Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 77
Filtrar
1.
Small ; 20(7): e2306258, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-37806759

RESUMO

Aqueous alkaline Zn-based batteries (AAZBs) possess great promise for large-scale applications thanks to their higher discharging plateau and unique reaction mechanism. However, the capacity and rate capability of Ni-based cathodes are still unsatisfactory due to their insufficient OH- adsorption and diffusion ability. Herein, heterostructured Ni3 S2 /Ni(OH)2 nanosheets with outstanding electrochemical performance are synthesized via a facile chemical etching strategy. The heterostructured Ni3 S2 /Ni(OH)2 nanosheet cathode shows significantly increased capacity and rate capability due to its boosted OH- adsorption and diffusion ability compared to Ni3 S2 . Consequently, the assembled Zn//Ni3 S2 /Ni(OH)2 cell can deliver an ultrahigh capacity of 2.26 mAh cm-2 , an excellent rate performance (0.91 mAh cm-2 at 100 mA cm-2 ) and a satisfying cycling stability (1.01 mAh cm-2 at 20 mA cm-2 after 500 cycles). Moreover, a prominent energy density of 3.86 mWh cm-2 is obtained, which exceeds the majority of recently reported AAZBs. This work is expected to provide a new modification direction for developing high-performance nickel sulfide cathode for AAZBs.

2.
Small ; 20(1): e2304782, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37649181

RESUMO

Rational designing electrocatalysts is of great significance for realizing high-efficiency H2 production in the water splitting process. Generally, reducing the usage of precious metals and developing low-potential nucleophiles oxidation reaction to replace anodic oxygen evolution reaction (OER) are efficient strategies to promote H2 generation. Here, NiS-coated nickel-carbon nanofibers (NiS@Ni-CNFs) are prepared for low-content Pt deposition (Pt-NiS@Ni-CNFs) to attain the alkaline HER catalyst. Due to the reconfiguration of NiS phase and synergistic effect between Pt and nickel sulfides, the Pt-NiS@Ni-CNFs catalyst shows a high mass activity of 2.74-fold of benchmark Pt/C sample. In addition, the NiS@Ni-CNFs catalyst performs a superior urea oxidation reaction (UOR) activity with the potential of 1.366 V versus reversible hydrogen electrode (RHE) at 10 mA cm-2 , which demonstrates the great potential in the replacement of OER. Thus, a urea-assisted water splitting electrolyzer of Pt-NiS@Ni-CNFs (cathode)||NiS@Ni-CNFs (anode) is constructed to exhibit small voltages of 1.44 and 1.65 V to reach 10 and 100 mA cm-2 , which is much lower than its overall water splitting process, and presents a 6.5-fold hydrogen production rate enhancement. This work offers great opportunity to design new catalysts toward urea-assisted water splitting with significantly promoted hydrogen productivity and reduced energy consumption.

3.
Small ; : e2404060, 2024 Sep 05.
Artigo em Inglês | MEDLINE | ID: mdl-39235565

RESUMO

In recent years, catalysts based on transition metal sulfides have garnered extensive attention due to their low cost and excellent electrocatalytic activity in the alkaline oxygen evolution reaction. Here, the preparation of Fe-doped Ni3S2 via a one-step hydrothermal approach is reported by utilizing inexpensive transition metals Ni and Fe. In an alkaline medium, Fe-Ni3S2 exhibits outstanding electrocatalytic activity and stability for the OER, and the current density can reach 10 mA cm-2 with an overpotential of 163 mV. In addition, Pt/C||Fe-Ni3S2 is used as the membrane electrode of the anion exchange membrane water electrolyzer, which is capable of providing a current density of 650 mA cm-2 at a cell voltage of 2.0 V, outperforming the benchmark Ir/C. The principle is revealed that the doping of Fe enhances the electrocatalytic water decomposition ability of Ni3S2 by in situ Raman and in situ X-ray absorption fine structure. The results indicate that the doping of Fe decreases the charge density near Ni atoms, which renders Fe-Ni3S2 more favorable for the adsorption of OH- and the formation of *OO- intermediates. This work puts forward an effective strategy to significantly improve both the alkaline OER activity and stability of low-cost electrocatalysts.

