Carbon-based metal-free catalysts are a promising substitute for the rare and expensive platinum （Pt） used in the oxygen reduction reaction. We herein report N-doped graphene （NG） that is exquisitely integrated in...Carbon-based metal-free catalysts are a promising substitute for the rare and expensive platinum （Pt） used in the oxygen reduction reaction. We herein report N-doped graphene （NG） that is exquisitely integrated into highly conductive frameworks, simultaneously providing more active sites and higher conductivity. The NG was in situ grown on carbon fibers derived from silk cocoon （SCCf） using a simple one-step thermal treatment. The resulting product （NG-SCCf）, possessing a meso-/macroporous structure with three-dimensional （3D） interconnected networks, exhibits an onset potential that is only 0.1 V less negative than that of Pt/C and shows stability and methanol tolerance superior to those of Pt/C in alkaline media. Moreover, in the absence of Pt as co-catalyst, NG-SCCf shows a photocatalytic H2 production rate of 66.0 ~tmol-h l.g 1, 4.4-fold higher than that of SCCf. This outstanding activity is intimately related to the in situ grown NG, hierarchically porous structure, and 3D interconnected networks, which not only introduce more active sites but also enable smooth electron transfer, mass transport, and effective separation of electron-hole pairs. Considering the abundance of the green raw material in combination with easy and low-cost preparation, this work contributes to the development of advanced sustainable catalysts in energy storage/conversion fields, such as electro- and photocatalysis.展开更多
In this work, we present a new versatile strategy to prepare noble metal （Au, Ag and Cu） nanoclusters on TiO2 nanosheets in large scales with exposed （001） facets with controlled size, crystalline interface, and l...In this work, we present a new versatile strategy to prepare noble metal （Au, Ag and Cu） nanoclusters on TiO2 nanosheets in large scales with exposed （001） facets with controlled size, crystalline interface, and loading amount. By precise in situ calcination, the metal （M = Au, Ag, and Cu） nanocrystals with controllable size and better crystalline interface with the TiO2 support have been prepared. The potential application of the as-prepared Au, Ag, and Cu nanoclusters on TiO2 nanosheets as potential heterogeneous catalysts for organic synthesis, such as catalytic reduction of 4-nitrophenol to 4-aminophenol, has been demonstrated. After calcination, Au, Ag, and Cu nanocrystals were found to be proficient cocatalysts for photocatalytic H2 evolution, particularly the Au cocatalyst. Based on precise high-resolution transmission electron microscopy （HRTEM） and inductively coupled plasma optical emission spectrometry （ICP-OES） analyses, the flexible control of their size and loading amount as well as their intimate contact with the TiO2 nanosheet enhanced the photocatalytic H2 evolution activity and the sensitivity of the photocurrent response of the film. Furthermore, this aqueous-directed synthesis of metal nanoclusters on a support will generate further interest in the field of nanocatalysis.展开更多
Synthesis of pure phase Mg1.2Ti1.8O5 and MgTiO3 nanocrystals has proven to be challenging. Here, pure phase Mg1.2Ti1.8O5 and MgTiO3 nanocrystals were prepared. Furthermore, a new magnesium titanate, Mg1.2Ti1.8O5, was ...Synthesis of pure phase Mg1.2Ti1.8O5 and MgTiO3 nanocrystals has proven to be challenging. Here, pure phase Mg1.2Ti1.8O5 and MgTiO3 nanocrystals were prepared. Furthermore, a new magnesium titanate, Mg1.2Ti1.8O5, was synthesized via a solution-based route for the first time. As hydrogen evolution photocatalysts, both pure phase Mg1.2TiLsO5 and MgTiO3 nanocrystals exhibit excellent hydrogen production efficiency. In comparison with pure MgTiO3 nanocrystals, the asprepared Mg1.2Ti1.8O5 nanocrystals exhibited four times as much photocatalytic hydrogen production activity, up to 40 μmol.h-1 Photoelectrochemical analysis, including linear sweep voltammetry, transient photocurrent measurement, electrochemical impedance spectroscopy, and construction of Mott-Schottky plots, demonstrated that the enhanced photocatalytic activity was attributed to the large surface area, fast photoelectron transfer, higher carrier density, and efficient charge separation of the Mg1.2Ti1.8O5 nanocrystals.展开更多
