Comparison of the Anode Side Catalyst Supports with and without Incorporation of Liquid Electrolyte Layer on the Performance of a Passive Direct Methanol Fuel Cell

Boni, Muralikrishna; Velisala, Venkateswarlu; Kattela, Sivaprasad; Sudheer, S. Venkata Sai; Pullagura, Gandhi; Barik, Debabrata

doi:https://doi.org/10.1155/2023/1224995

International Journal of Energy Research

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Abstract Introduction Results and Discussion Conclusions Data Availability Conflicts of Interest Acknowledgments References Copyright Related Articles

Research Article | Open Access

Volume 2023 | Article ID 1224995 | https://doi.org/10.1155/2023/1224995

Comparison of the Anode Side Catalyst Supports with and without Incorporation of Liquid Electrolyte Layer on the Performance of a Passive Direct Methanol Fuel Cell

Muralikrishna Boni,¹Venkateswarlu Velisala,²Sivaprasad Kattela,³S. Venkata Sai Sudheer,⁴Gandhi Pullagura,⁵and Debabrata Barik⁶

Academic Editor: Thangjam Ibomcha Singh

Received27 Jan 2023

Revised01 May 2023

Accepted06 May 2023

Published13 May 2023

Abstract

In the passive direct methanol fuel cell (DMFC) operation, the catalyst plays an important role in electrical energy production. Efficient catalyst support increases the power output and simultaneously decreases irreversible losses in the fuel cell (FC). Effective utilization of methanol at the anode end reduces methanol crossover by selecting good anode catalyst supports. In the present study, two types of anode catalyst support of carbon and carbon black are used. The two types of anode catalysts are Pt-Ru/C+ Pt-Ru/black and Pt-Ru/C along with a 2 mm thick liquid electrolyte (LE) layer placed in the middle of the two half MEAs. The LE layer is made of piled hydrophilic filter papers, which are soaked in a solution of 1 M H₂SO₄ concentration. The methanol concentration is varied from 1 M to 12 M and from 1 M to 5 M with and without LE-inserted FC, respectively. The passive DMFC with Pt-Ru/C+ Pt-Ru/black anode catalyst and the LE layer exhibit the best performance, producing an MPD of 5.328 mWcm^-2 at a 5 M methanol concentration. The MPD produced by the anode catalyst of Pt-Ru/C+ Pt-Ru/black and Pt-Ru/C along with the 2 mm thickness LE layer incorporated fuel cell is 75.26% higher than conventional-based FC of anode catalyst of single-layer catalyst of Pt-Ru/C.

1. Introduction

Population growth and industrialization are the major reasons for the ever-increasing energy demand. At present, fossil fuels are contributing to a large extent to global power generation. The fast depletion of fossil fuels and the nonuniform distribution of these fossil fuels are driving researchers to look for renewable sources of energy. Fuel cells, coming under the category of clean sources of energy, appear to be a promising source of potential energy. Fuel cell (FC) technology gives a possible result to accommodate the energy requirement of small power generation applications [1–3].

The DMFC has been the subject of a lot of research in the recent decade. In active DMFC, the fuel and oxidant were supplied by a pump and compressor. Because of these components, parasitic losses can be increased for a small amount of power generation. This can be reduced by eliminating external devices. In passive DMFC, fuel and oxidant are provided passively, with no external energy sources exposed. MCO (methanol crossover) is the most significant issue with a passive DMFC. This can be reduced by maximizing methanol utilization on the anode side while simultaneously resisting methanol flow from the anode to the cathode. Many researchers have experimented with various types of catalysts to improve reaction kinetics. Below is a discussion of some of the literature on anode catalyst supports and MCO reduction methods.

Liu et al. [4] examined the impact of various types of catalysts, carbon black and multiwalled carbon nanotube (MWNT), and reduced graphene oxide (rGO) on the DMFC performance. It was noticed that Pt/MWNT catalyst exhibited superior long-term stability than other supports, and Pt/r GO had higher ORR activity. Kim et al. [5] experimentally examined the effect of different cathode catalysts, viz., Pt black, Pt/c, Pt/black (inner layer)+Pt/C, and Pt black (outer layer)+Pt/C on the DMFC performance. It was noticed that Pt black (inner layer)+Pt/C gave better fuel cell performance among the four MEAs.

