Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 7 de 7
Filtrar
Mais filtros








Base de dados
Intervalo de ano de publicação
1.
Artigo em Inglês | MEDLINE | ID: mdl-38095359

RESUMO

MXenes, a class of two-dimensional materials, have garnered significant attention due to their versatile surface chemistry and customizable properties. In this study, we investigate the work function (WF) tuning capabilities of MXene Ti3C2Tx, where Tx denotes the surface termination, synthesized via both conventional hydrogen fluoride-etched and recently reported molten salt-etched routes. When MXene samples are subjected to gas phase reactions, WF variations exceeding 0.6 eV are achieved, highlighting the potential for precise WF control. Notably, the WF increases from ∼4.23 eV (in N-doped MXene etched using molten salt) to ∼4.85 eV (N-doped MXene etched using HF). Complementary density functional theory (DFT) calculations reveal WF tuning across a >1 eV range via modification of the surface with different terminal groups (bare metal, F*, O*, N*, and Cl*). These changes in WF are attributed to surface termination modifications and the formation of TiO2 and TiN phases during annealing. DFT calculations further unveil an inverse correlation between the WF and the electron affinity of surface terminations. The findings from this comprehensive study provide insights into the tunable WF of MXenes, paving the way for their potential applications as interfacial layers in photovoltaic, energy conversion, and storage technologies.

2.
Phys Chem Chem Phys ; 25(48): 33081-33093, 2023 Dec 13.
Artigo em Inglês | MEDLINE | ID: mdl-38037878

RESUMO

The work function (WF) of perovskite materials is essential for developing optoelectronic devices enabling efficient charge transfer at their interfaces. Perovskite's WF can be tuned by MXenes, a new class of two-dimensional (2D) early transition metal carbides, nitrides, and carbonitrides. Their variable surface terminations or the possibility of introducing elemental dopants could advance perovskites. However, the influence of doped-MXenes on perovskite materials is still not fully understood and elaborated. This study provides mechanistic insight into verifying the tunability of MAPbI3 WF by hybridizing with fluorine-terminated Ti3C2Tx (F-MXene) and nitrogen-doped Ti3C2Tx (N-MXene). We first reveal the interfacial interaction between MAPbI3 and MXenes via X-ray photoelectron spectroscopy (XPS), ultraviolet photoelectron spectroscopy (UPS), and photoluminescence spectroscopy (PL). UPS supported by density functional theory (DFT) calculations allowed the description of the influence of F and N on MXene's WF. Furthermore, we developed MAPbI3/MXene heterostructures using F- and N-MXenes. The F-MXenes extended the most WF of MAPbI3 from 4.50 eV up to 3.00 eV, compared to only a small shift for N-MXene. The underlying mechanism was charge transfer from low WF F-MXene to MAPbI3, as demonstrated by PL quenching in MAPbI3/F-MXene heterostructures. Altogether, this work showcases the potential of fluorine-doped MXenes over nitrogen-doped MXenes in advancing perovskite heterostructures, thus opening a door for efficient optoelectronic devices.

3.
ACS Appl Mater Interfaces ; 14(10): 12156-12167, 2022 Mar 16.
Artigo em Inglês | MEDLINE | ID: mdl-35255212

RESUMO

Two-dimensional (2D) catalysts often show extraordinary activity at low mass loading since almost all their atoms are exposed to electrolyte. Palladium (Pd) holds great promise for catalyzing oxygen reduction reaction (ORR) but 2D Pd-based ORR catalyst has rarely been reported. Herein, 2D ternary palladium phosphoronitride (Pd3P2Nx) is synthesized, for the first time, for ORR catalysis. The synthesis is guided by a rational design using first-principles density functional theory calculations, and then realized via a postsynthesis substitutional doping of ternary palladium thiophosphate (Pd3P2S8), which almost completely replaces sulfur atoms by nitrogen atoms without destroying the 2D morphology. The doping process exposes the interlocked Pd atoms of Pd3P2S8 and introduces ligands that improve the affinity of oxygen intermediates, resulting in greater kinetics and lower activation energy for ORR. The mass activity of the pristine Pd3P2S8 is dramatically increased as much as 5-fold (from 0.03 to 0.151 mA µg-1 Pd in Pd3P2Nx). The ORR diffusion-limited current density of Pd3P2Nx (6.2 mA cm-2) exceeds that of commercial Pt/C, and it shows fast kinetics and robust long-term stability. Our theoretical calculations not only guide the experimental doping process, but also provides insights into the underlying mechanism of the outstanding ORR activity and stability.

