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1.
Nano Lett ; 24(5): 1753-1760, 2024 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-38287247

RESUMO

Polymer based low evaporation enthalpy materials have become a universal selection for improving the efficiency of solar steam generation. Although water cluster and intermediate water mechanisms have been proposed to explain the low evaporation enthalpy, the production process and microstructure of activated water are still unclear. Here, crystal plane engineering is used to investigate the intermediate water state and the water cluster activation mechanism. The unique open-closed coordination structure on the optimized crystal surface promotes the generation of firm water clusters by optimizing the intermediate water state. Under the similar solar energy absorption of all materials, crystal plane engineering increased the solar steam generation rate of the evaporator by 31.2% and increased the energy efficiency to 94.8%. Exploring the micro-evaporation process and activated water structure is expected to stimulate the development of the next generation low evaporation enthalpy materials.

2.
Small ; 20(30): e2312173, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38409521

RESUMO

In heterogeneous persulfate-catalyzed oxidation systems, the mechanism underlying the crystal plane effects of the catalyst on the selective conversion of reactive oxygen species (ROS) remains ambiguous. In this study, nano-Co3O4 catalysts with varying crystallinity and exposure levels of (111) crystal planes are prepared via a hydrothermal method. Compared to low crystalline catalysts, high crystallinity catalysts predominantly expose (111) planes containing higher concentrations of Co2+ and oxygen vacancies (Ov), resulting in an increase degradation efficiency of p-nitrobenzaldehyde (4-NBA) from 74.5% to 100%. Radical quenching experiments and EPR characterization reveal that the degradation of 4-NBA occurs through a radical pathway, and quantification of radicals demonstrates that increasing exposure levels of (111) planes effectively promote radical yield (CSO4•- increase from 18.2 to 172.8 µm and C•OH increase from 1 to 58.9 µm). Furthermore, XPS and DFT calculations indicate that high crystallinity catalyst possesses more Ov active sites on (111) planes. The presence of Ov not only facilitates the adsorption of PMS molecules but also enhances electron transfer from Co2+ to PMS, leading to directed formation and efficient transformation of radicals. This study presents a novel strategy for promoting efficient radical formation in persulfate-activated systems.

3.
Small ; 20(30): e2312116, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38446107

RESUMO

Flexible zinc-ion batteries have garnered significant attention in the realm of wearable technology. However, the instability of hydrogel electrolytes in a wide-temperature range and uncontrollable side reactions of the Zn electrode have become the main problems for practical applications. Herein, N,N-dimethylformamide (DMF) to design a binary solvent (H2O-DMF) is introduced and combined it with polyacrylamide (PAM) and ZnSO4 to synthesize a hydrogel electrolyte (denoted as PZD). The synergistic effect of DMF and PAM not only guides Zn2+ deposition on Zn(002) crystal plane and isolates H2O from the Zn anode, but also breaks the hydrogen bonding network between water to improve the wide-temperature range stability of hydrogel electrolytes. Consequently, the symmetric cell utilizing PZD can stably cycle over 5600 h at 0.5 mA cm- 2@0.5 mAh cm-2. Furthermore, the Zn//PZD//MnO2 full cell exhibits favorable wide-temperature range adaptability (for 16000 cycles at 3 A g-1 under 25 °C, 750 cycles with 98 mAh g-1 at 0.1 A g-1 under -20 °C) and outstanding mechanical properties (for lighting up the LEDs under conditions of pressure, bending, cutting, and puncture). This work proposes a useful modification for designing a high-performance hydrogel electrolyte, which provides a reference for investigating the practical flexible aqueous batteries.

4.
Molecules ; 29(13)2024 Jul 07.
Artigo em Inglês | MEDLINE | ID: mdl-38999172

RESUMO

This article presents cyclic voltammetry, Tafel polarization, and ac. impedance spectroscopy examinations of resorcinol (RC) ion reactivity on Pt(511) single-crystal plane and the effect of surface-electrosorbed RC ions on the kinetics of UPD H (underpotentially deposited hydrogen) and HER (hydrogen evolution reaction) processes in 0.1 M NaOH solution. Obtained data delivered a proof for the RC ion surface adsorption and its later electroreduction over the potential range characteristic for the UPD H. A favourable role of platinum-adsorbed resorcinol anions on the kinetics of the UPD H and HER processes is also discussed. The above was explained via the recorded capacitance and charge-transfer resistance parameters (the presence of resorcinol at 1.5 × 10-3 M in 0.1 M NaOH caused significant reduction in the resistance parameter values by 3.9 and 2.6 times, correspondingly, for the UPD of H at 50 mV and the HER process, examined at -50 mV vs. RHE) along with the charge transients, produced by injecting small amounts of RC-based 0.1 M NaOH solution to initially RC-free base electrolyte on the Pt(511) electrode plane (a large cathodic charge-transient density of -90 µC cm-2 was recorded at the electrode potential of 50 mV).

