Floating conductive catalytic nano-rafts at soft interfaces for hydrogen evolution

被引:76
作者
Bian, Xiaojun [1 ,2 ,3 ]
Scanlon, Micheal D. [3 ]
Wang, Sinong [1 ,2 ]
Liao, Lei [1 ,2 ]
Tang, Yi [1 ,2 ]
Liu, Baohong [1 ,2 ]
Girault, Hubert H. [3 ]
机构
[1] Fudan Univ, Ctr Chem Energy Mat, Dept Chem, Shanghai 200433, Peoples R China
[2] Fudan Univ, Ctr Chem Energy Mat, Lab Mol Catalysis & Innovat Mat, Shanghai 200433, Peoples R China
[3] Ecole Polytech Fed Lausanne, Lab Electrochim Phys & Analyt, Stn 6, CH-1015 Lausanne, Switzerland
基金
瑞士国家科学基金会;
关键词
REDUCED GRAPHENE OXIDE; WALL CARBON NANOTUBES; MO2C MOSI2 TASI2; WORK-FUNCTIONS; ELECTROCHEMICAL INSTABILITY; PHOTOCATALYTIC REDUCTION; MOLYBDENUM BORIDE; ELECTRON; NANOPARTICLES; SEMICONDUCTOR;
D O I
10.1039/c3sc51290h
中图分类号
O6 [化学];
学科分类号
070301 [无机化学];
摘要
Mo2C nanowires and composites of Mo2C nanoparticles formed on multiwalled carbon nanotubes (Mo2C/CNT) were developed as advanced catalysts for hydrogen evolution at a polarised water-1,2-dichloroethane interface. Each catalyst acts as a catalytic nano-raft suspended at the interface to markedly enhance the rates of biphasic proton reduction in the presence of an organic solubilised electron donor, decamethylferrocene. Mo2C nanoparticles were grown in situ on the conductive CNT support, achieving a high dispersion and intimate contact, thereby facilitating electron transfer between the components. The high catalytic activity of each catalyst was successfully demonstrated by their respective impacts on the reaction kinetics. The reaction rate increased more than 1000 times when the Mo2C/CNT composite was present at a very low concentration of 25 mu M. CNTs have the ability to act as highly efficient conduits or "transport superhighways" for injected electrons to reach the catalytic sites of the nanoparticle. Electrochemical instabilities, similar to those observed for the transfer of surface-active ions, were observed under experimental conditions that produced an abundance of hydrogen at the interface. Finally, the movement of CNTs floating at the interface under the influence of a cycling applied interfacial Galvani potential difference was vividly captured in a short movie.
引用
收藏
页码:3432 / 3441
页数:10
相关论文
共 82 条
[1]
An KH, 2001, ADV FUNCT MATER, V11, P387, DOI 10.1002/1616-3028(200110)11:5<387::AID-ADFM387>3.0.CO
[2]
2-G
[3]
Atkins P. W., 1990, PHYS CHEM
[4]
Luminescent Carbon Nanodots: Emergent Nanolights [J].
Baker, Sheila N. ;
Baker, Gary A. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2010, 49 (38) :6726-6744
[5]
Nanocomposite of MoS2 on ordered mesoporous carbon nanospheres: A highly active catalyst for electrochemical hydrogen evolution [J].
Bian, Xiaojun ;
Zhu, Jie ;
Liao, Lei ;
Scanlon, Micheal D. ;
Ge, Peiyu ;
Ji, Chang ;
Girault, Hubert H. ;
Liu, Baohong .
ELECTROCHEMISTRY COMMUNICATIONS, 2012, 22 :128-132
[6]
Supramolecular assembly of nauoparticles at liquid-liquid interfaces [J].
Binder, WH .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2005, 44 (33) :5172-5175
[7]
A Novel Approach to Create a Highly Ordered Monolayer Film of Graphene Nanosheets at the Liquid-Liquid Interface [J].
Biswas, Sanjib ;
Drzal, Lawrence T. .
NANO LETTERS, 2009, 9 (01) :167-172
[8]
Metal-nanocluster-filled carbon nanotubes: Catalytic properties and possible applications in electrochemical energy storage and production [J].
Che, GL ;
Lakshmi, BB ;
Martin, CR ;
Fisher, ER .
LANGMUIR, 1999, 15 (03) :750-758
[9]
Electronic structure and optical limiting behavior of carbon nanotubes [J].
Chen, P ;
Wu, X ;
Sun, X ;
Lin, J ;
Ji, W ;
Tan, KL .
PHYSICAL REVIEW LETTERS, 1999, 82 (12) :2548-2551
[10]
Highly active and durable nanostructured molybdenum carbide electrocatalysts for hydrogen production [J].
Chen, W. -F. ;
Wang, C. -H. ;
Sasaki, K. ;
Marinkovic, N. ;
Xu, W. ;
Muckerman, J. T. ;
Zhu, Y. ;
Adzic, R. R. .
ENERGY & ENVIRONMENTAL SCIENCE, 2013, 6 (03) :943-951