Regulating active hydrogen supply and intermediate binding for pH-universal H<sub>2</sub>O<sub>2</sub> electrosynthesis at ampere-level current density.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 41315076.
- Also identified by DOI 10.1038/s41467-025-65830-9 and PMC identifier 12663119.
- Licence recorded as CC BY-NC-ND.
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Abstract
Electrocatalytic oxygen reduction is an attractive alternative for sustainable H<sub>2</sub>O<sub>2</sub> production. However, the electrocatalyst still suffers from low H<sub>2</sub>O<sub>2</sub> efficiency due to unsuitable intermediate binding, sluggish active hydrogen (*H) generation in neutral/alkaline solutions and high interfacial proton concentration in acid. Meanwhile, the modulation mechanism remains insufficiently understood. Here we report efficient pH-universal H<sub>2</sub>O<sub>2</sub> electrosynthesis at ampere-level current densities by modulating interfacial microenvironment via sulfonic acid (SO<sub>3</sub>H)-functionalization of carbon nanotubes (SCNT). Experimental and theoretical results show that SO<sub>3</sub>H-functionalization accelerates *H generation from water dissociation for neutral/alkaline H<sub>2</sub>O<sub>2</sub> electrosynthesis while creating more alkaline microenvironment in acid. Moreover, it not only optimizes *OOH binding energy and facilitates *OOH generation, but also reduces the energy barrier for *HOOH desorption (rate-determining step). It exhibits good H<sub>2</sub>O<sub>2</sub> electrosynthesis performance with Faradaic efficiencies of 81.7-97.2% and H<sub>2</sub>O<sub>2</sub> concentrations of 834-1537 mM (0.8 min) at pH 0.7-13 and 1.0-1.5 A cm<sup>-2</sup>. The estimated cost for H<sub>2</sub>O<sub>2</sub> electrosynthesis is 28.5% of industrial anthraquinone process. The on-site application of SCNT has been demonstrated by efficient pollutant degradation and sterilization.