4.
Chemistry ; : e202403030, 2024 Oct 11.
Artigo em Inglês | MEDLINE | ID: mdl-39392070

RESUMO

Anion exchange membrane (AEM) water electrolyser has shown its potential in green hydrogen production. One of the crucial tasks is discover novel cost-effective and sustainable electrocatalyst materials. In this study, a low-cost Ni-S-based catalyst for hydrogen evolution reaction was prepared via a simple electrodeposition process from a modified Watts bath recipe. Physical characterisation methods suggest this deposit film to be amorphous. Optimisation of the electrodeposition parameters of the NixSy catalyst was carried out using a rotating disk electrode setup. The optimised catalyst exhibited excellent catalytical performance in 1 M KOH on a microelectrode, with overpotentials of 41 mV, 111 mV and 202 mV at 10, 100 and 1000 mA cm-2 with Tafel slope of 67.9 mV dec-1 recorded at 333 K. Long-term testing of the catalyst demonstrated steady performance over a 24 h period on microelectrode at 100 mA cm-2 with only 71 mV and 37 mV overpotential increase at 293 K and 333 K respectively. Full cell testing with the optimised NixSy as cathode and NiFe(OH-)2 as anode showed 1.88 V after 1 h electrolysis at 500 mA cm-2 in 1 M KOH under 333 K with FAA-3-30 membrane.

5.
Nano Lett ; 23(11): 5027-5034, 2023 Jun 14.
Artigo em Inglês | MEDLINE | ID: mdl-37249308

RESUMO

Tuning the electroactive surface species of electrocatalysts remains a significant challenge for achieving highly efficient oxygen evolution reactions. Herein, we propose an innovative in situ leaching strategy, modulated by cationic oxidation, to achieve active self-reconstruction of these catalysts. Vanadium is introduced as a cation into Ni3S2 and oxidized under low oxidative potential, leading to subsequent leaching into the electrolyte and triggering self-reconstruction. The structural evolution from V-Ni3S2 to Ni(OH)2 and subsequently to NiOOH is identified by operando Raman as a three-step transition. In contrast, V-free Ni3S2 is unable to bypass the thermodynamically predicted nickel oxysulfide products to transform into active NiOOH. As a result, the self-restructured V-Ni3S2 only needs an ultralow overpotential of 155 mV at 10 mA cm-2, outperforming V-free Ni3S2 and many other advanced catalysts. This work provides new guidelines for manipulating in situ leaching to modulate the self-reconstruction of catalysts.

6.
Small ; 19(17): e2207425, 2023 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-36703521

RESUMO

Urea-assisted hybrid water splitting is a promising technology for hydrogen (H2 ) production, but the lack of cost-effective electrocatalysts hinders its extensive application. Herein, it is reported that Nitrogen-doped Co9 S8 /Ni3 S2 hybrid nanosheet arrays on nickel foam (N-Co9 S8 /Ni3 S2 /NF) can act as an active and robust bifunctional catalyst for both urea oxidation reaction (UOR) and hydrogen evolution reaction (HER), which could drive an ultrahigh current density of 400 mA cm-2 at a low working potential of 1.47 V versus RHE for UOR, and gives a low overpotential of 111 mV to reach 10 mA cm-2 toward HER. Further, a hybrid water electrolysis cell utilizing the synthesized N-Co9 S8 /Ni3 S2 /NF electrode as both the cathode and anode displays a low cell voltage of 1.40 V to reach 10 mA cm-2 , which can be powered by an AA battery with a nominal voltage of 1.5 V. The density functional theory (DFT) calculations decipher that N-doped heterointerfaces can synergistically optimize Gibbs free energy of hydrogen and urea, thus accelerating the catalytic kinetics of HER and UOR. This work significantly advances the development of the promising cobalt-nickel-based sulfide as a bifunctional electrocatalyst for energy-saving electrolytic H2 production and urea-rich innocent wastewater treatment.

