真空加热活化法提高内嵌钴粒子的碳纳米管的水裂解产氢催化活性

doi:10.7503/cjcu20170715

高等学校化学学报 ›› 2018, Vol. 39 ›› Issue (6): 1249.doi: 10.7503/cjcu20170715

真空加热活化法提高内嵌钴粒子的碳纳米管的水裂解产氢催化活性

邹佳运, 刘一蒲, 陈辉, 李国栋()

吉林大学化学学院, 无机合成与制备化学国家重点实验室, 长春 130012

收稿日期:2017-11-09 出版日期:2018-06-10 发布日期:2018-05-18
基金资助:
国家自然科学基金(批准号: 21371070)和吉林省自然科学基金(批准号: 20160101291JC)资助.

Enhanced Hydrogen Evolution Catalytic Activity of Cobalt-embedded Carbon Nanotubes by Thermal Vacuum Activation^†

ZOU Jiayun, LIU Yipu, CHEN Hui, LI Guodong^*()

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China

Received:2017-11-09 Online:2018-06-10 Published:2018-05-18
Contact: LI Guodong E-mail:lgd@jlu.edu.cn
Supported by:
† Supported by the National Natural Science Foundation of China(No.21371070) and the Natural Science Foundation of Jilin Province, China(No.20160101291JC).

摘要/Abstract

摘要：

采用真空加热活化法制备出高催化活性的内嵌金属钴纳米粒子的碳纳米管材料. 通过增加碳纳米管材料的本征碳缺陷位点, 显著提升了材料的催化活性(>7倍). 高分辨透射电子显微镜(HRTEM)、 X射线光电子能谱(XPS)和拉曼(Raman)光谱表征结果显示, 真空加热活化增加了碳纳米管的本征碳缺陷, 并减少了碳纳米管碳层的杂原子含量. 电化学表征和电催化水裂解实验结果表明, 增加碳纳米管的本征碳缺陷位既可以在碳纳米管上产生更多的催化位点, 又可以提高碳纳米管界面的电荷迁移能力, 进而提高对水裂解的催化性能.

关键词: 碳纳米管, 钴纳米粒子, 电催化, 水裂解

Abstract:

Cobalt-embedded carbon nanotubes with high catalytic activity were prepared by a facile thermal vacuum activation method. After the vacuum activation, intrinsic carbonaceous defects of the cobalt-embedded carbon nanotubes increased, resulting in greatly improved catalytic activity(>7-fold). The characterizations of high resolution transmission electron microscopy(HRTEM), X-ray photoelectron spectroscopy(XPS) and Raman spectroscopy revealed that the thermal vacuum post-treatment can lead to a great amount of intrinsic carbonaceous defects, which further relates to more catalytically active sites and thus enhances the interfacial electron-transfer properties, resulting in improved catalytic activity.

Key words: Carbon nanotubes, Cobalt nanoparticles, Electrocatalysis, Water splitting

中图分类号:

O646

TrendMD:

邹佳运, 刘一蒲, 陈辉, 李国栋. 真空加热活化法提高内嵌钴粒子的碳纳米管的水裂解产氢催化活性. 高等学校化学学报, 2018, 39(6): 1249.

ZOU Jiayun, LIU Yipu, CHEN Hui, LI Guodong. Enhanced Hydrogen Evolution Catalytic Activity of Cobalt-embedded Carbon Nanotubes by Thermal Vacuum Activation^†. Chem. J. Chinese Universities, 2018, 39(6): 1249.

图/表 7

Fig.1 XRD patterns of Co/CNT(a) and Co/CNT-V800(b)

Fig.2 SEM images of Co/CNT(A) and Co/CNT-800(D), TEM image of Co/CNT(B) and HRTEM images of Co/CNT(C), Co/CNT-V800(E) and Co/CNT-N800(F)

Fig.3 N/C and O/C atomic ratios in Co/CNT, Co/CNT-V800, Co/CNT-N800(A) and Raman spectra of Co/CNT(a), Co/CNT-V800(b) and Co/CNT-N800(c)(B)

Fig.4 Polarization curves(A) and overpotential at 10 mA/cm2(B) of Co/CNT treated at different temperature(500—1000 ℃) by thermal vacuum activation and untreated Co/CNT

Fig.5 Polarization curves of Co/CNT(a), Co/CNT-N800(b) and Co/CNT-V800(c) in 0.5 mol/L H2SO4(A) and polarization curves of Co/CNT-V800 in 0.5 mol/L H2SO4 before and after 1000, 3000 and 5000 cyclesj-t curve of Co/CNT-800 at η=97 mV for 35 h is shown in the inset of (B).

Fig.6 Schematic illustration of the change of microstructure before and after thermal vacuum activation

Fig.7 Difference of current density between the sweeps versus scan rate of Co/CNT(a) and Co/CNT-V800(b)(A) and Nyquist plots of Co/CNT(a) and Co/CNT-V800(b)(B) The slope of the ftting line is used for determination of the double-layer capacitance(Cdl).

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真空加热活化法提高内嵌钴粒子的碳纳米管的水裂解产氢催化活性

Enhanced Hydrogen Evolution Catalytic Activity of Cobalt-embedded Carbon Nanotubes by Thermal Vacuum Activation^†

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真空加热活化法提高内嵌钴粒子的碳纳米管的水裂解产氢催化活性

Enhanced Hydrogen Evolution Catalytic Activity of Cobalt-embedded Carbon Nanotubes by Thermal Vacuum Activation†

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Enhanced Hydrogen Evolution Catalytic Activity of Cobalt-embedded Carbon Nanotubes by Thermal Vacuum Activation^†