Ammonia modification of high-surface-area activated carbons as metal-free electrocatalysts for oxygen reduction reaction
Ammonia modification of high-surface-area activated carbons as metal-free electrocatalysts for oxygen reduction reaction
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高比表面积活性炭的氨改性作为氧还原反应的无金属电催化剂
DOI：
10.1016/j.electacta.2018.01.089
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发表时间：
2018-02
影响因子：
6.6
通讯作者：
Ya Liu
中科院分区：
文献类型：
--
作者：
Yongfang Wang;Songlin Zuo;Ya Liu
以椰壳基活性炭为原料，采用KOH活化，并采用三种氨改性方法制备了高比表面积的含氮活性炭。因此，开发了用于氧还原反应（ORR）的具有成本效益的、可扩展的且不含金属的电催化剂。采用元素分析、X射线光电子能谱（XPS）、扫描电子显微镜（SEM）和氮气吸附等方法对活性炭的理化性质进行了分析。采用循环伏安法和线性扫描伏安法研究了活性炭在碱性电解液中的电催化性能。结果表明，氨改性方法和氨改性温度对含氮基团的形态分布有显著影响。这些因素决定了改性活性炭的电催化性能。当通过方法I和II在950 °C下制备含氮活性炭时，其表现出在起始电位和极限电流密度方面与商业20%Pt/C催化剂相当的对ORR的电催化活性。此外，他们催化ORR大约在四电子途径，并表现出良好的耐受甲醇交叉。此外，我们研究了各种含氮物种对电催化性能的影响。
A coconut-shell-based carbon was activated with KOH and three methods of ammonia modification were used to prepare nitrogen-containing activated carbon of high surface area. Thus, a cost-effective, scalable, and metal-free electrocatalyst was developed for use in oxygen reduction reaction (ORR). Elemental analysis, X-ray photoelectron spectroscopy (XPS), Scanning electron microscopy (SEM) and nitrogen adsorption have been used to analyze the physicochemical properties of activated carbons. The electrocatalytic performance of activated carbons was investigated with respect to ORR using cyclic voltammetry and linear sweep voltammetry in an alkaline electrolyte. The results indicate that the species distribution of nitrogen-containing groups was significantly affected by the method and temperature of ammonia modification. These factors consequently determined the electrocatalytic performance of the modified activated carbons. When the nitrogen-containing activated carbon was prepared by methods I and II at 950 °C, it exhibited an electrocatalytic activity toward ORR that was comparable to that of commercial 20% Pt/C catalyst in terms of onset potential and limiting current density. Moreover, they catalyzed ORR approximately in a four-electron pathway and showed good tolerance toward methanol crossover. In addition, we investigated the influence of various nitrogen-containing species on the electrocatalytic performance.
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