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1.
In this paper, we present a solvothermal synthesis of iron phosphide electrocatalysts using a triphenylphosphine (TPP) precursor. The synthetic protocol generates Fe2P phase at 300 °C and FeP phase at 350 °C. To enhance the catalytic activities of obtained iron phosphide particles heat-treatments were carried out at elevated temperatures. Annealing at 500 °C under reductive atmosphere induced structural changes in the samples: (i) Fe2P provided a pure Fe3P phase (Fe3P−500 °C) and (ii) FeP transformed into a mixture of iron phosphide phases (Fe2P/FeP−500 °C). Pure Fe2P films was prepared under argon atmosphere at 450 °C (Fe2P−450 °C). The electrocatalytic activities of heat-treated Fe2P−450 °C, Fe3P−500 °C, and Fe2P/FeP−500 °C catalysts were studied for hydrogen evolution reaction (HER) in 0.5 M H2SO4. The HER activities of the iron phosphide catalyst were found to be phase dependent. The lowest electrode potential of 110 mV vs. a reversible hydrogen electrode (RHE) at 10 mA cm−2 was achieved with Fe2P/FeP−500 °C catalyst.  相似文献   

2.
The metal-free carbonaceous catalysts are one of the promising candidates for efficient electrocatalytic hydrogen production. Aiming at demonstrating the high electrocatalytic activity of the hydrogen evolution reaction (HER), we synthesized the biomass rice husk-derived corrugated graphene (RH-CG) nanosheets via the KOH activation. The 700 °C-activated RH-CG nanosheets exhibited the large specific surface area as well as the high electrical conductivity. When using the RH-CG nanosheets as a HER electrocatalyst in 0.5 M H2SO4, the excellent HER activities with a small overpotential (9 mV at 10 mA/cm2) and a small Tafel slope (31 mV/dec) were achieved. The results provide a new strategy for materializing the superb biomass-derived electrocatalyst for highly efficient hydrogen production.  相似文献   

3.
Developing an effective and low-cost bifunctional electrocatalyst for both OER and HER to achieve overall water splitting is remaining a challenge to meet the needs of sustainable development. Herein, an electroless plating method was employed to autogenous growth of ultrathin Ni–Fe2B nanosheet arrays on nickel foam (NF), in which the whole liquid phase reduction reaction took no more than 20 min and did not require any other treatments such as calcination. In 1.0 M KOH electrolyte, the resulted Ni–Fe2B ultrathin nanosheet displayed a low overpotential of 250 mV for OER and 115 mV for HER to deliver a current density of 10 mA cm?2, and both OER and HER activities remained stable after 26 h stability testing. Further, the couple electrodes composed of Ni–Fe2B could afford a current density of 10 mA cm?2 towards overall water splitting at a cell voltage of 1.64 V in 1.0 M KOH and along with excellent stability for 26 h. The outstanding electrocatalytic activities can be attributed to the synergistic effect of electron-coupling across Ni and Fe atoms and active sites exposed by large surface area. The effective combination of low cost and high electrocatalytic activity brings about a promising prospect for Ni–Fe2B nanosheet arrays in the field of overall water splitting.  相似文献   

4.
Exploring low-cost, highly efficient, and sustainable non-precious electrocatalysts for electrolytic H2 generation is driving research for the sustainable green urban development. Herein, we present a simple synthetic approach, through a two-step process, to prepare the bifunctional electrode of Co3O4–C@FeMoP hybrid micro rods/nanosheets anchored on nickel foam (NF), in which the Co3O4–C microrods grown on NF surface are decorated by FeMoP nanosheet layers, which is directly grown through a simple hydrothermal followed by post-phosphorization processes. The obtained hybrid hierarchical Co3O4–C@FeMoP/NF shows a significant enhancement in the electrocatalytic activities of oxygen/hydrogen evolution reactions (OER/HER) in comparison to the individual Co3O4–C and FeMoP nanostructures, thanks to more heterointerface active sites provided by FeMoP nanostructures with three-dimensional (3-D) layered architectures. The Co3O4–C@FeMoP/NF catalyst exhibits a relatively small overpotential of 200 mV vs. RHE for OER to achieve 20 mA/cm2 and 123 mV vs RHE at 10 mA/cm2 for HER along with excellent durability in alkaline electrolytes. We demonstrate the bifunctional electrocatalytic electrode as the electrolyzer for the generation of H2 via water splitting at small applied voltage of 1.61 V to achieve 10 mA/cm2 and good stability for 24-h continuous running.  相似文献   

