Andres Parra‐Puerto

Imperial College London

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Anthony Kucernak

Imperial College London

Javier Rubio‐García

University of Cambridge

Kieran F. Fahy

University of Toronto

Mary P. Ryan

Imperial College London

Kai Ling Ng

Imperial College London

Angela E. Goode

Johnson Matthey (United Kingdom)

Manuel Gómez

Universidad de Alcalá

Pilar Gómez‐Sal

Universidad de Alcalá

Matthew Markiewicz

Imperial College London

Miguel Galájov

Universidad de Alcalá

Cooperative Institutions

The Faraday Institution

Imperial College London

Transnational Press London

University College London

Universidad Autónoma de Madrid

Consejo Superior de Investigaciones Científicas

University of Oxford

London Centre for Nanotechnology

Biochemical Society

University of Cambridge

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Incorporation of Graphene and Graphene-Based Materials into Membranes As an Alternative Electrolyte Configuration for Low and High Temperature Polymeric Electrolyte Membranes Fuel Cells.

Meeting abstracts/Meeting abstracts (Electrochemical Society. CD-ROM) (2020)

María Pérez-Page Jianuo Chen Andres Parra‐Puerto Javier Rubio‐García Anthony Kucernak

The electrolyte plays an important role in the Membrane Electrode Assembly (MEA) of Polymeric Electrolyte Membranes Fuel Cells, (PEMFCs), having three main functions, to act as ion conductor, electronic insulator and a separator for the reactant gases [1]. The electrolyte is a Proton Exchange Membrane and Nafion is the most widely used polymeric membrane in this technology. However, because its particular structure it requires a good hydration to lead a high proton conductivity, which limit the operating temperature to lower than 100 o C. Poly[2,2′-m-(phenylene)-5,5′-benzimidazole (PBI) membrane doped with Phosphoric Acid, has been presented as an alternative to Nafion membranes allowing higher operating temperatures, 200 o C, which enhance the kinetics of the reactions. However, during the operation of High Temperature Fuel Cells (HT-PEMFCs) these membranes suffer Phosphoric Acid leaching leading to a low proton conductivity and degradation of the fuel cell [2]. The 2D honeycomb lattice of Graphene provides this material particular properties such as high surface area, exceptionally high electrical conductivity, good chemical and thermal stability and excellent barrier properties, which make it a potential material for a large number of applications. In addition to this [1], Hu. et al. [3] have demonstrated that Single Layer Graphene present a high proton conductivity being at the same time a barrier for other elements, which makes this material a potential electrolyte for PEMFC. However, SLG has some drawbacks notably due to the complex process to produce it and its high cost. These limitations leave an open window to Graphene based materials such as Graphene Oxide, which shows very attractive properties to act as filler in Nafion and PBI membranes due to its chemical functionalization and its non-porous structure, which provides additional resistance for mass transport and increases the tortuosity of the permeation pathways leading to higher selectivity [1]. Here we will describe the work carried out at University of Manchester incorporating SLG and GO composite membranes into the MEA of both PEM Fuel Cells, Low Temperature (LT-PEMFC) and HT-PEMFC. The addition of the SLG produced by CVD into the MEA of LT-PEMFC has demonstrated no change in the proton conductivity, supporting the hypothesis that SLG is a good proton conductor. In addition, for a particular LT-PEMFC, Direct Methanol Fuel Cells (DMFC), a decreasing of the methanol crossover has found leading a significant enhancement of the power density [4]. SLG has been also incorporated into the MEA of HT-PEMFC, which use PBI membrane instead of Nafion, to evaluate its proton conductivity and barrier properties, this time to stop the Phosphoric Acid leaching. Although positive results have been reported by adding SLG into the MEAs, a different approach has been conducted by the development of GO-composite membranes also for both type of PEMFC. Exfoliated Graphene Oxide has been synthesized by electrochemical exfoliation of graphite and has been incorporated as a filler into two different of matrix polymer, Nafion and PBI, to evaluate their performance in both PEMFC, high and low temperature. References: [1] Perez-Page Maria, Sahoo Madhumita, Holmes, M Stuart. Single Layer 2D Crystals for Electrochemical Applications of Ion Exchange Membranes and Hydrogen Evolution Catalyst. Advance Materials Interfaces (2019) 6, 1801838. [2] S. H. Eberhardt, M. Toulec, F. Marone, M. Stampanoni, F. N. Buchi and T. J. Schmidt. Dynamic Operation of HT-OEFC: In-Operando Imaging of Phosphoric Acid Profiles and (Re)distribution. Journal of The Electrochemical Society, (2015), 162, 3, F310-F316. [3] S. Hu, M. Lozada-Hidalgo, F. C. Wang, A. Mishchenko, F. Schedin, R. R. Nair, E. W. Hill, D. W. Boukhvalov, M. I. Katsnelson, R. A. W. Dryfe, I. V. Grigorieva, H. A. Wu, A. K. Geim. Proton transport one-atom-thick crystals. Nature (2014), 516, 227. [4] Stuart M. Holmes, Orabhuraj Balakrishnan, Vasu. S. Kalangi, Xiang Zhang, Marcelo Lozada-Hidalgo, Pulickel M Ajayan, Rahul R. Nair. 2D Crystals Significantly Enhance the Performance of a Working Fuel Cell. Advance Energy Materials, 7, (2017).

