Li Xuning, Huang Xiang, Xi Shibo, Miao Shu, Ding Jie, Cai Weizheng, Liu Song, Yang Xiaoli, Yang Hongbin, Gao Jiajian, Wang Junhu, Huang Yanqiang, Zhang Tao, Liu Bin
School of Chemical and Biomedical Engineering , Nanyang Technological University , 62 Nanyang Drive , Singapore 637459 , Singapore.
Department of Physics , Southern University of Science and Technology , Shenzhen 518055 , People's Republic of China.
J Am Chem Soc. 2018 Oct 3;140(39):12469-12475. doi: 10.1021/jacs.8b05992. Epub 2018 Sep 7.
The Fenton-like process presents one of the most promising strategies to generate reactive oxygen-containing radicals to deal with the ever-growing environmental pollution. However, developing improved catalysts with adequate activity and stability is still a long-term goal for practical application. Herein, we demonstrate single cobalt atoms anchored on porous N-doped graphene with dual reaction sites as highly reactive and stable Fenton-like catalysts for efficient catalytic oxidation of recalcitrant organics via activation of peroxymonosulfate (PMS). Our experiments and density functional theory (DFT) calculations show that the CoN site with a single Co atom serves as the active site with optimal binding energy for PMS activation, while the adjacent pyrrolic N site adsorbs organic molecules. The dual reaction sites greatly reduce the migration distance of the active singlet oxygen produced from PMS activation and thus improve the Fenton-like catalytic performance.
类芬顿过程是产生含活性氧自由基以应对日益严重的环境污染的最具前景的策略之一。然而，开发具有足够活性和稳定性的改进型催化剂仍是实际应用的长期目标。在此，我们展示了锚定在具有双反应位点的多孔氮掺杂石墨烯上的单钴原子，作为高活性和稳定的类芬顿催化剂，通过活化过一硫酸盐（PMS）对难降解有机物进行高效催化氧化。我们的实验和密度泛函理论（DFT）计算表明，具有单个钴原子的CoN位点作为PMS活化的具有最佳结合能的活性位点，而相邻的吡咯氮位点吸附有机分子。双反应位点极大地缩短了PMS活化产生的活性单线态氧的迁移距离，从而提高了类芬顿催化性能。
