关键字：electrocatalyst; hydrogen evolution reaction; microwave; osmium
摘要：Orbital hybridization is a promising approach to modulating the electronic structure of the designed electrocatalysts to boost reaction kinetics. In contrast to d-d hybridization, p-d orbital hybridization between p-block elements and d-block metals can provide new opportunities to modulate the electronic properties and thus promote the catalytic performance. Herein, a phosphorus-doped osmium (P-Os) catalyst is designed through ultrafast (20 s) microwave plasma engineering. Theoretical calculations verify the d-p orbital hybridization between P and Os, leading to the modulation of the d-band center of the Os active site. Specifically, P neighboring Os exhibit the highest catalytic activity, facilitating crucial processes such as H2O/H* adsorption and dissociation. The overpotential of P-Os in alkaline seawater is only 152 mV at 1 A cm-2, which is superior to the reported seawater electrocatalysts. Moreover, the synthesized P-Os catalysts are integrated into an anion exchange membrane (AEM) electrolyzer, demonstrating remarkable performance. The AEM electrolyzer requires 1.86/2.02 V to achieve 500/1000 mA cm-2 current densities. Then, the achieved P-Os have great potential for practical electrocatalytic water-splitting applications. Ultrafast microwave is developed for the first time to synthesize P-doped Os (P-Os). P doping effectively improves the electronic structure of Os and its proton adsorption/desorption capacity. The designed P-Os possess low overpotentials for HER with 34/108 mV in 1.0 m KOH to obtain 10/500 mA cm-2. An assembled AEM electrolyzer can work continuously for 100 h, proving the potential application of P-Os. image
卷号：34
期号：48
是否译文：否