Journal
ACS CATALYSIS
Volume 12, Issue 10, Pages 6092-6099Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c00819
Keywords
magnesium metal-organic frameworks; two-electron O-2 reduction reaction; in situ Raman spectroscopy; in situ infrared spectroscopy; density functional theory
Categories
Funding
- National Natural Science Foundation of China [22072015]
- Program for Science & Technology Innovation Talents in Universities of Henan Province [20HASTIT028]
Ask authors/readers for more resources
Direct electrosynthesis of H2O2 via a two-electron oxygen reduction reaction (2e(-) ORR) under ambient conditions has the potential to replace energy-consuming and waste-intensive processes. This study presents a conductive two-dimensionally layered Mg-3(hexaiminotriphenylene)(2) electrocatalyst with high catalytic efficiency and selectivity for H2O2 production. In situ spectroscopic monitoring and kinetic studies provide insights into the reaction mechanism and the role of the Mg2+ center as the active site.
Direct electrosynthesis of H2O2 via a two-electron oxygen reduction reaction (2e(-) ORR) under ambient conditions is emerging as a promising solution toward on-site applications for the replacement of the energy-consuming, waste-intensive, and indirect anthraquinone process. To date, state-of-the-art 2e(-) ORR catalysis is mostly performed with transition-metal-based materials, while main-group element-based catalysts are much less established, for which there is an urgent need of proper understanding. Herein, we report a conductive two-dimensionally layered Mg-3(hexaiminotriphenylene)(2) electrocatalyst for selective hydro-genation of O-2 to synthesize H2O2 (selectivity >90%) with a robust high catalytic efficiency. In situ spectroscopic monitoring of the catalytic reactions and kinetic studies not only illustrate the reaction mechanisms on Mg-3(hexaiminotriphenylene)(2) but confirm that the Mg2+ center serving as the real active site is responsible for the critical intermediate OOH* forming event. Additionally, in-depth density functional theory calculations further discuss the excellent activity and selectivity of Mg-3(hexaiminotriphenylene)(2) for H2O2 production.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available