5.
Angew Chem Int Ed Engl ; 63(21): e202402342, 2024 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-38491787

RESUMO

Zn deposition with a surface-preferred (002) crystal plane has attracted extensive attention due to its inhibited dendrite growth and side reactions. However, the nucleation and growth of the Zn(002) crystal plane are closely related to the interfacial properties. Herein, oriented growth of Zn(002) crystal plane is realized on Ag-modified surface that is directly visualized by in situ atomic force microscopy. A solid solution HCP-Zn (~1.10 at. % solubility of Ag, 30 °C) is formed on the Ag coated Zn foil (Zn@Ag) and possesses the same crystal structure as Zn to reduce its nucleation barrier caused by their lattice mismatch. It merits oriented Zn deposition and corrosion-resistant surface, and presents long cycling stability in symmetric cells and full cells coupled with V2O5 cathode. This work provides insights into interfacial regulation of Zn anodes for high-performance aqueous zinc metal batteries.

6.
Angew Chem Int Ed Engl ; 62(27): e202303953, 2023 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-37118911

RESUMO

Prussian blue analogues (PBAs) have been regarded as promising cathode materials for alkali-ion batteries owing to their high theoretical energy density and low cost. However, the high water and vacancy content of PBAs lower their energy density and bring safety issues, impeding their large-scale application. Herein, a facile "potassium-ions assisted" strategy is proposed to synthesize highly crystallized PBAs. By manipulating the dominant crystal plane and suppressing vacancies, the as-prepared PBAs exhibit increased redox potential resulting in high energy density up to ≈450 Wh kg-1 , which is at the same level of the well-known LiFePO4 cathodes for lithium-ion batteries. Remarkably, unconventional highly-reversible phase evolution and redox-active pairs were identified by multiple in situ techniques for the first time. The preferred guest-ion storage sites and migration mechanism were systematically analysed through theoretical calculations. We believe these results could inspire the design of safe with high energy density.

7.
Angew Chem Int Ed Engl ; 62(51): e202314456, 2023 Dec 18.
Artigo em Inglês | MEDLINE | ID: mdl-37929923

RESUMO

The parasitic side reaction on Zn anode is the key issue which hinders the development of aqueous Zn-based energy storage systems on power-grid applications. Here, a polymer additive (PMCNA) engineered by copolymerizing 2-methacryloyloxyethyl phosphorylcholine (MPC) and N-acryloyl glycinamide (NAGA) was employed to regulate the Zn deposition environment for satisfying side reaction inhibition performance during long-term cycling with high Zn utilization. The PMCNA can preferentially adsorb on Zn metal surface to form a uniform protective layer for effective water molecule repelling and side reaction resistance. In addition, the PMCNA can guide Zn nucleation and deposition along 002 plane for further side reaction and dendrite suppression. Consequently, the PMCNA additive can enable the Zn//Zn battery with an ultrahigh depth of discharge (DOD) of 90.0 % for over 420 h, the Zn//active carbon (AC) capacitor with long cycling lifespan, and the Zn//PANI battery with Zn utilization of 51.3 % at low N/P ratio of 2.6.

8.
Small ; 18(22): e2201443, 2022 06.
Artigo em Inglês | MEDLINE | ID: mdl-35502124

RESUMO

Some new insights into traditional metal pretreatment of anticorrosion for high stable Zn metal anodes are provided. A developed pretreatment methodology is employed to prefer the crystal plane of polycrystalline Zn and create 3.26 µm protective coatings mainly consisting of organic polymers and zinc salts on Zn foils (ROZ@Zn). In this process, Zn metal exhibits a surface-preferred (001) crystal plane proved by electron backscattered diffraction. Preferred (001) crystal planes and ROZ coatings can regulate Zn2+ diffusion, promote flat growth of Zn, and prevent side reactions. As a result, ROZ@Zn symmetrical cells exhibit superior plating/stripping performance over 1300 h. Impressively, it is significantly prolonged over 40 times in comparison to the bare Zn symmetric cell at 5 mA cm-2 . Moreover, Zn//MnO2  button cells have a high capacity retention of 96.3% after 1600 cycles and pouch cells have a high capacity 122 mAh g-1  after 200 cycle at 5 C. This work provides inspiration for high stable aqueous Zn metal batteries using the developed metal pretreatment of anticorrosion, which will be a viable, low-cost, and efficient technology. More interesting, it demonstrates the availability of reconstructing crystal planes by the largely heterogeneous reaction activation of the different crystal planes to H+ .