7.
Small ; 19(27): e2300194, 2023 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-36965012

RESUMO

Versatile electrocatalysis at higher current densities for natural seawater splitting to produce hydrogen demands active and robust catalysts to overcome the severe chloride corrosion, competing chlorine evolution, and catalyst poisoning. Hereto, the core-shell-structured heterostructures composed of amorphous NiFe hydroxide layer capped Ni3 S2 nanopyramids which are directly grown on nickel foam skeleton (NiS@LDH/NF) are rationally prepared to regulate cooperatively electronic structure and mass transport for boosting oxygen evolution reaction (OER) performance at larger current densities. The prepared NiS@LDH/NF delivers the anodic current density of 1000 mA cm-2 at the overpotential of 341 mV in 1.0 m KOH seawater. The feasible surface reconstruction of Ni3 S2 -FeNi LDH interfaces improves the chemical stability and corrosion resistance, ensuring the robust electrocatalytic activity in seawater electrolytes for continuous and stable oxygen evolution without any hypochlorite production. Meanwhile, the designed Ni3 S2 nanopyramids coated with FeNi2 P layer (NiS@FeNiP/NF) still exhibit the improved hydrogen evolution reaction (HER) activity in 1.0 m KOH seawater. Furthermore, the NiS@FeNiP/NF||NiS@LDH/NF pair requires cell voltage of 1.636 V to attain 100 mA cm-2 with a 100% Faradaic efficiency, exhibiting tremendous potential for hydrogen production from seawater.

8.
Small ; 19(50): e2304918, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37626450

RESUMO

Developing composite materials with the synergistic effects of heterogeneous structures and multiple components is considered as a promising strategy to achieve high-performance electromagnetic wave (EMW) absorbers. To further satisfy the demand of broadband and strong microwave absorption, a novel NiS/carbon nanofibers (CNFs)/porous carbon composite is successfully synthesized by hydrothermal and chemical vapor deposition using lotus leaves as a biomass carbon source. A few carbon nanotubes (CNTs) and uniformly dispersed Ni nanocrystals have also been found in the hybrid. Benefiting from the porous structure derived from lotus leaves, the combination of dielectric NiS, conductive carbon nanomaterials, and magnetic Ni nanoparticles, together with the three-dimensional conductive network of CNFs and CNTs, the remarkable EMW absorption properties with a minimum reflection loss up to -67.65 dB have been achieved at merely 2.32 mm. Besides, the widest effective absorption band can reach 5.9 GHz with a thin thickness of 2.07 mm, covering almost the entire Ku band. In addition, under the incident angle of 31°, the radar cross-section reduction value of LNSF-600 can reach 42.88 dBm2. Therefore, this work provides an efficient and facile method for manufacturing outstanding biomass-derived EMW absorbers.

9.
Small ; 19(50): e2304081, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37649183

RESUMO

Designing efficient and stable transition metal-based catalysts for electrocatalytic water splitting is vital for the development of hydrogen production. Herein, a facile synthetic strategy is developed to fabricate transition metal-based heterogeneous structural Co2 P-Ni3 S2 hollow nanowires supported on nickel foam (Co2 P-Ni3 S2 /NF). Owing to the multiple active sites provided by transition metal compounds, large surface area of the unique hollow nanowire morphology, and the synergistic effect of Co2 P-Ni3 S2 heterostructure interfaces, Co2 P-Ni3 S2 /NF requires ultralow overpotentials of 110, 164 mV for HER and 331.7, 358.3 mV for OER at large current densities of 100, 500 mA cm-2 in alkaline medium, respectively. Importantly, the two-electrode electrolyzer assembled by Co2 P-Ni3 S2 /NF displays a cell voltage of 1.54 V at 10 mA cm-2 and operates stably over 24 h at 100 mA cm-2 , which performs better than reported transition metal-based bifunctional electrocatalysts. This work presents a successful fabrication of transition metal-based bifunctional HER/OER electrocatalysts at large-current density and brings new inspiration for developing applicable energy conversion materials.

