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1.
MXene, a new class of 2D materials, has gained significant attention owing to its attractive electrical conductivity, tunable work function, and metallic nature for wide range of applications. Herein, delaminated few layered Ti3C2Tx MXene contacted Si solar cells with a maximum power conversion efficiency (PCE) of ≈11.5% under AM1.5G illumination are demonstrated. The formation of an Ohmic junction of the metallic MXene to n+‐Si surface efficiently extracts the photogenerated electrons from n+np+‐Si, decreases the contact resistance, and suppresses the charge carrier recombination, giving rise to excellent open‐circuit voltage and short‐circuit current density. The rapid thermal annealing process further improves the electrical contact between Ti3C2Tx MXene and n+‐Si surface by reducing sheet resistance, increasing electrical conductivity, and decreasing cell series resistance, thus leading to a remarkable improvement in fill factor and overall PCE. The work demonstrated here can be extended to other MXene compositions as potential electrodes for developing highly performing solar cells.  相似文献   

2.
To achieve the energy‐effective ammonia (NH3) production via the ambient‐condition electrochemical N2 reduction reaction (NRR), it is vital to ingeniously design an efficient electrocatalyst assembling the features of abundant surface deficiency, good dispersibility, high conductivity, and large surface specific area (SSA) via a simple way. Inspired by the fact that the MXene contains thermodynamically metastable marginal transition metal atoms, the oxygen‐vacancy‐rich TiO2 nanoparticles (NPs) in situ grown on the Ti3C2Tx nanosheets (TiO2/Ti3C2Tx) are prepared via a one‐step ethanol‐thermal treatment of the Ti3C2Tx MXene. The oxygen vacancies act as the main active sites for the NH3 synthesis. The highly conductive interior untreated Ti3C2Tx nanosheets could not only facilitate the electron transport but also avoid the self‐aggregation of the TiO2 NPs. Meanwhile, the TiO2 NPs generation could enhance the SSA of the Ti3C2Tx in return. Accordingly, the as‐prepared electrocatalyst exhibits an NH3 yield of 32.17 µg h?1 mg?1cat. at ?0.55 V versus reversible hydrogen electrode (RHE) and a remarkable Faradaic efficiency of 16.07% at ?0.45 V versus RHE in 0.1 m HCl, placing it as one of the most promising NRR electrocatalysts. Moreover, the density functional theory calculations confirm the lowest NRR energy barrier (0.40 eV) of TiO2 (101)/Ti3C2Tx compared with Ti3C2Tx or TiO2 (101) alone.  相似文献   

3.
To enable an efficient and cost‐effective electrocatalytic N2 reduction reaction (NRR) the development of an electrocatalyst with a high NH3 yield and good selectivity is required. In this work, Ti3C2Tx MXene‐derived quantum dots (Ti3C2Tx QDs) with abundant active sites enable the development of efficient NRR electrocatalysts. Given surface functional groups play a key role on the electrocatalytic performance, density functional theory calculations are first conducted, clarifying that hydroxyl groups on Ti3C2Tx offer excellent NRR activity. Accordingly, hydroxyl‐rich Ti3C2Tx QDs (Ti3C2OH QDs) are synthesized as NRR catalysts by alkalization and intercalation. This material offers an NH3 yield and Faradaic efficiency of 62.94 µg h?1 mg?1cat. and 13.30% at ?0.50 V, respectively, remarkably higher than reported MXene catalysts. This work demonstrates that MXene catalysts can be mediated through the optimization of both QDs sizes and functional groups for efficient ammonia production at room temperature.  相似文献   

