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1.
ACS Nano ; 17(5): 5083-5094, 2023 Mar 14.
Artículo en Inglés | MEDLINE | ID: mdl-36853201

RESUMEN

High-potential Mn3+/Mn2+ redox couple (>1.3 V vs SHE) in a static battery system is rarely reported due to the shuttle and disproportionation of Mn3+ in aqueous solutions. Herein, based on reversible stripping/plating of the Sn anode and stabilized Mn2+/Mn3+ redox couple in the cathode, an aqueous Sn-Mn full battery is established in acidic electrolytes. Sn anode exhibits high deposition efficiency, low polarization, and excellent stability in acidic electrolytes. With the help of H+ and a complexing agent, a reversible conversion between Mn2+ and Mn3+ ions takes place on the graphite surface. Pyrophosphate ligand is initially employed to form a protective layer through a complexation process with Sn4+ on the electrode surface, effectively preventing Mn3+ from disproportionation and hindering the uncontrollable diffusion of Mn3+ to electrolytes. Benefiting from the rational design, the full battery delivers satisfied electrochemical performance including a large capacity (0.45 mAh cm-2 at 5 mA cm-2), high discharge plateau voltage (>1.6 V), excellent rate capability (58% retention from 5 to 30 mA cm-2), and superior cycling stability (no decay after 30 000 cycles). The battery design strategy realizes a robustly stable Mn3+/Mn2+ redox reaction, which broadens research into ultrafast acidic battery systems.

2.
ACS Appl Mater Interfaces ; 14(18): 21668-21676, 2022 May 11.
Artículo en Inglés | MEDLINE | ID: mdl-35471960

RESUMEN

The current-induced magnetization switching and damping-like field in Pt/(Co/Pt)/PtMn trilayer films prepared with and without an in situ in-plane field of 600 Oe have been studied systematically. In the presence of the in situ field, a small in-plane bias field (HEB) is observed for films with PtMn thickness ≥5 nm, while there is no observable HEB for PtMn thickness ≤3 nm. Nevertheless, a field-free switching of perpendicular magnetization of Co/Pt is observed for all the films with the PtMn thickness of 1-7 nm. On the other hand, without the presence of the in situ field, HEB and field-free switching are not seen. Furthermore, the damping-like fields (HDL) are much enhanced in the presence of the in situ field, and the increasement can be up to 47%. We further revealed that the spin current is mainly from the Pt layer, while the noncollinear spin configuration at the interface caused by the in situ in-plane field may play a role in the HDL enhancement. Micromagnetic simulations indicate that the canting of antiferromagnet PtMn spins plays an important role in the field-free switching. Our findings clarify the source of spin current in the trilayer films and provide an easier approach to field-free switching and HDL enhancement for future low-power spintronic devices.

3.
Angew Chem Int Ed Engl ; 61(3): e202114681, 2022 Jan 17.
Artículo en Inglés | MEDLINE | ID: mdl-34755421

RESUMEN

As an emerging post-lithium battery technology, aluminum ion batteries (AIBs) have the advantages of large Al reserves and high safety, and have great potential to be applied to power grid energy storage. But current graphite cathode materials are limited in charge storage capacity due to the formation of stage-4 graphite-intercalated compounds (GICs) in the fully charged state. Herein, we propose a new type of cathode materials for AIBs, namely polycyclic aromatic hydrocarbons (PAHs), which resemble graphite in terms of the large conjugated π bond, but do not form GICs in the charge process. Quantum chemistry calculations show that PAHs can bind AlCl4 - through the interaction between the conjugated π bond in the PAHs and AlCl4 - , forming on-plane interactions. The theoretical specific capacity of PAHs is negatively correlated with the number of benzene rings in the PAHs. Then, under the guidance of theoretical calculations, anthracene, a three-ring PAH, was evaluated as a cathode material for AIBs. Electrochemical measurements show that anthracene has a high specific capacity of 157 mAh g-1 (at 100 mA g-1 ) and still maintains a specific capacity of 130 mAh g-1 after 800 cycles. This work provides a feasible "theory guides practice" research model for the development of energy storage materials, and also provides a new class of promising cathode materials for AIBs.

4.
ACS Appl Mater Interfaces ; 12(41): 46065-46072, 2020 Oct 14.
Artículo en Inglés | MEDLINE | ID: mdl-32955247

RESUMEN

The urgent need for large-scale, low-cost energy storage has driven a new wave of research focusing on innovative batteries. Due to the high capacity and the low-cost of elemental Al, aluminum-ion batteries (AIBs) are expected as promising candidates for future energy storage. However, further development of AIBs is restricted by the performance of existing carbon-based cathodes and metal chalcogenide cathode materials. In this work, we deposited polythiophene (Pth) on a graphene oxide (Pth@GO) composite and used it as an AIB cathode material. This Pth@GO composite possesses high exposure of Pth active sites, high conductivity, and high structure stability while providing a very high discharge capacity (up to 130 mAh g-1) and outstanding cyclic stability (maintaining above 100 mAh g-1 after 4000 cycles). First principles calculations and experimental results show that the charge is stored on Pth@GO through an electrostatic attraction between AlCl4- and ß-hydrogen (Cß-H) sites in polythiophene.

5.
ACS Appl Mater Interfaces ; 12(2): 3086-3095, 2020 Jan 15.
Artículo en Inglés | MEDLINE | ID: mdl-31849215

RESUMEN

Controlling effective separation of carriers at the interface is a key element to realize highly efficient halogenated perovskite-based optoelectronic devices. Here, a comprehensive study of interfacial properties for CsPbBr3 nanocrystals (NCs)/graphene heterostructure is performed by the combination of theoretical and experimental methods. Enhanced visible light absorption is observed experimentally in the CsPbBr3 NCs/graphene heterostructure. The strong photoluminescence quenching phenomenon and improved photoresponse prove the efficient interfacial charge transfer from the perovskite CsPbBr3 NC layer to the graphene side. Significantly, theoretical calculations suggest that an intrinsic built-in electric field, pointing from graphene toward CsPbBr3, promotes the separation of photoinduced carriers at the CsPbBr3 NCs/graphene interface and simultaneously inhibits the recombination of electron-hole pairs. Thus, the high optoelectronic performance can be obtained in the CsPbBr3 NCs/graphene heterostructure, as shown in our experiment. Moreover, the CsPbBr3 NCs/graphene heterostructure exhibits smaller effective mass than that of CsPbBr3 NCs, indicating that the heterostructure does possess a high carrier mobility, which can further accelerate the separation of photogenerated carriers. Furthermore, the calculated results reveal that, accounting for the presence of the stronger built-in electric field, larger band bending value, and smaller effective mass, the PbBr2/graphene interface can realize the separation of the photoinduced carriers more effectively than the CsBr/graphene interface and thus more efficiently facilitate electron transfer from the perovskite optical absorber side to the graphene electronic transport side. Our findings provide valuable insight into perovskite/graphene-based photodetector devices via the interface engineering project.

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