5.
Binder-free NiFe-based electrocatalyst with aligned pore channels has been prepared by freeze casting and served as a bifunctional catalytic electrode for oxygen and hydrogen evolution reaction (OER and HER). The synergistic effects between Ni and Fe result in the high electrocatalytic performance of porous NiFe electrodes. In 1.0 M KOH, porous Ni7Fe3 attains 100 mA cm−2 at an overpotential of 388 mV with a Tafel slope of 35.8 mV dec−1 for OER, and porous Ni9Fe1 exhibits a low overpotential of 347 mV at 100 mA cm−2 with a Tafel slope of 121.0 mV dec−1 for HER. The Ni9Fe1//Ni9Fe1 requires a low cell voltage of 1.69 V to deliver 10 mA cm−2 current density for overall water splitting. The excellent durability at a high current density of porous NiFe electrodes has been confirmed during OER, HER and overall water splitting. The fine electrocatalytic performances of the porous NiFe-based electrodes owing to the three-dimensionally well-connected scaffolds, aligned pore channels, and bimetallic synergy, offering excellent charge/ion transfer efficiency and sizeable active surface area. Freeze casting can be applied to design and synthesize various three-dimensionally porous non-precious metal-based electrocatalysts with controllable multiphase for energy conversion and storage.  相似文献   

6.
Constructing highly efficient nonprecious electrocatalysts for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is essential to improve the efficiency of overall water splitting, but still remains lots of obstacles. Herein, a novel 3D peony flower-like electrocatalyst was synthesized by employing Mo–Ni2S3/NF nanorod arrays as scaffolds to in situ growth ultrathin NiFe LDH nanosheets (Mo-Ni2S3@NiFe LDH). As expected, the novel peony flower-like Mo–Ni2S3@NiFe LDH displays superior electrocatalytic activity and stability for both OER and HER in alkaline media. Low overpotentials of only 228 mV and 109 mV are required to achieve the current densities of 50 mA cm?2 and 10 mA cm?2 for OER and HER, respectively. Additionally, the material remarkably accelerates water splitting with a low voltage of 1.54 V at 10 mA cm?2, which outperforms most transition metal electrodes. The outstanding electrocatalytic activity benefits from the following these features: 3D peony flower-like structure with rough surface provides more accessible active sites; superhydrophilic surfaces lead to the tight affinity between electrode with electrolyte; metallic Ni substrate and highly conductive Mo–Ni2S3 nanorods scaffold together with offer fast electron transfer; the nanorod arrays and porous Ni foam accelerate gas bubble release and ions transmission; the strong interfacial effect between Mo-doped Ni3S2 and NiFe LDH shortens transport pathway, which are benefit for electrocatalytic performance enhancement. This work paves a new avenue for construction and fabrication the 3D porous structure to boost the intrinsic catalytic activities for energy conversion and storage applications.  相似文献   

7.
Developing a bi-functional material which can meet both electrochemical water splitting and supercapacitors (SCs) is a hot spot in current research. In this study, hierarchical zigzag-like phosphorus doped CuCo2O4 nanosheets based 3D electrode materials were successfully synthesized via a hydrothermal method and followed by thermal treatment. Since the unique morphology of 2D nanosheets with zigzag-like edges could provide more reactive sites, which is not only conducive to the hydrogen evolution reaction (HER), but also conducive to the electrochemical energy storage. Meanwhile, the doping of phosphorus was adopted to improve the conductivity, which would further enhance the electrochemical properties of CuCo2O4. Thereafter, its performance for HER and SCs in 1 M KOH were systematically investigated. As an electrode for HER, it only required a low overpotential of 152 mV to reach 10 mA cm?2 with a Tafel slope of 115.7 mV dec?1. Furthermore, I-t test result showed an excellent stability. As an electrode for SCs, it exhibited a high specific capacity of 896.9C g?1 at 1 A g?1 in three-electrode system. All in all, the obtained hierarchical zigzag-like phosphorus doped CuCo2O4 nanosheets provided a feasible route for the design of bi-functional electrode materials both for energy conversion and storage.  相似文献   