4.
Pseudocapacitance is a key charge storage mechanism to advanced electrochemical energy storage devices distinguished by the simultaneous achievement of high capacitance and a high charge/discharge rate by using surface redox chemistries. MXene, a family of layered compounds, is a pseudocapacitor‐like electrode material which exhibits charge storage through exceptionally fast ion accessibility to redox sites. Here, the authors demonstrate steric chloride termination in MXene Ti2CTx (Tx : surface termination groups) to open the interlayer space between the individual 2D Ti2CTx units. The open interlayer space significantly enhances Li‐ion accessibility, leading to high gravimetric and volumetric capacitances (300 F g?1 and 130 F cm?3) with less diffusion limitation. A Li‐ion hybrid capacitor consisting of the Ti2CTx negative electrode and the LiNi1/3Co1/3Mn1/3O2 positive electrode displays an unprecedented specific energy density of 160 W h kg?1 at 220 W kg?1 based on the total weight of positive and negative active materials.  相似文献   

5.
Supercapacitors attract great interest because of the increasing and urgent demand for environment‐friendly high‐power energy sources. Ti3C2, a member of MXene family, is a promising electrode material for supercapacitors owing to its excellent chemical and physical properties. However, the highest gravimetric capacitance of the MXene‐based electrodes is still relatively low (245 F g?1) and the key challenge to improve this is to exploit more pseudocapacitance by increasing the active site concentration. Here, a method to significantly improve the gravimetric capacitance of Ti3C2Tx MXenes by cation intercalation and surface modification is reported. After K+ intercalation and terminal groups (OH?/F?) removing , the intercalation pseudocapacitance is three times higher than the pristine MXene, and MXene sheets exhibit a significant enhancement (about 211% of the origin) in the gravimetric capacitance (517 F g?1 at a discharge rate of 1 A g?1). Moreover, the as‐prepared electrodes show above 99% retention over 10 000 cycles. This improved electrochemical performance is attributed to the large interlayer voids of Ti3C2 and lowest terminated surface group concentration. This study demonstrates a new strategy applicable to other MXenes (Ti2CTx , Nb2CTx , etc.) in maximizing their potential applications in energy storage.  相似文献   

6.
The detrimental shuttle effect in lithium–sulfur batteries mainly results from the mobility of soluble polysulfide intermediates and their sluggish conversion kinetics. Herein, presented is a multifunctional catalyst with the merits of strong polysulfides adsorption ability, superior polysulfides conversion activity, high specific surface area, and electron conductivity by in situ crafting of the TiO2‐MXene (Ti3C2Tx) heterostructures. The uniformly distributed TiO2 on MXene sheets act as capturing centers to immobilize polysulfides, the hetero‐interface ensures rapid diffusion of anchored polysulfides from TiO2 to MXene, and the oxygen‐terminated MXene surface is endowed with high catalytic activity toward polysulfide conversion. The improved lithium–sulfur batteries deliver 800 mAh g?1 at 2 C and an ultralow capacity decay of 0.028% per cycle over 1000 cycles at 2 C. Even with a high sulfur loading of 5.1 mg cm?2, the capacity retention of 93% after 200 cycles is still maintained. This work sheds new insights into the design of high‐performance catalysts with manipulated chemical components and tailored surface chemistry to regulate polysulfides in Li–S batteries.  相似文献   

7.
Silicon is attracting enormous attention due to its theoretical capacity of 4200 mAh g?1 as an anode for Li‐ion batteries (LIBs). It is of fundamental importance and challenge to develop low‐temperature reaction route to controllably synthesize Si/Ti3C2 MXene LIBs anodes. Herein, a novel and efficient strategy integrating in situ orthosilicate hydrolysis and a low‐temperature reduction process to synthesize Si/Ti3C2 MXene composites is reported. The hydrolysis of tetraethyl orthosilicate leads to homogenous nucleation and growth of SiO2 nanoparticles on the surface of Ti3C2 MXene. Subsequently, SiO2 nanoparticles are reduced to Si via a low‐temperature (200 °C) reduction route. Importantly, Ti3C2 MXene not only provides fast transfer channels for Li+ and electrons, but also relieves volume expansion of Si during cycling. Moreover, the characteristics of excellent pseudocapacitive performance and high conductivity of Ti3C2 MXene can synergistically contribute to the enhancement of energy storage performance. As expected, Ti3C2/Si anode exhibits an outstanding specific capacity of 1849 mAh g?1 at 100 mA g?1, even retaining 956 mAh g?1 at 1 A g?1. The low‐temperature synthetic route to Si/Ti3C2 MXene electrodes and involved battery‐capacitive dual‐model energy storage mechanism has potential in the design of novel high‐performance electrodes for energy storage devices.  相似文献   

