Boosting electrochemical H2O2 synthesis via zinc doping in nickel hydroxide for enhanced activity and stability
摘要
As a highly promising route for hydrogen peroxide (H2O2) synthesis, the two-electron oxygen reduction reaction (2e− ORR) relies on oxygen as the feedstock. However, transition metal hydroxide catalysts for 2e− ORR suffer from low H2O2 selectivity and poor long-term stability. Additionally, the intrinsic mechanism by which metal cation doping regulates their catalytic activity and reaction pathways remains unclear. To address these challenges, this study adopts a hydrothermal synthesis approach, incorporating zinc ions (Zn2+) into the lattice of nickel hydroxide [Ni(OH)2] to construct a Zn-Ni(OH)2 composite catalyst. XRD and XPS results collectively confirm that Zn doping modulates both the crystal structure and electronic properties of Ni(OH)2. These structural and electronic modifications optimize the end-on adsorption of the key *OOH intermediate, thereby enhancing the catalytic stability and delivering superior 2e− ORR performance. Under alkaline conditions, the Zn-Ni(OH)2 catalyst achieves a H2O2 production rate of 6.78 ± 0.23 mol g(cat)−1 h−1, with a selectivity reaching up to 97.7% and a Faraday efficiency (FE) of 86.52 ± 2.7%. Notably, the catalyst demonstrates outstanding long-term stability compared to most reported transition metal hydroxide-based catalysts, showing only ~ 10% performance decay after 10 h of continuous operation. Furthermore, the in-situ generated H2O2 on the Zn-Ni(OH)2 catalyst triggers a Fenton-like reaction, yielding highly reactive hydroxyl radicals that enable efficient degradation of organic pollutants. This study offers a novel approach for the advancement of transition metal hydroxide catalysts for H2O2 production.
Graphical abstract