Glass et al. [6] analyzed the effect of anode catalyst layer thicknesses on the DMFC performance. The catalyst layer thicknesses were varied from 1 mil to 8 mils ( μm) with a Pt/Ru varied form of 0.25 mg/cm² to 2 mg/cm². It was observed that a 4 mil layer of 2 mg/cm² produced the highest peak power density, and 8 mils with 0.25 mg/cm² produced the highest normalized power density concerning 1 mil at 0.25 mg/cm² and 0.5 mg/cm². Chen et al. [7] evaluated the influence of the cathode catalyst layer of 20% wt. Nafion (S-CCL), double cathode catalyst layer (D-CCL), 10% wt. Nafion, and PTFE (M-CCL) on the passive DMFC performance. It was inferred that the M-CCL-contained fuel cell generated the highest MPD than the other two, i.e., D-CCL and S-CCL. Liu et al. [8] experimentally evaluated the impact of nanoporous Pt-Co alloy nanowire catalyst membranes on DMFC performance. It was found that the Pt-Co alloy nanowire catalyst on the anode side exhibited better MOR compared to the Pt/C catalysts.

Giorgi et al. [9] examined the effect of bimetallic catalysts of platinum and gold nanoparticles on DMFC performance. It was found that bimetallic catalysts increased electrocatalyst activity and gold decreased Pt poisoning. Abdullah and Kamarudin [10] analyzed the impact of three types of catalyst supports of Pt-Ru/TiO₂-CNF, Pt-Ru/C, Pt-Ru/CNF, and Pt-Ru/TiO₂ on the DMFC performance. It was inferred that the TiO₂-CNF support catalyst produced 5.54 times the current density concerning commercial Pt-Ru/C catalyst. Fuentes et al. [11] experimentally evaluated the influence of Pt-Ru catalyst supports of TiO₂ and Nb-TiO₂ on the DMFC performance. It was noticed that Nb-TiO₂ support enhanced the catalyst activity by 83% compared to the same catalyst with carbon support. Santos et al. [12] observed a high amount of carbonate in the methane oxidation products of the ADMEFC with Pd50Ni50/C as the anode catalyst.

Kakati et al. [13] experimentally analyzed the effect of anode catalysts of Pt-Ru/Mo on multiwall carbon nanotubes and Pt-Ru/MWCNT on the DMFC performance. It was shown that Pt-Ru/Mo on multiwall carbon nanotube catalyst has higher electrocatalytic activity compared to Pt-Ru/MWCNT catalyst. Saito et al.’s [14] highest surface functional group ratio was found in Marimonanocarbon (C₃H₈), while the lowest was found in Marimonanocarbon (C₃H₆). Kyu et al. [15] experimentally evaluated the effect of anode catalysts of pure Pt, Pt-Ru, and Pt₅Ru₄M (M = Ni, Sn, and Mo) on the methanol oxidation reaction (MOR). It was inferred that the specific activity, MOR of Pt-Ru/Ni electrocatalysts, was greater than that of Pt-Ru catalyst. Yang et al. [16] made a comparative study of PtR-Sn and Pt-Ru catalysts in the MOR process. It was observed that the PtRu-Sn electrocatalyst decreased the particle size and increased the MOR compared to the Pt-Ru catalyst. Rosli et al. [17] experimentally analyzed the effect of cathode catalysts of 5% wt. and 10% wt. Pd/C as well as in steps 2, 4, and 6 mg/cm² on the DMFC performance, and it was shown that the optimal conditions of 10% wt. Pd/C and in steps of 4 mg/cm² gave the best performance. Al-Akraa and Mohammad’s [18] spin-coated titanium oxide (TiO_x) anode catalyst enhanced the charge transfer kinetics, and a significant reduction of the catalyst’s poisoning could elaborate on the origin of catalysis.