8.
Although 2D Ti3C2Tx is a good candidate for supercapacitors, the restacking of nanosheets hinders the ion transport significantly at high scan rates, especially under practical mass loading (>10 mg cm?2) and thickness (tens of microns). Here, Ti3C2Tx‐NbN hybrid film is designed by self‐assembling Ti3C2Tx with 2D arrays of NbN nanocrystals. Working as an interlayer spacer of Ti3C2Tx, NbN facilitates the ion penetration through its 2D porous structure; even at extremely high scan rates. The hybrid film shows a thickness‐independent rate performance (almost the same rate capabilities from 2 to 20 000 mV s?1) for 3 and 50 µm thick electrodes. Even a 109 µm thick Ti3C2Tx‐NbN electrode shows a better rate performance than 25 µm thick pure Ti3C2Tx electrodes. This method may pave a way to controlling ion transport in electrodes composed of 2D conductive materials, which have potential applications in high‐rate energy storage and beyond.  相似文献   

9.
2D transition metal carbides and nitrides, known as MXenes, are an emerging class of 2D materials with a wide spectrum of potential applications, in particular in electrochemical energy storage. The hydrophilicity of MXenes combined with their metallic conductivity and surface redox reactions is the key for high‐rate pseudocapacitive energy storage in MXene electrodes. However, symmetric MXene supercapacitors have a limited voltage window of around 0.6 V due to possible oxidation at high anodic potentials. In this study, the fact that titanium carbide MXene (Ti3C2Tx) can operate at negative potentials in acidic electrolyte is exploited, to design an all‐pseudocapacitive asymmetric device by combining it with a ruthenium oxide (RuO2) positive electrode. This asymmetric device operates at a voltage window of 1.5 V, which is about two times wider than the operating voltage window of symmetric MXene supercapacitors, and is the widest voltage window reported to date for MXene‐based supercapacitors. The complementary working potential windows of MXene and RuO2, along with proton‐induced pseudocapacitance, significantly enhance the device performance. As a result, the asymmetric devices can deliver an energy density of 37 µW h cm?2 at a power density of 40 mW cm?2, with 86% capacitance retention after 20 000 charge–discharge cycles. These results show that pseudocapacitive negative MXene electrodes can potentially replace carbon‐based materials in asymmetric electrochemical capacitors, leading to an increased energy density.  相似文献   

10.
Selenium (Se), due to its high electronic conductivity and high energy density, has recently attracted considerable interest as a cathode material for rechargeable Li/Na batteries. However, the poor cycling stability originating from the severe shuttle effect of polyselenides hinders their practical applications. Herein, highly stable Li/Na–Se batteries are developed using ultrathin (≈270 nm, loading of 0.09 mg cm?2) cetrimonium bromide (CTAB)/carbon nanotube (CNT)/Ti3C2Tx MXene hybrid modified polypropylene (PP) (CCNT/MXene/PP) separators. The hybrid separator can immobilize the polyselenides via enhanced Lewis acid–base interactions between CTAB/MXene and polyselenides, which is demonstrated by theoretical calculations and X‐ray photoelectron spectroscopy. The incorporation of CNT helps to improve the electrolyte infiltration and facilitate the ionic transport. In situ permeation experiments are conducted for the first time to visually study the behavior of polyselenides, revealing the prohibited shuttle effect and protected Li anode from corrosion with CCNT/MXene/PP separators. As a result, the Li–Se batteries with CCNT/MXene/PP separators deliver an outstanding cycling performance over 500 cycles at 1C with an extremely low capacity decay of 0.05% per cycle. Moreover, the hybrid separators also perform well in Na–Se batteries. This study develops a preferable separator–electrolyte interface and the concept can be applied in other conversion‐type battery systems.  相似文献   

11.
A simple and scalable direct laser machining process to fabricate MXene‐on‐paper coplanar microsupercapacitors is reported. Commercially available printing paper is employed as a platform in order to coat either hydrofluoric acid‐etched or clay‐like 2D Ti3C2 MXene sheets, followed by laser machining to fabricate thick‐film MXene coplanar electrodes over a large area. The size, morphology, and conductivity of the 2D MXene sheets are found to strongly affect the electrochemical performance due to the efficiency of the ion‐electron kinetics within the layered MXene sheets. The areal performance metrics of Ti3C2 MXene‐on‐paper microsupercapacitors show very competitive power‐energy densities, comparable to the reported state‐of‐the‐art paper‐based microsupercapacitors. Various device architectures are fabricated using the MXene‐on‐paper electrodes and successfully demonstrated as a micropower source for light emitting diodes. The MXene‐on‐paper electrodes show promise for flexible on‐paper energy storage devices.  相似文献   

12.
Oxygen‐containing compounds are promising thermoelectric (TE) materials for their chemical and thermal stability. As compared with the high‐performance p‐type counterparts (e.g., ZT ≈1.5 for BiCuSeO), the enhancement of the TE performance of n‐type oxygen‐containing materials remains challenging due to their mediocre electrical conductivity and high thermal conductivity. Here, n‐type layered Bi2O2Se is reported as a potential TE material, of which the thermal conductivity and electrical transport properties can be effectively tuned via carrier engineering and hierarchical microstructure. By selective modification of insulating [Bi2O2]2+ layers with Ta dopant, carrier concentration can be increased by four orders of magnitude (from 1015 to 1019 cm?3) while relatively high carrier mobility can be maintained, thus greatly enhancing the power factors (≈451.5 µW K?2 m?1). Meanwhile, the hierarchical microstructure can be induced by Ta doping, and the phonon scattering can be strengthened by atomic point defects, nanodots of 5–10 nm and grains of sub‐micrometer level, which progressively suppresses the lattice thermal conductivity. Accordingly, the ZT value of Bi1.90Ta0.10O2Se reaches 0.36 at 773 K, a ≈350% improvement in comparison with that of the pristine Bi2O2Se. The average ZT value of 0.30 from 500 to 823 K is outstanding among n‐type oxygen‐containing TE materials. This work provides a desirable way for enhancing the ZT values in oxygen‐containing compounds.  相似文献   

13.
2D materials are of particular interest in light‐to‐heat conversion, yet challenges remain in developing a facile method to suppress their light reflection. Herein, inspired by the black scales of Bitis rhinoceros, a generalized approach via sequential thermal actuations to construct biomimetic 2D‐material nanocoatings, including Ti3C2Tx MXene, reduced graphene oxide (rGO), and molybdenum disulfide (MoS2) is designed. The hierarchical MXene nanocoatings result in broadband light absorption (up to 93.2%), theoretically validated by optical modeling and simulations, and realize improved light‐to‐heat performance (equilibrium temperature of 65.4 °C under one‐sun illumination). With efficient light‐to‐heat conversion, the bioinspired MXene nanocoatings are next incorporated into solar steam‐generation devices and stretchable solar/electric dual‐heaters. The MXene steam‐generation devices require much lower solar‐thermal material loading (0.32 mg cm?2) and still guarantee high steam‐generation performance (1.33 kg m?2 h?1) compared with other state‐of‐the‐art devices. Additionally, the mechanically deformed MXene structures enable the fabrication of stretchable and wearable heaters dual‐powered by sunlight and electricity, which are reversibly stretched and heated above 100 °C. This simple fabrication process with effective utilization of active materials promises its practical application value for multiple solar–thermal technologies.  相似文献   

14.
Fast ion adsorption processes in supercapacitors enable quick storage/delivery of significant amounts of energy, while ion intercalation in battery materials leads to even larger amounts of energy stored, but at substantially lower rates due to diffusional limitations. Intercalation of ions into the recently discovered 2D Ti3C2Tx (MXene) occurs with a very high rate and leads to high capacitance, posing a paradox. Herein, by characterizing the mechanical deformations of MXene electrode materials at various states‐of‐charge with a variety of cations (Li, Na, K, Cs, Mg, Ca, Ba, and three tetra­alkylammonium cations) during cycling by electrochemical quartz‐crystal admittance (EQCA, quartz‐crystal microbalance with dissipation monitoring) combined with in situ electronic conductance and electrochemical impedance, light is shone on this paradox. Based on this work, it appears that the capacitive paradox stems from cationic insertion, accompanied by significant deformation of the MXene particles, that occurs so rapidly so as to resemble 2D ion adsorption at solid‐liquid interfaces. The latter is greatly facilitated by the presence of water molecules between the MXene sheets.  相似文献   

15.
Based on the best peak theromoelectric figure‐of‐merit value (ZT) of ca. 0.8 in Hf0.5Zr0.5CoSb0.8Sn0.2 and ca. 1 in Hf0.8Ti0.2CoSb0.8Sn0.2, the effect of Ti on thermoelectric properties is studied in (Hf, Zr, Ti)CoSb0.8Sn0.2, with the aim of further improving the ZT and reducing the usage of Hf. By either partial replacement of Hf and Zr with Ti in Hf0.5Zr0.5CoSb0.8Sn0.2 or partial replacement of Hf and Ti with Zr in Hf0.8Ti0.2CoSb0.8Sn0.2, a peak ZT of ≥1 is achieved at 800°C in Hf0.44Zr0.44Ti0.12CoSb0.8Sn0.2. This composition has two advantages over the previous two best compositions: higher ZT than Hf0.5Zr0.5CoSb0.8Sn0.2 and less Hf than in Hf0.8Ti0.2CoSb0.8Sn0.2. A higher ZT with less Hf is very much desired since Hf is much more expensive than other constituent elements. The ZT improvement is the result of thermal conductivity reduction due to phonon scattering by both alloy and the nanostructure effect.  相似文献   

16.
NbFeSb‐based half‐Heusler alloys have been recently identified as promising high‐temperature thermoelectric materials with a figure of merit zT > 1, but their thermal conductivity is still relatively high. Alloying Ta at the Nb site would be highly desirable because the large mass fluctuation between them could effectively scatter phonons and reduce the lattice thermal conductivity. However, practically it is a great challenge due to the high melting point of refractory Ta. Here, the successful synthesis of Ta‐alloyed (Nb1?xTax)0.8Ti0.2FeSb (x = 0 – 0.4) solid solutions with significantly reduced thermal conductivity by levitation melting is reported. Because of the similar atomic sizes and chemistry of Nb and Ta, the solid solutions exhibit almost unaltered electrical properties. As a result, an overall zT enhancement from 300 to 1200 K is realized in the single‐phase Ta‐alloyed solid solutions, and the compounds with x = 0.36 and 0.4 reach a maximum zT of 1.6 at 1200 K. This work also highlights that the isoelectronic substitution by atoms with similar size and chemical nature but large mass difference should reduce the lattice thermal conductivity but maintain good electrical properties in thermoelectric materials, which can be a guide for optimizing the figure of merit by alloying.  相似文献   

17.
A step‐by‐step strategy is reported for improving capacitance of supercapacitor electrodes by synthesizing nitrogen‐doped 2D Ti2CTx induced by polymeric carbon nitride (p‐C3N4), which simultaneously acts as a nitrogen source and intercalant. The NH2CN (cyanamide) can form p‐C3N4 on the surface of Ti2CTx nanosheets by a condensation reaction at 500–700 °C. The p‐C3N4 and Ti2CTx complexes are then heat‐treated to obtain nitrogen‐doped Ti2CTx nanosheets. The triazine‐based p‐C3N4 decomposes above 700 °C; thus, the nitrogen species can be surely doped into the internal carbon layer and/or defect site of Ti2CTx nanosheets at 900 °C. The extended interlayer distance and c‐lattice parameters (c‐LPs of 28.66 Å) of Ti2CTx prove that the p‐C3N4 grown between layers delaminate the nanosheets of Ti2CTx during the doping process. Moreover, 15.48% nitrogen doping in Ti2CTx improves the electrochemical performance and energy storage ability. Due to the synergetic effect of delaminated structures and heteroatom compositions, N‐doped Ti2CTx shows excellent characteristics as an electrochemical capacitor electrode, such as perfectly rectangular cyclic voltammetry results (CVs, R2 = 0.9999), high capacitance (327 F g?1 at 1 A g?1, increased by ≈140% over pristine‐Ti2CTx), and stable long cyclic performance (96.2% capacitance retention after 5000 cycles) at high current density (5 A g?1).  相似文献   

18.
The thermoelectric properties of crystalline melt‐grown ingots of p‐type PbTe–xMgTe (x = 1–3 mol%) doped with Na2Te (1–2 mol%) were investigated over the temperature range of 300 K to 810 K. While the powder X‐ray diffraction patterns show that all samples crystallize in the NaCl‐type structure with no MgTe or other phases present, transmission electron microscopy reveals ubiquitous MgTe nanoprecipitates in the PbTe. The very small amounts of MgTe in PbTe have only a small effect on the electrical transport properties of the system, while they have a large effect on thermal transport significantly reducing the lattice thermal conductivity. A ZT of 1.6 at 780 K is achieved for the PbTe containing 2% MgTe doped with 2% Na2Te.  相似文献   

19.
The layered oxyselenide BiCuSeO system is known as one of the high‐performance thermoelectric materials with intrinsically low thermal conductivity. By employing atomic, nano‐ to mesoscale structural optimizations, low thermal conductivity coupled with enhanced electrical transport properties can be readily achieved. Upon partial substitution of Bi3+ by Ca2+ and Pb2+, the thermal conductivity can be reduced to as low as 0.5 W m?1 K?1 at 873 K through dual‐atomic point‐defect scattering, while a high power factor of ≈1 × 10?3 W cm?1 K?2 is realized over a broad temperature range from 300 to 873 K. The synergistically optimized power factor and intrinsically low thermal conductivity result in a high ZT value of ≈1.5 at 873 K for Bi0.88Ca0.06Pb0.06CuSeO, a promising candidate for high‐temperature thermoelectric applications. It is envisioned that the all‐scale structural optimization is critical for optimizing the thermoelectricity of quaternary compounds.  相似文献   

20.
AgPbmSbTem+2 (abbreviated as LAST) has received tremendous attention as a promising thermoelectric material at medium temperature. It can be synthesized by a simple process combining mechanical alloying (MA) and spark plasma sintering (SPS). This work reveals that the thermoelectric figure of merit (ZT value) of LAST can be increased by 50%, benefiting from enhanced electrical conductivity and thermopower due to refined grains and from nanostructuring realized by repeating the milling and SPS processes. This modified process and further compositional optimization enables ZT values of the LAST alloys up to 1.54 at 723 K. This supports the potential of the LAST alloy as a promising medium‐temperature thermoelectric material and reveals the validity of ZT enhancement by a simple microstructural refining and nanostructuring method.  相似文献   

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