Reveal Bronsted-Evans-Polanyi relation and attack mechanisms of reactive oxygen species for photocatalytic H2O2 production

Luo, Jun ¹Fan, Changzheng ¹Tang, Lin ¹Liu, Yani ²Gong, Zhixuan ¹Wu, Tangshan ¹Zhen, Xinlan ¹Feng, Chengyang ¹Feng, Haopeng ¹Wang, Lingling ³Xu, Liang ⁴Yan, Ming¹

扫码查看

作者信息

1. Hunan Univ, Coll Environm Sci & Engn, Key Lab Environm Biol & Pollut Control, Minist Educ, Changsha 410082, Hunan, Peoples R China
2. Hunan Res Acad Environm Sci, Key Lab Water Pollut Control Technol, Changsha 410004, Peoples R China
3. Hunan Univ, Sch Phys & Elect, Key Lab Micronano Phys & Technol Hunan Prov, Changsha 410082, Hunan, Peoples R China
4. Jiangxi Univ Sci & Technol, Energy Mat Comp Ctr, Nanchang 330013, Jiangxi, Peoples R China
折叠

Abstract

The generation of H+ by active species attacking proton donor (PD) is a key step in photocatalytic H2O2 production (PHP). Deeply analyzing the involved mechanism may be a crucial factor to break through the bottleneck of H2O2 yield. Here, nitrogen-deficient and boron-doped g-C3N4 are synthesized for PHP and the interaction mechanisms between active species and PD are revealed. The prepared photocatalyst exhibits a high H2O2 production rate (455 mu M h-1 g-1). The 1O2, center dot O2- and hole promoted by modification site dominate twelve different reaction mechanisms, respectively. For the oxidation pathways dominated by hole, H2O2 generation is limited by the dissociation of PD or desorption of H+ on catalyst surface. Interestingly, center dot O2- and 1O2 could directly attack PD, or diffuse into solution to react with PD to produce H2O2 with lower barriers. Moreover, there is a synergistic effect between doped-boron, 1O2 and water bridge, which further reduces the reaction barrier.

Key words

DFT/Bronsted-Evans-Polanyi relation/Reaction mechanism/Reactive oxygen species/Photocatalytic H(2)O(2 )production

引用本文复制引用

出版年

2022

Applied Catalysis

ISSN：0926-3373

被引量35

参考文献量56

段落导航