首页 | 官方网站   微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 203 毫秒
1.
Achieving high catalytic performance with the lowest possible amount of noble metal is critical for any catalytic applications. Herein, we report a controllable method of preparing low Ru loaded, N-doped porous carbon embedded with cobalt oxide species (Ru/CoOx@NPC) using core-shell metal-organic framework (MOF) as a template. The optimized catalyst exhibits a highly powerful yet stable performance of H2 production through sodium borohydride (NaBH4) hydrolysis. The Ru/CoOx@NPC catalyst shows a fast H2 generation rate (8019.5 mL min?1 gcat?1), high turnover frequency (1118.6 mol min?1 molRu?1), and reusability. The carbonized ZIF-8 core and the ZIF-67 outer shell supplies a porous carbon moiety that not only improves the conductivity and but also provides uniform distribution of the active sites. The XPS analysis indicates that there is a strong electronic interaction between Co species and Ru species. The superior catalytic performance can be attributable to the large specific surface area as well as the synergy between Co-oxide and Ru clusters.  相似文献   

2.
In our previous research, titanium-based nitride with high conductivity and superior corrosion resistance were developed as an ideal core material for replacing noble metal to form Pt-based core-shell catalysts by pulse electrodeposition. Meanwhile, the smaller sizes of nitride cores would also be available for pulse electrodeposition by dispersing them on carbon nanotubes (CNT). To achieve a better practice on the preparation of the Pt-based core-shell catalysts, in this work, both nitrogen-doped carbon nanotubes (N-CNT) and reduced graphene oxide (N-rGO) were used to support the copper-doped titanium nitride (Ti0.9Cu0.1N) cores. In the course of pulse electrodeposition, their influences as supports on the electronic states of electrodeposited Pt as well as their catalytic activities were compared. The results showed that the Pt preferred to electrodeposit on Ti0.9Cu0.1N cores supported by N-CNT and formed a core-shell structure. While with the same electrodeposition process, the Pt was found to be electrodeposited not only on the Ti0.9Cu0.1N cores supported by N-rGO with heavy aggregations but also on the N-rGO support. Raman spectroscopy analysis indicated that the higher degree of structural defects on N-rGO, as support, might have contributed to such divergence observation.  相似文献   

3.
Through annealing and electrochemical reduction methods, we successfully fabricates reduced graphene oxide layer (RGOL) modified carbon nanotube and reduced graphene oxide (CNT + RGO) doped polyphenylene sulfide (PPS) flexible thin film electrodes. These composite structure films can not only overcome the brittle nature of PPS, but also make good use of the thermal stability of PPS. Furthermore, carbon nanotube and reduced graphene oxide enhance the electrical conductivity of the composite films. Truncated octahedral and cuboctahedral Cu2O nanocrystals are synthesized on RGOL modified CNT + RGO doped PPS (RGOL@PPS/CNT + RGO) composite film by a facile electrodeposition method without using any surfactants or external heating. RGOL on the PPS/CNT + RGO substrate facilitates the formation of Cu2O morphology. The obtained Cu2O composite film shows a superior ability for the hydrogen evolution reaction (HER) compared with other Cu2O electrocatalysts. The Cu2O with a smaller loading less than 0.04 mg cm?2 on the composite film exhibits excellent HER activities with a low onset potential of 0.05 V and large current densities. The results of the HER performance indicates that the RGOL@PPS/CNT + RGO composite film has a potential application in flexible hydrogen-producing devices.  相似文献   

4.
Engineering multicomponent active materials as an advanced electrode with the rational designed core-shell structure is an effective way to enhance the electrochemical performances for supercapacitors. Herein, three-dimensional self-supported hierarchical CoMoO4@CoS core-shell heterostructures supported on reduced graphene oxide/Ni foam have been rationally designed and prepared via a facile approach. The unique structure and the synergistic effects between two different materials, as well as excellent electronic conductivity of the reduced graphene oxide, contribute to the increased electrochemically active site and enhanced capacitance. The core-shell CoMoO4@CoS composite displays the superior specific capacitance of 3380.3 F g−1 (1 A g−1) in the three-electrode system and 81.1% retention of the initial capacitance even after 6000 cycles. Moreover, an asymmetric device was successfully prepared using CoMoO4@CoS and activated carbon as positive/negative electrodes. It is worth mentioning that the device delivered the high energy density of 59.2 W h kg−1 at the power density of 799.8 W kg−1 and the excellent cycle performance (about 91.5% capacitance retention over 6000 cycles). These results indicate that the core-shell CoMoO4@CoS composites offers the novelty strategy for preparation of electrodes for energy conversion and storage devices.  相似文献   

