Publication date: 28th August 2024
Electrocatalytic water splitting is well suited for the production of hydrogen as a clean and renewable energy carrier to alleviate the current energy crisis. However, the sluggish kinetics of the anodic oxygen evolution reaction (OER), which involves the generation of triplet oxygen from singlet water on the electrocatalyst surface, results in a low overall energy efficiency and necessitates the use of high voltages to drive the spin transition. Herein, we harnessed the potential of topological chiral semimetals (RhSi, RhSn, and RhBiS) and their spin-polarized Fermi surfaces to promote the spin-dependent electron transfer in OER and overcome the volcano-plot limitation of conventional catalysts. The OER activity increases in the order of RhSi < RhSn < RhBiS, following the trend of spin-orbit-coupling (SOC). The chiral single crystals of RhSi, RhSn, and RhBiS exhibited higher OER activities than those of achiral crystals of RhTe2, RhTe, and the benchmark catalyst of RuO2. Especially, the specific activity of RhBiS exceeded that of RuO2 by two orders of magnitude. Our work reveals the pivotal roles of chirality and SOC in spin-dependent catalytic processes, facilitating the design of ultra-efficient chiral catalysts. Therefore, in future endeavors, the development of top-performing catalysts could encompass spin polarization as a fundamental property for chiral materials with SOC serving as a valuable descriptor.
This work was financially supported by the European Research Council (ERC Advanced Grant No. 742068 “TOPMAT”), the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) through SFB 1143 (project ID. 24731007), and the Würzburg-Dresden Cluster of Excellence on Complexity and Topology in Quantum Matter—ct.qmat (EXC 2147, project No. 390858490). C.F. thanks the DFG for 5249 (QUAST).
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