Publications
364 results found
Westhead O, Spry M, Bagger A, et al., 2023, The role of ion solvation in lithium mediated nitrogen reduction, Journal of Materials Chemistry A, Vol: 11, Pages: 12746-12758, ISSN: 2050-7488
Since its verification in 2019, there have been numerous high-profile papers reporting improved efficiency of lithium-mediated electrochemical nitrogen reduction to make ammonia. However, the literature lacks any coherent investigation systematically linking bulk electrolyte properties to electrochemical performance and Solid Electrolyte Interphase (SEI) properties. In this study, we discover that the salt concentration has a remarkable effect on electrolyte stability: at concentrations of 0.6 M LiClO4 and above the electrode potential is stable for at least 12 hours at an applied current density of −2 mA cm−2 at ambient temperature and pressure. Conversely, at the lower concentrations explored in prior studies, the potential required to maintain a given N2 reduction current increased by 8 V within a period of 1 hour under the same conditions. The behaviour is linked more coordination of the salt anion and cation with increasing salt concentration in the electrolyte observed via Raman spectroscopy. Time of flight secondary ion mass spectrometry and X-ray photoelectron spectroscopy reveal a more inorganic, and therefore more stable, SEI layer is formed with increasing salt concentration. A drop in faradaic efficiency for nitrogen reduction is seen at concentrations higher than 0.6 M LiClO4, which is attributed to a combination of a decrease in nitrogen solubility and diffusivity as well as increased SEI conductivity as measured by electrochemical impedance spectroscopy.
Hongrutai N, Nganglumpoon R, Watmanee S, et al., 2023, <i>In</i><i>-situ</i> electrodeposited Ag/Cu for electrochemical reduction of acetic acid to nanodiamond under ambient conditions, MATERIALS TODAY CHEMISTRY, Vol: 30, ISSN: 2468-5194
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- Citations: 1
Liang X, Wang S, Feng J, et al., 2023, Structural transformation of metal-organic frameworks and identification of electrocatalytically active species during the oxygen evolution reaction under neutral conditions, INORGANIC CHEMISTRY FRONTIERS, Vol: 10, Pages: 2961-2977, ISSN: 2052-1553
Baragau I-A, Buckeridge J, Nguyen KG, et al., 2023, Outstanding visible light photocatalysis using nano-TiO<sub>2</sub> hybrids with nitrogen-doped carbon quantum dots and/or reduced graphene oxide, JOURNAL OF MATERIALS CHEMISTRY A, Vol: 11, Pages: 9791-9806, ISSN: 2050-7488
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- Citations: 1
de Tomas C, Alabidun S, Chater L, et al., 2023, Doping carbon electrodes with sulfur achieves reversible sodium ion storage, JOURNAL OF PHYSICS-ENERGY, Vol: 5, ISSN: 2515-7655
Xu Y, Titirici M, Chen J, et al., 2023, 2023 roadmap for potassium-ion batteries, JOURNAL OF PHYSICS-ENERGY, Vol: 5, ISSN: 2515-7655
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- Citations: 5
Li F, Guo Z, Song Z, et al., 2023, Ultrafast synthesis of battery grade graphite enabled by a multi-physics field carbonization, CHEMICAL ENGINEERING JOURNAL, Vol: 461, ISSN: 1385-8947
Xie H, Xie R, Zhang Z, et al., 2023, Achieving highly selective electrochemical CO2 reduction to C2H4 on Cu nanosheets, JOURNAL OF ENERGY CHEMISTRY, Vol: 79, Pages: 312-320, ISSN: 2095-4956
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- Citations: 6
Barrio J, Pedersen A, Sarma SC, et al., 2023, FeNC Oxygen Reduction Electrocatalyst with High Utilization Penta-Coordinated Sites, ADVANCED MATERIALS, Vol: 35, ISSN: 0935-9648
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- Citations: 7
Madhu R, Periasamy AP, Schlee P, et al., 2023, Lignin: A sustainable precursor for nanostructured carbon materials for supercapacitors, CARBON, Vol: 207, Pages: 172-197, ISSN: 0008-6223
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- Citations: 7
Mercer MP, Nagarathinam M, Gavilan-Arriazu EM, et al., 2023, Sodiation energetics in pore size controlled hard carbons determined <i>via</i> entropy profiling, JOURNAL OF MATERIALS CHEMISTRY A, Vol: 11, Pages: 6543-6555, ISSN: 2050-7488
Westhead O, Barrio J, Bagger A, et al., 2023, Near ambient N<sub>2</sub> fixation on solid electrodes versus enzymes and homogeneous catalysts (vol 7, pg 184, 2023), NATURE REVIEWS CHEMISTRY, Vol: 7, Pages: 225-225
Westhead O, Barrio J, Bagger A, et al., 2023, Near ambient N2 fixation on solid electrodes versus enzymes and homogeneous catalysts, Nature Reviews Chemistry, Vol: 7, Pages: 184-201, ISSN: 2397-3358
The Mo/Fe nitrogenase enzyme is unique in its ability to efficiently reduce dinitrogen to ammonia at atmospheric pressures and room temperature. Should an artificial electrolytic device achieve the same feat, it would revolutionise fertilizers and even provide an energy dense, truly carbon-free fuel. This Review provides a coherent comparison of recent progress made in dinitrogen fixation on (i) solid electrodes, (ii) homogeneous catalysts and (iii) nitrogenases. Specific emphasis is placed on systems for which there is unequivocal evidence that dinitrogen reduction has taken place. By establishing the cross-cutting themes and synergies between these systems, we identify viable avenues for future research.