Boni et al. [19–21] experimentally analyzed the passive DMFC performance effect with the addition of the LE layer. It was found that an optimized thickness of 2 mm produced MCD and MPD at 5 mol/cm³ (5 M) methanol concentration. Ouellette et al. [22–25] investigated the influence of flowing electrolyte (FE) medium (formic acid and sulphuric acid) and membrane thickness on DMFC performance. It was inferred that the FE-DMFC had superior cell performance.

Li et al. [26] reported that the S-fa-PA/SPEEK composite membrane reduced the MCO more than Nafion membranes. Liu et al. observed that crosslink SPEEK membranes for reduced methanol crossover and 20% wt. crosslink membrane obtained higher power density than commercial Nafion 117 membrane at a 5 M concentration of methanol.

Thus, as listed above, it is observed from the literature review that most of the studies are related to different catalyst supports on the anode and cathode sides, viz., Pt/Ru, PtRu-Sn, and Pt-Ru Ni, to enhance the methanol oxidation reaction (MOR) with a single-coated catalyst layer on the anode side. This work focused on the Pt-Ru/black and Pt-Ru/c catalyst supports with two layers on the anode side and the LE layer to enhance fuel cell performance and reduce methanol crossover.

2. Experimentation

2.1. Fabrication of Membrane Electrode Assembly (MEA)

MEA is made up of three layers: catalyst layers (CL), membrane layers, and diffusion layers (DL). Carbon cloth is used to make DLs, which let the oxidant and fuel enter the reaction sites. Pt-Ru/black (inner layer)+Pt-Ru/C (outer layer) anode CL have a loading of 2.5 mg/cm^-2 and 1.5 mg/cm^-2, respectively. The cathode CL is coated with 60 percent Pt-Ru/C with a loading of 2 mg/cm^-2. The use of a Nafion 117 membrane with a 25 cm² active area is suggested. All of the MEA’s pieces were hot pressed at a pressure of 2 bar. Table 1 lists four varieties of MEAs, with two-layer anode side half MEAs depicted in Figure 1.

2.2. Liquid Electrolyte-MEA

The MEA of a conventional passive DMFC contains a single set of components, including diffusion layers, catalyst layers on the anode and cathode sides, and the membrane. On the anode and cathode sides of the LE-passive DMFC, heaped hydrophilic filter (Whatman filter papers) sheets with a thickness of 2 mm are positioned in the center of the two membranes. These papers are soaked in 1 M of H₂SO₄ solution. The membrane catalyst and diffusion layer are joined using a hot-pressing procedure for each membrane. The LE-passive DMFC is a full MEA with an LE-layer integrated fuel cell. The LE-MEA is shown in Figure 2.

2.3. Cell Assembly

Current collectors, MEAs, and end plates are the major components of a passive DMFC. MEA is positioned in the cell’s center. The MEA is connected to the current collectors. The parts are held in place by end plates. The current collector is composed of SS316L and has a 45.40 percent open ratio. The end plates are composed of PMMA. Methanol is stored in the anode end plate. The square aperture of the cathode plate is equal to the active area, allowing oxygen into the process. Nuts and bolts with a torque of 5 N-m are used to assemble all of the cell components. The exploded view of the passive DMFC is shown in Figure 3.

2.4. Experimental Setup and Test Conditions

Before starting the experiment, the MEA was activated for 12 hours at a 1 M methanol concentration with a constant load and at a voltage of 0.25 V. After connecting all terminals to the DC electronic load bank, wait for 60 minutes to achieve steady-state conditions. During the experimental process, they can be kept in a horizontal position. The voltage readings are noted down for a variation of current by using the knob. All the experiments can be conducted at room temperature. The complete experimental setup is shown in Figure 4.

3. Results and Discussion

The performance of a passive DMFC fitted with four different MEAs, i.e., with a single layer of anode catalyst and two layers of anode catalyst, with and without an LE layer, viz., MEA-1, MEA-2, MEA-3, and MEA-4, is the subject of this experimental investigation. The MEA-3 and MEA-4 both have an LE layer. The methanol concentration varied from 1 M to 12 M. Figures 5(a)–5(h) show the comparison of different catalyst supports with and without incorporated passive DMFC.

