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1.
J Colloid Interface Sci ; 673: 228-238, 2024 Jun 08.
Article in English | MEDLINE | ID: mdl-38875789

ABSTRACT

Designing cost-effective electrocatalysts for water decomposition is crucial for achieving environmental-friendly hydrogen production. A transition metal sulfide/hydroxide electrocatalyst (1T-MoS2/Ni3S2/LDH) with double heterogeneous interfaces was developed through a two-step hydrothermal assisted electrodeposition method. The presence of the two built-in electric fields not only accelerated the charge transfer at the interface, but also enhanced the adsorption of the reactants and intermediate groups, and therefore improved the reaction rate and overall catalytic performance. The results suggest that the 1T-MoS2/Ni3S2/LDH catalysts display exceptional electrocatalytic reactivity. Under alkaline conditions, the overpotential of the electrocatalyst was 187 (η50) mV for OER and 104 (η10) mV for HER. Furthermore, the two-electrode system assembled by the electrocatalyst needs only a voltage of 1.55 V to deliver a current density of 10 mA cm-2. Our result provides a simple and effective methodical approach to the design of dual heterogeneous interfacial electrocatalysts.

2.
Nanoscale ; 16(16): 8151-8161, 2024 Apr 25.
Article in English | MEDLINE | ID: mdl-38572680

ABSTRACT

The rational design of the dimension and geometry of a plasmonic semiconductor cocatalyst is vitally important for efficient utilization of near-infrared (NIR) light and superior photocatalytic hydrogen generation. Herein, hollow cubic CuSe@CdS composites with different sizes and strong localized surface plasmon resonance (LSPR) were prepared by selenizing size-tunable Cu2O templates and loading CdS nanoparticles. The size of hollow cubic CuSe can affect the surface area and the conduction band potential through the size effect, regulating the carrier behavior of the CuSe@CdS heterojunction. The CuSe@CdS composites show enhanced and wide absorption in the full spectrum due to the LSPR effect of CuSe. Meanwhile, the composites show excellent photocatalytic hydrogen capacity in the full spectrum in a 0.35 M Na2S/0.25 M Na2SO3 sacrificial reagent solution. The best hydrogen production rate of CSCE2 is 1.518 mmol g-1 h-1 (5.54 times higher than that of CdS) under Vis light (780 > λ > 420 nm) irradiation and 0.28 mmol g-1 h-1 under NIR light (λ > 780 nm) illumination. Interestingly, the photocatalytic activity for H2 under Vis-NIR light (λ > 420 nm) is about 3 times (up to 4.45 mmol g-1 h-1) higher than that without NIR light assistance, due to the photothermal effect. Various analyses and DFT calculations demonstrate that the p-n heterojunction formed in the composites consists of p-type CuSe and n-type CdS, which achieves efficient carrier transfer and separation under the synergistic effect of the size effect and the photothermal effect. In addition, the expansion of the photocatalytic performance to the NIR range is mainly due to the "hot-electron" injection mechanism induced by the LSPR effect of CuSe. The reasonable design coupled with the plasmonic materials offers a new path to achieving the highly efficient conversion of solar energy to hydrogen energy.

3.
J Environ Manage ; 339: 117818, 2023 Aug 01.
Article in English | MEDLINE | ID: mdl-37030238

ABSTRACT

The exploitation and utilization of secondary resources have the social benefits of saving resources, reducing pollution, and reducing production costs. Currently, less than 20% of titanium secondary resources can be recycled, and there are few reviews on titanium secondary resources recovery, which cannot fully reveal the technical information and progress of titanium secondary resources recovery. This work presents the current global distribution of titanium resources and market supply and demand, then focuses on an overview of technical studies on titanium extraction from different titanium-bearing secondary slags. The following types of titanium secondary resources are mainly available: sponge titanium production, the production of titanium ingot, titanium dioxide production, red mud, titanium-bearing blast furnace slag, spent SCR catalyst, and lithium titanate waste. The various methods of secondary resource recovery are compared, including the advantages and disadvantages, and the future development direction of the titanium recycling process is pointed out. On the one hand, recycling companies can classify and recover each type of residual waste according to its characteristics. On the other hand, solvent extraction technology can be the direction of attention due to the increased requirement for the purity of recovered materials. Meanwhile, the attention to lithium titanate waste recycling should also be enhanced.


