The development of highly efficient catalysts for cathodes remains an important objective of fuel cell research. Here, we report Co3O4 nanoparticles assembled on a polypyrrole/graphene oxide electrocatalyst （C...The development of highly efficient catalysts for cathodes remains an important objective of fuel cell research. Here, we report Co3O4 nanoparticles assembled on a polypyrrole/graphene oxide electrocatalyst （Co3O4/Ppy/GO） as an efficient catalyst for the oxygen reduction reaction （ORR） in alkaline media. The catalyst was prepared via the hydrothermal reaction of Co2＋ ions with Ppy-modified GO. The GO, Ppy/GO, and Co3O4/Ppy/GO were characterized using scanning electron microscopy, Fourier-transform infrared spectroscopy, and X-ray photoelectron spectroscopy. The incorporation of Ppy into GO nanosheets resulted in the formation of a nitrogen-modified GO po-rous structure, which acted as an efficient electron-transport network for the ORR. With further anchoring of Co3O4 on Ppy/GO, the as-prepared Co3O4/Ppy/GO exhibited excellent ORR activity and followed a four-electron route mechanism for the ORR in alkaline solution. An onset potential of -0.10 V vs. a saturated calomel electrode and a diffusion limiting current density of 2.30 mA/cm^2 were achieved for the Co3O4/Ppy/GO catalyst heated at 800 ℃; these values are comparable to those for noble-metal-based Pt/C catalysts. Our work demonstrates that Co3O4/Ppy/GO is highly active for the ORR. Notably, the Ppy coupling effects between Co3O4 and GO provide a new route for the preparation of efficient non-precious electrocatalysts with hierarchical porous structures for fuel cell applications.展开更多
Unique MoS_(2)‐SnS_(2)heterogeneous nanoplates have successfully in‐situ grown on poly(3‐(1‐vinylimidazolium‐3‐yl)propane‐1‐sulfonate)functionalized polypyrrole/graphene oxide(PVIPS/PPy/GO).PVIPS can attract h...Unique MoS_(2)‐SnS_(2)heterogeneous nanoplates have successfully in‐situ grown on poly(3‐(1‐vinylimidazolium‐3‐yl)propane‐1‐sulfonate)functionalized polypyrrole/graphene oxide(PVIPS/PPy/GO).PVIPS can attract heptamolybdate ion(Mo7O246−)and Sn^(4+)as the precursors by the ion‐exchange,resulting in the simultaneous growth of 1T’‐MoS2 and the berndtite‐2T‐type hexagonal SnS_(2)by the interfacial induced effect of PVIPS.The obtained MoS_(2)‐SnS_(2)/PVIPS/PPy/GO can serve as electrocatalysts,exhibiting good NRR performance by the synergistic effect.The semi‐conducting SnS_(2)would limit the surface electron accessibility for suppressing HER process of 1T’‐MoS_(2),while metallic 1T’‐MoS_(2)might efficiently improve the NRR electroactivity of SnS_(2)by the creation of Mo‐Sn‐Sn trimer catalytic sites.Otherwise,the irreversible crystal phase transition has taken place during the NRR process.Partial 1T’‐MoS_(2)and SnS_(2)have electrochemically reacted with N_(2),and irreversibly converted into Mo^(2)N and SnxNz due to the formation of Mo−N and Sn−N bonding,meanwhile,partial SnS_(2) has been irreversibly evolved into SnS due to the reduction by the power source in the electrochemical system.It would put forward a new design idea for optimizing the preparation method and electrocatalytic activity of transition metal dichalcogenides.展开更多
The corrosion inhibition of metallic substrates is a prime issue for many potential applications where corrosion plays a crucial role. The development of carbon based on functionalized coatings could increase the life...The corrosion inhibition of metallic substrates is a prime issue for many potential applications where corrosion plays a crucial role. The development of carbon based on functionalized coatings could increase the lifetime of metallic substrates by inhibiting the corrosion process. Present work is an effort to develop a corrosion inhibiting composite coating of graphene oxide and polypyrrole for AISI （American Iron and Steel Institute） type 304 stainless steel substrates. The electrochemical galvanostatic deposition process was applied for coating development. The coating morphology and ability to cover the substrate surface was analyzed with a high-resolution scanning electron microscope. The coating＇s structural and electronic properties were analyzed with Raman spectroscopy. The investigation of corrosion inhibition involved open circuit potential, Tafel, and voltammetry analysis. The standard salt test ASTM （American Society for Testing and Materials） G48A for stainless steel substrate has also been studied. Significant enhancement of corrosion potential as well as pitting potential for the composite coated substrates has been noted. Furthermore, corrosion and breakdown potential increased upon changing the material from graphene oxide to its composite coating. During the salt test analysis, the durability of the composite coating was noted up to 72 h, which is the standard time scale. Based on experimental analysis, this composite material can be used as an effective carbon based on functionalized corrosion inhibitor for stainless steel substrates to increase their lifetime.展开更多
