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Article ; Online: Optimization of a Perovskite Oxide-Based Cathode Catalyst Layer on Performance of Direct Ammonia Fuel Cells

Jeerh, Georgina / Zou, Peimiao / Zhang, Mengfei / Tao, Shanwen

ACS Applied Materials & Interfaces. 2022 Dec. 27, v. 15, no. 1 p.1029-1041

2022

Abstract: To maximize fuel cell performance, transport pathways for electrons, ions, and reactants should be connected well. This demands a well-constructed microstructure in the catalyst layer (CL). Herein we design and optimize a cathode CL for a direct ammonia ... ...

Abstract	To maximize fuel cell performance, transport pathways for electrons, ions, and reactants should be connected well. This demands a well-constructed microstructure in the catalyst layer (CL). Herein we design and optimize a cathode CL for a direct ammonia fuel cell (DAFC) using a perovskite oxide as the catalyst to reduce reliance on platinum group metals (PGMs). The effects of tailoring carbon, ionomer, and polytetrafluoroethylene (PTFE) content in cathode CLs (CCLs) were explored, and several DAFCs were tested. Using the same catalyst and operating conditions, the lowest maximum current density and peak power density obtained were 85.3 mA cm-² and 5.92 mW cm-², respectively, which substantially increased to 317 mA cm-² and 30.1 mW cm-² through proper carbon, ionomer, and PTFE optimization, illustrating the importance of an effective three-phase interface. The findings reveal that despite employment of an active catalyst for oxygen reduction at the cathode site, the true performance of the catalyst cannot be reflected unless it is supported by proper design of the CCL. The study also reveals that by optimizing the CCL, similar performances to those of Pt/C-based CCLs in literature can be obtained at a cost reduction.
Keywords	ammonia ; carbon ; catalysts ; cathodes ; cost effectiveness ; fuel cells ; fuels ; microstructure ; oxygen ; platinum ; polytetrafluoroethylene ; direct ammonia fuel cell (DAFC) ; perovskite ; cathode ; catalyst layer ; optimization
Language	English
Dates of publication	2022-1227
Size	p. 1029-1041.
Publishing place	American Chemical Society
Document type	Article ; Online
ISSN	1944-8252
DOI	10.1021/acsami.2c17253
Database	NAL-Catalogue (AGRICOLA)

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Article: Recent progress in ammonia fuel cells and their potential applications

Jeerh, Georgina / Zhang, Mengfei / Tao, Shanwen

Journal of materials chemistry A. 2021 Jan. 19, v. 9, no. 2

2021

Abstract: Conventional technologies are largely powered by fossil fuel exploitation and have ultimately led to extensive environmental concerns. Hydrogen is an excellent carbon-free energy carrier, but its storage and long-distance transportation remain big ... ...

Abstract	Conventional technologies are largely powered by fossil fuel exploitation and have ultimately led to extensive environmental concerns. Hydrogen is an excellent carbon-free energy carrier, but its storage and long-distance transportation remain big challenges. Ammonia, however, is a promising indirect hydrogen storage medium that has well-established storage and transportation links to make it an accessible fuel source. Moreover, the notion of ‘green ammonia’ synthesised from renewable energy sources is an emerging topic that may open significant markets and provide a pathway to decarbonise a variety of applications reliant on fossil fuels. Herein, a comparative study based on the chosen design, working principles, advantages and disadvantages of direct ammonia fuel cells is summarised. This work aims to review the most recent advances in ammonia fuel cells and demonstrates how close this technology type is to integration with future applications. At present, several challenges such as material selection, NOₓ formation, CO₂ tolerance, limited power densities and long term stability must still be overcome and are also addressed within the contents of this review.
Keywords	ammonia ; carbon dioxide ; chemistry ; comparative study ; energy ; fossil fuels ; hydrogen ; transportation
Language	English
Dates of publication	2021-0119
Size	p. 727-752.
Publishing place	The Royal Society of Chemistry
Document type	Article
Note	NAL-AP-2-clean
ZDB-ID	2702232-8
ISSN	2050-7496 ; 2050-7488
ISSN (online)	2050-7496
ISSN	2050-7488
DOI	10.1039/d0ta08810b
Database	NAL-Catalogue (AGRICOLA)

