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7.
J Am Chem Soc ; 140(15): 5118-5126, 2018 04 18.
Artigo em Inglês | MEDLINE | ID: mdl-29609454

RESUMO

The search for high active, stable, and cost-efficient hydrogen evolution reaction (HER) electrocatalysts for water electrolysis has attracted great interest. The coordinated water molecules in the hydronium ions will obviously reduce the positive charge density of H+ and hamper the ability of H+ to receive electrons from the cathode, leading to large overpotential of HER on nonprecious metal catalysts. Here we realize Pt-like hydrogen evolution electrocatalysis on polyaniline (PANI) nanodots (NDs)-decorated CoP hybrid nanowires (HNWs) supported on carbon fibers (CFs) (PANI/CoP HNWs-CFs) as PANI can effectively capture H+ from hydronium ions to form protonated amine groups that have higher positive charge density than those of hydronium ions and can be electro-reduced easily. The PANI/CoP HNWs-CFs as low-cost electrocatalysts show excellent catalytic performance toward HER in acidic solution, such as super high catalytic activity, small Tafel slope, and superior stability.

8.
Angew Chem Int Ed Engl ; 57(10): 2672-2676, 2018 03 01.
Artigo em Inglês | MEDLINE | ID: mdl-29418055

RESUMO

Iron-substituted CoOOH porous nanosheet arrays grown on carbon fiber cloth (denoted as Fex Co1-x OOH PNSAs/CFC, 0≤x≤0.33) with 3D hierarchical structures are synthesized by in situ anodic oxidation of α-Co(OH)2 NSAs/CFC in solution of 0.01 m (NH4 )2 Fe(SO4 )2 . X-ray absorption fine spectra (XAFS) demonstrate that CoO6 octahedral structure in CoOOH can be partially substituted by FeO6 octahedrons during the transformation from α-Co(OH)2 to Fex Co1-x OOH, and this is confirmed for the first time in this study. The content of Fe in Fex Co1-x OOH, no more than 1/3 of Co, can be controlled by adjusting the in situ anodic oxidation time. Fe0.33 Co0.67 OOH PNSAs/CFC shows superior OER electrocatalytic performance, with a low overpotential of 266 mV at 10 mA cm-2 , small Tafel slope of 30 mV dec-1 , and high durability.

9.
J Am Chem Soc ; 140(2): 610-617, 2018 01 17.
Artigo em Inglês | MEDLINE | ID: mdl-29058435

RESUMO

Low-cost transition-metal dichalcogenides (MS2) have attracted great interest as alternative catalysts for hydrogen evolution. However, a significant challenge is the formation of sulfur-hydrogen bonds on MS2 (S-Hads), which will severely suppress hydrogen evolution reaction (HER). Here we report Cu nanodots (NDs)-decorated Ni3S2 nanotubes (NTs) supported on carbon fibers (CFs) (Cu NDs/Ni3S2 NTs-CFs) as efficient electrocatalysts for HER in alkaline media. The electronic interactions between Cu and Ni3S2 result in Cu NDs that are positively charged and can promote water adsorption and activation. Meanwhile, Ni3S2 NTs are negatively charged and can weaken S-Hads bonds formed on catalyst surfaces. Therefore, the Cu/Ni3S2 hybrids can optimize H adsorption and desorption on electrocatalysts and can promote both Volmer and Heyrovsky steps of HER. The strong interactions between Cu and Ni3S2 cause the Cu NDs/Ni3S2 NTs-CFs electrocatalysts to exhibit the outstanding HER catalytic performance with low onset potential, high catalytic activity, and excellent stability.

10.
Angew Chem Int Ed Engl ; 56(28): 8120-8124, 2017 07 03.
Artigo em Inglês | MEDLINE | ID: mdl-28523796

RESUMO

Constructing inorganic-organic hybrids with superior properties in terms of water adsorption and activation will lead to catalysts with significantly enhanced electrocatalytic activity in the hydrogen evolution reaction (HER) in environmentally benign neutral media. Herein, we report SiO2 -polypyrrole (PPy) hybrid nanotubes supported on carbon fibers (CFs) (SiO2 /PPy NTs-CFs) as inexpensive and high-performance electrocatalysts for the HER in neutral media. Because of the strong electronic interactions between SiO2 and PPy, the SiO2 uniquely serves as the centers for water adsorption and activation, and accordingly promotes the HER. The metal-free SiO2 /PPy NTs-CFs displayed high catalytic activity in the HER in neutral media, such as a low onset potential and small Tafel slope, as well as excellent long-term durability.

