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1.
Angew Chem Int Ed Engl ; 62(34): e202305397, 2023 Aug 21.
Artigo em Inglês | MEDLINE | ID: mdl-37394690

RESUMO

Capacitive analogues of semiconductor diodes (CAPodes) present a new avenue for energy-efficient and nature-inspired next-generation computing devices. Here, we disclose the generalized concept for bias-direction-adjustable n- and p-CAPodes based on selective ion sieving. Controllable-unidirectional ion flux is realized by blocking electrolyte ions from entering sub-nanometer pores. The resulting CAPodes exhibit charge-storage characteristics with a high rectification ratio (96.29 %). The enhancement of capacitance is attributed to the high surface area and porosity of an omnisorbing carbon as counter electrode. Furthermore, we demonstrate the use of an integrated device in a logic gate circuit architecture to implement logic operations ('OR', 'AND'). This work demonstrates CAPodes as a generalized concept to achieve p-n and n-p analogue junctions based on selective ion electrosorption, provides a comprehensive understanding and highlights applications of ion-based diodes in ionologic architectures.

2.
Angew Chem Int Ed Engl ; 62(13): e202217473, 2023 Mar 20.
Artigo em Inglês | MEDLINE | ID: mdl-36738169

RESUMO

Atomically dispersed metal catalysts show potential advantages in N2 reduction reaction (NRR) due to their excellent activity and efficient metal utilization. Unfortunately, the reported catalysts usually exhibit unsatisfactory NRR activity due to their poor N2 adsorption and activation. Herein, we report a novel Sn atomically dispersed protuberance (ADP) by coordination with substrate C and O to induce positive charge accumulation on Sn site for improving its N2 adsorption, activation and NRR performance. The extended X-ray absorption fine structure (EXAFS) spectra confirmed the local coordination structure of the Sn ADPs. NRR activity was significantly promoted via Sn ADPs, exhibiting a remarkable NH3 yield (RNH3 ) of 28.3 µg h-1 mgcat -1 (7447 µg h-1 mgSn -1 ) at -0.3 V. Furthermore, the enhanced N2 Hx intermediates was verified by in situ experiments, yielding consistent results with DFT calculation. This work opens a new avenue to regulate the activity and selectivity of N2 fixation.

3.
Angew Chem Int Ed Engl ; 61(50): e202212250, 2022 12 12.
Artigo em Inglês | MEDLINE | ID: mdl-36260635

RESUMO

Switchable supercapacitors (SCs) enable a reversible electrically-driven uptake/release of bioactive ions by polarizing porous carbon electrodes. Herein we demonstrate the first example of a bioactive ion-based switchable supercapacitor. Based on choline chloride and porous carbons we unravel the mechanism of physisorption vs. electrosorption by nuclear magnetic resonance, Raman, and impedance spectroscopy. Weak physisorption facilitates electrically-driven electrolyte depletion enabling the controllable uptake/release of electrolyte ions. A new 4-terminal device is proposed, with a main capacitor and a detective capacitor for monitoring bioactive ion adsorption in situ. Ion-concentration control in printed choline-based switchable SCs realizes switching down to 8.3 % residual capacitance. The exploration of adsorption mechanisms in printable microdevices will open an avenue of manipulating bioactive ions for the application of drug delivery, neuromodulation, or neuromorphic devices.


Assuntos
Carbono , Eletrólitos , Capacitância Elétrica , Íons , Eletrodos , Carbono/química
4.
J Hazard Mater ; 404(Pt B): 124113, 2021 02 15.
Artigo em Inglês | MEDLINE | ID: mdl-33068998

RESUMO

This work demonstrated that electroplating sludges (EPS) of specific composition may be used for the synthesis of layered double hydroxide (LDH) materials for energy applications after appropriate treatment. The unique composition and structure of EPS render it with good electrochemical energy storage performance. The EPS containing Ni, Fe, and Al was dissolved by acid and added with urea precipitator. The LDH material was prepared by a facile hydrothermal method. The increase of urea in a certain range is conducive to the formation of intact LDH. However excessive urea levels promoted the transformation from LDH to Ni(HCO3)2. Various active Ni bridged by N in ‒O‒CN promoted electron transfer, ‒O‒CN content in LDHs was proportional to the urea amount. The prepared LDHs exhibited a specific capacitance of 1652.20 F g-1 at 0.5 A g-1, and the value remained at 766.69 F g-1 after 1000 cycles. The prepared LDH has excellent supercapacitor performance, which is closely related to its structure. Therefore, the proposed recycling strategy of EPS resources can be used to prepare LDH supercapacitors, paving the way for new applications of EPS in the field of energy storage.

5.
J Hazard Mater ; 359: 365-372, 2018 10 05.
Artigo em Inglês | MEDLINE | ID: mdl-30048951

RESUMO

Organophosphorus pesticides (OPs) have been widely used to control agricultural insects. Soil acidification is a major problem in soil of intensive agricultural systems, especially in red soil with a low pH buffer capacity. However, the effects of soil acidification on the toxicity of pesticides are still unclear. In the present study, the toxicity of three OPs on E. fetida was determined at individual (14-day lethal test) and biochemical levels (antioxidative defence enzymes) by using acidified soils (pH = 5.5, 4.3 and 3.1). The results showed that the toxicity of tested OPs was slightly increased with the decrease of soil pH. To interpret the phenomena, an optimum Quantitative Structure Activity Relationship (QSAR) model was developed based on the toxicity mechanism and the partial least squares regression (PLS) method. The model indicated bioavailability and toxicodynamics are key factors of soil acidification affecting the toxicity of the OPs. Further results revealed the bioavailability of the OPs was strongly related to their hydrolysis and biodegradation character, whereas the effects of soil acidification on toxicodynamics were mainly caused by the interaction between the acetylcholinesterase (AchE) and the OPs. Results will increase understanding of the effects of soil acidification on the toxicity of pesticides and its mechanism.


Assuntos
Oligoquetos/efeitos dos fármacos , Compostos Organofosforados/toxicidade , Praguicidas/toxicidade , Solo/química , Animais , Biodegradação Ambiental , Disponibilidade Biológica , Concentração de Íons de Hidrogênio , Hidrólise , Compostos Organofosforados/química , Compostos Organofosforados/metabolismo , Praguicidas/química , Praguicidas/metabolismo , Relação Quantitativa Estrutura-Atividade , Microbiologia do Solo
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