Solid oxide electrolysis cells(SOECs)represent a crucial stride toward sustainable hydrogen generation,and this review explores their current scientific challenges,significant advancements,and potential for large-scal...Solid oxide electrolysis cells(SOECs)represent a crucial stride toward sustainable hydrogen generation,and this review explores their current scientific challenges,significant advancements,and potential for large-scale hydrogen production.In SOEC technology,the application of innovative fabrication tech-niques,doping strategies,and advanced materials has enhanced the performance and durability of these systems,although degradation challenges persist,implicating the prime focus for future advancements.Here we provide in-depth analysis of the recent developments in SOEC technology,including Oxygen-SOECs,Proton-SOECs,and Hybrid-SOECs.Specifically,Hybrid-SOECs,with their mixed ionic conducting electrolytes,demonstrate superior efficiency and the concurrent production of hydrogen and oxygen.Coupled with the capacity to harness waste heat,these advancements in SOEC technology present signif-icant promise for pilot-scale applications in industries.The review also highlights remarkable achieve-ments and potential reductions in capital expenditure for future SOEC systems,while elaborating on the micro and macro aspects of sOECs with an emphasis on ongoing research for optimization and scal-ability.It concludes with the potential of SOEC technology to meet various industrial energy needs and its significant contribution considering the key research priorities to tackle the global energy demands,ful-fillment,and decarbonization efforts.展开更多
An effective photocatalytic hydrogen production catalyst comprising MgTiO3/ MgTi2O5/TiO2 heterogeneous belt-junctions was prepared using magnesium ions by a thermally driven doping method. The tri-phase heterogeneous ...An effective photocatalytic hydrogen production catalyst comprising MgTiO3/ MgTi2O5/TiO2 heterogeneous belt-junctions was prepared using magnesium ions by a thermally driven doping method. The tri-phase heterogeneous junction was confirmed by X-ray powder diffraction （XRD）, transmission electron microscopy （TEM）, and high-resolution TEM （HRTEM）. The as-prepared MgTiOg/MgTi2OJ TiO2 heterojunctions exhibited a very high photocatalytic hydrogen production activity （356.1 mol·g0.1mgcat·h^-1） and an apparent quantum efficiency （50.69% at 365 nm） that is about twice of that of bare TiO2 nanobelts （189.4mol·g0.1mgcat·h^-1）. Linear sweep voltage and transient photocurrent characterization as well as analysis of the electrochemical impedance spectra and Mott-Schottky plots revealed that the high photocatalytic performance is caused by the one-dimensional structure, which imparts excellent charge transportation characteristic, and the MgTiO3/MgTi2O5/TiO2 tri-phase heterojunction, which effectively drives the charge separation through the inherent electric field. This titanate-based tri-phase heterogeneous junction photocatalyst further enriches the catalyst system for photocatalytic hydrogen production.展开更多
Nanostructured semiconductors have been researched intensively for energy conversion and storage applications in recent decades.Despite of tremendous findings and achievements,the performance of the devices resulted f...Nanostructured semiconductors have been researched intensively for energy conversion and storage applications in recent decades.Despite of tremendous findings and achievements,the performance of the devices resulted from the nanomaterials in terms of energy conversion efficiency and storage capacity needs further improvement to become economically viable for subsequent commercialization.Hydrogenation is a simple,efficient,and cost-effective way for tailoring the electronic and morphological properties of the nanostructured materials.This work reviews a series of hydrogenated nanostructured materials was produced by the hydrogenation of a wide range of nanomaterials.These materials with improved inherent conductivity and changed characteristic lattice structure possess much enhanced performance for energy conversion application,e.g.,photoelectrocatalytic production of hydrogen,and energy storage applications,e.g.,lithium-ion batteries and supercapacitors.The hydrogenation mechanisms as well as resultant properties responsible for the efficiency improvement are explored in details.This work provides guidance for researchers to use the hydrogenation technology to design functional materials.展开更多
基金The work was financially supported by National Natural Science Foundation of China （Nos. 51203182 and 51173202）, Foundation for the Author of Excellent Doctoral Dissertation of Hunan Province （No. YB2014B004）, Aeronautical Science Foundation of China （No. 20143188004）, Key Laboratory of Advanced Textile Materials and Manufacturing Technology （Zhejiang Sci-Tech University）, Ministry of Education （No. 2015001）, Key Laboratory of Lightweight and Reliability Technology for Engineering Vehicle, College of Hunan Province （No. 2016kfjj01）, Research Project of NUDT. We thank Tengyuan Wang for help in ORR experiment and helpful discussions.