10.
Small ; 19(52): e2304435, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37642532

RESUMO

Heterogeneous crystalline-amorphous structures, with tunable electronic structures and morphology, hold immense promise as catalysts for lithium-oxygen batteries (LOBs). Herein, a nanotube network constructed by crystalline nickel sulfide/amorphous nickel phosphate (NiS/NiPO) heterostructure is prepared on Ni foam through the sulfurization of the precursor generated hydrothermally. Used as cathodes, the NiS/NiPO nanotubes with optimized electronic structure can induce the deposition of the highly porous and interconnected structure of Li2 O2 with rich Li2 O2 -electrolyte interfaces. Abundant active sites can be created on NiS/NiPO through the charge redistribution for the uniform nucleation and growth of Li2 O2 . Moreover, nanotube networks endow cathodes with efficient transport channels and sufficient space for the accommodation of Li2 O2 . A high discharge capacity of 27 003.6 mAh g-1 and a low charge overpotential of 0.58 V at 1000 mAh g-1 can be achieved at 200 mA g-1 . This work provides valuable insight into the unique role of the electronic structure and morphology of catalysts in the formation mechanisms of Li2 O2 and the performances of LOBs.

11.
Small ; 19(16): e2206679, 2023 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-36651137

RESUMO

The development of a competent (pre)catalyst for the oxygen evolution reaction (OER) to produce green hydrogen is critical for a carbon-neutral economy. In this aspect, the low-temperature, single-source precursor (SSP) method allows the formation of highly efficient OER electrocatalysts, with better control over their structural and electronic properties. Herein, a transition metal (TM) based chalcogenide material, nickel sulfide (NiS), is prepared from a novel molecular complex [NiII (PyHS)4 ][OTf]2 (1) and utilized as a (pre)catalyst for OER. The NiS (pre)catalyst requires an overpotential of only 255 mV to reach the benchmark current density of 10 mA cm-2 and shows 63 h of chronopotentiometry (CP) stability along with over 95% Faradaic efficiency in 1 m KOH. Several ex situ measurements and quasi in situ Raman spectroscopy uncover that NiS irreversibly transformed to a carbonate-intercalated γ-NiOOH phase under the alkaline OER conditions, which serves as the actual active structure for the OER. Additionally, this in situ formed active phase successfully catalyzes the selective oxidation of alcohol, aldehyde, and amine-based organic substrates to value-added chemicals, with high efficiencies.

12.
Environ Res ; 236(Pt 1): 116782, 2023 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-37517497

RESUMO

Sulfide-containing wastewater, characterized by its foul odor, corrosiveness, and toxicity, can endanger human health. Fluidized-bed homogeneous crystallization (FBHC) avoids the excessive sludge production commonly associated with conventional chemical precipitation methods. In this study, FBHC is used to treat sulfur-containing synthetic wastewater. Furthermore, nickel-containing wastewater was utilized as a precipitant in the system, hence the advantage of simultaneous sulfur and nickel removal from the wastewater. The operating parameters, including pH, a precipitant dosage of [Ni2+]0/[S2-]0, and cross-sectional surface loading (LS, kg/m2h) are optimized. The optimum operating conditions of pH 9.8 ± 0.3, [Ni2+]0/[S2-]0 = 0.8, and LS = 1.5 kg/m2h results in total sulfur removal (TR) of 95.7% and crystallization ratio (CR) of 94.8%. The effect of organic compounds (acetic acid, oxalic acid, EDTA, and citric acid) and inorganic ions (NO3-, CO32-, PO43-, F-, and Cl-) on the nickel sulfide granulation process was discussed.

