Zhang Guobing, Zhao Mingshi, Su Linghui, Yu Hao, Wang Chenxi, Sun Dengrong, Ding Yunsheng
Special Display and Imaging Technology Innovation Center of Anhui Province, Academy of Optoelectronic Technology, Anhui Province Key Laboratory of Measuring Theory and Precision Instrument, Hefei University of Technology, Hefei 230009, China.
Key Laboratory of Advance Functional Materials and Devices of Anhui Province, School of Chemistry and Chemical Engineering, Hefei University of Technology, Hefei 230009, China.
ACS Appl Mater Interfaces. 2023 Apr 26;15(16):20310-20316. doi: 10.1021/acsami.3c00786. Epub 2023 Mar 30.
Donor-acceptor two-dimensional covalent-organic frameworks (COFs) have great potential as photocatalysts for hydrogen evolution because of their tunable structures, ordered and strong stacking, high crystallinity, and porosity. Herein, an acceptor unit, namely phthalimide, has been employed for the first time to construct COFs. Two donor-acceptor COFs ( and ) have been successfully synthesized via a Schiff base reaction using phthalimide as the acceptor and 1,3,6,8-tetrakis(4-aminophenyl)pyrene () and 1,3,5-tris(4-aminophenyl)benzene () as donors. The synthesized COFs exhibited high crystallinity, permanent porosity, excellent chemical stability, suitable band gaps, and broad visible-light absorption. In the presence of ascorbic acid (sacrificial reagent), the COF exhibited an efficient photocatalytic performance with a hydrogen evolution rate of 1763 μmol g h. Moreover, the photocatalytic performance was further improved by the addition of Pt (1 wt %) as a cocatalyst, and the hydrogen evolution rate reached 2718 μmol g h.
供体-受体二维共价有机框架（COF）由于其可调节的结构、有序且紧密的堆积、高结晶度和孔隙率，作为光催化析氢材料具有巨大潜力。在此，首次采用受体单元即邻苯二甲酰亚胺来构建COF。通过席夫碱反应，以邻苯二甲酰亚胺为受体，1,3,6,8-四（4-氨基苯基）芘（）和1,3,5-三（4-氨基苯基）苯（）为供体，成功合成了两种供体-受体COF（和）。合成的COF表现出高结晶度、永久孔隙率、优异的化学稳定性、合适的带隙以及宽泛的可见光吸收。在抗坏血酸（牺牲试剂）存在下，COF表现出高效的光催化性能，析氢速率为1763 μmol g h。此外，通过添加1 wt%的Pt作为助催化剂，光催化性能进一步提高，析氢速率达到2718 μmol g h。
