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Catalysts for Polymer Membrane Fuel Cells

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A special issue of Catalysts (ISSN 2073-4344). This special issue belongs to the section "Electrocatalysis".

Deadline for manuscript submissions: closed (31 January 2019) | Viewed by 61701

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Special Issue Editors

Prof. Dr. William Mustain

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Guest Editor

Department of Chemical Engineering, University of South Carolina, Swearingen Engineering Center, Columbia SC 29208, USA
Interests: electrochemical energy conversion and storage

Dr. Bryan Pivovar

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Guest Editor

National Renewable Energy Laboratory, Golden, CO, USA
Interests: advanced electrodes and electrocatalysts; novel membranes
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Special Issue Information

Dear Colleagues,

Polymer membrane fuel cells are at an exciting time in their development. State-of-the-art proton exchange membrane fuel cells (PEMFCs) have high activity, stable Pt-based catalysts that have been integrated into cells, and stacks that can operate over many thousands of hours—providing clean power for a myriad of applications and PEMFCs have seen near-exponential growth in their commercial application over the last decade. However, for many applications (e.g., automotive) the overall cost remains above government and industrial targets.

Two approaches with the potential to revolutionize the fuel cell market and allow for cost to be substantively decreased are: 1) Platinum group metal (PGM) free catalysts. PGM-free catalysts present a new learning curve from a catalysis perspective because of the uncertainty in the nature of the active site, generally low active site density and often low turnover frequencies. This leads to high catalyst loadings and thick catalyst layers, which can impart mass transport limitations into the system. 2) Rethink the chemistry of the system. Anion exchange membrane fuel cells (AEMFCs) have been rapidly increasing in popularly. It is thought that AEMFCs will allow for lower cost catalysts, bipolar plates and balance-of-plant than PEMFCs. However, from a catalysis perspective, AEMFCs suffer from sluggish kinetics at the anode and the cathode, and the choices for catalysts outside of the PGM family are limited.

This Special Issue will focus on experimental and theoretical investigations into new catalysts for the hydrogen oxidation reaction (HOR) and oxygen reduction reaction (ORR) in PEMFCs and AEMFCs with a particular interest in the realization of Pt-free and PGM-free materials. Both fundamental and applied studies (focusing on investigating catalysts in realistic environments and improving stability) are of interest. Additionally relevant are reports that detail new methodologies for in situ and operando catalyst characterization. The hope is to compile a set of manuscripts that inform the field of the state-of-the-art in catalysis

Prof. Dr. William Mustain
Dr. Bryan Pivovar
Guest Editors

Manuscript Submission Information

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Keywords

Electrocatalysts
Activity
Stability
Platinum Group Metal Free
Platinum Free
Oxygen Reduction
Hydrogen Oxidation
Proton Exchange Membrane Fuel Cell
Anion Exchange Membrane Fuel Cell
Reversible or Unitized Regenerative Fuel Cell

Published Papers (11 papers)

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Editorial

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3 pages, 157 KiB

Open AccessEditorial

Catalysts for Polymer Membrane Fuel Cells

by William Mustain and Bryan Pivovar

Catalysts 2020, 10(1), 86; https://doi.org/10.3390/catal10010086 - 07 Jan 2020

Cited by 7 | Viewed by 1708

Abstract

Low-temperature fuel cells with a polymer membrane electrolyte are at an exciting time in their development [...] Full article

(This article belongs to the Special Issue Catalysts for Polymer Membrane Fuel Cells)

Research

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12 pages, 3122 KiB

Open AccessFeature PaperArticle

High-Performing PGM-Free AEMFC Cathodes from Carbon-Supported Cobalt Ferrite Nanoparticles

by Xiong Peng, Varchaswal Kashyap, Benjamin Ng, Sreekumar Kurungot, Lianqin Wang, John R. Varcoe and William E. Mustain

Catalysts 2019, 9(3), 264; https://doi.org/10.3390/catal9030264 - 15 Mar 2019

Cited by 54 | Viewed by 6230

Abstract

Efficient and durable non-precious metal electrocatalysts for the oxygen reduction reaction (ORR) are highly desirable for several electrochemical devices, including anion exchange membrane fuel cells (AEMFCs). Here, cobalt ferrite (CF) nanoparticles supported on Vulcan XC-72 carbon (CF-VC) were created through a facile, scalable solvothermal method. The nano-sized CF particles were spherical with a narrow particle size distribution. The CF-VC catalyst showed good ORR activity, possessing a half-wave potential of 0.71 V. Although the intrinsic activity of the CF-VC catalyst was not as high as some other platinum group metal (PGM)-free catalysts in the literature, where this catalyst really shined was in operating AEMFCs. When used as the cathode in a single cell 5 cm⁻² AEMFC, the CF-VC containing electrode was able to achieve a peak power density of 1350 mW cm⁻² (iR-corrected: 1660 mW cm⁻²) and a mass transport limited current density of more than 4 A cm⁻² operating on H₂/O₂. Operating on H₂/Air (CO₂-free), the same cathode was able to achieve a peak power density of 670 mW cm⁻² (iR-corrected: 730 mW cm⁻²) and a mass transport limited current density of more than 2 A cm⁻². These peak power and achievable current densities are among the highest reported values in the literature to date. Full article

