Ana Carolina Lemos de Morais, Allef Gabriel da Silva Fortes, Iago Rodrigues de Abreu, Corinne van Noordenne-Bos, Vincent S D Voet, Rudy Folkersma, Katja Loos
{"title":"Blending PHBV with P(3HB-<i>co</i>-4HB) for superior thermal stability, mechanical strength, and environmental degradation.","authors":"Ana Carolina Lemos de Morais, Allef Gabriel da Silva Fortes, Iago Rodrigues de Abreu, Corinne van Noordenne-Bos, Vincent S D Voet, Rudy Folkersma, Katja Loos","doi":"10.1039/d5fd00035a","DOIUrl":"https://doi.org/10.1039/d5fd00035a","url":null,"abstract":"<p><p>Polyhydroxyalkanoates (PHAs) hold significant potential as sustainable alternatives to fossil-based plastics because of their bio-based origin and inherent biodegradability. Poly-3-hydroxybutyrate-<i>co</i>-3-hydroxyvalerate (PHBV) is a well-known commercial member of the PHA family characterized by good mechanical resistance and thermal behavior similar to that of some conventional polymers, such as polypropylene. However, its high crystallinity and fragility limit its application. Poly3-hydroxybutyrate-<i>co</i>-4-hydroxybutyrate (P(3HB-<i>co</i>-4HB)) is a new commercial copolymer containing a 4-hydroxybutyrate (4HB) segment that provides increased flexibility because of its amorphous phase. In this study, PHBV and P(3HB-<i>co</i>-4HB) were blended by extrusion, varying the percentage of P(3HB-<i>co</i>-4HB) to improve the PHBV properties without losing the PHA assets and potentializing the insertion of this biopolymer in the market. The results indicate that the impact energy required for fracture was increased in the polymer blends. These blends exhibited greater thermal stability than pure PHBV, with no significant changes observed in the melting and crystallization temperatures. Furthermore, blending was found to reduce shrinkage in injection-molded samples. The degradation in the soil increased with the highest P(3HB-<i>co</i>-4HB) content. Through 3D printing, it was observed that the blends led to an increase in the melt flow index and a reduction in warpage in the printed objects, thereby facilitating the processing of these materials. Consequently, incorporating P(3HB-<i>co</i>-4HB) into PHBV has emerged as a promising strategy to address the inherent limitations of PHBV. This approach not only enhances the mechanical properties and thermal stability but also improves the overall processability, thereby expanding the potential applications of this biopolymer blend.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145273250","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Bing Zhu, Qiqi Huang, Okkyun Seo, Yee Yan Tay, Jiayi Tang, Huayu Gu, Tong Li, Dongshuang Wu
{"title":"Tailoring Pd content for optimal stability in FeCoNiCu multielement alloy electrocatalysts for oxygen evolution reaction.","authors":"Bing Zhu, Qiqi Huang, Okkyun Seo, Yee Yan Tay, Jiayi Tang, Huayu Gu, Tong Li, Dongshuang Wu","doi":"10.1039/d5fd00084j","DOIUrl":"https://doi.org/10.1039/d5fd00084j","url":null,"abstract":"<p><p>Multielemental alloys (MEAs) based on Earth-abundant 3d transition metals hold significant promise as low-cost electrocatalysts for the oxygen evolution reaction (OER), but their long-term stability under oxidative conditions remains a major challenge. In this study, we investigate the effect of palladium incorporation on the electrochemical performance and structural durability of FeCoNiCu MEA nanoparticles. Building upon our previous findings that trace Pd addition significantly enhances catalyst durability, an accelerated durability test (ADT) performed at 100 mA cm<sup>-2</sup> reveals that the degradation rate (0.356 mV h<sup>-1</sup>) decreased dramatically to approximately 1/350th that of Pd-free FeCoNiCu (125 mV h<sup>-1</sup>). In this study, we systematically synthesized a series of Pd-FeCoNiCu alloys with Pd contents ranging from 0.177 to 1.97 at%. Advanced characterization techniques including inductively coupled plasma optical emission spectroscopy (ICP-OES), electron microscopy, synchrotron-based spectroscopy, and electrochemical measurements, were employed to elucidate the correlation between composition, structure, and performance. Our findings reveal a highly non-linear dependence of catalyst performance on Pd content: an optimal range (0.336-0.389 at%) enables long-range d-d/sp orbital hybridization that delocalizes the local density of states (LDOS) of surrounding 3d metals, thereby suppressing oxidative dissolution. In contrast, higher Pd concentrations lead to Pd-Pd interactions, localize electronic perturbation, and accelerate degradation. This volcano-type correlation between Pd content and durability, highlights a general strategy for engineering catalyst longevity <i>via</i> minimal noble-metal doping and spatially cooperative electronic modulation.