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Article Cite This: ACS Omega 2018, 3, 18323−18333
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High-Power Abiotic Direct Glucose Fuel Cell Using a Gold−Platinum Bimetallic Anode Catalyst Kanjiro Torigoe,*,†,‡ Masatoshi Takahashi,† Koji Tsuchiya,†,§ Kazuki Iwabata,†,§ Toshinari Ichihashi,∥ Kengo Sakaguchi,†,⊥ Fumio Sugawara,†,⊥ and Masahiko Abe†,§ †
Acteiive Co. Ltd., 2641 Yamazaki, Noda 278-8510, Japan Department of Pure and Applied Chemistry, §Research Institute for Science and Technology, ∥Research Equipment Center, and ⊥ Department of Applied Biological Science, Tokyo University of Science, 2641 Yamazaki, Noda 278-8510, Japan
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‡
S Supporting Information *
ABSTRACT: We developed a high-power abiotic direct glucose fuel cell system using a Au−Pt bimetallic anode catalyst. The high power generation (95.7 mW cm−2) was attained by optimizing operating conditions such as the composition of a bimetallic anode catalyst, loading amount of the metal catalyst on a carbon support, ionomer/carbon weight ratio when the catalyst was applied to the anode, glucose and KOH concentrations in the fuel solution, and operating temperature and flow rate of the fuel solution. It was found that poly(N-vinyl-2-pyrrolidone)stabilized Au80Pt20 nanoparticles (mean diameter 1.5 nm) on a carbon (Ketjen Black 600) support function as a highly active anode catalyst for the glucose electrooxidation. The ionomer/carbon weight ratio also greatly affects the cell properties, which was found to be optimal at 0.2. As for the glucose concentration, a maximum cell power was derived at 0.4−0.6 mol dm−3. A high KOH concentration (4.0 mol dm−3) was preferable for deriving the maximum power. The cell power increased with the increasing flow rate of the glucose solution up to 50 cm3 min−1 and leveled off thereafter. At the optimal condition, the maximum power density and corresponding cell voltage of 58.2 mW cm−2 (0.36 V) and 95.7 mW cm−2 (0.34 V) were recorded at 298 and 328 K, respectively.
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INTRODUCTION Currently, there is an urgent demand on the circumvention from global warming.1 For this purpose, a rapid change of energy sources from fossil fuels to clean and sustainable ones is indispensable. Glucose is one of the most abundantly available clean fuels, derivable by degradation of polysaccharides, for example, starch and cellulose.2 Moreover, glucose is a safe (nonhazardous, nonvolatile, and biocompatible) energy source bearing a large inherent chemical energy, which can be released with the oxidation (2.87 MJ mol−1 or 15.9 kJ g−1 for the complete oxidation to carbon dioxide and water).3 Direct glucose fuel cell (DGFC) operates with the oxidation of glucose at the anode and the reduction of oxygen at the cathode.4
to construct separator-free fuel cell systems. Abiotic systems can work at harsh pH and temperature conditions. However, there is a severe issue in common with all these systems, that is, low current density (50 cm3 min−1), the current is governed by the reaction rate. The maximum power density and corresponding cell voltage were 58.2 mW cm−2 (0.36 V) and 95.7 mW cm−2 (0.34 V) at 298 and 328 K, respectively. Stability of the Power. Finally, stability of the power density of this DGFC was investigated at the optimal condition 18330
DOI: 10.1021/acsomega.8b02739 ACS Omega 2018, 3, 18323−18333
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Figure 12. Stability of the power density at the constant voltage of 0.37 V at (a) 328 K and (b) 298 K. [Glucose] = 0.4 mol dm−3, [KOH] = 4.0 mol dm−3, flow rate = 50 cm3 min−1.
Nafion solution (5 wt % in lower aliphatic alcohol/water) were provided from Sigma-Aldrich. Ketjen Black 600 (KB600) was purchased from Lion. Water was deionized with a Milli-Q system (18.2 mΩ cm in resistivity). Preparation of the Anode Catalyst. The anode catalyst used here was Au−Pt bimetallic nanoparticles prepared by the chemical reduction of mixed HAuCl4/H2PtCl6 aqueous solutions in presence of a stabilizer (PVP). For instance, Au80Pt20 nanoparticles were prepared by mixing 8.0 cm3 of HAuCl4 (2 mmol dm−3), 2.0 cm3 of H2PtCl6 (2 mmol dm−3), 20 cm 3 of PVP (10 mmol dm −3 in repeating unit concentration), and 68 cm3 of water in a 150 cm3 vial and stirred for 15 min. Subsequently, to this solution, 2 cm3 of NaBH4 (100 mmol dm−3) was quickly added under vigorous stirring to reduce metal ions. Separately, a calculated amount of carbon powder (KB600) was placed in a 200 cm3 vial. After adding 50 cm3 of water, it was sonicated for 1 h to obtain homogeneous dispersion. Then these two dispersions were mixed together and vigorously stirred for 12 h to attain an adsorption/desorption equilibrium. Finally, the carbon-supported metal catalysts were filtrated, washed with copious amount of water, and dried at 60 °C for 24 h in vacuum. The metal catalysts were observed with TEM (Hitachi H-7650 at 120 kV and JEOL JEM-2100F at 200 kV). EDS analysis was performed with a JEOL JED-2300T using Au Lα line (9.441 keV) and Pt Lα line (9.712 keV). Particle size distributions were determined from about 2000 particles using ImageJ program. Cyclic Voltammetry. The electrocatalytic properties of Au−Pt bimetallic nanoparticles for glucose oxidation were evaluated from CV. The samples were prepared as follows. In a plastic centrifugation tube, 2 mg of the carbon−supported metal catalysts (5 wt % metal/carbon) was suspended in 2 cm3 of mixed ethanol/water (1/1; v/v), then it was centrifuged, and the supernatant was discarded. The precipitate was mixed with 8 mm3 of 5 wt % Nafion in 1-propanol/water (7/3; v/v) and sonicated for 20 min to obtain the catalyst ink. Then, a 1.5 mm3 aliquot of the ink was placed on a Teflon-lined glassy carbon disk electrode (Toyo Corporation G0229, 2 mm ϕ). After drying at 393 K for 15 min, it was used as a working electrode. A Pt wire (Toyo G0228) was used as a counter electrode, and an Ag|AgCl electrode with saturated KCl (Toyo K0265) was employed as a reference electrode. These three electrodes were immersed in 10 cm3 of 0.2 mol dm−3 KOH solution in presence or absence of 0.1 mol dm−3 glucose. The CV profile was recorded in the range between −0.8 and +0.8 V
determined above. As shown in Figure 12a, under the constant voltage of 0.37 V, the initial power density at 328 K was 89.7 mW cm−2. After 28 min, the power density dropped by 8.0% to 82.5 mW cm−2. At 298 K (Figure 12b), the initial power density was 64.2 mW cm−2, which dropped by 27.4% to 46.6 mW cm−2 after 180 min. A plausible reason for the deactivation is adsorption of reaction intermediates and byproducts on the catalyst surface.
