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1.
J Colloid Interface Sci ; 669: 228-235, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-38713961

RESUMO

The development of heterogeneous supported nanocatalysts with a high kinetics combined with low cost is off importance but remains still challenged for hydrazine hydrate served as a promising hydrogen storage material. Herein, by virtue of surficial functional groups, ultrafine NiRh NPs were monodispersed on the two-dimensional V2C surface via a conventional wet chemical co-reduction. The optimized NiRh/V2C system demonstrates an excellent catalytic performance toward selectively catalyzing dehydrogenation of hydrazine hydrate, affording 100% H2 selectivity with the turnover frequency (TOF) value of 987.5 h-1 at 323 K. Such an enhancement is mainly attributed to synergistic effect of nanosystem, which will optimize local surface energy and promote electron transfer in NiRh/V2C system, thereby improving the kinetic selectivity of catalytic hydrazine hydrate decomposition. This work has provided a facile strategy for developing nanocatalysts with high kinetics that could enable huge industrial applications in the future.

2.
J Phys Chem Lett ; 14(24): 5692-5700, 2023 Jun 22.
Artigo em Inglês | MEDLINE | ID: mdl-37315210

RESUMO

The electrocatalytic oxygen evolution reaction (OER) is important for many renewable energy technologies. Developing cost-effective electrocatalysts with high performance remains a great challenge. Here, we successfully demonstrate our novel interface catalyst comprised of Ni3Fe1-based layered double hydroxides (Ni3Fe1-LDH) vertically immobilized on a two-dimensional MXene (Ti3C2Tx) surface. The Ni3Fe1-LDH/Ti3C2Tx yielded an anodic OER current of 100 mA cm-2 at 0.28 V versus reversible hydrogen electrode (RHE), nearly 74 times lower than that of the pristine Ni3Fe1-LDH. Furthermore, the Ni3Fe1-LDH/Ti3C2Tx catalyst requires an overpotential of only 0.31 V versus RHE to deliver an industrial-level current density as high as 1000 mA cm-2. Such excellent OER activity was attributed to the synergistic interface effect between Ni3Fe1-LDH and Ti3C2Tx. Density functional theory (DFT) results further reveal that the Ti3C2Tx support can efficiently accelerate the electron extraction from Ni3Fe1-LDH and tailor the electronic structure of catalytic sites, resulting in enhanced OER performance.

3.
Small ; 19(9): e2206859, 2023 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-36564350

RESUMO

Electrocatalytic hydrogen evolution reaction (HER) in alkaline media is important for hydrogen economy but suffers from sluggish reaction kinetics due to a large water dissociation energy barrier. Herein, Pt5 P2 nanocrystals anchoring on amorphous nickel phosphate nanorods as a high-performance interfacial electrocatalyst system (Pt5 P2 NCs/a-NiPi) for the alkaline HER are demonstrated. At the unique polycrystalline/amorphous interface with abundant defects, strong electronic interaction, and optimized intermediate adsorption strength, water dissociation is accelerated over abundant oxophilic Ni sites of amorphous NiPi, while hydride coupling is promoted on the adjacent electron-rich Pt sites of Pt5 P2 . Meanwhile, the ultra-small-sized Pt5 P2 nanocrystals and amorphous NiPi nanorods maximize the density of interfacial active sites for the Volmer-Tafel reaction. Pt5 P2 NCs/a-NiPi exhibits small overpotentials of merely 9 and 41 mV at -10 and -100 mA cm-2 in 1 M KOH, respectively. Notably, Pt5 P2 NCs/a-NiPi exhibits an unprecedentedly high mass activity (MA) of 14.9 mA µgPt -1 at an overpotential of 70 mV, which is 80 times higher than that of Pt/C and represents the highest MA of reported Pt-based electrocatalysts for the alkaline HER. This work demonstrates a phosphorization and interfacing strategy for promoting Pt utilization and in-depth mechanistic insights for the alkaline HER.

