Carbon‐Shielded Single‐Atom Alloy Material Family for Multi‐Functional Electrocatalysis
Yueyu Tong, Jiaxin Liu, Jiaxin Liu, Liqun Wang, Bing‐Jian Su, Kuang‐Hsu Wu, Jenh‐Yih Juang, Feng Hou, Lichang Yin, Shi Xue Dou, Jian Liu, Jian Liu, Ji Liang
Abstract
Abstract Encapsulating metal‐based catalysts inside carbon sheaths is a frequently‐adopted strategy to enhance their durability under various harsh situations and improve their catalytic activity simultaneously. Such carbon encapsulation, however, imposes significant complications for directly modifying materials’ surface atomic/electronic configurations, fundamentally impeding the accurate tuning of their catalytic capabilities. Herein, a universal single‐atom alloy (SAA) strategy is reported to indirectly yet precisely manipulate the surface electronic structure of carbon‐encapsulated electrocatalysts. By versatilely constructing a SAA core inside an N‐doped carbon sheath, material's electrocatalytic capability can be flexibly tuned. The one with Ru‐SAA cores serves as an excellent bifunctional electrocatalyst for oxygen/hydrogen evolution, exhibiting minimal cell voltage of 1.55 V (10 mA cm −2 ) and outstanding mass activity of 1251 mA m for overall water splitting, while the one with Ir‐SAA cores possesses superior oxygen reduction activity with a half‐wave potential of 919 mV. Density functional theory calculations reveal that the doped atoms can simultaneously optimize the adsorption of protons (H*) and oxygenated intermediates (OH*, O*, and OOH*) to achieve the remarkable thermoneutral hydrogen evolution and enhanced oxygen evolution. This work thus demonstrates a versatile strategy to precisely modify the surface electronic properties of carbon‐shielded materials for optimized performances.