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1.
In this work, a Co–N doped carbon nanotube (CNT) catalyst was fabricated via a simple pyrolysis approach and the effects of solvothermal processing on the catalytic activity of the as-prepared material were investigated in detail. The results show that after solvothermal processing (Co-NC) the catalyst has a more homogeneous anemone structure, a higher nitrogen content, a larger BET surface area and a higher degree of graphitization compared to the catalyst produced after non-solvothermal processing (Co-MA). The results of electrochemical tests indicate that Co-NC, compared to commercial 20% Pt/C and Co-MA, has an improved mass transfer process and sufficient active site exposure, which brings about superb oxygen reduction electrocatalytic activity, a higher reduction potential (−0.2 V vs. Ag/AgCl), a limiting diffusion current (5.44 mA cm−2) and excellent stability in 0.1 M KOH solution.

In this work, a Co–N doped carbon nanotube (CNT) catalyst was fabricated via a simple pyrolysis approach.  相似文献   

2.
A highly efficient and low-cost oxygen evolution reaction electrocatalyst is essential for water splitting. Herein, a simple and cost-effective autologous growth method is developed to prepare NiFe-based integrated electrodes for water oxidation. In this method, a Ni(OH)2 nanosheet film is first developed on nickel foam by oxidative deposition in a chemical bath solution. The as-prepared nanosheet electrode is then immersed into a solution containing Fe(iii) cations to form an Fe-doped Ni(OH)2 electrode by utilization of the different solubility of metal cations. Benefiting from its unique and integrated nanostructure, this hierarchically structured electrode displays extremely high catalytic activity toward water oxidation. In 1 M KOH, the electrode can deliver a current density of 1000 mA cm−2 at an overpotential of only 330 mV. This work provides a facile way to produce an efficient, durable, and Earth-abundant OER electrocatalyst with no energy input, which is attractive for large-scale water splitting.

We report here a simple and cost-effective autologous growth method to prepare a NiFe-based integrated electrode for efficient electrocatalytic water oxidation.  相似文献   

3.
Low-cost and efficient electrocatalysts with high dispersion of active sites and high conductivity are of high importance for oxygen evolution reaction (OER). Herein, we use amorphous mesoporous fumed silica (MFS) as a skeleton material to disperse Ni2+ and Fe3+ through a simple impregnation strategy. The MFS is in situ etched away during the OER process in 1 M KOH to prepare a stable mesoporous Ni–Fe electrocatalyst. The high specific surface area and abundant surface silanol groups in the mesoporous fumed silica afford rich anchor sites for fixing metal atoms via strong chemical metal–oxygen interactions. Raman and XPS investigations reveal that Ni2+ formed covalent bonds with surface Si–OH groups, and Fe3+ inserted into the framework of fumed silica forming Fe–O–Si bonds. The mesoporous Ni–Fe catalysts offer high charge transfer abilities in the OER process. When loaded on nickel foam, the optimal 2Ni1Fe-MFS catalyst exhibits an overpotential of 270 mV at 10 mA cm−2 and a Tafel slope of 41 mV dec−1. Notably, 2Ni1Fe-MFS shows a turnover frequency value of 0.155 s−1 at an overpotential of 300 mV, which is 80 and 190 times higher than that of the state-of-the-art IrO2 and RuO2 catalysts. Furthermore, 2Ni1Fe-MFS exhibits 100% faradaic efficiency, large electrochemically active surface area, and good long-term durability, confirming its outstanding OER performance. Such high OER efficiency can be ascribed to the synergistic effect of high surface area, dense metal active sites and interfacial conductive path. This work provides a promising strategy to develop simple, cost-effective, and highly efficient porous Ni–Fe based catalysts for OER.

A stable mesoporous Ni–Fe–O electrocatalyst with high OER efficiency is constructed using mesoporous fumed silica as a template.  相似文献   

4.
The fabrication of cost effective and efficient electrocatalysts with functional building blocks to replace noble metal ones is of great importance for energy related applications yet remains a great challenge. Herein, we report the fabrication of a hierarchical structure containing CNTs/graphene/transition-metal hybrids (h-NCNTs/Gr/TM) with excellent bifunctional oxygen electrocatalytic activity. The synthesis was rationally designed by the growth of shorter nitrogen-doped CNTs (S-NCNTs) on longer NCNTs arrays (L-NCNTs), while graphene layers were in situ generated at their interconnecting sites. The hybrid material shows excellent OER and ORR performance, and was also demonstrated to be a highly active bifunctional catalyst for Zn–air batteries, which could be due to rapid electron transport and full exposure of active sites in the hierarchical structure.

