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1.
Hydrogen has attracted huge interest globally as a durable, environmentally safe and renewable fuel. Electrocatalytic hydrogen evolution reaction (HER) is one of the most promising methods for large scale hydrogen production, but the high cost of Pt-based materials which exhibit the highest activity for HER forced researchers to find alternative electro-catalyst. In this study, we report noble metal free a 3D hybrid composite of tungsten-molybdenum oxide and reduced graphene oxide (GO) prepared by a simple one step hydrothermal method for HER. Benefitting from the synergistic effect between tungsten-molybdenum oxide nanowires and reduced graphene oxide, the obtained W-Mo-O/rGO nanocomposite showed excellent electro-catalytic activity for HER with onset potential 50 mV, a Tafel slope of 46 mV decade?1 and a large cathodic current, while the tungsten-molybdenum oxide nanowires itself is not as efficient HER catalyst. Additionally, W-Mo-O/rGO composite also demonstrated good durability up to 2000 cycles in acidic medium. The enhanced and durable hydrogen evolution reaction activity stemmed from the synergistic effect broadens noble metal free catalysts for HER and provides an insight into the design and synthesis of low-cost and environment friendly catalysts in electrochemical hydrogen production.  相似文献   

2.
The design and development of inexpensive and highly efficient electrocatalysts for hydrogen production from water splitting are highly crucial for green energy and the hydrogen economy. Herein, we report phosphine reduced an iron-doped tungsten oxide nanoplate/reduced graphene oxide nanocomposite (Fe-WOxP/rGO) as an excellent electrocatalyst for the hydrogen evolution reaction. This electrocatalyst was synthesized using a hydrothermal method, followed by reduction with phosphine (PH3), which was generated from sodium hypophosphite. The catalyst onset potential, Tafel slope, and stability were investigated. Accordingly, Fe-WOxP/rGO exhibited impressively high electrocatalytic activity with a low overpotential of 54.60 mV, which is required to achieve a current density of 10 mAcm?2. The Tafel slope of 41.99 mV dec?1and the linear sweep voltammetry curve is almost the same as 2000 cycles and electrolysis under static overpotential (54.60 mV) is remain for more than 24 h in 0.5 M H2SO4. The catalytic activity and conductivity of Fe-WOxP/rGO were higher than WOXP, Fe-WOxP and WOxP/rGO. Such an outstanding performance of the Fe-WOxP/rGO nanocomposite is attributed to the coupled synergic effect between high oxygen vacancies formation on tungsten oxide in the nanoplate-like structure of Fe-WOxP and rGO nanosheet, making it as an excellent electrocatalyst for hydrogen evolution reaction.  相似文献   

3.
Functionalized carbon based 2D materials are promising candidates for low cost and environment friendly electrocatalyst for hydrogen evolution reaction (HER) and supercapacitor applications. To overcome the limitations posed by the noble metals and transition metal based composites, we have successfully synthesized metal free polysulfide functionalized reduced graphene oxide (GPS) in a simple chemical route. Structure and morphology of the material are characterized via XRD, FTIR, Raman, TEM, XPS measurements. The material behaves as an efficient HER electrocatalyst in acidic medium as well as energy storage device. It shows an onset potential of 97 mV and overpotential of 254 mV to reach a high current density of 10 mA/cm2. DFT calculations are carried out to understand the structural stability and identification of active sites of the material. Boosting catalytic activity via increasing the number of active sites is an elegant approach. In this material we have used the S atoms of polysulfide polymer to facilitate hydrogen adsorption and desorption, thus improving the hydrogen evolution ability. The supecapacitor attains the high specific capacitance 347 F/g at the current density of 1 A/g. The origin of such performances is due to synergistic effect of both the graphene network and the polysulfide functionalizations.  相似文献   

4.
Integrating MoS2 with carbon-based materials, especially graphene, is an effective strategy for preparing highly active non-noble-metal electrocatalysts in the hydrogen evolution reaction (HER). This work demonstrates a convenient hydrothermal method to fabricate molybdenum disulfide nanosheets/nitrogen-doped reduced graphene oxide (MoS2/NGO) hybrids using polyoxomolybdate as the Mo precursor. Introducing more defects and expanding interlayer spacing of MoS2 can be achieved through decreasing the pH value of the reactive system due to the existed high-nuclear polyoxometalate clusters. MoS2/NGO hybrids prepared at low pH exhibit superior HER activity to those obtained at high pH. MoS2/NGO-pH1.5 exhibits an ultralow overpotential of 81 mV at 10 mA cm−2, a low Tafel slope of 60 mV·dec−1 and good stability in alkaline electrolyte. Such excellent electrocatalytic activity is contributed by the abundant HER catalytic active sites, the increased electrochemically-accessible area and the synergetic effects between the active MoS2 catalyst and NGO support.  相似文献   

