Adjacent Oxygen Research Articles

Amides Enable Room-Temperature CO2 Conversion: Simple Organic Molecules Challenging Metal Catalysts.

The conversion of carbon dioxide (CO2) into valuable chemicals has been intensively pursued for sustainable chemistry. It is highly desirable to achieve the conversion under ambient conditions using organocatalysts instead of precious or pollutive metal catalysts. Herein, we disclose a new class of organocatalysts for direct C(sp)-H carboxylation with CO2. Amide molecules such as N-methylacetamide and valerolactam behave as efficient bifunctional catalysts to promote the conversion of aromatic alkynes to propiolic acids. In particular, the simple organic catalysts enable the reaction to occur at room temperature, which has been achieved only with complex transition metal catalysts prior to this report. In the presence of the optimal base of Cs2CO3, the adjacent nitrogen and oxygen sites of the amide group concurrently activate CO2 and C(sp)-H and position them in favor of C-C coupling, affording a high catalytic activity on par with those of transition metal catalysts. The work sheds new light on the catalytic chemistry of CO2 and also illustrates the great potential of discovering new organocatalysts from simple molecules.

Oxygen Evolution Reaction of Amorphous/Crystalline Composites of NiFe(OH)x/NiFe2O4.

Orbital structures are strongly correlated with catalytic performance, whereas their regulation strategy is still in pursuit. Herein, the Fe 3d and O 2p orbital hybridization was optimized by controlling the content of amorphous NiFe(OH)x (a-NiFe(OH)x), which was grown in situ on crystalline NiFe2O4 (c-NiFe2O4) using an ultrasonic reduction method. The results of electron energy loss spectroscopy (EELS) and X-ray absorption spectra (XAS) revealed that the Fe-Oa orbital hybridization in a-NiFe(OH)x is effectively strengthened by jointing with the adjacent oxygen (Oc) in c-NiFe2O4, which is further confirmed by the higher antibonding orbital energies based on density functional theory (DFT) calculations. The resultant Oa-Fe-Oc at the composite interface leads to balanced adsorption and desorption energies. Accordingly, the optimal composite with strong Fe 3d-O 2p hybridization results in enhanced OER performance, and the overpotential is 150 mV, lower than that of the pristine sample. This work represents a promising approach to orbital hybridization via the introduction of an amorphous phase to construct highly efficient catalysts.

Site-Specific for CO2 Photoreduction with Single-Atom Ni on Strained TiO2-x Derived from Bimetallic Metal-Organic Frameworks.

The photocatalytic reduction of CO2 in water to produce fuels and chemicals is promising while challenging. However, many photocatalysts for accomplishing such challenging task usually suffer from unspecific catalytic active sites and the inefficient charge carrier's separation. Here, a site-specific single-atom Ni/TiO2-x catalyst is reported by in situ topological transformation of Ni-Ti-EG bimetallic metal-organic frameworks. The loading of nickel nanoparticles or individual atoms, which act as specific active sites, can be precisely regulated by chelating agents through the partial removal of nickel and adjacent oxygen atoms. Furthermore, the degree of lattice strain in Ni/TiO2-x catalysts, which improves the separation efficiency of charge carriers, can be modulated by fine-tuning the transformation process. By leveraging the anchored nickel atoms and the strained TiO2, the optimized NiSA0.27/TiO2-x shows a CO generation rate of 86.3 µmol g-1 h-1 (288 times higher than that of NiNPs/TiO2-x) and CO selectivity of up to 92.5% for CO2 reduction in a pure-water system. This work underscores the importance of tailoring lattice strain and creating specific single-atom active sites to facilitate the efficient and selective reduction of CO2.

Rare Earth Selectivity and Electric Potentials at Mica Interfaces.

Controlling materials' composition and structure to selectively adsorb rare earth elements (REE) is critical for better separations. Understanding how local electric potentials affect REE adsorption and how they can be modified via chemical substitution is of fundamental importance. We present calculated mean inner potentials for muscovite and phlogopite micas in excellent agreement with measured values of +10.6 V. Natural substituents for aluminum significantly influence the electric potentials at the basal surface, altering the REE adsorption energies (Ead). Nd3+ adsorption is generally favored over that of Yb3+ on both micas. Substituents with lower charge than aluminum increase the Lewis basicity of adjacent oxygen atom lone electron pairs, enhancing Ead by 20 to 30 kcal/mol. These substitutions modify the electric potential's magnitude and spatial extent, highlighting the role of high-resolution electron holography/tomography and the importance of understanding atomic-scale variations in electric potentials for improving REE cation adsorption and selectivity on micas. In summary, the adsorption energies of REE cations are correlated with the substituent charge and local electrostatic potential variations because these factors dictate the electrostatic interactions between the cations and the interface.