A hierarchical structure containing aligned CNTs/graphene/transition-metal was fabricated and worked as a highly active bifunctional catalyst for Zn–air batteries.  相似文献   

5.
Carbon fiber is an absorbing material with high strength, acid and alkali resistance, high temperature resistance, flexibility, and processability and plays an important role in the electromagnetic (EM) wave absorption of civil buildings and military equipment. However, its EM wave-absorption performance is poor because of its large complex permittivity and no magnetic loss ability. In this study, dopamine hydrochloride and FeCl3 were used as precursors, and the Fe3O4/N-doped carbon coating was successfully grown in situ on the surface of short carbon fiber (SCF) via dopamine deposition, autopolymerization, FeCl3 solution immersion, and calcination at high temperature to improve its EM wave-absorption property. The obtained Fe3O4/N-doped carbon particles were uniformly attached to the SCF in the form of a thin layer to constitute a unique hierarchical structure. The Fe3O4/N-doped carbon coating/SCF displayed an excellent EM wave-absorption performance. An effective bandwidth of 8.64 GHz and lowest reflection loss of −31.38 dB at 3 mm were achieved because of the significant reduction in complex permittivity and improvement in complex permeability, wave impedance, and EM loss ability of the SCF. The Fe3O4/N-doped carbon coating is expected to show great potential in EM wave-absorption fields.

Carbon fiber is an absorbing material with high strength, acid and alkali resistance, high temperature resistance, flexibility, and processability and plays an important role in the electromagnetic (EM) wave absorption of civil buildings and military equipment.  相似文献   

6.
The interesting g-C3N4 nanosheet morphology has drawn huge attention in photocatalytic applications because of its special features. Nonetheless, the relative activity of these nanosheets is still controversial due to the low available active sites and the high recombination probability of photo-induced charge carriers. In this work, in situ sol–gel approach was applied to synthesize holey g-C3N4 nanosheets/hydroxyapatite (HAp) nanospheres with plentiful in-plane holes. Herein, the presence of Ca2+ plays a key role in the formation of holey defects on 2D g-C3N4. In-plane holes provide nanosheets with more active edges and diffusion channelsv, resulting in a tremendous enhanced mass and photo-induced charge transfer speed. Moreover, the holes make highly numbered boundaries, which lead to the prevention of aggregation. On the other hand, distributed nano-HAp spheres on these nanosheets can form effective heterojunctions having high photo-degradation ability of pollutants. Intrinsic O-vacancies inside HAp unit cells mainly affect the capture of photogenerated electrons, pollutant molecules, and O2 gas. The synergistic presence of O-vacancies and holey defects (C-vacancies) on 2D g-C3N4 plays a key role in raising the photocatalytic performance of holey g-C3N4/HAp. It can be concluded that the proposed preparation method is a promising approach for simultaneous synthesis of holey g-C3N4 and surface heterojunctions of Ca-based materials. This new structure has shown significant degradation ability of bisphenol A, a prominent pollutant, with a low amount (0.01 g) and short time.

The interesting g-C3N4 nanosheet morphology has drawn huge attention in photocatalytic applications because of its special features.  相似文献   

7.
A nanocomposite of Ag@C nanocapsules dispersed in a multi-walled carbon nanotube (MWCNT) matrix was fabricated in situ by a facile arc-discharge plasma approach, using bulk Ag as the raw target and methane gas as the carbon source. It was found that the Ag@C nanocapsules were ∼10 nm in mean diameter, and the MWCNTs had 17–32 graphite layers in the wall with a thickness of 7–10 nm, while a small quantity of spherical carbon cages (giant fullerenes) were also involved with approximately 20–30 layers of the graphite shell. Typical dielectric behavior was dominant in the electronic transport of Ag@C/MWCNT nanocomposites; however, this was greatly modified by metallic Ag cores with respect to pure MWCNTs. A temperature-dependent resistance and IV relationship provided evidence of a transition from Mott–David variable range hopping [ln ρ(T) ∼ T−1/4] to Shklovskii–Efros variable range hopping [ln ρ(T) ∼ T−1/2] at 5.4 K. A Coulomb gap, ΔC ≈ 0.05 meV, was obtained for the Ag@C/MWCNT nanocomposite system.

