Li Jingwen, Lan Yingying, Yi Chengfeng, Liu Zhigang
Advanced Catalytic Engineering Research Centre of the Ministry of Education, College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, China.
Nanoscale. 2024 Sep 26;16(37):17426-17432. doi: 10.1039/d4nr02927e.
Enhancing the exposure of metal active sites and maximizing metal atom utilization are critical challenges in heterogeneous catalysis. To solve these issues, heterogeneous catalysts are usually activated by chemicals. Herein, potassium chloride (KCl) was used as an activator to prepare cobalt-nitrogen co-doped (Co-N) hollow periodic mesoporous organosilica spheres (Co-N/HPMOs-KCl). Co-N/HPMOs-KCl showed outstanding catalytic activity for the selective oxidation of ethylbenzene to acetophenone, with a conversion of up to 94.0% for ethylbenzene and a high selectivity of 98.4% towards acetophenone. Additionally, Co-N/HPMOs-KCl maintained excellent catalytic performance for the oxidation of ethylbenzene after six cycles. The excellent performance of Co-N/HPMOs-KCl was attributed to the activation of KCl, which increased the specific surface area of the catalyst and thus facilitated the exposure of more metal active sites. After the removal of unstable metal species through further acid treatment, the remaining metal active sites were thus fully exposed and stably embedded in the framework of the hollow periodic mesoporous organosilica spheres (HMPOs). This work presents an efficient catalyst and offers new insights for the improvement of heterogeneous catalysts.
提高金属活性位点的暴露程度并最大化金属原子利用率是多相催化中的关键挑战。为了解决这些问题,多相催化剂通常通过化学物质进行活化。在此,氯化钾(KCl)被用作活化剂来制备钴氮共掺杂(Co-N)的中空周期性介孔有机硅球(Co-N/HPMOs-KCl)。Co-N/HPMOs-KCl对乙苯选择性氧化为苯乙酮表现出出色的催化活性,乙苯转化率高达94.0%,对苯乙酮的选择性高达98.4%。此外,Co-N/HPMOs-KCl在六个循环后仍保持对乙苯氧化的优异催化性能。Co-N/HPMOs-KCl的优异性能归因于KCl的活化作用,它增加了催化剂的比表面积,从而促进了更多金属活性位点的暴露。通过进一步的酸处理去除不稳定的金属物种后,剩余的金属活性位点得以充分暴露并稳定地嵌入中空周期性介孔有机硅球(HMPOs)的骨架中。这项工作展示了一种高效的催化剂,并为多相催化剂的改进提供了新的见解。