Strain-Induced Antiferroelectric-Ferroelectric-Antiferroelectric Phase Transitions in Epitaxial LaTaO4 Films.

We employed first-principles to delve into the strain-induced structural phase transitions in epitaxial LaTaO4 films. The ground state of bulk LaTaO4 adopts a monoclinic antiferroelectric phase, characterized by the antiphase rotation of two adjacent oxygen octahedra layers. Under epitaxial tensile strain, LaTaO4 thin films undergo a consecutive phase transition, namely, antiferroelectric-ferroelectric-antiferroelectric phase transitions. The ferroelectricity in the orthorhombic phase under tensile strain originates from the in-phase rotation of two adjacent oxygen octahedra layers, in contrast to the case of perovskite systems, in which octahedra rotation suppresses the conventional proper ferroelectricity. With spin-orbit coupling effects, a pronounced Rashba effect at the Brillouin zone center naturally leads to the formation of opposite directions of spin texture. Moreover, the tensile strain also synergistically enhances the corresponding Rashba parameters. Our findings may provide novel insights for controlling oxygen octahedra rotation to achieve control over the ferroelectricity and Rashba effect, which holds promising implications for applications in electronics and spintronics.

Softening of the optical phonon by reduced interatomic bonding strength without depolarization.

Softening of the transverse optical (TO) phonon, which could trigger ferroelectric phase transition, can usually be achieved by enhancing the long-range Coulomb interaction over the short-range bonding force1, for example, by increasing the Born effective charges2. However, it suffers from depolarization effects3,4 as the induced ferroelectricity is suppressed on size reduction of the host materials towards high-density nanoscale electronics. Here, we present an alternative route to drive the TO phonon softening by showing that the abnormal soft TO phonon in rocksalt-structured ultrawide-bandgap BeO (ref. 5) is mainly induced by a substantial reduction in the short-range bonding interaction due to the Be-O bond stretching caused by an electron cloud-overlap-induced Coulomb repulsion between two adjacent oxygen ions that are arranged octahedrally around an extremely small Be ion. We further demonstrate the emergence of robust ferroelectricity in strain-induced perovskite BaZrO3 and ultrathin HfO2 and ZrO2 films6,7 grown epitaxially on lattice-mismatched SiO2/Si substrate arising from the softening of the TO phonon driven by a reduction in the short-range bonding strength of biaxial strain-induced stretching bonds. These findings shed light on developing a unified theory for ferroelectricity enhancement in ultrathin films free from depolarization fields by tailoring chemical bonds using ionic radius differences, strains, doping and lattice distortions.

Boron-doped carbon dots with time-resolved room temperature phosphorescence for detection of ciprofloxacin hydrochloride and information encryption applications.

Novel boron-doped carbon dots (BCDs) with extended afterglow characteristics were synthesized via a one-step solvothermal method using acrylamide, sulfosalicylic acid, and sodium tetraborate as protective matrices. The presence of boron from sodium tetraborate introduced an empty orbital, allowing it to form a more extended conjugated system with adjacent oxygen atoms, thereby lowering the energy level of the lowest unoccupied molecular orbital in the system. The phosphorescence emission of these BCDs exhibits a red shift over time from 450 to 500 nm. These BCDs have been effectively utilized to produce anti-counterfeit phosphorescent powder. Additionally, the BCDs display optimal fluorescence excitation at 330 nm and optimal emission at 420 nm. They demonstrate a detection limit for ciprofloxacin hydrochloride of 37 nM in the 1-100 µM concentration range and 26 nM in the 100-210 µM range. This fluorescence detection is governed by an inner filter effect. Real sample testing further confirms that these BCDs serve as excellent sensors for ciprofloxacin hydrochloride.