文摘Carbon-based metal-free catalysts are a promising substitute for the rare and expensive platinum （Pt） used in the oxygen reduction reaction. We herein report N-doped graphene （NG） that is exquisitely integrated into highly conductive frameworks, simultaneously providing more active sites and higher conductivity. The NG was in situ grown on carbon fibers derived from silk cocoon （SCCf） using a simple one-step thermal treatment. The resulting product （NG-SCCf）, possessing a meso-/macroporous structure with three-dimensional （3D） interconnected networks, exhibits an onset potential that is only 0.1 V less negative than that of Pt/C and shows stability and methanol tolerance superior to those of Pt/C in alkaline media. Moreover, in the absence of Pt as co-catalyst, NG-SCCf shows a photocatalytic H2 production rate of 66.0 ~tmol-h l.g 1, 4.4-fold higher than that of SCCf. This outstanding activity is intimately related to the in situ grown NG, hierarchically porous structure, and 3D interconnected networks, which not only introduce more active sites but also enable smooth electron transfer, mass transport, and effective separation of electron-hole pairs. Considering the abundance of the green raw material in combination with easy and low-cost preparation, this work contributes to the development of advanced sustainable catalysts in energy storage/conversion fields, such as electro- and photocatalysis.
文摘In this work, we present a new versatile strategy to prepare noble metal （Au, Ag and Cu） nanoclusters on TiO2 nanosheets in large scales with exposed （001） facets with controlled size, crystalline interface, and loading amount. By precise in situ calcination, the metal （M = Au, Ag, and Cu） nanocrystals with controllable size and better crystalline interface with the TiO2 support have been prepared. The potential application of the as-prepared Au, Ag, and Cu nanoclusters on TiO2 nanosheets as potential heterogeneous catalysts for organic synthesis, such as catalytic reduction of 4-nitrophenol to 4-aminophenol, has been demonstrated. After calcination, Au, Ag, and Cu nanocrystals were found to be proficient cocatalysts for photocatalytic H2 evolution, particularly the Au cocatalyst. Based on precise high-resolution transmission electron microscopy （HRTEM） and inductively coupled plasma optical emission spectrometry （ICP-OES） analyses, the flexible control of their size and loading amount as well as their intimate contact with the TiO2 nanosheet enhanced the photocatalytic H2 evolution activity and the sensitivity of the photocurrent response of the film. Furthermore, this aqueous-directed synthesis of metal nanoclusters on a support will generate further interest in the field of nanocatalysis.
基金This work was supported by the National Natural Sdence Foundation of China （Nos. 21171052, 21471050, 21501052 and 21473051）, the Program for New Century Excellent Talents in University of Ministry of Education of China （No. NCET-11-0959）, the China Postdoctoral Science Foundation （No. 2015M570304）, the Postdoctoral Science Foundation of Heilongjiang Province （No. LBH-Q11009）, Program for Innovative Research Team in University （No. IRT-1237）, Heilongjiang Province Natural Science Foundation of Key Projects （No. ZD201301）, Heilongjiang Province Natural Science Foundation Youth Fund （No. QC2015010） and Harbin Technological Innovation Talent of Special Funds （No. RC2013QN017028）.
文摘Synthesis of pure phase Mg1.2Ti1.8O5 and MgTiO3 nanocrystals has proven to be challenging. Here, pure phase Mg1.2Ti1.8O5 and MgTiO3 nanocrystals were prepared. Furthermore, a new magnesium titanate, Mg1.2Ti1.8O5, was synthesized via a solution-based route for the first time. As hydrogen evolution photocatalysts, both pure phase Mg1.2TiLsO5 and MgTiO3 nanocrystals exhibit excellent hydrogen production efficiency. In comparison with pure MgTiO3 nanocrystals, the asprepared Mg1.2Ti1.8O5 nanocrystals exhibited four times as much photocatalytic hydrogen production activity, up to 40 μmol.h-1 Photoelectrochemical analysis, including linear sweep voltammetry, transient photocurrent measurement, electrochemical impedance spectroscopy, and construction of Mott-Schottky plots, demonstrated that the enhanced photocatalytic activity was attributed to the large surface area, fast photoelectron transfer, higher carrier density, and efficient charge separation of the Mg1.2Ti1.8O5 nanocrystals.
