期刊
CATALYSIS SCIENCE & TECHNOLOGY
卷 12, 期 19, 页码 5899-5907出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d2cy01135b
关键词
-
资金
- National Natural Science Foundation of China [51979081, 52100179]
- Fundamental Research Funds for the Central Universities [B210202052]
- China Postdoctoral Science Foundation [2020M680063, 2021T140176]
- PAPD
In this study, ultrathin g-C3N4 nanosheets with high H2O2 generation rate were successfully prepared by modifying the g-C3N4 precursor with iodine ions. Moreover, excited states calculations revealed that the modified nanosheets exhibited better O-2 activation ability. This study is of great importance for understanding the mechanism of photocatalytic H2O2 production and exploring the photocatalytic applications of other semiconductors.
Graphitic carbon nitride (g-C3N4) being a non-metallic oxygen reduction reaction (ORR) photocatalyst has attracted much attention in the generation of H2O2. Nevertheless, the weak O-2 adsorption capacity and inefficient separation of charge carriers greatly restrict the production efficiency of H2O2. Herein, iodine ions were used as invisible chemical scissors to tailor the tubular g-C3N4 (TCN) precursor, and relatively ultrathin g-C3N4 nanosheets were prepared (TCN/NaI). The obtained TCN/NaI exhibits alkali metal (Na+) and hydroxyl (-OH) co-modification, and shows the highest H2O2 generation rate (1935.61 mu M h(-1)), greatly exceeding that of bulk g-C3N4 (BCN, 31.96 mu M h(-1)) and TCN (129.32 mu M h(-1)). In addition, excited states calculations of BCN + O-2 and TCN/NaI + O-2 further reveal that the electron of the beta spin-orbital in TCN/NaI can transfer to the pi* orbital of O-2 more easily than that in BCN, thus enhancing the activation of O-2. This work not only provides in-depth insights into the photocatalytic ORR for the H2O2 production mechanism, but also shows that the synergy of structure modification and doping can be further expanded to other semiconductors for photocatalytic applications.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据