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145273201","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Stabilisation of FeCoNiCuPt high-entropy alloy nanoparticles by surface capping.","authors":"Anurag Sharma, Andrew L Hector","doi":"10.1039/d5fd00088b","DOIUrl":"https://doi.org/10.1039/d5fd00088b","url":null,"abstract":"<p><p>High-entropy alloys (HEA) are a distinct class of materials made up of multiple principal components (≥5) in near-equimolar ratios, resulting in extraordinary properties, including high catalytic activity, corrosion and oxidation resistance, and tunable magnetic properties. In nanoparticle form, these alloys are highly promising for a variety of advanced applications, such as catalysis, magnetic storage, and biomedical technology [Zoubi <i>et al.</i>, <i>Nano Energy</i>, 2023, <b>110</b>, 108362]. This study used an isolating-medium-assisted solid-state reaction to synthesise FeCoNiCuPt HEA nanoparticles with ultrafine NaCl particles as the isolating medium [Meng <i>et al.</i>, <i>Mater. Adv.</i>, 2024, <b>5</b>, 719]. The nanoparticles were stabilised with a range of hydrophobic and hydrophilic capping agents, such as polyethylenimine, polyvinylpyrrolidone, stearic acid, octadecylamine, <i>etc.</i>, introduced before or after the removal of the isolating medium. The formation of single-phase nanoparticles and the chemical composition of FeCoNiCuPt was validated using X-ray diffraction and energy-dispersive X-ray spectroscopy. Transmission electron microscopy and dynamic light scattering were used to determine particle sizes, effective capping agent thickness, and particle stability. The results highlight the successful synthesis of the FeCoNiCuPt nanoparticles, the effect of capping agents on the control of particle size, and the stability of capped-nanoparticle suspensions in water and organic solvents. The study emphasises the importance of selecting the appropriate capping agent to maintain nanoparticle stability and prevent agglomeration.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145256917","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jan Lukas Bürgel, Rico Zehl, Felix Thelen, Ridha Zerdoumi, Olga A Krysiak, Benedikt Kohnen, Ellen Suhr, Wolfgang Schuhmann, Alfred Ludwig
{"title":"Exploration of nanostructured high-entropy alloys for key electrochemical reactions: a comparative study for the solid solution systems Cu-Pd-Pt-Ru, Ir-Pd-Pt-Ru and Ni-Pd-Pt-Ru.","authors":"Jan Lukas Bürgel, Rico Zehl, Felix Thelen, Ridha Zerdoumi, Olga A Krysiak, Benedikt Kohnen, Ellen Suhr, Wolfgang Schuhmann, Alfred Ludwig","doi":"10.1039/d5fd00082c","DOIUrl":"https://doi.org/10.1039/d5fd00082c","url":null,"abstract":"<p><p>Electrocatalysis is critical for mitigating climate change by providing green energy solutions, <i>e.g.</i> for hydrogen production by electrolysis of water implying high catalytic activity not only for hydrogen evolution but also for oxygen evolution as the counter reaction. Moreover, reactions such as oxygen reduction and nitrate reduction are of high importance in fuel cells or for environmental remediation. This study focuses on the exploration of electrocatalysts in the enormous composition spaces encountered in multinary materials like high-entropy alloys in the form of compositionally complex solid solutions. These provide paradigm-changing design principles for new electrocatalysts based on their tuneable surface atom arrangements resulting from their multinary composition. However, to master the combinatorial explosion problem of polyelemental catalysts, efficient exploration approaches need to be adapted. For this purpose, we present a comprehensive strategy to compare the electrocatalytic activity for different reactions in alkaline media, namely the oxygen evolution reaction (OER), oxygen reduction reaction (ORR), hydrogen evolution reaction (HER) and nitrate reduction reaction (NO<sub><i>x</i></sub>RR) over large compositional spaces in three multinary systems: Cu-Pd-Pt-Ru, Ir-Pd-Pt-Ru and Ni-Pd-Pt-Ru. To generate the necessary large and multidimensional experimental