Phosphoric acid

Separator (oil production)

Nafion

Proton Transport

10.1149/ma2020-02352247mtgabs

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Supported Transition Metal Phosphides: Activity Survey for HER, ORR, OER, and Corrosion Resistance in Acid and Alkaline Electrolytes

Meeting abstracts/Meeting abstracts (Electrochemical Society. CD-ROM) (2020)

Andres Parra‐Puerto Kai Ling Ng Kieran F. Fahy Angela E. Goode Mary P. Ryan

One of the main bottle necks for the introduction of fuel cell technology in the market, is their dependency on precious metals as catalyst. Focusing on the electrochemical reactions involved, the most sluggish is the Oxygen Reduction Reaction (ORR). Significant research has been performed to optimize for the amount of the precious metal used, whilst keeping the same activity. On the other hand, many investigations have been carried out to find non-precious metal catalysts with the same performance for ORR, Oxygen Evolution Reaction (OER), Hydrogen Evolution Reaction (HER) and Hydrogen Oxidation Reaction (HOR) [1]. One of those candidates are the metal phosphides [2], however, these catalysts nowadays only are active for ORR, HER, OER and they have very poor activity towards the HOR [3]. Here we present the work done related to the simple synthesis of different MP catalysts (M = Ni, Co, W, Cr and Mo) [4]; their catalytic activity towards H 2 and O 2 reactions; and their corrosion resistance in acidic and alkaline electrolytes. Co 2 P was found to have a very interesting ORR catalytic behaviour and peroxide generation under alkaline and acidic conditions respectively. To understand the activity of Co 2 P, an HRTEM analysis was done to understand the changes in the morphology before and after the ORR reaction. References [1] M. S. Faber and S. Jin, “Earth-abundant inorganic electrocatalysts and their nanostructures for energy conversion applications,” Energy Environ. Sci. , vol. 7, no. 11, pp. 3519–3542, Oct. 2014, doi: 10.1039/C4EE01760A. [2] A.-M. Alexander et al. , “Alternative catalytic materials: carbides, nitrides, phosphides and amorphous boron alloys,” Chem. Soc. Rev. , vol. 39, no. 11, pp. 4388–4401, Oct. 2010, doi: 10.1039/b916787k. [3] R. Prins and M. E. Bussell, “Metal Phosphides: Preparation, Characterization and Catalytic Reactivity,” Catal. Letters , vol. 142, no. 12, pp. 1413–1436, Dec. 2012, doi: 10.1007/s10562-012-0929-7. [4] A. Parra-Puerto, K. L. Ng, K. Fahy, A. E. Goode, M. P. Ryan, and A. Kucernak, “Supported Transition Metal Phosphides: Activity Survey for HER, ORR, OER, and Corrosion Resistance in Acid and Alkaline Electrolytes,” ACS Catal. , vol. 9, pp. 11515–11529, Nov. 2019, doi: 10.1021/acscatal.9b03359. Figure 1

Alkaline fuel cell

Electrochemical energy conversion

Oxygen evolution

10.1149/ma2020-02372392mtgabs

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Citations (2)

CCDC 812062: Experimental Crystal Structure Determination

The Cambridge Structural Database (2011)

Miguel Galájov A. Galindo Carmelo García Pérez Manuel Gómez Pilar Gómez‐Sal

An entry from the Cambridge Structural Database, the world’s repository for small molecule crystal structures. The entry contains experimental data from a crystal diffraction study. The deposited dataset for this entry is freely available from the CCDC and typically includes 3D coordinates, cell parameters, space group, experimental conditions and quality measures.

