This article presents the development and characterization of a tilted fiber Bragg grating (TFBG) hydrogen sensor functionalised with a nanometre-scale multilayer thin film stack comprising tantalum (Ta), palladium-gold (Pd0.6Au0.4), and polytetrafluoroethylene (PTFE). Ta is introduced as a novel optical fiber sensing material for hydrogen detection, offering unique advantages in sensitivity, reversibility, and hysteresis-free behavior. The optical design of the TFBG ensures efficient coupling to cladding modes, enabling a stable and repeatable hydrogen-induced spectral response when coated with Ta. The sensor was tested over a wide hydrogen concentration range from 0.001% to 100% H ₂ at room temperature. Experimental results demonstrate a measurable and reversible optical response in the mean center wavelength of the cladding mode resonances, averaged over the 1520–1580-nm spectral envelope, with a minimum detection limit of 0.001% (~10 ppm) H ₂ and a maximum mean wavelength shift of approximately 15 pm at 100% H ₂. The Ta coating provides excellent optical performance, characterized by an absence of hysteresis and a large, nearly constant relative sensitivity across an exceptionally wide sensing range spanning at least five orders of magnitude in hydrogen concentration. Sensor stability and repeatability were further confirmed through extended cycling between 0.1% and 4% H ₂, validating the robustness of the cladding mode response. These results highlight both the unique TFBG-based optical architecture and the role of Ta as a highperformance coating, supporting the potential of the Ta-TFBG sensor for sensitive, low-level hydrogen detection in aerospace and energy applications.

Thin film metal hydrides have traditionally been studied (as a model system) for hydrogen storage applications. Meanwhile, other applications including optical switchable mirrors, optical hydrogen sensors, and the use of thin film metal hydrides to study diffusion have emerged. From a more fundamental point of view, surface effects and the fact that thin film metal hydrides have to obey constraints on their volumetric expansion which may lead to high internal stresses. This ensures that thin film metal hydrides may have a significantly different response to hydrogen as their bulk counter parts. This can lead to fascinating phenomena such as suppression of phase transitions, altering the nature of phase transitions and shifting of plateau pressures. This chapter discusses the thermodynamics of thin film metal hydrides, common experimental techniques, and several thin film metal hydrides grouped by application. First, we discuss thin film metal hydrides for hydrogen storage applications focussing on magnesium and magnesium alloys. Next, we consider switchable mirrors based on rare-earth metal hydrides. Third, we discuss metal hydrides including palladium-based and tantalum-based materials for hydrogen sensing applications. In addition, we discuss experimental techniques including hydrogenography and neutron reflectometry that are specifically suited to studying metal hydride thin films as well as how thin film metal hydrides can be applied to study hydrogen diffusion.

Palladium hydride is a model system for studying metal-hydrogen interactions. Yet, its bulk electronic structure has proven difficult to directly probe, with most studies to date limited to surface-sensitive photoelectron spectroscopy approaches. This work reports the first in situ ambient-pressure hard X-ray photoelectron spectroscopy (AP-HAXPES) study of hydrogen incorporation in Pd thin films, providing direct access to bulk chemical and electronic information at elevated hydrogen pressures. Structural characterization by in situ X-ray diffraction and neutron reflectometry under comparable conditions establishes a direct correlation between hydrogen loading, lattice expansion, and electronic modifications. Comparison with density functional theory (DFT) reveals how hydrogen stoichiometry and site occupancy govern the density of occupied states near the Fermi level. These results resolve long-standing questions regarding PdH and establish AP-HAXPES as a powerful tool for probing the bulk electronic structure of metal hydrides under realistic conditions.

Nanoconfined water exhibits unique properties compared to bulk water due to limited quantities, frustrated hydrogen bonding, and surface interactions, which are fundamental for energy storage and transport applications. We integrate machine learning–accelerated ab initio molecular dynamics with x-ray diffraction (XRD) and inelastic neutron scattering (INS) to systematically analyze the thermodynamic and dynamic behavior of water confined between functionalized (-F, -O, and -OH) two-dimensional (2D) Ti₃C₂T_x MXene layers. As water intercalates between layers, the interlayer spacing exhibits layer-dependent staging characteristics. The water polarization can be flipped by the count and morphology of intercalated molecules interacting with MXene surface groups, resulting in varying electrostatic potential profiles. On the basis of interfacial electrostatic potential, hydrogen bond lifetime, and molecular orientation, we establish a linear combination of exponential model describing water diffusivity. These computational insights align well with experimental x-ray and neutron measurements, suggesting strategies for tuning water morphology and transport by tailoring MXene surface chemistry and water content for electrochemical energy storage and nanofluidic applications.

