The mixture of graphene oxide (GO) and dye molecules may provide some new applications due to unique electronic, optical, and structural properties. Methylene blue (MB), a typ- ical anionic dye, can attach on GO v...The mixture of graphene oxide (GO) and dye molecules may provide some new applications due to unique electronic, optical, and structural properties. Methylene blue (MB), a typ- ical anionic dye, can attach on GO via π-π stacking and electrostatic interaction, and the molecule removal process on GO has been observed. However, it remains unclear about the ultrafast carrier dynamics and the internal energy transfer pathways of the system which is composed of GO and MB. We have employed ultrafast optical pump-probe spectroscopy to investigate the excited dynamics of the GO-MB system dispersed in water by exciting the samples at 400 nm pump pulse. The pristine MB and GO dynamics are also analyzed in tandem for a direct comparison. Utilizing the global analysis to fit the measured signal via a sequential model, five lifetimes are acquired:(0.61±0.01) ps, (3.52±0.04) ps, (14.1±0.3) ps, (84±2) ps, and (3.66±0.08) ns. The ultrafast dynamics corresponding to these lifetimes was analyzed and the new relaxation processes were found in the GO-MB system, compared with the pristine MB. The results reveal that the functionalization of GO can alter the known decay pathways of MB via the energy transfer from GO to MB in system, the increased intermediate state, and the promoted energy transfer from triplet state MB to ground state oxygen molecules dissolved in aqueous sample.展开更多
Prussian blue(PB) was used as catalyst to improve the extent of graphitization of polyacrylonitrile(PAN)-based carbon fibers.PB was deposited on carbon fibers by anodic electrodeposition and the thickness of PB coatin...Prussian blue(PB) was used as catalyst to improve the extent of graphitization of polyacrylonitrile(PAN)-based carbon fibers.PB was deposited on carbon fibers by anodic electrodeposition and the thickness of PB coating(PB content) was controlled by adjusting the electrodeposition time.PAN-based carbon fibers with PB coating were heat-treated and the extent of graphitization was measured by X-ray diffractometry and Raman spectroscopy.The results indicate that the extent of graphitization of PAN-based carbon fibers is enhanced in the presence of the coating.When the PB-coated carbon fibers were heat-treated at 1 900 ℃,interlayer spacing(d002) and crystallite size(Lc) reach 0.336 8 and 21.2 nm respectively.Contrarily,the values of d002 and Lc are 0.341 4 and 7.4 nm respectively when the bare carbon fibers were heat-treated at 2 800 ℃.Compared with the bare carbon fibers,PB can make the heat treatment temperature(HTT) drop more than 500 ℃ in order to reach the same extent of graphitization.Furthermore,the research results show that PB content also has a certain influence on the extent of graphitization at the same HTT.展开更多
We differentiated the effects of Cu films deposited on single crystalline a-,r-,and c-plane sapphire substrates upon graphene films synthesized with atmospheric pressure chemical vapor deposition(CVD).The data illustr...We differentiated the effects of Cu films deposited on single crystalline a-,r-,and c-plane sapphire substrates upon graphene films synthesized with atmospheric pressure chemical vapor deposition(CVD).The data illustrate that the realization of high-crystalline Cu film is dependent not only on the crystallinity of underlying substrate,but also on the symmetric match of crystallographic geometry between metal film and substrate.We also systematically investigated the effects of PMMA removal on the Raman ID/IG and IG/I2D values of transferred graphene.The results reveal that different PMMA removal methods do not alter the ID/IG values;instead,the residue of PMMA increases the IG/I2D values and the thermal decomposition of PMMA leads to higher IG/I2D values than the removal of PMMA with acetone.The effects of PMMA removal on variations of the Raman spectra are also discussed.展开更多
We report a general method to graft aromatic molecules onto graphene thin film electrodes through a simple immersion process. Large-area electroactive graphene thin films grafted with methylene blue (MB) have been d...We report a general method to graft aromatic molecules onto graphene thin film electrodes through a simple immersion process. Large-area electroactive graphene thin films grafted with methylene blue (MB) have been developed as electrocatalytic electrodes for the oxidation of β-nicotinamide adenine dinucleotide (NADH). The oxidation of NADH starts from -0.08 V (vs. Ag/AgC1) at the graphene-MB thin film electrodes, showing a decrease of 530 mV in overpotential compared to a Ti metal electrode. The graphene-MB thin films have promising applications in biosensors and biofuel cells due to their ability to promote NADH electron transfer reaction.展开更多