4.
Front Chem ; 10: 1073175, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-36531324

RESUMO

Hydrogen (H2) has been considered an ideal alternative energy source for solving energy supply security and greenhouse gas reduction. Although platinum group metal (PGM) catalysts have excellent performance in hydrogen electrocatalysis, their scarcity and high cost limit their industrial application. Therefore, it is necessary to develop low-cost and efficient non-PGM catalysts. Transition metal nitrides (TMNs) have attracted much attention because of their excellent catalytic performance in hydrogen electrochemistry, including hydrogen evolution reaction (HER)/hydrogen oxidation reaction (HOR). In this paper, we review and discuss the mechanism of HER/HOR in alkaline media. We compare and evaluate electrocatalytic performance for the HER/HOR TMN catalysts recently reported. Finally, we propose the prospects and research trends in sustainable alkaline hydrogen electrocatalysis.

5.
J Phys Chem Lett ; 12(46): 11361-11370, 2021 Nov 25.
Artigo em Inglês | MEDLINE | ID: mdl-34784226

RESUMO

Development of efficient bifunctional nonprecious metallic electrocatalysts for hydrogen electrochemistry in alkaline solution is of importance to enable commercialization of a low-cost alkaline hydrogen fuel cell and water electrolyzer, but it is very challenging. Two-dimensional (2D) MXene-based electrocatalysts hold tremendous potential for the applications of hydrogen fuel cell and water electrolyzer. Here, we successfully immobilized transition-metal-based NiMo nanoparticles (NPs) on 2D Ti3C2Tx (Tx: surface terminations, such as O, OH, or F) surfaces by a wet chemical method. Our results demonstrate that the NiMo NPs are monodispersed on Ti3C2Tx with surface functionalization. These monodisperse NPs resulted in superior hydrogen evolution reaction (HER) and hydrogen oxidation reaction (HOR) activities in an alkaline media. The NiMo NPs/Ti3C2Tx in 1.0 M KOH yielded an HER current of -10 mA cm-2 at -0.044 V vs reversible hydrogen electrode (RHE), nearly 232 mV smaller than that of the parent NiMo NPs. The NiMo NPs/Ti3C2Tx produced an HOR current density of 1.5 mA cm-2 at 0.1 V vs RHE. Density functional theory (DFT) results further reveal that Ti3C2Tx support can facilitate the charge transfer to metallic NPs and tailor the electronic structure of catalytic sites, resulting in optimized adsorption free energies of H* species for hydrogen electrochemistry. This work provides a facile and universal strategy in the development of 2D Ti3C2Tx with nonprecious metals for low-cost bifunctional hydrogen electrocatalysts.

6.
Nat Commun ; 9(1): 4531, 2018 10 31.
Artigo em Inglês | MEDLINE | ID: mdl-30382092

RESUMO

Electrocatalysts of the hydrogen evolution and oxidation reactions (HER and HOR) are of critical importance for the realization of future hydrogen economy. In order to make electrocatalysts economically competitive for large-scale applications, increasing attention has been devoted to developing noble metal-free HER and HOR electrocatalysts especially for alkaline electrolytes due to the promise of emerging hydroxide exchange membrane fuel cells. Herein, we report that interface engineering of Ni3N and Ni results in a unique Ni3N/Ni electrocatalyst which exhibits exceptional HER/HOR activities in aqueous electrolytes. A systematic electrochemical study was carried out to investigate the superior hydrogen electrochemistry catalyzed by Ni3N/Ni, including nearly zero overpotential of catalytic onset, robust long-term durability, unity Faradaic efficiency, and excellent CO tolerance. Density functional theory computations were performed to aid the understanding of the electrochemical results and suggested that the real active sites are located at the interface between Ni3N and Ni.