All-solid-state batteries have great potential to outperform conventional lithium-ion batteries in both safety and energy density, as the solid electrolyte can potentially accommodate high-energy-density anodes such as metallic lithium or silicon more safely. However, the high-valence cations present in most highly conductive solid electrolytes facilitate reductive decomposition at low potentials, leading to significant irreversible lithium inventory loss. Preventing this requires the development of solid electrolytes that are thermodynamically stable at low operating potentials while providing high ionic conductivity and sufficient oxidative stability. To realize this, we explored a new family of Li-rich antifluorite irreducible solid electrolytes, Li2.65S0.35NxP0.65–x, the first reported nitrido-phosphido-sulfide, and investigated their application in all-solid-state batteries. The optimized composition Li2.65S0.35N0.15P0.5 possesses a remarkably high ionic conductivity of 1.05 mS cm–1, as well as a relatively high oxidative stability of 1.15 V vs Li+/Li for this class of materials. Ab initio molecular dynamics and density functional theory simulations reveal that enhanced Li diffusion is the result of enlarged diffusion bottleneck sizes. These are a consequence of (i) substitution with smaller anions or (ii) increased electrostatic repulsion from the substitution with high-valence anions. Importantly, the oxidative stability makes Li2.65S0.35N0.15P0.5 exhibit good compatibility with Si anodes, and in conjunction with the high ionic conductivity, this enables a high initial Coulombic efficiency of 94.2% as well as a stable cycle life of a full cell with a micron silicon–Li2.65S0.35N0.15P0.5 anode and a LiCoO2–Li3InCl6 cathode. This work highlights the potential of irreducible solid electrolytes for the design of all-solid-state batteries with low-potential and high-energy-density anodes.

Hydrogen is a cornerstone of the emerging net-zero carbon economy, and its widespread deployment demands sensitive, stable, and scalable detection technologies. In this study, we present a comparative performance analysis of Fibre Bragg Grating (FBG) sensors coated with nanometre-thick metal hydride-forming layers—tantalum (Ta), tantalum-palladium alloy (Ta_0.88 Pd_0.12), palladium (Pd), and palladium-gold alloy (Pd _0.6 Au_0.4)—for optical hydrogen sensing. The integration of Ta and Ta _0.88 Pd_0.12, two tantalum-based metal hydrides, with FBG sensors is introduced here for the first time, offering a promising alternative to conventional Pd-based materials. All coatings were deposited via magnetron sputtering and tested under controlled hydrogen exposure across concentrations ranging from 0.001% to 100% H₂. The Ta-based FBGs exhibited outstanding performance, showing a remarkably linear relative wavelength shift over the full tested range (0.001% to 100% H₂), with sensitivity detectable down to 10 ppm—the lowest concentration achievable in the current setup. Both Ta and Ta_0.88 Pd_0.12 sensors exhibited fully reversible and hysteresis-free response characteristics, with rapid response and recovery. Among them, the Ta_0.88 Pd_0.12 sensor with a 100 nm coating demonstrated the highest logarithmic sensitivity of ∼9 pm/decade(%H₂), corresponding to a 9 pm wavelength shift for every tenfold increase in hydrogen concentration between 0.001% and 100% H₂. In contrast, Pd and Pd _0.6 Au_0.4 sensors showed degraded performance at low concentrations and greater signal hysteresis. These results underscore the potential of Ta and Ta _0.88 Pd_0.12 coatings as robust and high-performance alternatives to conventional Pd-based materials for next-generation distributed fibre-optic hydrogen sensing systems.