5.
The research and developments of porous, highly active non-noble metal cathode materials are the current hot spots. In our work, ZIF-9 (Zeolitic imidazolate framework-9) as a cobalt source provide porous structure, we have sulfurized the ZIF-9 into CoS2 by a simple hydrothermal method. Ultimately, the porous CoS2/RGO cathode material was obtained. Through a series of characterization analyses (powder X-ray diffraction, X-ray photoelectron spectroscopy), it is confirmed that the CoS2/RGO composite was successfully formed. Furthermore, electrochemical tests demonstrated that the pursued catalyst exhibited remarkable hydrogen evolution reaction (HER) activities with a favorable overpotential (only 180 mV for 10 mA cm?2 vs reversible hydrogen electrode), a low Tafel slopes (75 mV decade?1) and high stability in acidic condition (more than 18 h).  相似文献   

6.
In recent years, graphene oxide membranes showed interesting performances in terms of high permeating flux and perm-selectivity in several applications of gas separation because of their inherent properties combined to a low energy consumption. In this paper, a graphene oxide layer is coated on modified TiO2-alumina tubular substrate in order to prepare graphene oxide nanocomposite membranes useful for hydrogen separation. Nanocomposite graphene oxide membrane samples were obtained by using vacuum deep coating method, depositing the graphene oxide solution as single layers on TiO2-alumina substrate. Temperature and pressure variations were evaluated to achieve high H2 permeance, high H2/CO2 selectivity and membrane performance stability during the experimental tests. Furthermore, it was found that the temperature increase causes a perm-selectivity (H2/N2 and H2/CO2) decrease, while the transmembrane pressure increase involves a general improvement of the perm-selectivity.  相似文献   

7.
Developing the novel catalysts with an excellent performance of hydrogen generation is essential to facilitate the application of hydrogen evolution reaction (HER). Herein, a heterostructured cobalt phosphide/nickel phosphide/carbon cloth (CoP/Ni2P/CC) composite was fabricated via an interfacial engineering strategy to achieve the modification of CoP nanoleaf on Ni2P nanosheet skeleton supported by carbon cloth. By virtue of the unique heterostructure, abundant exposing active sites and the synergistic coupling effect of CoP and Ni2P nanoparticles, the elaborated CoP/Ni2P/CC composite exhibits a robust catalytic property. Among fabricated composites, the optimal CoP/Ni2P/CC-4 catalyst behaves an excellent HER performance at a wide pH range (overpotentials of 67, 71 and 95 mV to afford 10 mA cm?2 in 0.5 M H2SO4, 1 M KOH and 1 M PBS, respectively). The HER current density of this composite shows a negligible degradation after continuous test for 24 h. Charmingly, the HER process of this catalyst was innovatively applied to reduce graphene oxide, and thus exploiting the fabrication route of reduced graphene oxide (rGO). We are sure that this work will provide a firm guideline for the exploitation of pH-universal HER catalysts and the exploration of HER application.  相似文献   

8.
Designing an efficient and stable electrocatalyst made of earth abundant elements to take over expensive noble metal based for Hydrogen Evolution Reaction (HER) have been focused. Cobalt disulfide-molybdenum disulfide nanocomposite supported by nitrogen doped reduced graphene oxide and multiwalled carbon nanotubes (CoS2/MoS2@NrGO-MWCNT) is reported as an efficient electrocatalyst for HER. CoS2/MoS2@N-rGO-MWCNT and ternary hybrids composed of CoS2, MoS2 and N-rGO/MWCNT have been investigated. The catalysts were prepared by facile hydrothermal method, and the optimal doping ratio referred to date cobalt to molybdenum as 2:1 was chosen. It is found that co-existence of CoS2, MoS2 brings abundant active sites and incorporation of MWCNT offered stability. Good dispersion of CoS2 nanoparticles on graphene and MoS2 sheets is observed. Additionally nitrogen doping on rGO sheets has been carried out to boost up the electronegativity of the catalyst as a support to enhance the catalytic activity of CoS2/MoS2 for refine structure and better electrical conductance. Precisely, CoS2/MoS2@N-rGO-MWCNT exhibited smaller tafel slope 73 mV dec?1 at overpotential 281 mV for current density 10 mA cm?2 and the substantial stability of 14 h is recorded in 0.5 M H2SO4 medium, results suggest that catalyst is viable alternate for HER.  相似文献   

