Trace sulfur promoted Fe, N-codoped carbon black as electrocatalyst for oxygen reduction reaction
Trace sulfur promoted Fe, N-codoped carbon black as electrocatalyst for oxygen reduction reaction
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DOI：
10.1016/j.ijhydene.2018.12.082
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发表时间：
2019-02-05
影响因子：
7.2
通讯作者：
Li, Guozhu
中科院分区：
文献类型：
--
作者：
Guo, Mengya;Wang, Li;Li, Guozhu
掺杂铁和氮的碳材料在制备ORR电极中具有高性能和低成本的应用前景，受到了广泛的关注。本课题组此前以碳材料、多巴胺和FeCl3为原料，通过简单的一锅法合成了Fe， N共掺杂催化剂（Fe/N/C）。然而，活性不稳定和选择性低（电子转移数约为3.5）是需要解决的关键问题。本文采用2-巯基乙醇作为硫的粘结前驱体，将微量硫引入到Fe， n共掺杂炭黑中。在Fe， n共掺杂碳框架中掺入微量S原子（约0.25 at%），无需酸蚀或补氮等再处理，即可明显提高ORR性能。通过改变初始硫前驱体的量，系统地研究了这一过程的机理。适量的微量硫由于Fe、N、S和C元素之间的适当相互作用，可以有效地提高Fe、N共掺杂炭黑的ORR性能。微量硫可以改变和控制炭黑表面铁、氮的含量和状态。合成的1.0 S-Fe/N/C催化剂表现出良好的ORR活性(E-1/2 = 0.749 V， J（k) = 54.56 mA cm(-2)）和总4电子选择性。1.0 S-Fe/N/C也比20 wt% Pt/C表现出更好的催化稳定性和甲醇耐受性。(C) 2018氢能源出版有限责任公司，由爱思唯尔有限公司出版。版权所有。
Doping carbon materials with Fe and N attracts great attention due to its promising application in preparing ORR electrode with high performance and low cost. Previously, Fe, N-codoped catalyst (Fe/N/C) had been synthesized via a simple one-pot method using carbon materials, dopamine and FeCl3 by our group. However, the unstable activity and low selectivity (electron transfer number of similar to 3.5) are key problems that should be solved. Herein, trace sulfur has been introduced into Fe, N-codoped carbon black by using 2-mercaptoethanol as an adhesive sulfur precursor. By the doping of trace S atoms (similar to 0.25 at%) into Fe, N-codoped carbon frameworks, the ORR performance has been obviously improved simply without any re-treatment process, such as acid-etching or nitrogen supplement. The mechanism of this process has been systematically investigated by changing the amount of initial sulfur precursor. A moderate amount of trace sulfur can effectively enhance the ORR performance of Fe, N-codoped carbon black due to suitable interactions among Fe, N, S and C elements. Both the content and the state of Fe and N species on the surface of carbon black can be changed and controlled by trace sulfur. The as-synthesized 1.0 S-Fe/N/C catalyst exhibits a good ORR activity (E-1/2 = 0.749 V, J(k) = 54.56 mA cm(-2)) and a total 4-electron selectivity. 1.0 S-Fe/N/C also shows better catalytic stability and methanol tolerance than 20 wt% Pt/C. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.