13.
Molecules ; 28(11)2023 May 24.
Artigo em Inglês | MEDLINE | ID: mdl-37298783

RESUMO

A one-step sulfurization method to fabricate Ni3S2 nanowires (Ni3S2 NWs) directly on a Ni foam (NF) was developed as a simple, low-cost synthesis method for use as a supercapacitor (SC), aimed at optimizing energy storage. Ni3S2 NWs have high specific capacity and are considered a promising electrode material for SCs; however, their poor electrical conductivity and low chemical stability limit their applications. In this study, highly hierarchical three-dimensional porous Ni3S2 NWs were grown directly on NF by a hydrothermal method. The feasibility of the use of Ni3S2/NF as a binder-free electrode for achieving high-performance SCs was examined. Ni3S2/NF exhibited a high specific capacity (255.3 mAh g-1 at a current density of 3 A g-1), good rate capability (2.9 times higher than that of the NiO/NF electrode), and competitive cycling performance (capacity retention of specific capacity of 72.17% after 5000 cycles at current density of 20 A g-1). Owing to its simple synthesis process and excellent performance as an electrode material for SCs, the developed multipurpose Ni3S2 NWs electrode is expected to be a promising electrode for SC applications. Furthermore, the synthesis method of self-growing Ni3S2 NW electrodes on 3D NF via hydrothermal reactions could potentially be applied to the fabrication of SC electrodes using a variety of other transition metal compounds.


Assuntos
Fontes de Energia Elétrica , Porosidade , Condutividade Elétrica , Eletrodos
14.
Nanotechnology ; 32(27)2021 Apr 14.
Artigo em Inglês | MEDLINE | ID: mdl-33770782

RESUMO

Rechargeable Zn-air batteries are a promising type of metal-air batteries for high-density energy storage. However, their practical use is limited by the use of costly noble-metal electrocatalysts for the sluggish kinetics of the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) occurred at the air electrode of the Zn-air batteries. This work reports a new non-precious bifunctional OER/ORR electrocatalyst of NiSx/carbon nanotubes (CNTs), which is made by atomic layer deposition (ALD) of nickel sulfide (NiSx) on CNTs, for the applications for the air electrode of the Zn-air batteries. The NiSx/CNT electrocatalyst on a carbon cloth electrode exhibits a low OER overpotential of 288 mV to reach 10 mA cm-2in current density, and the electrocatalyst on a rotating disk electrode exhibits a half-wave ORR potential of 0.81 V in alkaline electrolyte. With the use of the NiSx/CNT electrocatalyst for the air electrode, the fabricated aqueous rechargeable Zn-air batteries show a fairly good maximum output power density of 110 mW cm-2, which highlights the great promise of the ALD NiSx/CNT electrocatalyst for Zn-air batteries.

15.
Mikrochim Acta ; 188(2): 34, 2021 01 08.
Artigo em Inglês | MEDLINE | ID: mdl-33417060

RESUMO

Nickel sulfide nanoworm (Ni3S2 NW) network architecture was directly grown on the poly (3,4-ethylenedioxythiophene)-reduced graphene oxide hybrid films (PEDOT-rGO HFs) modified on glassy carbon electrode (GCE), acting as a binder-free sensor for high-performance non-enzymatic glucose monitoring. The sensor exhibited the satisfactory sensitivity (2123 µA mM-1 cm-2), wide linear range (15~9105 µM), low detection limit (0.48 µM), and rapid response time (< 1.5 s) at a potential of 0.5 V (vs. SCE) in 0.1 M NaOH and possessed good selectivity, reproducibility, and stability. The enhanced electrocatalytic activity of the sensor towards glucose oxidation was attributed to the particular morphology, satisfying hydrophilic nature, strong combination between Ni3S2 NWs, PEDOT-rGO, and bare GCE. Moreover, it can be used for assaying glucose in human serum samples without dilution, indicating potential for clinical diagnostic applications. Graphical abstract Nickel sulfide nanoworms (Ni3S2 NWs)/poly (3,4-ethylenedioxythiophene)-reduced graphene oxide hybrid films (PEDOT-rGO HFs) were used to construct a binder-free high-performance non-enzymatic glucose sensor with satisfactory sensitivity, wide linear range, low detection limit, good selectivity, amazing reproducibility, and stability.


