Saved in:
| Main Authors: | , , , , , |
|---|---|
| Format: | Preprint |
| Published: |
2026
|
| Subjects: | |
| Online Access: | https://arxiv.org/abs/2606.00779 |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1866910276329144320 |
|---|---|
| author | Thelen, Felix Kim, Moonjoo de Oliveira, Geovane Arruda Buergel, Jan Lukas Schuhmann, Wolfgang Ludwig, Alfred |
| author_facet | Thelen, Felix Kim, Moonjoo de Oliveira, Geovane Arruda Buergel, Jan Lukas Schuhmann, Wolfgang Ludwig, Alfred |
| contents | Alloying is a central strategy in electrocatalysis, enabling fine-tuning of electronic structure. In particular, compositionally complex solid solutions (CCSS) often called high-entropy alloys are of high interest as they allow active site design. However, the "combinatorial explosion" in the number of possible compositions poses a critical bottleneck for the discovery of active CCSS electrocatalysts. We present an autonomous scanning electrochemical cell microscopy (SECCM) system for ultrahigh-throughput and large-scale CCSS activity screening. The platform rapidly establishes composition-electrocatalytic activity relationships for large compositional spaces across multiple thin-film CCSS materials libraries via active learning and automated library exchange. Embedding analytical expressions of voltammetry in the algorithm enables the learning of whole voltammograms rather than a single selected metric. As a demonstration, we investigated hydrogen evolution reaction (HER) activities of Au-Ir-Rh, where Ir and Rh exhibit strong metal-hydrogen binding and Au exhibits relatively weak binding as derived from the HER volcano plot. The composition-activity trend was accurately predicted after measuring only 15% of all 966 measurement areas. Au30Ir20Rh50 and Au10Ir35Rh55 exhibit highest activities with standard rate constants of about 0.012 cm/s, demonstrating positive synergistic contributions from elemental mixing. The autonomous robotic SECCM platform is broadly applicable to a wide range of electrocatalytic reactions, providing a general pathway for accelerating CCSS electrocatalyst discovery and optimization. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2606_00779 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Autonomous scanning electrochemical cell microscopy enables rapid exploration of large compositionally complex material spaces Thelen, Felix Kim, Moonjoo de Oliveira, Geovane Arruda Buergel, Jan Lukas Schuhmann, Wolfgang Ludwig, Alfred Materials Science Alloying is a central strategy in electrocatalysis, enabling fine-tuning of electronic structure. In particular, compositionally complex solid solutions (CCSS) often called high-entropy alloys are of high interest as they allow active site design. However, the "combinatorial explosion" in the number of possible compositions poses a critical bottleneck for the discovery of active CCSS electrocatalysts. We present an autonomous scanning electrochemical cell microscopy (SECCM) system for ultrahigh-throughput and large-scale CCSS activity screening. The platform rapidly establishes composition-electrocatalytic activity relationships for large compositional spaces across multiple thin-film CCSS materials libraries via active learning and automated library exchange. Embedding analytical expressions of voltammetry in the algorithm enables the learning of whole voltammograms rather than a single selected metric. As a demonstration, we investigated hydrogen evolution reaction (HER) activities of Au-Ir-Rh, where Ir and Rh exhibit strong metal-hydrogen binding and Au exhibits relatively weak binding as derived from the HER volcano plot. The composition-activity trend was accurately predicted after measuring only 15% of all 966 measurement areas. Au30Ir20Rh50 and Au10Ir35Rh55 exhibit highest activities with standard rate constants of about 0.012 cm/s, demonstrating positive synergistic contributions from elemental mixing. The autonomous robotic SECCM platform is broadly applicable to a wide range of electrocatalytic reactions, providing a general pathway for accelerating CCSS electrocatalyst discovery and optimization. |
| title | Autonomous scanning electrochemical cell microscopy enables rapid exploration of large compositionally complex material spaces |
| topic | Materials Science |
| url | https://arxiv.org/abs/2606.00779 |