Nanoconfined impulse synthesis of high-entropy nanocarbides for active and stable electrocatalysis
摘要
Nanocarbides exhibit interesting mechanical properties and strong oxidation and corrosion resistance. The use of high-entropy effects has enhanced the performance of nanomaterials and enabled new functionalities. Despite the successful development of high-entropy nanoalloys and nanoceramics, controlled synthesis of high-entropy nanocarbides (HENCs) remains challenging due to high growth temperatures, agglomeration of nanoproducts and multi-component immiscibility. Here we achieve synthesis of HENCs containing 5–22 metal elements through a nanoconfined impulse synthetic strategy enabled by Joule heating-induced in situ reactions in carbon nanotube films. These HENCs exhibit multi-element effects and enhanced electrocatalytic activities due to nanoscale size and modification of catalytic sites. In particular, (Pt0.15WTaFe0.15Ni)Cx is highly stable for the hydrogen evolution reaction at 5 A cm−2 and demonstrates low overall-water-splitting cell voltages under industrial conditions. Moreover, (Pt0.5WTaHfCe)Cx shows high mass activities for alcohol oxidation. Density functional theory calculations elucidate the mechanism by which specific sites are modified to achieve optimal adsorption capabilities in HENC catalysts. These results demonstrate the promise of our approach for the synthesis of high performance HENC electrocatalysts.