基金the support of the Natural Sciences and Engineering Research Council of Canada(NSERC)Tier 1 Canada Research Chair in Green Hydrogen Production,the Québec Ministere de I'Economie,de I'lnnovation et de I'Energie(MEIE)[Développement de catalyseurs et d'electrodes innovants,a faibles couts,performants et durables pour la production d'hydrogene vert,funding reference number 00393501]。
文摘Solid oxide electrolysis cells(SOECs)represent a crucial stride toward sustainable hydrogen generation,and this review explores their current scientific challenges,significant advancements,and potential for large-scale hydrogen production.In SOEC technology,the application of innovative fabrication tech-niques,doping strategies,and advanced materials has enhanced the performance and durability of these systems,although degradation challenges persist,implicating the prime focus for future advancements.Here we provide in-depth analysis of the recent developments in SOEC technology,including Oxygen-SOECs,Proton-SOECs,and Hybrid-SOECs.Specifically,Hybrid-SOECs,with their mixed ionic conducting electrolytes,demonstrate superior efficiency and the concurrent production of hydrogen and oxygen.Coupled with the capacity to harness waste heat,these advancements in SOEC technology present signif-icant promise for pilot-scale applications in industries.The review also highlights remarkable achieve-ments and potential reductions in capital expenditure for future SOEC systems,while elaborating on the micro and macro aspects of sOECs with an emphasis on ongoing research for optimization and scal-ability.It concludes with the potential of SOEC technology to meet various industrial energy needs and its significant contribution considering the key research priorities to tackle the global energy demands,ful-fillment,and decarbonization efforts.
基金Acknowledgements This work was supported by the National Natural Sdence Foundation of China （Nos. 21471050, 21501052 and 21473051）, the China Postdoctoral Science Foundation （No. 2015M570304）, the Postdoctoral Science Foundation of Heilongjiang Province （Nos. LBH-Ql1009 and LBH-TZ06019）, Heilongjiang Province Natural Science Foundation （Nos. ZD201301 and QC2015010）, and Harbin Technological Innovation Talent of Special Funds （No. RC2013QN017028）.
文摘An effective photocatalytic hydrogen production catalyst comprising MgTiO3/ MgTi2O5/TiO2 heterogeneous belt-junctions was prepared using magnesium ions by a thermally driven doping method. The tri-phase heterogeneous junction was confirmed by X-ray powder diffraction （XRD）, transmission electron microscopy （TEM）, and high-resolution TEM （HRTEM）. The as-prepared MgTiOg/MgTi2OJ TiO2 heterojunctions exhibited a very high photocatalytic hydrogen production activity （356.1 mol·g0.1mgcat·h^-1） and an apparent quantum efficiency （50.69% at 365 nm） that is about twice of that of bare TiO2 nanobelts （189.4mol·g0.1mgcat·h^-1）. Linear sweep voltage and transient photocurrent characterization as well as analysis of the electrochemical impedance spectra and Mott-Schottky plots revealed that the high photocatalytic performance is caused by the one-dimensional structure, which imparts excellent charge transportation characteristic, and the MgTiO3/MgTi2O5/TiO2 tri-phase heterojunction, which effectively drives the charge separation through the inherent electric field. This titanate-based tri-phase heterogeneous junction photocatalyst further enriches the catalyst system for photocatalytic hydrogen production.
基金supported by the ARC Discovery Grants from the Australian Research Council Discovery Projectthe National Natural Science Foundation of China(21328301)
文摘Nanostructured semiconductors have been researched intensively for energy conversion and storage applications in recent decades.Despite of tremendous findings and achievements,the performance of the devices resulted from the nanomaterials in terms of energy conversion efficiency and storage capacity needs further improvement to become economically viable for subsequent commercialization.Hydrogenation is a simple,efficient,and cost-effective way for tailoring the electronic and morphological properties of the nanostructured materials.This work reviews a series of hydrogenated nanostructured materials was produced by the hydrogenation of a wide range of nanomaterials.These materials with improved inherent conductivity and changed characteristic lattice structure possess much enhanced performance for energy conversion application,e.g.,photoelectrocatalytic production of hydrogen,and energy storage applications,e.g.,lithium-ion batteries and supercapacitors.The hydrogenation mechanisms as well as resultant properties responsible for the efficiency improvement are explored in details.This work provides guidance for researchers to use the hydrogenation technology to design functional materials.