The development of non-precious metal-based electrocatalysts has attracted much research attention because of their high oxygen reduction reaction （ORR） activities, low cost, and good durability. By one-step in-situ...The development of non-precious metal-based electrocatalysts has attracted much research attention because of their high oxygen reduction reaction （ORR） activities, low cost, and good durability. By one-step in-situ ball milling of graphite, pyrrole, and cobalt salt without resorting to high-temperature annealing, we developed a general and facile strategy to synthesize bio-inspired cobalt oxide and polypyrrole coupled with a graphene nanosheet （Co3O4-PPy/GN） complex. Herein, the exfoliation of graphite and polymerization of pyrrole occurred simultaneously during the ball milling process. Meanwhile, the Co3O4 and Co-Nx ORR active sites were generated from the oxidized cobalt ion, cobalt-PPy, and the newly exfoliated graphene nanosheets via strong π-π stacking interactions. The resultant Co3O4-PPy/GN catalysts showed efficient electrocatalytic performances for ORRs in an alkaline medium with a positive onset and reduction potentials of -0.102 and -0.196 V （vs. Ag/AgCl）, as well as a high diffusion-limited current density （4.471 mA·cm^-2）, which was comparable to that of a Pt/C catalyst （4.941 mA·cm^-2）. Compared to Pt/C, Co3O4-PPy/GN catalysts displayed better long-term stability, methanol tolerance, and anti-CO-poisoning effects, which are of great significance for the design and development of advanced non-precious metal electrocatalysts.展开更多
In this paper, composite film based on polyvinylpyrrolidone(PVP)/graphene oxide(GO) was fabricated by spray method on AT-cut 9.986 MHz quartz crystal microbalance(QCM) for NH_3 sensing. The thin films were characteriz...In this paper, composite film based on polyvinylpyrrolidone(PVP)/graphene oxide(GO) was fabricated by spray method on AT-cut 9.986 MHz quartz crystal microbalance(QCM) for NH_3 sensing. The thin films were characterized by scanning electron microscope(SEM), Fourier transform infrared spectroscopy(FTIR) and ultraviolet-visible spectroscopy(UV-VIS) to investigate the morphologies and the composition contents, respectively. The experimental results reveal that PVP/GO based sensor holds higher sensitivity, larger responsiveness and smaller baseline drift than those based on pure PVP at room temperature. Besides, the prepared sensor exhibits greater response to NH_3 than other gases such as CO, CO_2 and NO_2 at the same concentration. The good linearity, reproducibility and stability demonstrate the practicability of PVP/GO hybrid film in detecting NH_3.展开更多
基金supported by the National Natural Science Foundation of China(21373042)~~
文摘The development of highly efficient catalysts for cathodes remains an important objective of fuel cell research. Here, we report Co3O4 nanoparticles assembled on a polypyrrole/graphene oxide electrocatalyst （Co3O4/Ppy/GO） as an efficient catalyst for the oxygen reduction reaction （ORR） in alkaline media. The catalyst was prepared via the hydrothermal reaction of Co2＋ ions with Ppy-modified GO. The GO, Ppy/GO, and Co3O4/Ppy/GO were characterized using scanning electron microscopy, Fourier-transform infrared spectroscopy, and X-ray photoelectron spectroscopy. The incorporation of Ppy into GO nanosheets resulted in the formation of a nitrogen-modified GO po-rous structure, which acted as an efficient electron-transport network for the ORR. With further anchoring of Co3O4 on Ppy/GO, the as-prepared Co3O4/Ppy/GO exhibited excellent ORR activity and followed a four-electron route mechanism for the ORR in alkaline solution. An onset potential of -0.10 V vs. a saturated calomel electrode and a diffusion limiting current density of 2.30 mA/cm^2 were achieved for the Co3O4/Ppy/GO catalyst heated at 800 ℃; these values are comparable to those for noble-metal-based Pt/C catalysts. Our work demonstrates that Co3O4/Ppy/GO is highly active for the ORR. Notably, the Ppy coupling effects between Co3O4 and GO provide a new route for the preparation of efficient non-precious electrocatalysts with hierarchical porous structures for fuel cell applications.
