Scalable Synthesis of Ir Cluster Anchored on Porous Hollow Carbon Nanobowls for Enhancing pH-Universal Hydrogen Evolution

Design high-loading with superior activity and high atomic efficiency has consistently been a new frontier of heterogeneous catalysis while challenging in synthetic technology. In this work, a universal solid-state strategy is proposed for large scalable production of high-loading Ir clusters on porous hollow carbon nanobowls (Ir CSs/PHCNBs). The strong electronic interaction between metallic Ir cluster and C on PHCNBs leads to electron redistribution, which significantly improves the electron transfer rate on the interface. The obtained Ir CSs/PHCNBs only require overpotentials of 35, 34, and 37 mV for the hydrogen evolution reaction (HER) with stable outputting of 10 mA cm-2 under acidic, alkaline, and neutral conditions, respectively, which exceeds the state-of-the-art HER electrocatalysts. Meanwhile, the Tafel slopes of Ir CSs/PHCNBs for the HER process are 23.07, 48.76, and 28.95 mV dec-1, greatly lower than that of PHCNBs (152.73, 227.96, and 140.29 mV dec-1) and commercial Pt/C (20%) (36.33, 66.10, and 36.61 mV dec-1). These results provide a new strategy for the universal synthesis of clusters catalysts and insight into understanding the interface effects between clusters and carbon substrate, facilitating the industrial application of hydrogen production. The Ir clusters anchoring on porous hollow carbon nanobowls (Ir CSs/PHCNBs) are synthesized by an interface atomic diffusion control technology of a universal solid-state strategy, which exhibits lower overpotentials for HER in pH-universal conditions due to the increasing Ir charge density at the heterointerface that are favorable for H2O adsorption and activation and H* adsorption/desorption.image