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Material Sciences 2022
二维ZIF8衍生的Fe-N-C纳米片的制备及其氧还原催化性能研究
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Abstract:
开发先进的氧还原反应(ORR)电催化剂是提升燃料电池、金属空气电池器件效率的关键，对可再生清洁能源的存储与转换利用具有重要意义。本文首先通过无机盐氯化钾辅助热解制备了二维氮掺杂碳(2D-NC)纳米片，再利用浸渍和两步退火的方法将铁掺杂到2D-NC基质中，得到二维Fe-N-C (2D-Fe-N-C)纳米片，相对于已被广泛报道的三维Fe-N-C，二维Fe-N-C纳米片将更多的活性位点暴露在表面，有利于提升催化活性。结果表明，通过加入氯化钾，2D-NC在较低温度(700℃)下即可碳化，且通过浸渍和两步低温退火实现铁掺杂，避免了铁物种的团聚。通过优化无机盐的用量，得到2D-Fe-N-C-5催化剂在碱性溶液中具有比较优异的催化活性，相对可逆氢电极，起始电位达0.999 V，半波电位为0.808 V，其氧还原反应的动力学电流密度与商业Pt/C相当，本文的研究工作对金属–氮–碳催化剂的制备具有一定参考意义。
The development of advanced electrocatalysts for oxygen reduction reaction (ORR) is the key to improve the efficiency of fuel cells and metal-air cells, and is of great significance for the storage, conversion and utilization of renewable clean energy. In this paper, two-dimensional nitrogen-doped carbon nanosheets (2D-NC) were prepared by inorganic salt KCl assisted pyrolysis, and then iron was doped into the 2D-NC matrix by immersion and two-step annealing to obtain two-dimensional Fe-N-C nanosheets (2D-Fe-N-C). Compared with the widely reported three-dimensional Fe-N-C, two- dimensional Fe-N-C nanosheets expose more active sites on the surface, which is conducive to improving catalytic activity. The results show that 2D-NC can be carbonized at a lower temperature (700℃) by adding KCl, and iron doping can be achieved by immersion and two-step low temperature annealing, avoiding the agglomeration of iron species. By optimizing the amount of inorganic salts, 2D-Fe-N-C-5 catalyst has excellent catalytic activity in alkaline solution. The onset potential is 0.999 V (vs RHE), and the half-wave potential is 0.808 V (vs RHE). The kinetic current density of its oxygen reduction reaction is equivalent to that of commercial Pt/C. The research work in this paper has certain reference significance for the preparation of metal nitrogen carbon catalysts.
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