By integrating photocatalytic H_(2)O_(2) production with furfuryl alcohol(FAL)oxidation,this coupled process establishes an atom-economical pathway for sustainable chemical synthesis,simultaneously achieving energy st...By integrating photocatalytic H_(2)O_(2) production with furfuryl alcohol(FAL)oxidation,this coupled process establishes an atom-economical pathway for sustainable chemical synthesis,simultaneously achieving energy storage and biomass valorization.This study introduces a meticulously engineered MOF@MOF hierarchical photocatalytic architecture,specifically the PCN-134@MOF-525(PM-X series)composite,designed for synergistic catalysis of these processes.By strategically integrating two distinct MOF materials,we circumvent the limitations of single-component systems,such as facile charge carrier recombination,and establish a redox dualactive site catalytic system.This rational design transcends simple additivity,yielding emergent catalytic behaviors driven by precise control over interfacial electric fields and dynamic structural modulation.The resultant hierarchical organization enhances light harvesting,promotes efficient charge separation,and accelerates charge transfer kinetics.Mechanistic insights,derived from photoelectrochemical,spectroscopic,and in-situ IR analyses,reveal a synergistic interplay that suppresses electron-hole recombination and spatially segregates redox processes.PM-3 demonstrates a significant enhancement in catalytic efficiency(the highest value reported),exhibiting a 4.5-fold increase in both H_(2)O_(2) production and FAL oxidation rates compared to the individual MOF components,achieving near-quantitative FAL conversion and exceptional selectivity.This work provides a potent design blueprint,emphasizing interfacial engineering and structural synergy for unprecedented efficiency and selectivity in sustainable chemical transformations.展开更多
This paper focuses on research e-infrastructures in the open science era.We analyze some of the challenges and opportunities of cloud-based science and introduce an example of a national solution in the China Science ...This paper focuses on research e-infrastructures in the open science era.We analyze some of the challenges and opportunities of cloud-based science and introduce an example of a national solution in the China Science and Technology Cloud(CSTCloud).We selected three CSTCloud use cases in deploying open science modules,including scalable engineering in astronomical data management,integrated Earth-science resources for SDG-13 decision making,and the coupling of citizen science and artificial intelligence(AI)techniques in biodiversity.We conclude with a forecast on the future development of research e-infrastructures and introduce the idea of the Global Open Science Cloud(GOSC).We hope this analysis can provide some insights into the future development of research e-infrastructures in support of open science.展开更多
Advanced satellite tracking technologies provide biologists with long-term location sequence data to understand movement of wild birds then to find explicit correlation between dynamics of migratory birds and the spre...Advanced satellite tracking technologies provide biologists with long-term location sequence data to understand movement of wild birds then to find explicit correlation between dynamics of migratory birds and the spread of avian influenza. In this paper, we propose a hierarchical clustering algorithm based on a recursive grid partition and kernel density estimation （KDE） to hierarchically identify wild bird habitats with different densities. We hierarchically cluster the GPS data by taking into account the following observations： 1） the habitat variation on a variety of geospatial scales; 2） the spatial variation of the activity patterns of birds in different stages of the migration cycle. In addition, we measure the site fidelity of wild birds based on clustering. To assess effectiveness, we have evaluated our system using a large-scale GPS dataset collected from 59 birds over three years. As a result, our approach can identify the hierarchical habitats and distribution of wild birds more efficiently than several commonly used algorithms such as DBSCAN and DENCLUE.展开更多
Solar light driven hydrogen production from water splitting and oxidation of biomass-derivatives is attractive for the conversion of solar energy to high value-added chemicals.The fabrication of heterostructure photoc...Solar light driven hydrogen production from water splitting and oxidation of biomass-derivatives is attractive for the conversion of solar energy to high value-added chemicals.The fabrication of heterostructure photocatalysts with matched band structure between two semiconductors is a promising approach for efficient photocatalysis.In this work,a novel In_(2)O_(3)/In_(2)S_(3)heterostructured hollow fiber photocatalyst was successfully fabricated through two-step ion exchange and chemical bath deposition methods,where the In_(2)S_(3)nanoparticles(NPs)anchored on the surface of In_(2)O_(3)hollow fibers via strong interfacial interaction between the In_(2)O_(3)(222)and In_(2)S_(3)(220)facets.The photocatalyst was used for efficient visible-light-driven photocatalytic hydrogen production integrated with selective oxidation of 5-hydroxymethylfurfural(HMF)to 2,5-diformylfuran(DFF).Compared with pristine In_(2)O_(3)and In_(2)S_(3),the optimal In_(2)O_(3)/In_(2)S_(3)heterostructure exhibits an enhanced photocatalytic hydrogen pro-duction rate(111.2μmol h^(-1)g^(-1)),HMF conversion efficiency(56%)and DFF selectivity(68%)under visible light irradiation.The experimental and theoretical investigations illustrate the phase interface between well matched In_(2)O_(3)(222)and In_(2)S_(3)(220)facets gives rise to facilitated photogenerated charge separation and transfer.This study presents the development of high-performance heterostructured photocatalysts for high efficient hydrogen production coupled with biomass oxidation.展开更多
基金supported by National Natural Science Foundation of China(22378219)Project ZR2023QB173 supported by Shandong Provincial Natural Science Foundation and Postdoctoral Application Project of Qingdao(QHBSH20230102024)Prof.H.Tang gratefully acknowledges financial support from Taishan Youth Scholar Program of Shandong Province.
