Shifting the O2 reduction pathway from H2O to H2O2via in situ reconstruction of Ti2O3 nanoparticles

被引:26
作者
Yao, Yongchao [1 ,2 ]
Wang, Huiqing [3 ]
Dong, Kai [2 ]
Li, Haobo [4 ]
Liang, Jie [2 ]
Li, Ruizhi [2 ]
Sun, Shengjun [5 ]
Cai, Zhengwei [5 ]
He, Xun [5 ]
Zheng, Dongdong [5 ]
Luo, Yonglan [2 ]
Alfaifi, Sulaiman [6 ]
Ma, Dongwei [4 ]
Hu, Wenchuang [1 ]
Sun, Xuping [2 ,5 ]
机构
[1] Sichuan Univ, West China Hosp, Precis Med Ctr, Dept Lab Med, Chengdu 610041, Sichuan, Peoples R China
[2] Univ Elect Sci & Technol China, Inst Fundamental & Frontier Sci, Chengdu 610054, Sichuan, Peoples R China
[3] Sichuan Univ, West China Univ Hosp 2, Med Simulat Ctr, Chengdu 610041, Sichuan, Peoples R China
[4] Henan Univ, Sch Mat Sci & Engn, Key Lab Special Funct Mat, Minist Educ, Kaifeng 475004, Henan, Peoples R China
[5] Shandong Normal Univ, Coll Chem Chem Engn & Mat Sci, Jinan 250014, Shandong, Peoples R China
[6] King Abdulaziz Univ, Fac Sci, Chem Dept, Jeddah 21589, Saudi Arabia
基金
中国国家自然科学基金;
关键词
HYDROGEN-PEROXIDE; TIO2; SPECTROSCOPY; WATER;
D O I
10.1039/d3ta05092k
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The direct electrosynthesis of hydrogen peroxide (H2O2) through a two-electron oxygen reduction reaction (2e- ORR) under ambient conditions has emerged as a promising solution for on-site applications, aiming to replace the energy-intensive, waste-generating, and indirect anthraquinone process. Recent advancements have focused on developing catalysts to enhance their activity and efficiency. However, the dynamic evolution and in situ construction behavior of electrocatalysts during operation have often been overlooked. Herein, we investigate the in situ electrochemical reconstruction process of oxygen-deficient TiO2, which forms on the surface of Ti2O3 during the ORR process. The reconstructed catalyst exhibits a complete transition from a 4e- ORR pathway to a 2e- pathway, exhibiting exceptional performance in synthesizing H2O2 with a faradaic efficiency exceeding 90%. Furthermore, by cross-confirmation with density functional calculations, we validate the transition process of the phase and ORR pathway by in situ electrochemical Raman and infrared spectroscopy.
引用
收藏
页码:22154 / 22160
页数:7
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