(This article belongs to the Special Issue Catalysts for Polymer Membrane Fuel Cells)

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16 pages, 3555 KiB

Open AccessArticle

The Challenge of Achieving a High Density of Fe-Based Active Sites in a Highly Graphitic Carbon Matrix

by Jingkun Li, Qingying Jia, Sanjeev Mukerjee, Moulay-Tahar Sougrati, Goran Drazic, Andrea Zitolo and Frédéric Jaouen

Catalysts 2019, 9(2), 144; https://doi.org/10.3390/catal9020144 - 02 Feb 2019

Cited by 27 | Viewed by 5608

Abstract

As one of the most promising platinum group metal-free (PGM-free) catalysts for oxygen reduction reaction (ORR), Fe–N–C catalysts with a high density of FeN_x moieties integrated in a highly graphitic carbon matrix with a proper porous structure have attracted extensive attention to combine the high activity, high stability and high accessibility of active sites. Herein, we investigated a ZnCl₂/NaCl eutectic salts-assisted ionothermal carbonization method (ICM) to synthesize Fe–N–C catalysts with tailored porous structure, high specific surface area and a high degree of graphitization. However, it was found to be challenging to anchor a high density of FeN_x sites onto highly graphitized carbon. Iron precursors with preexisting Fe–N coordination were required to form FeN_x sites in the nitrogen-doped carbon with a high degree of graphitization, while individual Fe and N precursors led to a Fe–N–C catalyst with poor-ORR activity. This provides valuable insights into the synthesis-structure relationship. Moreover, the FeN_x moieties were identified as the major active sites in acidic conditions, while both FeN_x sites and Fe₂O₃ were found to be active in alkaline medium. Full article

(This article belongs to the Special Issue Catalysts for Polymer Membrane Fuel Cells)

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15 pages, 3234 KiB

Open AccessArticle

Oxygen Reduction Reaction Electrocatalysis in Alkaline Electrolyte on Glassy-Carbon-Supported Nanostructured Pr₆O₁₁ Thin-Films

by Rakesh K. Sharma, Verónica Müller, Marian Chatenet and Elisabeth Djurado

Catalysts 2018, 8(10), 461; https://doi.org/10.3390/catal8100461 - 17 Oct 2018

Cited by 5 | Viewed by 3753

Abstract

In this work, hierarchical nanostructured Pr₆O₁₁ thin-films of brain-like morphology were successfully prepared by electrostatic spray deposition (ESD) on glassy-carbon substrates. These surfaces were used as working electrodes in the rotating disk electrode (RDE) setup and characterized in alkaline electrolyte (0.1 M NaOH at 25 ± 2 °C) for the hydrogen evolution reaction (HER), the oxygen evolution reaction (OER), and the oxygen reduction reaction (ORR) for their potential application in alkaline electrolyzers or in alkaline fuel cells. The electrochemical performances of these electrodes were investigated as a function of their crystallized state (amorphous versus crystalline). Although none of the materials display spectacular HER and OER activity, the results show interesting performances of the crystallized sample towards the ORR with regards to this class of non-Pt group metal (non-PGM) electrocatalysts, the activity being, however, still far from a benchmark Pt/C electrocatalyst. Full article

(This article belongs to the Special Issue Catalysts for Polymer Membrane Fuel Cells)

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19 pages, 2060 KiB

Open AccessArticle

Hydrogen Oxidation on Ni-Based Electrocatalysts: The Effect of Metal Doping

by Elena S. Davydova, Jérémie Zaffran, Kapil Dhaka, Maytal Caspary Toroker and Dario R. Dekel

Catalysts 2018, 8(10), 454; https://doi.org/10.3390/catal8100454 - 15 Oct 2018

Cited by 78 | Viewed by 8777

Abstract

Carbon supported nanoparticles of monometallic Ni catalyst and binary Ni-Transition Metal (Ni-TM/C) electrocatalytic composites were synthesized via the chemical reduction method, where TM stands for the doping elements Fe, Co, and Cu. The chemical composition, structure and morphology of the Ni-TM/C materials were characterized by X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning transmission electron microscopy (STEM) and energy-dispersive X-ray spectroscopy (EDS). The electrochemical properties towards hydrogen oxidation reaction in alkaline medium were studied using the rotating disc electrode and cycling voltammetry methods. A significant role of the TM dopants in the promotion of the hydrogen electrooxidation kinetics of the binary Ni-TM/C materials was revealed. A record-high in exchange current density value of 0.060 mA cm²_Ni was measured for Ni₃Fe₁/C, whereas the monometallic Ni/C counterpart has only shown 0.039 mA cm²_Ni. In order to predict the feasibility of the electrocatalysts for hydrogen chemisorption, density functional theory was applied to calculate the hydrogen binding energy and hydroxide binding energy values for bare Ni and Ni₃TM₁. Full article

