Matthew Roland Hill

Lithium‐sulfur (Li‐S) batteries are attractive for next‐generation energy storage owing to their high theoretical energy density and low cost, yet their practical performance is limited by sluggish redox kinetics. Here, we introduce a soft catalyst in which a polymer‐metal complex is directly integrated into the binder, creating a catalytically active microenvironment that enables efficient and bidirectional sulfur catalysis. A polyvinyl alcohol (PVA) scaffold stabilizes metal ions through chelation with the electron‐donating ‐OH groups of PVA, forming homogeneously distributed catalytic domains in the sulfur cathode. Among the systems investigated, PVA‐Cu exhibits the highest catalytic activity, arising from optimal sulfur binding energies, Cu‐S d‐p hybridization, and additional electronic states near the Fermi level. As a result, the PVA‐Cu cells deliver high capacities at 3 mg cm ⁻² of 1,100 mAh g ⁻¹ at 1 C with 82% capacity retention over 300 cycles, while at higher loadings of 9 mg cm ⁻² , the cells deliver 813 mAh g ⁻¹ (7.3 mAh cm ⁻² ) at 0.5 C. In a pouch cell prototype, stable cycling at 0.5 C delivers a discharge capacity of 790 mAh g ⁻¹ and a power density of 150 W kg ⁻¹ , which lies within the upper range of reported Li‐S pouch‐cell performance in terms of operating rate and power density.

Metal–organic frameworks (MOFs) have emerged as promising candidates for selective gas adsorption due to their tunable structures, high porosity, and numerous open metal sites (OMSs). This research synthesizes and characterizes bimetallic FexCo1–x-MOF-74 frameworks containing both iron (Fe) and cobalt (Co) metal centers to investigate and improve their oxygen (O2) adsorption performances. Monometallic Fe-MOF-74 and Co-MOF-74, as well as bimetallic versions with Fe/Co ratios of 0.1:0.9, 0.5:0.5, and 0.9:0.1, were synthesized by a solvothermal method. A thorough characterization analysis was performed to verify their structural integrity, porosity, thermal stability, and metal composition. O2 adsorption isotherms were assessed at 204, 273, and 298 K to analyze adsorption capacity and temperature-dependent characteristics. Cyclability experiments at 298 K examined the reusability of the materials during multiple adsorption–desorption cycles. Advanced characterization techniques, such as vibrating sample magnetometry (VSM), 57Fe–Mössbauer spectroscopy, and X-ray photoelectron spectroscopy (XPS), unveiled the possible adsorption mechanism. The findings indicate that monometallic Fe-MOF-74 has a significant initial O2 adsorption capacity of 2.58 mmol/g at 298 K due to strong chemisorption at Fe sites. However, its cyclability is poor due to the irreversible oxidation of Fe2+ to Fe3+ at 298 K, resulting in a large drop after the first cycle. In contrast, Co-MOF-74 has a lower initial capacity of 0.36 mmol/g at 298 K, but demonstrates superior reversibility, maintaining consistent performance throughout several cycles owing to weaker, reversible physisorption. Among the bimetallic variants, Fe0.5Co0.5-MOF-74 achieves an optimum balance, exhibiting a moderate initial capacity of 0.82 mmol/g at 298 K and maintaining steady performance of around 0.65 mmol/g over seven cycles. The addition of Co stabilizes the Fe sites against oxidation and improves the material’s reusability. Mechanistic investigations demonstrate that Co mitigates Fe oxidation by facilitating reversible interactions and preventing the formation of irreversible Fe–O2 bonds. The results underscore the promise of bimetallic MOFs as adaptable platforms for effective and sustainable O2 capture, where the Fe/Co ratio can be adjusted to optimize adsorption capacity and cyclability.

