Carbon Dioxide Hydrogenation over a Metal-Free Carbon-Based Catalyst,ACS Catalysis

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Carbon Dioxide Hydrogenation over a Metal-Free Carbon-Based Catalyst
ACS Catalysis ( IF 11.3 ) Pub Date : 2017-06-02 00:00:00 , DOI: 10.1021/acscatal.7b00729
Jingjie Wu ₁ , Cun Wen ₂ , Xiaolong Zou ₃ , Juan Jimenez ₂ , Jing Sun ₄ , Yujian Xia ₅ , Marco-Tulio Fonseca Rodrigues ₁ , Soumya Vinod ₁ , Jun Zhong ₅ , Nitin Chopra ₆ , Ihab N. Odeh ₆ , Guqiao Ding ₄ , Jochen Lauterbach ₂ , Pulickel M. Ajayan ₁

Affiliation

The hydrogenation of CO₂ into useful chemicals provides an industrial-scale pathway for CO₂ recycling. The lack of effective thermochemical catalysts currently precludes this process, since it is challenging to identify structures that can simultaneously exhibit high activity and selectivity for this reaction. Here, we report, for the first time, the use of nitrogen-doped graphene quantum dots (NGQDs) as metal-free catalysts for CO₂ hydrogenation. The nitrogen dopants, located at the edge sites, play a key role in inducing thermocatalytic activity in carbon nanostructures. Furthermore, the thermocatalytic activity and selectivity of NGQDs are governed by the doped N configurations and their corresponding defect density. The increase of pydinic N concentration at the edge site of NGQDs leads to lower initial reaction temperature for CO₂ reduction and also higher CO₂ conversion and selectivity toward CH₄ over CO.

中文翻译：

无金属碳基催化剂上的二氧化碳加氢

CO ₂氢化成有用的化学物质为CO _2的回收提供了工业规模的途径。当前缺乏有效的热化学催化剂阻止了该过程，因为鉴定对于该反应可以同时表现出高活性和选择性的结构是具有挑战性的。在这里，我们首次报道了氮掺杂石墨烯量子点（NGQDs）作为无金属的CO ₂催化剂的用途。氢化。位于边缘位置的氮掺杂剂在诱导碳纳米结构中的热催化活性中起关键作用。此外，NGQD的热催化活性和选择性受掺杂的N构型及其相应的缺陷密度控制。NGQDs边缘位置的吡啶氮浓度增加，会导致降低CO ₂还原反应的初始反应温度，并导致较高的CO ₂转化率和相对于CO的CH ₄选择性。

更新日期：2017-06-28

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