Assuntos
Compostos de Manganês , Óxidos , Fontes de Energia Elétrica , Eletrodos , Zinco
9.
Nano Lett ; 21(16): 7021-7029, 2021 Aug 25.
Artigo em Inglês | MEDLINE | ID: mdl-34369781

RESUMO

Hydrogen ion is an attractive charge carrier for energy storage due to its smallest radius. However, hydrogen ions usually exist in the form of hydronium ion (H3O+) because of its high dehydration energy; the choice of electrode materials is thus greatly limited to open frameworks and layered structures with large ionic channels. Here, the desolvation of H3O+ is achieved by using anatase TiO2 as anodes, enabling the H+ intercalation with a strain-free characteristic. Density functional theory calculations show that the desolvation effects are dependent on the facets of anatase TiO2. Anatase TiO2 (001) surface, a highly reactive surface, impels the desolvation of H3O+ into H+. When coupled with a MnO2 cathode, the proton battery delivers a high specific energy of 143.2 Wh/kg at an ultrahigh specific power of 47.9 kW/kg. The modulation of the interactions between ions and electrodes opens new perspectives for battery optimizations.

10.
Small ; 15(36): e1902463, 2019 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-31310439

RESUMO

Hexagonal nickel-organic framework (Ni-MOF) [Ni(NO3 )2 ·6H2 O, 1,3,5-benzenetricarboxylic acid, 4-4'-bipyridine] is fabricated through a one-step solvothermal method. The {001} crystal plane is exposed to the largest hexagonal surface, which is an ideal structure for electron transport and ion diffusion. Compared with the surrounding rectangular crystal surface, the ion diffusion length through the {001} crystal plane is the shortest. In addition, the cross-linked porous mesh structures growing on the {001} crystal plane strengthen the mixing with conductive carbon, inducing preferable conductivity, as well as increasing the area of ion contact and the number of active sites. These advantages enable the hexagonal Ni-MOF to exhibit excellent electrochemical performance as supercapacitor electrode materials. In a three-electrode cell, specific capacitance of hexagonal Ni-MOF in the 3.0 m KOH electrolyte is 977.04 F g-1 and remains at the initial value of 92.34% after 5,000 cycles. When the hexagonal Ni-MOF and activated carbon are assembled into aqueous devices, the electrochemical performance remains effective.

11.
J Colloid Interface Sci ; 667: 44-53, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38615622

RESUMO

The construction of high-asymmetrical structures demonstrates significant potential in improving the functionality and distinctness of nanomaterials, but remains a considerable challenge. Herein, we develop a one-pot method to fabricate regioselective super-assembly of Prussian blue analogue (PBA) -- a PBA anisotropic structure (PBA-AS) decorated with epitaxial modules--using a step-by-step epitaxial growth on a rapidly self-assembled cubic substrate guided by thiocyanuric acid (TCA) molecules. The epitaxial growth units manifest as diverse geometric shapes, which are predominantly concentrated on the {100}, {111}, or {100}+{111} crystal plane of the cubic substrate. The crystal plane and morphology of epitaxial module can be regulated by changing the TCA concentration and reaction temperature, enabling a high level of controllability over specific assembly sites and structures. To illustrate the advantage of the asymmetrical structure, phosphated PBA-AS demonstrates improved performance in the oxygen evolution reaction compared to simple phosphated PBA nanocube. This method offers valuable insights for designing asymmetrical nanomaterials with intricate architectures and versatile functionalities.