Chen Y, Li F, Guo Z, et al., 2023, Sustainable and scalable fabrication of high-performance hard carbon anode for Na-ion battery, JOURNAL OF POWER SOURCES, Vol: 557, ISSN: 0378-7753
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- Citations: 4
Spry M, Westhead O, Tort R, et al., 2023, Water increases the Faradaic selectivity of Li-mediated nitrogen reduction, ACS ENERGY LETTERS, Vol: 8, Pages: 1230-1235, ISSN: 2380-8195
The lithium-mediated system catalyzes nitrogen to ammonia under ambient conditions. Herein we discover that trace amount of water as an electrolyte additive─in contrast to prior reports from the literature–can effect a dramatic improvement in the Faradaic selectivity of N2 reduction to NH3. We report that an optimal water concentration of 35.9 mM and LiClO4 salt concentration of 0.8 M allows a Faradaic efficiency up to 27.9 ± 2.5% at ambient pressure. We attribute the increase in Faradaic efficiency to the incorporation of Li2O in the solid electrolyte interphase, as suggested by our X-ray photoelectron spectroscopy measurements. Our results highlight the extreme sensitivity of lithium-mediated N2 reduction to small changes in the experimental conditions.
Tort R, Westhead O, Spry M, et al., 2023, Nonaqueous Li-mediated nitrogen reduction: taking control of potentials, ACS Energy Letters, Vol: 8, Pages: 1003-1009, ISSN: 2380-8195
The performance of the Li-mediated ammonia synthesis has progressed dramatically since its recent reintroduction. However, fundamental understanding of this reaction is slower paced, due to the many uncontrolled variables influencing it. To address this, we developed a true nonaqueous LiFePO4 reference electrode, providing both a redox anchor from which to measure potentials against and estimates of sources of energy efficiency loss. We demonstrate its stable electrochemical potential in operation using different N2- and H2-saturated electrolytes. Using this reference, we uncover the relation between partial current density and potentials. While the counter electrode potential increases linearly with current, the working electrode remains stable at lithium plating, suggesting it to be the only electrochemical step involved in this process. We also use the LiFePO4/Li+ equilibrium as a tool to probe Li-ion activity changes in situ. We hope to drive the field toward more defined systems to allow a holistic understanding of this reaction.
Westhead O, Spry M, Bagger A, et al., 2023, Correction: The role of ion solvation in lithium mediated nitrogen reduction, Journal of Materials Chemistry A, Vol: 11, Pages: 13039-13039, ISSN: 2050-7488
Correction for ‘The role of ion solvation in lithium mediated nitrogen reduction’ by O. Westhead et al., J. Mater. Chem. A, 2023, https://doi.org/10.1039/D2TA07686A.
Guo Q, Zhao Q, Crespo-Otero R, et al., 2023, Single-Atom Iridium on Hematite Photoanodes for Solar Water Splitting: Catalyst or Spectator?, JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, ISSN: 0002-7863
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- Citations: 7
Li Q, Xu Y, Pedersen A, et al., 2023, Investigating the Role of Fe-Pyrrolic N4 Configuration in the Oxygen Reduction Reaction via Covalently Bound Porphyrin Functionalized Carbon Nanotubes, Advanced Functional Materials, ISSN: 1616-301X
Atomically dispersed iron–nitrogen–carbon catalysts are promised, low-cost, and high-performance electrocatalysts for the Oxygen Reduction Reaction (ORR) in fuel cells. However, most Fe–N–C materials are produced via pyrolysis at a high temperature and it is difficult to characterise the precise Fe–N configurations. This can lead to confusion surrounding the best chemical and coordination environment for Fe and understanding the subsequent ORR mechanisms. In this work, Fe porphyrin is used to produce a specific Fe–N environment, therefore allowing the role and activity of this environment to be studied. Carbon nanotubes (CNTs) are covalently functionalized with iron 5,10,15,20-triphenylporphyrin (FeTPP) motifs via aryl diazonium methodology, enabling the exact role of only the Fe-Pyrrolic N4 configuration of FeTPP in ORR to be studied and better understood. Upon covalent functionalization, a high electrochemical active site density of 1.12 × 1015 sites cm−2, approximately six-fold more than that of noncovalently functionalized samples with 12.7% electrochemical active site. The heightened active site density and superior electrochemical active site utilization (12.7%) lead to the more favorable 4-electron pathway for the ORR. Furthermore, a preliminary discussion regarding the selectivity of the ORR pathway is initiated.
