文献类型：期刊文献

中文题名：纳米碳纤维的表面改性对水电解析氢反应催化活性的影响

英文题名：Effects of Surface Modification of Carbon Nanofibers on Their Electrocatalytic Activity for Hydrogen Evolution Reaction of Water Electrolysis

作者：钮东方[1];丁勇[1];马智兴[2];王明辉[2];刘洲[2];张博文[2];张新胜[1]

机构：[1]华东理工大学化学工程联合国家重点实验室,上海200237;[2]华东理工大学材料科学与工程学院,上海200237

年份：2015

卷号：73

期号：7

起止页码：729

中文期刊名：化学学报

外文期刊名：Acta Chimica Sinica

收录：CSTPCD;;Scopus;WOS:【SCI-EXPANDED(收录号:WOS:000360199200010)】；北大核心:【北大核心2014】；CSCD:【CSCD2015_2016】；

基金：Project supported by the National Natural Science Foundation of China (No. 21073061) and Shanghai university student innovative activities plan.

语种：中文

中文关键词：纳米碳纤维;析氢反应;表面改性;电催化性能;电解水

外文关键词：carbon nanofibers; hydrogen evolution reaction; surface modification; electrocatalytic activity; water electroly-sis

摘要：主要研究纳米碳纤维(CNF)的表面改性对析氢反应(HER)催化活性的影响.首先采用一种简单易行的超声处理方法,以混酸(浓硫酸和浓硝酸)为溶剂对CNF进行了表面化学处理,以在其表面引入含氧(CNF-OX)官能团,然后将CNF-OX在氨水中超声处理,以引入含氮(CNF-ON)官能团,以及将CNF-OX和硼酸混合经高温热解对CNF-OX进行掺B处理(B-CNF-OX).XPS结果表明,超声处理可以成功地在CNF表面引入含氧和含氮官能团,硼酸高温处理可以掺入B原子.电化学测试结果表明,经过表面改性后的CNF的HER催化性能都要好于未处理过的CNF-UN,其中N掺杂的CNF-ON表现出最好的HER催化活性,且CNF-OX经掺B处理后,B-CNF-OX的性能也较CNF-OX有所增强,即三者的催化活性大小如下:CNF-OXThe effects of surface modification of CNF on their electrocatalytic activity for hydrogen evolution reaction （HER） were investigated. Firstly, Oxygen-containing functional groups were introduced onto the CNF surface （labeled as CNF-OX） by a simple sonochemical oxidation in mixed acids （concentrated sulfuric acid and nitric acid） and then the nitro- gen-containing functional groups were introduced onto the CNF-OX surface （labeled as CNF-ON） by sonochemical treat- ment in ammonia, and the B-doped CNF was synthesized by mixing CNF-OX and boric acid in a ratio following by pyrolysis at 800℃ under N2 atmosphere （labeled as B-CNF-OX）. The XPS results showed that the ultrasonic treatments could intro- duce oxygen- and nitrogen-containing functional groups onto the CNF surface successfully, the oxygen atoms content of CNF-OX was increased from 1.96% to 6.01% compared to the untreated CNF （CNF-UN）, and nitrogen atoms content of CNF-ON was increased from 0% to 1.02% compared to CNF-OX. The pyrolysis of boric acid could introduce B element onto the CNF-OX surface where the B atoms content of B-CNF-OX was 1.00%. The linear sweep voltammetry （LSV） test results showed that the HER electrocatalytic activity of the modified CNFs were higher than CNF-UN, and among them CNF-ON had the highest electrocatalytic activities for HER than the others, the onset overpotential of CNF-ON was 344 mV, which shifted 240 mV positively compared to CNF-UN, and the electrocatalytic activity of B-CNF-OX was enhanced by B-doping treatment compared to CNF-OX. The Tafel test indicated CNF-ON had smallest Tafel slop of 154 mV/dec and largest exchange current density of 6.68 p.A/cm^2. The electrochemical impedance spectroscopy （EIS） was carried out to in- vestigate the complex interfacial properties of the CNFs modified electrode, and the results showed that CNF-ON had the smallest charge transfer resistance of 1578 Ω among all the catalysts, which means the nitrogen-doped CNF had higher activ- ity than the oxygen- and boron-doped CNF. All above indicated that the doping of heteroatom （O, B, N） onto the CNFs sur- face had effects on their electrocatalytic activity for HER, especially the introduction of N atom onto the CNF surface had excellent improvement.