Zeolitic imidazolate frameworks (ZIFs) have emerged as promising candidates for high O₂ adsorption capacity, O₂/N₂ selectivity and cyclability due to their tunable chemical and structural properties governed by the selection of organic ligands, metal centres and synthesis methods. Therefore, this research engineers ZIF-7, ZIF-8, ZIF-62 and their mixed-metal derivatives containing cobalt (Co) or iron (Fe) (ZIF-8-derived Fe-mIM where applicable) to improve O₂ adsorption. Because performance metrics trade off, no single ZIF maximised all objectives, and application-specific leads were identified. The highest O₂ capacity was delivered by ZIF-8(Zn : Co = 90 : 10)-MS, reaching 0.35 mmol g⁻¹ with selectivity of 2.01, and 9.9% decrease over 3 cycles. The greatest selectivity was achieved by ZIF-8-derived Fe-mIM material (Zn : Fe = 0 : 100)-MS, giving selectivity of 2.60 at a low adsorption of 0.09 mmol g⁻¹ and 9.6% loss over 3 cycles. The most robust 3-cycle performance was observed for ZIF-8-US, which retained capacity with 0.5% loss while providing 0.26 mmol g⁻¹ and selectivity of 1.06. For a balanced generalist over 3 cycles, ZIF-62-US offered the strongest overall combination, providing 0.34 mmol g⁻¹, selectivity of 1.01, and 1.3% loss. These results underscore the delicate balance among O₂ adsorption performance with structural integrity, coordination chemistry, adsorption characteristics, and cyclability in ZIFs shaped by organic ligand, metal centres, and synthesis method choices.

Lithium–sulfur (Li–S) batteries promise exceptional gravimetric energy densities but are hindered by their poor volumetric performance. This is further exacerbated when taking into account the considerable volume expansion of sulfur during cycling. Intrinsically ion‐diffusion‐limited sulfur cathodes make electrode densification and therefore volumetric energy density a critical challenge. In this work, we introduce a protein‐foamed binder (PFB) that, upon drying, templates cylindrical pores within the cathode. Strategically engineered with high density physical cross‐links, PFB forms a mechanically robust and adhesive binder matrix capable of withstanding significant electrode densification (from 0.51 to 1.62 g cm ⁻³ ), while fully preserving its templated structure. These noncollapsible pores form a network of ion transport channels, enabling excellent sulfur utilization and rate capability despite its high density, delivering 1,361 mAh g ⁻¹ at 0.05C and 625 mAh g ⁻¹ at 4C. This translates to a volumetric capacity of 1,550 mAh cm ⁻³ and volumetric energy density ( E _V ) of 3,285 Wh L ⁻¹ , rivaling state‐of‐the‐art Li–S batteries and surpassing lithium‐ion battery benchmarks even when considering sulfur volume changes. Moreover, we demonstrate high areal loadings of up to 16 mg cm ⁻² , delivering 16.6 mAh cm ⁻² . This work introduces an electrode design philosophy which reconciles high cathode density with efficient ion transport for volumetrically efficient Li–S batteries.

Plastics have revolutionised modern society; however, they have also caused environmental damage via waste accumulation. To balance their advantages with the negative impact on the environment, it is necessary to enhance recycling procedures, since the existing techniques are ineffective, require significant energy consumption, and yield recycled items of poor quality. One promising pathway is to utilise membranes. While membrane technology has been extensively studied in wastewater treatment and organic solvent recovery, its direct application to plastic recycling, particularly using real plastic feedstocks like PET, remains underexplored. This paper aims to address the gap by exploring different plastic recycling technologies, followed by an analysis of the current state of the art and then the prospective integration of membrane technology into plastic recycling processes with an emphasis on PET as a case study. This study provides a forward-looking discussion on some exciting opportunities including using conventional membrane processes and emerging membrane processes. These include separating impurities and additives from the recycling stream, recovery of valuable catalysts, and treating wastewater produced during PET recycling processes. This study also investigates emerging membrane research in PET recycling via use of mixed matrix membranes (MMMs) and implementation of hybrid membrane systems (HMSs). This study also aims to identify current challenges and future opportunities for membrane technology implementation in the field of plastic recycling, considering its impact on recycled product quality, energy consumption, and economic feasibility. Membrane technology is demonstrated to have the potential to transform the plastic recycling industry, and contribute to a more sustainable and circular economy.

Liquid organic hydrogen carriers (LOHCs) are infrastructure‐compatible media for hydrogen storage and transport under ambient conditions, addressing hydrogen's volatility, low density, and high reactivity. Separating liquid hydrogen‐lean/hydrogen‐rich hydrocarbons without resorting to energy‐intensive phase changes is a key barrier to LOHC system implementation. Membrane operations that can separate hydrogen‐lean/hydrogen‐rich species can drive equilibria of dehydrogenation processes, enabling them to run at lower temperatures. Here, new photopolymerized mixed‐matrix membranes composed of a cyclic monomer and a metal organic framework (MOF)/palladium‐doped activated carbon mixture are presented. By leveraging an in situ photopolymerization strategy, high–filler‐loaded mixed‐matrix membranes exhibiting ideal aromatic/aliphatic selectivities of ≈12 and a toluene/methylcyclohexane (MCH) separation factor of 1.8 for membranes with filler loading of 20 wt.% are fabricated. This fabrication approach enables high filler loadings in the monomer and, for multi‐layer films, delivers a stratified structure where it induces the formation of multiple internal polymeric dense “skin” layers, which is ideal for the promotion of selective transport. It is compared that the early studies reported using only commonly reported metrics, rejection versus mixture permeance, with the present system, demonstrating the highest performance to date. This work highlights a high‐performance solvent nanofiltration platform for LOHC separation aligned with sustainable hydrogen production goals.

