期刊
ACS CATALYSIS
卷 6, 期 3, 页码 1929-1941出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.5b02485
关键词
palladium nanoparticle; graphitic carbon nitride; hydrogen evolution and oxidation reaction; underpotential deposition; hydrogen binding energy
资金
- DST, Government of India [SR/S1/PC-10/2011]
The hydrogen evolution reaction (HER) and hydrogen oxidation reaction (HOR) in aqueous medium are two fundamental reactions for the development of non-fossil energy storage and conversion devices. In the polymer electrolyte membrane fuel cell (PEMFC) carbon supported platinum (Pt/C) based catalysts are universally used in cathodes and anodes; however, the poor durability of Pt/C due to degradation of the catalyst in the strongly oxidizing environment prevents its widespread applications. It remains a great challenge to develop new electrocatalysts with superior activity and very high durability for the HER/HOR. Here, we report the synthesis of a porous palladium nanoparticle- carbon nitride composite (Pd-CNx) for its superior activity and high durability toward the HER/HOR in acidic and alkaline media. The Pd-CNx composites exhibited high catalytic activity for hydrogen evolution in acidic media with a small onset potential of -12 mV and a Tafel slope of 35 mV dec(-1). At a small Pd loading of 0.043 mg cm(-2), this catalyst also exhibits a current density of 10 mA cm(-2) at a low overpotential of -55 mV with an excellent stability. The HER activity on Pd-CNx composite is comparable to that of commercial Pt/C in acid media. The stability tests of this catalyst were done through a large number of repeated potential cycles and long-term electrolysis. These confirm the exceptional durability of this catalyst, which is much better than that of Pt/C catalysts. Furthermore, this catalyst has also displayed superior HOR activity, measured by a rotating-disk experiment with a broad range of pH (0-14) in different buffer solutions. The HER/HOR activities of porous Pd-CNx composite in different buffer solutions were correlated with the hydrogen binding energy (HBE) of the catalyst surface. The HER/HOR activity gradually decreases with an increase in the HBE as the solution pH increases. The superior HER/HOR activities and very high durability at porous Pd-CNx composite are due to strong bonding between Pd and carbon (Pd-C bond), the porous morphology, and synergistic interactions between Pd-NPs and the carbon nitride (CNx) support.
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