高活性位点密度Fe-N共掺杂碳纳米片的制备及氧还原性能  被引量:3

Preparation and Oxygen Reduction Performance of Fe,N co-Doped Carbon Nanoplate with High Density of Active Sites

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作  者:殷雯婧 刘啸 钱汇东[1] 邹志青[1] YIN Wenjing;LIU Xiao;QIAN Huidong;ZOU Zhiqing(Shanghai Advanced Research Institute,Chinese Academy of Sciences,Shanghai 201210,China;University of Chinese Academy of Sciences,Beijing 100049,China)

机构地区:[1]中国科学院上海高等研究院,上海201210 [2]中国科学院大学,北京100049

出  处:《高等学校化学学报》2019年第7期1480-1487,共8页Chemical Journal of Chinese Universities

基  金:国家重点研究发展计划项目(批准号:2017YFA0206500);国家自然科学基金(批准号:21673275,21533005,21872165)资助~~

摘  要:从三聚氰胺和均苯四甲酸酐单体出发,通过熔融盐法合成了三嗪结构聚酰亚胺纳米片,借助类石墨相氮化碳(g-C3N4)与铁离子的配位作用,经高温热处理形成了高效掺杂的Fe-N/C催化剂.研究结果表明,该催化剂为表面粗糙的纳米片结构,比表面积高达1794 m^2/g.通过g-C3N4的引入和含量的调控,催化剂中铁元素的掺杂量最高可达1.13%(摩尔分数),为未引入g-C3N4的3.3倍,其原因可归结于g-C3N4配位锚定了铁离子,其较强的配位作用可以避免高温热处理时铁元素的迁移和聚集.该催化剂在酸性条件下氧还原反应半波电位为0.79V,10000周加速测试后的半波电位衰减了30mV,表现出较好的氧还原活性.Fe,N co-doped carbon nanoplate catalyst with high active sites was developed via methods of polymerization of triazine polyimide and carbonization within melting salt of ZnCl2/KCl with the aid of g-C3N4 to anchor Fe^3+.The as-prepared NPT-C3N4-0.5 catalyst displays high specific surface area of 1794 m^2/g.The iron atoms uniformly distribute in the carbon skeleton with an increased doping amount up to the molar percentage of 1.13%,3.3 times of the one without g-C3N4,which can be attributed to the coordination between g-C3N4 and iron to decrease its aggregation under high temperature.The catalyst exhibits excellent catalytic activity for oxygen reduction reaction(ORR)in acid media.Typically,the half-wave potential(E1/2)of the catalyst can reach up to 0.79V(vs.RHE)and only decreases by 30 mV after 10000 potential cycles of accelerated durability test in acid media,showing high activity towards ORR.

关 键 词:非贵金属催化剂 氧还原反应 类石墨相氮化碳 配位作用 聚酰亚胺 

分 类 号:O646[理学—物理化学]

 

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