Iron oxide supported Au nanomaterials are one of the most studied catalysts for low-temperature CO oxidation.Catalytic performance not only critically depends on the size of the supported Au nanoparticles(NPs)but also...Iron oxide supported Au nanomaterials are one of the most studied catalysts for low-temperature CO oxidation.Catalytic performance not only critically depends on the size of the supported Au nanoparticles(NPs)but also strongly on the chemical nature of the iron oxide.In this study,Au NPs supported on iron oxide nanorods with different surface properties throughβ-FeOOH annealing,at varying temperatures,were synthesized,and applied in the CO oxidation.Detailed characterizations of the interactions between Au NPs and iron oxides were obtained by X-ray diffraction,transmission electron microscopy(TEM),and X-ray photoelectron spectroscopy.The results indicate that the surface hydroxyl group on the Au/FeOOH catalyst,before calcination(Au/FeOOH-fresh),could facilitate the oxygen adsorption and dissociation on positively charged Au,thereby contributing to the low-temperature CO oxidation reactivity.After calcination at 200℃,under air exposure,the chemical state of the supported Au NP on varied iron oxides partly changed from metal cation to Au0,along with the disappearance of the surface OH species.Au/FeOOH with the highest Au0 content exhibits the highest activity in CO oxidation,among the as-synthesized catalysts.Furthermore,good durability in CO oxidation was achieved over the Au/FeOOH catalyst for 12 h without observable deactivation.In addition,the advanced identical-location TEM method was applied to the gas phase reaction to probe the structure evolution of the Au/iron oxide series of the catalysts and support structure.A Au NP size-dependent Ostwald ripening process mediated by the transport of Au(CO)x mobile species under certain reaction conditions is proposed,which offers a new insight into the validity of the structure-performance relationship.展开更多
This work describes a simple yet powerful scalable solution chemistry strategy to create back‐contact rich interfaces between substrates such as commercial transparent conducting fluorine‐doped tin oxide coated glas...This work describes a simple yet powerful scalable solution chemistry strategy to create back‐contact rich interfaces between substrates such as commercial transparent conducting fluorine‐doped tin oxide coated glass(FTO)and photoactive thin films such as hematite for low‐cost water oxidation reaction.High‐resolution electron microscopy(SEM,TEM,STEM),atomic force microscopy(AFM),elemental chemical mapping(EELS,EDS)and photoelectrochemical(PEC)investigations reveal that the mechanical stress,lattice mismatch,electron energy barrier,and voids between FTO and hematite at the back‐contact interface as well as short‐circuit and detrimental reaction between FTO and the electrolyte can be alleviated by engineering the chemical composition of the precursor solutions,thus increasing the overall efficiency of these low‐cost photoanodes for water oxidation reaction for a clean and sustainable generation of hydrogen from PEC water‐splitting.These findings are of significant importance to improve the charge collection efficiency by minimizing electron‐hole recombination observed at back‐contact interfaces and grain boundaries in mesoporous electrodes,thus improving the overall efficiency and scalability of low‐cost PEC water splitting devices.展开更多
Spin engineering is recognized as a promising strategy that modulates the association between d‐orbital electrons and the oxygenated species,and enhances the catalytic kinetics.However,few efforts have been made to c...Spin engineering is recognized as a promising strategy that modulates the association between d‐orbital electrons and the oxygenated species,and enhances the catalytic kinetics.However,few efforts have been made to clarify whether spin engineering could make a considerable enhancement for electrocatalytic water oxidation.Herein,we report the spin engineering of a nanocage‐structured(Co,Ni)Se_(2)/C@FeOOH,that showed significant oxygen evolution reaction(OER)activity.Magnetization