Emerging frontiers of high-entropy materials for catalytic CO2 reduction

Abstract

Driven by the global carbon neutrality strategy, the efficient catalytic conversion of CO₂ is a crucial component for achieving the recycling of carbon resources. However, conventional catalysts are limited by issues such as single active sites, insufficient stability, and low energy efficiency, making it difficult to meet the demands of industrial-scale applications. High-entropy materials (HEMs), a novel class of functional systems composed of five or more principal elements, offer a promising breakthrough for CO₂ reduction reaction (CO₂RR) catalysts. They leverage the structural stability conferred by the high-entropy effect, synergistic regulation from multi-component systems, and tunable electronic structures. This article systematically reviews the recent advancements in high-entropy alloys (HEAs), high-entropy oxides (HEOs), high-entropy sulfides (HESs), and other HEMs for CO₂RR via photocatalytic, electrocatalytic, and thermocatalytic pathways. It further explores the application of machine learning-driven high-throughput design strategies and component modulation methods in HEMs development. Focusing on the promising HEMs, this review establishes a theoretical framework for designing next-generation CO₂RR catalysts, providing critical guidance for carbon neutrality advancements.