Abstract

Carbon-supported PtRu nanoalloy (PtRu/C) is widely used as the anode catalyst for direct methanol fuel cells (DMFC), and an aqueous phase synthesis of PtRu/C is in high demand due to for energy-saving and environmentally-benign considerations, however, it is very challenging to attain stoichiometric reduction, good dispersion and a high alloying degree. Herein, we report a facile aqueous phase approach with dimethylamine borane (DMAB) as the reducing agent to synthesize a PtRu/C(DMAB). TEM, XRD, XPS and ICP-AES characterizations indicate that the structural parameters in the PtRu/C(DMAB) are improved significantly as compared to those obtained in a PtRu/C(NaBH4) and a commercial PtRu/C, contributing to an enhanced electrocatalytic performance. It turns out that the PtRu/C(DMAB) exhibits the highest methanol electro-oxidation (MOR) performance among all of the tested samples, with the peak current up to 1.8 times as much as that of the state-of-the-art commercial PtRu/C, corroborating the highest output power density in comparative DMFC tests. In-situ attenuated total reflection infrared (ATR-IR) spectroscopy correlates the higher methanol electro-oxidation performance of the PtRu/C(DMAB) with its enhanced CO resistance and CO2 generation. This simple aqueous synthetic approach may provide an alternative route for developing efficient anode electrocatalysts of DMFCs.

Highlights

  • Direct methanol fuel cells (DMFC) are promising energy-converter to drive portable devices owing to their high efficiency, low emissions and rich fuel supply [1]

  • dimethylamine borane (DMAB) is initially used in this work as the reductant to synthesis of a PtRu/C catalyst

  • The smaller apparent Tafel slope on the PtRu/C(DMAB) together with the larger oxidation peak current suggests that the DMAB-derived PtRu/C catalyst at least demonstrates a higher activity in a half cell measurement condition, deserving of a further test as the real anode catalyst FFigiguurere55

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Summary

Introduction

Direct methanol fuel cells (DMFC) are promising energy-converter to drive portable devices owing to their high efficiency, low emissions and rich fuel supply [1]. Dimethylamine borane (DMAB, (CH3)2NH·BH3), a water soluble small molecule with a milder but sufficiently strong reducing power [30], was initially developed in our group for the synthesis of a series of carbon supported catalysts such as Pd-B/C [31], Pt-B/C [32], Pt3Ni-B/C [32] and Pt3Co/C catalysts [33]. It is unknown whether the DMAB-derived PtRu/C(DMAB) yields better structure and performance towards MOR than the NaBH4-derived PtRu/C(NaBH4). In-situ attenuated total reflection infrared (ATR-IR) spectroscopy is applied to monitor the interfacial species on the catalyst surfaces during MOR to provide a molecular-level understanding of different performances

Results and Discussion
Physicochemical Characterization
Preliminary DMFC Test
Interfacial Species Evolved during MOR
Material Characterization
Electrochemical Measurements
Fuel Cell Performance Test
In-Situ ATR-IR Measurement
Conclusions
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