Mechanisms of direct hydrogen peroxide synthesis on silicon and phosphorus dual-doped graphene: a DFT-D study

Shuo Li; Zhansheng Lu; Yi Zhang; Dongwei Ma; Zongxian Yang

doi:10.1039/c6cp08668c

Mechanisms of direct hydrogen peroxide synthesis on silicon and phosphorus dual-doped graphene: a DFT-D study

Phys Chem Chem Phys. 2017 Mar 29;19(13):9007-9015. doi: 10.1039/c6cp08668c.

Authors

Shuo Li¹, Zhansheng Lu², Yi Zhang¹, Dongwei Ma³, Zongxian Yang⁴

Affiliations

¹ College of Physics and Materials Science, Henan Normal University, Xinxiang 453007, China. zslu@henannu.edu.cn.
² College of Physics and Materials Science, Henan Normal University, Xinxiang 453007, China. zslu@henannu.edu.cn and State Key Laboratory of Surface Physics and Department of Physics, Fudan University, Shanghai 200433, P. R. China.
³ School of Physics, Anyang Normal University, Anyang 455000, China.
⁴ College of Physics and Materials Science, Henan Normal University, Xinxiang 453007, China. zslu@henannu.edu.cn and Collaborative Innovation Center of Nano Functional Materials and Applications, Kaifeng, China.

PMID: 28304021
DOI: 10.1039/c6cp08668c

Abstract

Hydrogen peroxide (H₂O₂) is an important chemical commodity, with demand growing significantly in chemical synthesis due to its green characteristics. The mechanisms of the direct synthesis of hydrogen peroxide (DSHP) on metal-free silicon and phosphorus dual-doped graphene (Si-P-G) catalyst, based on a dispersion-corrected density functional theory (DFT-D) method, are systematically investigated. The most stable Si-P-G catalyst is presented, with the local region of dopants shown to play an important role in the adsorption and reduction of oxygen. A two-electron pathway is probable for DSHP on Si-P-G according to kinetic and thermodynamic analyses. The hydrogenation of O₂ to OOH is the rate-limiting step, with a small barrier energy of 0.66 eV, and the potential energy surface is downhill by Gibbs free energy calculations. All results indicate that Si-P-G is a novel catalyst with high activity and good selectivity for DSHP.