文摘By integrating photocatalytic H_(2)O_(2) production with furfuryl alcohol(FAL)oxidation,this coupled process establishes an atom-economical pathway for sustainable chemical synthesis,simultaneously achieving energy storage and biomass valorization.This study introduces a meticulously engineered MOF@MOF hierarchical photocatalytic architecture,specifically the PCN-134@MOF-525(PM-X series)composite,designed for synergistic catalysis of these processes.By strategically integrating two distinct MOF materials,we circumvent the limitations of single-component systems,such as facile charge carrier recombination,and establish a redox dualactive site catalytic system.This rational design transcends simple additivity,yielding emergent catalytic behaviors driven by precise control over interfacial electric fields and dynamic structural modulation.The resultant hierarchical organization enhances light harvesting,promotes efficient charge separation,and accelerates charge transfer kinetics.Mechanistic insights,derived from photoelectrochemical,spectroscopic,and in-situ IR analyses,reveal a synergistic interplay that suppresses electron-hole recombination and spatially segregates redox processes.PM-3 demonstrates a significant enhancement in catalytic efficiency(the highest value reported),exhibiting a 4.5-fold increase in both H_(2)O_(2) production and FAL oxidation rates compared to the individual MOF components,achieving near-quantitative FAL conversion and exceptional selectivity.This work provides a potent design blueprint,emphasizing interfacial engineering and structural synergy for unprecedented efficiency and selectivity in sustainable chemical transformations.
基金supported by funding from the National Key R&D Program of China(No.2021YFE0111500)the National Natural Science Foundation of China(No.72104229)+1 种基金the CAS Program for fostering international mega-science(No.241711KYSB20200023)the CAS President's International Fellowship Initiative(No.2021VTA0006).
文摘This paper focuses on research e-infrastructures in the open science era.We analyze some of the challenges and opportunities of cloud-based science and introduce an example of a national solution in the China Science and Technology Cloud(CSTCloud).We selected three CSTCloud use cases in deploying open science modules,including scalable engineering in astronomical data management,integrated Earth-science resources for SDG-13 decision making,and the coupling of citizen science and artificial intelligence(AI)techniques in biodiversity.We conclude with a forecast on the future development of research e-infrastructures and introduce the idea of the Global Open Science Cloud(GOSC).We hope this analysis can provide some insights into the future development of research e-infrastructures in support of open science.
文摘Advanced satellite tracking technologies provide biologists with long-term location sequence data to understand movement of wild birds then to find explicit correlation between dynamics of migratory birds and the spread of avian influenza. In this paper, we propose a hierarchical clustering algorithm based on a recursive grid partition and kernel density estimation （KDE） to hierarchically identify wild bird habitats with different densities. We hierarchically cluster the GPS data by taking into account the following observations： 1） the habitat variation on a variety of geospatial scales; 2） the spatial variation of the activity patterns of birds in different stages of the migration cycle. In addition, we measure the site fidelity of wild birds based on clustering. To assess effectiveness, we have evaluated our system using a large-scale GPS dataset collected from 59 birds over three years. As a result, our approach can identify the hierarchical habitats and distribution of wild birds more efficiently than several commonly used algorithms such as DBSCAN and DENCLUE.
基金supported by the Natural Science Foundation of Shandong Province(ZR2021QB022)National Natural Science Foundation of China(52102362,52302272,22376110)+1 种基金Taishan Scholar Program of Shandong Province(ts201712030,tstp20230665)Technology Support Program for Youth Innovation Team of Shandong Universities(2023KJ225).
文摘Solar light driven hydrogen production from water splitting and oxidation of biomass-derivatives is attractive for the conversion of solar energy to high value-added chemicals.The fabrication of heterostructure photocatalysts with matched band structure between two semiconductors is a promising approach for efficient photocatalysis.In this work,a novel In_(2)O_(3)/In_(2)S_(3)heterostructured hollow fiber photocatalyst was successfully fabricated through two-step ion exchange and chemical bath deposition methods,where the In_(2)S_(3)nanoparticles(NPs)anchored on the surface of In_(2)O_(3)hollow fibers via strong interfacial interaction between the In_(2)O_(3)(222)and In_(2)S_(3)(220)facets.The photocatalyst was used for efficient visible-light-driven photocatalytic hydrogen production integrated with selective oxidation of 5-hydroxymethylfurfural(HMF)to 2,5-diformylfuran(DFF).Compared with pristine In_(2)O_(3)and In_(2)S_(3),the optimal In_(2)O_(3)/In_(2)S_(3)heterostructure exhibits an enhanced photocatalytic hydrogen pro-duction rate(111.2μmol h^(-1)g^(-1)),HMF conversion efficiency(56%)and DFF selectivity(68%)under visible light irradiation.The experimental and theoretical investigations illustrate the phase interface between well matched In_(2)O_(3)(222)and In_(2)S_(3)(220)facets gives rise to facilitated photogenerated charge separation and transfer.This study presents the development of high-performance heterostructured photocatalysts for high efficient hydrogen production coupled with biomass oxidation.