12.
J Colloid Interface Sci ; 673: 346-353, 2024 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-38878369

RESUMO

Employing electric energy to convert carbon dioxide (CO2) into valuable small molecules is a potentially practical method in energy storage and greenhouse gas alleviation. A huge challenge for electrocatalytic CO2 reduction is to reduce overpotential to improve energy efficiency. Herein, we demonstrate that doping alloy Pd49Ag30Te4 (PAT) with rare-earth element Tb is beneficial for selective exposure of (111) crystal plane, which is a highly active crystal plane for producing carbon monoxide (CO). The as-prepared Tb2.9PAT exhibited high electrocatalytic performance with 95.7 % CO faradic efficiency at - 0.8 V (vs RHE), far exceeding that of PAT, and coupled with good durability. In situ spectral study and theoretical calculations disclose that the introduction of Tb regulates the d-band center of PAT alloy, weakens the Pd - C bonding ability, and promotes the desorption of *CO in the rate-determining step. This study provides a method for doping induced selective exposure of crystal face, which provides new idea for improving catalytic performance.

13.
Sci Rep ; 14(1): 6260, 2024 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-38491074

RESUMO

The α-calcium sulfate hemihydrate whiskers (α-CSHWs) were first prepared using phosphogypsum (PG) and electrolytic manganese residue (EMR) as raw materials for coating urea, demonstrating excellent controlled-release properties. The effects of different reaction conditions on α-CSHWs, achieved by optimizing the reaction time, the concentrations of NH4+, Mn2+, and other factors, were discussed. Results showed that when the EMR content was 25 wt%, the reaction temperature was 100 °C, and the reaction time was 3 h, α-CSHWs with a length-to-diameter ratio of 39 were obtained. Through experiments and density functional theory (DFT), the mechanism of α-CSHWs preparation was elucidated. The results show that the addition of EMR reduces the content of impurity ions PO43- and F- in PG while introducing NH4+ and Mn2+. Interestingly, both NH4+ and Mn2+ can reduce the nucleation time of α-CSHWs, while PO43-, Mn2+, and F- are more likely to adsorb on the (0 0 6) crystal plane of α-CSHWs, NH4+ readily adsorbs on the (4 0 0) crystal plane. The controlled-release performance of modified α-CSHWs incorporated into polyurethane-coated urea (PCU) was investigated, and it was found that the addition of Mα significantly prolonged the nutrient release period, with the period extending up to 116 days for coatings of 5wt% and above. This work not only enhances the efficiency of PG and EMR utilization but also serves as a reference for the straightforward synthesis and application of α-CSHWs.

14.
Nanomaterials (Basel) ; 14(13)2024 Jun 22.
Artigo em Inglês | MEDLINE | ID: mdl-38998676

RESUMO

The efficient separation of photogenerated charge carriers and strong oxidizing properties can improve photocatalytic performance. Here, we combine the construction of a tightly connected S-scheme heterojunction with the exposure of an active crystal plane to prepare g-C3N4/BiOBr for the degradation of high-concentration organic pollutants. This strategy effectively improves the separation efficiency of photogenerated carriers and the number of active sites. Notably, the synthesized g-C3N4/BiOBr displays excellent photocatalytic degradation activity towards various organic pollutants, including methylene blue (MB, 90.8%), congo red (CR, 99.2%), and tetracycline (TC, 89%). Furthermore, the photocatalytic degradation performance of g-C3N4/BiOBr for MB maintains 80% efficiency under natural water quality (tap water, lake water, river water), and a wide pH range (pH = 4-10). Its excellent photocatalytic activity is attributed to the tight connection between g-C3N4 and BiOBr in the S-scheme heterojunction interface, as well as the exposure of highly active (001) crystal planes. These improve the efficiency of the separation of photogenerated carriers, and maintain their strong oxidation capability. This work presents a simple approach to improving the separation of electrons and holes by tightly combining two components within a heterojunction.

