Electrochemical hydrogen production is central to future renewable energy systems, yet conventional water electrolyzers tightly couple electricity supply and hydrogen generation, limiting operational flexibility and increasing system cost. Decoupled water electrolysis offers an alternative architecture by separating the hydrogen and oxygen evolution reactions in time or space, enabling simultaneous energy storage and on-demand hydrogen production. A promising implementation is the Zn-H2 hybrid electrolysis concept, where water oxidation is coupled to zinc deposition during charging and hydrogen evolution occurs during discharge. However, its viability critically depends on bifunctional gas-evolving electrodes capable of repeatedly switching between the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in highly alkaline, zinc-containing electrolyte, an extreme and largely unexplored regime. Here we report robust, noble-metal-free catalyst coatings based on transition-metal-modified steel that enable stable HER <-> OER cycling under realistic Zn-H2 electrolysis conditions. By systematically comparing electrodeposition and microwave-assisted solvothermal synthesis, we identify nanostructured cobalt coatings grown directly on low-carbon steel as a highly active and durable bifunctional catalyst platform. These electrodes sustain catalytic activity during repeated HER/OER switching and maintain performance even in concentrated alkaline electrolyte saturated with ZnO, where conventional coatings rapidly degrade. Electrochemical measurements during cycling indicate dynamic changes in catalytic behavior, while ex situ surface characterization before and after HER and OER operation reveals the formation of a cobalt oxyhydroxide phase associated with OER activity alongside metallic cobalt sites that promote HER. This combination enables efficient bifunctional operation. The optimized electrodes show strong resistance to dissolution and minimal susceptibility to zinc interference. These findings establish a scalable catalyst design strategy for decoupled Zn-H2 electrolysis and demonstrate stable bifunctional electrocatalysis under realistic Zn-rich alkaline cycling conditions, advancing integrated hydrogen production and electrochemical energy storage technologies.

The development of platinum-group-metal (PGM)-free electrodes is essential for cost-effective alkaline water electrolysis. Herein, we report steel-based electrodes for a fully PGM-free, ionomer-free anion exchange membrane water electrolyzer (AEMWE). A Ni layer deposited on stainless steel (ss) was modified via hydrothermal NiMo growth followed by reductive annealing, yielding a hierarchical NiMo@ss catalyst. Structural characterization revealed MoO2-derived needle-like structures decorated with metallic Ni and intimate NiMo interfaces. In 0.1 M KOH, the catalyst exhibited an overpotential of -70 mV at -10 mA cm-2 with an apparent Tafel slope of 132 mV dec-1, demonstrating significantly improved hydrogen evolution reaction kinetics compared to bare stainless steel and electrodeposited Ni. Oxygen evolution reaction (OER) activity of the porous transport layer was enhanced via a simple Ni deposition and anodization procedure, resulting in an overpotential of 284 mV at 10 mA cm-2. Integration of both electrodes into a PGM-free AEMWE single cell (5 × 5 cm2) enabled a current density of 1 A cm-2 at 1.92 V in 1 M KOH at 60 °C. The cell further demonstrated stable operation for 60 h under dynamic conditions cycling between 0.1 and 1 A cm-2. These results highlight the potential of engineered steel-supported electrodes for scalable noble-metal-free hydrogen production.

Cu 2 O nanocubes coated with porous covalent organic framework (COF) layers enable efficient and selective electrochemical CO 2 reduction to C 2+ products. The Cu@COF core–shell catalysts show high activity, good current density and enhanced stability.

Development of efficient electrocatalyst materials for performing both the oxygen evolution reaction (OER) and the electrochemical oxidation of ethylene glycol (EGOR) is crucial for advancing energy-efficient electrolysis and valorization of plastic waste-derived chemicals. In this study, we present a comprehensive investigation of self-supported Ni-based catalysts grown on nickel foam and systematically tuned with Mn, Fe, Co, and Pd to achieve controllable bifunctional activity. Among these materials, Fe-NiO x H y exhibits superior OER performance in 1 M KOH, delivering an overpotential of 250 ± 7 mV at 100 mA cm-2 with a Tafel slope of 35 ± 2 mV/dec. Hierarchical architectures and their crystal structure, confirmed by scanning electron microscopy and X-ray diffraction, provide abundant active sites and enhance mass transport kinetics. Quasi in situ Raman spectroscopy and ex situ X-ray photoelectron spectroscopy reveal potential, reactant concentration and activation-dependent reconstruction of metal active sites, demonstrating how controlled tuning of metal oxidation states affects both OER activity and EGOR selectivity. Electrochemical activation enhances the valence of metal centers, enabling precise control over EGOR product selectivity. Pd incorporation stabilizes *C2 intermediates, favoring glycolate formation at low anodic potentials, while Mn-, Fe-, and Co-modified Ni promote a *C1 pathway leading to formate at relatively higher potentials, with Fe-NiO x H y achieving a Faradaic efficiency (FE) of up to 86.2% toward formate. In contrast, Pd-NiO x H y /NF delivers a glycolate FE of up to 92.5%. Optimized reaction conditions, including applied potential, EG concentration, and activation protocol, allow selective production of either glycolate or formate during EGOR. This work provides an active site and mechanistic understanding connecting catalyst composition, activation, and oxidation-state dynamics to selectivity, providing a detailed insight for integrating PET-derived EG valorization with energy-efficient hydrogen production.

