Effect of Heteroatoms in Ordered Microporous Carbons on Their Electrochemical Capacitance
Effect of Heteroatoms in Ordered Microporous Carbons on Their Electrochemical Capacitance
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DOI：
10.1021/acs.langmuir.6b02667
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发表时间：
2016-11-22
期刊：
影响因子：
3.9
通讯作者：
Kyotani, Takashi
中科院分区：
文献类型：
--
作者：
Itoi, Hiroyuki;Nishihara, Hirotomo;Kyotani, Takashi
微孔比中孔和大孔在提高电化学电容方面起着更重要的作用，因此，杂原子掺杂到微孔中对电化学行为的影响是有趣的。然而，杂原子掺杂到多孔碳材料中会潜在地改变其孔结构和孔径，这也影响其电化学电容行为。为了深入了解杂原子对电化学电容行为的内在影响，沸石模板碳（ZTC）可能是最合适的候选者。ZTC是一种有序的微孔碳，具有1.2 nm的均匀粒径，高表面积和大的微孔体积。在这项工作中，一系列的ZTC含有氧，氮，或硼作为杂原子，具有有序的孔结构和相同的孔径，制备。通过研究它们在有机电解质中的电化学电容行为，可以分离和讨论杂原子掺杂的影响，而不考虑孔结构和孔径的影响。发现酸酐基团在两个电位范围内产生赝电容，-1.0至-0.3 V（vs Ag/AgClO 4）和-0.2至0.4 V。B仅作为-B（OH）（2）引入ZTC骨架中，发现其是电化学惰性物质。N以吡啶（3.0%）、吡啶酮/吡咯（23.8%）、季铵（66.6%）和氧化N（6.6%）的形式引入，并且这些物质在微孔碳中表现出明显的赝电容。
Micropores play a more important role in enhancing the electrochemical capacitance than mesopores and macropores; therefore, the effect of heteroatom doping into micropores on the electrochemical behavior is interesting. However, heteroatom doping into porous carbon materials would potentially change their pore structures and pore sizes, which also affect their electrochemical capacitive behaviors. To gain insight into the intrinsic effects of heteroatoms on the electrochemical capacitive behaviors, zeolite-templated carbon (ZTC) may be the most suitable candidate. ZTC is an ordered microporous carbon with a uniform micropore size of 1.2 nm, a high surface area, and a large micropore volume. In this work, a series of ZTCs containing oxygen, nitrogen, or boron as heteroatoms, with an ordered pore structure and the same pore size, are prepared. By examining their electrochemical capacitive behaviors in an organic electrolyte, the effect of heteroatom doping can be isolated and discussed without considering the effects of pore structure and pore size. Acid anhydride groups are found to generate pseudocapacitance in two potential ranges, -1.0 to -0.3 V (vs Ag/AgClO4) and -0.2 to 0.4 V. B is introduced into the ZTC framework solely as -B(OH)(2), which is found to be an electrochemically inert species. N is introduced as pyridine (3.0%), pyridone/pyrrole (23.8%), quaternary (66.6%), and oxidized N (6.6%), and these species exhibit noticeable pseudocapacitance in the microporous carbon.