9.
Hydrogen is considered as the most important energy carrier for the future. Water electrolysis is a green method for hydrogen production and simple technology that produces very clean gases. However, the main problems with this method are that this process possesses slow kinetic, consumes many energies and its common electrocatalyst is platinum (Pt) based which is an expensive and rare substance. The use of accessible electrocatalyst materials with new shape or structure, which can reduce the overpotential for the hydrogen evolution reaction (HER) is one of the ways to increase the efficiency of the electrolyzers. Herein, first, a graphite sheet was modified with graphene oxide (GO) and then a hyperbranched structure of gold was electrodeposited on it by controlling the electrodeposition conditions. The electrode surface was characterized by scanning electron microscopy (SEM), field emission scanning electron microscopy (FE-SEM), X-ray diffraction (XRD), energy dispersive X-ray spectroscopy (EDS) and Fourier transform infrared spectroscopy (FT-IR). The HER performance of the prepared electrodes was evaluated using linear sweep voltammetry (LSV) and electrochemical impedance spectroscopy (EIS) methods in 0.5 M H2SO4 solution. The as-prepared electrode revealed outstanding HER performance with a near-zero onset overpotential (4.7 mV), overpotential of 44 mV at 10 mA cm−2, a high current density of 127.9 mA cm−2 at 200 mV and also satisfactory stability. Such results suggest that this electrocatalyst is promising for generating clean energy on an industrial scale.  相似文献   

10.
Advanced electrocatalysts for the fabrication of sustainable hydrogen from water splitting are innermost to energy research. Herein, we report the growth of iron diselenide (FeSe2) nanorods on graphene oxide (GO) sheets using two-step process viz., simple hydrothermal reduction and followed by wet chemical process. The orthorhombic phase of FeSe2 incorporated GO nanosheet was developed as a low-cost and efficient electrocatalyst for hydrogen evolution reaction (HER) by water splitting. The phase purity, crystalline structure, surface morphology and elemental composition of the synthesized samples have been investigated by UV–visible absorption spectroscopy (UV–vis), fourier transform-infrared spectroscopy (FT-IR), X-ray diffraction (XRD), field emission scanning electron microscopy (FE-SEM) and energy dispersive X-ray analysis (EDS). Voltammetry and Tafel polarization methods have been utilized to assess the performance of various weight ratio of GO nanosheet in FeSe2 nanorods towards H2 evolution. Detailed electrochemical investigations revealed that the 30% FeSe2/GO composite showed a tremendous electrocatalytic HER activity in acidic medium with high cathodic current density of 9.68 mA/cm2 at η = 250 mV overpotential and with a Tafel slope of 64 mV/dec. The 30% FeSe2/GO composite offers a high synergistic effect towards HER activity, which is mainly due to high electrochemical active catalytic sites, low charge-transfer resistance and enhanced electrocatalytic performances of H2 production. The present analysis revealed the possible application of FeSe2/GO composite as a promising low-cost alternative to platinum based electrocatalysts for H2 production.  相似文献   

11.
Facile fabrication of high-performance catalyst based on low-cost metals for sustainable hydrogen evolution is still a matter of cardinal significance. However, synthetic approaches for electrocatalyst are usually complicated and the yields are often low. Herein, we report a one-step simple method for the large-scale synthesis of Co/Ni-MoO2 composite as efficient and stable hydrogen evolution reaction (HER) electrocatalyst to drive 10 mA cm?2 current density with a low overpotential of 103 mV in basic media. Co-MoO2 and Ni-MoO2 were also prepared using this method with overpotential of 137 and 130 mV, respectively, to gain the same current density. These results indicate that this facile synthesis approach is of great practical importance as it can be easily used for large-scale preparation of electrocatalysts in industry.  相似文献   

12.
Benefiting from improved electrical conductivity, the N-doped MoSe2 nanosheets show substantially enhanced HER activity with a lower onset overpotential of approximately ?135 mV and a smaller Tafel slope of 62 mV dec?1, which exhibiting enhanced catalytic performance compared with that of pure MoSe2. The success of improving the HER performance via the introduction of N dopant offers a new opportunity in the development of high performance MoSe2-based electrocatalyst.  相似文献   