An electric transition from ln ρ(T) ∼ T−1/4 to ln ρ(T) ∼ T−1/2 hopping conduction happened at 5.4 K in situ synthesis of Ag@C/MWCNTs nanocomposite.  相似文献   

8.
A solvent-free, low-cost, high-yield and scalable single-step ball milling process is developed to construct 2D MoS2/graphene hybrid electrodes for lithium-ion batteries. Electron microscopy investigation reveals that the obtained hybrid electrodes consist of numerous nanosheets of MoS2 and graphene which are randomly distributed. The MoS2/graphene hybrid anodes exhibit excellent cycling stability with high reversible capacities (442 mA h g−1 for MoS2/graphene (40 h); 553 mA h g−1 for MoS2/graphene (20 h); 342 mA h g−1 for MoS2/graphene (10 h)) at a high current rate of 250 mA g−1 after 100 cycles, whereas the pristine MoS2 electrode shows huge capacity fading with a retention of 37 mA h g−1 at 250 mA g−1 current after 100 cycles. The incorporation of graphene into MoS2 has an extraordinary effect on its electrochemical performance. This work emphasises the importance of the construction of the 2D MoS2/graphene hybrid structure to prevent capacity fading issues with the MoS2 anode in lithium-ion batteries.

A solvent-free, low-cost, high-yield and scalable single-step ball milling process is developed to construct 2D MoS2/graphene hybrid electrodes for lithium-ion batteries.  相似文献   

9.
Hierarchical porous carbon (HPC) consists of micropores, mesopores and macrospores which are synthesized by in situ formation of template followed by acid etching. The obtained pores are three-dimensional and interconnected, and evenly distributed in the carbon matrix. By adjusting the ratio of the raw materials, the high specific surface area and large pore volume is afforded. The obtained HPC-3 samples possess graphite flakes and locally graphited-carbon walls, which provide good electrical conductivity. These unique characteristics make these materials suitable cathode scaffolds for Li–S batteries. After encapsulating 61% sulfur into HPC-3 host, the S/HPC-3 composite exhibits excellent cycling stability, high columbic efficiency, and superior rate cycling as a cathode material. The S/HPC-3 composite cathode displays an initial discharge capacity of 1059 mA h g−1, and a reversible capacity of 797 mA h g−1 after 200 cycles at 0.2C. The discharge capacities of the S/HPC-3 composite cathode after every 10 cycles at 0.1, 0.2, 0.5, 1, and 2C are 1119, 1056, 982, 921, and 829 mA h g−1, respectively.

In situ template synthesis of HPCs used for lithium–sulfur batteries, which exhibits excellent cycling stability and superior rate cycling.  相似文献   

10.
Direct integration of monolayer graphene on a silicon (Si) substrate is realized by a simple thermal annealing process, involving a top copper (Cu) layer as the catalyst and an inserted polymethylmethacrylate (PMMA) as the carbon source. After spin-coating the PMMA carbon source on the Si substrate, the Cu catalyst was deposited on PMMA/Si by electron beam evaporation. After that, graphene was directly synthesized on Si by decomposition and dehydrogenation of PMMA and the catalyzation effect of Cu under a simple thermal annealing process. Furthermore, under an optimized growth condition, monolayer graphene directly formed on the Si substrate was demonstrated. Utilizing the as-grown graphene/Si heterojunction, near-infrared photodetectors with high detectivity (∼1.1 × 1010 cm Hz1/2 W−1) and high responsivity (50 mA W−1) at 1550 nm were directly fabricated without any post-transfer process. The proposed approach for directly growing graphene on silicon is highly scalable and compatible with present nano/micro-fabrication systems, thus promoting the application of graphene in microelectronic fields.

