首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 15 毫秒
1.
Nano ferrites of the formula MFe2O4 (M = Ni, Cu, Zn), synthesized using sol–gel technique, were employed to catalyze the reductive transformation of nitrophenols to aminophenols. The catalytic reduction was carried out in the excess of NaBH4 as reducing agent in aqueous medium at room temperature. CuFe2O4 and NiFe2O4 were found to be active for the reduction of nitrophenols with significant difference in their activities whereas ZnFe2O4 was found to be inactive. The kinetics of the reduction of nitrophenols to aminophenols was also investigated. The reaction followed pseudo first order kinetics. The first order rate constant values for 30 mol% of CuFe2O4 and NiFe2O4 for the reduction of 2-nitrophenol were observed to be 3.68 min−1 and 0.33 min−1 respectively. The rates of reduction for the three isomers of nitrophenol were also studied and were observed to follow the order – 2-nitrophenol > 4-nitrophenol > 3-nitrophenol. The selective formation of aminophenol was confirmed using LC-MS, 1H NMR and FT-IR spectroscopic techniques.  相似文献   

2.
Four different earth-abundant ferrite nanoparticles (MFe2O4, M: Mn, Fe, Co, Ni) with spinel structure were synthesized by using the surfactant-assisted high temperature thermal decomposition methods and then assembled on mesoporous graphitic carbon nitride (mpg-CN) to study their comparative catalysis for the photocatalytic hydrogen evolution reaction (HER) in the presence of Eosin-Y (EY) as a visible-light sensitizer. The yielded monodisperse ferrite nanoparticles and the MFe2O4/mpg-CN nanocomposites were characterized by using advanced analytical techniques including TEM, XPS, XRD, ICP-MS, and UV–Vis DRS. All the tested MFe2O4/mpg-CN nanocomposites provided the better catalytic performance than that of pristine mpg-CN in the photocatalytic HER and their photocatalytic HER rates are in the order of NiFe2O4/mpg-CN > CoFe2O4/mpg-CN > MnFe2O4/mpg-CN > Fe3O4/mpg-CN > mpg-CN. Among the tested MFe2O4/mpg-CN nanocomposites, NiFe2O4/mpg-CN nanocomposite provided the highest hydrogen generation of 14.56 mmol g−1, which is 6.75 times greater than that of pristine mpg-CN and, using EY as a visible light sensitizer and triethanolamine (TEOA) as a sacrificial reagent. According to the optical properties and energy band positions of the nanocomposites, a plausible mechanism for the NiFe2O4/mpg-CN catalyzed HER is proposed to give insights on the highest activity of NiFe2O4/mpg-CN nanocomposites among others.  相似文献   

3.
Constructing high-efficient and nonprecious electrocatalysts is of primary importance for improving the efficiency of water splitting. Herein, a novel sunflower plate-like NiFe2O4/CoNi–S nanosheet heterostructure was fabricated via facile hydrothermal and electrodeposition methods. The as-fabricated NiFe2O4/CoNi–S heterostructure array exhibits remarkable bifunctional catalytic activity and stability toward oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in alkaline media. It presents a small overpotential of 219 mV and 149 mV for OER and HER, respectively, to produce a current density of 10 mA cm?2. More significantly, when the obtained electrodes are used as both the cathode and anode in an electrolyzer, a voltage of 1.57 V is gained at 10 mA cm?2, with superior stability for 72 h. Such outstanding properties are ascribed to: the 3D porous network structure, which exposes more active sites and accelerates mass transfer and gas bubble emission; the high conductivity of CoNi–S, which provides faster charge transport and thus promotes the electrocatalytic reaction of the composites; and the effective interface engineering between NiFe2O4 (excellent performance for OER) and CoNi–S (high activity for HER), which leads to a shorter transport pathway and thus expedites electron transfer. This work provides a new strategy for designing efficient and inexpensive electrocatalysts for water splitting.  相似文献   