Subject(s)
Lithium , Titanium , Environmental Pollution , Recycling/methods
4.
Inorg Chem ; 62(17): 6825-6832, 2023 May 01.
Article in English | MEDLINE | ID: mdl-37074303

ABSTRACT

Photocatalysts with hollow structures have drawn great interest owing to their high specific surface area, which can enhance the photocatalytic performance. Herein, we designed the hollow cubic Cu2-xS@Ni-Mo-S nanocomposites by vulcanizing from the Cu2O template and loading the Ni-Mo-S lamellas. The Cu2-xS@Ni-Mo-S composites greatly improved the photocatalytic hydrogen performance. Among them, Cu2-xS-NiMo-5 achieved the optimal photocatalytic rate of 1326.07 µmol/g h, which is approximately 3.85 times higher than that of hollow Cu2-xS (344 µmol/g h) and had good stability for 16 h. The enhanced photocatalytic property was attributed to the metallic behavior of bimetallic Ni-Mo-S lamellas and the LSPR (localized surface plasmon resonance) effect of Cu2-xS. The bimetallic Ni-Mo-S can effectively capture the photogenerated electrons and quickly transfer-diffuse to produce H2. Meanwhile, the hollow Cu2-xS not only provided many more active sites to take part in the reaction but also introduced the LSPR effect to increase the solar utilization. This work provides valuable insights into the synergistic effect of using non-precious metal co-catalysts and the LSPR materials to assist in the photocatalytic hydrogen evolution.

5.
Small ; 17(31): e2101315, 2021 Aug.
Article in English | MEDLINE | ID: mdl-34160911

ABSTRACT

Water splitting to H2 by photocatalysis remains an effective strategy to alleviate the energy crisis. Unfortunately, single-component photocatalyst still suffers from sluggish reaction kinetics. In this work, a noble-metal free photocatalytic system of nitrogen-doped carbon@Co embedded in carbon nanotubes (NC@Co-NCT)/cadmium sulfide (CdS) is fabricated by coupling CdS nanorods with the metal-organic framework-derived Co encapsulated nitrogen-doped carbon (NC) material. The optimal photocatalytic activity of NC@Co-NCT/CdS is determined to be 3.8 mmol h-1  g-1 , which is ≈5.8 times of CdS. By combining the experimental evidences and density functional theory calculations, a novel photoelectron transfer channel in the heterojunction interfaces is revealed, expediting the migration and separation of photo-induced charge carriers of CdS. Moreover, the presence of Co nanoclusters can act as the active sites, boosting the H2 evolution reaction. This study can present a new avenue to design advanced photocatalysts with high-efficiency electrons and holes separation.

6.
ACS Appl Mater Interfaces ; 12(15): 17364-17375, 2020 Apr 15.
Article in English | MEDLINE | ID: mdl-32212636

ABSTRACT

Co-substituted LaFeO3 was electrodeposited on the surface of BiVO4 as a co-catalyst to enhance the water splitting performance. Compared to bare BiVO4, the BiVO4/Co-LaFeO3 composite photoanode shows a water oxidation photocurrent of 3.4 mA/cm2 at 1.23 V versus reverse hydrogen electrode, accompanied by a notable cathodic shift in the onset potential for 300 mV. Combined optical and electrochemical characterizations show that the solid/electrolyte charge transfer efficiency of BiVO4 are dramatically improved by the incorporation of Co-substituted LaFeO3. From the surface kinetic study of charge carriers by intensity-modulated photocurrent spectroscopy, a suppressed surface recombination rate constant is observed and the enhanced photoelectrochemical water splitting performance observed in the BiVO4/Co-LaFeO3 photoanode is attributed to the surface passivation effect of Co-substituted LaFeO3.