ABSTRACT Transition metal nitrides (TMNs) are attractive for cutting‐edge energy storage technology, especially emerging lithium–sulfur (Li–S) batteries, owing to their electronic structures resembling those of noble metals. Herein, we unveil the underlying mechanism by which TMNs accelerate reaction kinetics, showcasing two nanostructured TMNs (Mo2N and VN) embedded within tailored carbon architectures. A novel, unexplored self‐nitriding approach was developed to synthesize TMNs with precisely controlled solid (sC) or hollow (hC) carbon architectures, achieved through a colloidal route using imidazolium‐based poly(ionic liquid) (PIL) nanoparticles as both a nitrogen‐rich template and morphology‐directing agent. Compact TMN architectures as sulfur hosts enhance ion diffusion and reaction kinetics, enabling efficient active site access and delivering high performance, such as VN@sC with high initial capacity of 792 mAh g−1 at 2 C and cyclability up to 650 cycles. Meanwhile, hollow architectures (VN@hC and Mo2N@hC) featuring hierarchical porous structures serve as cathode electrocatalytic additives, enabling high sulfur loading and delivering an initial capacity of 1143 mAh g−1 at 0.1 C. Remarkably, this performance is achieved with only 5 wt% additive content in scalable 7.9 × 11 cm2 and 12‐layer pouch cells designed for drone power systems.

The electrochemical reduction of CO2 (CO2RR) to C2+ products offers a sustainable approach for carbon utilization and the production of valuable chemicals. Cu2O nanocubes (NCs) have emerged as effective electrocatalysts for the formation of C2+ products. In this study, we applied a coating of Cu2O NCs with robust covalent organic framework (COF) layers prepared by multicomponent reactions. Compact layers of COFs are formed, which, due to their porosity, allow full accessibility of the Cu2O catalytic surfaces to CO2 molecules. Furthermore, the thickness and chemical functionality of the COF layers can be continuously varied by changing the type and quantity of monomers used to cover the Cu2O NCs. Electrocatalytic measurements demonstrate that these hybrid core-shell Cu@COF systems remain active in CO2 reduction, achieving good current density and faradaic efficiency, while maintaining selectivity for the desired CO2 reduction products. Additionally, the COF shell provides remarkable stability to the system under electrochemical conditions.

This study compares the fiber-matrix bonding of acrylonitrile-styrene-acrylate (ASA) terpolymer reinforced with standard-finish (A1) and adhesion-activated finish (A2) aramid fibers (Twaron (R)) manufactured using an in-situ additive manufacturing (AM) material extrusion technique. A2 fibers showed a slightly higher total surface energy (gamma(s) similar to 49.45 mN/m) compared to A1 fibers (gamma(s) similar to 44.20 mN/m) indicating potentially higher interfacial interaction of A2 fibers with polymer matrix. For single-line manufactured composites, the fiber-matrix bonding performance of the A2-ASA composite improved significantly on increasing the processing temperature from 240 degrees C to 300 degrees C resulting in an increase in ultimate tensile strength (UTS) from 694 MPa to 870 MPa. In contrast, A1-ASA composites showed a reduction in UTS from 674 MPa to 544 MPa over the same temperature. Improved mechanical performance of the composite reinforced with A2 fibers was also observed in the multi-layer manufactured composite, where UTS reached 450 MPa and a Young's modulus of 33 GPa, compared to 426 MPa and 15 GPa for the standard finish fibers. The flexural properties confirm the observed improvements in the mechanical properties of A2-ASA composite. The observation derived from the experimental results indicates that the properties of the fiber surface are crucial for enhancing the fiber-matrix bonding, particularly during the manufacturing process of continuous fiber-reinforced composites utilising material extrusion AM techniques. This ASA-aramid composite can be further exploited as a high-performance composite with improved weatherability for outdoor applications.

