Exploration of phase stability, functional and mechanical properties in refractory- and noble-metal-based multiple-principal element alloys

• Applicants: Professor Dr. Ralf Drautz; Professor Dr.-Ing. Alfred Ludwig
• Subject Area: Thermodynamics and Kinetics as well as Properties of Phases and Microstructure of Materials ; Synthesis and Properties of Functional Materials ; Mechanical Properties of Metallic Materials and their Microstructural Origins
• Term: from 2018 to 2023
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 403582885

• Final Report Year: 2023

Final Report Abstract

The concept of multi-principal element alloys (MPEAs) as alloys that do not have a base element opens up a gigantic multi-element and multi-composition phase space. We addressed this space in a two-step procedure bringing together physical metallurgy with data analysis on the one hand and combinatorial synthesis of thin film materials libraries and computational high-throughput methods on the other hand, in line with recent propositions for a more systematic development of MPEAs. We set up simplified models that allowed us to navigate the composition space of MPEAs and developed machine learning potentials that based on high-throughput density functional enable accurate simulations of multi-component systems. Parallel to the work in theory and simulation, combinatorial experiments were carried out. The synthesized libraries were investigated by high-throughput characterization of structural, mechanical, electrical and electrochemical properties.

Publications

• Bayesian Optimization of High‐Entropy Alloy Compositions for Electrocatalytic Oxygen Reduction**. Angewandte Chemie International Edition, 60(45), 24144-24152.
  Pedersen, Jack K.; Clausen, Christian M.; Krysiak, Olga A.; Xiao, Bin; Batchelor, Thomas A. A.; Löffler, Tobias; Mints, Vladislav A.; Banko, Lars; Arenz, Matthias; Savan, Alan; Schuhmann, Wolfgang; Ludwig, Alfred & Rossmeisl, Jan
  
• Complex‐Solid‐Solution Electrocatalyst Discovery by Computational Prediction and High‐Throughput Experimentation**. Angewandte Chemie International Edition, 60(13), 6932-6937.
  Batchelor, Thomas A. A.; Löffler, Tobias; Xiao, Bin; Krysiak, Olga A.; Strotkötter, Valerie; Pedersen, Jack K.; Clausen, Christian M.; Savan, Alan; Li, Yujiao; Schuhmann, Wolfgang; Rossmeisl, Jan & Ludwig, Alfred
  
• Design of refractory compositionally complex alloys with optimal mechanical properties. Physical Review Materials, 5(6).
  Ferrari, Alberto; Lysogorskiy, Yury & Drautz, Ralf
  
• Phase constitution of the noble metal thin-film complex solid solution system Ag-Ir-Pd-Pt-Ru in dependence of elemental compositions and annealing temperatures. Nano Research, 15(6), 4827-4836.
  Xiao, Bin; Wang, Xiao; Savan, Alan & Ludwig, Alfred
  
• Zooming‐in – Visualization of active site heterogeneity in high entropy alloy electrocatalysts using scanning electrochemical cell microscopy. Electrochemical Science Advances, 2(3).
  Tetteh, Emmanuel Batsa; Banko, Lars; Krysiak, Olga A.; Löffler, Tobias; Xiao, Bin; Varhade, Swapnil; Schumacher, Simon; Savan, Alan; Andronescu, Corina; Ludwig, Alfred & Schuhmann, Wolfgang
  
• Correlations of Composition, Structure, and Hardness in the High-Entropy Alloy System Nb–Mo–Ta–W. High Entropy Alloys & Materials, 1(1), 110-119.
  Xiao, Bin; Lysogorskiy, Yury; Savan, Alan; Bögershausen, Heidi; Pfetzing-Micklich, Janine; Raabe, Dierk; Drautz, Ralf & Ludwig, Alfred
  
• Efficient parametrization of the atomic cluster expansion. Physical Review Materials, 6(1).
  Bochkarev, Anton; Lysogorskiy, Yury; Menon, Sarath; Qamar, Minaam; Mrovec, Matous & Drautz, Ralf
  
• Elemental (im-)miscibility determines phase formation of multinary nanoparticles co-sputtered in ionic liquids. Nanoscale Advances, 4(18), 3855-3869.
  Meischein, Michael; Garzón-Manjón, Alba; Hammerschmidt, Thomas; Xiao, Bin; Zhang, Siyuan; Abdellaoui, Lamya; Scheu, Christina & Ludwig, Alfred
  
• Multilayer atomic cluster expansion for semilocal interactions. Physical Review Research, 4(4).
  Bochkarev, Anton; Lysogorskiy, Yury; Ortner, Christoph; Csányi, Gábor & Drautz, Ralf
  
• Unravelling Composition–Activity–Stability Trends in High Entropy Alloy Electrocatalysts by Using a Data‐Guided Combinatorial Synthesis Strategy and Computational Modeling. Advanced Energy Materials, 12(8).
  Banko, Lars; Krysiak, Olga A.; Pedersen, Jack K.; Xiao, Bin; Savan, Alan; Löffler, Tobias; Baha, Sabrina; Rossmeisl, Jan; Schuhmann, Wolfgang & Ludwig, Alfred
  
• Active learning strategies for atomic cluster expansion models. Physical Review Materials, 7(4).
  Lysogorskiy, Yury; Bochkarev, Anton; Mrovec, Matous & Drautz, Ralf
  
• Isopropanol electro-oxidation on Pt-Ru-Ir: A journey from model thin-film libraries towards real electrocatalysts. Electrochimica Acta, 444, 142032.
  Minichová, Mária; Van, Pham Chuyen; Xiao, Bin; Savan, Alan; Hutzler, Andreas; Körner, Andreas; Khalakhan, Ivan; Rodríguez, Miquel Gamón; Mangoufis-Giasin, Iosif; Briega-Martos, Valentín; Kormányos, Attila; Katsounaros, Ioannis; Mayrhofer, Karl J.J.; Ludwig, Alfred; Thiele, Simon & Cherevko, Serhiy
  
• Local structure and magnetic properties of a nanocrystalline Mn-rich Cantor alloy thin film down to the atomic scale. Nano Research, 16(4), 5626-5639.
  Smekhova, Alevtina; Kuzmin, Alexei; Siemensmeyer, Konrad; Luo, Chen; Taylor, James; Thakur, Sangeeta; Radu, Florin; Weschke, Eugen; Buzanich, Ana Guilherme; Xiao, Bin; Savan, Alan; Yusenko, Kirill V. & Ludwig, Alfred
  
• Reorganization energy in a polybromide ionic liquid measured by scanning electrochemical cell microscopy. The Journal of Chemical Physics, 158(13).
  Kim, Moonjoo; Tetteh, Emmanuel Batsa; Savan, Alan; Xiao, Bin; Ludwig, Alfred; Schuhmann, Wolfgang & Chung, Taek Dong
  
• Stability of high-entropy alloys under electrocatalytic conditions. iScience, 26(10), 107775.
  Kormányos, Attila; Dong, Qi; Xiao, Bin; Li, Tangyuan; Savan, Alan; Jenewein, Ken; Priamushko, Tatiana; Körner, Andreas; Böhm, Thomas; Hutzler, Andreas; Hu, Liangbing; Ludwig, Alfred & Cherevko, Serhiy