Direct growth of graphene on insulators is expected to yield significant improvements in performance of graphene-based electronic and spintronic devices. In this study, we successfully reveal the atomic arrangement an...Direct growth of graphene on insulators is expected to yield significant improvements in performance of graphene-based electronic and spintronic devices. In this study, we successfully reveal the atomic arrangement and electronic properties of a coherent heterostructure of single-layer graphene and α-Al2O3(0001). The analysis of the atomic arrangement of single-layer graphene on α-Al2O3(0001) revealed an apparentcontradiction. The in-plane analysis shows that single-layer graphene grows not in a single-crystalline epitaxial manner, but rather in polycrystalline form, with two strongly pronounced preferred orientations. This suggests relatively weak interfacial interactions are operative. However, we demonstrate that unusually strong physical interactions between graphene and α-Al2O3(0001) exist, as evidenced by the small separation between the graphene and the α-Al2O3(0001) surface. The interfacial interaction is shown to be dominated by the electrostatic forces involved in the graphene n-system and the unsaturated electrons of the topmost O layer of α-Al2O3(0001), rather than the van der Waals interactions. Such features causes graphene hole doping and enable the graphene to slide on the α-Al2O3(0001) surface with only a small energy barrier despite the strong interfacial interactions.展开更多
基金This work was supported by the National Natural Basic Research Program of China (No.2013CB922200),the National Natural Science Foundation of China (No.11674128, No.11474129, and No.11504129), Jilin Province Scientific and Technological Development Program, China (No.20170101063JC), the Thirteenth Five- Year Scientific and Technological Research Project of the Education Department of Jilin Province, China (No.n00).
文摘The mixture of graphene oxide (GO) and dye molecules may provide some new applications due to unique electronic, optical, and structural properties. Methylene blue (MB), a typ- ical anionic dye, can attach on GO via π-π stacking and electrostatic interaction, and the molecule removal process on GO has been observed. However, it remains unclear about the ultrafast carrier dynamics and the internal energy transfer pathways of the system which is composed of GO and MB. We have employed ultrafast optical pump-probe spectroscopy to investigate the excited dynamics of the GO-MB system dispersed in water by exciting the samples at 400 nm pump pulse. The pristine MB and GO dynamics are also analyzed in tandem for a direct comparison. Utilizing the global analysis to fit the measured signal via a sequential model, five lifetimes are acquired:(0.61±0.01) ps, (3.52±0.04) ps, (14.1±0.3) ps, (84±2) ps, and (3.66±0.08) ns. The ultrafast dynamics corresponding to these lifetimes was analyzed and the new relaxation processes were found in the GO-MB system, compared with the pristine MB. The results reveal that the functionalization of GO can alter the known decay pathways of MB via the energy transfer from GO to MB in system, the increased intermediate state, and the promoted energy transfer from triplet state MB to ground state oxygen molecules dissolved in aqueous sample.
基金Project(2006CB600903) supported by the National Basic Research Program of China
文摘Prussian blue(PB) was used as catalyst to improve the extent of graphitization of polyacrylonitrile(PAN)-based carbon fibers.PB was deposited on carbon fibers by anodic electrodeposition and the thickness of PB coating(PB content) was controlled by adjusting the electrodeposition time.PAN-based carbon fibers with PB coating were heat-treated and the extent of graphitization was measured by X-ray diffractometry and Raman spectroscopy.The results indicate that the extent of graphitization of PAN-based carbon fibers is enhanced in the presence of the coating.When the PB-coated carbon fibers were heat-treated at 1 900 ℃,interlayer spacing(d002) and crystallite size(Lc) reach 0.336 8 and 21.2 nm respectively.Contrarily,the values of d002 and Lc are 0.341 4 and 7.4 nm respectively when the bare carbon fibers were heat-treated at 2 800 ℃.Compared with the bare carbon fibers,PB can make the heat treatment temperature(HTT) drop more than 500 ℃ in order to reach the same extent of graphitization.Furthermore,the research results show that PB content also has a certain influence on the extent of graphitization at the same HTT.
