Chen Sheng, Wu Yujie, Jie Shanshan, Au Chak Tong, Liu Zhigang
State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University Changsha 410082 China
College of Chemistry and Chemical Engineering, Hunan Institute of Engineering Xiangtan 411104 China.
RSC Adv. 2019 Mar 25;9(17):9462-9467. doi: 10.1039/c9ra00672a. eCollection 2019 Mar 22.
Heteroatom doping has been demonstrated to be an effective strategy for improving the performance of catalysts. In this paper, cobalt carbon catalysts co-doped with nitrogen and sulfur (N and S) were synthesized through a hydrothermal method with chelate composites involving melamine, thioglycolic acid (CHOS), and tetrahydrate cobalt acetate (Co(OAc)·4HO). In addition, the selective oxidation of ethylbenzene under solvent-free conditions with molecular oxygen was used as a probe reaction to evaluate the activity of the catalysts. The optimized catalyst shows an ethylbenzene conversion of 48% with an acetophenone selectivity of 85%. Furthermore, the catalysts were systematically characterized by techniques such as TEM, SEM, XRD, Raman, and XPS. The results reveal that the species of cobalt sulfides and synergistic effects between N and S has inserted a key influence on their catalytic performance.
杂原子掺杂已被证明是提高催化剂性能的有效策略。本文通过水热法,以三聚氰胺、巯基乙酸(CHOS)和四水合醋酸钴(Co(OAc)·4HO)的螯合复合物合成了氮硫共掺杂的钴碳催化剂。此外,以分子氧在无溶剂条件下对乙苯的选择性氧化作为探针反应来评估催化剂的活性。优化后的催化剂乙苯转化率为48%,苯乙酮选择性为85%。此外,还通过透射电子显微镜(TEM)、扫描电子显微镜(SEM)、X射线衍射(XRD)、拉曼光谱和X射线光电子能谱(XPS)等技术对催化剂进行了系统表征。结果表明,硫化钴物种以及氮和硫之间的协同效应对其催化性能有着关键影响。