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1.
Nature ; 616(7955): 77-83, 2023 04.
Artigo em Inglês | MEDLINE | ID: mdl-37020008

RESUMO

Inorganic superionic conductors possess high ionic conductivity and excellent thermal stability but their poor interfacial compatibility with lithium metal electrodes precludes application in all-solid-state lithium metal batteries1,2. Here we report a LaCl3-based lithium superionic conductor possessing excellent interfacial compatibility with lithium metal electrodes. In contrast to a Li3MCl6 (M = Y, In, Sc and Ho) electrolyte lattice3-6, the UCl3-type LaCl3 lattice has large, one-dimensional channels for rapid Li+ conduction, interconnected by La vacancies via Ta doping and resulting in a three-dimensional Li+ migration network. The optimized Li0.388Ta0.238La0.475Cl3 electrolyte exhibits Li+ conductivity of 3.02 mS cm-1 at 30 °C and a low activation energy of 0.197 eV. It also generates a gradient interfacial passivation layer to stabilize the Li metal electrode for long-term cycling of a Li-Li symmetric cell (1 mAh cm-2) for more than 5,000 h. When directly coupled with an uncoated LiNi0.5Co0.2Mn0.3O2 cathode and bare Li metal anode, the Li0.388Ta0.238La0.475Cl3 electrolyte enables a solid battery to run for more than 100 cycles with a cutoff voltage of 4.35 V and areal capacity of more than 1 mAh cm-2. We also demonstrate rapid Li+ conduction in lanthanide metal chlorides (LnCl3; Ln = La, Ce, Nd, Sm and Gd), suggesting that the LnCl3 solid electrolyte system could provide further developments in conductivity and utility.

2.
Adv Mater ; 34(32): e2202688, 2022 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-35766726

RESUMO

Superior fast charging is a desirable capability of lithium-ion batteries, which can make electric vehicles a strong competition to traditional fuel vehicles. However, the slow transport of solvated lithium ions in liquid electrolytes is a limiting factor. Here, a Lix Cu6 Sn5 intermetallic network is reported to address this issue. Based on electrochemical analysis and X-ray photoelectron spectroscopy mapping, it is demonstrated that the reported intermetallic network can form a high-speed solid-state lithium transport matrix throughout the electrode, which largely reduces the lithium-ion-concentration polarization effect in the graphite anode. Employing this design, superior fast-charging graphite/lithium cobalt oxide full cells are fabricated and tested under strict electrode conditions. At the charging rate of 6 C, the fabricated full cells show a capacity of 145 mAh g-1 with an extraordinary capacity retention of 96.6%. In addition, the full cell also exhibits good electrochemical stability at a high charging rate of 2 C over 100 cycles (96.0% of capacity retention) in comparison to traditional graphite-anode-based cells (86.1% of capacity retention). This work presents a new strategy for fast-charging lithium-ion batteries on the basis of high-speed solid-state lithium transport in intermetallic alloy hosts.

3.
Nat Commun ; 12(1): 4296, 2021 Jul 14.
Artigo em Inglês | MEDLINE | ID: mdl-34262051

RESUMO

Photoelectrochemical catalysis is an attractive way to provide direct hydrogen production from solar energy. However, solar conversion efficiencies are hindered by the fact that light harvesting has so far been of limited efficiency in the near-infrared region as compared to that in the visible and ultraviolet regions. Here we introduce near-infrared-active photoanodes that feature lattice-matched morphological hetero-nanostructures, a strategy that improves energy conversion efficiency by increasing light-harvesting spectral range and charge separation efficiency simultaneously. Specifically, we demonstrate a near-infrared-active morphological heterojunction comprised of BiSeTe ternary alloy nanotubes and ultrathin nanosheets. The heterojunction's hierarchical nanostructure separates charges at the lattice-matched interface of the two morphological components, preventing further carrier recombination. As a result, the photoanodes achieve an incident photon-to-current conversion efficiency of 36% at 800 nm in an electrolyte solution containing hole scavengers without a co-catalyst.

4.
Nat Commun ; 11(1): 1761, 2020 Apr 09.
Artigo em Inglês | MEDLINE | ID: mdl-32273513

RESUMO

Fabricating a robust interfacial layer on the lithium metal anode to isolate it from liquid electrolyte is vital to restrain the rapid degradation of a lithium metal battery. Here, we report that the solution-processed metal chloride perovskite thin film can be coated onto the lithium metal surface as a robust interfacial layer to shield the lithium metal from liquid electrolyte. Via phase analysis and density functional theory calculations, we demonstrate that the perovskite layer can allow fast lithium ion shuttle under a low energy barrier of 0.45 eV without the collapse of framework. Such perovskite modification can realize stable cycling of LiCoO2|Li cells with an areal capacity of 2.8 mAh cm-2 using thin lithium metal foil (50 µm) and limited electrolyte (20 µl mAh-1) for over 100 cycles at 0.5 C. The metal chloride perovskite protection strategy could open a promising avenue for advanced lithium metal batteries.

5.
Research (Wash D C) ; 2019: 6262719, 2019.
Artigo em Inglês | MEDLINE | ID: mdl-31549073

RESUMO

Solid acid catalysts (SACs) have attracted continuous research interest in past years as they play a pivotal role in establishing environmentally friendly and sustainable catalytic processes for various chemical industries. Development of low-cost and efficient SACs applicable to different catalysis processes are of immense significance but still very challenging so far. Here, we report a new kind of SACs consisting of sulfonated carbon nanofibers that are prepared via incomplete carbonization of low-cost natural nanofibrous cellulose followed by sulphonation with sulfuric acid. The prepared SACs feature nanofibrous network structures, high specific surface area, and abundant sulfonate as well as hydroxyl and carboxyl groups. Remarkably, the nanofibrous SACs exhibit superior performance to the state-of-the-art SACs for a wide range of acid-catalyzed reactions, including dimerization of α-methylstyrene, esterification of oleic acid, and pinacol rearrangement. The present approach holds great promise for developing new families of economic but efficient SACs based on natural precursors via scalable and sustainable protocols in the future.

6.
Nat Commun ; 9(1): 2533, 2018 06 28.
Artigo em Inglês | MEDLINE | ID: mdl-29955067

RESUMO

Transition metal dichalcogenide materials have been explored extensively as catalysts to negotiate the hydrogen evolution reaction, but they often run at a large excess thermodynamic cost. Although activating strategies, such as defects and composition engineering, have led to remarkable activity gains, there remains the requirement for better performance that aims for real device applications. We report here a phosphorus-doping-induced phase transition from cubic to orthorhombic phases in CoSe2. It has been found that the achieved orthorhombic CoSe2 with appropriate phosphorus dopant (8 wt%) needs the lowest overpotential of 104 mV at 10 mA cm-2 in 1 M KOH, with onset potential as small as -31 mV. This catalyst demonstrates negligible activity decay after 20 h of operation. The striking catalysis performance can be attributed to the favorable electronic structure and local coordination environment created by this doping-induced structural phase transition strategy.

7.
Adv Mater ; 26(36): 6262-7, 2014 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-25091210

RESUMO

Conductive fullerene electron-transporting layers (ETLs) are developed to facilitate the solution processing of highly efficient inverted OSCs with power conversion efficiency (PCE) reaching 9.6%. Its high conductivity also allows devices to be fabricated independently of the ETL thickness (up to ca. 50 nm). Transient photovoltage (TPV) measurements are used to shed light on how these conductive ETLs help suppress charge recombination in solar cells.

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