Effective Screening of Metal Dopants for In2O3 Catalyst to Tune Catalytic Performance of CO2 Hydrogenation to Formic Acid

AbstractThe metal doping is an effective strategy to adjust catalytic performance for indium oxide catalyst in CO2 hydrogenation. In current work, a series dopant, Co, Fe, Ni, Pd, Pt, Rh, and Ru, are selected and examined in CO2 hydrogenation to formic acid by DFT based microkinetic simulation. It is found that substitutional doping is local effect, which mainly promotes the reactivity of adjacent oxygen atoms. The calculations of both CO2 adsorption and hydrogen molecule dissociation certify the positive effects induced by doping, and the adsorption energy of CO2 has a linear relation with the transferred charges for all investigated catalysts which helps to explain the C─O bond activation mechanism. Two pathways, formate and carboxyl, are investigated under same footing. It is noted that doping significantly reduces the hydrogenation barriers on two pathways compared with undoped surfaces. Moreover, the calculated TOF of formic acid formation is greatly increased on doped surfaces and Pt, Pd, and Ru are identified as the most active dopants. In the end, it is concluded that reaction obeys carboxyl mechanism and a valid descriptor of trans‐HCOOH* and H* formation energy is proposed for the screening of effective dopants.

A Study on Oxygen Vacancy Resistance Mechanism of V2O5

Introduction: Due to its magnetic and semiconductor properties, V2O5 has shown tremendous potential in resistive switching memory. Method: Therefore, this paper investigates the resistive mechanism of oxygen vacancies in V2O5. The formation energies of different oxygen vacancies are calculated. Results: The results indicate that oxygen vacancies tend to form single-component conductive filaments. In mixed oxygen vacancies clusters, the charge transfer characteristics and density of states of the V2O5-VO 13 vacancies are the most significant, which is consistent with the analysis of formation energy data. Conclusions: Additionally, the charge transfer of cluster oxygen vacancies was calculated, showing that V atoms directly connected to oxygen vacancies tend to lose electrons, while adjacent oxygen atoms are more likely to gain electrons. In V2O5-VO 12 and V2O5-VO 13, the number of electrons obtained by O2 and O16 exceeds the average by 36.4% and 33.2%. Thus, the formation of oxygen vacancies effectively improves the resistance characteristics of the V2O5.

Promoting the hydrogen spillover via dual active sites synergistically for efficient photo-driven nitrogen fixation

Photocatalytic ammonia synthesis is heralded as the most promising field that will certainly gain increasing attention as a sustainable strategy for low-carbon NH3 production and H2 storage. However, one great challenge is to design ideal catalysts, which can provide the energetic active sites for nitrogen activation and hydrogen dissociation at the same time. In this study, we report that efficient photo-driven ammonia synthesis can be realized by synergetic effect of abundant Mo (V) species and Pt under ambient conditions. More specifically, the optimized Pt-loaded MoO3-x photocatalyst has attained the superior NH3 production rates of 3456 μg·g−1·h−1 under visible light irradiation (≥400 nm). As evidenced experimentally and theoretically, the enhanced photocatalytic performance can be ascribed to dual-active sites, where the loaded Pt co-catalyst can boost hydrogen spillover from Pt to MoO3-x induced by OV due to the low barrier of H* migration between hydrogen activation sites (Pt-O bridge) and nitrogen activation sites (low-valence Mo species), further increasing the number of Mo (V) active sites. And Mo (V) species adjacent oxygen vacancy with outstanding electron-donating capability and strong nitrogen chemisorption played a crucial role in facilitating nitrogen dissociation. Therefore, synergizing abundant Mo (V) species and loaded-Pt can optimize the photo-driven nitrogen reduction and hydrogen oxidation. This work provides a new idea for the rational design of efficient photo-driven ammonia synthesis.

Oxygen plasma-assisted magnetron sputtering deposition of non-stoichiometric Y2O3 films: Influence of oxygen vacancies on etching resistance

Yttrium oxide (Y2O3) films are widely used to protect equipment in plasma etching, a crucial technique in semiconductor processing, due to their exceptional resistance to plasma etching. Since oxygen vacancy affects the performance of Y2O3 and may impact physical etching resistance, the internal relationship necessitates further investigation. In this article, Y2O3 films with varying oxygen vacancy concentrations are prepared by reactive magnetron sputtering with the assistance of oxygen plasma. The formation and development of oxygen vacancies in cubic Y2O3 films and their impact on the physical etching resistance were investigated. The experiment results indicate that the accumulation of oxygen vacancies causes non-stoichiometry and the etching rate is significantly reduced. Combined with density-functional theory, it is revealed that oxygen vacancy distorts the lattice, which increases covalent Y–O bonding and the formation energy of atoms. Moreover, the vacancy line defects resulting from diffusion and aggregation of oxygen vacancies exert a similar influence on the adjacent yttrium and oxygen layers. The enhancement of physical etching resistance is attributed to the strengthened internal Y–O bonds led by increasing oxygen vacancy concentration in the cubic Y2O3 films without inducing phase transition. The discovery enriches the understanding of how plasma interacts with Y2O3, and the etching mechanism.

