Frontiers in CO2 reduction: employing alloy and high-entropy catalysts via photocatalytic and electrocatalytic pathways

Abstract

Since the Industrial Revolution, the large-scale extraction and utilization of fossil fuels have driven the rapid development of human society while causing an exponential increase in CO₂ emissions. Photocatalysis and electrocatalysis are regarded as some of the most promising strategies for carbon neutralization due to their ability to utilize renewable solar energy and electricity to drive the CO₂ reduction reaction (CO₂RR), respectively. Binary alloy and high-entropy catalysts have shown excellent ability to precisely modulate geometrical configurations on the atomic scale, which can be used to construct additional CO₂RR active sites, and have attracted much attention as commonly used photo/electrocatalytic catalysts. In this review, we systematically review various synthesis strategies for binary alloy and high-entropy catalysts, analyze the synergistic effects of the elements in binary alloys and high-entropy materials in the photo/electrocatalytic CO₂RR to generate a variety of energy materials, and focus on the mechanism of the CO₂RR in binary alloys and high-entropy materials, which achieves a simultaneous enhancement in the activity, selectivity and durability. In addition, we have deeply examined the opportunities and major challenges for the development of binary alloy and high entropy catalysts. Binary alloys and high-entropy materials are becoming the centerpiece of the development of next-generation high-efficiency carbon-recycling catalysts due to their unique electronic structure tunability, synergistic active sites, and excellent stability.