Developing low-cost, highly active, and stable catalysts for the acidic oxygen evolution reaction (OER) at the proton exchange membrane (PEM) water electrolyzer anodes remains a scientific priority. Reducing the iridium loading while increasing the intrinsic activity of the catalysts is essential for cost-effective hydrogen production. Here, we address a family of TiO2-supported Raney-IrO x catalysts with low iridium loading and high activity in single-cell PEM water electrolyzer anode environments. A controlled Raney-type Ni leaching process of pristine, supported IrNi alloy phases forms crystalline IrO x nanoparticles (NPs) featuring metallic Ir-rich cores surrounded by more amorphous IrO x surfaces. This structure is shown to be conducive to catalytic activity and the suppression of membrane poisoning due to Ni degradation. The trace amounts of Ni remaining after leaching in the IrO x NPs result in heterogeneous crystal structure and induce local lattice strain. Further, we synthetically strike a balance between conductivity and activity and succeed to narrow down the notorious large performance gap between liquid electrolyte rotating disk electrodes (RDEs) and single-cell membrane electrode assembly (MEA) electrolyzer measurements. OER stability numbers (S-numbers) of the identified Raney-IrO x anode catalysts surpass commercial IrO2 catalysts, confirming the stability of these catalysts. The PEM electrolyzer tests reveal that Raney-IrO x anodes achieve 3 A cm-2 at 1.8 V with a low geometric Ir loading of ca. 0.3 mgIr cm-2, meeting the technically important power specific Ir utilization target of 0.05 gIr/kW.

The development of efficient and environmentally-friendly technologies for green hydrogen production is essential to achieve the net-zero emission scenario by 2050. Specifically, Proton exchange membrane water electrolyzers (PEMWEs) have gained significant attention due to their high efficiency and ability to operate at high current densities. The limited availability and elevated cost of platinum-group metals (PGMs), particularly iridium, which serves as the state-of-art catalyst for the oxygen evolution reaction (OER) at the anode, poses significant barriers to the widespread implementation of PEMWEs technology. Enhancing the intrinsic activity and durability of Ir-based catalysts and lower Ir loadings can directly lower the overall costs and improve efficiency of PEMWEs. Modifying the crystal structures of Ir-based catalysts is a widely explored strategy for boosting their electrochemical performance in OER. In addition to the commonly studied rutile-type IrO₂, other crystal structures such as hollandite-type IrOₓ, perovskite-type IrOₓ, and layered IrOₓ have been investigated as highly efficient OER catalysts. 1-3 In this work, we synthesized a series of alkali cation intercalated iridates. Techniques including transmission electron microscopy (TEM) and X-ray fluorescence (XRF) spectrometer were employed to examine their composition and morphology, while X-ray absorption spectroscopy (XAS) and synchrotron-based wide-angel X-ray scattering (WAXS) were utilized to investigate their geometric and electronic structures. Half-cell tests and full cell tests were performed to explore the relationship between structures and electrochemical performance. We use pair distribution function (PDF) analysis to uncover primary structural changes in both amorphous and crystalline IrO x , which are rarely detectable using other methods. These structural changes play a critical role in balancing the tradeoff between stability and activity. (1) Chen, H.; Shi, L.; Sun, K.; Zhang, K.; Liu, Q.; Ge, J.; Liang, X.; Tian, B.; Huang, Y.; Shi, Z.; et al. Protonated Iridate Nanosheets with a Highly Active and Stable Layered Perovskite Framework for Acidic Oxygen Evolution. ACS Catal. 2022 , 12 (14), 8658-8666. (2) Falling, L. J.; Jang, W.; Laha, S.; Götsch, T.; Terban, M. W.; Bette, S.; Mom, R.; Velasco-Vélez, J.-J.; Girgsdies, F.; Teschner, D.; et al. Atomic Insights into the Competitive Edge of Nanosheets Splitting Water. Journal of the American Chemical Society 2024 , 146 (40), 27886-27902. (3) Zhu, L.; Ma, C.-l.; Cao, L.-m.; Yang, J. 3R-IrO2 Two-Dimensional Nanosheets with Varying Layer Spacing and [IrO6] Distortion for OER. ACS Appl. Energy Mater. 2023 , 6 (9), 4757-4765.

