Enhancing the activity and stability of earth‐abundant, heterogeneous catalysts remains a key challenge, requiring new materials design strategies to replace platinum‐group metals. Herein, it is demonstrated that increasing the configurational disorder of spinel metal oxides (M₃O₄, where M is a combination of Cr, Mn, Fe, Co, Ni, Cu, and Zn) leads to significant improvements in carbon monoxide (CO) oxidation performance. A substantial 63% decrease in the T₁₀ value (temperature to reach 10% CO oxidation) is observed by systematically increasing the number of first‐row transition metals within the spinel oxide. Long‐term stability studies reveal that the most disordered 7‐metal spinel oxide exhibited superior resistance to catalyst deactivation compared to the 4‐metal variant, showing a decrease in activity of only 4.7% versus 12.2% during 14 h of operation. A solventless thermolysis approach is developed to synthesize a series of medium entropy spinel oxide (MESO) and high entropy spinel oxides (HESOs) from discrete, air‐stable molecular precursors. Comprehensive crystal structure determination, elemental distribution analysis, and surface characterization are conducted, establishing a clear structure‐function relationship between elemental composition, configurational disorder, and catalytic performance. This work highlights how configurational disorder can serve as an effective design principle for developing both active and stable catalysts.

The temperature-dependence of photoemission from a gold alloy, n-type β-Ga ₂ O ₃ and p-type diamond reveals reversible and irreversible changes in energy, due to changes in surface chemistry, band-bending, thermal expansion and a surface photovoltage.

This study describes the utilization of near edge X‐ray absorption fine structure (NEXAFS) to investigate the hole transporting material (HTM) 2,2ʹ,7,7ʹ‐tetrakis(N,N‐di‐p‐methoxyphenylamine)‐ 9,9ʹ‐spirobifluorene (Spiro‐OMeTAD) and its most common dopants, lithium bis‐(trifluoromethylsulfonyl) imide (LiTFSI), 4‐tert‐butylpiridine (tBP), and 2,3,5,6‐tetrafluoro‐7,7,8,8‐tetracyanoquinodimethane (F4‐TCNQ). By changing the angle of the sample with respect to the beam, the orientation of the molecules on the surface can be observed. The data suggest that it is difficult to determine any orientational preference for Spiro‐OMeTAD deposited on a surface due to the 3D propeller‐like geometry of this molecule. Both doped and undoped samples show thermal stability beyond the glass transition temperature of the molecules. Significant changes to the Spiro‐OMeTAD spectra are observed with the addition of the dopants, in particular the C K‐edge. Differences are also observed in the valence band spectra when dopants are added. It is also demonstrated how the doping combination of LiFTSI with tBP and, F4‐TCNQ act as p‐type dopants by altering the position of the HOMO levels. The F4‐TCNQ induces a larger change in the HOMO levels when compared to the LiTFSI and tBP. These results are important to increase the understanding of Spiro‐OMeTAD and the effect dopants have on this material for next generation solar cells.

Heteroatom doping of graphene is a promising approach for tailoring its chemical and electronic properties—a prerequisite for many applications such as sensing, catalysis, and energy storage. Doping chemical vapour deposition (CVD) graphene with nitrogen during growth (in situ doping) is a common strategy, but it produces a distribution of inequivalent dopant sites and requires substantial modifications to the CVD growth process. In this study, we demonstrate a novel and simple oxide-mediated approach to introduce nitrogen dopants into pre-existing CVD graphene (ex situ doping) which achieves comparable doping densities to in situ doping methodologies. Furthermore, we demonstrate that thermal annealing of N-doped graphene can selectively remove pyridinic, retaining graphitic and pyrrolic nitrogen dopants, offering an attractive route to further modify graphene functionality. The methodologies we present are simple and scalable to precisely tailor graphene properties without the need to alter CVD growth protocols.

Transition metal dichalcogenides are promising alternatives to noble metal catalysts, e.g., for (photo‐)activation of greenhouse gases or hydrogenations. Herein, a direct synthetic route for 2D TiS ₂ nanosheets on Au(111) by titanium deposition in the presence of a mild, organic, non‐oxidizing sulfur source is presented. High‐resolution scanning tunneling microscopy (STM) is used to gain atomic‐level insights into the TiS ₂ nanosheet morphology. In contrast to the literature, this protocol gains mostly hexagonal and truncated triangular nanosheets with an increased edge contrast in STM, analog to metallic edge states in MoS ₂ . Synchrotron‐based photoelectron spectroscopy allows insights into compositional details, specifically to distinguish different S sites on the TiS ₂ sheets and other S species on the sample. Further, a minimum size is identified (9 S atoms side length), which underlines the importance of moiré reconstructions for stress relief. The TiS ₂ sheets coexist with [Au]Ti ₁ S ₃ clusters, in which a single gold atom is alloyed into the surface and capped by three S atoms. Together with the finding of a critical sheet size, this points toward on‐surface Ostwald ripening as a relevant process in the sheet formation. Ab‐initio calculations (density functional theory) underscore that the chemical potential of S is an essential descriptor to maintain shape control.

PtCoO₂ is an attractive candidate for next-generation interconnects due to its exceptionally low in-plane resistivity, but its susceptibility to degradation under reducing conditions necessitates effective surface passivation strategies. In this work, the deposition of organic adlayers on PtCoO₂ was systematically investigated using octadecylphosphonic acid (ODPA), octylphosphonic acid (OPA), 1-octadecanethiol (ODT), and trifluoroacetic acid (TFA). The influence of immersion time (0.5–48 h) and surface pre-treatment (untreated, ethanol-cleaned, and UV-ozone-treated surfaces) was evaluated using water contact angle (WCA), X-ray photoelectron spectroscopy (XPS), and atomic force microscopy (AFM). Low-energy ion scattering (LEIS) confirmed a CoOx-rich surface termination, which strongly influenced adsorption behaviour. Among the molecules studied, phosphonic acids exhibited the strongest interaction with the surface, with ODPA producing the highest WCAs (97–99°) and clear evidence of phosphonate bonding. Comparison with OPA revealed the importance of alkyl chain length in promoting hydrophobicity and molecular organisation, yielding values of 77–88°. In contrast, ODT exhibited heterogeneous adsorption, sulphur oxidation, and aggregate formation, while TFA showed limited surface retention. Overall, ODPA was identified as the most effective adsorbate, establishing phosphonic acid-based self-assembled monolayers as promising candidates for the passivation of PtCoO₂ and related conductive oxide materials.