High-Pressure CO2 and CH4 Transport in Smooth Crystalline Silica Mesopores: A Molecular Dynamics Study.

In this study, we use molecular dynamics (MD) simulation to study pressure-driven CO2 and CH4 flows and their slippage behaviors in β-cristobalite mesopores. The result illustrates that both CO2 and CH4 have an apparent adsorption layer on pore surface. However, significant differences in gas slippage are observed: CH4 flow shows considerable slippage, while it is negligible for CO2 flow. This disparity is attributed to the collective effect of gas molecular configurations and surface structure. The linear molecular structure of CO2 allows it to align perpendicular to the surface, even penetrating into the surface. Notably, the perpendicular orientation of CO2 molecules is energetically favored near the center of the equilateral triangle formed by adjacent oxygen atoms on β-cristobalite surface. Conversely, the symmetric molecular structure of CH4, coupled with its larger size, prevents its penetration into pore surfaces. Therefore, despite smooth crystalline surfaces, CO2 topological accessible plane is much more curved than that of CH4. Consequently, CO2 displays hesitating motions undergoing rotational movements, which significantly hinders its slippage. This study highlights the collective influences of gas molecular characteristics and surface structure on gas slippage, affording important insights into gas sequestration and the development of functional materials for gas separation.

Theoretical investigation of 4d noble metal (Ru, Rh or Pd) single atom structures influencing surface oxygen behavior on SnO2(1 1 0)

Surface oxygen species play a key role in determining the chemi-resistive gas sensing performance of SnO2. Through surface modification, the type of oxygen species at different working temperatures can be modulated, leading to changes in carrier concentration and surface activity. Single atom structures (SAS) hold enormous potential in the gas sensing domain; however, the impact of different SAS on surface oxygen species on SnO2 remains unclear, resulting in inconsistent improvements in sensing properties. This study conducted a theoretical investigation of different 4d noble metal SAS (Ru, Rh, and Pd) modified SnO2(110) surface, encompassing both electronic and chemical sensitization. All three SAS, when substituting penta-coordinated Sn atom (Sn5c), can inject holes and create a thicker depletion layer to varying degrees. Ru and Rh SAS can accelerate the decomposition of adsorbed O2 and O3. More importantly, Ru and Rh can hinder the combination of adsorbed O* species with adjacent two-coordinated lattice oxygen (O2c), enhancing the chemical stability of O*, which plays a decisive role in detecting reducing gases, with Ru exhibiting a better effect. This theoretical work not only enhances methods and mechanisms for adjusting surface oxygen species and improving the sensing performance of SnO2-based gas sensors, but also provides useful guidance for screening and designing SAS in experimental procedures on different semiconductor metal oxide surfaces.

Porous Frustrated Lewis Pairs Catalyst Constructed on Defective Zirconium-Based Metal-Organic Frameworks for Hydrogenation Reactions with H2.

A porous metal-organic framework (MOF)-based frustrated Lewis pairs (FLPs) were prepared via a ligand replacement strategy to generate organic linker defects in zirconium-based MOF (MOF-808), thereby exposing Zr sites as Lewis acid. Due to the rigid features of the MOF skeleton, the unsaturated metal cluster and the adjacent lattice oxygen (Lewis bases) are in sterically hindered positions, which formed FLP sites with efficient H2 activation ability. This porous heterogeneous FLP catalyst [MOF-808-OH (15%)] exhibits high performance styrene hydrogenation to ethylbenzene with 99% yield. The high structural stability and reusability enabled the catalyst to maintain an over 98% activity after five cycles. This work provides a defect modulation strategy to prepare MOF-based solid FLP catalysts.

