A 3D nitrogen⁃doped graphene/multi⁃walled carbon nanotube(CS⁃GO⁃NCNT)crosslinked network mate⁃rial was successfully synthesized utilizing chitosan and melamine as carbon and nitrogen sources,concomitant with the incor...A 3D nitrogen⁃doped graphene/multi⁃walled carbon nanotube(CS⁃GO⁃NCNT)crosslinked network mate⁃rial was successfully synthesized utilizing chitosan and melamine as carbon and nitrogen sources,concomitant with the incorporation of multi⁃wall carbon nanotubes and employing freeze drying technology.The material amalgamates the merits of 1D/2D hybrid carbon materials,wherein 1D carbon nanotubes confer robustness and expedited elec⁃tron transport pathways,while 2D graphene sheets facilitate rapid ion migration.Furthermore,the introduction of nitrogen heteroatoms serves to furnish additional active sites for lithium storage.When served as an anode material for lithium⁃ion batteries,the CS⁃GO⁃NCNT electrode delivered a reversible capacity surpassing 500 mAh·g^(-1),mark⁃edly outperforming commercial graphite anodes.Even after 300 cycles at a high current density of 1 A·g^(-1),it remained a reversible capacity of up to 268 mAh·g^(-1).展开更多
The development of highly active DFT catalysts for an electrocatalytic N_(2)reduction reaction(NRR)under mild conditions is a difficult challenge.In this study,a series of atom‐pair catalysts(APCs)for an NRR were fab...The development of highly active DFT catalysts for an electrocatalytic N_(2)reduction reaction(NRR)under mild conditions is a difficult challenge.In this study,a series of atom‐pair catalysts(APCs)for an NRR were fabricated using transition‐metal(TM)atoms(TM=Sc−Zn)doped into g‐CN monolayers.The electrochemical mechanism of APCs for an NRR has been reported by well‐defined density functional theory calculations.The calculated limiting potentials were−0.47 and−0.78 V for the Fe_(2)@CN and Co_(2)@CN catalysts,respectively.Owing to its high suppression of hydrogen evolution reactions,Co_(2)@CN is a superior electrocatalytic material for a N_(2)fixation.Stable Fe_(2)@CN may be a strongly attractive material for an NRR with a relatively low overpotential after an improvement in the selectivity.The two‐way charge transfer affirmed the donation‐acceptance procedure between N_(2)and Fe_(2)@CN or Co_(2)@CN,which play a crucial role in the activation of inert N≡N bonds.This study provides an in‐depth investigation into atom‐pair catalysts and will open up new avenues for highly efficient g‐CN‐based nanostructures for an NRR.展开更多
Graphitic carbon nitride quantum dots(CNQDs) are emerging as attractive photoluminescent(PL)materials with excellent application potential in fluorescence imaging and heavy-metal ion detection. However, three limitati...Graphitic carbon nitride quantum dots(CNQDs) are emerging as attractive photoluminescent(PL)materials with excellent application potential in fluorescence imaging and heavy-metal ion detection. However, three limitations, namely, low quantum yields(QYs), self-quenching,and excitation-dependent PL emission behaviors, severely impede the commercial applications of crystalline CNQDs.Here we address these three challenges by synthesizing borondoped amorphous CNQDs via a hydrothermal process followed by the top±down cutting approach. Structural disorder endows the amorphous boron-doped CNQDs(B-CNQDs)with superior elastic strain performance over a wide range of pH values, thus effectively promoting mass transport and reducing exciton quenching. Boron as a dopant could fine-tune the electronic structure and emission properties of the PL material to achieve excitation-independent emission via the formation of uniform boron states. As a result, the amorphous B-CNQDs show unprecedented fluorescent stability(i.e., no obvious fading after two years) and a high QY of 87.4%;these values indicate that the quantum dots obtained are very promising fluorescent materials. Moreover, the B-CNQDs show bright-blue fluorescence under ultraviolet excitation when applied as ink on commercially available paper and are capable of the selective and sensitive detection of Fe^(2+) and Cd^(2+) in the parts-per-billion range. This work presents a novel avenue and scientific insights on amorphous carbon-based fluorescent materials for photoelectrical devices and sensors.展开更多
Graphitized nanocarbon materials can be an ideal catalyst support for heterogeneous catalytic systems. Their unique physical and chemical properties, such as large surface area, high adsorption capacity, excellent the...Graphitized nanocarbon materials can be an ideal catalyst support for heterogeneous catalytic systems. Their unique physical and chemical properties, such as large surface area, high adsorption capacity, excellent thermal and mechanical stability, outstanding electronic properties, and tunable porosity, allow the anchoring and dispersion of the active metals. Therefore, currently they are used as the key support material in many catalytic processes. This review summarizes recent relevant applications in supported catalysts that use graphitized nanocarbon as supports for catalytic oxidation, hydrogenation, dehydrogenation, and C-C coupling reactions in liquid-phase and gas-solid phase-reaction systems. The latest developments in specific features derived from the morphology and characteristics of graphitized na- nocarbon-supported metal catalysts are highlighted, as well as the differences in the catalytic behavior of graphitized nano- carbon-supported metal catalysts versus other related cata- lysts. The scientific challenges and opportunities in this field are also discussed.展开更多
文摘A 3D nitrogen⁃doped graphene/multi⁃walled carbon nanotube(CS⁃GO⁃NCNT)crosslinked network mate⁃rial was successfully synthesized utilizing chitosan and melamine as carbon and nitrogen sources,concomitant with the incorporation of multi⁃wall carbon nanotubes and employing freeze drying technology.The material amalgamates the merits of 1D/2D hybrid carbon materials,wherein 1D carbon nanotubes confer robustness and expedited elec⁃tron transport pathways,while 2D graphene sheets facilitate rapid ion migration.Furthermore,the introduction of nitrogen heteroatoms serves to furnish additional active sites for lithium storage.When served as an anode material for lithium⁃ion batteries,the CS⁃GO⁃NCNT electrode delivered a reversible capacity surpassing 500 mAh·g^(-1),mark⁃edly outperforming commercial graphite anodes.Even after 300 cycles at a high current density of 1 A·g^(-1),it remained a reversible capacity of up to 268 mAh·g^(-1).
