苄胺
共价键
接受者
光催化
光化学
化学
联轴节(管道)
调制(音乐)
有机化学
材料科学
催化作用
哲学
物理
美学
冶金
凝聚态物理
作者
Jinfang Kou,Ganping Wang,Hongyan Guo,Liang Li,Jian Fang,Jiantai Ma,Zhengping Dong
标识
DOI:10.1016/j.apcatb.2024.124020
摘要
The strong excitonic effect is widely prevalent in covalent organic frameworks (COFs)-based catalysts, while the high exciton binding energies (Eb) of COFs seriously limit their photocatalytic performance. Herein, theoretical calculations are conducted to evaluate the Eb values of potential COFs derived from benzo[1,2-b:3,4-b'-b'']trithiophene-2,5,8-tricarbaldehyde (BTT) and 2,4,6-trihydroxybenzene-1,3,5-tricarbaldehyde (Bp) as aldehyde monomers. Diverse aromatic amine linkers including dipyridine diamine (BPy), biphenyl diamine (BPh), and p-phenylenediamine (MPh) with different molecular lengths and N-sites are used as linker models to regulate the excitonic effect. The obtained BTT-BPy-COF with a long BPy linker and the lowest calculated Eb value possesses the best photocatalytic performance for benzylamine coupling, with conversion and selectivity up to 99% accompanied by a high oxidation rate, outperforming most of the reported works. Further mechanistic investigation reveals that the bipyridine-N sites in BTT-BPy-COF exhibit strong electron transfer as well as enhanced O2 adsorption and activation that is beneficial to photocatalytic benzylamine coupling.
科研通智能强力驱动
Strongly Powered by AbleSci AI