15.
ACS Appl Mater Interfaces ; 16(27): 35143-35154, 2024 Jul 10.
Artigo em Inglês | MEDLINE | ID: mdl-38943565

RESUMO

Presently, realizing high ethanol selectivity in CO2 electroreduction remains challenging due to difficult C-C coupling and fierce product competition. In this work, we report an innovative approach for improving the efficiency of Cu-based electrocatalysts in ethanol generation from electrocatalytic CO2 reduction using a crystal plane modification strategy. These novel Cu-based electrocatalysts were fabricated by electrochemically activating three-dimensional (3D) flower-like CuO micro/nanostructures grown in situ on copper foils and modifying with surfactants. It was demonstrated that the fabricated Cu-based electrocatalyst featured a predominantly exposed Cu(100) surface loaded with high-density Cu nanoparticles (NPs). The optimal Cu-based electrocatalyst displayed considerably improved CO2 electroreduction performance, with a Faraday efficiency of 37.9% for ethanol and a maximum Faraday efficiency of 68.0% for C2+ products at -1.4 V vs RHE in an H-cell, accompanied by a high current density of 69.9 mA·cm-2, much better than the particulate Cu-based electrocatalyst. It was unveiled that the Cu(100)-rich surface of nanoscale petals with abundant under-coordinated copper atoms from CuNPs was conducive to the formation and stabilization of key *CH3CHO and *OC2H5 intermediates, thereby promoting ethanol generation. This study highlighted the critical role of CuNP-loaded Cu(100) surface structures on structured Cu-based electrocatalysts in enhancing ethanol production for the CO2 electroreduction process.

16.
ACS Nano ; 2024 Feb 05.
Artigo em Inglês | MEDLINE | ID: mdl-38315444

RESUMO

Correlating the microscopic structural characteristics with the macroscopic electrochemical performance in electrode materials is critical for developing excellent-performance lithium-ion batteries, which however remains largely unexplored. Here, we show that the Zn2SnO4 (ZTO) nanowires (NWs) with smaller diameters (d < 5 nm) exhibit slower capacity fade rate and better cycling stability, as compared with the NWs with larger diameters ranging from tens to hundreds of nanometers. By applying in situ transmission electron microscopy (TEM), we discover a strong correlation of cracking behavior with the NW diameter. Upon the first lithiation, there exists a critical diameter of ∼80 nm, below which the NWs neither crack nor fracture, and above which the cracks could easily nucleate and propagate along the specific planes, resulting in the deteriorated cycling stability in larger sized electrodes. Further theoretical calculations based on the finite element model and the climbing image nudged elastic band method faithfully predict the size-dependent cracking behaviors, which may result from the synergistic effect of axial stress evolution as well as preferential Li-ion migration directions during the first lithiation. This work provides a real-time tracking of the tempo-spatial structural evolution of a single ZTO NW, which facilitates a fundamental understanding of how the sample size affects the electrochemical behavior and thus offers a reference for future battery design and application strategy.

17.
J Colloid Interface Sci ; 650(Pt B): 1003-1012, 2023 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-37459724

RESUMO

Geologic carbon sequestration (GCS) via injecting CO2 into deep carbonate reservoirs (mainly calcite and dolomite) is a promising strategy to reduce CO2 level. However, the dissolution or precipitation of calcite/dolomite planes on minerals/solution interface during long-term GCS process develops intergranular porosity and thus affects the permeability and stability of reservoirs. To investigate this process, both calcite and dolomite were dissolved in acetic and carbonic acids. A diffusion-controlled process was identified, with greater diffusion rates in acetic acid than that in carbonic acid. Quantified planes activity of both minerals follows (110) > (116) > (101) > (113) > (018) > (104) through density functional theory. Accomplished with preferential dissolution of calcite (110) planes in carbonic acid, calcite crystals precipitated with (104) planes at 423.15 K, under which, more calcite crystals were observed on dolomite surface, producing Ca-deplete surface. Molecular dynamic calculations showed higher dissolution rates of calcite/dolomite (110) planes than (104). In addition, the dissolution coefficients of Ca2+ were approximately triple of that Mg2+. Therefore, this study reveals the interface dissolution mechanisms of calcite and dolomite, especially on (110) and (104) planes at an atomic level, for the first time, providing better understanding for the stability of long-term GCS process.