All-solid-state batteries receive ample attention due to their promising safety characteristics and energy density. The latter holds true if they are compatible with next-generation high-capacity anodes, but most highly ion-conductive solid electrolytes decompose at low operating potentials, leading to lithium loss and increased cell resistances. Here the dynamic stability of solid electrolytes that can improve all-solid-state battery performance is demonstrated. Halide electrolytes Li₃YCl₃Br₃ and Li₂ZrCl₆, considered unstable at low potentials, are found to exhibit structurally reversible redox activity beyond their electrochemical stability windows, increasing compatibility with anodes and contributing to capacity without compromising ionic conductivity. The benefit of this dynamic stability window is demonstrated with cost-effective red phosphorus anodes, resulting in high reversible capacities (2,308 mAh g⁻¹), high rate capacity retention (1,024 mAh g⁻¹ at 7.75 mA cm⁻²) and extended cycle life (61% retention after 1,780 cycles). Furthermore, high areal capacity (7.65 mAh cm⁻²) and stability (70% retention after 1,000 cycles) are achieved for halide-based full cells with red phosphorous anodes. The beneficial redox activity of halide electrolytes greatly expands their application scenarios and suggests valuable battery design principles to enhance performance.

One of the major challenges in advancing polymer-inorganic hybrid solid electrolytes (HSEs) lies in comprehending and controlling their internal structure. In addition, the intricate interplay between multiple phases further complicates efforts to establish the structure-property relationships. In this study, by introducing a multifunctional LiI additive to an HSE compromising of polyethylene oxide (PEO) polymeric electrolyte and the fast lithium-ion conductor Li₆PS₅Cl, the relationship between the bulk and interface structure and ascertaining their impact on lithium-ion dynamics within the HSE is disentangled. Using multidimensional solid-state nuclear magnetic resonance, we find that the addition of LiI stabilizes the internal interfaces and enhances lithium-ion mobility. A kinetically stable solid-electrolyte interphase is formed at the lithium-metal anode, increasing the critical current density to 1.3 mA cm⁻², and enabling long-term stable cycling of lithium symmetric cells (>1200 h). This work sheds light on tailoring the structure of HSEs to improve their conductivity and stability for enabling all-solid-state lithium-metal batteries.

Optical hydrogen sensors have the power to reliably detect hydrogen in an inherently safe way, which is crucial to ensure safe operation and prevent emissions of hydrogen as an indirect greenhouse gas. These sensors rely on metal hydride material that can reversibly absorb hydrogen when it is present in the environment, and as a result, change their optical properties. To apply this technology along hydrogen infrastructure, in hydrogen-powered planes and other vehicles, it is crucial that these sensors can operate down to −60 °C, a challenge so far unaddressed. Here, it is showed that metal hydride hydrogen sensing materials can be used to detect hydrogen optically down to −60 °C in just a couple of seconds and across a hydrogen concentration range of 0.02–100% with a 1% change in transmission per order of magnitude change in hydrogen concentration. The in-situ X-ray diffraction and optical transmission measurements show that Ta, Ta₈₈Pd₁₂, Ta₈₈Ru₁₂, and Pd₆₀Au₄₀ can gradually, reversibly and hysteresis-free absorb hydrogen while providing sufficient optical contrast. Specifically, Ta₈₈Ru₁₂ possesses the largest optical contrast and the swiftest response down to 6 s at −60 °C. These results confirm the operational viability and foretell new applications of metal hydride hydrogen sensing in cold conditions.

Here, we show that we can synthesize free-standing palladium nanoparticles with a size of about 5 nm embedded in a fluorinated polymer matrix using magnetron codeposition and a subsequent annealing step. Indeed, we deposit with magnetron sputtering at the same time PTFE and Pd, and a subsequent thermal annealing step under a hydrogen atmosphere ensures agglomeration of the Pd atoms into small nanoparticles. This scalable vapor-based method allows deposition on all kinds of surfaces, including substrates and optical fibers. Using a combination of transmission electron microscopy, grazing-incidence diffraction, neutron and X-ray reflectometry, and X-ray photoelectron spectroscopy, we characterize the nanocomposite films and the palladium particles inside. These palladium nanoparticles could have a variety of applications in catalysis, hydrogen compressors, and optical hydrogen sensors. For the later application, we show using optical transmission measurements that the nanoparticles can reversibly absorb hydrogen, having well-defined steps in optical transmission when the hydrogen pressure is changed. Owing to their small size, the polymer matrix, and high surface-to-volume ratio, the nanoparticles show subsecond response times to changes in hydrogen concentration.