Covalent organic frameworks (COFs) have emerged as promising metal-free sulfur hosts to facilitate the conversion kinetics and suppress the shuttling effect of lithium polysulfides (LiPSs) in lithium-sulfur (Li-S) batteries. However, constructing COFs with stable and high electrocatalytic functionality for LiPS conversion remains unexplored. Herein, we develop a radical-cationic COF (R-TTF•+-COF) with superior electrical conductivity of 3.9 S m-1 at room temperature, which features both nucleophilic and electrophilic sites for effective LiPS chemisorption and conversion. With this novel radical-based catalyst, the Li-S battery achieves superior longevity of 1500 cycles with a capacity fading of 0.027% per cycle at a current density of 0.5 C. The capacity retention of the Li-S battery based on R-TTF•+-COF at the current density of 2.0 C is nearly twice as high compared to a COF without radicals. The crucial role of radical cations in catalyzing LiPS conversion has been systematically elucidated through solid-state nuclear magnetic resonance spectroscopy, electron paramagnetic resonance spectroscopy, and theoretical simulations, which verify the reversible interactions between LiPSs and [TTF]2•+ moieties. This intriguing radical-assisted mechanism opens a new avenue for designing efficient catalytic sulfur hosts using organic molecules, offering a significant step toward the practical application of Li-S batteries.

Core-shell structures offer the unique ability to integrate multiple functionalities within a single nanoparticle (NP), presenting significant potential for the development of advanced catalytic processes. Optimizing such systems requires a fundamental understanding of the structure-performance relations, particularly the impact of spatial configuration on catalytic behavior. In this study, we systematically evaluate a "dragon fruit'' catalyst morphology, in which Pt NPs are uniformly distributed throughout a mesoporous silica shell. This architecture is introduced as an efficient alternative to the "peach" structure, where Pt NPs are concentrated in the center of a core-shell NP. Both morphologies were synthesized via a rational and straightforward two-step approach under identical shell chemistry. The dragon fruit accommodates a significantly higher Pt loading compared to the peach morphology, with comparable particle sizes, surface areas, and surface chemistry. Cyclohexane dehydrogenation was used as a model reaction to evaluate catalytic performance. The dragon fruit structure achieved the highest specific benzene yield per mg of catalyst, while both morphologies exhibited comparable activity per mg of Pt. A qualitative simulation model based on experimental characterization corroborated these results. Comprehensive mass transfer analysis verified the absence of internal and external diffusion limitations under the studied conditions. This assessment further supports that the variation in catalytic performance can be attributed primarily to the ability of the dragon fruit morphology to contain a higher amount of Pt in spatial distribution. These findings underscore the influence of active site configuration and suggest the dragon fruit morphology as a promising and scalable design for next-generation core-shell catalysts.

The osseointegration of the implant material PEEK (polyether ether ketone) regularly represents a challenge due to its inert properties. This in vitro study evaluates the effect of hydrogen/oxygen low-pressure plasma treatment on the soft and hard tissue integration of PEEK. For this, 255 PEEK discs (diameter: 16 mm; thickness: 3 mm) were divided into 7 groups according to different low-pressure plasma treatment durations: 0 min, 1/6 min, 1/ 2 min, 1 min, 4 min, 10 min and 15 min. Afterwards, water contact angle (WCA) was measured to determine the hydrophilicity. Surface roughness and microhardness were measured to characterize the topography and mechanical behavior of the surfaces. X-ray photoelectron spectroscopy was used to determine the effect of plasma treatment on the chemical bonds on the PEEK surfaces. Cell culture tests with immortalized human gingival fibroblasts (iHGFs) were conducted to test the effect of PEEK plasma treatment on the cell adhesion, proliferation, and morphology, while human osteosarcoma cell line (Saos-2) was used to investigate the osteoconductivity. After plasma treatment, the hydrophilicity of PEEK was significantly improved: the WCA of untreated PEEK was 75.72 degrees f 1.31 degrees, while after 10 s of plasma treatment, the WCA decreased to 28 degrees f 2.29 degrees. XPS results showed that plasma treatment introduced hydrophilic groups onto the PEEK surfaces. Cell culture tests confirmed that cell adhesion, proliferation and osteoconductivity were also significantly improved due to low-pressure H/O plasma treatment. Taken together, the study suggests that hydrogen/oxygen low-pressure plasma can effectively improve the biocompatibility for both soft and hard tissue.