4.
Searching for low-cost electrocatalysts with high activity towards the hydrogen evolution reaction (HER) is of great significance to enable large-scale hydrogen production via water electrolysis. In this study, by using inverse spinel MFe2O4(M = Mn, Fe, Co, Cu) nanoparticles (NPs) as the precursors, monodisperse bimetallic phosphide M-Fe-P NPs/C with hollow structures were readily obtained by a gas-solid annealing method. These hollow phosphide NPs displayed excellent HER activity in an acidic medium with a low loading amount of 0.2 mg cm−2. In particular, the Co–Fe–P NPs/C shows highest HER activity that only requiring an overpotential of 97 mV to retain a current density of 10 mA cm−2. A volcano relation between activity and incorporated elements was revealed. Incorporation of cation with high electronegativity stabilized the FeP active centres, while phase segregation resulted in the loss of activity for Cu–Fe–P NPs/C.  相似文献   

5.
Transition metal phosphides have been known as promising electrocatalysts for hydrogen evolution and oxygen evolution reactions (HER and OER) due to their high catalytic activity. In this work, the FeCoP nanoparticles decorated on N-doped electrospun carbon nanofibers (FeCoP@NCNFs) was successfully synthesized through depositing Fe, Co-based Prussian blue analogue Co3[Fe(CN)6]2·10H2O (FeCo-PBA) onto the electrospun PVP/PAN nanofibers via layer-by-layer approach, followed by carbonization and phosphorization treatments. Benefiting from the high electrical conductivity, abundant catalytic active sites and the synergistic effect between FeCoP nanoparticles and N-doped carbon nanofibers network, the obtained FeCoP@NCNFs displays good bifunctional electrocatalytic activity. In 1 M KOH, the FeCoP@NCNFs achieves 10 mA cm?2 at an overpotential of 290, 226 mV for OER and HER, respectively. Moreover, it demands overpotential of 196 mV to achieve 10 mA cm?2 for HER in 0.5 M H2SO4. The FeCoP@NCNFs is used as both anode and cathode for overall water splitting, it requires a low voltage of 1.65 V to achieve a current density of 10 mA cm?2 and maintains outstanding stability over 10 h. Herein, a strategy for preparing bifunctional electrocatalysts of compositing transition metal phosphides with carbon nanofibers is proposed, and the application of metal-organic framework in electrocatalytic field is further extended.  相似文献   

6.
Active site engineering for electrocatalysts is an essential strategy to improve their intrinsic electrocatalytic capability for practical applications and it is of great significance to develop a new excellent electrocatalyst for overall water splitting. Here, Co3O4/nickel foam (NF) and Co2(P4O12)/NF electrocatalysts with flower-shaped and sea urchin-shaped structures are synthesized by a simple hydrothermal process and followed by a post-treatment method. Among them, Co2(P4O12)/NF shows good catalytic activity for hydrogen evolution reaction (HER), and at the current density of 10 mA cm?2, the overpotential is only 113 mV Co3O4/NF exhibits good catalytic activity for oxygen evolution reaction (OER), and the overpotential is 327 mV at 20 mA cm?2. An alkaline electrolyzer with Co3O4/NF and Co2(P4O12)/NF catalysts respectively as anode and cathode displays a current density of 10 mA cm?2 at a cell voltage of 1.59 V. This work provides a simple way to prepare high efficient, low cost and rich in content promising electrocatalysts for overall water splitting.  相似文献   