文摘Unique MoS_(2)‐SnS_(2)heterogeneous nanoplates have successfully in‐situ grown on poly(3‐(1‐vinylimidazolium‐3‐yl)propane‐1‐sulfonate)functionalized polypyrrole/graphene oxide(PVIPS/PPy/GO).PVIPS can attract heptamolybdate ion(Mo7O246−)and Sn^(4+)as the precursors by the ion‐exchange,resulting in the simultaneous growth of 1T’‐MoS2 and the berndtite‐2T‐type hexagonal SnS_(2)by the interfacial induced effect of PVIPS.The obtained MoS_(2)‐SnS_(2)/PVIPS/PPy/GO can serve as electrocatalysts,exhibiting good NRR performance by the synergistic effect.The semi‐conducting SnS_(2)would limit the surface electron accessibility for suppressing HER process of 1T’‐MoS_(2),while metallic 1T’‐MoS_(2)might efficiently improve the NRR electroactivity of SnS_(2)by the creation of Mo‐Sn‐Sn trimer catalytic sites.Otherwise,the irreversible crystal phase transition has taken place during the NRR process.Partial 1T’‐MoS_(2)and SnS_(2)have electrochemically reacted with N_(2),and irreversibly converted into Mo^(2)N and SnxNz due to the formation of Mo−N and Sn−N bonding,meanwhile,partial SnS_(2) has been irreversibly evolved into SnS due to the reduction by the power source in the electrochemical system.It would put forward a new design idea for optimizing the preparation method and electrocatalytic activity of transition metal dichalcogenides.
文摘The corrosion inhibition of metallic substrates is a prime issue for many potential applications where corrosion plays a crucial role. The development of carbon based on functionalized coatings could increase the lifetime of metallic substrates by inhibiting the corrosion process. Present work is an effort to develop a corrosion inhibiting composite coating of graphene oxide and polypyrrole for AISI （American Iron and Steel Institute） type 304 stainless steel substrates. The electrochemical galvanostatic deposition process was applied for coating development. The coating morphology and ability to cover the substrate surface was analyzed with a high-resolution scanning electron microscope. The coating＇s structural and electronic properties were analyzed with Raman spectroscopy. The investigation of corrosion inhibition involved open circuit potential, Tafel, and voltammetry analysis. The standard salt test ASTM （American Society for Testing and Materials） G48A for stainless steel substrate has also been studied. Significant enhancement of corrosion potential as well as pitting potential for the composite coated substrates has been noted. Furthermore, corrosion and breakdown potential increased upon changing the material from graphene oxide to its composite coating. During the salt test analysis, the durability of the composite coating was noted up to 72 h, which is the standard time scale. Based on experimental analysis, this composite material can be used as an effective carbon based on functionalized corrosion inhibitor for stainless steel substrates to increase their lifetime.
基金Acknowledgements The work is supported by the National Natural Science Foundation of China （Nos. 51273008 and 51473008）, the National Basic Research Program of China （No. 2012CB933200）, and the National High-tech R＆D Program of China （No. 2012AA030305）. L. M. D. is grateful to the support from NSF （Nos. AIR-IIP-1343270 and CMMI-1400274）.
文摘The development of non-precious metal-based electrocatalysts has attracted much research attention because of their high oxygen reduction reaction （ORR） activities, low cost, and good durability. By one-step in-situ ball milling of graphite, pyrrole, and cobalt salt without resorting to high-temperature annealing, we developed a general and facile strategy to synthesize bio-inspired cobalt oxide and polypyrrole coupled with a graphene nanosheet （Co3O4-PPy/GN） complex. Herein, the exfoliation of graphite and polymerization of pyrrole occurred simultaneously during the ball milling process. Meanwhile, the Co3O4 and Co-Nx ORR active sites were generated from the oxidized cobalt ion, cobalt-PPy, and the newly exfoliated graphene nanosheets via strong π-π stacking interactions. The resultant Co3O4-PPy/GN catalysts showed efficient electrocatalytic performances for ORRs in an alkaline medium with a positive onset and reduction potentials of -0.102 and -0.196 V （vs. Ag/AgCl）, as well as a high diffusion-limited current density （4.471 mA·cm^-2）, which was comparable to that of a Pt/C catalyst （4.941 mA·cm^-2）. Compared to Pt/C, Co3O4-PPy/GN catalysts displayed better long-term stability, methanol tolerance, and anti-CO-poisoning effects, which are of great significance for the design and development of advanced non-precious metal electrocatalysts.
基金supported by the Funds for Creative Research Groups of China(Grant No.61421002)the National Natural Science Foundation of China(Grant No.61571097)
文摘In this paper, composite film based on polyvinylpyrrolidone(PVP)/graphene oxide(GO) was fabricated by spray method on AT-cut 9.986 MHz quartz crystal microbalance(QCM) for NH_3 sensing. The thin films were characterized by scanning electron microscope(SEM), Fourier transform infrared spectroscopy(FTIR) and ultraviolet-visible spectroscopy(UV-VIS) to investigate the morphologies and the composition contents, respectively. The experimental results reveal that PVP/GO based sensor holds higher sensitivity, larger responsiveness and smaller baseline drift than those based on pure PVP at room temperature. Besides, the prepared sensor exhibits greater response to NH_3 than other gases such as CO, CO_2 and NO_2 at the same concentration. The good linearity, reproducibility and stability demonstrate the practicability of PVP/GO hybrid film in detecting NH_3.