Assuntos
Glicemia/análise , Técnicas Eletroquímicas/métodos , Nanopartículas Metálicas/química , Níquel/química , Glicemia/química , Compostos Bicíclicos Heterocíclicos com Pontes/química , Técnicas Eletroquímicas/instrumentação , Eletrodos , Grafite/química , Humanos , Limite de Detecção , Oxirredução , Polímeros/química , Reprodutibilidade dos Testes
16.
Mikrochim Acta ; 187(8): 468, 2020 07 22.
Artigo em Inglês | MEDLINE | ID: mdl-32700244

RESUMO

An enzyme-free electrochemical sensor platform is reported based on hollow sphere structured nickel sulfide (HS-NiS) nanomaterials for the sensitive lactic acid (LA) detection in human urine. Hollow sphere nickel sulfide nanostructures directly grow on the nickel foam (NiF) substrate by using facile and one-step electrochemical deposition strategy towards the electrocatalytic lactic acid oxidation and sensing for the first time. The as-developed nickel sulfide nanostructured electrode (NiF/HS-NiS) has been successfully employed as the enzyme mimic electrode towards the enhanced electrocatalytic oxidation and detection of lactic acid. The NiF/HS-NiS electrode exhibits an excellent electrocatalytic activity and sensing ability with low positive potential (~ 0.52 V vs Ag/AgCl), catalytic current density (~ 1.34 mA), limit of detection (LOD) (0.023 µM), linear range from 0.5 to 88.5 µM with a correlation coefficient of R2 = 0.98, sensitivity (0.655 µA µM-1 cm-2), and selectivity towards the lactic acid owing to the ascription of high inherent electrical conductivity, large electrochemical active surface area (ECASA), high electrochemical active sites, and strong adsorption ability. The sensors developed in this work demonstrate the selectivity against potential interferences, including uric acid (UA), ascorbic acid (AA), paracetamol (PA), Mg2+, Na+, and Ca2+. Furthermore, the developed sensors show practicability by sensing lactic acid in human urine samples, suggesting that the HS-NiS nanostructures device has promising clinical diagnostic potential. Graphical abstract.


Assuntos
Técnicas Eletroquímicas/métodos , Ácido Láctico/urina , Nanoestruturas/química , Níquel/química , Adulto , Catálise , Humanos , Ácido Láctico/química , Limite de Detecção , Oxirredução , Adulto Jovem
17.
Small ; 15(49): e1904433, 2019 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31643136

RESUMO

In this work, a facile strategy for the construction of single crystalline Ni3 S2 nanowires coated with N-doped carbon shell (NC) forming Ni3 S2 @NC core/shell arrays by one-step chemical vapor deposition process is reported. In addition to the good electronic conductivity from the NC shell, the nanowire structure also ensures the accommodation of large volume expansion during cycling, leading to pre-eminent high-rate capacities (470 mAh g-1 at 0.05 A g-1 and 385 mAh g-1 at 2 A g-1 ) and outstanding cycling stability with a capacity retention of 91% after 100 cycles at 1 A g-1 . Furthermore, ex situ transmission electron microscopy combined with X-ray diffraction and Raman spectra are used to investigate the reaction mechanism of Ni3 S2 @NC during the charge/discharge process. The product after delithiation consists of Ni3 S2 and sulfur, suggesting that the capacity of the electrode comes from the conversion reaction of both Ni3 S2 and sulfur with Li2 S.