5.
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   

6.
Research on water splitting reaction is on priority to explore an alternative source of energy with little to no carbon emissions. Among the two half reactions of electrochemical water splitting, oxygen evolution reaction (OER) is highly desirable yet challenging to prepare a cost effective and viable electrocatalyst to boost the OER activity. Herein, we have prepared a novel electrocatalyst, CoOx-CoP/N-CNTs, by the phosphidization of cobalt oxides (CoOx) encapsulated N- doped carbon nanotubes (CoOx/N-CNTs). The CoOx/N-CNTs composite is derived via pyrolysis of cobalt based zeolitic imidazole framework (ZIF-12) at 950 °C under argon atmosphere. The CoOx/N-CNTs is phosphidized at various temperatures ranging from 320 °C to 400 °C. The optimized temperature to attain the best catalytic activity is 380 °C. The phosphatized material, CoOx-CoP/N-CNTs, shows superior performance towards OER with an overpotential of 250 mV @ 20 mAcm?2 vs 532 mV @ 20 mAcm?2 of un-phosphidized material, CoOx/N-CNTs, which shows significant effect of phosphidization. The maximum current density of 160 mAcm?2 in 1 M KOH solution is achieved.  相似文献   

7.
A phytic acid-derived Co2-xNixP2O7-C/RGO composite was designed and facilely synthesized, in which phytic acid acted as both a phosphoric source and carbon source. Both carbon derived from phytic acid and reduced graphene oxide (RGO) in composite, enhanced the conductivity and thus improve its electrocatalytical capability. As-synthesized Co1.22Ni0.78P2O7-C/RGO composite exhibited excellent oxygen evolution reaction (OER) catalytic performances: At the current density of 10 mA cm−2, only a low overpotential of 283 mV and a small Tafel slope of 51 mV dec−1 were observed. Good OER catalytic performance was retained even after 10 h continuously running at a constant voltage, which is even comparable to those of first-rate noble metal catalyst RuO2. In addition, the performances of Co2-xNixP2O7-C/RGO catalysts were also strongly dependent on Ni content.  相似文献   

8.
Methanol oxidation catalyzed by bi-layered or mixed oxides of cobalt and cerium was studied at atmospheric pressure by temperature-programmed reaction technique. The catalysts were deposited in the form of thin films by magnetron sputtering from Co and CeO2 targets, forming double layer structures of CeO2/CoOx or CoOx/CeO2. Reaction selectivity and hydrogen production rates were monitored at O2:CH3OH reactant stoichiometries varied in the range 4:1–1:4, spanning from oxygen rich to oxygen lean reaction conditions. A complementary information in regard to thermal stability of the catalytic layers was obtained by X-ray photoelectron spectroscopy. A strong synergistic interaction between cerium and cobalt within the mixed oxide (driving dynamics of the Co2+/Co3+ and Ce4+/Ce3+ redox pairs and oxygen exchange) leads to a bi-functional catalyst. Particularly the CeO2/CoOx configuration proved to be significantly more active than the CoOx alone and more stable, especially under reducing environments. Further optimization of reactivity can be provided via control of the adlayer coverage.  相似文献   

9.
A novel hybrid composite RGO-CeO2 NWS with the nanowire-sheet structure was synthesized by a facile hydrothermal process using ethanol/water as the solvent without any organic additives. The graphene oxide proceeds to reduce to graphene and chemical bonds form between graphene oxide and CeO2 NWS. Pt-based catalysts with the RGO-CeO2 NWS composite as the support were then prepared by a microwave-assisted polyol process. The resultant catalysts were characterized by X-ray diffraction, Raman spectroscopy, Scanning tunneling microscopy, X-ray photoelectron spectroscopy, High resolution transmission electron microscopy and electrochemical tests. The results show that the hybrid Pt/RGO4-CeO2 NWS exhibits the best catalytic activity and the increased catalytic efficiency of Pt in the hybrid catalysts is evidence that CeO2 NWS are anchored onto the chemical defects in the wrinkles and edges of the graphene surface. This avoids the restacking of graphene oxide, thus hindering the Pt nanoparticles embedded in folding and increasing the exposed active sites. The changed valence state from Ce4+ to Ce3+ in CeO2 NWS will introduce oxygen vacancies and thus promote the tolerance of intermediate species in methanol oxidation.  相似文献   

