Publication date: 21st July 2025
Mechanochemistry has a great potential for the solvent-free synthesis of complex multinary metal halides. [1, 2] Indeed, typical bottlenecks related to the different solubilities of metal halide precursors and the difficulty in ensuring a precise stoichiometry in final crystals when utilizing solution processes can be overcome by dry mechanochemical synthesis. Herein I will show how this strategy can be employed to achieve high-entropy 3D halide perovskites for the first time. [3]
More precisely, we have achieved substantial simultaneous alloying in three of the four sublattices of halide double perovskites with general formula Cs2(B1:B2)(C1:C2)(X1:X2)6 by means of ball-milling and thermal annealing. This leads to highly relevant properties such as pronounced bandgap bowing and full visible light absorption even for pure-chloride compositions.
The fundamental processes involved in such high-entropy alloying are revealed through a combination of detailed structural characterization and DFT calculations, highlighting the different ion-exchange kinetics and how these are linked to defect formation energies in different phases.
Eventually, I will show how these materials can be implemented as photoelectrocatalysts in the highly-sought after oxygen evolution reaction which is a key process in many energy-related applications.
The authors acknowledge funding for 22747/FPI/24. Fundacion Séneca. Región de Murcia (Spain),CNS2023-144331, funded by MCIN/AEI /10.13039/501100011033, MCIU/AEI/10.13039/501100011033 and by the European Union NextGenerationEU/ PRTR and Grant PID2022-139191OB-C32 funded by MICIU/AEI /10.13039/501100011033 and FEDER, UE as well as grant RYC2020-028803-I funded by MCIN/AEI/10.13039/501100011033 and “ESF Investing in your future.
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