Shifting the O2 reduction pathway from H2O to H2O2 via in situ reconstruction of Ti2O3 nanoparticles,Journal of Materials Chemistry A

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Shifting the O2 reduction pathway from H2O to H2O2 via in situ reconstruction of Ti2O3 nanoparticles
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2023-10-09 , DOI: 10.1039/d3ta05092k
Yongchao Yao _{1,

2} , Huiqing Wang ₃ , Kai Dong ₂ , Haobo Li ₄ , Jie Liang ₂ , Ruizhi Li ₂ , Shengjun Sun ₅ , Zhengwei Cai ₅ , Xun He ₅ , Dongdong Zheng ₅ , Yonglan Luo ₂ , Sulaiman Alfaifi ₆ , Dongwei Ma ₄ , Wenchuang (Walter) Hu ₁ , Xuping Sun _{2,

5}

Affiliation

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.

中文翻译：

通过原位重建 Ti2O3 纳米颗粒将 O2 还原途径从 H2O 转变为 H2O2

在环境条件下通过双电子氧还原反应 (2e ⁻ ORR)直接电合成过氧化氢 (H ₂ O ₂ ) 已成为现场应用的一种有前途的解决方案，旨在取代能源密集型、废物利用的方法。生产和间接蒽醌过程。最近的进展集中在开发催化剂以提高其活性和效率。然而，电催化剂在运行过程中的动态演化和原位构建行为常常被忽视。在此，我们研究了在ORR过程中在Ti ₂ O ₃表面形成的缺氧TiO ₂的原位电化学重构过程。^{重构的催化剂表现出从4e -} ORR途径到2e ^-途径的完全转变，在合成H ₂ O ₂方面表现出优异的性能，法拉第效率超过90%。此外，通过密度泛函计算的交叉验证，我们通过原位电化学拉曼和红外光谱验证了相和ORR途径的转变过程。

更新日期：2023-10-13

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