Tang Haiyan, Zhang Jin, Huang Meng, Zhang Jie, Zhou Yufeng, Wang Gang, Wang Ruilin, Chen Jinwei
College of Materials Science and Engineering, Sichuan University, Chengdu 610065, China.
College of Materials Science and Engineering, Sichuan University, Chengdu 610065, China; Engineering Research Center of Alternative Energy Materials & Devices, Ministry of Education, Chengdu 610065, China.
J Colloid Interface Sci. 2022 Oct 15;624:527-536. doi: 10.1016/j.jcis.2022.05.164. Epub 2022 May 31.
The single atom catalysts have been widely studied in the catalytic reaction due to their 100% atomic utilization and ultra-high catalytic activity. However, the catalytic removal of formaldehyde on single atom catalysts have not been studied extensively and its catalytic mechanism is still unclear. In this work, atomically dispersed Co catalysts anchored in porous nitrogen-doped carbon were synthetized and the coordination environment of single Co atoms were further proved by the results of XAFS spectrum. The optimal atomically dispersed Co catalysts preformed outstanding removal performance for low-concentration HCHO (∼1 ppm) at room temperature. Furthermore, DFT calculations reveal the HCHO removal mechanism on atomically dispersed Co catalysts, which showed that HCHO molecules can react with O molecules adsorbed on single-atom Co sites through the Langmuir-Hinshelwood (L-H) pathway to generate CO and HO at room temperature (HCHO → HCOO* → CO). This work provides a promising lead for exploring single-atom Co catalysts for HCHO oxidation.
由于单原子催化剂具有100%的原子利用率和超高的催化活性,因此在催化反应中得到了广泛的研究。然而,单原子催化剂对甲醛的催化去除尚未得到广泛研究,其催化机理仍不清楚。在这项工作中,合成了锚定在多孔氮掺杂碳中的原子分散钴催化剂,XAFS光谱结果进一步证明了单个钴原子的配位环境。优化后的原子分散钴催化剂在室温下对低浓度HCHO(约1 ppm)表现出优异的去除性能。此外,DFT计算揭示了原子分散钴催化剂上的HCHO去除机理,结果表明,HCHO分子可以通过Langmuir-Hinshelwood(L-H)途径与吸附在单原子钴位点上的O分子反应,在室温下生成CO和HO(HCHO→HCOO*→CO)。这项工作为探索用于HCHO氧化的单原子钴催化剂提供了一个有前景的线索。