8.
Tailoring surface composition and structures of catalysts affects their catalytic performance in hydrogen evolution reaction owing to the geometric and electronic effects. Herein, Ru nanoparticles embedded in 2D N-doped carbon nanosheets decorated with 2D Fe3O4–Fe3C heterostructures (Ru/Fe3O4–Fe3C/NC) are fabricated via pyrolysis of the mixture containing 2D-Fe2O3 nanosheets, dopamine hydrochloride, RuCl3·xH2O, and melamine. Interestingly, the good hydrogen evolution behavior is achieved on Ru/Fe3O4–Fe3C/NC with the high reactivity and stability. Ru/Fe3O4–Fe3C/NC offers an overpotential of 141 mV to realize the current density of 10 mA/cm2 in 0.5 mol/L (M) H2SO4 electrolyte. As for 1 M KOH, Ru/Fe3O4–Fe3C/NC promotes hydrogen evolution reactivity with 148 mV to achieve 10 mA/cm2. The current density slightly degrades after continuous I-t tests, verifying the good stability for Ru/Fe3O4–Fe3C/NC. The high reactivity might stem from high dispersion of Ru nanoparticles, enhanced conductivity due to doping N into carbon nanosheets, and heterointerfaces between Fe–O and Fe–C.  相似文献   

9.
Fe2O3–TiO2 composite incorporated NiP coating is a known promising catalytic coating for electrocatalytic Hydrogen Evolution Reaction (HER). It is explored in the present study that the activity of the coating can be enhanced by incorporation of rGO. The Fe2O3–TiO2/rGO, electrocatalyst is synthesized by a facile hydrothermal method. Various compositions of the Fe2O3–TiO2/rGO incorporated NiP coatings on mild steel substrate are developed by a chemical reduction method. The developed Fe2O3–TiO2/rGO composite coating exhibits effective hydrogen evolution reaction activity with a Tafel slope of 98 mV dec−1 and a low overpotential of 96 mV at a current density of 10 mA cm−2. The hydrogen evolution reaction mechanism comprises of Volmer (adsorption of Hydrogen atom) followed by Heyrovskii (reduction to H2). The enhanced catalytic activity by the incorporation of rGO into the coating is due to three dimensional projections of nano Fe2O3–TiO2 on the folded surface of rGO. It effectively enhances the electrochemically active surface area of the coated electrode. The electrode is highly stable during alkaline HER. These results reveal that Fe2O3–TiO2/rGO can be treated as an effective electrocatalyst during HER from alkaline solutions. The conclusions pave the way for exploration of new similar catalysts for other applications.  相似文献   

10.
Designing and synthesizing high-activity, durable, and low-cost catalysts for the electrochemically transformation of water to hydrogen are vitally important to future energy systems. Herein, a simple but effective strategy for manganese-metal-heteroatom doping is adopted to intrinsically elevate the electrocatalytic activities of SnS2 nanosheets by a facile two steps hydrothermal-sulfurization approach. Electrocatalytic hydrogen evolution (HER) performance of Mn–SnS2 nanosheets grown on 3D nickel foam (Mn–SnS2/NF) is efficiently optimized since the dopants and defects endow the Mn–SnS2/NF vast active sites. An overpotential as low as 71 mV is required to drive a current density of 10 mA/cm2 with a low Tafel slope of 72 mV dec?1 in alkaline environment (1 M KOH). In addition, the Mn–SnS2/NF exhibits prominent stability in 1 M KOH electrolyte, which is an indispensable index for the potential HER electrocatalysts. The present work demonstrates that the heteroatom manganese doping strategy renders a meaningful route for synthesizing cost-efficient HER electrocatalysts in alkaline condition.  相似文献   

