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1.
ACS Nano ; 16(4): 6255-6265, 2022 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-35302347

RESUMO

Sodium and potassium ions energy storage systems with low cost and high energy/power densities have recently drawn increasing interest as promising candidates for grid-level applications, while the lack of suitable anode materials with fast ion diffusion kinetics highly hinders their development. Herein, we develop a nanoscale confined in situ oxidation polymerization process followed by a conventional carbonization treatment to generate phosphorus and nitrogen dual-doped hollow carbon spheres (PNHCS), which can realize superior sodium and potassium ion storage performance. Importantly, the density functional theory calculation and combined characterizations, e.g., in situ Raman spectroscopy and ex situ X-ray photoelectron spectroscopy, decipher that the P/N doping can enhance the electronic transfer dynamics and ion adsorption capability, which are responsible for enhanced electrochemical performance. Inspiringly, the practicability of the PNHCS anode is demonstrated by assembling the potassium ion hybrid capacitors (KIHCs), where the prominent energy density is 178.80 Wh kg-1 at a power density of 197.65 W kg-1, with excellent cycling stability, can be achieved. This work not only promotes the development of efficient anode material for sodium/potassium ion storage devices but also deciphers the embedded ion storage mechanism.

2.
ACS Appl Mater Interfaces ; 13(3): 3881-3890, 2021 Jan 27.
Artigo em Inglês | MEDLINE | ID: mdl-33464037

RESUMO

Designing highly active transition-metal-based electrocatalysts for energy-saving electrochemical hydrogen evolution coupled with hydrazine oxidation possesses more economic prospects. However, the lack of bifunctional electrocatalysts and the absence of intrinsic structure-property relationship research consisting of adsorption configurations and dehydrogenation behavior of N2H4 molecules still hinder the development. Now, a V-doped Ni3N nanosheet self-supported on Ni foam (V-Ni3N NS) is reported, which presents excellent bifunctional electrocatalytic performance toward both hydrazine oxidation reaction (HzOR) and hydrogen evolution reaction (HER). The resultant V-Ni3N NS achieves an ultralow working potential of 2 mV and a small overpotential of 70 mV at 10 mA cm-2 in alkaline solution for HzOR and HER, respectively. Density functional theory calculations reveal that the vanadium substitution could effectively modulate the electronic structure of Ni3N, therefore facilitating the adsorption/desorption behavior of H* for HER, as well as boosting the dehydrogenation kinetics for HzOR.

3.
Angew Chem Int Ed Engl ; 60(11): 5984-5993, 2021 Mar 08.
Artigo em Inglês | MEDLINE | ID: mdl-33306263

RESUMO

Electrochemical water splitting for H2 production is limited by the sluggish anode oxygen evolution reaction (OER), thus using hydrazine oxidation reaction (HzOR) to replace OER has received great attention. Here we report the hierarchical porous nanosheet arrays with abundant Ni3 N-Co3 N heterointerfaces on Ni foam with superior hydrogen evolution reaction (HER) and HzOR activity, realizing working potentials of -43 and -88 mV for 10 mA cm-2 , respectively, and achieving an industry-level 1000 mA cm-2 at 200 mV for HzOR. The two-electrode overall hydrazine splitting (OHzS) electrolyzer requires the cell voltages of 0.071 and 0.76 V for 10 and 400 mA cm-2 , respectively. The H2 production powered by a direct hydrazine fuel cell (DHzFC) and a commercial solar cell are investigated to inspire future practical applications. DFT calculations decipher that heterointerfaces simultaneously optimize the hydrogen adsorption free energy (ΔGH* ) and promote the hydrazine dehydrogenation kinetics. This work provides a rationale for advanced bifunctional electrocatalysts, and propels the practical energy-saving H2 generation techniques.

4.
RSC Adv ; 10(23): 13507-13516, 2020 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-35493022

RESUMO

In this study, new α-indolylacrylate derivatives were synthesized by the reaction of 2-substituted indoles with various pyruvates using a Brønsted acid ionic liquid catalyst in butyl acetate solvent. This is the first report on the application of pyruvate compounds for the synthesis of indolylacrylates. The acrylate derivatives could be obtained in good to excellent yields. A preliminary biological evaluation revealed their promising anticancer activity (IC50 = 9.73 µM for the compound 4l) and indicated that both the indole core and the acrylate moieties are promising for the development of novel anticancer drugs. The Lipinski's rule and Veber's parameters were assessed for the newly synthesized derivatives.

5.
Org Biomol Chem ; 17(24): 5982-5989, 2019 06 18.
Artigo em Inglês | MEDLINE | ID: mdl-31166351

RESUMO

A straightforward access to tricyclic indoles bearing 3,4-fused seven-membered rings has been established by using 4-aminoindoles as 1,4-bisnucleophiles in three-component reactions. 1H-Azepino[4,3,2-cd]indoles, 4,6-dihydro-1H-azepino[4,3,2-cd]indoles and 1,3,4,6-tetrahydro-5H-azepino[4,3,2-cd]indol-5-ones could thus be synthesized in one pot in moderate to good yields. Beyond opening access to 3,4-fused tricyclic indoles, the use of easily accessible 4-aminoindoles as C,N-1,4-bisnucleophiles also provides a new platform to be used in a diversity-oriented synthesis strategy, fully displaying its benefits of maximizing molecular complexity and reaction diversity.


Assuntos
Indóis/química , Indóis/síntese química , Estrutura Molecular , Estereoisomerismo
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