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Article: Improved stability and activity of Fe-based catalysts through strong metal support interactions due to extrinsic oxygen vacancies in Ce₀.₈Sm₀.₂O₂₋δ for the efficient synthesis of ammonia

Humphreys, John / Lan, Rong / Chen, Shigang / Tao, Shanwen

Journal of materials chemistry A. 2020 Aug. 18, v. 8, no. 32

2020

Abstract: In this article, hematite α-Fe₂O₃ was used as the precursor for the iron-based ammonia synthesis catalyst. Ce₀.₈Sm₀.₂O₂₋δ (SDC), with extrinsic oxygen vacancies was used as a promoter for forming an Fe–SDC composite catalyst. The new Fe–SDC catalyst ... ...

Abstract	In this article, hematite α-Fe₂O₃ was used as the precursor for the iron-based ammonia synthesis catalyst. Ce₀.₈Sm₀.₂O₂₋δ (SDC), with extrinsic oxygen vacancies was used as a promoter for forming an Fe–SDC composite catalyst. The new Fe–SDC catalyst achieves both high catalytic activity and excellent oxygenate tolerance, working with excellent stability at a feed-gas purity of 99.996%. At 500 °C, 10 MPa for the 80% Fe–20% SDC catalyst, and 15 MPa for the industrial Fe catalysts, and at an impurity level of 150 ppm, with known injected 107.5 ppm O₂, the activity of Fe–SDC retains 47.3% of that measured in purified gases while it is only 26.4% and 7.6% for the wüstite and magnetite – based industrial Fe catalysts respectively. It is believed that the introduction of extra extrinsic oxygen vacancies strengthen the strong metal-support interaction (SMSI), preventing the growth of formed Fe particles, leading to excellent stability and high tolerance to oxygenates. The SMSI between Fe and oxygen vacancies in SDC may also help to weaken and break the strong NN bonds in N₂, increasing the catalytic activity. The use of promoters with extrinsic oxygen and potentially other anion vacancies provides a new strategy to develop oxygenate tolerant catalysts for efficient synthesis of ammonia from less pure feed gases at reduced pressures.
Keywords	ammonia ; catalysts ; catalytic activity ; gases ; hematite ; iron ; magnetite ; nitrogen ; oxygen
Language	English
Dates of publication	2020-0818
Size	p. 16676-16689.
Publishing place	The Royal Society of Chemistry
Document type	Article
ZDB-ID	2702232-8
ISSN	2050-7496 ; 2050-7488
ISSN (online)	2050-7496
ISSN	2050-7488
DOI	10.1039/d0ta05238h
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: A fast ceramic mixed OH

Zou, Peimiao / Iuga, Dinu / Ling, Sanliang / Brown, Alex J / Chen, Shigang / Zhang, Mengfei / Han, Yisong / Fortes, A Dominic / Howard, Christopher M / Tao, Shanwen

Nature communications

2024 Volume 15, Issue 1, Page(s) 909

Abstract: Low temperature ionic conducting materials such as ... ...

Abstract	Low temperature ionic conducting materials such as OH
Language	English
Publishing date	2024-01-30
Publishing country	England
Document type	Journal Article
ZDB-ID	2553671-0
ISSN	2041-1723 ; 2041-1723
ISSN (online)	2041-1723
ISSN	2041-1723
DOI	10.1038/s41467-024-45060-1
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Investigation of Perovskite Oxide SrCo

Zou, Peimiao / Chen, Shigang / Lan, Rong / Tao, Shanwen

ChemSusChem

2019 Volume 12, Issue 12, Page(s) 2788–2794

Abstract: Single-phase perovskite oxide ... ...