(a)

(b)

(c)

(d)

(e)

(f)

(g)

(h)

Figures 5(a)–5(h) show the polarisation and power density curves of the passive DMFC with the four different MEAs. Methanol crossover (MCO) is a serious issue that harms fuel cell performance. Diffusion, electroosmotic drag, and pressure gradients all contribute to MCO. Diffusion contributes the most to MCO out of the three methods. Figures 5(a)–5(e) show that the performance of each of these four cells improves as the methanol concentration increases. This is because as the methanol concentration increases, a greater amount of methanol reaches the anode catalyst layer. This allows for more methanol to be consumed on the anode side of the reaction.

Figures 5(a)–5(e) also show that, regardless of methanol content, the cell using MEA-4 delivers the best results. MEA-4 features two catalyst support layers: Pt-Ru/black (inner layer) and Pt-Ru/C (outer layer), with the LE layer sandwiched between two half MEAs [19]. The diluted methanol solution first passes through the diffusion layer and into the Pt-Ru/black catalyst layer. Because Pt-Ru/black has a higher electrochemical surface activity [5], the methanol solution reacts faster here. More methanol fuels are consumed in this first layer, and the residual methanol solution reaches the second layer of the conventional Pt-Ru/C catalyst layer. Additionally, the second layer also helped in the reduction of methanol crossover. Furthermore, because this MEA-4 has the LE layer, the methanol crossover will be decreased by the addition of the LE layer [19]. The cumulative result is that the cell with MEA-4 performs the best. The MEA-1 based cell, on the other hand, has the worst performance. The MEA-1 based cell contains only one layer of Pt-Ru/C anode catalyst and no LE layer. When compared to the Pt-Ru/black catalyst, the Pt-Ru/C layer shows lower electrochemical activity. The Pt-Ru/black catalyst has a lower thickness (5.6 μm) than the Pt-Ru/C (11.8 μm) catalyst and a larger porosity (0.7 porosity) than the Pt-Ru/C (0.6 porosity) catalyst. The Pt-Ru/black catalyst improves the catalyst’s poisoning tolerance and stability. Due to the smaller thickness and increased porosity of the catalyst, a single layer of Pt-Ru/black catalyst on the anode side enhances the tendency of MCO [20].

Finally, the increased passive DMFC performance is owing to improved reaction kinetics and lower MCO due to the two-layer catalyst and LE layer. For the MEA-4 integrated fuel cell, the maximum MPD and MCD are produced at a methanol concentration of 5 M. The cells containing MEA-4, MEA-2, MEA-3, and MEA-1, respectively, are in decreasing order of performance, as shown in the figures. This suggests that a two-layer catalyst (MEA-2) has a greater beneficial impact on cell performance than a single-layer catalyst plus a liquid electrolyte layer (MEA-3).

Figures 5(f)–5(h) show the performance of the LE-DMFC with a single layer of catalyst and two layers of catalyst, namely, MEA-3 and MEA-4, with methanol concentrations ranging from 7 M to 12 M. The cell with MEA-4 only outperforms the cell with MEA-3 in the region of 7 M-12 M methanol concentration. MEA-3 has a single layer of anode catalyst in between the two half MEAs and the LE layer, whereas MEA-4 has two layers of anode catalyst in between the two half MEAs and the LE layer. As a result, it can be inferred that the two-layer catalyst provides the best performance in LE DMFCs as well.

The MCD and MPD for the cells with the four MEAs in the range of 1 M to 5 M methanol concentration are seen in Figures 6 and 7. The figures show that the MCD and MPD for each of the four cells increase monotonously as the methanol concentration rises and that the cell with MEA-4 has the best performance across the whole range of methanol concentrations. In the range of 1 M to 12 M methanol concentration, as shown in Figures 6 and 7, the MCD and MPD of the LE-DMFC with a single-layer and two-layer anode catalyst support were compared. The cell with MEA-4 gives the best performance throughout this range, as can be seen in Figure 7. It can be seen that the cell performance does not grow uniformly as the methanol concentration rises.