18.
Materials (Basel) ; 16(20)2023 Oct 16.
Artigo em Inglês | MEDLINE | ID: mdl-37895686

RESUMO

Feldspar is a high-abundance mineral in the earth's crust, and its natural weathering and dissolution processes are an important phenomenon on the earth's surface. This study focused on the dissolution behavior of silicon (Si) and aluminum (Al) in feldspar minerals (microcline and albite) when exposed to low-molecular-weight organic acids (LMWOAs). Various analytical techniques, including atomic absorption spectrophotometer, X-ray diffraction, scanning electron microscope, and Fourier-transform infrared spectroscopy, were employed to investigate these processes. The results revealed that the concentration of Si and Al released from alkali feldspar increased after treatment with LMWOAs, exhibiting non-stoichiometric dissolution. The Si/Al release ratio from feldspar deviated from the expected value of three. Among the LMWOAs tested, oxalic acid was found to be more effective in dissolving aluminum, while citric acid showed greater efficacy in dissolving silicon. Notably, the composite acid demonstrated the highest capacity for feldspar dissolution, with values of 538 µM (Si) and 287 µM (Al) after treatment for 720 h, respectively. The dissolution data for Si and Al in the organic acid solution was fittingly described by a first-order equation, with high correlation coefficients (R2 ≥ 0.992). The characterization of feldspar powders indicated that the (040) crystal plane of feldspar was particularly susceptible to attack by organic acids. In the presence of these acids, the chemical bonds Si (Al)-O, Si-Si(Al), and O-Si(Al)-O shifted to higher wavenumbers. Additionally, the surface corrosion morphology of feldspar exhibited distinct nanostructures, which became more pronounced with increasing exposure time. It was also observed that the reactivity of feldspar increased over time. These findings provide valuable insights into the natural dissolution process of feldspar and offer a new perspective for the study of this phenomenon.

19.
Environ Sci Pollut Res Int ; 30(30): 76143-76156, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-37231133

RESUMO

In order to avoid the high cost of existing precious metal catalyst like Pt, Ag/CeO2 was the most promising catalysts for mobile source soot emission control technologies, but there was a clear trade-off between hydrothermal aging resistance and catalytic oxidation performance hindered the application of this catalyst. In order to reveal the hydrothermal aging mechanism of Ag/CeO2 catalysts, the TGA (thermogravimetric analysis) experiments were investigated to reveal the mechanism of Ag modification on catalytic activity of CeO2 catalyst between fresh and hydrothermal aging and were also characterized with the related characterization experiments to in-depth research the lattice morphology and valence changes. The degradation mechanism of Ag/CeO2 catalysts in vapor with high-temperature was also explained and demonstrated based on density functional and molecular thermodynamics theories. The experimental and simulation data showed that the catalytic activity of soot combustion within Ag/CeO2 decreased more significantly after hydrothermal aging than CeO2 due to the less agglomerated, which caused by the decreased in OII/OI and Ce3+/Ce4+ compared with CeO2. As shown in density function theory (DFT) calculation, the decreased surface energy and the increased oxygen vacancy formation energy of the low Mille index surface after Ag modification led to the instability structure and the high catalytic activity. Ag modification also increased the adsorption energy and Gibbs free energy of H2O on the low Miller index surface compared to CeO2, indicating that the desorption temperature of H2O molecules in (1 1 0) and (1 0 0) was higher than (1 1 1) in CeO2 and Ag/CeO2, which led to the migration of (1 1 1) crystal surfaces to (1 1 0) and (1 0 0) in the vapor environment. These conclusions can provide a valuable addition to the regenerative application of Ce-based catalysts in diesel exhaust aftertreatment system the aerial pollution.


Assuntos
Cério , Fuligem , Fuligem/química , Teoria da Densidade Funcional , Cério/química , Oxirredução , Emissões de Veículos , Poeira
20.
ACS Appl Mater Interfaces ; 15(9): 12061-12069, 2023 Mar 08.
Artigo em Inglês | MEDLINE | ID: mdl-36848237

RESUMO

PbS colloidal quantum dot (CQD) infrared photodiodes have attracted wide attention due to the prospect of developing cost-effective infrared imaging technology. Presently, ZnO films are widely used as the electron transport layer (ETL) of PbS CQDs infrared photodiodes. However, ZnO-based devices still suffer from the problems of large dark current and low repeatability, which are caused by the low crystallinity and sensitive surface of ZnO films. Here, we effectively optimized the device performance of PbS CQDs infrared photodiode via diminishing the influence of adsorbed H2O at the ZnO/PbS CQDs interface. The polar (002) ZnO crystal plane showed much higher adsorption energy of H2O molecules compared with other nonpolar planes, which could reduce the interface defects induced by detrimentally adsorbed H2O. Based on the sputtering method, we obtained the [002]-oriented and high-crystallinity ZnO ETL and effectively suppressed the adsorption of detrimental H2O molecules. The prepared PbS CQDs infrared photodiode with the sputtered ZnO ETL demonstrated lower dark current density, higher external quantum efficiency, and faster photoresponse compared with the sol-gel ZnO device. Simulation results further unveiled the relationship between interface defects and device dark current. Finally, a high-performance sputtered ZnO/PbS CQDs device was obtained with a specific detectivity of 2.15 × 1012 Jones at -3 dB bandwidth (94.6 kHz).

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