Abstract	Single-phase perovskite oxide SrCo
Language	English
Publishing date	2019-05-22
Publishing country	Germany
Document type	Journal Article
ISSN	1864-564X
ISSN (online)	1864-564X
DOI	10.1002/cssc.201900451
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: A symmetric direct ammonia fuel cell using ternary NiCuFe alloy embedded in a carbon network as electrodes

Zhang, Mengfei / Zhang, Jie / Jeerh, Georgina / Zou, Peimiao / Sun, Boyao / Walker, Marc / Xie, Kui / Tao, Shanwen

Journal of materials chemistry A. 2022 Sept. 20, v. 10, no. 36

2022

Abstract: Recently, due to the high energy density of ammonia, low source-to-tank energy cost and carbon free fuel, low-temperature direct ammonia fuel cells (DAFCs) have attracted extensive attention and play an important role in ammonia economy. In DAFCs, Pt- ... ...

Abstract	Recently, due to the high energy density of ammonia, low source-to-tank energy cost and carbon free fuel, low-temperature direct ammonia fuel cells (DAFCs) have attracted extensive attention and play an important role in ammonia economy. In DAFCs, Pt-based materials have been the most studied electrocatalysts for the anodic ammonia oxidation reaction (AOR) and cathodic oxygen reduction reaction (ORR) over the past decade. However, the high cost of precious metal has markedly inhibited the large-scale application of DAFCs. Herein, a bifunctional material of ternary Ni4Cu5Fex (x = 0, 0.5, 1, 3, 5) alloy embedded in a carbon network was prepared by a simple solvothermal approach, and showed superior activity and durability towards both AOR and ORR. The excellent bifunctional catalytic activity of the Ni4Cu5Fe1/C sample was analyzed by experimental and calculational methods. Utilizing the bifunctional activities of this alloy, a symmetric DAFC was assembled with Ni4Cu5Fe1/C as both the anode and cathode, with a commercial anion exchange membrane (AEM) as electrolyte. The symmetric DAFC-Ni4Cu5Fe1/C showed a maximum current density of 67 mA cm⁻² at 80 °C. To the best of our knowledge, this is the first report on a symmetric DAFC. This work not only reports a new AOR/ORR bifunctional catalyst, but also moves towards the development of low-cost DAFCs with simple structure.
Keywords	alloys ; ammonia ; anion-exchange membranes ; anodes ; carbon ; catalysts ; catalytic activity ; cathodes ; durability ; electrochemistry ; electrolytes ; energy costs ; energy density ; fuel cells ; fuels ; oxidation
Language	English
Dates of publication	2022-0920
Size	p. 18701-18713.
Publishing place	The Royal Society of Chemistry
Document type	Article
ZDB-ID	2702232-8
ISSN	2050-7496 ; 2050-7488
ISSN (online)	2050-7496
ISSN	2050-7488
DOI	10.1039/d2ta04129d
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: A simple high-performance matrix-free biomass molten carbonate fuel cell without CO2 recirculation.

Lan, Rong / Tao, Shanwen

Science advances

2016 Volume 2, Issue 8, Page(s) e1600772

Abstract: In previous reports, flowing CO2 at the cathode is essential for either conventional molten carbonate fuel cells (MCFCs) based on molten carbonate/LiAlO2 electrolytes or matrix-free MCFCs. For the first time, we demonstrate a high-performance matrix-free ...