13.
Various reduced graphene oxide supported CuS (RGO-CuS) composites were obtained via a hydrothermal way in this work. The as-obtained RGO-CuS with a low bandgap of ~1.24 eV showed significant light absorption in near-infrared (NIR) region. In acidic media, the optimized 0.1RGO-CuS needed an overpotential of 179 mV (at 10 mA cm−2) to trigger the hydrogen evolution reaction under NIR light. And the lowest Tafel slope of 0.1RGO-CuS (61 mV dec−1), suggesting that the photoelectrocatalytic hydrogen evolution was performed under the Volmer-Heyrovsky mechanism. The 0.1RGO-CuS displayed a good durability after 5000 cycles in acid. According to the results of EIS measurement, both NIR irradiation and RGO modification could effectively lower charge transfer resistance and improve charge transport rate of the photoelectrochemical process. The introduction of RGO could improve the electron and hole separation ability of the photoelectrochemical process, which resulted in an enhanced photoelectrocatalytic HER performance.  相似文献   

14.
Developing low cost co-catalysts is crucial for both fundamental research and practical application of g-C3N4. In this work, we prepared ternary Ni2P/rGO/g-C3N4 nanotubes with different Ni2P contents for visible-light-driven photocatalytic H2 generation from triethanolamine aqueous solution. The optimal Ni2P/rGO/g-C3N4 produced H2 at a rate of 2921.9 μmol h−1 g−1, which is about 35, 16 and 9 times as large as that of g-C3N4, binary rGO/g-C3N4 and Ni2P/g-C3N4, respectively. The apparent quantum efficiency of optimal Ni2P/rGO/g-C3N4 was 5.6% at λ = 420 nm. We believe that the improved photocatalytic performance of Ni2P/rGO/g-C3N4 originates from the synergistic effect of rGO as electron transfer medium and Ni2P as reaction site, which is supported by photoelectrochemical and photoluminescence measurements. Cyclic experiment demonstrated an excellent stability of Ni2P/rGO/g-C3N4. Moreover, we further studied the effect of other nickel-based compounds by replacing Ni2P with NiS, Ni3C, and Ni3N, respectively. The order of the H2-generation rate is Ni2P/rGO/CNNT > NiS/rGO/CNNT > Ni3C/rGO/CNNT > Ni3N/rGO/CNNT, which could be reasonably explained based on Mott–Schottky plots. Our work reveals that Ni2P can be used as a promising cocatalyst for photocatalytic H2 evolution.  相似文献   

15.
Reduced graphene oxide (rGO) supported g-C3N4-TiO2 ternary hybrid layered photocatalyst was prepared via ultrasound assisted simple wet impregnation method with different mass ratios of g-C3N4 to TiO2. The synthesized composite was investigated by various characterization techniques, such as XRD, FTIR, Raman Spectra, FE-SEM, HR-TEM, UV vis DRS Spectra, XPS Spectra and PL Spectra. The optical band gap of g-C3N4-TiO2/rGO nanocomposite was found to be red shifted to 2.56 eV from 2.70 eV for bare g-C3N4. It was found that g-C3N4 and TiO2 in a mass ratio of 70:30 in the g-C3N4-TiO2/rGO nanocomposite, exhibits the highest hydrogen production activity of 23,143 μmol g?1h?1 through photocatalytic water splitting. The observed hydrogen production rate from glycerol-water mixture using g-C3N4-TiO2/rGO was found to be 78 and 2.5 times higher than g-C3N4 (296 μmol g?1 h?1) and TiO2 (11,954 μmol g?1 h?1), respectively. A direct contact between TiO2 and rGO in the g-C3N4-TiO2/rGO nanocomposite produces an additional 10,500 μmol g?1h?1 of hydrogen in 4 h of photocatalytic reaction than the direct contact between g-C3N4 and rGO. The enhanced photocatalytic hydrogen production activity of the resultant nanocomposite can be ascribed to the increased visible light absorption and an effective separation of photogenerated electron-hole pairs at the interface of g-C3N4-TiO2/rGO nanocomposite. The effective separation and transportation of photogenerated charge carriers in the presence of rGO sheet was further confirmed by a significant quenching of photoluminescence intensity of the g-C3N4-TiO2/rGO nanocomposite. The photocatalytic hydrogen production rate reported in this work is significantly higher than the previously reported work on g-C3N4 and TiO2 based photocatalysts.  相似文献   