Proton exchange membrane fuel cells (PEMFCs) provide efficient, green power solutions. However, the sluggish kinetics of the oxygen reduction reaction (ORR) at the cathode, with its need for elevated Pt loadings, lowers efficiency and raises cost, which hinders their wider implementation. Pt-based designer alloy electrocatalysts, more specifically ternary PtNiX nanocatalysts, hold great potential for improving ORR activity and thus overall cell performance. This study explores synthesis and performance evaluations of novel ternary PtNiIr ORR catalysts prepared using seed-mediation at different catalyst loadings and deposited on various carbon support materials. Membrane electrode assembly (MEA) performance evaluations are carried out to assess catalyst activity and stability under operating conditions, revealing better performance and durability for seed-mediated catalysts compared to the non-seed-mediated catalyst used as a reference. The results showed further improved performance and durability of the seed-mediated catalysts on porous carbon than solid carbon, due to the deposition of catalyst nanoparticles inside the carbon pores. Degradation analysis using online inductively coupled plasma - mass spectrometry (ICP-MS) indicated the dissolution of metals during contact with the electrolyte and under operating conditions, confirming the observed catalyst stability trends in MEA. The experiments highlighted the impact of catalyst composition and supports on the stability of the materials.

Thrifting the rare iridium in proton exchange membrane water electrolyzer (PEMWE) anodes is an effective means to preempt undesired future iridium supply shortages aiding wider deployment of PEMWEs in coming years. This work explores a new family of MnO x ‐supported IrO x and IrRuO x electrocatalysts for the acidic oxygen evolution reaction (OER). Comprehensive ex situ and in situ characterization uncovers synthesis‐structure‐activity relationships of the OER materials with insight into the origin of their exceptional activity: The MnO x support provides beneficial dispersion while the introduction of Ru into IrO x /MnO x leads to a modulation of the chemical state of Ir coupled with a strong surface reconstruction. In half‐cell tests, IrRuO x /MnO x reveals an Ir mass activity of 964.7 A g Ir −1 at 1.53 V RHE , which is 36 times higher than that of the commercial IrO 2 (C‐IrO 2 ). It is also demonstrated that this promising catalytic OER activity translates into a realistic PEMWE performance. IrRuO x /MnO x and IrO x /MnO x thin catalyst layers are developed in low Ir‐loaded membrane electrode assemblies (MEAs) and an outstanding PEMWE cell performance is reported with cell voltages of 1.66 V at 2 A cm −2 . This translates into a favorable (Ir + Ru) platium group metal (PGM) demand of <0.05 g PGM kW −1 at 70% voltage efficiency, meeting a 2035 technical demand target.

Hydrothermal humification (HTH) is an emerging green route for converting biomass into artificial humic substances (A-HS), oxygen-rich macromolecules resembling natural humics and relevant for carbon sequestration and soil improvement. HTH represents the alkaline version of hydrothermal carbonization (HTC), acidic and yielding to insoluble hydrochars. Here, we investigate the pathways behind this transition by treating glucose, cellulose, and lignin at 220 °C for 4 h under controlled concentrations of alkali (KOH). Under HTH, carbohydrates undergo retro-aldol cleavage, yielding low solid yields and lactic acid and aldehydes that condense into phenolic/aromatic A-HS, as shown by solid-state NMR. In contrast, HTC mainly forms furanic hydrochars. Lignin under HTH undergoes near-complete depolymerization/defragmentation (<1.1 % residue), yielding oxygen-rich aromatic A-HS, whereas it remains unreacted under HTC. Overall, the resulting A-HS are aromatic, rich in oxygenated functionalities, and fluorescent, resembling natural HS and highlighting the potential of HTH for producing soil-relevant humics from biomass.

Anionic microporous polymer networks are prepared from a fluorinated tetraarylborate precursor via the Yamamoto reaction. The charge density can be continuously varied by adjusting the ratio of a neutral tetraphenylmethane comonomer. The obtained polymer networks are stable under ambient conditions and exhibit a surface area of up to 1500 m2 g‐1. Cationic molecular complexes can be embedded in the anionic network by simple ion exchange, making them viable for gas phase catalytic reactions. In this case, the cationic complex of the Crabtree’s catalyst is introduced to prepare a solid material for the gas phase hydrogenation of ethylene to ethane at room temperature.

