Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 28, Pages 33182-33187Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c09871
Keywords
TiC; amorphous TiO2-x; 2e(-) oxygen reduction; H2O2 production; density functional theory
Funding
- National Natural Science Foundation of China [22072015, 12074099]
- Key Research Program from Science and Technology Department of Sichuan Province [20ZDYF2773]
- Program for Science & Technology Innovation Talents in Universities of Henan Province [20HASTIT028]
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An acid oxidation strategy is proposed to boost the 2e(-) ORR activity of metallic TiC by generating a surface amorphous oxygen-deficient TiO2-x layer, resulting in high H2O2 selectivity and stability.
The electrochemical oxygen reduction reaction (ORR) is regarded as an attractive alternative to the anthraquinone process for sustainable and on-site hydrogen peroxide (H2O2) production. It is however hindered by low selectivity due to strong competition from the four-electron ORR and needs efficient catalysts to drive the 2e(-) ORR. Here, an acid oxidation strategy is proposed as an effective strategy to boost the 2e(-) ORR activity of metallic TiC via in-site generation of a surface amorphous oxygen-deficient TiO2-x layer. The resulting a-TiO2-x/TiC exhibits a low overpotential and high H2O2 selectivity (94.1% at 0.5 V vs reversible hydrogen electrode (RHE)), and it also demonstrates robust stability with a remarkable productivity of 7.19 mol g(cat).(-1) h(-1) at 0.30 V vs RHE. The electrocatalytic mechanism of a-TiO2-x/TiC is further revealed by density functional theory calculations.
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