金属掺杂氮碳材料的调控及其在电催化还原CO_2中的应用
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摘要
氮碳材料被认为是能将CO_2转化生成CO和H_2合成气的有效催化剂,但是其过电位较大、选择性较低、以及活性位点不明确等因素限制它的进一步应用发展[1-3]。本文使用三聚氰胺作为氮源,蔗糖作为碳源,掺杂不同含量的氯化铁通过模板法制备出了金属掺杂的氮碳材料,表现出高活性和低的过电位,CO法拉第效率(FE)能够达到83.4%,而且在-0.9 V vs SCE时CO的FE就能够达到60%,CO的质量密度电流在-1.3 V高达7.5 Ag~(-1)超过了之前氮碳材料(≈7A g~(-1)[4]),同时通过铁盐含量的调控,观察到氮碳材料中的铁与CO的选择性无关,但是与生成CO催化活性成正相关。
Nitrogen-doped Carbon materials is known as an efficient electrocatalyst for the conversion of CO_2 to CO. However, the low selectivity and the high overpotential toward CO on nitrogenated carbon materials is still very limited. Herein, a novel N-doped metal catalyst was prepared via template method. Specifically, sucrose and melamine were served as carbon and nitrogen resouces, respectively, while different content of FeCl_3 was introduced during pyrolysis. The catalyst exhibits negligible overpotential(0.13 V) for CO_2 reduction when the FE come up to 60%, and the highest faradaic efficiency of CO could be 83.4%, and magnitude higher current density compared with the other nitrogenated carbon materials under similar experimental conditions.
引文
[1]Sharma,P.;Wu,J.;Yadav,R.;Liu,M.;et al.Angew.Chem.2015,127:3905.
    [2]Wu,J.;Liu,M.;Sharma,P.;Yadav,R.;et al.Nano Lett.2016,16:466.
    [3]Kumar,B.;Asadi,M.;Pisasale,D.;Sinha-Ray,S;et al.Nat.Commun.2013,4:1.
    [4]Varela,A.;Sahraie,N.;Steinberg,J.;Ju,W.;et al.Angew.Chem.int.Ed.2015,54:10758.

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