Electron distribution tuning of fluorine-doped carbon for ammonia electrosynthesis

文献情報

出版日 2019-06-25

DOI 10.1039/C9TA04141A

インパクトファクター 12.732

著者

Di Yuan, Zengxi Wei, Peng Han, Chao Yang, Linsong Huang, Zhengxiang Gu, Yu Ding, Jianmin Ma, Gengfeng Zheng

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要旨

The electrochemical N2 reduction reaction (N2RR), as a key reaction to realize the electrosynthesis of ammonia under ambient conditions, is significantly inhibited by the low efficiency of electrocatalysts. In this study, we report the improvement of the N2RR efficiency using a nonmetal, fluorine-doped carbon. The fluorine doping enables the tuning of the electron distribution of carbon, which provides positively charged carbon sites that are prone to adsorb N2 than H+ under acidic aqueous conditions. Density-functional theory calculations indicate that the N2 molecule is adsorbed on the two contrapuntal carbon atoms in the form of a side-on pattern, and the pathway of N2 turning to NH3 has the lowest energy barrier. The fluorine-doped carbon exhibits better N2RR performance than the undoped carbon, with a peak ammonia production rate (6.9 μg h−1 cm−2) and a corresponding high faradaic efficiency (12.1%) at −0.55 V versus the reversible hydrogen electrode (RHE). Our work shows the attractive features of developing doped carbon materials as nonmetal N2RR electrocatalysts.

掲載誌

Journal of Materials Chemistry A

CiteScore: 19.5

自己引用率: 4.7%

年間論文数: 2211

Journal of Materials Chemistry A, B & C cover high quality studies across all fields of materials chemistry. The journals focus on those theoretical or experimental studies that report new understanding, applications, properties and synthesis of materials. The journals have a strong history of publishing quality reports of interest to interdisciplinary communities and providing an efficient and rigorous service through peer review and publication. The journals are led by an international team of Editors-in-Chief and Associate Editors who are all active researchers in their fields. Journal of Materials Chemistry A, B & C are separated by the intended application of the material studied. Broadly, applications in energy and sustainability are of interest to Journal of Materials Chemistry A, applications in biology and medicine are of interest to Journal of Materials Chemistry B, and applications in optical, magnetic and electronic devices are of interest to Journal of Materials Chemistry C. More than one Journal of Materials Chemistry journal may be suitable for certain fields and researchers are encouraged to submit their paper to the journal that they feel best fits for their particular article. Example topic areas within the scope of Journal of Materials Chemistry A are listed below. This list is neither exhaustive nor exclusive. Artificial photosynthesis Batteries Carbon dioxide conversion Catalysis Fuel cells Gas capture/separation/storage Green/sustainable materials Hydrogen generation Hydrogen storage Photocatalysis Photovoltaics Self-cleaning materials Self-healing materials Sensors Supercapacitors Thermoelectrics Water splitting Water treatment

Electron distribution tuning of fluorine-doped carbon for ammonia electrosynthesis

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Journal of Materials Chemistry A

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