Direct integration of monolayer graphene on a silicon (Si) substrate is realized by a simple thermal annealing process, involving a top copper (Cu) layer as the catalyst and an inserted polymethylmethacrylate (PMMA) as the carbon source.  相似文献   

11.
Durable and efficient electrocatalysts toward the oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) are crucial to the development of sustainable energy conversion. In this article, we report a highly active bifunctional electrocatalyst derived from ZIF-8 through simple heat-treatment activation. The resultant catalyst is enriched with Rh nanoparticles in the carbon matrix, showing excellent ORR performance with a half-wave potential (E1/2) of 0.803 V in alkaline electrolytes; it is simultaneously active for catalyzing the HER with an overpotential of 89 mV to reach a current density of 10 mA cm2 in acidic electrolytes. The prepared RhNC-900 catalyst (1.47 wt% Rh) is comparable to the commercial Pt/C catalyst (20 wt% Pt) in terms of the ORR in alkaline media and might inspire new ideas for the development of fuel cells and water splitting.

ZIF-derived RhNC-900 bifunctional electrocatalysts for the oxygen reduction reaction and hydrogen evolution reaction have been prepared via a simple and scalable method, exhibiting excellent catalytic activity and promising performance.  相似文献   

12.
The prevention of photocorrosion in photocatalysts allows for the use of a wide variety of visible-light-responsive photocatalysts, leading to highly efficient photocatalytic reactions. This study aimed to avoid the photocorrosion issues associated with pure CdS, a known photocorrosive photocatalyst, by forming a stable CdWO4 shell on the surface of a CdS core. The CdS/CdWO4 core–shell composite was formed using a unique method based on CdS elution under acidic conditions. An optimal CdWO4 nanorod shell was formed at a pH of 0.8, a reaction time of 30 min, and a calcination temperature of 400 °C, where the core remained intact and was sufficiently coated. The prepared CdS/CdWO4 core–shell composite was shown to be stable when exposed to light irradiation in pure water. Furthermore, it was successfully used in water splitting with an oxidation reaction side photocatalyst. This core–shell synthesis method based on core dissolution was easily and highly controlled, and is suitable for use in other similar core–shell composite applications.

The prevention of photocorrosion in photocatalysts allows for the use of a wide variety of visible-light-responsive photocatalysts, leading to highly efficient photocatalytic reactions.  相似文献   

13.
This paper reports the facile and scalable synthesis of hybrid N-doped carbon quantum dots/multi-walled carbon nanotube (CD/CNT) composites, which are efficient alternative catalysts for the oxygen reduction reaction (ORR) in fuel cells. The N-doped CDs for large-scale production were obtained within 5 minutes via a one-step polyol process using ethylenediamine (ED) in the presence of hydrogen peroxide as an oxidizing agent. For comparison, different CDs were also prepared using ethylene glycol (EG) and ethanolamine (EA) in the same manner. Physicochemical characterization suggested the successful formation of a CD(ED)/CNT hybrid without individual CD(ED)s and CNTs. The N-doped CD(ED)/CNT catalyst exhibited excellent electrocatalytic activity in an alkaline solution compared to other composites (CD(EG)/CNT and CD(EA)/CNT). The Tafel slope (−60.9 mV dec−1) and durability (∼9.1% decay over 10 h) for CD(ED)/CNT were superior to high-performance Pt/C catalysts. The electrochemical double-layer capacitance on the CD(ED)/CNT hybrid showed apparent improvement of the active surface area because of N-doping and highly decorated CDs on the CNT wall. These results provide an innovative approach for the potential application of all carbon hybrid structures in electrocatalysis.

The ORR measurements showed that the CD(ED)/CNT catalyst was superior to CD(EG)/CNT and CD(EA)/CNT. They even surpassed the activity of commercial Pt/C in terms of durability, Tafel slope, and MeOH tolerance.  相似文献   

