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1.
Angew Chem Int Ed Engl ; 58(19): 6244-6249, 2019 May 06.
Artículo en Inglés | MEDLINE | ID: mdl-30843633

RESUMEN

This study presents synthesis and characterizations of two novel curved nanographenes that strongly bind with fullerene C60 to form photoconductive heterojunctions. Films of the self-assembled curved nanographene/fullerene complexes, which served as the photoconductive layer, generated a significant photocurrent under light irradiation. Gram-scale quantities of these curved nanographenes (TCR and HCR) as the "crown" sidewalls can be incorporated into a carbon nanoring to form molecular crowns, and the molecular structure of C60 @TCR is determined by single-crystal X-ray diffraction. The UV/Vis absorption and emission spectra, and theoretical studies revealed their unique structural features and photophysical properties. Time-resolved spectroscopic results clearly suggest fast photoinduced electron transfer process in the supramolecular heterojunctions.

2.
Adv Mater ; 29(46)2017 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-29058346

RESUMEN

The development of efficient water-oxidation electrocatalysts based on inexpensive and earth-abundant materials is significant to enable water splitting as a future renewable energy source. Herein, the synthesis of novel FeNiP solid-solution nanoplate (FeNiP-NP) arrays and their use as an active catalyst for high-performance water-oxidation catalysis are reported. The as-prepared FeNiP-NP catalyst on a 3D nickel foam substrate exhibits excellent electrochemical performance with a very low overpotential of only 180 mV to reach a current density of 10 mA cm-2 and an onset overpotential of 120 mV in 1.0 m KOH for the oxygen evolution reaction (OER). The slope of the Tafel plot is as low as 76.0 mV dec-1 . Furthermore, the long-term electrochemical stability of the FeNiP-NP electrode is investigated by cyclic voltammetry (CV) at 1.10-1.55 V versus reversible hydrogen electrode (RHE), demonstrating very stable performance with negligible loss in activity after 1000 CV cycles. This present FeNiP-NP solid solution is thought to represent the best OER catalytic activity among the non-noble metal catalysts reported so far.

3.
ChemSusChem ; 9(17): 2365-73, 2016 09 08.
Artículo en Inglés | MEDLINE | ID: mdl-27530422

RESUMEN

Scalable and robust catalysts for the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) are required for the implementation of water splitting technologies as a globally applicable method of producing renewable hydrogen. Herein, we report nitrogen-enriched porous carbon materials containing copper/copper oxide, derived from copper porphyrin-based conjugated mesoporous polymers (CMPs), as a bifunctional catalyst for both HER and OER. These catalysts have a high surface area, unique tubular structure, and strong synergistic effect of copper/copper oxide and porous carbons, resulting in excellent performance for water splitting. Under optimal conditions, the catalyst exhibits a quite low overpotential for OER (350 mV to reach 1.0 mA cm(-2) and 450 mV to reach 10 mA cm(-2) ) in alkaline media, which places it among the best copper-based water oxidation catalysts reported in the literature. Furthermore, the catalyst shows good catalytic activity for HER at a low overpotential (190 mV to reach 1.0 mA cm(-2) ) as well as a high current density (470 mV to reach 50 mA cm(-2) ). The results suggest that hybridized copper/carbon materials are attractive noble-metal-free catalysts for water splitting.


Asunto(s)
Cobre/química , Hidrógeno/química , Metaloporfirinas/química , Oxígeno/química , Polímeros/química , Catálisis , Electroquímica , Electrólisis , Porosidad
4.
Chem Commun (Camb) ; 52(32): 5546-9, 2016 Apr 25.
Artículo en Inglés | MEDLINE | ID: mdl-27020763

RESUMEN

Developing efficient water oxidation catalysts made up of earth-abundant elements has attracted much attention as a step toward for future clean energy production. Herein we report a simple one-step method to generate a low cost copper oxide catalyst film in situ from a copper(ii) ethylenediamine complex. The resulting catalyst has excellent activity toward the oxygen evolution reaction in alkaline solutions. A catalytic current density of 1.0 mA cm(-2) and 10 mA cm(-2) for the catalyst film requires the overpotentials of only ∼370 mV and ∼475 mV in 1.0 M KOH, respectively. This catalytic performance shows that the new catalyst is one of the best Cu-based heterogeneous OER catalysts to date.

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