7.
To achieve high activity and stability for both hydrogen and oxygen evolution reactions through the non-precious-metal based electrocatalysts is still facing the great challenge. Herein, we demonstrate a facile strategy to prepare CoP nanoparticles (NPs) loaded on N, P dual-doped carbon (NPC) electrocatalysts with high concentration N and P dopants through a pyrolysis-deposition-phosphidation process. The great bifunctional electrocatalytic activity for both HER (the overpotential of 98 mV and 86 mV at 10 mA cm−2 in both 0.5 M H2SO4 and 1 M KOH electrolytes, respectively) and OER (the overpotential of 300 mV at 10  mA cm−2 in 1 M KOH electrolyte) were achieved. When CoP@NPC hybrid was used as two electrodes in the 1 M KOH electrolyte system for overall water splitting, the needed cell potential for achieving the current density of 10 mA cm−2 is 1.6 V, and it also showed superior stability for HER and OER after 10 h’ test with almost negligible decay. Experimental results revealed that the P atoms in CoP were the active sites for HER and the CoP@NPC hybrid showed excellent bifunctional electrocatalytic properties due to the synergistic effects between the high catalytic activity of CoP NPs and NPC, in which the doping of N and P in carbon led to a stronger polarization between Co and P in CoP, promoting the charge transfer from Co to P in CoP, enhancing the catalytic activity of P sites and Co sites in CoP for HER and OER, respectively. Specifically, the improvements could result from the changed charge state, the increased active specific surface area, and the facilitated reaction kinetics by N, P co-doping and admixture. This work provides a high-efficient, low-cost and stable electrocatalyst for overall water splitting, and throws light on rational designing high performance electrocatalysts.  相似文献   

8.
A facile three-step approach for tubular CoP preparation and its catalytic activity for HER and OER are reported. The CoP microtubes show superior HER performance in a wide pH range with low overpotentials of 91, 101 and 113 mV at 10 mA cm?2 in 0.5 M H2SO4, 1 M KOH and 1 M PBS, respectively. Additionally, it also depicts superior OER performance with an overpotential of 300 mV at 10 mA cm?2, which is lower than reported precious metal oxides. The improved electrocatalytic performance of tubular CoP is likely attributed to the porous tube-like structural features, which not only afford rich exposed active sites, but also accelerate the charge or mass transfer efficiency, and thus efficiently promote the HER performance. The synthesis of tubular CoP confirms the importance of morphology features and provides a new insight to rationally design and synthesize highly effective non-noble metal phosphide-based pH-universal electrocatalysts for HER.  相似文献   

9.
Transition metal-based heterostructure materials are considered as promising alternatives to state-of-the-art noble metal-based catalysts toward the oxygen evolution reaction (OER). Herein, for the first time, a simple interface engineering strategy is presented to synthesize efficient electrocatalysts based on a novel CoFe2O4/β-Ni(OH)2 heterogeneous structure for the electrochemical OER. Remarkably, the optimized CoFe2O4/β-Ni(OH)2 electrocatalyst, benefiting from its hierarchical hexagonal heterostructure with strong electronic interaction, enhanced intrinsic activity, and electrochemically active sites, exhibits outstanding OER electrocatalytic performance with a low overpotential of 278 mV to reach a current density of 10 mA cm−2, a small Tafel slope of 67 mV dec−1, and long-standing durability for 30 h. Its exceptional OER performance makes the CoFe2O4/β-Ni(OH)2 heterostructure a prospective candidate for water oxidation in alkaline solution. The proposed interface engineering provides new insights into the fabrication of high-performance electrocatalysts for energy-related applications.  相似文献   

10.
Synthesis of highly efficient, non-noble and bi-functional electrocatalysts is exceedingly challenging and necessary for water splitting devices. In this work, three-dimensional spherical Ni(OH)2/NiCo2O4 heterojunctions are prepared by a one-step hydrothermal method and the hybrids are explored as efficient electrocatalysts for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in an alkaline electrolyte via tuning different Ni/Co atomic ratios of heterojunctions. The optimized Ni(OH)2/NiCo2O4 (S (1:1)) exhibits high electrocatalytic activity with an ultralow over-potential of 189 mV at 10 mA cm−2 for the HER. With regard to the OER, the over-potential of the as-synthesized S (1:1) heterojunction is only 224 mV at the current density of 10 mA cm−2. The improved catalytic performance of the Ni(OH)2/NiCo2O4 heterojunctions is attributed to the chemical synergic combining of Ni(OH)2 and NiCo2O4, large specific surface area for exposing more accessible active sites, and heterointerface for activating the intermediates that facilitates electron/electrolyte transport. The prepared catalyst exhibits good durability and stability in HER and OER catalyzing conditions. This study provides a feasible approach for the building of highly efficient bifunctional water splitting electrocatalysts and stimulates the development of renewable energy conversion and storage devices.  相似文献   