Abstract	In previous reports, flowing CO2 at the cathode is essential for either conventional molten carbonate fuel cells (MCFCs) based on molten carbonate/LiAlO2 electrolytes or matrix-free MCFCs. For the first time, we demonstrate a high-performance matrix-free MCFC without CO2 recirculation. At 800°C, power densities of 430 and 410 mW/cm(2) are achieved when biomass-bamboo charcoal and wood, respectively-is used as fuel. At 600°C, a stable performance is observed during the measured 90 hours after the initial degradation. In this MCFC, CO2 is produced at the anode when carbon-containing fuels are used. The produced CO2 then dissolves and diffuses to the cathode to react with oxygen in open air, forming the required [Formula: see text] or [Formula: see text] ions for continuous operation. The dissolved [Formula: see text] ions may also take part in the cell reactions. This provides a simple new fuel cell technology to directly convert carbon-containing fuels such as carbon and biomass into electricity with high efficiency.
MeSH term(s)	Bioelectric Energy Sources ; Biomass ; Carbon Dioxide/chemistry ; Carbonates/chemistry ; Catalysis ; Electricity ; Electrodes ; Oxygen/chemistry
Chemical Substances	Carbonates ; Carbon Dioxide (142M471B3J) ; Oxygen (S88TT14065)
Language	English
Publishing date	2016
Publishing country	United States
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ZDB-ID	2810933-8
ISSN	2375-2548 ; 2375-2548
ISSN (online)	2375-2548
ISSN	2375-2548
DOI	10.1126/sciadv.1600772
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: High ionic conductivity in a LiFeO2-LiAlO2 composite under H2/air fuel cell conditions.

Lan, Rong / Tao, Shanwen

Chemistry (Weinheim an der Bergstrasse, Germany)

2015 Volume 21, Issue 3, Page(s) 1350–1358

Abstract: New ionic conducting materials for electrolytes for electrochemical devices have been attracting the interest of researchers in energy materials. Here, for the first time, we report a conductive composite with high ionic conductivity derived from an ... ...

Abstract	New ionic conducting materials for electrolytes for electrochemical devices have been attracting the interest of researchers in energy materials. Here, for the first time, we report a conductive composite with high ionic conductivity derived from an electronic conductor α-LiFeO2 and an insulator γ-LiAlO2. High conductivity was observed in the α-LiFeO2-γ-LiAlO2 composite when prepared by a solid state reaction method. However, the conductivity enhancement in α-LiFeO2-γ-LiAlO2 composite was not observed when the two oxides were mechanically mixed. The α-LiFeO2-γ-LiAlO2 composite also exhibits O(2-) or/and H(+) ionic conduction which was confirmed through H2/air fuel cell measurements. An exceptionally high conductivity of 0.50 S cm(-1) at 650 °C was observed under H2/air fuel cell conditions. This provides a new approach to discover novel ionic conductors from composite materials derived from electronic conductors.
Language	English
Publishing date	2015-01-12
Publishing country	Germany
Document type	Journal Article
ZDB-ID	1478547-x
ISSN	1521-3765 ; 0947-6539
ISSN (online)	1521-3765
ISSN	0947-6539
DOI	10.1002/chem.201404476
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Article: Electricity Generation from Ammonia in Landfill Leachate by an Alkaline Membrane Fuel Cell Based on Precious-Metal-Free Electrodes

Zhang, Mengfei / Zou, Peimiao / Jeerh, Georgina / Chen, Shigang / Shields, Jane / Wang, Huanting / Tao, Shanwen

ACS sustainable chemistry & engineering. 2020 Aug. 06, v. 8, no. 34

2020

Abstract: Ammonia contaminated wastewater poses a great hazard to the safety and quality of water resources. Use of ammonia fuel cells to remove ammonia from wastewater is a promising strategy, which not only eliminates ammonia but also generates electricity as a ... ...