14.
Developing efficient electrocatalysts for ORR/OER is the key issue for the large-scale application of rechargeable Zn–air batteries. The design of Co and N co-doped carbon matrices has become a promising strategy for the fabrication of bi-functional electrocatalysts. Herein, the surface-oxidized Co nanoparticles (NPs) encapsulated into N-doped hierarchically porous carbon materials (Co/NHPC) are designed as ORR/OER catalysts for rechargeable Zn–air batteries via dual-templating strategy and pyrolysis process containing Co2+. The fabricated electrocatalyst displays a core–shell structure with the surface-oxidized Co nanoparticles anchored on hierarchically porous carbon sheets. The carbon shells prevent Co NP cores from aggregating, ensuring excellent electrocatalytic properties for ORR with a half-wave potential of 0.82 V and a moderate OER performance. Notably, the obtained Co/NHPC as a cathode was further assembled in a zinc–air battery that delivered an open-circuit potential of 1.50 V, even superior to that of Pt/C (1.46 V vs. RHE), a low charge–discharge voltage gap, and long cycle life. All these results demonstrate that this study provides a simple, scalable, and efficient approach to fabricate cost-effective high-performance ORR/OER catalysts for rechargeable Zn–air batteries.

The surface-oxidized Co nanoparticles incorporated in N-doped hierarchically porous carbon materials are designed as ORR/OER catalyst for rechargeable Zn–air batteries via dual-templating strategy and pyrolysis process.  相似文献   

15.
In this article, an exquisite flexible hybrid MoS2/graphene free-standing electrocatalyst paper was fabricated by a one-step in situ solvothermal process. The assembled MoS2/graphene catalysts exhibit significantly enhanced electrocatalytic activity and cycling stability towards the splitting of water in acidic solution. Furthermore, a strategic balance of abundant active sites at the edge of the S–Mo–S layers with efficient electron transfer in the MoS2/graphene hybrid catalyst plays a key role in controlling the electrochemical performance of the MoS2 nanosheets. Most importantly, the hybrid MoS2/graphene nanosheet paper shows excellent flexibility and high electrocatalytic performance under the various bending states. This work demonstrates an opportunity for the development of flexible electrocatalysts, which have potential applications in renewable energy conversion and energy storage systems.

An improved flexible hybrid MoS2/graphene free-standing electrocatalyst paper was fabricated by a one-step in situ solvothermal process for hydrogen evolution reaction applications.  相似文献   

16.
In this work, a series of C-doped BiVO4 (BiVO4-T) with natural leaf structures were synthesized by a dipping-calcination method with the leaf of Chongyang wood seedling as a template under different calcination temperatures. The structures and morphologies of BiVO4-T were observed by FE-SEM observations. The doped carbon in BiVO4-T was formed in situ from the natural leaf during the calcination process and the amount of doping could be regulated from 0.51–1.16 wt% by controlling the calcination temperature. It was found that the sample calcined at 600 °C (BiVO4-600) with a C-doping content of 1.16 wt% showed the best photocatalytic degradation activity. After 120 min visible light irradiation, the photocatalytic decomposition efficiency of RhB for BiVO4-600 is 2.2 times higher than that of no template BiVO4. The enhanced photocatalytic performance is ascribed to the combined action of the unique morphology and doped-carbon. It is considered that the unique structures and carbon doping of BiVO4-600 are in favor of the enhancement of visible light absorption, which was supported by UV-vis DRS. Furthermore, the C-doping can enhance the efficient separation and transfer of the photo-generated electron–hole pairs, as proved by PL measurements. This study provides a simple dipping-calcination method and found the best calcination temperature to fabricate a high-performance BiVO4, which simultaneously achieves morphology and C-doping control in one step.

A series of C-doped BiVO4 with natural leaf as a template were synthesized under different calcination temperatures by the dipping-calcination method, which simultaneously achieves morphology and C-doping control in one step.  相似文献   

17.
Multi-color-emissive fluorescent polymer nanocomposite films have potential applications in optoelectronic devices. Herein, stretchable, mechanically stable multi-color carbon-dots-based films are in situ fabricated by condensation and aging of carboxylated polyurethane in the presence of various carbon sources. As-prepared CDs/PU films emit different colors covering from blue (414 nm) to red (620 nm) by tuning reaction conditions. Moreover, CDs are fixed and have good dispersion in the PU matrix due to the interactions of amine groups from the carbon sources with the carboxylate group of PU. Thus, phase separation of composite films can be avoided. And, more than 90% of their emission intensity is preserved after soaking in water for 30 days, aging for up to 6 h at 100 °C, and subjecting to several cycles of stretching and natural recovery. These advantages are encouraging for the use of CDs/PU composite films in solid-state lighting applications. Remote multi-color LEDs have been fabricated by placing a down-conversion layer of CDs/PU films separated through coating them on the same chips (emission at 365 nm), with Commission Internationale de l''Eclairage color coordinates of (0.22, 0.23), (0.43, 0.53), (0.49, 0.46), and (0.41, 0.28), respectively.