Zhang Y, Miao N, Xin X, et al., 2022, Boosting the photocatalytic performance via defect-dependent interfacial interactions from electrostatic adsorption to chemical bridging, NANO ENERGY, Vol: 104, ISSN: 2211-2855
Titirici M-M, Szilagyi PA, 2022, Hydroxide ion-conducting metal-organic frameworks for anion-exchange membrane applications, MATERIALS ADVANCES, Vol: 3, Pages: 8815-8829
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- Citations: 1
Ng KL, Maciejewska BM, Qin L, et al., 2022, Direct Evidence of the Exfoliation Efficiency and Graphene Dispersibility of Green Solvents toward Sustainable Graphene Production, ACS SUSTAINABLE CHEMISTRY & ENGINEERING, ISSN: 2168-0485
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- Citations: 6
Luo H, Yukuhiro VY, Fernandez PS, et al., 2022, Role of Ni in PtNi Bimetallic Electrocatalysts for Hydrogen and Value-Added Chemicals Coproduction via Glycerol Electrooxidation, ACS CATALYSIS, Vol: 12, Pages: 14492-14506, ISSN: 2155-5435
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- Citations: 4
Wang J, Xu Z, Zhang Q, et al., 2022, Stable Sodium-Metal Batteries in Carbonate Electrolytes Achieved by Bifunctional, Sustainable Separators with Tailored Alignment, ADVANCED MATERIALS, Vol: 34, ISSN: 0935-9648
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- Citations: 1
Latham KG, Edathil AA, Rezaei B, et al., 2022, Challenges and opportunities in free-standing supercapacitors research, APL Materials, Vol: 10, Pages: 1-14, ISSN: 2166-532X
The design of commercial supercapacitors has remained largely unchanged since the 1970s, comprising powdered electrodes housed in rigid metal cylinders or pouches. To power the next generation of integrated technologies, an evolution in supercapacitor materials and design is needed to create multifunctional materials that allow energy storage while imparting additional material properties (e.g., flexibility and strength). Conductive free-standing electrodes produced from fibers or 3D printed materials offer this opportunity as their intrinsic mechanical properties can be transferred to the supercapacitor. Additionally, their conductive nature allows for the removal of binders, conductive agents, and current collectors from the supercapacitor devices, lowering their economic and environmental cost. In this Perspective, we summarize the recent progress on free-standing supercapacitors from new methods to create free-standing electrodes to novel applications for these devices, together with a detailed discussion and analysis on their electrochemical performance and physicochemical and mechanical properties. Furthermore, the potential directions and prospects of future research in developing free-standing supercapacitors are proposed.
Barrio J, Pedersen A, Favero S, et al., 2022, Bioinspired and Bioderived Aqueous Electrocatalysis, CHEMICAL REVIEWS, ISSN: 0009-2665
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- Citations: 9
Beaucamp A, Muddasar M, Amiinu IS, et al., 2022, Lignin for energy applications - state of the art, life cycle, technoeconomic analysis and future trends, GREEN CHEMISTRY, Vol: 24, Pages: 8193-8226, ISSN: 1463-9262
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- Citations: 51
Martin-Martinez FJ, Yeo J, Ryan JW, et al., 2022, Editorial: Biobased nanomaterials: New trends and applications, FRONTIERS IN CHEMISTRY, Vol: 10, ISSN: 2296-2646
Li AY, Pedersen A, Feng J, et al., 2022, From haemoglobin to single-site hydrogenation catalyst, Green Chemistry, Vol: 24, Pages: 7574-7583, ISSN: 1463-9262
Iron-based single-site catalysts hold immense potential for achieving highly selective chemical processes, with the added advantage of iron being an earth-abundant metal. They are widely explored in electrocatalysis for oxygen reduction and display promising catalytic activity for organic transformations. In particular, FeNx@C catalysts are active for the reduction of nitroarene into aromatic amines. Yet, they are difficult to mass-produce, and most preparation methods fail to avoid single site aggregation. Here we prepared FeNx@C catalysts from bio-derived compounds, xylose and haemoglobin, in a simple two-step process. Since haemoglobin naturally contains FeNx single-sites, we successfully repurposed them into hydrogenation catalytic centers and avoided their aggregation during the preparation of the material. Their single-site nature was demonstrated by aberration-corrected transmission electron microscopy and X-ray absorption techniques. They were shown to be active for transfer hydrogenation of nitroarenes into anilines, with excellent substrate selectivity and recyclability, as demonstrated by the preserved yield across seven catalytic cycles. We also showed that FeNx@C could be used to prepare 2-phenylbenzimidazole through a reduction/condensation tandem. Our work shows for the first time the viability of biomass precursors to prepare Fe single-site hydrogenation catalysts.
Olsson E, Cottom J, Alptekin H, et al., 2022, Investigating the Role of Surface Roughness and Defects on EC Breakdown, as a Precursor to SEI Formation in Hard Carbon Sodium-Ion Battery Anodes, SMALL, Vol: 18, ISSN: 1613-6810
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- Citations: 1
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