Promotional mechanism of nitrogen-doping in activated carbon for formaldehyde removal: Enhanced attractive noncovalent interactions coupled with Cannizzaro-type disproportionation reaction

歧化 化学 物理吸附 吡啶 吸附 光化学 路易斯酸 无机化学 药物化学 催化作用 有机化学
作者
N. Xiang,Jie Tian,Qiaoyan Li,Yaqin Hou,Zhanggen Huang
出处
期刊:Separation and Purification Technology [Elsevier BV]
卷期号:332: 125761-125761 被引量:2
标识
DOI:10.1016/j.seppur.2023.125761
摘要

Inserting nitrogen (N) heteroatoms into the carbonaceous adsorbents has been confirmed to be one of efficient strategies for enhancing HCHO removal. However, the essential promotion mechanisms of specific N-containing groups (such as pyridinic-N, pyrrolic-N, and quaternary-N) remain blurred. Herein, a series of N-doped activated carbons were prepared by annealing the melamine impregnated activated carbons at 600–900 °C and used for HCHO elimination. It manifested that the HCHO elimination performance of samples was remarkably improved after N-doping and their HCHO adsorption capacities were in the order of ACN-600 (16.37 mg/g) > ACN-750 (9.87 mg/g) > ACN-900 (7.28 mg/g) > AC (5.09 mg/g). DFT calculation results revealed that there existed stronger attractive noncovalent interactions between pyrrolic-N doped carbon and HCHO due to the formation of stronger H-bonds. Therefore, the HCHO physisorption energy on pyrrolic-N doped carbon was the highest (−32.83 kJ/mol). Compared with the single physisorption mechanism of previous studies, the in-situ DRIFTS results manifested that the pyridinic-N atom (as a typical strong Lewis base) could trigger the Cannizzaro-type disproportionation reaction, which would transform toxic HCHO into relatively less toxic methanol and formic acid. Benefiting from the dual enhanced mechanisms of attractive noncovalent interactions and Cannizzaro-type disproportionation reaction, the ACN-600 manifested excellent HCHO removal performance. This study not only intrinsically discloses the promotion mechanism of specific N-containing groups on HCHO removal at molecular level but also provides guidelines for rational design and development of carbonaceous materials for effective HCHO elimination.
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