10.
Fe-, Ni- and Zn- doped La0·9Sr0·1CoO3 are prepared and a single-component solid oxide fuel cell composed of 30 wt% perovskite oxide and 70 wt% samarium-doped ceria (SDC)-(Li0·67Na0.33)2CO3 is fabricated and characterized. When doping with either Fe, Ni or Zn, most cations occupy the Co3+ sites. X-ray photoelectron spectroscopy and oxygen temperature-programmed desorption characterizations show that Zn-doped La0·9Sr0·1CoO3 exhibits notably high surface oxygen, causing higher catalytic activity for oxygen reduction reaction (ORR) than that of nondoped La0·9Sr0·1CoO3. Fe or Ni doping into La0·9Sr0·1CoO3 decreases surface oxygen, resulting in a lower catalytic activity toward ORR than La0·9Sr0·1CoO3. Furthermore, X-ray diffraction, temperature-programmed reduction and transmission electron microscopy characterizations prove that after reduction, Fe-doped La0·9Sr0·1CoO3 is reduced to Co0·72Fe0.28 alloy-oxide core-shell nanoparticles, resulting in a high catalytic activity for hydrogen oxygen reaction (HOR). However, NiCo2O4 are formed during the reduction of Ni-doped La0·9Sr0·1CoO3, exhibiting a low catalytic activity for the HOR. Similarly, the low catalytic activity of reduced Zn-doped La0·9Sr0·1CoO3 for the HOR is caused by the formation of ZnCo2O4. A single component fuel cell composed with Fe-doped La0·9Sr0·1CoO3-SDC-(Li0·67Na0.33)2CO3 exhibits the highest Pmax of 239.1 mW cm−2 at 700 °C with H2 as fuel, indicating that HOR processes are rate-determining steps.  相似文献   

11.
In this study, nanocomposite electrocatalysts composed of cobalt molybdenum sulfide flower-like nanosheets intermixed with reduced graphene oxide (CoxMo(1?x)S2/rGO) were prepared by a facile one-step hydrothermal method and were used to prepare counter electrodes (CE) of high-performance dye-sensitized solar cells (DSSCs). The structural and morphological analysis of the nanocomposites were carried out using field emission scanning electron microscopy, micro-Raman, and X-ray photoelectron spectroscopies, which revealed 2-dimensional petal-like nanosheets of the ternary metal sulfides intermixed with the reduced graphene oxide sheets. The DSSCs fabricated using CoxMo(1?x)S2/rGO (CMS-2/rGO) as the counter electrode material exhibited power conversion efficiency (PCE) of 9.04%, which was found to be superior to the PCEs of DSSCs with CEs made of MoS2/rGO (7.56%), CoxMo(1-x)S2 (7.04–7.78%), and conventional Pt (8.72%). The electrochemical measurements showed that the excellent electrocatalytic activity of the CoxMo(1?x)S2/rGO on I3- can be attributed to the expanded active sites, improved charge transfer across the CE, and reduced electrode/electrolyte interface resistance. The facile preparation approach and outstanding catalytic behavior of CoxMo(1?x)S2/rGO indicate that the nanostructured CoxMo(1-x)S2/rGO intermix would be a cost-effective material over the platinum used in the CE of DSSCs.  相似文献   

12.
The sluggish kinetics of oxygen-evolution reaction (OER) through water-oxidation reaction results in high overpotentials for water splitting. Among different compounds, carbon-based material/Mn oxide composites were reported as OER catalysts. Fullerene soot (FS), which contains a mixture of fullerenes and carbon blacks, is low-cost compared to fullerenes and is commercially available. Herein, the Mn oxide/fullerene soot (MnOx/FS) composite was investigated as an OER catalyst under neutral conditions. The composite was prepared through the reaction of KMnO4 and FS as a facile, easy, and low-cost procedure. In this method, amorphous Mn oxide is formed directly on FS. The material was characterized by a number of methods. Then, the OER catalytic activity of MnOx/FS was studied in a LiClO4 solution (pH ≈ 6.3). Compared to pristine FS, the OER activity of MnOx/FS is 2.5 times higher at 2.25 V vs. RHE. The Tafel slopes for OER are 450 and 240 mV per decade for FS and the reported composite, respectively.  相似文献   