7.
Dalton Trans ; 49(6): 1776-1784, 2020 Feb 14.
Article in English | MEDLINE | ID: mdl-31967134

ABSTRACT

The development and utilization of low-cost and efficient electrocatalysts for overall water splitting is of great significance for future energy supplies. Herein, a Co-doped NiCu mixed oxide film on Ni foam as a bifunctional electrocatalyst for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is synthesized by a facile solvothermal method using methanol as a reactant followed by annealing in air and it exhibits remarkably enhanced HER and OER activities. The well-constructed surface and porous skeleton structure with a large volume provide a large number of catalytically active sites during the electrochemical reaction. Notably, CuO plays an important role in improving the catalytic activity of the electrode; meanwhile, Co doping is beneficial for increasing the conductivity and activating the Ni sites at lower overpotentials via the charge transfer effect. Accordingly, the optimized CuO-NiO/Ni foam electrode exhibits a comparatively low overpotential of 38 mV and 172 mV at 10 mA cm-2 for the HER and OER in 1.0 M KOH, respectively. Moreover, the electrode shows excellent long-term stability for 1000 cyclic voltammetric cycles in both the HER and OER. A self-assembled overall water splitting device using this electrode as both the anode and cathode achieves a current density of 10 mA cm-2 at a low cell voltage of 1.51 V. This study is promising and provides a simple method for depositing a multimetal mixed oxide on a metal substrate resulting in an efficient bifunctional electrocatalyst, holding great significance for future energy applications.

8.
ACS Appl Mater Interfaces ; 10(46): 39713-39722, 2018 Nov 21.
Article in English | MEDLINE | ID: mdl-30346126

ABSTRACT

Fe2TiO5 was synthesized via the solvothermal method and adopted as co-catalyst to improve the photoelectrochemical (PEC) water splitting performance of BiVO4 photoanode. After surface modification by Fe2TiO5, the BiVO4/Fe2TiO5 photoanode shows a 300 mV cathodic shift in onset potential and 3 times enhancement in photocurrent, which delivers a photocurrent density of 3.2 mA/cm2 at 1.23 V vs reverse hydrogen electrode. Systematic optical, electrochemical, and intensity-modulated photocurrent spectroscopy characterizations were performed to explore the role of Fe2TiO5 and reveal that the enhanced PEC performance is mainly caused by the surface passivation effect of Fe2TiO5.

9.
Dalton Trans ; 47(2): 348-356, 2018 Jan 02.
Article in English | MEDLINE | ID: mdl-29215106

ABSTRACT

Semiconductor-based photocatalytic hydrogen evolution from water with earth-abundant and low cost co-catalysts has attracted much attention. Herein, novel Cu2(OH)2CO3 decorated 2D TiO2 nanosheets for photocatalytic water splitting were synthesized by a facile in situ synthetic method. The chemical and photophysical properties of Cu2(OH)2CO3/TiO2 nanosheets were investigated by X-ray diffractometry (XRD), transmission electron microscopy (TEM), UV-vis diffusion reflectance spectroscopy (DRS), X-ray photoelectron spectroscopy (XPS) and cyclic voltammetry (CV) analysis. At an optimal Cu2(OH)2CO3 loading content of 1.5 mol%, the hybrid photocatalyst delivers a high photocatalytic H2 production rate of 1555.07 µmol g-1 h-1. Such enhanced photocatalytic activity is attributed to tight interfaces formed between Cu2(OH)2CO3 nanoparticles and TiO2 nanosheets, which play a vital role in the separation of photo-excited carriers, and the formation of active Cu1+ and Cu0 species can also benefit the charge separation process by reducing the over-potential of water reduction. Based on the above results, a possible mechanism is proposed and further verified using photoluminescence (PL) spectra. This work may provide more insight into the synthesis of novel Cu2(OH)2CO3/TiO2 nanosheets with high photocatalytic H2 evolution activity for solar-to-chemical conversion and utilization.

10.
Appl Phys Lett ; 110(22): 223903, 2017 May 29.
Article in English | MEDLINE | ID: mdl-28652643

ABSTRACT

Monolithically integrated hybrid tandem solar cells that effectively combine solution-processed colloidal quantum dot (CQD) and organic bulk heterojunction subcells to achieve tandem performance that surpasses the individual subcell efficiencies have not been demonstrated to date. In this work, we demonstrate hybrid tandem cells with a low bandgap PbS CQD subcell harvesting the visible and near-infrared photons and a polymer:fullerene-poly (diketopyrrolopyrrole-terthiophene) (PDPP3T):[6,6]-phenyl-C60-butyric acid methyl ester (PC61BM)-top cell absorbing effectively the red and near-infrared photons of the solar spectrum in a complementary fashion. The two subcells are connected in series via an interconnecting layer (ICL) composed of a metal oxide layer, a conjugated polyelectrolyte, and an ultrathin layer of Au. The ultrathin layer of Au forms nano-islands in the ICL, reducing the series resistance, increasing the shunt resistance, and enhancing the device fill-factor. The hybrid tandems reach a power conversion efficiency (PCE) of 7.9%, significantly higher than the PCE of the corresponding individual single cells, representing one of the highest efficiencies reported to date for hybrid tandem solar cells based on CQD and polymer subcells.

