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氮物种对氮掺杂石墨烯催化性能的影响。

The effect of nitrogen species on the catalytic properties of N-doped graphene.

作者信息

Skorupska Malgorzata, Ilnicka Anna, Lukaszewicz Jerzy P

机构信息

Faculty of Chemistry, Nicolaus Copernicus University in Torun, Gagarina 7, 87-100, Toruń, Poland.

Centre for Modern Interdisciplinary Technologies, Nicolaus Copernicus University in Torun, Wilenska 4, 87-100, Toruń, Poland.

出版信息

Sci Rep. 2021 Dec 14;11(1):23970. doi: 10.1038/s41598-021-03403-8.

DOI:10.1038/s41598-021-03403-8
PMID:34907258
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC8671485/
Abstract

The production of effective catalysts in the oxygen reduction reaction (ORR) continues to be a great challenge for scientists. A constant increase in demand for energy storage materials is followed by a proportionate increase in the number of reports on electrocatalyst synthesis. The scientific world focuses on environmentally friendly materials synthesized in accordance with the safest possible. In this work, we developed a facile method of obtaining heavy-metal-free electrode materials that are effective in ORR. Graphene-based catalysts were doped using azodicarbonamide (ADC) as the source of nitrogen, then carbonized at high temperatures in the range of 700-900 °C under inert gas flow. The produced materials were tested as catalysts for ORR, which is the most important reaction for Zn-air batteries and fuel cells. All obtained nitrogen-doped graphene foams showed increased catalytic activity in ORR owing to active sites created by nitrogen functional groups on the graphene surface. This paper shows that carbonization temperature has a significant impact on nitrogen content and that a small percentage of nitrogen may have a positive effect on the catalytic activity of the obtained materials. The number of transferred electrons in ORR was found to range from three to the maximal theoretical value, i.e., four.

摘要

对于科学家而言,在氧还原反应(ORR)中制备高效催化剂仍然是一项巨大挑战。随着对储能材料需求的持续增长,关于电催化剂合成的报道数量也相应增加。科学界关注按照尽可能安全的方式合成的环境友好型材料。在这项工作中,我们开发了一种简便的方法来制备在ORR中有效的无重金属电极材料。以偶氮二甲酰胺(ADC)作为氮源对基于石墨烯的催化剂进行掺杂,然后在惰性气流下于700 - 900°C的高温范围内进行碳化。所制备的材料作为ORR的催化剂进行了测试,ORR是锌空气电池和燃料电池中最重要的反应。所有获得的氮掺杂石墨烯泡沫由于石墨烯表面氮官能团产生的活性位点而在ORR中表现出增强的催化活性。本文表明碳化温度对氮含量有显著影响,并且少量的氮可能对所制备材料的催化活性产生积极作用。发现ORR中转移电子数范围为3至最大理论值,即4。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ff76/8671485/dfffdac0b37d/41598_2021_3403_Fig9_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ff76/8671485/a07fdd3e954a/41598_2021_3403_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ff76/8671485/67f904c24281/41598_2021_3403_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ff76/8671485/54c5d6794393/41598_2021_3403_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ff76/8671485/f644ace68d01/41598_2021_3403_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ff76/8671485/e072a580c707/41598_2021_3403_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ff76/8671485/1a53ddf3fd5d/41598_2021_3403_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ff76/8671485/843365c8995d/41598_2021_3403_Fig7_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ff76/8671485/a9546a7880d6/41598_2021_3403_Fig8_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ff76/8671485/dfffdac0b37d/41598_2021_3403_Fig9_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ff76/8671485/a07fdd3e954a/41598_2021_3403_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ff76/8671485/67f904c24281/41598_2021_3403_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ff76/8671485/54c5d6794393/41598_2021_3403_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ff76/8671485/f644ace68d01/41598_2021_3403_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ff76/8671485/e072a580c707/41598_2021_3403_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ff76/8671485/1a53ddf3fd5d/41598_2021_3403_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ff76/8671485/843365c8995d/41598_2021_3403_Fig7_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ff76/8671485/a9546a7880d6/41598_2021_3403_Fig8_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ff76/8671485/dfffdac0b37d/41598_2021_3403_Fig9_HTML.jpg

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