11.
Molybdenum sulfide (MoS2) as a graphene-like sheet material has attracted wide attention owing to the potential for hydrogen evolution reaction (HER). However, the large-scale application of MoS2 is still difficult due to the inherent poor conductivity and insufficient active edge sites. Herein, we develop a simple method to grow P-doped MoS2 nanosheets on carbon cloth for high efficiency HER. The 2D carbon cloth can prevent the stacking of MoS2 nanosheets and improve the conductivity with the doping of P atoms. As a result, the P–MoS2/CC-300 shows the excellent electrocatalytic activity with an overpotential of 81 mV at 10 mA cm?2 and the lower Tafel slope of 98 mV/dec. Furthermore, it also shows the good electrocatalytic durability for 15 h. This work provides an opportunity for the design of excellent and robust MoS2-based catalyst via structural engineering and doping method.  相似文献   

12.
It is of great significance to develop a highly active, durable and inexpensive bifunctional electrocatalyst for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Herein, we report a tungsten-doped nickel phosphide nanosheets based on carbon cloth (W–Ni2P NS/CC) as an efficient bifunctional catalyst through simple hydrothermal and phosphorization for overall water splitting in 1 M KOH. The W–Ni2P NS/CC exhibits excellent electrochemical performance with low overpotentials for HER (η10 = 71 mV, η50 = 160 mV) and OER (η20 = 307 mV, η50 = 382 mV) in 1 M KOH, as well as superior long-term stability. Moreover, W–Ni2P NS/CC as a bifunctional catalyst reveals remarkable activity with a low voltage of 1.55 V to reach a current density of 20 mA cm−2. This work provides a viable bifunctional catalyst for the overall water splitting.  相似文献   

13.
Water splitting is an appealing way of producing hydrogen fuel, which requires efficient and affordable electrode materials to make the overall process viable. In the last couple years, abundant transition metals (and their compounds and hybrids) attracted ever-growing attention as the alternatives of noble metals. Particularly the layered transition metal dichalcogenide (TMDs) are interesting with their stability and promising electrocatalytic performance for hydrogen evolution reaction (HER). However, the neat TMDs are often poor in terms of the abundance of catalytically active sites and electrical conductivity, which limit their application potential significantly. Herein, as a proof-of-concept, we report on the design of a high-performance electrocatalyst system formed by the decoration of ultrasmall molybdenum sulfide (MoS2) nanosheets on carbon nanotubes (CNTs). The ultrasmall MoS2 nanosheets provide distorted lattice, confined size and rich defects, which endows the resulting electrocatalysts (MoS2/CNT) with abundant active sites. The CNTs, on the other hand, serve as the conductive net for ensuring electrocatalytic performance. As a result, the hybrid electrocatalyst exhibits excellent electrocatalytic performance for HER, achieving a large current density of 100 mA cm−2 at overpotential of only 281 mV and a small Tafel slope of 43.6 mV dec−1 along with a decent stability. Our results are of high interest for electrocatalyst technologists as well as hydrogen fuel researchers.  相似文献   

14.
Perovskite-type metal oxides have emerged as important materials in renewable energy because the high electrocatalytic performance for oxygen evolution reaction (OER). Hence, we perform a study on the electrocatalytic properties of LaNi1-xFexO3 (x = 0.0, 0.3, 0.6, and 0.9 mol%) for OER, mainly analyzing the influence provoked by the incorporation of Fe3+ in the lattice as well as the use of pyrolytic graphite sheet (PGS) as a potential substrate for electrocatalysis. These perovskites were synthesized by the co-precipitation method. The thin film electrodes were prepared depositing the obtained powders on PGS substrates via drop-casting. Depending on the Fe3+ level, structural changes and morphological modifications were identified for these materials. The highest electrocatalytic activity for OER was detected for LaNi0.4Fe0.6O3. Besides the low charge transfer resistance, LaNi0.4Fe0.6O3 exhibited a lower overpotential (439 mV) and a smaller Tafel slope (52 mV dec−1) than the LaNiO3 (465 mV and 76 mV dec−1).  相似文献   

15.
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   

16.
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   

17.
Developing an efficient and stable electrocatalyst for hydrogen evolution reaction (HER) remains critically signi?cance for renewable hydrogen production. Herein, a facile electrochemical reduction method was proposed to fabricate Ru nanoparticles (NPs) evenly anchored on Ti3C2Tx nanosheets (Ti3C2Tx-NS) electrocatalyst (Ru@Ti3C2Tx-NS). Interestingly, owing to the interaction between Ru NPs and Ti3C2Tx-NS, the resultant Ru@Ti3C2Tx-NS electrocatalyst performed a Pt-like electrocatalytic property for HER under the acidic solution with an ultra-low overpotential of 46.75 mV to reach ?10 mA/cm2, a small Tafel slope of 30.6 mV/dec, and long-term stability. Simultaneously, the Ru@Ti3C2Tx-NS also displayed splendid HER electrocatalytic performance in the basic condition. Furthermore, Ru@Ti3C2Tx-NS showed a lower value of Gibbs free energy for HER (?0.21 eV) than either pure Ru or Ti3C2Tx-NS from the theoretical calculation results. It is expected that such a promising approach would be extended to design and fabricate other noble metal NPs anchored MXene nanosheets for HER application.  相似文献   

18.
As a clean, high calorific value and renewable energy, hydrogen is considered to be an ideal green energy to replace traditional fossil energy. Among various methods for preparing hydrogen, electrolytic water hydrogen evolution has attracted the attention of researchers because of its high efficiency, easy separation of products and green and pollution-free advantages. In this experiment, starting from the porous foam iron, Fe2O3 nanosheets are obtained by anodic oxidation, and then the material is phosphated by in-situ phosphating in a tubular furnace to obtain FeP nanosheets. Finally, the Ru dopants are deposited into the lattice of FeP nanosheets by electrodeposition to obtain the Ru-doped FeP nanosheets. Through the characterization of morphology and the test of electrocatalytic hydrogen evolution performance, the Ru-doped FeP nanosheets show ultra-high electrochemical hydrogen evolution activity and have regular nanosheets array structure.  相似文献   

19.
It is extremely necessary to develop highly efficient and low-cost non-noble metal electrocatalysts for hydrogen evolution reaction (HER) under a pH-universal condition in the realm of sustainable energy. Herein, we have successfully prepared phosphorus doped Fe3O4 nanoflowers on three-dimensional porous graphene (denoted as P–Fe3O4@3DG) via a simple hydrothermal and low-temperature phosphating reaction. The P–Fe3O4@3DG hybrid composite not only demonstrates superior performance for HER in 1.0 M KOH with low overpotential (123 mV at 10 mA/cm2), small Tafel slope (65 mV/dec), and outstanding durability exceeding 50 h, but also exhibits satisfying performances under neutral and acidic medium as well. The 3D graphene foam with large porosity, high conductivity, and robust skeleton conduces to more active sites, and faster electron and ion transportation. The phosphorus dopant provides low Gibbs free energy and ability of binging H+. The synergistic effect of 3DG substrate and P–Fe3O4 active material both accelerates the catalytic activity of Fe-based hybrid composite for HER.  相似文献   

20.
Co3S4 nanosheets on Ni foam (NS/NF) were prepared by sulfurization for various time after calcination of electrodeposited Co(OH)2. In our FE-SEM images, we observed that Co3S4 NS was vertically, or obliquely, deposited on the Ni foam. As a result, the structure contained more active sites, and active sites were highly accessible to the electrolyte for the hydrogen evolution reaction (HER). Furthermore, results of XPS and XRD analysis confirmed S-conversion from Co3O4 to Co3S4 during sulfurization. 3-Co3S4 NS/NF with sulfurization for 3 h exhibited the highest sulfur content, while Co3S4 began to desulfurize to Co9S8 after sulfurization for 4 h. The 3-Co3S4 NS/NF electrocatalyst showed a lowest overpotential of 93 mV at −10 mA/cm2, with a Tafel slope of −55.1 mV/dec in N2-purged 1 M KOH. Also, the single cell anion exchange membrane water electrolyzer (AEMWE) showed a high current density of 431 mA/cm2 with cell voltage 2.0 Vcell at 40–45 °C.  相似文献   

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