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1.
Nanoscale ; 16(14): 7076-7084, 2024 Apr 04.
Artigo em Inglês | MEDLINE | ID: mdl-38482599

RESUMO

The development of advanced multi-functional electrocatalysts and their industrial operation on paired electrocatalysis systems presents a promising avenue for the gradual penetration of renewable energy into practical production. Herein, a self-supported conductive network of silverene nanobelts (Ag-ene NBs) was delicately assembled (Ag-NB-NWs), in which ultralong and few-atom-layer Ag-ene NBs with a high edge-to-facet ratio were interconnected, serving as "superreactors" for electron transfer and mass transport during the reaction. Such superstructures as electrocatalysts delivered an unparalleled performance toward the CO2-to-CO conversion with exclusively high faradaic efficiency (FE) and partial current densities of up to 1 A cm-2. Remarkably, the membrane electrode assembly (MEA) cell with Ag-NB-NWs as the cathode was capable of ultrastable and continuous operation for over 240 h at 0.4 A with ∼100% selectivity. More importantly, by further using Ag-NB-NWs as a bifunctional electrocatalyst, a record-low voltage overall CO2 electrolysis system coupling cathodic CO2 reduction with anodic formaldehyde oxidation in MEA cell was performed to achieve concurrent feed gas generation and formate production, substantially improving electrochemical techno-economic feasibility.

2.
Sci Bull (Beijing) ; 66(7): 708-719, 2021 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-36654446

RESUMO

Zinc-air batteries (ZnABs) with high theoretical capacity and environmental benignity are the most promising candidates for next-generation electronics. However, their large-scale applications are greatly hindered due to the lack of high-efficient and cost-effective electrocatalysts. Transition metal phosphides (TMPs) have been reported as promising electrocatalysts. Notably, (Ni1-xCrx)2P (0 ≤ x ≤ 0.15) is an unstable electrocatalyst, which undergoes in-situ electrochemical oxidation during the initial oxygen evolution reaction (OER) and even in the activation cycles, and is eventually converted to Cr-NiOOH serving as the actual OER active sites with high efficiency. Density functional theory (DFT) simulations and experimental results elucidate that the OER performance could be significantly promoted by the synergistic effect of surface engineering and electronic modulations by Cr doping and in-situ phase transformation. The constructed rechargeable ZnABs could stably cycle for more than 208 h at 5 mA cm-2, while the voltage degradation is negligible. Furthermore, the developed catalytic materials could be assembled into flexible and all-solid-state ZnABs to power wearable electronics with high performance.

3.
ACS Appl Mater Interfaces ; 12(49): 54637-54643, 2020 Dec 09.
Artigo em Inglês | MEDLINE | ID: mdl-33226206

RESUMO

Hybrid polymer electrolytes with excellent performance at high temperatures are very promising for developing solid-state lithium batteries for high-temperature applications. Herein, we use a self-supporting hydroxyapatite (HAP) nanowire membrane as a filler to improve the performance of a poly(ethylene oxide) (PEO)-based solid-state electrolyte. The HAP membrane could comprehensively improve the properties of the hybrid polymer electrolyte, including the higher room-temperature ionic conductivity of 1.05 × 10-5 S cm-1, broad electrochemical windows of up to 5.9 V at 60 °C and 4.9 V at 160 °C, and a high lithium-ion migration of 0.69. In addition, the LiFePO4//Li full battery with a solid electrolyte possesses good rate capability, cycling, and Coulomb efficiency at extreme high temperatures, that is, after 300 continuous charge and discharge cycles at 4 C rate, the discharge capacity retention rate is 77% and the Coulomb efficiency is 99%. The use of the flexible self-supporting HAP nanowire membrane to improve the PEO-based solid composite electrolyte provides new strategies and opportunities for developing rechargeable lithium batteries in extreme high-temperature applications.

4.
ACS Appl Mater Interfaces ; 9(3): 2500-2508, 2017 Jan 25.
Artigo em Inglês | MEDLINE | ID: mdl-27996237

RESUMO

Water splitting is one of the ideal technologies to meet the ever increasing demands of energy. Many materials have aroused great attention in this field. The family of nickel-based sulfides is one of the examples that possesses interesting properties in water-splitting fields. In this paper, a controllable and simple strategy to synthesize nickel sulfides was proposed. First, we fabricated NiS2 hollow microspheres via a hydrothermal process. After a precise heat control in a specific atmosphere, NiS porous hollow microspheres were prepared. NiS2 was applied in hydrogen evolution reaction (HER) and shows a marvelous performance both in acid medium (an overpotential of 174 mV to achieve a current density of 10 mA/cm2 and the Tafel slope is only 63 mV/dec) and in alkaline medium (an overpotential of 148 mV to afford a current density of 10 mA/cm2 and the Tafel slope is 79 mV/dec). NiS was used in oxygen evolution reaction (OER) showing a low overpotential of 320 mV to deliver a current density of 10 mA/cm2, which is meritorious. These results enlighten us to make an efficient water-splitting system, including NiS2 as HER catalyst in a cathode and NiS as OER catalyst in an anode. The system shows high activity and good stabilization. Specifically, it displays a stable current density of 10 mA/cm2 with the applying voltage of 1.58 V, which is a considerable electrolyzer for water splitting.

5.
Nanoscale ; 4(21): 6786-91, 2012 Nov 07.
Artigo em Inglês | MEDLINE | ID: mdl-23001031

RESUMO

Nickel cobalt oxides with various Ni/Co ratios were synthesized using a facile template-free approach for electrochemical supercapacitors. The texture and morphology of the nanocomposites were characterized by powder X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and Brunauer-Emmett-Teller analysis (BET). The results show that a hierarchical porous structure assembled from nanoflakes with a thickness of ∼10 nm was obtained, and the ratio of nickel to cobalt in the nanocomposites was very close to the precursors. Cyclic voltammetry (CV) and galvanostatic charge and discharge tests were carried out to study the electrochemical performance. Both nickel cobalt oxides (Ni-Co-O-1 with Ni : Co = 1, Ni-Co-O-2 with Ni : Co = 2) outperform pure NiO and Co(3)O(4). The Ni-Co-O-1 and Ni-Co-O-2 possess high specific capacities of 778.2 and 867.3 F g(-1) at 1 A g(-1) and capacitance retentions of 84.1% and 92.3% at 10 A g(-1), respectively. After full activation, the Ni-Co-O-1 and Ni-Co-O-2 could achieve a maximum value of 971 and 1550 F g(-1) and remain at ∼907 and ∼1450 F g(-1) at 4 A g(-1), respectively. Also, the nickel cobalt oxides show high capacity retention when fast charging.

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