The concept of non‐Crystalline Metal–Organic Frameworks (MOFs) is both theoretically exciting and rich in potential applications. Since their conceptual introduction, research in this field has experienced significant growth. This review provides a comprehensive overview of the design, synthesis, and applications of non‐crystalline MOFs, highlighting the current state of the art. It examines the fundamental principles of non‐crystalline MOFs, the various synthetic approaches, and the nature of non‐crystalline MOFs. Additionally, the review outlines their pathway from the laboratory to industrial applications, emphasizing challenges and opportunities for further development.

Redox flow batteries show promise for large‐scale grid stabilisation. Of these, organic redox flow batteries (ORFBs) harbour the potential for sustainable and economic operation due to the materials deployed. Their long‐term operation requires exquisite transport control of species across the cell, with movement of cations key for high current density, and anionic rejection needed for cycling stability. Nafion, although promising as a commercial separator, faces cost and sustainability limitations due to its fluorinated nature and per‐ and polyfluroralkyl substances (PFAS) generation. Here, we report the tailored combination of a hydrophilic mixed‐matrix membrane, SPEEK‐SX, with sulphonated polydichloroxylene (S p ‐DCX) as the additive and sulphonated poly(ether ether ketone) (SPEEK) as the matrix. Compared to Nafion‐212, the dense aromatic backbone of SPEEK efficiently rejected the crossover of electrolytes, with sulfonate groups housed within S p ‐DCX micropores increasing Na ⁺ mobility. SPEEK‐SX2 exhibited 190 times higher Na ⁺ / Fe(CN) ₆ ⁴⁻ selectivity and 6 times higher Na ⁺ / 2,6‐DHAQ ²⁻ selectivity compared to Nafion‐212. This enabled stable operation for 600 cycles at a high current density of 160 mA cm ⁻² with only 0.00935% per cycle capacity decay. In contrast, the SPEEK membrane exhibited 0.07% per cycle decay, whereas Nafion‐212 failed to run at this high current density.

The purpose of this study was to design and develop a self-supporting glass MOF membrane (GMM) including its design, fabrication under different heat treatment temperatures, analysis of its physical–chemical properties, and assessment of its separation performance. Glass MOFs preserve metal–ligand bonding structures similar to their crystalline counterparts, providing intrinsic gas separation properties alongside the benefits of amorphous materials, including reduced grain boundaries and ease of processing. In this work, ZIF-62 was melted and then cooled to fabricate GMMs using vitrification to enhance molecular sieving. This study systematically examines the impact of varying thermal treatment temperatures (400–475 °C) on the physical and chemical transformations of GMMs, revealing their effects on the porosity, defect formation, and molecular sieving performance through advanced characterization techniques (e.g., solid-state nuclear magnetic resonance (13C NMR), X-ray photoelectron spectroscopy (XPS), He pycnometry, and positron annihilation lifetime spectroscopy (PALS)). The optimal GMM exhibits an impressive separation performance, particularly for H2 separation. The GMM at 4 bar and 25 °C exhibited He, H2, CO2, N2, and CH4 gas permeations of 576.37, 509.23, 146.07, 3.45, and 2.28 barrer, respectively. The ideal selectivities of H2/CH4, CO2/N2, CO2/CH4, H2/N2, and H2/CO2 gas pairs were 223.47, 42.37, 64.10, 147.71, and 3.49, respectively, which significantly exceed earlier reported values for ZIF-62 membranes, demonstrating the significant potential for GMMs as high-performance molecular sieve membranes, particularly for H2 separation. This work by optimizing the vitrification process through systematic temperature control highlights GMM’s ability to achieve high selectivity and permeability, positioning it as a promising candidate for industrial gas separation applications.