Wang Junhui, Yu Jiaxing, Fu Qi, Yang Huangsheng, Tong Qing, Hao Zhengping, Ouyang Gangfeng
MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen University, Guangzhou, Guangdong 510275, China.
School of Materials Science and Engineering, Sun Yat-Sen University, Guangzhou, Guangdong 510275, China.
ACS Cent Sci. 2021 Feb 24;7(2):355-364. doi: 10.1021/acscentsci.0c01600. Epub 2021 Jan 11.
Holes ( ) on heterogeneous photocatalysts could act as important oxidative species or precursors for reactive oxygen species (ROS). However, due to the ultrafast recombination of photoinduced electrons and holes, a majority of carriers are consumed prior to surface reactions. Herein, we report an unprecedented nonphotomediated hole oxidation system constructed from carbon nanotubes (CNTs) and superoxides. This system exhibited high catalytic activity for the degradation of organic pollutants, which outperforms the classical oxidation processes in the remediation of actual wastewater and is comparable to that of the best single cobalt atom catalyst. Theoretical and experimental results reveal that the intrinsic defects with unpaired spins on CNTs served as adsorptive sites to activate superoxides. This is the first report on exploring the oxidation properties of nonphotomediated hole carriers on heterogeneous catalysts, which will be of broad interest for researchers in environmental remediation, chemical synthesis, and biological fields.
异质光催化剂上的空穴（ ）可作为重要的氧化物种或活性氧（ROS）的前体。然而，由于光生电子和空穴的超快复合，大多数载流子在表面反应之前就被消耗掉了。在此，我们报道了一种由碳纳米管（CNT）和超氧化物构建的前所未有的非光介导空穴氧化体系。该体系对有机污染物的降解表现出高催化活性，在实际废水修复中优于传统氧化工艺，与最佳的单钴原子催化剂相当。理论和实验结果表明，碳纳米管上具有未成对自旋的固有缺陷作为吸附位点来激活超氧化物。这是首次探索非光介导空穴载流子在异质催化剂上的氧化性质的报告，这将引起环境修复、化学合成和生物领域研究人员的广泛兴趣。
