氮掺杂石墨烯的一步法低温合成及用作微生物燃料电池阴极催化剂的产电特性

doi:10.7503/cjcu20130806

高等学校化学学报 ›› 2014, Vol. 35 ›› Issue (4): 825.doi: 10.7503/cjcu20130806

氮掺杂石墨烯的一步法低温合成及用作微生物燃料电池阴极催化剂的产电特性

付融冰¹, 杨兰琴², 冯雷雨²(), 郭伟³

1. 上海市环境科学研究院, 上海 200233
2. 同济大学环境科学与工程学院, 上海 200092
3. 中国石油天然气管道局天津设计院, 天津 300457

收稿日期:2013-08-19 出版日期:2014-04-10 发布日期:2013-12-05
作者简介:联系人简介: 冯雷雨, 男, 博士, 讲师, 主要从事微生物燃料电池新型电极材料制备及新功能研究. E-mail: leiyufeng@tongji.edu.cn
基金资助:
国家自然科学基金(批准号: 51108332)和江苏省自然科学基金(批准号: BK2011416)资助

One-pot Low-temperature Synthesis of Nitrogen-doped Graphene and It Application as Cathode Catalyst in Microbial Fuel Cells for Electricity Generation^†

FU Rongbing¹, YANG Lanqin², FENG Leiyu^2,^*(), GUO Wei³

1. Shanghai Academy of Environmental Scineces, Shanghai 200233, China
2. School of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
3. Tianjin Designing Institute of China Petroleum Pipeline Bureau, Tianjin 300457, China

Received:2013-08-19 Online:2014-04-10 Published:2013-12-05
Contact: FENG Leiyu E-mail:leiyufeng@tongji.edu.cn
Supported by:
† Supported by the National Natural Science Foundation of China(No.51108332) and the Natural Science Foundation of Jiangsu Province, China(No.BK2011416)

摘要/Abstract

摘要：

利用爆炸法低温合成了氮掺杂石墨烯(NG), 并通过高分辨透射电子显微镜、 X射线光电子能谱仪、 Raman光谱仪以及X射线衍射仪对其进行了表征. 电化学性能检测结果表明, 所合成的NG在中性磷酸盐电解液中具有优异的氧还原催化活性, 完全能够与贵重金属铂催化剂(Pt/C)相媲美, 氧还原催化稳定性甚至优于Pt/C. 当NG用作微生物燃料电池(MFCs)的阴极氧还原催化剂时, 在外阻为1000 Ω情况下, MFCs的最大功率密度为1345 mW/m², 产电稳定性优于以Pt/C为阴极催化剂的MFCs, 可以成为Pt催化剂的理想替代品.

关键词: 微生物燃料电池, 氧还原反应, 氮掺杂石墨烯, 阴极催化剂

Abstract:

Nitrogen-doped graphene(NG) was synthesized by denotation process at low temperature, and characterized by high-resolution transmission electron microscopy(HRTEM), X-ray photoelectron spectrometry(XPS), Raman spectrometry and X-ray diffraction(XRD). Electrochemical examinations demonstrated that in the neutral phosphate electrolyte the synthesized NG had an excellent electrocatalytic activity for oxygen reduction reaction(ORR), comparable to that of platinum catalyst(Pt/C), and its electrocatalytic stability was even better than Pt/C. When NG was used as cathode catalyst in single-chamber microbial fuel cells(MFCs), the maximal power density at external resistance of 1000 Ω was 1345 mW/m², and the stability of power generation in MFCs even outperformed that with Pt/C as cathode catalyst, indicating that NG might be a perfect alternative to Pt catalyst in MFCs.

Key words: Microbial fuel cell, Oxygen reduction reaction, Nitrogen-doped graphene, Cathode catalyst

中图分类号:

O646

TrendMD:

付融冰, 杨兰琴, 冯雷雨, 郭伟. 氮掺杂石墨烯的一步法低温合成及用作微生物燃料电池阴极催化剂的产电特性. 高等学校化学学报, 2014, 35(4): 825.

FU Rongbing, YANG Lanqin, FENG Leiyu, GUO Wei. One-pot Low-temperature Synthesis of Nitrogen-doped Graphene and It Application as Cathode Catalyst in Microbial Fuel Cells for Electricity Generation^†. Chem. J. Chinese Universities, 2014, 35(4): 825.

图/表 9

Fig.1 TEM(A) and HRTEM(B) images of synthesized NG

Fig.2 AFM image(A) and Raman spectrum(B) of synthesized NG

Fig.3 CVs of synthesized NG(a) and Pt/C(b) at a scan rate(v) of 0.1 V/s(A) and CVs of NG electrode at different scan rates(B) in O2-saturated 50 mmol/L neutral PBS(B) Scan rate/(V·s-1): a. 0.1, b. 0.2, c. 0.3. Inset of (B): j vs. scan rate.

Fig.4 CVs of NG electrode before(a) and after(b) a continuous potentiodynamic swept for 100000 cycles at 25 ℃

Fig.5 Effect of sodium formate on electrocatalytic activity for oxyegen reduction in O2-satura-ted 50 mmol/L neutral PBSa. No sodium formate addition; b. 5 mmol/L sodium formate. Current scan rate: 10-7 A/s.

Fig.6 Current-time chronoamperometric res-ponse of Pt/C(a) and NG(b) electrodes to COThe arrow indicates the addition of 10%(volume ratio) CO into O2-saturated neutral PBS at -0.4 V.

Fig.7 RRDE voltammograms for ORR in O2-saturated neutral PBS on NG(a and a') and Pt/C(b and b') electrodesThe electrode rotation rate was 1200 r/min.

Fig.8 XPS survey(A) of synthesized NG and high-resolutio N1s spectrum(B)

Fig.9 Cell voltage(a, b) and power density(c, d) vs. current density in NG-MFCs(a, c) and Pt/C-MFCs(b, d)(A) and decrease of the maximum power density in NG-MFCs as a function of cycle number at an external resistance of 1000 Ω(B)

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氮掺杂石墨烯的一步法低温合成及用作微生物燃料电池阴极催化剂的产电特性

One-pot Low-temperature Synthesis of Nitrogen-doped Graphene and It Application as Cathode Catalyst in Microbial Fuel Cells for Electricity Generation^†

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氮掺杂石墨烯的一步法低温合成及用作微生物燃料电池阴极催化剂的产电特性

One-pot Low-temperature Synthesis of Nitrogen-doped Graphene and It Application as Cathode Catalyst in Microbial Fuel Cells for Electricity Generation†

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One-pot Low-temperature Synthesis of Nitrogen-doped Graphene and It Application as Cathode Catalyst in Microbial Fuel Cells for Electricity Generation^†