dataset, thin-film materials libraries were synthesised and analysed using high-throughput characterisation methods. This allows for a comparative overview over correlations between composition and electrocatalytic activity, considering also relevant information on crystal structure and surface morphology. Similarities and differences, trends, maxima and minima in electrocatalytic activity are revealed and discussed. Main findings include that for the OER Ir<sub>23</sub>Pd<sub>3</sub>Pt<sub>8</sub>Ru<sub>66</sub> exhibits the highest activity, exceeding any alloy of the other two systems by 51% (Ni-Pd-Pt-Ru) and 74% (Cu-Pd-Pt-Ru). For HER, Ir<sub>36</sub>Pd<sub>4</sub>Pt<sub>48</sub>Ru<sub>12</sub> surpasses any of its elemental constituents by 26% and maxima in other systems by 5% (Ni-Pd-Pt-Ru) and 23% (Cu-Pd-Pt-Ru). For the NO<sub><i>x</i></sub>RR, only a marginal increase of 4% was found between the most active measured alloy and the elemental constituent Cu. By comparing activity across systems, we demonstrate the tunability of electrochemical activity on compositionally complex solid solutions, achievable through variations in composition both within and across different material systems for four different reactions.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145248968","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Martin L S Nielsen, Jack K Pedersen, Marcus F Nygaard, Mads K Plenge, Henrik H Kristoffersen, Jan Rossmeisl
{"title":"Modelling adsorbate coverage on complex alloy surfaces.","authors":"Martin L S Nielsen, Jack K Pedersen, Marcus F Nygaard, Mads K Plenge, Henrik H Kristoffersen, Jan Rossmeisl","doi":"10.1039/d5fd00089k","DOIUrl":"10.1039/d5fd00089k","url":null,"abstract":"<p><p>In order to extend catalysis theory to complex alloys and multiple adsorbates, we have to face the fact that the number of possible surface site-adsorbate combinations gets too large to calculate. We, instead, define rules for adsorbate-adsorbate interactions; specifically, blocking rules in terms of disallowed local adsorbate-adsorbate configurations. We then conduct simple simulations to investigate how different rules entail certain outcomes. For the PdAg intermetallic and PdAg solid solutions, we find that the presence of Ag atoms hinders O* species from covering the whole (111) surface, which is the case for unary Pd(111), and instead allows for adsorbed *OH species. We predict that the adsorbed *OH species improves the oxygen reduction reaction activity because they have adsorption energies at the top of the activity volcano. Experiments can use our results to distinguish between the different possible PdAg(111) alloy surface manifestations, and to better understand adsorbate coverage on complex alloys. Lastly, we use our approach on Ag<sub>14</sub>Ir<sub>16</sub>Pd<sub>30</sub>Pt<sub>14</sub>Ru<sub>26</sub> high-entropy alloys, but find that the choice of adsorbate-adsorbate interaction rules affects the oxygen reduction in less distinguishable ways compared to the binary PdAg alloys.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12502897/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145237449","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Surface segregation and mixing propensity in noble metal AgAuCuPdPt nanoalloys upon element enrichment - a computational perspective.","authors":"Florent Calvo","doi":"10.1039/d5fd00077g","DOIUrl":"https://doi.org/10.1039/d5fd00077g","url":null,"abstract":"<p><p>High-entropy Ag-Au-Cu-Pd-Pt nanoparticles in the 2400-6300-atom size range were computationally studied at thermodynamical equilibrium and room temperature using a combination of well established many-body potentials and Monte Carlo methods. Tools from percolation theory are used to further quantify the deviations to ideal behavior from noninteracting solid solutions. Upon varying the concentration of each element one at a time, the possible surface enrichment in the various metals is determined and the fragment statistics provide insight into the spatial distribution of atoms within the nanoparticles and their tendency for mixing or segregation. The effects of size and dimensionality are addressed separately, by comparing the results obtained for the 0D (nanoparticle) system with those for the 2D (slabs) and 3D (periodic) samples. Although these properties are found to depend on the underlying many-body potential to some extent, some robust trends are predicted, notably for silver and platinum, which strongly segregate and preferentially reside at the surface and in the core of the nanoparticles, respectively.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145237505","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hossein Mahdavi, Armin Asghari Alamdari, Jonathan Quinson, Uğur Ünal, Hadi Jahangiri