Unraveling the oxygen evolution in layered LiNiO2 with the role of Li/Ni disordering

Oxygen loss is widely recognized as a major factor in the structural degradation of Ni-rich layered cathode materials, while a study on the detailed oxygen evolution process and the role of inevitable Li/Ni disordering defects is still lacking. Using ab initio calculations with van der Waals correction, we performed an in-depth study on the oxygen evolution in layered LiNiO2 and considered the role of Li/Ni disordering. We find that excess Ni in Li slab act as a pillar role for the structural framework and increases bond strength of adjacent oxygen ions, both of which are beneficial to the thermal and kinetic stability of lattice oxygen in LiNiO2, thus inhibiting the oxygen evolution. For Li/Ni exchange and Excess Li defects, the Li ion in Ni slab preferred to return to the vacancy in Li slab with delithiation in both surface and bulk LiNiO2. This situation induces the weaken binding and fast migration of lattice oxygen, even Ni slab collapse and oxygen release in the surface. Furthermore, the ab-initio molecular dynamics simulations for LiNiO2 surface reveal three stages of oxygen loss in the pristine state: (i) the formation of pre-O-O dimer; (ii) the pre-O-O dimer oxidizing to O-O dimer; (iii) O2 release with oxygen oxidation and Ni migration. The Li/Ni exchange and Excess Li defects accelerate this process because of Li ion in Ni slab returning to Li slab, while the Excess Ni defects will inhibit this process. We hope this work will improve the understanding of oxygen evolution in layered LiNiO2 and provide theoretical guidance for the design of Ni-rich layered cathode materials with improved stability.

Application of South African heulandite (HEU) zeolite for the adsorption and removal of Pb2+ and Cd2+ ions from aqueous water solution: Experimental and computational study

The capacity of South African Heulandite (HEU) zeolite to remove Pb2+ and Cd2+ ions from aqueous solution was investigated using batch experiments and molecular simulations studies. The effect of different factors on the adsorption of these ions onto the zeolite was investigated; contact time, initial metal ion concentration and the amount of HEU adsorbent. Molecular simulations was done using Monte Carlo and density functional theory. Experimental results obtained indicate that the maximum adsorption for the two ions occur at pH 5 and after 240 min of contact time. The percent removal based on contact time of Pb2+ and Cd2+ ions from water by the heulandite zeolite were 99.7 and 76.7 %, respectively. The adsorption of two metal ions onto the HEU zeolite follows the Langmuir adsorption isotherm. From the molecular simulation findings, the adsorption of Pb2+ ions onto the HEU window is equidistant from the two adjacent oxygen atoms within the HEU structure while the Cd2+ ion is adsorbed in the upper left side of the 8-ring HEU window. It was observed that the performance of the zeolite can significantly be improved by doping with germanium, aluminum, thallium indium, and sodium cations. These results indicate that the application of HEU zeolite as an adsorbent holds a great promise in heavy metal removal from aqueous solutions.

Protons intercalation induced hydrogen bond network in δ-MnO2 cathode for high-performance aqueous zinc-ion batteries

Birnessite-type MnO2 (δ-MnO2) exhibits great potential as a cathode material for aqueous zinc-ion batteries (AZIBs). However, the structural instability and sluggish reaction kinetics restrict its further application. Herein, a unique protons intercalation strategy was utilized to simultaneously modify the interlayer environment and transition metal layers of δ-MnO2. The intercalated protons directly form strong O H bonds with the adjacent oxygens, while the increased H2O molecules also establish a hydrogen bond network (O H···O) between H2O molecules or bond with adjacent oxygens. Based on the Grotthuss mechanism, these bondings ultimately enhance the stability of layered structures and facilitate the rapid diffusion of protons. Moreover, the introduction of protons induces numerous oxygen vacancies, reduces steric hindrance, and accelerates ion transport kinetics. Consequently, the protons intercalated δ-MnO2 (H-MnO2-x) demonstrates exceptional specific capacity of 401.7 mAh/g at 0.1 A/g and a fast-charging performance over 1000 cycles. Density functional theory analysis confirms the improved electronic conductivity and reduced diffusion energy barrier. Most importantly, electrochemical quartz crystal microbalance tests combining with ex-situ characterizations verify the inhibitory effect of the interlayer proton environment on basic zinc sulfate formation. Protons intercalation behavior provides a promising avenue for the development of MnO2 as well as other cathodes in AZIBs.