基金supported by the National Basic Research Program of China(2012CB215500)the National Natural Science Foundation of China(51272296)+1 种基金the Natural Science Foundation of Chongqing(CSTC2012jjA50014)Fundamental Research Funds for the Central Universities(CDJZR12225501,CQDXWL-2013-016)
文摘We differentiated the effects of Cu films deposited on single crystalline a-,r-,and c-plane sapphire substrates upon graphene films synthesized with atmospheric pressure chemical vapor deposition(CVD).The data illustrate that the realization of high-crystalline Cu film is dependent not only on the crystallinity of underlying substrate,but also on the symmetric match of crystallographic geometry between metal film and substrate.We also systematically investigated the effects of PMMA removal on the Raman ID/IG and IG/I2D values of transferred graphene.The results reveal that different PMMA removal methods do not alter the ID/IG values;instead,the residue of PMMA increases the IG/I2D values and the thermal decomposition of PMMA leads to higher IG/I2D values than the removal of PMMA with acetone.The effects of PMMA removal on variations of the Raman spectra are also discussed.
文摘We report a general method to graft aromatic molecules onto graphene thin film electrodes through a simple immersion process. Large-area electroactive graphene thin films grafted with methylene blue (MB) have been developed as electrocatalytic electrodes for the oxidation of β-nicotinamide adenine dinucleotide (NADH). The oxidation of NADH starts from -0.08 V (vs. Ag/AgC1) at the graphene-MB thin film electrodes, showing a decrease of 530 mV in overpotential compared to a Ti metal electrode. The graphene-MB thin films have promising applications in biosensors and biofuel cells due to their ability to promote NADH electron transfer reaction.
基金We are grateful to the 'Chebishev' and 'Lomonosov' supercomputers of Moscow State University for providing the chance of using a cluster computer for quantum-chemical calculations. S.E. thanks Prof. H. Kondo (Keio University) and Prof. T. Shimada (Hirosaki University) for NIXSW measurements. This work was partly supported by Grants-in-Aid for Young Scientists B (Grant No. 22760033) from the Japan Society for the Promotion of Science. The present work has been performed under the approval of the Photon Factory Program Advisory Committee (PF PAC Nos. 2010G660 and 2012G741). P.V.A., P.B.S. and L.Y.A. acknowledge the support from the Russian Science Foundation (project No. 14-13-00139).
文摘Direct growth of graphene on insulators is expected to yield significant improvements in performance of graphene-based electronic and spintronic devices. In this study, we successfully reveal the atomic arrangement and electronic properties of a coherent heterostructure of single-layer graphene and α-Al2O3(0001). The analysis of the atomic arrangement of single-layer graphene on α-Al2O3(0001) revealed an apparentcontradiction. The in-plane analysis shows that single-layer graphene grows not in a single-crystalline epitaxial manner, but rather in polycrystalline form, with two strongly pronounced preferred orientations. This suggests relatively weak interfacial interactions are operative. However, we demonstrate that unusually strong physical interactions between graphene and α-Al2O3(0001) exist, as evidenced by the small separation between the graphene and the α-Al2O3(0001) surface. The interfacial interaction is shown to be dominated by the electrostatic forces involved in the graphene n-system and the unsaturated electrons of the topmost O layer of α-Al2O3(0001), rather than the van der Waals interactions. Such features causes graphene hole doping and enable the graphene to slide on the α-Al2O3(0001) surface with only a small energy barrier despite the strong interfacial interactions.