16.
Application of carbonic materials as catalysts has recently been considered due to some advantages like tunable molecular structures, easy synthesis methods, abundance, and high tolerance in acidic and alkaline media. Here, a new metal-free electrocatalyst of halogenated reduced graphene oxide was prepared using cyclic voltammetry X (F, Br, and I)-RGO electrodeposition method. The prepared electrocatalysts were studied as a novel metal-free electrocatalyst for the hydrogen evolution reaction, and the presence of several halogen and oxygen functional groups on the surface of nanosheets was verified by the furrier transform infra-red, FT-IR, spectroscopy, and the presence of doped halogens on the RGO surface was confirmed by energy-dispersive X-ray, EDX, spectroscopy. The structural features and surface morphology of electrocatalysts were investigated by scanning electron microscopy (SEM) analysis. The electrochemical treatment of the X (F, Br, I)-RGO electrode was studied by some techniques like electrochemical impedance spectroscopy, EIS, chronoamperometry, CA, and linear sweep voltammetry, LSV. The X (F, Br, I)-RGO catalyst showed a lower onset potential (?0.81 V. vs. SHE), higher exchange current density (3.1 × ×10?1 mA cm?2), and lower charge transfer resistance (1.09 Ω cm2) related to the RGO catalyst due to the high active sites by heteroatoms and graphene nanosheets.  相似文献   

17.
A facile approach to synthesize reduced graphene oxide (RGO) loaded potassium niobate microspheres was reported. The composition, microstructure and electron-transfer properties of the obtained product were characterized. Compared to pure potassium niobate microspheres and commercial P25 TiO2, the as-prepared potassium niobate microspheres/RGO composite showed much higher photocatalytic activity for generating hydrogen under UV irradiation. It was ascribed to the enhanced separation efficiency of electron/hole pairs as testified by electrochemical impedance spectrum and fluorescence spectrum. Importantly, the composite photocatalyst was stable and easy to recycle, and the amount of hydrogen evolution did not decrease after six recycles. The results are potentially applicable to a range of semiconductors useful in water reduction as well as other areas of heterogeneous photocatalysis.  相似文献   

18.
Herein, reduced graphene oxide supported well-dispersed bimetallic AuPt alloy nanodendrites (AuPt ANDs/rGO) were fabricated by a one-pot coreduction approach using ionic liquid (1-aminopropyl-3-methylimidazolium bromide, [APMIm]Br) as the stabilizer and capping agent. There is no any other polymer or seed involved. Characterized measurements include transmission electron microscopy (TEM), high angle annular dark-field scanning TEM (HAADF-STEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The typical samples displayed excellent electrocatalytic activity and durability towards hydrogen evolution reaction (HER) and methanol oxidation reaction (MOR) in contrast with Pt nanocrystals/rGO and commercial Pt/C (50%) catalysts, which make it promising for practical catalysis in energy conversion and storage.  相似文献   

19.
Hydrogen energy has received great attention because of its advantages such as large energy density and not producing carbon dioxide, and it is currently considered to be one of the most valuable green energy sources. Therefore, the development of efficiently hydrogen production is of great importance. Hydrogen production from water electrolysis has large application prospects due to its cleanliness and no pollution. However, how to prepare an efficient, stable and low-cost electrocatalyst for this process is still challenging. Here, we develop a reduced graphene oxide-supported ruthenium (Ru) nanoparticle electrocatalyst synthesized by a simple method. The ruthenium precursors are encapsulated and isolated with N,N-dimethylformamide (DMF) (Ru3+-DMF), which effectively inhibits the further agglomeration growth of ruthenium. After Ru3+-DMF being loaded on graphene oxide, Ru is supported on reduced graphene oxide (Ru/rGO) by the liquid phase chemical reduction method and the remaining organic solvent could be removed by calcination to form a well-dispersed Ru-based electrocatalyst. Ru/rGO shows excellent electrocatalytic activity and long-term stability for hydrogen evolution reaction (HER). In a solution of 1.0 M KOH, the overpotential of 3.0 wt%Ru/rGO for the HER at 100 mA cm?2 is only 111.7 mV, and the Tafel slope is 31.5 mV dec?1. It exhibits better HER performance compared to commercial Pt/C and other Ru/rGO catalysts with different Ru loadings. The work could give a new strategy for the synthesis of efficient electrocatalysts.  相似文献   

20.
Up to now, it is still a great challenge to develop active, durable and low-cost non-precious metal catalysts toward hydrogen evolution reaction (HER). In this paper, we synthesized ultrafine Co6Mo6C nanocrystals on reduced graphene oxide (RGO) support (Co6Mo6C/RGO). The Co6Mo6C/RGO shows Pt-like HER performance, which exhibits almost zero onset overpotential, and very small overpotential of 64 mV at 10 mA cm?2. In addition, the Co6Mo6C/RGO has a very small Tafel slope of 44 mV dec?1 and a high exchange current density of 0.402 mA cm?2, suggesting fast reaction kinetics. Furthermore, the Co6Mo6C/RGO demonstrates superior durability in acid electrolyte. The distinguished HER performance makes Co6Mo6C/RGO the promising candidate as non-precious metal catalyst for HER in acid electrolyte.  相似文献   

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