Herein,a simple and effective outer-surface interactions assisted supramolecular hierarchical assembly has been first exploited to uniformly distribute tungstosilicic acid(TSA)inside the porous structure of cucurbit[1...Herein,a simple and effective outer-surface interactions assisted supramolecular hierarchical assembly has been first exploited to uniformly distribute tungstosilicic acid(TSA)inside the porous structure of cucurbit[10]uril-based single-layer 2D supramolecular-organic-frameworks(Q[10]-SOFs)in water.Importantly,the 2D Q[10]-SOFs can further serve as light harvesting antenna,achieving fast energy transfer to the embedded redox-active TSA upon photoexcitation,resulting in efficient visible light-driven selective oxidation of benzyl alcohols into the corresponding aldehydes in high yield at room temperature.Further studies revealed that the integrated of 2D Q[10]-SOFs and TSA played a key role in the catalytic process,due to the presence of a novel stepwise electron transfer route in the single-layer hybrid 2D structures.展开更多
Extracellular electron transfer(EET)plays a critical role in bioelectrochemical processes,allowing cou-pling between microorganisms and extracellular solid-state electrodes,metals,or other cells in energy metabolism.P...Extracellular electron transfer(EET)plays a critical role in bioelectrochemical processes,allowing cou-pling between microorganisms and extracellular solid-state electrodes,metals,or other cells in energy metabolism.Previous studies have suggested a role for outer-surface c-type cytochromes in direct metal-to-microbe electron transfer by Geobacter sulfurreducens,a model electroactive bacterium.Here,we ex-amined the possibility of other microbially produced electrical contacts by deleting the gene for PilA,the protein monomer that G.sulfurreducens assembles into electrically conductive protein nanowires(e-pili).Deleting pilA gene inhibited electron extraction from pure iron and 316L stainless steel up to 31%and 81%,respectively more than deleting the gene for the outer-surface cytochrome OmcS.This PilA-deficient phenotype,and the observation that relatively thick biofilms(21.7μm)grew on the metal surfaces at multi-cell distances from the metal surfaces suggest that e-pili contributed significantly to microbial cor-rosion via direct metal-to-microbe electron transfer.These results have implications for the fundamental understanding of electron harvest via e-pili by electroactive microbes,their uses in bioenergy production,as well as in monitoring and mitigation of metal biocorrosion.展开更多
Comprehensive Summary Structural transformation of metal-organic frameworks(MOFs)involving significant rearrangement of coordination bonds represents a powerful strategy to construct novel structures with distinct fun...Comprehensive Summary Structural transformation of metal-organic frameworks(MOFs)involving significant rearrangement of coordination bonds represents a powerful strategy to construct novel structures with distinct functionalities.While such transformations are typically driven by solvent,ion,or heat stimuli,the potential of functional macrocycles to trigger framework reconstruction remains unexplored.展开更多
基金supported by the National Natural Science Foundation of China(No.22271090)。
文摘Herein,a simple and effective outer-surface interactions assisted supramolecular hierarchical assembly has been first exploited to uniformly distribute tungstosilicic acid(TSA)inside the porous structure of cucurbit[10]uril-based single-layer 2D supramolecular-organic-frameworks(Q[10]-SOFs)in water.Importantly,the 2D Q[10]-SOFs can further serve as light harvesting antenna,achieving fast energy transfer to the embedded redox-active TSA upon photoexcitation,resulting in efficient visible light-driven selective oxidation of benzyl alcohols into the corresponding aldehydes in high yield at room temperature.Further studies revealed that the integrated of 2D Q[10]-SOFs and TSA played a key role in the catalytic process,due to the presence of a novel stepwise electron transfer route in the single-layer hybrid 2D structures.
基金supported by the National Natu-ral Science Foundation of China(Nos.U2006219 and 52101078)China Baowu Low Carbon Metallurgy Innovation Foundation(No.BWLCF202120)+2 种基金the National Key Research and Development Pro-gram of China(No.2020YFA0907300)the Fundamental Research Funds for the Central Universities of the Ministry of Education of China(Nos.N2102009 and N2002019)the Liaoning Revitaliza-tion Talents Program(No.XLYC1907158).
文摘Extracellular electron transfer(EET)plays a critical role in bioelectrochemical processes,allowing cou-pling between microorganisms and extracellular solid-state electrodes,metals,or other cells in energy metabolism.Previous studies have suggested a role for outer-surface c-type cytochromes in direct metal-to-microbe electron transfer by Geobacter sulfurreducens,a model electroactive bacterium.Here,we ex-amined the possibility of other microbially produced electrical contacts by deleting the gene for PilA,the protein monomer that G.sulfurreducens assembles into electrically conductive protein nanowires(e-pili).Deleting pilA gene inhibited electron extraction from pure iron and 316L stainless steel up to 31%and 81%,respectively more than deleting the gene for the outer-surface cytochrome OmcS.This PilA-deficient phenotype,and the observation that relatively thick biofilms(21.7μm)grew on the metal surfaces at multi-cell distances from the metal surfaces suggest that e-pili contributed significantly to microbial cor-rosion via direct metal-to-microbe electron transfer.These results have implications for the fundamental understanding of electron harvest via e-pili by electroactive microbes,their uses in bioenergy production,as well as in monitoring and mitigation of metal biocorrosion.
基金supported by fund from the Key Laboratory of Hubei Province for Coal Conversion and New Carbon Materials(Wuhan University of Science and Technology,WKDM202308)the Scientific Research Project of Education Department of Hubei Province(B2023007).
文摘Comprehensive Summary Structural transformation of metal-organic frameworks(MOFs)involving significant rearrangement of coordination bonds represents a powerful strategy to construct novel structures with distinct functionalities.While such transformations are typically driven by solvent,ion,or heat stimuli,the potential of functional macrocycles to trigger framework reconstruction remains unexplored.