13.
In this present paper, cobalt oxide (CoOx) is studied as an effective cocatalyst in a photocatalytic hydrogen production system. CoOx-loaded titanium dioxide/cadmium sulfide (TiO2/CdS) semiconductor composites were prepared by a simple solvothermal method and characterized by powder X-ray diffraction (XRD), transmission electron microscopy (TEM), ultraviolet–visible diffuse reflectance spectroscopy (UV–Vis DRS), and X-ray photoelectron spectroscopy (XPS). Photocatalytic hydrogen production was studied using the as-synthesized photocatalysts in aqueous solution containing sodium sulfide (Na2S)/sodium sulfite (Na2SO3) as hole scavengers under visible light irradiation (λ > 400 nm). The optimal cobalt content in CoOx-loaded TiO2/CdS composite is determined to be 2.1 wt% and the corresponding rate of hydrogen evolution is 660 μmol g−1 h−1, which is about 7 times higher than TiO2/CdS and CdS photocatalysts under the same condition. Visible light-driven photocurrents of the semiconductor composites were further measured on a photoelectrochemical electrode, revealing that the photocorrosion of CdS can be prevented due to the presence of TiO2–CoOx.  相似文献   

14.
Titanium carbide is a good candidate for tritium permeation barrier in a fusion reactor. However, its oxidation susceptibility and the mismatch between the ceramic coating and substrate are still a challenge. In this study, a promising candidate as a hydrogen permeation barrier, comprising a titanium-based ceramic TiO2/TiCx composite coating, was proposed. The preparation process of this TiO2/TiCx composite coating involves two steps of carbon ion implantation and oxidation under ultra-low oxygen partial pressure. According to the results, the optimal oxidation temperature for TiO2 coating is 550 °C, with the increase of the oxidation temperature, the particles on the surface of the oxide layer become coarse and loosely arranged, and the protective performance of the oxide layer is greatly reduced. The hydrogen barrier permeation behavior of the composite coating in a fusion reactor was simulated via hydrogen plasma discharge environment, the results show that the hydrogen barrier permeation performance of the composite is significantly better than that of a single TiO2 coating. In addition, the coatings treated with hydrogen plasma showed a certain self-repairing performance through the diffusion growth of the TiCx layer. These findings illustrate a novel method for preparing composite coatings to restrain hydrogen permeation, providing insight into the development of hydrogen permeation barrier materials.  相似文献   

15.
Developing highly efficient and stable supported bimetallic nanoparticles catalysts via a facile strategy is one of the most admirable methods for sustainable hydrogen production from borohydride hydrolysis. Herein, we developed a facile technology for rapidly and straightforwardly manufacturing Pt–Ni bimetallic nanoparticles (BNPs) supported by partially reduced graphene oxide (prGO) with excellent catalytic activity and outstanding durability for hydrogen production from KBH4 and NH3BH3 alkaline solution. The uniformly dispersed Pt40–Ni60 BNPs with a statistical size of around 2.6 nm exhibited a surprising catalytic activity of 23,460 mol-H2·h?1·mol-Pt?1 at 308 K, moreover, whose activity was high up to 80% of the first time even after 30 runs, demonstrating an outstanding stability. The apparent activation energy for dehydrogenation of KBH4 and NH3BH3 were respectively about 27.8 and 33.6 kJ/mol for the prepared Pt40–Ni60/prGO catalyst. The extraordinary catalytic activity of the Pt40–Ni60/prGO catalyst owing to the strong charge transfer effect between Pt–Ni BNPs and graphene.  相似文献   

16.
Photo-electro-catalytic degradation of antibiotics such as berberine in water with simultaneous hydrogen evolution is an attractive option. It can control pollution using solar energy and provide clean energy. The photo electrodes play vital role in this kind of photocatalytic electrolytic cell. To obtain better electrode with high degradation capacity and fast hydrogen generation rate, using a facile one-pot hydrothermal process, a series of nano-structured composite FeMoO4-GO (graphene oxide) catalysts with improved absorbance in 250–800 nm were synthesized, and loaded on CFC (carbon fiber cloth). Their photo electrode performance were compared. Using SEM(scanning electron microscope), XRD (X-ray diffraction) and XPS(X-ray photoelectron spectroscopy), the catalysts were characterized, and LSV(linear sweep voltammetry), CV(cyclic voltammetry) and EIS(electrochemical impedance) were used to characterize the electrodes. In 1 M KCl supporting electrolyte, at current density 10 mA cm−2, 90% berberine was removed in 30 min and hydrogen generation rate was 3.1 μmol cm−2 min−1 in photo-electro-catalysis system. The results show rapid hydrogen generation and enhanced pollutant degradation.  相似文献   