(This article belongs to the Special Issue Catalysts for Polymer Membrane Fuel Cells)

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11 pages, 2275 KiB

Open AccessArticle

Experimental Study on the Effect of Hydrogen Sulfide on High-Temperature Proton Exchange Membrane Fuel Cells by Using Electrochemical Impedance Spectroscopy

by Ren-Jun Kang and Yong-Song Chen

Catalysts 2018, 8(10), 441; https://doi.org/10.3390/catal8100441 - 09 Oct 2018

Cited by 6 | Viewed by 3742

Abstract

When the fuel supplied to a high-temperature proton exchange membrane fuel cell (HT-PEMFC) is produced by hydrocarbon formation, hydrogen sulfide (H₂S) may appear, resulting in decreased cell performance and durability. To study the effects of H₂S on the performance and durability of the HT-PEMFC, a series of experiments was conducted. In the first step, the effects of polyvinylidene fluoride (PVDF) and platinum loading on cell performance were investigated and discussed under pure hydrogen operation conditions. Optimal PVDF and platinum compositions in the catalyst layer are suggested. Then, the effect of H₂S on membrane electrode assembly (MEA) performance with various platinum loadings was investigated by supplying hydrogen containing 5.2 ppm of H₂S to the anode of the MEA. An electrochemical impedance spectroscope was employed to measure the impedance of the MEAs under various operating conditions. Finally, degradation of the MEA when supplied with hydrogen containing 5.2 ppm of H₂S was analyzed and discussed. The results suggest that the performance of an MEA with 0.7 mg Pt cm⁻² and 10% PVDF can be recovered by supplying pure hydrogen. The rate of voltage decrease is around 300 μV h⁻¹ in the presence of H₂S. Full article

(This article belongs to the Special Issue Catalysts for Polymer Membrane Fuel Cells)

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11 pages, 1947 KiB

Open AccessFeature PaperArticle

Optimization and Tunability of 2D Graphene and 1D Carbon Nanotube Electrocatalysts Structure for PEM Fuel Cells

by Emeline Remy, Yohann. R. J. Thomas, Laure Guetaz, Frédéric Fouda-Onana, Pierre-André Jacques and Marie Heitzmann

Catalysts 2018, 8(9), 377; https://doi.org/10.3390/catal8090377 - 05 Sep 2018

Cited by 7 | Viewed by 3665

Abstract

In this work, N-doped Multi-Walled Carbon Nanotubes (MWCNTs) and Few Graphene Layers (FGLs) have been functionalized with platinum nanoparticles using two methods starting with hexachloroplatinic acid as precursor: (i) ethylene glycol (EG) reduction and (ii) impregnation followed by reduction in hydrogen atmosphere. Morphological scanning transmission electron microscopy (STEM) analyses showed a homogenous dispersion of metal particles with narrow-size distribution onto both carbon supports (Pt/C loadings between 30 wt % and 40 wt %). Electrocatalytic properties of the as-synthetized catalysts toward the Oxygen Reduction Reaction (ORR) was evaluated in aqueous electrolyte using a three electrodes electrochemical cell by cyclic voltammetry (CV) in rotating disk electrode (RDE). It is shown that a mixture of Pt supported on MWCNT and FGLs allows to enhance both the electrochemical surface area and the activity of the catalyst layer. Ageing tests performed on that optimized active layer showed higher stability than conventional Pt/C. Full article

(This article belongs to the Special Issue Catalysts for Polymer Membrane Fuel Cells)

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15 pages, 10778 KiB

Open AccessArticle

Assessing the Potential of Co-Pt Bronze for Electrocatalysis in Acidic Media

by Yuji Kamitaka, Noboru Taguchi and Yu Morimoto

Catalysts 2018, 8(7), 258; https://doi.org/10.3390/catal8070258 - 25 Jun 2018

Cited by 7 | Viewed by 3846

Abstract

An electron-conducting mixed oxide, Co-Pt bronze was synthesized and examined as a candidate for a highly durable electrocatalyst for both the polymer electrolyte fuel cells and electrolyzers. The motivation of this study comes from the fact that this material has not been studied as an electrocatalyst in acidic media, although past studies showed a high electronic conductivity and a high corrosion resistance. Co-Pt bronze without metallic Pt was obtained by solid-state synthesis and hot aqua regia rinsing. The OER activity was found to be among the highest as a material without Ir and Ru in acidic media, and it showed extremely high electrochemical stability in the OER potential range. Its oxygen reduction reaction (ORR) was obtained after potential cycles down to the hydrogen region, which formed a thin Pt metallic layer over the oxide. While its specific activity was not more than that of pure platinum nanoparticles, its durability against the potential cycles was much higher. Full article

