Li Jiaqi, Mei Yuqing, Ma Shouchun, Yang Qingfeng, Jiang Baojiang, Xin Baifu, Yao Tongjie, Wu Jie
Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education, School of Chemistry and Materials Science, Heilongjiang University, Harbin, China.
State Key Lab Urban Water Resource and Environment, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, China.
J Colloid Interface Sci. 2022 Feb 15;608(Pt 2):2075-2087. doi: 10.1016/j.jcis.2021.10.119. Epub 2021 Oct 28.
Herein, a type-I phosphorus-doped carbon nitride/oxygen-doped carbon nitride (P-CN/O-CN) heterojunction was designed for photocatalysis-self-Fenton reaction (photocatalytic HO production and following Fenton reaction). In P-CN/O-CN, the photoinduced charge carriers were effectively separated with the help of internal-electric-field near the interface, ensuring the high catalytic performance. As a result, the production rate of HO in an air-saturated solution was 179 μM·h, about 7.2, 2.5, 2.5 and 2.1 times quicker than that on CN, P-CN, O-CN, and phosphorus and oxygen co-doped CN, respectively. By taking advantage of the cascade mode in photocatalysis-self-Fenton reaction, HO utilization efficiency was remarkably improved to 77.7%, about 9.0 times higher than that of traditional homogeneous Fenton reaction. Befitting from the superior yield and utilization efficiency, the degradation performance of P-CN/O-CN was undoubtedly superior than other photocatalysts. This work well addressed two bottlenecks in traditional Fenton reaction: source of HO and their low utilization efficiency, and the findings were beneficial to understand the mechanism and advantage of the photocatalysis-self-Fenton system in environmental remediation.
在此，设计了一种I型磷掺杂氮化碳/氧掺杂氮化碳（P-CN/O-CN）异质结用于光催化自芬顿反应（光催化产生羟基自由基以及后续的芬顿反应）。在P-CN/O-CN中，光生载流子在界面附近内建电场的帮助下有效分离，确保了高催化性能。结果，在空气饱和溶液中羟基自由基的产生速率为179 μM·h，分别比在CN、P-CN、O-CN以及磷氧共掺杂CN上快约7.2倍、2.5倍、2.5倍和2.1倍。通过利用光催化自芬顿反应中的级联模式，羟基自由基的利用效率显著提高到77.7%，比传统均相芬顿反应高约9.0倍。得益于优异的产率和利用效率，P-CN/O-CN的降解性能无疑优于其他光催化剂。这项工作很好地解决了传统芬顿反应中的两个瓶颈：羟基自由基的来源及其低利用效率，这些发现有助于理解光催化自芬顿体系在环境修复中的机理和优势。