{"title":"Mechanically alloyed NiCuMnWX (X = Co, Fe, or Mo) high-entropy alloy electrocatalysts for alkaline water splitting.","authors":"Hossein Mahdavi, Armin Asghari Alamdari, Jonathan Quinson, Uğur Ünal, Hadi Jahangiri","doi":"10.1039/d5fd00094g","DOIUrl":"https://doi.org/10.1039/d5fd00094g","url":null,"abstract":"<p><p>High-entropy alloys have great potential as electrocatalysts for water-splitting reactions. Benefiting from the cocktail effect and lattice distortion, high-entropy alloys exhibit relatively low overpotentials and significant stability, making them excellent candidates for electrocatalytic water splitting. These materials offer a cost-effective and abundant alternative to conventional noble-metal catalysts such as Pt and IrO<sub>2</sub>, which are limited by high costs and scarcity. This study investigates the electrocatalytic performance of high-entropy alloy powders prepared with equimolar ratios of Ni, Cu, Mn, and W, with additional elements (Co, Fe, or Mo) introduced to optimize their activity for the hydrogen evolution reaction and oxygen evolution reaction. The high-entropy alloy powders are synthesized <i>via</i> ball milling, involving both dry milling and wet milling in ethanol, followed by washing and drying at room temperature. Comprehensive characterization techniques, including X-ray diffraction, field-emission scanning electron microscopy, scanning transmission electron microscopy with energy-dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy, are employed to analyze their structure and properties. Electrochemical studies reveal that Fe and Mo significantly enhance hydrogen evolution reaction activity, achieving overpotentials of 301 mV and 305 mV, respectively, with corresponding Tafel slopes of 200.9 mV dec<sup>-1</sup> and 153.3 mV dec<sup>-1</sup>. Meanwhile, Co incorporation improves oxygen evolution reaction performance, reducing the overpotential to 326 mV with a Tafel slope of 143.7 mV dec<sup>-1</sup>. These findings underscore the potential of high-entropy alloy powders for advancing renewable energy technologies.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145231062","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Anissa Acheche, Jaysen Nelayah, Riccardo Gatti, Damien Alloyeau, Christian Ricolleau, Hakim Amara
{"title":"Thermal stability of CoNiPtCuAu nanoalloys: from segregation to melting properties.","authors":"Anissa Acheche, Jaysen Nelayah, Riccardo Gatti, Damien Alloyeau, Christian Ricolleau, Hakim Amara","doi":"10.1039/d5fd00096c","DOIUrl":"https://doi.org/10.1039/d5fd00096c","url":null,"abstract":"<p><p>Recent breakthroughs in the field of high-entropy alloy nanoparticles (HEA NPs) have significantly expanded their potential applications (such as catalysis or energy storage) making them promising candidates for use over a wide temperature range. However, their thermal stabilities are not yet fully understood, which is crucial to their future development. To better understand these phenomena and the underlying mechanisms, we performed molecular dynamics simulations by adopting an incremental approach to investigate the structural and thermal stability of CoNiPtCuAu HEA NPs, as well as their ternary and quaternary sub-alloys. More precisely, CoNiPt ternary system is first considered and then Cu and Au atoms are progressively introduced with the aim to analyse and quantify the thermal stability of HEA NPs in terms of their melting temperature and segregation mechanisms. Through our atomic-scale simulations, we demonstrate the negative impact of Au and Cu atoms on thermal stabilisation, whose presence at the surface tends to favour melting of the NPs because of their low melting point. These detailed analyses provide a robust and relevant research approach for identifying the key parameters influencing the thermal stability of HEA NPs, which is essential for obtaining such nano-objects with optimised structural and thermal properties.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145231189","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
