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
Because hydrogen(H_(2))is an explosive gas and the volumetric energy density is quite low,it is highly desired to develop liquid or solid solar fuels as safe hydrogen storage alternatives.This review article focuses o...Because hydrogen(H_(2))is an explosive gas and the volumetric energy density is quite low,it is highly desired to develop liquid or solid solar fuels as safe hydrogen storage alternatives.This review article focuses on catalytic interconversion between hydrogen and liquid or solid solar fuels using metal complexes as redox catalysts.The first candidate of a liquid solar fuel is formic acid(HCOOH),which is liquid at room temperature and has a fairly high volumetric density of 1.22 g cm^(-3).展开更多
Y zeolite is presently used as an important active component in oil refining catalysts.The efficient synthesis of NaY zeolite still faces many huge challenges.Herein,a novel method for the rapid synthesis of nano-plat...Y zeolite is presently used as an important active component in oil refining catalysts.The efficient synthesis of NaY zeolite still faces many huge challenges.Herein,a novel method for the rapid synthesis of nano-plate-like small crystal-sized NaY zeolite through an artificial-fish-reef-breeding negative crystal strategy is reported.It was discovered that cationic polyacrylamide(CPAM)could act as an artificial fish-reef to breed negative crystals,which promoted NaY zeolite nucleation and accelerated the crystallization of NaY zeolite.The crystallization time of NaY zeolite was shortened by 9 h.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.
基金support from the NRF of Korea through CRI(NRF-2021R1A3B1076539 to W.N.)the Basic Science Research Program(NRF-2023R1A2C1007668 to Y.-M.L.)+1 种基金the Brain Pool Program(NRF-2022H1D3A2A01045098 to W.N.and S.F.)Grants-in-Aid(no.16H02268 and 23K04686 to S.F.)from MEXT,Japan.
文摘Because hydrogen(H_(2))is an explosive gas and the volumetric energy density is quite low,it is highly desired to develop liquid or solid solar fuels as safe hydrogen storage alternatives.This review article focuses on catalytic interconversion between hydrogen and liquid or solid solar fuels using metal complexes as redox catalysts.The first candidate of a liquid solar fuel is formic acid(HCOOH),which is liquid at room temperature and has a fairly high volumetric density of 1.22 g cm^(-3).
基金financial support provided for this project by the Foundation for the Innovative Research Groups of the National Natural Science Foundation of China(22021004).
文摘Y zeolite is presently used as an important active component in oil refining catalysts.The efficient synthesis of NaY zeolite still faces many huge challenges.Herein,a novel method for the rapid synthesis of nano-plate-like small crystal-sized NaY zeolite through an artificial-fish-reef-breeding negative crystal strategy is reported.It was discovered that cationic polyacrylamide(CPAM)could act as an artificial fish-reef to breed negative crystals,which promoted NaY zeolite nucleation and accelerated the crystallization of NaY zeolite.The crystallization time of NaY zeolite was shortened by 9 h.