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CONCLUSIONS We demonstrated here that a high power density (maximum 95.7 mW cm−2) can be generated with DGFC by optimizing the following seven parameters: composition of the Au−Pt bimetallic anode catalyst, ionomer/carbon weight ratio, loading amount of the catalyst on the anode, glucose and KOH concentrations in the fuel solution, and flow rate and operation temperature. It was found that among different bimetallic compositions, the Au80Pt20 system shows the highest catalytic activity for the glucose oxidation. Optimal conditions were found at I/C = 0.2 (in weight ratio), 0.4 mol dm−3 glucose, 4.0 mol dm−3 KOH, and 50 cm3 min−1 flow rate of fuel solution. Regarding the I/C ratio, too low concentration of the ionomer is ineffective for making the electric contact between the metal catalyst and the anode, whereas a too high concentration of the ionomer covers the catalyst surface and impedes the approach of the fuel molecules to the catalyst surface. A too high concentration of glucose remarkably increases the solution viscosity, thereby reducing the diffusion of the fuel to the catalyst surface. Although the increase in the base concentration promotes the transformation of glucose molecules from the ring to chain conformation, too high a base concentration induces the spontaneous oxidation of glucose in the solution, which impedes the electrooxidation on the catalyst surface. The cell power is also affected by the flow rate of the glucose fuel solution. It increased with an increase in the flow rate up to 50 cm3 min−1 but stagnated at higher flow rates, implying the transition from the diffusion-determining current to reaction-determining one. At the condition where all these parameters were optimized, the maximum power densities and corresponding cell voltage of 58.2 mW cm−2 (0.36 V) and 95.7 mW cm−2 (0.34 V) were recorded at 298 and 328 K, respectively.
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EXPERIMENTAL SECTION Materials. HAuCl4·4H2O, H2PtCl6·6H2O, NaBH4, ethanol, 1-propanol, and β-D-glucose were of reagent grade from Wako and used without further purification. PVP (Mw = 50 000) and 18331
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versus Ag|AgCl (saturated KCl) at the scan rate of 20 mV s−1 on a Hokuto Denko HZ5000 potentio-galvanostat. Fuel Cell Setup and Operation. The DGFC used here was a CHEMIX DFC-010-01 comprising a cation exchange membrane, two electrodes, two silicon gaskets, two graphite separators, two current collectors made of Au-plated Cu, and two stainless plates, located from the center to both ends in this order. The anode was carbon cloth (Fuel Cell Earth CCP40, 3.2 × 3.2 cm2) on which the catalyst ink was deposited. Here, the metal concentration in the catalyst ink was 60 wt % with respect to the carbon support. The cathode used here was a commercial Pt/C paper (Toray EC-E20-1007). These two electrodes were separated from each other with a monovalent CPM (Astom CIMS, 0.15 mm thick). On the graphite separators, a serpentine flow channel was graved to provide the glucose fuel solution or oxygen gas. Concentrations of glucose and KOH were 0.4 and 4.0 mol dm−3, respectively, unless otherwise noticed. The flow rates of glucose fuel solution and air were 10 cm3 min−1 and 2.0 dm3 min−1, respectively. The current−power (I−W) and the current−voltage (I−V) properties of the glucose fuel cell were conducted with a Toyo PEMTest8900DM system. The cell properties were measured at 298 K unless otherwise noticed.
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ASSOCIATED CONTENT
S Supporting Information *
The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsomega.8b02739.
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Variation of the mean particle diameter of Au−Pt bimetallic nanoparticles as a function of the composition, TEM images of Au−Pt bimetallic nanoparticle catalysts on the carbon (KB600) support, EDS point analysis data for four Au80Pt20 bimetallic nanoparticles with different sizes, and EDS line analysis data of a Au80Pt20 bimetallic nanoparticle (PDF)
AUTHOR INFORMATION
Corresponding Author
*E-mail:
[email protected] (Kanjiro Torigoe). ORCID
Kanjiro Torigoe: 0000-0001-7257-8774 Notes
The authors declare no competing financial interest.
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