11.
Angew Chem Int Ed Engl ; 56(11): 2960-2964, 2017 03 06.
Artigo em Inglês | MEDLINE | ID: mdl-28140498

RESUMO

TiO2 Co nanotubes decorated with nanodots (TiO2 NDs/Co NSNTs-CFs) are reported as high-performance earth-abundant electrocatalysts for the hydrogen evolution reaction (HER) in alkaline solution. TiO2 NDs/Co NSNTs can promote water adsorption and optimize the free energy of hydrogen adsorption. More importantly, the absorbed water can be easily activated in the presence of the TiO2 -Co hybrid structure. These advantages will significantly promote HER. TiO2 NDs/Co NSNTs-CFs as electrocatalysts show a high catalytic performance towards HER in alkaline solution. This study will open up a new avenue for designing and fabricating low-cost high-performance HER catalysts.

12.
Adv Mater ; 28(23): 4698-703, 2016 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-27072073

RESUMO

FeOOH/CeO2 heterolayered nanotubes supported on Ni foam as efficient oxygen evolution electrocatalysts are reported. The hybrid structure can obviously promote the catalytic performance for the oxygen evolution reaction, such as low onset potential, high electroactivity, and excellent long-term durability. This study provides a new route to the design and fabrication of electrocatalysts with high electroactivity and durability for oxygen evolution.

13.
Angew Chem Int Ed Engl ; 55(11): 3694-8, 2016 Mar 07.
Artigo em Inglês | MEDLINE | ID: mdl-26879125

RESUMO

Herein, we developed FeOOH/Co/FeOOH hybrid nanotube arrays (HNTAs) supported on Ni foams for oxygen evolution reaction (OER). The inner Co metal cores serve as highly conductive layers to provide reliable electronic transmission, and can overcome the poor electrical conductivity of FeOOH efficiently. DFT calculations demonstrate the strong electronic interactions between Co and FeOOH in the FeOOH/Co/FeOOH HNTAs, and the hybrid structure can lower the energy barriers of intermediates and thus promote the catalytic reactions. The FeOOH/Co/FeOOH HNTAs exhibit high electrocatalytic performance for OER, such as low onset potential, small Tafel slope, and excellent long-term durability, and they are promising electrocatalysts for OER in alkaline solution.

14.
Adv Mater ; 27(44): 7051-7, 2015 Nov 25.
Artigo em Inglês | MEDLINE | ID: mdl-26436879

RESUMO

Hybrid electrocatalysts with excellent electrocatalytic activity for hydrogen reduction are fabricated using an efficient and facile electrochemical route. The electronic and synergistic effects between Co(OH)2 and polyaniline (PANI) in the composite structure are the key factors that generate the high electrocatalytic activity and excellent stability. A highly efficient, non-precious metal-based flexible electrocatalyst for high-performance electrocatalysts is shown, which reveals a novel route for the design and synthesis of electrocatalysts.


Assuntos
Compostos de Anilina/química , Cobalto/química , Hidrogênio/química , Hidróxidos/química , Nanoestruturas/química , Nanotecnologia , Catálise , Eletroquímica , Fenômenos Mecânicos , Níquel/química
15.
ACS Appl Mater Interfaces ; 7(21): 11444-51, 2015 Jun 03.
Artigo em Inglês | MEDLINE | ID: mdl-25961565

RESUMO

Here we synthesize novel asymmetric all-solid-state paper supercapacitors (APSCs) based on amorphous porous Mn3O4 grown on conducting paper (NGP) (Mn3O4/NGP) negative electrode and Ni(OH)2 grown on NGP (Ni(OH)2/NGP) as positive electrode, and they have attracted intensive research interest owing to their outstanding properties such as being flexible, ultrathin, and lightweight. The fabricated APSCs exhibit a high areal Csp of 3.05 F/cm3 and superior cycling stability. The novel asymmetric APSCs also exhibit high energy density of 0.35 mW h/cm3, high power density of 32.5 mW/cm3, and superior cycling performance (<17% capacitance loss after 12,000 cycles at a high scan rate of 100 mV/s). This work shows the first example of amorphous porous metal oxide/NGP electrodes for the asymmetric APSCs, and these systems hold great potential for future flexible electronic devices.