Abstract	Ammonia contaminated wastewater poses a great hazard to the safety and quality of water resources. Use of ammonia fuel cells to remove ammonia from wastewater is a promising strategy, which not only eliminates ammonia but also generates electricity as a bonus. For ammonia fuel cells, the key challenge is to identify stable and highly active precious-metal-free catalysts to be used as electrodes. In this study, a composite material α-MnO₂/C was prepared through a simple reaction of potassium permanganate with carbon black in a concentrated H₂SO₄ solution. An alkaline membrane fuel cell was prepared using the as-synthesized α-MnO₂/C as the cathode, previously reported NiCu/C as the anode, and an alkaline membrane as the electrolyte. The electrochemical activities of the MnO₂/C cathode and the performance of this fuel cell utilizing ammonia as the fuel were investigated. Finally, leachate from a local landfill site was tested in the fuel cell. Without the addition of alkali, the ammonia concentration in landfill leachate was reduced from 2711 to 95 ppm. Over the operational period of approximately 6 h, 96.5% of the ammonia in the leachate was removed by the fuel cell. These results demonstrate that the ammonia present within wastewater can efficiently be removed by a fuel cell employing non-precious metal electrodes at room temperature, while simultaneously generating electricity as a bonus. This provides an exciting new technology for the treatment of ammonia-rich wastewater.
Keywords	ambient temperature ; ammonia ; anodes ; catalysts ; cathodes ; composite materials ; electricity ; electricity generation ; electrochemistry ; electrolytes ; fuel cells ; fuels ; landfill leachates ; landfills ; manganese dioxide ; potassium permanganate ; soot ; sulfuric acid ; technology ; wastewater ; water resources
Language	English
Dates of publication	2020-0806
Size	p. 12817-12824.
Publishing place	American Chemical Society
Document type	Article
ISSN	2168-0485
DOI	10.1021/acssuschemeng.0c02926
Database	NAL-Catalogue (AGRICOLA)

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Article: N,N-Dimethylacetamide-Diluted Nitrate Electrolyte for Aqueous Zn//LiMn₂O₄ Hybrid Ion Batteries

Chen, Shigang / Sun, Pan / Humphreys, John / Zou, Peimiao / Zhang, Mengfei / Jeerh, Georgina / Sun, Boyao / Tao, Shanwen

ACS applied materials & interfaces. 2021 Sept. 27, v. 13, no. 39

2021

Abstract: N,N-Dimethylacetamide (DMA) cooperated with LiNO₃ salt has previously shown to be a promising electrolyte for a Li//O₂ battery, showing good stability against both the O₂ electrode reaction and Li stripping/plating. In this work, DMA is hybridized with a ...

Abstract	N,N-Dimethylacetamide (DMA) cooperated with LiNO₃ salt has previously shown to be a promising electrolyte for a Li//O₂ battery, showing good stability against both the O₂ electrode reaction and Li stripping/plating. In this work, DMA is hybridized with a concentrated nitrate electrolyte [2.5 m Zn(NO₃)₂ + 13 m LiNO₃ aqueous solution] for better electrochemical stability while using less dissolved salts. The widest electrochemical stability window for this DMA-diluted electrolyte is determined as 3.1 V, the negative critical stability potential of which is −1.6 V versus Ag/AgCl, indicating desirable stability against hydrogen evolution and Zn deposition. The findings can be attributed to the weakened Li⁺/Zn²⁺ solvation sheath caused by low permittivity of DMA, as revealed through Raman spectra characterization and molecular dynamics simulation. A Zn//Zn symmetrical cell and Zn//LiMn₂O₄ hybrid ion batteries are assembled in air directly, attributed to the stability of DMA toward O₂. Zn stripping/plating with a dendrite-free morphology is delivered for 110 h and 200 charge/discharge cycles under 1 C rate, achieving 99.0% Coulombic efficiency. The maximum capacity of the battery is 121.0 mA h·g–¹ under 0.2 C rate (based on the mass of LiMn₂O₄), delivering an energy density of 165.8 W h·kg–¹ together with 2.0 V working voltage. This work demonstrates the feasibility and validity of utilizing a relatively dilute electrolyte dissolved in oxygen for a highly stable aqueous rechargeable battery.
Keywords	air ; aqueous solutions ; batteries ; electric potential difference ; electrochemistry ; electrodes ; electrolytes ; energy density ; hydrogen production ; molecular dynamics ; nitrates ; oxygen ; solvation
Language	English
Dates of publication	2021-0927
Size	p. 46634-46643.
Publishing place	American Chemical Society
Document type	Article
ISSN	1944-8252
DOI	10.1021/acsami.1c12911
Database	NAL-Catalogue (AGRICOLA)

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