11.
The development of highly efficient and low-cost electrocatalysts for large-scale hydrogen evolution reaction (HER) is great important but remains a significant challenge. Transition-metal phosphides (TMPs) have attracted intense attention as promising non-noble-metal HER electrocatalysts due to their unique electronic properties and high intrinsic catalytic activities. Herein, we directly grew NiXCo2-XP nanorod wrapped with N-doped carbon shell on 3D Ni foam to fabricate a self-supported electrode with core-shell nanorod array morphology. The obtained hybrid electrode exhibits remarkable electrocatalytic HER activity over a wide pH range with low overpotentials of 121 mV and 181 mV to obtain the current density of 200 mA cm−2 in 0.5 M H2SO4 and 1 M KOH electrolytes, respectively, which is comparable to that of the current state-of-the-art Pt/C electrocatalyst. The experimental results indicate that the elaborate architectural superiority and compositional synergy of this hybrid electrode give rise to the boosted HER performance.  相似文献   

12.
Hydrogen production is of significance in solving urgent energy and environmental issues, so it is necessary to develop superior electrocatalysts to catalyze the sustainable hydrogen evolution process efficiently. This study reports the synthesis of the Ni modified ultrafine MoxC (x = 1, 2) wrapped by nitrogen-doped carbon through a facile one-pot strategy, which can be applied for catalyzing the hydrogen evolution reaction (HER) in both acid and alkaline conditions. Benefiting from the regulating effect of Ni towards MoxC (x = 1, 2) and the synergistic mechanism among Ni, Mo2C and MoC, Ni/MoxC-NC exhibits superior electrocatalytic activity, displaying a low overpotential of 141 mV in 0.5 M H2SO4 and 110 mV in 1 M KOH at a current density of 10 mA cm−2 for HER, as well as long-term durability for 20 h.  相似文献   

13.
Nickel ferrite (NiFe2O4) has been explored as a promising oxygen evolution reaction (OER) electrocatalyst for water splitting owning to its earth-abundant and considerable water oxidation catalytic activity. Nevertheless, its practical electrocatalytic performance towards OER is still undesirable due to the sluggish OER kinetics and high overpotential gap on the water oxidation anode side. In this work, in order to enhance the electrochemical water oxidation performance of NiFe2O4, the surface of NiFe2O4 is functionalized with phosphate ions (Pi) by using a facile incipient impregnation and following calcination process. Results demonstrate that the OER properties of NiFe2O4 under alkaline conditions can be dramatically boosted by the surface Pi functionalization. In 1.0 M KOH solution, the resulting NiFe2O4-Pi on glassy carbon (GC) electrode demonstrates quite lower overpotential of 332 mV (10 mA/cm2) and Tafel slope of 57 mV/dec compared to that of pristine NiFe2O4 (443 mV@10 mA/cm2 and 96 mV/dec), which is also better than that of commercial RuO2 electrocatalysts (348 mV@10 mA/cm2 and 80 mV/dec). Moreover, such electrocatalyst on nickel foam electrode also realizes superior OER durability to afford a current density of 70 mA/cm2 at overpotential of only 300 mV for at least 28 h. The excellent electrocatalytic water oxidation activities of NiFe2O4-Pi can be attributed to the tuning electronic property and surface wettability by Pi ions functionalization. This work provides us a novel and effective approach to modify the photo-/electrocatalytic activity for transition metal oxides.  相似文献   