measurement presented that the(Co,Ni)Se_(2)/C@FeOOH sample possesses higher polarization spin number(μb=6.966μB/f.u.)compared with that of the(Co,Ni)Se_(2)/C sample(μb=6.398μB/f.u.),for which the enlarged spin polarization number favors the adsorption and desorption energy of the intermediate oxygenated species,as confirmed by surface valance band spectra.Consequently,the(Co,Ni)Se_(2)/C@FeOOH affords remarkable OER product with a low overpotential of 241 mV at a current of 10 mA cm^(-2) and small Tafel slope of 44 mV dec^(-1) in 1.0 mol/L KOH alkaline solution,significantly surpassing the parent(Co,Ni)Se_(2)/C catalyst.This work will trigger a solid step for the design of highly‐efficient OER electrocatalysts.展开更多
Iron oxides, including α-Fe2O3, γ-Fe2O3, Fe3O4, etc. are one of the most widely investigated materials for their fundamental properties and potential applications. One-dimensional (1-D) iron oxides nanostructures ...Iron oxides, including α-Fe2O3, γ-Fe2O3, Fe3O4, etc. are one of the most widely investigated materials for their fundamental properties and potential applications. One-dimensional (1-D) iron oxides nanostructures are the focus of recent research activi- ties because of their wide applications in magnetic refrigeration, information storage, electronics, catalysts, Li-ion battery, pigment, gas sensors, etc. This review covers the recent progress in the synthesis, properties and applications of 1-D iron oxides nanostructures. The paper begins with the introduction to 1-D iron oxides nanostructures, followed by the typical synthetic methods developed for the synthesis of 1-D iron oxides nanostructures. Then, the typical 1-D iron oxides nanostructures, in- cluding nanowires/nanorods, nanotubes, nanobelts, nanochalns, and special 3-D structures built on 1-D building blocks, are introduced in detail. The properties of 1-D iron oxides nanostructures are then discussed, focusing on the magnetic, gas sensing, and electrochemical and photocatalytic properties. Finally, we draw conclusions and look at the prospects of 1-D iron oxides nanostructures.展开更多
基金supported by the National Natural Science Foundation of China(21773269,21761132025,91545119,21703262)the Youth Innovation Promotion Association CAS(2015152)+1 种基金the Joint Foundation of Liaoning Province Natural Science FoundationShenyang National Laboratory for Materials Science(20180510047)~~
文摘Iron oxide supported Au nanomaterials are one of the most studied catalysts for low-temperature CO oxidation.Catalytic performance not only critically depends on the size of the supported Au nanoparticles(NPs)but also strongly on the chemical nature of the iron oxide.In this study,Au NPs supported on iron oxide nanorods with different surface properties throughβ-FeOOH annealing,at varying temperatures,were synthesized,and applied in the CO oxidation.Detailed characterizations of the interactions between Au NPs and iron oxides were obtained by X-ray diffraction,transmission electron microscopy(TEM),and X-ray photoelectron spectroscopy.The results indicate that the surface hydroxyl group on the Au/FeOOH catalyst,before calcination(Au/FeOOH-fresh),could facilitate the oxygen adsorption and dissociation on positively charged Au,thereby contributing to the low-temperature CO oxidation reactivity.After calcination at 200℃,under air exposure,the chemical state of the supported Au NP on varied iron oxides partly changed from metal cation to Au0,along with the disappearance of the surface OH species.Au/FeOOH with the highest Au0 content exhibits the highest activity in CO oxidation,among the as-synthesized catalysts.Furthermore,good durability in CO oxidation was achieved over the Au/FeOOH catalyst for 12 h without observable deactivation.In addition,the advanced identical-location TEM method was applied to the gas phase reaction to probe the structure evolution of the Au/iron oxide series of the catalysts and support structure.A Au NP size-dependent Ostwald ripening process mediated by the transport of Au(CO)x mobile species under certain reaction conditions is proposed,which offers a new insight into the validity of the structure-performance relationship.