In situ fabrication of atomically adjacent dual-vacancy sites for nearly 100% selective CH4 production

The photocatalytic CO2-to-CH4 conversion involves multiple consecutive proton-electron coupling transfer processes. Achieving high CH4 selectivity with satisfactory conversion efficiency remains challenging since the inefficient proton and electron delivery path results in sluggish proton-electron transfer kinetics. Herein, we propose the fabrication of atomically adjacent anion-cation vacancy as paired redox active sites that could maximally promote the proton- and electron-donating efficiency to simultaneously enhance the oxidation and reduction half-reactions, achieving higher photocatalytic CO2 reduction activity and CH4 selectivity. Taking TiO2 as a photocatalyst prototype, the operando electron paramagnetic resonance spectra, quasi in situ X-ray photoelectron spectroscopy measurements, and high-angle annular dark-field-scanning transmission electron microscopy image analysis prove that the VTi on TiO2 as initial sites can induce electron redistribution and facilitate the escape of the adjacent oxygen atom, thereby triggering the dynamic creation of atomically adjacent dual-vacancy sites during photocatalytic reactions. The dual-vacancy sites not only promote the proton- and electron-donating efficiency for CO2 activation and protonation but also modulate the coordination modes of surface-bound intermediate species, thus converting the endoergic protonation step to an exoergic reaction process and steering the CO2 reduction pathway toward CH4 production. As a result, these in situ created dual active sites enable nearly 100% CH4 selectivity and evolution rate of 19.4 μmol g-1 h-1, about 80 times higher than that of pristine TiO2. Thus, these insights into vacancy dynamics and structure-function relationship are valuable to atomic understanding and catalyst design for achieving highly selective catalysis.

Unlocking ethane production in photocatalytic methanol reforming based on a novel carbon–carbon coupling mechanism

Photocatalytic methanol reforming represents a promising solution to energy and environmental challenges, yet the CO2 by-product poses significant environmental concerns. Recent advancements enhance the economic and environmental sustainability of this process by yielding valuable by-products like ethylene and ethylene–glycol. However, synthesizing ethane (C2H6), a crucial material, remains unattainable through this reaction, with an unclear mechanism. Herein, we synthesized oxygen-deficient two-dimensional TiO2 nanosheets to achieve ethane production via methanol reforming. Through theoretical calculations and in situ characterization, we unveil a novel carbon–carbon (C–C) coupling mechanism driving ethane production. It is discovered that methanol preferentially adsorbs on the oxygen vacancies of the defective TiO2 surface, forming methoxy radicals (*CH3O), facilitating C–C coupling for ethane formation. Furthermore, prolonged hydrogenation creates additional oxygen vacancies, leading to more adjacent oxygen vacancies. This results in more neighboring *CH3O, facilitating C–C coupling and elevating C2H6 production. Our study clarifies ethane production feasibility in photocatalytic methanol reforming, providing valuable references for future research.

Creating Atomically Iridium-Doped PdOx Nanoparticles for Efficient and Durable Methane Abatement.

The urgent environmental concern of methane abatement, attributed to its high global warming potential, necessitates the development of methane oxidation catalysts (MOC) with enhanced low-temperature activity and durability. Herein, an iridium-doped PdOx nanoparticle supported on silicalite-1 zeolite (PdIr/S-1) catalyst was synthesized and applied for methane catalytic combustion. Comprehensive characterizations confirmed the atomically dispersed nature of iridium on the surface of PdOx nanoparticles, creating an Ir4f-O-Pdcus microstructure. The atomically doped Ir transferred more electrons to adjacent oxygen atoms, modifying the electronic structure of PdOx and thus enhancing the redox ability of the PdIr/S-1 catalysts. This electronic modulation facilitated methane adsorption on the Pd site of Ir4f-O-Pdcus, reducing the energy barrier for C-H bond cleavage and thereby increasing the reaction rate for methane oxidation. Consequently, the optimized PdIr0.1/S-1 showed outstanding low-temperature activity for methane combustion (T50 = 276 °C) after aging and maintained long-term stability over 100 h under simulated exhaust conditions. Remarkably, the novel PdIr0.1/S-1 catalyst demonstrated significantly enhanced activity even after undergoing harsh hydrothermal aging at 750 °C for 16 h, significantly outperforming the conventional Pd/Al2O3 catalyst. This work provides valuable insights for designing efficient and durable MOC catalysts, addressing the critical issue of methane abatement.