14.
In this work, we developed a novel hybrid with N-doped bamboo-like carbon nanotubes combined with the CoFe alloy and its oxide (denoted as CoFe–CoFe2O4/N-CNTs) via an extremely facile one-step pyrolysis method. When applied as an electrocatalyst towards OER in 1.0 M KOH solution, CoFe–CoFe2O4/N-CNTs exhibits a small overpotential of 334 mV to afford a current density of 10 mA cm−2 associated with a low Tafel slope of 80 mV dec−1 and long-term stability. The remarkable OER electrocatalytic performance of CoFe–CoFe2O4/N-CNTs is mainly attributed to the synergistic effect between CoFe and CoFe2O4 as well as the increased active sites resulting from the introduction of N-CNTs. More impressively, the introduction of Fe can significantly cut down the usage of relatively toxic and expensive Co accompanied with the dramatic enhancement of OER electrocatalytic performance originating from the robust synergistic effect between Co and Fe.  相似文献   

15.
The development of inexpensive electrocatalysts with excellent electrocatalytic activity for the hydrogen and oxygen evolution reactions (HER and OER, respectively) has been challenging. In this study, we synthesized cobalt molybdenum ruthenium oxide with porous, loosely-assembled nanoplate morphology. The CoMoRu0.25Ox/NF electrocatalyst exhibited the highest electrocatalytic activity, requiring overpotentials of 230 and 78 mV for the OER and HER, respectively, to attain a current density of 10 mA cm?2; moreover, its long-term stability was outstanding. The electrocatalyst required a cell voltage of only 1.51 V for overall water splitting in an alkaline medium, which was lower than that required by many CoMo-based catalysts.  相似文献   

16.
Interfacial charge redistribution induced by a strong built-in electric field can expertly optimize the adsorption energy of hydrogen and hydroxide for improving the catalytic activity. Herein, we develop a well-defined hierarchical NiFe2O4/NiFe layered double hydroxides (NFO/NiFe LDH) catalysts, exhibiting superior performance due to the strong interfacial electric field interaction between NiFe2O4 nanoparticle layers and NiFe LDH nanosheets. In 1 M KOH, NFO/NiFe LDH needs 251 mV and 130 to drive 50 and 10 mA cm?2 for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). Moreover, only 1.517 V cell voltage is needed to reach 10 mA cm?2 towards overall water splitting. Notably, under simulated industrial electrolysis conditions, NFO/NiFe LDH only needs 289 mV to drive 1000 mA cm?2. This work puts a deep insight into the role of the built-in electric field in transition metal-based catalysts for accelerating water splitting and scalable industrial electrolysis applications.  相似文献   

17.
The work undertaken involved the synthesis of mesoporous M-ferrites (M = Co, Ni) by facile PEG-assisted microemulsion method and exploration of their electrocatalytic potential for water splitting. The onset potential for oxygen evolution befalls at nearly 1.53 VRHE (η = 300 mV), which is 400–450 mV lesser than those reported for simple ferrites and iron oxides thin-film as electrocatalysts. These electrocatalysts exhibit the good electroactive zone having the lowest Tafel slope value, 68 mVdec−1, as compared to that reported for nickel and cobalt based materials. High TOF value is attributed to the superior catalytic activity of the catalysts. NiFe2O4 exhibits the turn over frequency (TOF) of 2.4 s−1 just at overpotential value of 0.42 VRHE with 1.2 μmol of the prepared sample used in electrochemical analysis. The long-term catalytic stability of Ni and Co-Ferrites spectacle a remarkable and stable current density of >15 mAcm−2 for oxygen evolution and maintained for several hours.  相似文献   