17.
Al and its alloys are studied extensively for hydrogen generation through water splitting. Alloying Al with metal activators such as bismuth, indium, gallium, etc., leads to the formation of micro galvanic cells during hydrolysis reaction, resulting in an improved hydrogen generation rate. Activation of Al by adding carbon-based materials such as graphite, carbon nanotubes (CNTs), graphene, etc., can instantaneously generate hydrogen at room temperature. When carbon particles are desorbed from the Al matrix during hydrolysis, new Al is exposed, resulting in an increased reaction rate. In Al-Graphite composites which form core-shell structures, H2O molecules penetrate through the graphite layers and break down the core-shell structure during hydrolysis, and the new Al surfaces are exposed to water. It was found that Al with nano bismuth and graphene nanosheets showed better hydrogen generation rate and hydrogen yield. Graphene nanosheets control the agglomeration of Al and enhance the specific surface area for hydrolysis. During the hydrolysis of Al-CNTs composites, CNTs act as a cathode, resulting in galvanic corrosion between CNTs and the Al matrix. CNTs can also effectively control the agglomeration of Al during ball milling. Spark plasma sintered Al–Bi-CNT composites showed an enhanced hydrogen generation rate during hydrolysis. This paper presents an overview of hydrogen generation by hydrolysis of Al and its alloys, emphasising the addition of carbon-based materials such as graphite, graphene, CNTs, etc.  相似文献   

18.
Iron/carbon-black composite nanoparticles were synthesized by chemically reducing the iron salt mixing with carbon black by adding NaBH4 in the aqueous solution. Carbon-black particles, with a mean particle size of approximately 40 nm, function as the nucleation cores for iron deposition. Additionally, core-shell iron composite particles are observed to be 30-100 nm with spherical sharp. At the first time discharge, the iron/carbon-black composite nanoparticle discharged 1200 mAh g−1(Fe) at plateau one and 400 mAh g−1at plateau two at a high current density of 200 mA g−1(Fe). The capacity is larger than the theoretical value, which is attributed to the formation of iron hydride (FeHx) while the iron was reduced by NaBH4, followed the hydrogen reaction as an active material while the battery discharge occurs. In further cycles, the iron/carbon-black composite iron electrode shows a good reversibility of about 600 mAh g−1(Fe) when the nickel-iron battery operated between 1.65 and 0.8 V. XRD analysis results indicate that the carbon black in the core of the iron/carbon-black composite enhances the reduction/oxidation reactions of iron, as achieved by the carbon black forming an enhanced electronic conductive network while iron is discharged as the insulator species such as Fe(OH)2 and Fe3O4. SEM images reveal that the iron/carbon-black composite keeps particle sizes smaller than 300 nm during the electrode cycling, indicating that carbon black also acts as the nucleation cores for the dissolution-deposition of iron.  相似文献   

19.
A Ni and MoxC hybrid (Ni-MoxC) supported on N-doped reduced graphene oxide (N-rGO) electrocatalyst with high hydrogen evolution reaction (HER) activity was prepared by ultrasonication and lyophilization. Notably, benefiting from the synergistic effect between Ni and MoxC nanoparticles, the optimized electrocatalyst displayed excellent catalytic activity with low overpotentials of 183 mV and 216 mV for the HER at the current density 10 mA cm−2 in 1.0 M KOH and 0.5 M H2SO4 solution. The stability of the electrocatalyst could be well maintained for 24 h. These results indicate that the method to prepare hybrid (Ni-MoxC) is a simple way to produce cost-effective and high-efficient molybdenum carbide for hydrogen evolution.  相似文献   

20.
Highly dispersed Pd and MnOx nanoparticles supported on the graphitic carbon nitride with different composition have been prepared by a simple liquid deposition-reduction method and used as an efficient FA decomposition catalyst for hydrogen generation. The catalytic activity depends on the Pd-MnOx composition of catalyst, the FA/SF ratio and the reaction temperature. The Pd-MnOx/CN-1 catalyst exhibited excellent catalytic activity for hydrogen generation with the initial TOF of 465 h?1 from formic acid-sodium formate mixture aqueous solution with a FA/SF ratio of 1:8 at 348 K. The synergetic effect between Pd nanoparticles and the carbon nitride support, the Mn/Pd ratios, the good dispersion of nanoparticles and the nature of the carbon nitride support were suggested to be responsible for the efficient catalytic performance of the Pd-MnOx/CN nanocatalysts.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司    京ICP备09084417号-23

京公网安备 11010802026262号