10.5517/ccw80kp

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Carbon Materials for Energy Storage from Redox Flow Batteries to Lithium Sulfur Batteries, Catalyst for Alkaline Electrolysers and Hybrid Redox Flow Batteries

Proceedings of the Materials for Sustainable Development Conference (MAT-SUS) (2022)

Andres Parra‐Puerto Jack Dawson Mengjun Gong Javier Rubio‐García Anthony Kucernak

Carbon fibers

10.29363/nanoge.nfm.2022.171

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Enhanced Photovoltaic Performance of Nanowire Dye-Sensitized Solar Cells Based on Coaxial TiO₂@TiO Heterostructures with a Cobalt(II/III) Redox Electrolyte

ACS Applied Materials & Interfaces (2013)

Jiandong Fan Cristian Fàbrega Reza R. Zamani Yan Hao Andres Parra‐Puerto

The growth of a TiO shell at the surface of TiO2 nanowires (NWs) allowed us to improve the power conversion efficiency of NW-based dye-sensitized solar cells (DSCs) by a factor 2.5. TiO2@TiO core–shell NWs were obtained by a two-step process: First, rutile-phase TiO2 NWs were hydrothermally grown. Second, a hongquiite-phase TiO shell was electrochemically deposited at the surface of the TiO2 NWs. Bare TiO2 and heterojunction TiO2@TiO NW-based DSCs were obtained using a cobalt(II/III) redox electrolyte and LEG4 as the dye. With this electrolyte/dye combination, DSCs with outstanding Voc values above 900 mV were systematically obtained. While TiO2@TiO NW-based DSCs had slightly lower Voc values than bare TiO2 NW-based DSCs, they provided 3-fold higher photocurrents, overall reaching 2.5-fold higher power conversion efficiencies. The higher photocurrents were associated with the larger surface roughness and an enhanced charge-carrier separation/transfer at the NW/dye interface.

Rutile

10.1021/am402344d

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Citations (23)

Metal Phosphides As Electrocatalyst and Supports for PEM Fuel Cells

Meeting abstracts/Meeting abstracts (Electrochemical Society. CD-ROM) (2018)

Andres Parra‐Puerto Kieran F. Fahy Angela E. Goode Mary P. Ryan Anthony Kucernak

One of the main bottle neck for the complete introduction of the fuel cells technology in the market, is their dependency on precious metals as catalyst. Focusing on the electrochemical reactions involved, the most sluggish is the Oxygen Reduction Reaction (ORR). Many techniques and research were done to reach the high optimization for the amount of the precious metal used, keeping the same activity. In the other hand, many investigations were carried on to find non-precious metal catalyst with the same performance for the different reactions (ORR, HER, OER and HOR)[1]. One of those candidates are the metal phosphides [2], however, this catalysts nowadays only are active for ORR, HER, OER and they have very poor activity related to HOR [3]. Here we present the work done related to the really simple synthesis of CoP catalyst with a very interesting ORR catalytic behaviour and peroxide generation under acid and alkaline conditions. Some TEM characterization was done to understand the changes in the morphology before and after the ORR reaction. Another application of these materials is to use thezzm as support, due to their chemical resistance and low cost. As well, depositing platinum on them gives the possibility to obtain an interesting synergistically effect improving the activity with lower loadings of Pt deposited [4]. [1] M. S. Faber and S. Jin, “Earth-abundant inorganic electrocatalysts and their nanostructures for energy conversion applications,” Energy Environ. Sci. , vol. 7, no. 11, pp. 3519–3542, Oct. 2014. [2] A.-M. Alexander et al. , “Alternative catalytic materials: carbides, nitrides, phosphides and amorphous boron alloys,” Chem. Soc. Rev. , vol. 39, no. 11, p. 4388, Oct. 2010. [3] R. Prins and M. E. Bussell, “Metal Phosphides: Preparation, Characterization and Catalytic Reactivity,” Catal. Letters , vol. 142, no. 12, pp. 1413–1436, Dec. 2012. [4] H.-Y. Park et al. , “Pd nanocrystals on WC as a synergistic electrocatalyst for hydrogen oxidation reactions.,” Phys. Chem. Chem. Phys. , vol. 15, no. 6, pp. 2125–30, 2013.