Anode-free aqueous zinc metal batteries (AZMBs) offer significant potential for energy storage due to their low cost and environmental benefits. Ti₃C₂T_x MXene provides several advantages over traditional metallic current collectors like Cu and Ti, including better Zn plating affinity, lightweight, and flexibility. However, self-freestanding MXene current collectors in AZMBs remain underexplored, likely due to challenges with Zn deposition reversibility. This study investigates the combination of a Ti₃C₂T_x self-freestanding film with advanced electrolyte engineering, specifically examining the effects of Li-salt and propylene carbonate (PC) as additives on Zn plating reversibility. While using Li⁺ ions as an additive alone facilitates uniform Zn deposition on bulk metals through the electrostatic shielding effect, the addition of Li-salt negatively impacts Zn plating uniformity on Ti₃C₂T_x. Meanwhile, using PC additive alone forms an organic SEI layer on Ti₃C₂T_x and causes Zn agglomeration. The use of both additives together results in a ZnF₂-containing hybrid SEI layer with improved interfacial kinetics, promoting more uniform Zn deposition. This approach achieves an average Coulombic efficiency (CE) of 96.8% over 150 cycles (a maximum CE of 97.8%). The study highlights the strategic difference in electrolyte design, emphasizing the need for tailored approaches to optimize Zn deposition on MXenes, contrasting with traditional metallic current collectors.

Optical hydrogen sensors based on metal hydrides have distinct advantages over other types of hydrogen sensors as they can be made small, do not require the presence of oxygen, and have a large sensing range. The working principle is based on the fact that when exposed to an atmosphere containing hydrogen, a metal hydride absorbs hydrogen, which in turn changes the optical properties. In a micro-mirror configuration, this change in optical properties can be measured by measuring the reflectivity of light. Tantalum alloys have been identified as suitable sensing material owing to their large sensing range, hysteresis-free response and fast response times. Here, we rationally develop a micro-mirror hydrogen sensor based on a tantalum-alloy as sensing layer. We first study the optical contrast of Ta_0.88Pd_0.12 thin films with a Pd_0.6Au_0.4 catalyst layer deposited on substrates with various catalyst and sensing layer thicknesses in reflection. Modeling the experimental results shows that the total optical contrast, that is the change of the reflectivity with a changing hydrogen concentration, is a strong interplay of wavelength and hydrogen-concentration dependent reflection, attenuation and amplification coefficients of both the Ta_0.88Pd_0.12 thin films with a Pd_0.6Au_0.4 catalyst layer. These effects may either constructively or destructively contribute to the overall signal, making carefully choosing the wavelength and layer thicknesses essential. Using optimal values of the wavelength and layer thicknesses, we successfully construct and test a micro-mirror sensor that can detect hydrogen over at least 5 orders of magnitude in hydrogen concentration without any hysteresis.

The development of reliable hydrogen sensing materials for subzero environments is crucial for aviation, cryogenic storage, and hydrogen infrastructure applications. In this study, we investigate tetragonal β-tantalum (β-Ta) thin films at −60 °C to assess their potential for optical hydrogen sensing. In situ X-ray diffraction (XRD) measurements reveal a reversible lattice expansion upon hydrogen exposure, with β-Ta exhibiting a smaller volumetric expansion compared to α-Ta, indicating lower hydrogen solubility. Optical transmission measurements demonstrate a monotonic and fully reversible optical response across a range of hydrogen pressures, free of any hysteresis. However, β-Ta exhibits prolonged response times at low temperatures due to diffusion-limited kinetics, as confirmed by power-law response rate analysis and direct diffusion front measurements. Although β-Ta offers a temperature-independent resolution and structural robustness, its slower response time suggests the need for further microstructural optimizations to enhance hydrogen diffusion.

Hydrogen, a key component of a net-carbon free society, requires precise sensing solutions. This research focuses on the development of metal hydride-coated Fibre Bragg Grating (FBG) based hydrogen sensors, marking a significant step towards the realisation of multipoint hydrogen sensing systems - a growing demand in the industry. The performance of three FBG sensors coated with nanometre-thick tantalum, palladium, and palladium-gold hydrogen sensing metal thin films, deposited via magnetron sputtering, is presented. Among these, the novel tantalum sensor exhibited the best performance, achieving a minimum detection limit of 50 ppm and and an enhanced sensitivity below 0.1% H₂ levels at room temperature.