11.
Dalton Trans ; 46(32): 10620-10629, 2017 Aug 15.
Article in English | MEDLINE | ID: mdl-28401230

ABSTRACT

Novel layer-like Ni(OH)2 co-catalyst-decorated ZnIn2S4 microsphere photocatalysts were synthesized for the first time via a facile in situ deposition method to boost the photocatalytic H2-production performance. The physical and optical properties of the as-prepared Ni(OH)2-ZnIn2S4 composite samples were characterized via X-ray diffraction (XRD), transmission electron microscopy (TEM), UV-vis diffusion reflectance spectroscopy (DRS), X-ray photoelectron spectroscopy (XPS), and surface photovoltage spectroscopy (SPV). The results indicate that the photocatalytic H2 evolution activity of the ZnIn2S4 microspheres under visible light irradiation significantly enhances by introducing inexpensive Ni(OH)2 as a co-catalyst. The 5 mol% Ni(OH)2-ZnIn2S4 sample shows the highest H2-production rate of 8.35 mmol g-1 h-1, which is 18 times higher than that of pure ZnIn2S4. Moreover, photocatalytic activity of the Ni(OH)2-ZnIn2S4 sample remains stable even after 4 cycling photocatalytic experiments. In addition, a possible mechanism on the enhanced photocatalytic activity was proposed and verified by surface photovoltage spectroscopy.

12.
Dalton Trans ; 46(32): 10578-10585, 2017 Aug 15.
Article in English | MEDLINE | ID: mdl-28146151

ABSTRACT

Cobalt oxide decorated octahedral ceria hollow structures (CoOx/CeO2) with various contents of CoOx nanoparticles were prepared via a simple chemical impregnation method. The obtained samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), high resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS), UV-Vis diffuse-reflectance spectroscopy (DRS), surface photovoltage spectroscopy (SPV) and transient photovoltage spectroscopy (TPV). The photocatalytic oxygen evolution via water oxidation was investigated for the as-prepared CoOx/CeO2 nanocage composites. The photocatalytic results indicate that the CoOx/CeO2 nanocage composite with 1 mol% CoOx shows the highest photocatalytic activity. The excellent photocatalytic activity can be attributed to the improved visible-light absorption of CoOx/CeO2 composites and the efficient separation of excited electron-hole pairs between CoOx and CeO2, which can effectively enhance the lifetime of charge carriers in the CoOx-modified samples and then improve the oxygen evolution activity. Cobalt oxide is expected to be an excellent water oxidation co-catalyst for semiconductor photocatalysts.

13.
Adv Mater ; 28(17): 3366-73, 2016 05.
Article in English | MEDLINE | ID: mdl-26946165

ABSTRACT

Efficient homo-tandem and triple-junction polymer solar cells are constructed by stacking identical subcells composed of the wide-bandgap polymer PBDTTPD, achieving power conversion efficiencies >8% paralleled by open-circuit voltages >1.8 V. The high-voltage homo-tandem is used to demonstrate PV-driven electrochemical water splitting with an estimated solar-to-hydrogen conversion efficiency of ≈6%.

14.
ACS Appl Mater Interfaces ; 6(4): 2219-23, 2014 Feb 26.
Article in English | MEDLINE | ID: mdl-24495100

ABSTRACT

Highly transparent and UV-resistant superhydrophobic arrays of SiO2-coated ZnO nanorods are prepared in a sequence of low-temperature (<150 °C) steps on both glass and thin sheets of PET (2 × 2 in.(2)), and the superhydrophobic nanocomposite is shown to have minimal impact on solar cell device performance under AM1.5G illumination. Flexible plastics can serve as front cell and backing materials in the manufacture of flexible displays and solar cells.

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