18.
Small ; 14(8)2018 02.
Artigo em Inglês | MEDLINE | ID: mdl-29286583

RESUMO

Exploration of the relationship between electrocatalytic activities and their chemical valence is very important in rational design of high-efficient electrocatalysts. A series of porous nickel sulfides hybridized with N and S co-doped carbon nanoparticles (Nix Sy -NSCs) with different chemical valences of Ni, Ni9 S8 -NSCs, Ni9 S8 -NiS1.03 -NSCs, and NiS1.03 -NSCs are successfully fabricated, and their electrocatalytic performances as oxygen evolution reaction electrocatalysts are systematically investigated. The Nix Sy -NSCs are obtained via a two-step reaction including a low-temperature synthesis of Ni-Cys precursor followed by thermal decomposing of the precursor in Ar atmosphere. By controlling the sulfidation process during the formation of Nix Sy -NSCs, Ni9 S8 -NSCs, Ni9 S8 -NiS1.03 -NSCs, and NiS1.03 -NSCs are obtained, respectively, giving rise to the increase of high-valence Ni component, and resulting in gradually enhanced oxygen evolution reaction electrocatalytic activities. In particular, the NiS1.03 -NSCs show an exceptional low overpotential of ≈270 mV versus reversible hydrogen electrode at a current density of 10 mA cm-2 and a small Tafel slope of 68.9 mV dec-1 with mass loading of 0.25 mg cm-2 in 1 m KOH and their catalytic activities remained for at least 10 h, which surpass the state-of-the-art IrO2 , RuO2 , and Ni-based electrocatalysts.

19.
Molecules ; 23(7)2018 Jun 25.
Artigo em Inglês | MEDLINE | ID: mdl-29941846

RESUMO

The selective oxidation of H2S to elemental sulfur was carried out on a NiS2/SiCfoam catalyst under reaction temperatures between 40 and 80 °C using highly H2S enriched effluents (from 0.5 to 1 vol.%). The amphiphilic properties of SiC foam provide an ideal support for the anchoring and growth of a NiS2 active phase. The NiS2/SiC composite was employed for the desulfurization of highly H2S-rich effluents under discontinuous mode with almost complete H2S conversion (nearly 100% for 0.5 and 1 vol.% of H2S) and sulfur selectivity (from 99.6 to 96.0% at 40 and 80 °C, respectively), together with an unprecedented sulfur-storage capacity. Solid sulfur was produced in large aggregates at the outer catalyst surface and relatively high H2S conversion was maintained until sulfur deposits reached 140 wt.% of the starting catalyst weight. Notably, the spent NiS2/SiCfoam catalyst fully recovered its pristine performance (H2S conversion, selectivity and sulfur-storage capacity) upon regeneration at 320 °C under He, and thus, it is destined to become a benchmark desulfurization system for operating in discontinuous mode.


Assuntos
Compostos Inorgânicos de Carbono/química , Sulfeto de Hidrogênio/química , Níquel/química , Compostos de Silício/química , Catálise , Temperatura Baixa , Oxirredução , Enxofre/química
20.
Small ; 13(18)2017 05.
Artigo em Inglês | MEDLINE | ID: mdl-28296136

RESUMO

Efficient and durable oxygen evolution reaction (OER) catalysts are highly required for the cost-effective generation of clean energy from water splitting. For the first time, an integrated OER electrode based on one-step direct growth of metallic iron-nickel sulfide nanosheets on FeNi alloy foils (denoted as FeNi3 S2 /FeNi) is reported, and the origin of the enhanced OER activity is uncovered in combination with theoretical and experimental studies. The obtained FeNi3 S2 /FeNi electrode exhibits highly catalytic activity and long-term stability toward OER in strong alkaline solution, with a low overpotential of 282 mV at 10 mA cm-2 and a small Tafel slope of 54 mV dec-1 . The excellent activity and satisfactory stability suggest that the as-made electrode provides an attractive alternative to noble metal-based catalysts. Combined with density functional theory calculations, exceptional OER performance of FeNi3 S2 /FeNi results from a combination of efficient electron transfer properties, more active sites, the suitable O2 evolution kinetics and energetics benefited from Fe doping. This work not only simply constructs an excellent electrode for water oxidation, but also provides a deep understanding of the underlying nature of the enhanced OER performance, which may serve as a guide to develop highly effective and integrated OER electrodes for water splitting.

SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA