摘要
The low intrinsic activity of Fenton catalytic site and high demand for light-energy input inhibit the organic-pollution control efficiency of photo-Fenton process.Here,through structural design with density functional theory(DFT)calculations,Ce is predicted to enable the construction of coordinatively unsaturated metal centers(CUCs)in Prussian blue analogue(PBA),which can strongly adsorb H_(2)O_(2)and donate sufficient electrons for directly splitting the O-O bond to produceOH.Using a substitution-co-assembly strategy,binary Ce-Fe PBA is then prepared,which rapidly degrades sulfamethoxazole with the pseudo-first-order kinetic rate constant exceeding reported values by 1-2 orders of magnitude.Meanwhile,the photogenerated electrons reduce Fe(Ⅲ)and Ce(Ⅳ)to promote the metal valence cycle in CUCs and make sulfamethoxazole degradation efficiency only lose 6.04%in 5 runs.Overall,by introducing rare earth metals into transition metal-organic frameworks,this work guides the whole process for highly active CUCs from design and construction to mechanism exploration with DFT calculations,enabling ultrafast and stable photo-Fenton catalysis.
基金
supported by the National Natural Science Foundation of China(No.22072064,51522805,51908273,and 22176086)
the State Key Laboratory of Pollution Control and Resource Reuse(PCRR-ZZ-202106)
Start-Up Funds for Jiangsu Distinguished Professor.
作者简介
Wenting Zheng,Dr.,contributed equally to this work;Changqing Zhu,Dr;Cailiang Yue,Dr;Wenlei Zhu,Prof.,Dr;Fuqiang Liu,Prof.,Dr.,E-mail:lfq@nju.edu.cn;Hui Guo,Dr.,contributed equally to this work;Zhaoxu Chen,Prof.,Dr.,E-mail:zxchen@nju.edu.cn
