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1.
The development of a distinguished and high-performance catalyst for H2 and O2 generation is a rational strategy for producing hydrogen fuel via electrochemical water splitting. Herein, a flower-like Co9S8@MoS2 heterostructure with effective bifunctional activity was achieved using a one-pot approach via the hydrothermal treatment of metal-coordinated species followed by pyrolysis under an N2 atmosphere. The heterostructures exhibited a 3D interconnected network with a large electrochemical active surface area and a junctional complex with hydrogen evolution reaction (HER) catalytic activity of MoS2 and oxygen evolution reaction (OER) catalytic activity of Co9S8, exhibiting low overpotentials of 295 and 103 mV for OER and HER at 10 mA cm−2 current density, respectively. Additionally, the catalyst-assembled electrolyser provided favourable catalytic activity and strong durability for overall water splitting in 1 M KOH electrolyte. The results of the study highlight the importance of structural engineering for the design and preparation of cost-effective and efficient bifunctional electrocatalysts.

A flower-like Co9S8@MoS2 heterostructure was prepared as efficient bifunctional electrocatalyst for overall water splitting by a sample one-pot approach.  相似文献   

2.
Correction for ‘Microflower-like Co9S8@MoS2 heterostructure as an efficient bifunctional catalyst for overall water splitting’ by Chaohai Pang et al., RSC Adv., 2022, 12, 22931–22938, https://doi.org/10.1039/D2RA04086G.

The authors regret that an incorrect grant number was shown in the acknowledgements section of the published article. The corrected section should read:This work was financially supported by the Central Public-interest Scientific Institution Basal Research Fund (No.1630082022008). China Agriculture Research System of MOF and MARA (CARS-31). Key Laboratory of Tropical Fruits and Vegetables Quality and Safety for State Market Regulation (Grant no. ZX-2022002). Additional support was provided by the Foundation from Chemistry and Chemical Engineering Guangdong Laboratory (Grant No. 2111016) and the Basic and Applied Basic Research Foundation of Guangdong Province (Grant no. 2021A1515110111).The Royal Society of Chemistry apologises for these errors and any consequent inconvenience to authors and readers.  相似文献   

3.
Overall water splitting and CO2 reduction are two very important reactions from the environmental viewpoint. The former produces hydrogen as a clean fuel and the latter decreases the amount of CO2 emissions and thus reduces greenhouse effects. Here, we prepare two types of copper molybdate, CuMoO4 and Cu3Mo2O9, and electrochemically investigate them for water splitting and CO2 reduction. Our findings show that Cu3Mo2O9 is a better electrocatalyst for full water splitting compared to CuMoO4. It provides overpotentials, which are smaller than the overpotentials of CuMoO4 by around 0.14 V at a current density of 1 mA cm−2 and 0.10 V at −0.4 mA cm−2, for water oxidation and hydrogen evolution reactions, respectively. However, CuMoO4 adsorbs CO2 and the reduced intermediates/products more strongly than Cu3Mo2O9. Such different behaviors of these electrocatalysts can be attributed to their different unit cells.

Comparing overall water splitting on the surface two types of copper molybdate.  相似文献   

4.
In this study, we constructed a highly effective, low-cost, non-noble-metal-based electrocatalyst to replace Pt catalysts, with a CoS@SNC catalyst being successfully synthesized. The obtained nanocatalyst was characterized via scanning electron microscopy, energy-dispersive X-ray spectroscopy, transmission electron microscopy, powder X-ray diffraction studies, and X-ray photoelectron spectroscopy. Herein, an initially prepared N-containing Co MOF formed flower-like particles, which were obtained via a solvothermal method; further it was used for a sulfuration process as a template to achieve an S,N (heteroatom)-doped carbon electrocatalyst with embedded CoS (CoS@SNC). The synthesized flower-like CoS@SNC electrocatalyst derived from a novel MOF showed a uniform distribution of Co, S, N, and C at the molecular level in the MOF and it was rich in active sites, facilitating enhanced electrocatalytic performance. During the HER and OER in 0.1 M KOH solution, to reach a current density of 10 mA cm−2, lower overpotentials of −65 mV and 265 mV, respectively, were required and Tafel slopes of 47 mV dec−1 and 59.8 mV dec−1, respectively, were seen. In addition, due to a synergistic effect between CoS and the S,N-doped carbon matrix, long-term durability and stability were obtained. This facile synthetic strategy, which is also environmentally favorable, produces a promising bifunctional electrocatalyst.

In this study, we constructed a highly effective, low-cost, non-noble-metal-based electrocatalyst to replace Pt catalysts, with a CoS@SNC catalyst being successfully synthesized.  相似文献   

5.
The development of bifunctional electrocatalysts based on highly efficient non-noble metals is pivotal for overall water splitting. Here, a composite electrode of Co3O4@CoWP is synthesized, where an ultrathin layer composed of Co3O4 nanoparticles is grown on CoWP nanowires supported on a carbon cloth (CC). The Co3O4@CoWP/CC electrode exhibits excellent electrocatalytic activity and improved kinetics towards both the oxygen and hydrogen evolution reactions (OER and HER). The Co3O4@CoWP/CC electrode achieves a current density of 10 mA cm−2 at a low overpotential of 269 mV for the OER and −10 mA cm−2 at 118 mV for the HER in 1.0 M KOH solution. The voltage applied to a two-electrode water electrolyzer for overall water splitting, while employing the Co3O4@CoWP/CC electrode as both an anode and a cathode, in order to reach a current density of 10 mA cm−2, is 1.61 V, which is better than that for the majority of reported non-noble electrocatalysts. Moreover, the Co3O4@CoWP/CC electrode exhibits good stability over 24 h with slight attenuation. The electrode benefits from the enhanced adsorption of oxygen intermediates on Co3O4 during the OER, the increased ability for water dissociation and the optimized H adsorption/desorption ability of CoWP nanowires during the HER. This study provides a feasible approach for cost-effective and high-performance non-noble metal bifunctional catalysts for overall water electrolysis.

A hierarchical 3D self-supporting CoWP nanowire array shelled with an ultrathin Co3O4 nanolayer on carbon cloth (Co3O4@CoWP/CC) exhibits superior overall water electrolysis capability.  相似文献   

6.
Design and synthesis of electrocatalysts with high activity and low cost is an important challenge for water splitting. We report a rapid and facile synthetic route to obtain IrxNi clusters via polyol reduction. The IrxNi clusters show excellent activity for the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in acidic electrolytes. The optimized Ir2Ni/C clusters exhibit an electrochemical active area of 18.27 mF cm−2, with the overpotential of OER being 292 mV and HER being 30 mV at 10 mA cm−2, respectively. In addition, the Ir2Ni/C used as the cathode and anode for the H-type hydrolysis tank only needs 1.597 V cell voltages. The excellent electrocatalytic performance is mainly attributed to the synergistic effect between the metals and the ultra-fine particle size. This study provides a novel strategy that has a broad application for water splitting.

A method of preparing IrxNi/C clusters by polyol reduction using a XC-72R support was proposed. Due to the 2 nm size of the catalyst particles, more active sites are exposed. This is a promising route for the development of efficient water splitting electrocatalysts.  相似文献   

7.
The search for efficient and low-cost electrocatalysts for the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER) is of utmost importance for the production of hydrogen and oxygen via water splitting. In this work, the catalytic performance of the OER and HER on transition metal doped boron nanotubes (BNTs) was investigated using density functional theory. It was found that the doped transition metal atoms determine the catalytic activity of the BNTs. Rhodium-doped BNTs exhibited excellent OER activity, while cobalt-doped BNTs displayed great catalytic activity toward the HER. Volcano relationships were found between the catalytic activity and the adsorption strength of reaction intermediates. Rhodium- and cobalt-doped BNTs exhibited great OER and HER catalytic activity due to the favorable adsorption strength of reaction intermediates. This work sheds light on the design of novel electrocatalysts for water splitting and provides helpful guidelines for the future development of advanced electrocatalysts.

Rhodium-doped BNTs demonstrated excellent OER activity, while cobalt-doped BNTs exhibited the best catalytic activity toward the HER among 12 different transition metal-doped BNTs.  相似文献   

8.
The iron–nitrogen–carbon (FeNC) catalyst, as a highly active and stable non-precious metal catalyst, has emerged as one of the most promising alternatives to replace the platinum catalyst for oxygen reduction reaction (ORR). Herein, a novel FeNC/MXene hybrid nanosheet was, for the first time, explored via pyrolysis of an iron–ligand complex and MXene nanosheets. The structure and morphology characterizations reveal that a thin and rugged FeNC coating was closely attached on the surface of MXene, forming a hybrid nanosheet structure with an excellent conductive substrate and many electrocatalytic active sites on the substrate. The electrochemical measurements disclose that the FeNC/MXene hybrid nanosheet exhibited a remarkable electrocatalytic performance, with a 25 mV higher half-wave potential (0.814 V versus RHE) than the Pt/C counterpart. More importantly, this hybrid presented a superb durability, with only 2.6% decay after a 20 000 s continuous test, much better than the 15.8% degradation for Pt/C. This work not only demonstrates the promising performance of the FeNC/MXene hybrid nanosheet for ORR, but more importantly provides new insight into the rational design of non-noble-metal catalysts using an MXene support.

A novel FeNC/MXene hybrid nanosheet with a rugged FeNC coating closely attached on the MXene surface was explored, which exhibited remarkable electrocatalytic activity with a superb durability (only 2.6% decay after a 20 000 s continuous test).  相似文献   

9.
Designing electrode structures with high activity is very significant for energy conversion systems. However, single electrode materials often exhibit poor electronic transportation. To address this issue, we prepared P-Fe2O3 nanowire arrays through a convenient hydrothermal and phosphation method. The as-obtained electrode materials exhibited excellent electrocatalytic performance, which could be attributed to the P element decoration improving the reaction active sites. The as-obtained P-Fe2O3-0.45 nanowire arrays exhibited excellent OER activity with a low overpotential of 270 mV at 10 mA cm−2 (72.1 mV dec−1), excellent HER performance with a low overpotential of 126.4 mV at −10 mA cm−2, a small Tafel slope of 72.5 mV dec−1 and long durability. At the same time, the P-Fe2O3-0.45 nanowire arrays possessed a low cell voltage of 1.56 V at 10 mA cm−2.

Designing electrode structures with high activity is very significant for energy conversion systems.  相似文献   

10.
CuO has been considered a promising candidate for photoelectrochemical water splitting electrodes owing to its suitable bandgap, favorable band alignments, and earth-abundant nature. In this paper, a novel gas-phase cation exchange method was developed to synthesize CuO nanorod arrays by using ZnO nanorod arrays as the template. ZnO nanorods were fully converted to CuO nanorods with aspect ratios of 10–20 at the temperature range from 350 to 600 °C. The as-synthesized CuO nanorods exhibit a photocurrent as high as 2.42 mA cm−2 at 0 V vs. RHE (reversible hydrogen electrode) under 1.5 AM solar irradiation, demonstrating the potential as the photoelectrode for efficient photoelectrochemical water splitting. Our method provides a new approach for the rational fabrication of high-performance CuO-based nanodevices.