4.
Nat Commun ; 12(1): 5087, 2021 Aug 24.
Artigo em Inglês | MEDLINE | ID: mdl-34429419

RESUMO

The creation of pseudo-magnetic fields in strained graphene has emerged as a promising route to investigate intriguing physical phenomena that would be unattainable with laboratory superconducting magnets. The giant pseudo-magnetic fields observed in highly deformed graphene can substantially alter the optical properties of graphene beyond a level that can be feasible with an external magnetic field, but the experimental signatures of the influence of such pseudo-magnetic fields have yet to be unveiled. Here, using time-resolved infrared pump-probe spectroscopy, we provide unambiguous evidence for slow carrier dynamics enabled by the pseudo-magnetic fields in periodically strained graphene. Strong pseudo-magnetic fields of ~100 T created by non-uniform strain in  graphene on nanopillars are found to significantly decelerate the relaxation processes of hot carriers by more than an order of magnitude. Our findings offer alternative opportunities to harness the properties of graphene enabled by pseudo-magnetic fields for optoelectronics and condensed matter physics.

5.
Adv Sci (Weinh) ; 8(18): e2100875, 2021 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-34309229

RESUMO

Investigations on external electrostatic field (EEF)-enhanced liquid water evaporation have been reported decades ago, which suggest that molecular alignment and polarization tuned by EEF accelerating the phase change process could be responsible for EEF-enhanced water evaporation. However, a detailed study revealing the role of EEF in altering the intermolecular and intramolecular water structure is lacking. Herein, an EEF is proved to tune water state by accelerating the thermal movement of water molecules, lowering the molecular escaping energy, and loosening the hydrogen bond structure. The detailed mechanisms and field interactions (heat and electrostatic) are investigated by in situ Raman characterizations and molecular dynamic simulations, which reveal that an EEF can effectively reduce the free energy barrier of water evaporation and then increase the evaporated water molecule flux. As a proof of concept, an EEF is integrated into an interfacial two-dimentional solar steam generator, enhancing the efficiency by up to 15.6%. Similar to a catalyst lowing activation energy and enhancing kinetics of a chemical reaction, the EEF enhances water state tuning, lowers evaporation enthalpy, and then boosts steam generation rate with negligible additional energy consumption, which can serve as a generic method for water evaporation enhancement in water harvesting, purification, and beyond.

6.
Nat Commun ; 12(1): 2008, 2021 03 31.
Artigo em Inglês | MEDLINE | ID: mdl-33790295

RESUMO

Despite the tremendous progress of coupling organic electrooxidation with hydrogen generation in a hybrid electrolysis, electroreforming of raw biomass coupled to green hydrogen generation has not been reported yet due to the rigid polymeric structures of raw biomass. Herein, we electrooxidize the most abundant natural amino biopolymer chitin to acetate with over 90% yield in hybrid electrolysis. The overall energy consumption of electrolysis can be reduced by 15% due to the thermodynamically and kinetically more favorable chitin oxidation over water oxidation. In obvious contrast to small organics as the anodic reactant, the abundance of chitin endows the new oxidation reaction excellent scalability. A solar-driven electroreforming of chitin and chitin-containing shrimp shell waste is coupled to safe green hydrogen production thanks to the liquid anodic product and suppression of oxygen evolution. Our work thus demonstrates a scalable and safe process for resource upcycling and green hydrogen production for a sustainable energy future.


Assuntos
Acetatos/química , Quitina/química , Eletrólise/métodos , Hidrogênio/química , Energia Renovável , Acetatos/metabolismo , Biomassa , Quitina/metabolismo , Eletrodos , Eletrólise/instrumentação , Hidrogênio/metabolismo , Modelos Químicos , Estrutura Molecular , Oxirredução , Espectroscopia de Prótons por Ressonância Magnética , Espectrometria de Massas por Ionização e Dessorção a Laser Assistida por Matriz
7.
Nanoscale Adv ; 1(12): 4783-4789, 2019 Dec 03.
Artigo em Inglês | MEDLINE | ID: mdl-36133140

RESUMO

Exciton/trion-involved optoelectronic properties have attracted exponential amount of attention for various applications ranging from optoelectronics, valleytronics to electronics. Herein, we report a new chemical (MXene) doping strategy to modulate the negative trion and neutral exciton for achieving high photoluminescence yield of atomically thin transition metal dichalcogenides, enabled by the regulation of carrier densities to promote electron-bound trion-to-exciton transition via charge transfer from TMDCs to MXene. As a proof of concept, the MXene nano-flake-doped tungsten disulfide is demonstrated to obtain an enhanced PL efficiency of up to ∼five folds, which obviously exceeds the reported efficiency upon electrical and/or plasma doping strategies. The PL enhancement degree can also be modulated by tuning the corresponding surface functional groups of MXene nano-flakes, reflecting that the electron-withdrawing functional groups play a vital role in this charge transfer process. These findings offer promising clues to control the optoelectronic properties of TMDCs and expand the scope of the application of MXene nano-flakes, suggesting a possibility to construct a new heterostructure junction based on MXenes and TMDCs.

SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA