LOHC for now. Herein, we report a facile synthesis of Pd nanoparticles enclosed by {100}, {110} and {111} facets supported on reduced graphene oxide. Combined with catalyst characterization, dehydrogenation performance study and DFT calculations, we found that the conversion rate and selectivity were strongly correlated with the facet structure of Pd, and {100} facet exhibited superior activity. We also identified the rate-determining step in the dehydrogenation of tetrahydro-N-ethylcarbazole to N-ethylcarbazole on Pd {100} facet. This work provides a basis for research requiring template Pd catalysts on rGO and broaden design methods for LOHC catalysts.



中文翻译:

Pd / rGO的方面依赖性催化活性:探索十二氢-N-乙基咔唑的脱氢机理

小平面结构在许多反应中起着重要作用。通常,仅具有CH键断裂的脱氢反应通常被认为是对结构不敏感的反应,因此,目前尚无关于LOHC反应中的刻面效应的报道。本文中,我们报道了由还原的氧化石墨烯支撑的{100},{110}和{111}面所包围的Pd纳米粒子的简便合成。结合催化剂的表征,脱氢性能研究和DFT计算,我们发现转化率和选择性与Pd的小面结构密切相关,{100}小面表现出优异的活性。我们还确定了在Pd {100}面上四氢-N-乙基咔唑脱氢为N-乙基咔唑的速率确定步骤。

更新日期:2020-01-22
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