(a)

(b)

(a)

(b)

The cell performance improves with increasing methanol concentrations up to 5 M and then declines as the methanol concentration increases. The best performance is obtained at a methanol concentration of 5 M, as shown in Figures 6 and 7. The MEA-4 based fuel cell produces the maximum MPD and MCD at 5 M methanol concentration, which is 5.328 mWcm^-2 and 55.2 mAcm^-2, respectively. MEA-1’s included fuel cell yields the lowest MPD and MCD values, which are 3.04 mWcm^-2 and 29.6 mAcm^-2, respectively. The MPD and MCD of the MEA-4 based fuel cell are 75.26 percent and 86.48 percent, respectively, higher than those of the MEA-1, a single catalyst layer fuel cell with no LE layer. Table 2 gives the MCD and MPD values for the four MEAs at a 5 M methanol concentration. Table 3 gives a comparison of experimental results with the literature.

Figure 8 shows the comparison of the long-term operation of the fuel cells incorporated with the four MEAs at 5 M of methanol concentration. In each of these cases, the cell was operated at a constant current density of 9.6 mAcm^-2. It can be observed from Figure 8 that higher and lower voltage stability were exhibited by the MEA-4 and MEA-1 incorporated cells, respectively. The higher voltage stability of the MEA-4 is due to the reduced cathode overpotential. The cathode overpotential depends on the methanol and water crossover. The methanol and water crossover are more for MEA-1 based fuel cells. On the other hand, the methanol and water crossover were considerably reduced for the MEA-4 incorporated cell because the MEA-4 has two layers of anode catalyst and the LE layer in between the two half MEAs. It can also be observed from Figure 8 that in the increasing order of the voltage, stability is found in the MEA-1, MEA-2, MEA-3, and MEA-4 incorporated cells,respectively.

4. Conclusions

The performance of a passive DMFC fitted with four different MEAs, i.e., with a single layer of anode catalyst and two layers of anode catalyst, with and without an LE layer, viz., MEA-1, MEA-2, MEA-3, and MEA-4, is the subject of this experimental investigation. Based on the experimental results, it appears that the MEA-4 configuration, which includes two layers of anode catalyst and an LE layer, provides the best performance for the passive DMFC across the entire range of methanol concentrations (1 M to 12 M) tested. From the present study, the following conclusions are drawn: (i)From the experimental results, it is observed that the cell with the MEA-4 configuration (two anode catalyst layers and an LE layer) consistently outperformed the other configurations across the entire range of methanol concentrations tested. The results suggest that the additional anode catalyst layer and the LE layer contributed to improved reaction kinetics and reduced methanol crossover, which ultimately led to better fuel cell performance. It was also observed that the best performance was obtained at a 5 M methanol concentration for all the cells(ii)The MCD (maximum power density) of MEA-4 based fuel cells is 5.328 mW cm^-2, which is 75.26% higher than that of MEA-1-based fuel cells at the same methanol concentration. This indicates that MEA-4 based fuel cells can generate more electrical power per unit area than MEA-1-based fuel cells under the same conditions(iii)Based on the given information, it appears that fuel cells with MEA-4 have the highest performance, followed by MEA-2, MEA-3, and MEA-1 in decreasing order. This suggests that fuel cells with a double-layer catalyst (MEA-2) have a more positive effect on cell performance than those with a single-layer catalyst along with the LE (MEA-3) or those with only a single-layer catalyst (MEA-1)(iv)The fuel cell incorporating MEA-4 has good voltage stability, suggesting that this MEA may be more resistant to catalyst degradation

Data Availability

The data is available in the manuscript.

Conflicts of Interest

The authors declare that they have no conflicts of interest.

Acknowledgments

The authors sincerely thank Karpagam Academy of Higher Education, Coimbatore, India, for providing the necessary facilities to carry out the research work.

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Copyright © 2023 Muralikrishna Boni et al. This is an open access article distributed under the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.

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