Modulation of the charge transfer behavior of Ni(II)-doped NH2-MIL-125(Ti): Regulation of Ni ions content and enhanced photocatalytic CO2 reduction performance

被引:113
作者
Chen, Siyuan [1 ]
Hai, Guangtong [1 ]
Gao, Hongyi [1 ,3 ]
Chen, Xiao [2 ]
Li, Ang [4 ]
Zhang, Xiaowei [2 ]
Dong, Wenjun [1 ]
机构
[1] Univ Sci & Technol Beijing, Sch Mat Sci & Engn, Beijing Key Lab Funct Mat Mol & Struct Construct, Beijing 100083, Peoples R China
[2] Beijing Normal Univ, Inst Adv Mat, Beijing 100875, Peoples R China
[3] Univ Sci & Technol Beijing, Shunde Grad Sch, Foshan 528399, Peoples R China
[4] Suzhou Univ Sci & Technol, Sch Chem Biol & Mat Engn, Suzhou 215009, Peoples R China
基金
中国国家自然科学基金;
关键词
Modulation; Charge transfer; Metal organic frameworks; Nickel ion dopants; Photocatalytic CO2 reduction; METAL-ORGANIC FRAMEWORK; CATALYST; EFFICIENT; OXIDE; DEGRADATION; NANOSHEETS; EVOLUTION; DESIGN; WATER; MOF;
D O I
10.1016/j.cej.2020.126886
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Regulation of the electronic structure of metal oxo clusters in metal organic frameworks (MOFs) is a promising way to modulate charge transfer efficiency and photocatalytic performance. Herein, a series of Ni2+ doped NH2-MIL-125-Ti (NH2-MIL-125-Ni-x/Ti) with different Ni2+/Ti4+ molar ratio (x = 0.5%-1.5%) are prepared via an in-situ doping method. Correlations between the electronic structure of (Ti/Ni)(8)O-8(OH)(4) nodes and charge transfer efficiency, bandgap and energy position of band edges of the NH2-MIL-125-Ni-x/Ti are systematically investigated based on experimental and computational method. The doped Ni2+ was confirmed to be an efficient mediator to promote the electron transfer from photoexcited terephthalate ligand to the (Ti/Ni)(8)O-8(OH)(4) nodes in NH2-MIL-125-Ni-x/Ti. The NH2-MIL-125-Ni-1%/Ti exhibited the highest CO2 conversion rate with 98.6% CO selectivity and the factors affecting the photocatalytic CO2 reduction performance are also studied. It provides some guidance for developing MOFs photocatalyst with targeted performance via modification of the electronic structure of metal oxo clusters.
引用
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页数:9
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