Electrochemical energy conversion

Precious metal

10.1149/ma2018-01/30/1784

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Hydrogen/functionalized benzoquinone for a high-performance regenerative fuel cell as a potential large-scale energy storage platform

Journal of Materials Chemistry A (2020)

Javier Rubio‐García Anthony Kucernak Andres Parra‐Puerto Rutao Liu Barun Kumar Chakrabarti

A functionalised benzoquinone redox species is coupled to the hydrogen/proton reaction to achieve a respectable reversible redox fuel cell (RFC).

Benzoquinone

10.1039/c9ta12396b

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Citations (35)

Data used for the paper Andres Parra-Puerto, Kai Ling NG, Kieran Fahy, Angela E Goode, Mary P. Ryan, and Anthony Kucernak Supported Transition Metal Phosphides: Activity Survey for HER, ORR, OER and Corrosion Resistance in Acid and Alkaline Electrolytes ACS Catalysis, 2019 DOI: 10.1021/acscatal.9b03359

Zenodo (CERN European Organization for Nuclear Research) (2019)

Andres Parra‐Puerto Kai Ling Ng Kieran F. Fahy Angela E. Goode Mary P. Ryan

The data in this spreadsheet was used to produce the figures in the paper Andres Parra-Puerto, Kai Ling NG, Kieran Fahy, Angela E Goode, Mary P. Ryan, and Anthony Kucernak Supported Transition Metal Phosphides: Activity Survey for HER, ORR, OER and Corrosion Resistance in Acid and Alkaline Electrolytes ACS Catalysis, 2019 DOI: 10.1021/acscatal.9b03359Please cite the above reference if you wish to use this data

10.5281/zenodo.3539510

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Synthetic and structural studies of monocyclopentadienyl cyclometalated aryl tantalum(v) compounds

Dalton Transactions (2011)

Miguel Galájov Agustı́n Galindo Carlos J. Gómez‐García Manuel Gómez Pilar Gómez‐Sal

Cyclometalated aryl tetra- or trichlorido cyclopentadienyl tantalum complexes [TaXCl(3){C(6)H(4)(2-CH(2)NMe(2))-κ(2)C,N}] (X = Cl 1, η(5)-C(5)H(5)2, η(5)-C(5)H(4)(SiMe(3)) 3, η(5)-C(5)Me(5)4) containing a five-membered TaC(3)N chelate ring were synthesized by reaction of the TaXCl(4) (X = Cl, η(5)-C(5)H(5), η(5)-C(5)H(4)(SiMe(3)), η(5)-C(5)Me(5)) with the appropriate lithium aryl reagent [Li{C(6)H(4)(2-CH(2)NMe(2))}]. The reported complexes were studied by IR and NMR spectroscopy and the X-ray molecular structures of compounds 2, 3 and 4 were determined by diffraction methods. These compounds were theoretically analyzed by the DFT method and their structures were rationalized. The preferential coordination of the 2-{(dimethylamino)methyl}phenyl ligand was justified by an analysis of the molecular orbitals of the Ta(η(5)-C(5)H(5))Cl(3) and C(6)H(4)(2-CH(2)NMe(2)) fragments. In addition, the exchange pathways that account for the NMR equivalency of the Me(2)N- methyl groups and -CH(2)- hydrogen atoms of the coordinated C(6)H(4)(2-CH(2)NMe(2))-κ(2)C,N ligand were theoretically studied.

10.1039/c1dt10223k

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Citations (2)

CCDC 812061: Experimental Crystal Structure Determination

The Cambridge Structural Database (2011)

Miguel Galájov A. Galindo Celeste García-Gallarín Manuel Gómez Pilar Gómez‐Sal

10.5517/ccw80jn

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