7.
J Nanosci Nanotechnol ; 13(4): 3115-20, 2013 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-23763209

RESUMO

The binary Ba0.5Sr0.5Fe12O19 (BSFO)/Ni0.5Zn0.5Fe2O4 (NZFO) nanocomposite ferrites hollow microfibers with high aspect ratios have been prepared by the gel precursor transformation process. These microfibers possess a high specific surface area about 45.2 m2 g(-1), and a ratio of the hollow diameter to the fiber diameter estimated about 5/7. The binary nanocomposite ferrites are formed after the precursor calcined at 750 degrees C for 3 h. Their minimum reflection loss (RL) is -38.1 dB at 10.4 GHz. The microwave absorption bandwidth with RL value exceeding -20 dB covers the whole X-band (8.2-12.4 GHz) and Ku-band (12.4-18 GHz). This enhancement in microwave absorption can be attributed to the exchange-coupling interaction, interfacial polarization and small size effect in nanocomposite hollow microfibers.

8.
J Nanosci Nanotechnol ; 11(8): 6979-85, 2011 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-22103109

RESUMO

SrFe12O19/Ni(0.5)Zn(0.5)Fe2O4 composite ferrite nanofibers of diameters about 100 nm with mass ratio 1:1 have been prepared by the electrospinning and calcination process. The SrFe12O19/Ni(0.5)Zn(0.5)Fe2O4 composite ferrites are formed after calcined at 700 degrees C for 2 hours. The composite ferrite nanofibers are fabricated from nanosized Ni(0.5)Zn(0.5)Fe2O4 and SrFe12O19 ferrite grains with a uniform phase distribution. The ferrite grain size increases from about 11 to 36 nm for Ni(0.5)Zn(0.5)Fe12O4 and 24 to 56 nm for SrFe12O19 with the calcination temperature increasing from 700 to 1100 degrees C. With the ferrite grain size increasing, the coercivity (Hc) and remanence (Mr) for the SrFe12O19/Ni(0.5)Zn(0.5)Fe2O4 composite ferrite nanofibers initially increase, reaching a maximum value of 118.4 kA/m and 31.5 Am2/kg at the grain size about 40 nm (SrFe12O19) and 24 nm (Ni(0.5)Zn(0.5)Fe2O4) respectively, and then show a reduction tendency with a further increase of the ferrite grain size. The specific saturation magnetization (Msh) of 63.2 Am2/kg for the SrFe12O19/Ni(0.5)Zn(0.5)Fe2O4 composite ferrite nanofibers obtained at 900 degrees C for 2 hours locates between that for the single SrFe12O19 ferrite (48.5 Am2/kg) and the single Ni(0.5)Zn(0.5)Fe2O4 ferrite (69.3 Am2/kg). In particular, the Mr value 31.5 Am2/kg for the SrFe12O19/Ni(0.5)Zn(0.5)Fe2O4 composite ferrite nanofibers is much higher than that for the individual SrFe12O19 (25.9 Am2/kg) and Ni(0.5)Zn(0.5)Fe2O4 ferrite (11.2 Am2/kg). These enhanced magnetic properties for the composite ferrite nanofibers can be attributed to the exchange-coupling interaction in the composite.

9.
J Colloid Interface Sci ; 354(1): 413-6, 2011 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-21144534

RESUMO

The nanocomposite SrFe(12)O(19)/Ni(0.5)Zn(0.5)Fe(2)O(4) ferrite aligned hollow microfibers with the hollow diameter to the fiber diameter estimated about 3/5 have been prepared by the gel precursor transformation process. The nanocomposite binary ferrites with different mass ratios are formed after the precursor calcined at 900°C for 2h, fabricating from SrFe(12)O(19) nanoparticles and Ni(0.5)Zn(0.5)Fe(2)O(4) nanoparticles with a uniform phase distribution. These nanocomposite ferrite microfibers show a combination of magnetic characteristics for the hard (SrFe(12)O(19)) and soft (Ni(0.5)Zn(0.5)Fe(2)O(4)) phase with an enhanced remanence owing to the exchange-coupling interactions. The aligned microfibers exhibit a shape anisotropy.

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