基金supported by CNPq,CAPES,FAPESP(2017/02317-2),FAPESP(2017/11986-5)Shell and the strategic importance of the support given by ANP(Brazil’s National Oil,Natural Gas and Biofuels Agency)through the R&D levy regulation+2 种基金PRH49/UFABC-ANP for the fellowshipthe National Natural Science Foundation of China(NSFC)the Outstanding Talent Program of Shaanxi Province as well as FAPESP(2017/11986-5)
文摘This work describes a simple yet powerful scalable solution chemistry strategy to create back‐contact rich interfaces between substrates such as commercial transparent conducting fluorine‐doped tin oxide coated glass(FTO)and photoactive thin films such as hematite for low‐cost water oxidation reaction.High‐resolution electron microscopy(SEM,TEM,STEM),atomic force microscopy(AFM),elemental chemical mapping(EELS,EDS)and photoelectrochemical(PEC)investigations reveal that the mechanical stress,lattice mismatch,electron energy barrier,and voids between FTO and hematite at the back‐contact interface as well as short‐circuit and detrimental reaction between FTO and the electrolyte can be alleviated by engineering the chemical composition of the precursor solutions,thus increasing the overall efficiency of these low‐cost photoanodes for water oxidation reaction for a clean and sustainable generation of hydrogen from PEC water‐splitting.These findings are of significant importance to improve the charge collection efficiency by minimizing electron‐hole recombination observed at back‐contact interfaces and grain boundaries in mesoporous electrodes,thus improving the overall efficiency and scalability of low‐cost PEC water splitting devices.
文摘Spin engineering is recognized as a promising strategy that modulates the association between d‐orbital electrons and the oxygenated species,and enhances the catalytic kinetics.However,few efforts have been made to clarify whether spin engineering could make a considerable enhancement for electrocatalytic water oxidation.Herein,we report the spin engineering of a nanocage‐structured(Co,Ni)Se_(2)/C@FeOOH,that showed significant oxygen evolution reaction(OER)activity.Magnetization measurement presented that the(Co,Ni)Se_(2)/C@FeOOH sample possesses higher polarization spin number(μb=6.966μB/f.u.)compared with that of the(Co,Ni)Se_(2)/C sample(μb=6.398μB/f.u.),for which the enlarged spin polarization number favors the adsorption and desorption energy of the intermediate oxygenated species,as confirmed by surface valance band spectra.Consequently,the(Co,Ni)Se_(2)/C@FeOOH affords remarkable OER product with a low overpotential of 241 mV at a current of 10 mA cm^(-2) and small Tafel slope of 44 mV dec^(-1) in 1.0 mol/L KOH alkaline solution,significantly surpassing the parent(Co,Ni)Se_(2)/C catalyst.This work will trigger a solid step for the design of highly‐efficient OER electrocatalysts.
基金supported by the National Natural Science Foundation of China (Grant No. 51002059)the National Basic Research Program of China (Grant No. 2011CBA00700)+2 种基金the Natural Science Foundation of Hubei Province (Grant No. 2009CDB326)the Research Fund for the Doctoral Program of Higher Education (Grant Nos. 20090142120059, 20100142120053)the Director Fund of WNLO. Special thanks to the Analysis and Testing Center of HUST
文摘Iron oxides, including α-Fe2O3, γ-Fe2O3, Fe3O4, etc. are one of the most widely investigated materials for their fundamental properties and potential applications. One-dimensional (1-D) iron oxides nanostructures are the focus of recent research activi- ties because of their wide applications in magnetic refrigeration, information storage, electronics, catalysts, Li-ion battery, pigment, gas sensors, etc. This review covers the recent progress in the synthesis, properties and applications of 1-D iron oxides nanostructures. The paper begins with the introduction to 1-D iron oxides nanostructures, followed by the typical synthetic methods developed for the synthesis of 1-D iron oxides nanostructures. Then, the typical 1-D iron oxides nanostructures, in- cluding nanowires/nanorods, nanotubes, nanobelts, nanochalns, and special 3-D structures built on 1-D building blocks, are introduced in detail. The properties of 1-D iron oxides nanostructures are then discussed, focusing on the magnetic, gas sensing, and electrochemical and photocatalytic properties. Finally, we draw conclusions and look at the prospects of 1-D iron oxides nanostructures.