Water oxidation to molecular dioxygen driven by visible light is essential but difficult in solar fuel production due to its sluggish reaction kinetics.Although the catalytic process is highly dependent on the coordin...Water oxidation to molecular dioxygen driven by visible light is essential but difficult in solar fuel production due to its sluggish reaction kinetics.Although the catalytic process is highly dependent on the coordination-unsaturated metal sites in coordination catalysts,the controllable design of catalysts with such catalytic sites remains challenging.Herein,we report two new Co-MOFs(CoBIM-1 and CoBIM-2)for photocatalytic water oxidation under visible light.The coordination environment of Co in Co-MOFs can be easily manipulated by changing the atmosphere and concentration of deprotonated solvent during synthesis.CoBIM-1 with coordinatively unsaturated Co sites showed good performance with an O_(2)production of 2.0 mmol g^(−1)h^(−1),in sharp contrast to its counterpart CoBIM-2.Furthermore,through isotope tracing experiments,we confirmed that the dioxygen was produced from water oxidation.This work highlights that the atmosphere during synthesis and solvent selection greatly regulate the crystal structures of MOFs and further manipulate their photocatalytic performance.展开更多
基金supported by the National Natural Science Foundation of China(No.22171106,21871172,22201101,and 22001094)the Guangdong Major Project of Basic and Applied Research(No.2019B030302009)+4 种基金Guangdong Natural Science Foundation(No.2022A1515011937)the Fundamental Research Funds for the Central Universities(No.21622103)the Guangdong Basic and Applied Basic Research Foundation(No.2022A1515110523)open fund of Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications(No.2022A06)Jinan University.
文摘Water oxidation to molecular dioxygen driven by visible light is essential but difficult in solar fuel production due to its sluggish reaction kinetics.Although the catalytic process is highly dependent on the coordination-unsaturated metal sites in coordination catalysts,the controllable design of catalysts with such catalytic sites remains challenging.Herein,we report two new Co-MOFs(CoBIM-1 and CoBIM-2)for photocatalytic water oxidation under visible light.The coordination environment of Co in Co-MOFs can be easily manipulated by changing the atmosphere and concentration of deprotonated solvent during synthesis.CoBIM-1 with coordinatively unsaturated Co sites showed good performance with an O_(2)production of 2.0 mmol g^(−1)h^(−1),in sharp contrast to its counterpart CoBIM-2.Furthermore,through isotope tracing experiments,we confirmed that the dioxygen was produced from water oxidation.This work highlights that the atmosphere during synthesis and solvent selection greatly regulate the crystal structures of MOFs and further manipulate their photocatalytic performance.