(This article belongs to the Special Issue Catalysts for Polymer Membrane Fuel Cells)

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15 pages, 5807 KiB

Open AccessArticle

MgO-Templated Mesoporous Carbon as a Catalyst Support for Polymer Electrolyte Fuel Cells

by Yuji Kamitaka, Tomohiro Takeshita and Yu Morimoto

Catalysts 2018, 8(6), 230; https://doi.org/10.3390/catal8060230 - 01 Jun 2018

Cited by 34 | Viewed by 5981

Abstract

An MgO-templated mesoporous carbon, CNovel^®, was employed as a catalyst support for the cathode of polymer electrolyte fuel cells (PEFCs) after modifying its dimensional, crystalline, surface and porous structures and the electrochemical oxygen reduction reaction (ORR) activities were examined by the thin-film rotating disk electrode (RDE) method and as well as the membrane electrode assembly (MEA) method. Although the catalytic activity of Pt on CNovel^® was comparable with that on a non-porous carbon, Vulcan^®, in the RDE configuration without Nafion^®, Pt/CNovel showed a considerably higher activity than Pt/Vulcan in the MEA condition with Nafion^®. The mechanism inducing this difference was discussed from the results of electrochemical surface area and sulfonic coverage measurements which suggested that Pt particles on inside pores of CNovel^® are not covered with Nafion^® ionomer while protons can still reach those Pt particles through water network. The MEA performance in the middle and high current-density regions was drastically improved by heat-treatment in air, which modified the pore structure to through-pored ones. Full article

(This article belongs to the Special Issue Catalysts for Polymer Membrane Fuel Cells)

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Review

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18 pages, 9465 KiB

Open AccessFeature PaperEditor’s ChoiceReview

The Use of Power Ultrasound for the Production of PEMFC and PEMWE Catalysts and Low-Pt Loading and High-Performing Electrodes

by Bruno G. Pollet

Catalysts 2019, 9(3), 246; https://doi.org/10.3390/catal9030246 - 07 Mar 2019

Cited by 57 | Viewed by 8339

Abstract

This short review paper highlights some of the research works undertaken over the years by Pollet’s research groups in Birmingham, Cape Town, and Trondheim, in the use of power ultrasound for the fabrication of low temperature fuel cell and electrolyzer catalysts and electrodes. Since the publication of ‘The use of ultrasound for the fabrication of fuel cell materials’ in 2010, there has been an upsurge of international interest in the use of power ultrasound, sonochemistry, and sonoelectrochemistry for the production of low temperature fuel cell and electrolyzer materials. This is because power ultrasound offers many advantages over traditional synthetic methods. The attraction of power ultrasound is the ability to create localized transient high temperatures and pressures, as a result of cavitation, in solutions at room temperature. Full article

(This article belongs to the Special Issue Catalysts for Polymer Membrane Fuel Cells)

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41 pages, 10858 KiB

Open AccessReview

Earth-Abundant Electrocatalysts in Proton Exchange Membrane Electrolyzers

by Xinwei Sun, Kaiqi Xu, Christian Fleischer, Xin Liu, Mathieu Grandcolas, Ragnar Strandbakke, Tor S. Bjørheim, Truls Norby and Athanasios Chatzitakis

Catalysts 2018, 8(12), 657; https://doi.org/10.3390/catal8120657 - 13 Dec 2018

Cited by 56 | Viewed by 8942

Abstract

In order to adopt water electrolyzers as a main hydrogen production system, it is critical to develop inexpensive and earth-abundant catalysts. Currently, both half-reactions in water splitting depend heavily on noble metal catalysts. This review discusses the proton exchange membrane (PEM) water electrolysis (WE) and the progress in replacing the noble-metal catalysts with earth-abundant ones. The efforts within this field for the discovery of efficient and stable earth-abundant catalysts (EACs) have increased exponentially the last few years. The development of EACs for the oxygen evolution reaction (OER) in acidic media is particularly important, as the only stable and efficient catalysts until now are noble-metal oxides, such as IrO_x and RuO_x. On the hydrogen evolution reaction (HER) side, there is significant progress on EACs under acidic conditions, but there are very few reports of these EACs employed in full PEM WE cells. These two main issues are reviewed, and we conclude with prospects for innovation in EACs for the OER in acidic environments, as well as with a critical assessment of the few full PEM WE cells assembled with EACs. Full article

(This article belongs to the Special Issue Catalysts for Polymer Membrane Fuel Cells)

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