V Chaudhary, S Dasari, A Sharma, R V Ramanujan, R Banerjee
{"title":"Processing-driven chemical ordering and its effect on magnetic properties in a high entropy alloy.","authors":"V Chaudhary, S Dasari, A Sharma, R V Ramanujan, R Banerjee","doi":"10.1039/d5fd00105f","DOIUrl":"https://doi.org/10.1039/d5fd00105f","url":null,"abstract":"<p><p>The influence of chemical ordering and its length scale on the magnetic behaviour of the Al<sub>0.2</sub>Ti<sub>0.3</sub>Co<sub>1.5</sub>CrFeNi<sub>1.5</sub> high entropy alloy (HEA) was investigated across three distinct microstructural conditions, including a solution annealed state, an annealed condition at 750 °C, and a cold rolled plus annealed condition. These processing routes produced changes in the volume fraction, size, and morphology of L1<sub>2</sub> ordered precipitates along with the formation of a minor L2<sub>1</sub> phase in the annealed states. Magnetic measurements performed between 2 K and 300 K revealed clear differences in saturation magnetization, coercivity, and magnetic transition temperatures across the three conditions. The solution annealed condition exhibited a single magnetic transition near 48 K and low coercivity, consistent with a fine dispersion of coherent L1<sub>2</sub> precipitates. In the annealed and cold rolled conditions, coarsening and morphological evolution of the L1<sub>2</sub> phase led to the emergence of a second magnetic transition at lower temperatures, attributed to partial magnetic decoupling of the precipitates. Coercivity increased significantly in these conditions due to enhanced domain wall pinning, while residual hysteresis at 300 K is attributed to a combination of minor L2<sub>1</sub> phase at grain boundaries and microstructural features in the cold-worked condition. These results demonstrate that chemical ordering and its structural evolution play a central role in governing low temperature magnetic behaviour in this alloy system. The findings contribute to the broader understanding of multifunctional HEAs that combine tunable magnetic properties with excellent mechanical performance.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145231177","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Menglong Liu, Divyansh Gautam, Christian M Clausen, Ahmad Tirmidzi, Gustav K H Wiberg, Jan Rossmeisl, Matthias Arenz
{"title":"Electrochemical synthesis of high entropy nanoparticles and the exploration of the Pd-Ag-Au composition space for the oxygen reduction reaction.","authors":"Menglong Liu, Divyansh Gautam, Christian M Clausen, Ahmad Tirmidzi, Gustav K H Wiberg, Jan Rossmeisl, Matthias Arenz","doi":"10.1039/d5fd00095e","DOIUrl":"10.1039/d5fd00095e","url":null,"abstract":"<p><p>Multi-metallic alloys such as high entropy alloys (HEAs) span an extensive compositional space, potentially offering materials with enhanced activity and stability for various catalytic reactions. However, experimentally identifying the optimal composition within this vast compositional space poses significant challenges. In this study, we present a medium-throughput approach to screen the composition-activity correlation of electrodeposited multi-metallic and HEA nanoparticles. We apply the approach for exploring the Pd-Ag-Au composition subspace for the alkaline Oxygen Reduction Reaction (ORR). The Pd-Ag-Au alloy nanoparticles were synthesized electrochemically, characterized and evaluated for the ORR using a rotating disk electrode (RDE) setup. From 107 individual measurements, a composition-activity correlation model was constructed using Gaussian Process Regression (GPR), pinpointing the optimal composition around Pd<sub>85</sub>Ag<sub>1</sub>Au<sub>14</sub>. The experimental results are then compared to theoretical predictions based on the well-established descriptor approach utilizing density functional theory (DFT) calculations. While some discrepancies exist, the experimental DFT-derived models show partial overlap, validating the utility of computational screening for multi-metallic systems. This work provides valuable insights for the efficient screening of multi-metallic catalysts for catalytic applications and exemplifies advanced pathways on how to compare and analyze experimental data to simulations based on well-defined hypotheses.</p>","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12495384/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145224789","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}