16.
Chem Sci ; 6(12): 6991-6998, 2015 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-28757980

RESUMO

The catalytic activity and durability are crucial for the development of high-performance electrocatalysts. To design electrocatalysts with excellent electroactivity and durability, the structure and composition are two important guiding principles. In this work, novel Pt/Ni(OH)2-NiOOH/Pd multi-walled hollow nanorod arrays (MHNRAs) are successfully synthesized. The unique MHNRAs provide fast transport and short diffusion paths for electroactive species and high utilization rate of catalysts. Because of the special surface and synergistic effects, the Pt/Ni(OH)2-NiOOH/Pd MHNRA electrocatalysts exhibit high catalytic activity, high durability and superior CO poisoning tolerance for the electrooxidation of formic acid in comparison with Pt@Pd MHNRAs, commercial Pt/C, Pd/C and PtRu/C catalysts.

17.
J Am Chem Soc ; 135(29): 10703-9, 2013 Jul 24.
Artigo em Inglês | MEDLINE | ID: mdl-23837995

RESUMO

Low cost, high activity, and long-term durability are the main requirements for commercializing fuel cell electrocatalysts. Despite tremendous efforts, developing non-Pt anode electrocatalysts with high activity and long-term durability at low cost remains a significant technical challenge. Here we report a new type of hybrid Pd/PANI/Pd sandwich-structured nanotube array (SNTA) to exploit shape effects and synergistic effects of Pd-PANI composites for the oxidation of small organic molecules for direct alcohol fuel cells. These synthesized Pd/PANI/Pd SNTAs exhibit significantly improved electrocatalytic activity and durability compared with Pd NTAs and commercial Pd/C catalysts. The unique SNTAs provide fast transport and short diffusion paths for electroactive species and high utilization rate of catalysts. Besides the merits of nanotube arrays, the improved electrocatalytic activity and durability are especially attributed to the special Pd/PANI/Pd sandwich-like nanostructures, which results in electron delocalization between Pd d orbitals and PANI π-conjugated ligands and in electron transfer from Pd to PANI.

18.
Nanoscale ; 5(10): 4056-69, 2013 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-23584514

RESUMO

Electrochemical synthesis represents a highly efficient method for the fabrication of nanostructured energy materials, and various nanostructures, such as nanorods, nanowires, nanotubes, nanosheets, dendritic nanostructures, and composite nanostructures, can be easily fabricated with advantages of low cost, low synthetic temperature, high purity, simplicity, and environmental friendliness. The electrochemical synthesis, characterization, and application of electrochemical energy nanomaterials have advanced greatly in the past few decades, allowing an increasing understanding of nanostructure-property-performance relationships. Herein, we highlight some recent progress in the electrochemical synthesis of electrochemical energy materials with the assistance of additives and templates in solution or grafted onto metal or conductive polymer supports, with special attention to the effects on surface morphologies, structures and, more importantly, electrochemical performance. The methodology for preparing novel electrochemical energy nanomaterials and their potential applications has been summarized. Finally, we outline our personal perspectives on the electrochemical synthesis and applications of electrochemical energy nanomaterials.


Assuntos
Técnicas Eletroquímicas , Nanoestruturas , Nanotecnologia , Técnicas Eletroquímicas/métodos , Técnicas Eletroquímicas/tendências , Nanoestruturas/química , Nanoestruturas/ultraestrutura , Nanotecnologia/métodos , Nanotecnologia/tendências , Retratos como Assunto , Propriedades de Superfície
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