CuO nanorod arrays were synthesized by a novel gas-phase cation exchange method using ZnO nanorod arrays as the template, demonstrating promising photoelectrochemical water splitting performance.  相似文献   

11.
The utilization of solar energy in photoelectrochemical water splitting is a popular approach to store solar energy and minimize the dependence on fossil fuels. Herein, defected ZnWO4-decorated WO3 nanorod arrays with type II heterojunction structures were synthesized via a two-step solvothermal method. By controlling the amount of Zn precursor, WO3 nanorods were decorated in situ with tunable amounts of ZnWO4 nanoparticles. Characterization confirmed the presence of abundant W5+ species in the defected ZnWO4-decorated WO3 samples, leading to enhanced light absorption and charge-separation efficiency. Therefore, the decorated WO3 nanorod arrays show much higher photoelectrochemical (PEC) activity than pure WO3 nanorod arrays. Specifically, the sample with optimal ZnWO4 decoration and surface defects exhibits a current density of 1.87 mA cm−2 in water splitting at 1.23 V vs. RHE under 1 sun irradiation (almost 2.36 times higher than that of pure WO3), a high incident photon-to-current efficiency of nearly 40% at 350 nm, and a relatively high photostability. However, the decoration of WO3 with too much ZnWO4 blocks the light absorption of WO3, inhibiting the PEC performance, even when many defects are present. This work provides a promising approach to rationally construct defected heterojunctions as highly active PEC anodes for practical applications.

A strategy based on a solvothermal method was developed to construct defected ZnWO4-decorated WO3 photoanodes for efficient photoelectrochemical water splitting.  相似文献   

12.
A g-C3N4/CuO nanostructure featuring improved photoelectrochemical properties was successfully prepared using a facile and cost-effective method involving electrodeposition and thermal oxidation. The improved photoelectrochemical properties were mainly ascribed to the increased surface area and improved charge transportation of the g-C3N4/CuO photocathode. This photocathode can be used in novel strategies for resolving problems associated with low-efficiency CuO photocathodes.

A g-C3N4/CuO nanostructure featuring improved photoelectrochemical properties was successfully prepared using a facile and cost-effective method involving electrodeposition and thermal oxidation.  相似文献   

13.
The morphology of nano-arrays plays an important role in their applications for catalysis, energy, environment. However, the morphology modulation of nano-arrays generally involves complex optimization of synthetic conditions including surfactants, pH, and solvent. In this work, we synthesize a NiMoO4·H2O nano-array by a simple hydrothermal method under mild conditions (pH = 6.47, aqueous solution, and without the aid of surfactants). The morphology modulation of the NiMoO4·H2O nano-array is realized by simply changing the hydrothermal temperature. When the hydrothermal temperature below 150 °C, a NiMoO4·H2O nanorod array is obtained. While the hydrothermal temperature is as high as 180 °C, the array on Ni foam is nanosheet instead of nanorod. The NiMoO4·H2O nanorod array synthesized at 150 °C shows a superior water splitting activity compared to the NiMoO4·H2O nanosheet array, affording a large current density of 10 mA cm−2 at an overpotential of <240 and 200 mV toward oxygen evolution reaction and hydrogen evolution reaction, respectively. Furthermore, the electrolyzer using NiMoO4·H2O nanorod array as both anode and cathode electrodes for catalyzing overall water splitting exhibits great performance, obtaining a current density of 10 mA cm−2 at 1.67 V, comparable to the integration of commercial noble-metal Pt/C and IrO2 electrodes.

We realize the modulation of nanoarray morphology from nanorod to nanosheet and improve the catalytic activity for water splitting by simply changing the hydrothermal temperature.  相似文献   

14.
The scalable fabrication of flexible membranes for efficient oil/water separation is in high demand but still significantly underdeveloped. Here, we present a flexible membrane using Ti3C2Tx (MXene) as the functional layer on conventional print paper as the substrate. With a simple coating process using MXene ink, we developed a highly hydrophilic and oleophobic membrane with an underwater oil contact angle of 137°. Such a simple membrane shows outstanding flexibility and robustness, and demonstrates a facile approach for membrane scale-up using MXene ink on low-cost print paper. The membrane shows high separation efficiency for oil/water emulsions, of over 99%, and a high water permeation flux of over 450 L per m2 per h per bar. We demonstrate the excellent anti-fouling property of this membrane by cleaning the membranes without chemicals. These low-cost, highly efficient, anti-fouling membranes can provide new opportunities for industrial oil/water separation applications.

A highly hydrophilic and oleophobic membrane based on Ti3C2Tx (MXene) coated paper demonstrated high separation efficiency for oil/water emulsions with excellent antifouling properties.  相似文献   

15.
In this work, several commonly used conductive substrates as electrocatalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) under alkaline conditions were studied, including nickel foam (Ni foam), copper foam (Cu foam), nickel mesh (Ni mesh) and stainless steel mesh (SS mesh). Ni foam and SS mesh are demonstrated as high-performance and stable electrocatalysts for HER and OER, respectively. For HER, Ni foam exhibited an overpotential of 0.217 V at a current density of 10 mA cm−2 with a Tafel slope of 130 mV dec−1, which were larger than that of the commercial Pt/C catalyst, but smaller than that of the other conductive substrates. Meanwhile, the SS mesh showed the best electrocatalytic performance for OER with an overpotential of 0.277 V at a current density of 10 mA cm−2 and a Tafel slope of 51 mV dec−1. Its electrocatalytic performance not only exceeded those of the other conductive substrates but also the commercial RuO2 catalyst. Moreover, both Ni foam and SS mesh exhibited high stability during HER and OER, respectively. Furthermore, in the two-electrode system with Ni foam used as the cathode and SS mesh used as the anode, they enable a current density of 10 mA cm−2 at a small cell voltage of 1.74 V. This value is comparable to or exceeding the values of previously reported electrocatalysts for overall water splitting. In addition, NiO on the surface of Ni foam may be the real active species for HER, NiO and FeOx on the surface of SS mesh may be the active species for OER. The abundant and commercial availability, long-term stability and low-cost property of nickel foam and stainless steel mesh enable their large-scale practical application in water splitting.

Efficient electrocatalytic overall water splitting is achieved with commercially-available and low-cost nickel foam and stainless steel mesh as cathode and anode electrodes.  相似文献   

16.
A cross-linked sulfonated polyether ether ketone (C-SPEEK) was incorporated with MXene/potassium titanate nanowire (MKT-NW) as a filler and applied as a proton exchange membrane for photocatalytic water splitting. The prepared hybrid composite PEM had proton conductivity of 0.0097 S cm−1 at room temperature with an ion exchange capacity of 1.88 meq g−1. The hybrid composite proton exchange membrane is a reactive membrane which was able to generate hydrogen gas under UV light irradiation. The efficiency of hydrogen gas production was 0.185066 μmol within 5 h for 12% wt of MKT-NW loading. The results indicated that the MKT-NW/C-SPEEK membrane is a promising candidate for ion exchange with hydrogen gas evolution in photocatalytic water splitting and could be applied as a renewable source of energy to use in various fields of applications.

A cross-linked sulfonated polyether ether ketone (C-SPEEK) was incorporated with MXene/potassium titanate nanowire (MKT-NW) as a filler and applied as a proton exchange membrane for photocatalytic water splitting.  相似文献   

17.
Exploring low-cost and highly efficient non-noble bifunctional electrocatalysts with high performances for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is essential for large-scale sustainable energy systems. Herein, the Ni–Co–O–C–P hollow tetragonal microtubes grown on 3D Ni foam (Ni–Co–O–C–P/NF) was synthesized via a one-step solvothermal method and followed by a simple carbon coating and in situ phosphorization treatment. Benefiting from the unique open and hierarchical nano-architectures, the as prepared Ni–Co–O–C–P/NF presents a high activity and durability for both the HER and OER in alkaline media. The overall-water-splitting reaction requires a low cell voltage (1.54 V @ 10 mA cm−2) in 1 M KOH when Ni–Co–O–C–P/NF is used as both the anode and cathode. The highly flexible structure can provide a large amount of exposed active sites and shorten the mass transport distance. Furthermore, bimetallic phosphides also favor the electrocatalysis due to the higher electronic conductivity and the synergetic effect. This work demonstrated a promising bifunctional electrocatalyst for water electrolysis in alkaline media with potential in future applications.

Herein, the Ni–Co–O–C–P hollow tetragonal microtubes grown on 3D Ni foam (Ni–Co–O–C–P/NF) was delicately designed and synthesized, which presented a high activity and durability for electrocatalytic overall-water-splitting in alkaline media.  相似文献   

18.
We use SiO2 as a template and dopamine as a carbon source to synthesize a hollow C shell, and we load Co and Ru nanoparticles onto it to obtain a Co–Ru@C shell composite. The diameter and thickness of the C shell are 100 nm and 5–10 nm, respectively, and numerous holes of different sizes exist on the C shell. Meanwhile, numerous C shells stack together to form macropores, thereby forming a hierarchical porous structure in the material. Brunauer–Emmett–Teller surface area analysis reveals that the specific surface area and pore volume of the Co–Ru@C shell are 631.57 m2 g−1 and 2.20 cc g−1, respectively, which can result in many three-phase interfaces and provide more space for the deposition of discharge products. Compared with Co@C shell and C shell electrodes, the obtained Co–Ru@C shell-based electrodes exhibit the highest discharge capacity, the lowest oxygen reduction reaction/oxygen evolution reaction overpotential and the best cycle stability, indicating the excellent catalytic ability of the Co–Ru@C shell.

We use SiO2 as a template and dopamine as a carbon source to synthesize a hollow C shell, and we load Co and Ru nanoparticles onto it to obtain a Co–Ru@C shell composite.  相似文献   

19.
A nanoscale core–shell NiO@CoO composite is prepared on flexible carbon cloth for electrodes in supercapacitors and overall water splitting. The needle-like CoO nanowires with NiO nanosheets as the active materials improve the elemental constituents as well as surface area. The NiO@CoO electrode boasts a capacity of 2.87 F cm−2 (1024.05 F g−1) at 1 A g−1 current density, and even at a large current density of 20 A g−1 the retention ratio is 80.9% after 5000 cycles. The excellent specific capacity with high rate capability can be ascribed to the unique structure which increases the area of the liquid–solid interface and facilitates electron and ion transport, improving the utilization efficiency of active materials. The asymmetric hybrid supercapacitor prepared with the core–shell electrode shows the energy output of 40.3 W h kg−1 at 750 W kg−1 with a better retention (71.7%) of specific capacitance after 15 000 cycles. In addition, linear sweep voltammetry is performed to assess the performance of the electrode in water splitting and the electrode shows excellent activity in the OER as manifested by a Tafel slope of 88.04 mV dec−1. Our results show that the bifunctional structure and design strategy have large potential in energy applications.

A nanoscale core–shell NiO@CoO composite is prepared on flexible carbon cloth for electrodes in supercapacitors and overall water splitting.  相似文献   

20.
The development of green, economical and sustainable chemical processes is one of the primary challenges in organic synthesis. Herein, we report an efficient and heterogeneous palladium-catalyzed sulfonylation of vinyl cyclic carbonates with sodium sulfinates via decarboxylative cross-coupling. Both aliphatic and aromatic sulfinate salts react with various vinyl cyclic carbonates to deliver the desired allylic sulfones featuring tri- and even tetrasubstituted olefin scaffolds in high yields with excellent selectivity. The process needs only 2 mol% of Pd2(dba)3 and the in situ formed palladium nano-particles are found to be the active catalyst.

Heterogenous catalysis: economical and sustainable synthesis of allylic sulfone featuring tri- and even tetrasubstituted olefin scaffold via decarboxylative cross-coupling from vinyl cyclic carbonates with sodium sulfinates using PdNPs as a catalyst.  相似文献   

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