A unique feature of flexible metal-organic frameworks (MOFs) is their ability to respond dynamically towards molecular stimuli by structural transitions, resulting in pore-opening and closing processes. One of the most intriguing modes is the "gating", where the material transforms from the dense to the porous state. The conditions required for the solid phase structural transition are controlled by the kinetic barriers, including nucleation of the new phase commencing on the crystallite's outer surface. Thus, surface deformation may influence the nucleation, enabling deliberate tailoring of the responsivity. In the present contribution, we investigate how chemical surface treatments (surface deformation) affect the gate opening characteristics of a typical representative of gate pressure MOFs, DUT-8(Ni) ([Ni2(ndc)2(dabco)] n , ndc = 2,6-naphthalenedicarboxylate, dabco = 1,4-diazabicyclo[2.2.2]octane). A combination of various complementary advanced characterization techniques, such as NMR, nanoFTIR, terahertz, in situ XPS, in situ EPR spectroscopies, and inverse gas chromatography, are applied to unravel the changes in surface energy and mechanism of surface deformation.

Lithium-sulfur (Li-S) batteries, known for their high theoretical energy density, have been considered as one of the most promising candidates for next-generation batteries. However, further optimization of their electrochemical performance is often hindered by a sluggish polysulfide conversion process. Recently, amorphous metal-organic frameworks (aMOFs) with numerous unsaturated metal sites have emerged as efficient catalysts, particularly in boosting polysulfide conversion. However, the collapse of the long-range periodic porous structure makes it difficult to access the internal part of micrometer-sized aMOFs, thereby limiting the further improvement of their catalytic activity. Herein, we propose a promising core-shell structure, constructed by using a sustainable halloysite nanotube as a substrate to support aMOF. The triethylamine vapor diffusion method is applied to regulate the kinetics of aMOF growth by modulating the deprotonation of organic ligands, leading to the successful deposition of nanosized aMOF shells onto halloysite nanotubes. This aMOF/halloysite composite structure exhibits better catalytic activity toward polysulfide adsorption and conversion in the Li-S battery when compared with the pure halloysite. In addition, the composite also shows a better cycling performance, retaining a specific capacity of 510 mAh g-1 after 350 cycles at 1.0 C. This work presents an efficient amorphous MOF shell-coating structure as a catalyst in facilitating the process of polysulfide conversion, paving the way for the development of highly active aMOF-based catalysts in the future.

Photocatalytic hydrogen evolution is a direct pathway to store solar energy in chemicals. Conjugated microporous polymers (CMPs) are porous organic photocatalysts, that are typically applied in powder form in heterogenous catalytic reactions. However, the use of powder photocatalysts in dispersion poses some major challenges when it comes to practical applications in larger scales. In this manuscript, the photocatalytic performance of a carbazole-based porous organic polymer (C-POP) film produced by electro polymerizing 1,2,3,5-Tetrakis(carbazol-9-yl)-4,6-dicyanobenzene (4CzIPN) is investigated, well-known for its intriguing photocatalytic properties. The thickness of the intrinsic microporous film is tuneable by the amount of cyclic voltammetry cycles but it is shown that the hydrogen production is not dependent on film thickness. It can therefore be concluded that catalysis is mainly occuring on the outer surface of the films, questioning whether high surface areas are always required for efficient photocatalysis. A microstructured film offers the advantage that, with a reduced amount of polymer material, a constant or even increased external surface area of the film can be achieved. The approach presented here is therefore advantageous for achieving high hydrogen production per unit area with minimal amounts of polymer, as very thin layers are already sufficient for high activity.

Preventing the agglomeration and sintering of catalytically active platinum nanoparticles under reaction conditions is crucial for achieving enhanced catalytic performance, particularly in dehydrogenation processes. This work aims to design a core-sheath structure to protect Pt nanoparticles from agglomeration on a substrate such as ceria (CeO2) and study the performance and stability of Pt nanoparticles under sheath protection. An electrospinning technique was employed to fabricate CeO2 nanofibers (NFs), followed by impregnating Pt and introducing a silica (SiO2) sheath layer to obtain Pt-CeO2@SiO2 core-sheath NFs. The structural, morphological, and physical properties of the resulting materials were evaluated by using X-ray diffraction (XRD), etching depth-profile X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and high-angle annular dark-field high-resolution scanning transmission electron microscopy (HAADF-STEM). The in situ XRD measurement followed by the Rietveld refinement showed the protective effect of the sheath layer against the agglomeration of Pt nanoparticles in Pt-CeO2@SiO2 materials. In the catalytic cyclohexane dehydrogenation (CDH) reaction, Pt-CeO2@SiO2 materials show a 4-fold increase in benzene yield compared to the Pt-CeO2 structure without the sheath layer, with both catalysts exhibiting full selectivity for benzene.