Stretchable, mechanically stable multi-color carbon-dots-based polymer films are in situ fabricated, and showed potential for application in optoelectronic devices.  相似文献   

18.
A novel ZnO–GO/CGH composite was prepared using an in situ synthesis process for photodegradation of methylene blue under visible light illumination. The chitin–graphene composite hydrogel (CGH) was used to provide uniform binding of the nano ZnO–GO composite to the hydrogel surface and prevent their agglomeration. GO provides multi-dimensional protons and electron transport channels for ZnO with a flower-like structure, which possessed improved photo-catalytic activity. SEM analysis indicates that the hydrogel has good adsorption properties with rougher surfaces and porous microstructure, which enables it to adsorb the dyes effectively. Under synergetic enhancement of adsorption and photo-catalysis, catalytic activity and nano ZnO–GO/CGH recycling improved greatly. Synthesized nano ZnO–GO/CGH showed high dye removal efficiency of 99%, about 2.2 times that of the pure chitin gel under the same condition. This suggests the potential application of the new photocatalytic composites to remove organic dyes from wastewater.

A novel ZnO–GO/CGH composite was prepared using an in situ synthesis process for photodegradation of methylene blue under visible light illumination.  相似文献   

19.
Porous electrospun carbon nanofibers (CNFs) can be produced by a more advantageous ‘in situ activation’ method by electrospinning polyacrylonitrile (PAN) with an activation agent. However, most in situ activated electrospinning processes yield porous CNFs with rather limited surface area and less porosity due to the inappropriately selected activation agents. Here we found K2S could perfectly meet both compatibility and reactivity requirements of PAN electrospinning to generate hierarchical meso/micropores inside electrospun CNFs. During the whole fabrication process, K2S experiences a phase evolution loop and the hierarchical pore structures are formed by the reaction between K2S oxidative derivatives and the as-formed carbon during heat treatment. The hierarchical meso/microporous CNFs not only showed a large surface area (835.0 m2 g−1) but also exhibited a high PAN carbonization yield (84.0 wt%) due to improved cyclization of PAN''s nitrile group during the pre-oxidation stage. As an electrode material for supercapacitors, the corresponding electrodes have a capacitance of 210.7 F g−1 at the current density of 0.2 A g−1 with excellent cycling durability. The hierarchically porous CNFs produced via in situ activation by K2S combine the advantages of interconnected meso/micropores and are a promising candidate for electrochemical energy conversion and storage devices.

K2S was found to be an excellent in situ activation agent for the fabrication of electrospun carbon nanofibers with large surface area (835.0 m2 g−1) and hierarchical meso/microporous structures.  相似文献   

20.
Herein, MWCNT-graft-polyimides (MWCNT-g-PIs) were prepared by the in situ grafting method. Strengthening the interfacial interaction between MWCNTs and polyimide chains decreased their interfacial thermal resistance (RC). In contrast to the RC of 10% MWCNT/PIs, the RC of 10% MWCNT-g-PI decreased by 16.7%. Hence, MWCNT-g-PIs possessed higher thermal conductivity than MWCNT/polyimides (MWCNT/PIs). Meanwhile, the Tg values of all the samples (MWCNT/PIs and MWCNT-g-PIs) were greater than 399 °C (by DMA). Compared with MWCNT/PIs, 5% and 10% MWCNT-g-PIs showed enhancement in thermal stability in air. The storage modulus retentions were greater than 63% at 200 °C and 45% at 300 °C. Also, 5% and 10% MWCNT-g-PIs maintained the high tensile strength of pure PI, and the tensile modulus increased up to 2.59 GPa on increasing the loading amount of MWCNTs. This study sheds light on improving the thermal conductivity of polyimides effectively at relatively low loadings.

In situ synthesis of MWCNT-graft-polyimides enhanced thermal conductivity at a relatively low loading.  相似文献   

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