18.
The synthesis of cost-effective and high-performance electrocatalysts for water splitting is the main challenge in electrochemical hydrogen production. In this study, we adopted a high throughput method to prepare bi-metallic catalysts for oxygen/hydrogen evolution reactions (OER/HER). A series of Ni–Mo alloy electrocatalysts with tunable compositions were prepared by a simple co-sputtering method. Due to the synergistic effect between Ni and Mo, the intrinsic electrocatalytic activity of the Ni–Mo alloy electrocatalysts is improved, resulting in excellent HER and OER performances. The Ni90Mo10 electrocatalyst shows the best HER performance, with an extremely low overpotential of 58 mV at 10 mA cm?2, while the Ni40Mo60 electrocatalyst shows an overpotential of 258 mV at 10 mA cm?2 in OER. More significantly, the assembled Ni40Mo60//Ni90Mo10 electrolyzer only needs a cell voltage of 1.57 V to reach 10 mA cm?2 for overall water splitting.  相似文献   

19.
An ongoing challenge still lies in the exploration of proficient electrocatalysts from earth-abundant non-precious metals instead of noble metal-based catalysts for clean hydrogen energy through large-Scale electrochemical water splitting. However, developing a non-precious transition metals based, stable electrocatalyst for cathodic hydrogen evolution reaction (HER) and anodic oxygen evolution reaction (OER) is important challenge for modern energy conversion technology. In this report Vanadium doped bimetallic nickel-iron nanoarray, fabricated by carbon supported architecture through carbonization process for electrochemical water splitting. Three types of catalysts were prepared in different molar ratio of Ni/Fe. The electrocatalytic performance demonstrated that the catalyst with equal mole ratio (0.06:0.06) of Ni/Fe possess high catalytic activity for both OER and HER in alkaline and acidic medium. Besides, our findings revealed that the doping of vanadium could play a strong synergetic effect with Ni/Fe, which provide a small overpotential of 90 mV and 210 mV at 10 mA cm?2 for HER and OER respectively compared to the other two catalyst counterparts. Also, the catalyst with 1:1 (Ni/Fe) molar ratio showed a high current density of 208 mA cm?2 for HER at 0.5 M H2SO4 and 579 mA cm?2 for OER at 1 M KOH solution, the both current densities are much higher than the other two catalysts (different Ni/Fe ratio). In addition, the presented catalysts showed extremely good durability, reflecting in more than 20 h of consistent Chronoamprometry study at fixed overpotential η = 250 mV without any visible voltage elevation. Similarly, the (Ni/Fe) equal ratio catalyst showed better corrosion potential 0.209 V vs Ag/AgCl and lower current density 0.594 × 10?12 A cm?2 in high alkaline medium. The V-doping, MOF/GO surface defects are significantly increased the corrosion potential of the V-NixFey-MOF/GO electrocatalyst. Besides, the water electrolyzed products were analysed by gas chromatography to get clear insights on the formed H2 and O2 products.  相似文献   

20.
We designed and fabricated non-precious and highly efficient electrocatalysts of nickelmolybdenum/copper-nanosheets/nickel-foam composites (NiMo/Cu-NS/NF) by step electrodepositions, combining with chemical oxidation method. The catalysts were charaterized by means of SEM, XRD and XPS spectra. Their electrocatalytic activities were assessed by hydrogen evolution reactions (HER) over a wide pH range, where acidic, neutral and alkaline electrolytes were used, respectively. Benefiting from the unique midlayer Cu nanosheets (NS) architecture and optimum Mo–Ni composition at the surface layer which led to high electronic conductivity and large electrochemically active surface area (ECSA), the NiMo/Cu-NS/NF-2 catalyst displayed superior electrocatalytic activities with low overpotentials of η10 = 43, 86 and 89 mV in 0.5 M H2SO4, 1.0 M PBS and 1.0 M KOH electrolyte, respectively. Especially in the acidic condition, it exhibited the best electrocatalytic activity with smaller Tafel slope of 54 mV dec?1 and higher exchange current density of 1.93 mA cm?2.  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