文摘The development of highly active DFT catalysts for an electrocatalytic N_(2)reduction reaction(NRR)under mild conditions is a difficult challenge.In this study,a series of atom‐pair catalysts(APCs)for an NRR were fabricated using transition‐metal(TM)atoms(TM=Sc−Zn)doped into g‐CN monolayers.The electrochemical mechanism of APCs for an NRR has been reported by well‐defined density functional theory calculations.The calculated limiting potentials were−0.47 and−0.78 V for the Fe_(2)@CN and Co_(2)@CN catalysts,respectively.Owing to its high suppression of hydrogen evolution reactions,Co_(2)@CN is a superior electrocatalytic material for a N_(2)fixation.Stable Fe_(2)@CN may be a strongly attractive material for an NRR with a relatively low overpotential after an improvement in the selectivity.The two‐way charge transfer affirmed the donation‐acceptance procedure between N_(2)and Fe_(2)@CN or Co_(2)@CN,which play a crucial role in the activation of inert N≡N bonds.This study provides an in‐depth investigation into atom‐pair catalysts and will open up new avenues for highly efficient g‐CN‐based nanostructures for an NRR.
基金supported by the National Natural Science Foundation of China (51772085 and 12072110)the Natural Science Foundation of Hunan Province (2020JJ4190)。
文摘Graphitic carbon nitride quantum dots(CNQDs) are emerging as attractive photoluminescent(PL)materials with excellent application potential in fluorescence imaging and heavy-metal ion detection. However, three limitations, namely, low quantum yields(QYs), self-quenching,and excitation-dependent PL emission behaviors, severely impede the commercial applications of crystalline CNQDs.Here we address these three challenges by synthesizing borondoped amorphous CNQDs via a hydrothermal process followed by the top±down cutting approach. Structural disorder endows the amorphous boron-doped CNQDs(B-CNQDs)with superior elastic strain performance over a wide range of pH values, thus effectively promoting mass transport and reducing exciton quenching. Boron as a dopant could fine-tune the electronic structure and emission properties of the PL material to achieve excitation-independent emission via the formation of uniform boron states. As a result, the amorphous B-CNQDs show unprecedented fluorescent stability(i.e., no obvious fading after two years) and a high QY of 87.4%;these values indicate that the quantum dots obtained are very promising fluorescent materials. Moreover, the B-CNQDs show bright-blue fluorescence under ultraviolet excitation when applied as ink on commercially available paper and are capable of the selective and sensitive detection of Fe^(2+) and Cd^(2+) in the parts-per-billion range. This work presents a novel avenue and scientific insights on amorphous carbon-based fluorescent materials for photoelectrical devices and sensors.
基金supported by the Ministry of Science and Technology (2016YFA0204100)the National Natural Science Foundation of China (21573254 and 91545110)+1 种基金the Youth Innovation Promotion Association (CAS)the Sinopec China and Strategic Priority Research Program of the Chinese Academy of Sciences (XDA09030103)
文摘Graphitized nanocarbon materials can be an ideal catalyst support for heterogeneous catalytic systems. Their unique physical and chemical properties, such as large surface area, high adsorption capacity, excellent thermal and mechanical stability, outstanding electronic properties, and tunable porosity, allow the anchoring and dispersion of the active metals. Therefore, currently they are used as the key support material in many catalytic processes. This review summarizes recent relevant applications in supported catalysts that use graphitized nanocarbon as supports for catalytic oxidation, hydrogenation, dehydrogenation, and C-C coupling reactions in liquid-phase and gas-solid phase-reaction systems. The latest developments in specific features derived from the morphology and characteristics of graphitized na- nocarbon-supported metal catalysts are highlighted, as well as the differences in the catalytic behavior of graphitized nano- carbon-supported metal catalysts versus other related cata- lysts. The scientific challenges and opportunities in this field are also discussed.