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1.
Phys Rev Lett ; 133(9): 096803, 2024 Aug 30.
Artículo en Inglés | MEDLINE | ID: mdl-39270175

RESUMEN

The efficient detection of the Néel vector in antiferromagnets is one of the prerequisites toward antiferromagnetic spintronic devices and remains a challenging problem. Here, we propose that the layer Hall effect can be used to efficiently detect the Néel vector in centrosymmetric magnetoelectric antiferromagnets. Thanks to the robust surface magnetization of magnetoelectric antiferromagnets, the combination of sizable exchange field and an applied electric field results in the layer-locked spin-polarized band edges. Moreover, the Berry curvature can be engineered efficiently by an electric field, which consequently gives rise to the layer-locked Berry curvature responsible for the layer Hall effect. Importantly, it is demonstrated that the layer Hall conductivity strongly depends on the Néel vector orientation and exhibits rich electromagnetic responses, which can be used to detect the Néel vector reversal. Based on density functional theory calculations, we exemplify those phenomena in the prototypical Cr_{2}O_{3} compound. A complete list of the magnetic point groups sustaining the layer Hall effect is presented, aiding the search for realistic materials. Our work proposes a novel approach to detect the Néel vector and holds great promise for antiferromagnetic spintronic applications.

2.
J Phys Chem Lett ; 15(38): 9787-9794, 2024 Sep 26.
Artículo en Inglés | MEDLINE | ID: mdl-39323367

RESUMEN

Organic materials with thermally activated delayed fluorescence (TADF) and room-temperature phosphorescence (RTP) dual emission have attracted great attention in recent years, but the regulation mechanism via internal and external heavy atoms is not clear enough. Here, we carry out a systematic theoretical investigation on the photophysical properties of the materials by introducing aliphatic or aromatic bromine atoms. The molecule with aromatic bromine atoms exhibits obvious TADF owing to the effective reverse intersystem crossing (RISC) with matchable energy levels and enhanced spin orbit couplings, the molecule with aliphatic bromine atoms shows a long RTP lifetime because of the reduced nonradiative transition of triplet excitons, and the molecule with both aliphatic and aromatic bromine atoms presents balanced TADF and RTP emissions thanks to the synergy internal and external heavy-atom effects. Besides, the internal and external heavy atoms induce multisite intermolecular interactions, effectively suppressing the nonradiative process in the solid phase. The efficient RISC process and the suppressed nonradiative process of triplet excitons should be key to regulating the dual emission property. These findings and insights are of great importance for revealing the structure-performance relationship, providing theoretical guidance for the design of TADF and RTP dual emission molecules via internal and external heavy-atom effects.

3.
Appl Environ Microbiol ; : e0094224, 2024 Sep 17.
Artículo en Inglés | MEDLINE | ID: mdl-39287396

RESUMEN

The biochemical and structural characteristics of PtLam, a laminarinase from deep-sea Planctomycetota, have been extensively elucidated, unveiling the fundamental molecular mechanisms governing substrate recognition and enzymatic catalysis. PtLam functions as an exo-laminarinase with the ability to sequentially hydrolyze laminarin, cleaving glucose units individually. Notably, PtLam exhibits proficient transglycosylation capabilities, utilizing various sugar alcohols as acceptors, with lyxose, in particular, yielding exclusively transglycosylated products. Structural analysis of both apo-PtLam and its laminarin oligosaccharide-bound complex revealed significant conformational alterations in active residues upon substrate binding. Moreover, pivotal residues involved in substrate recognition were identified, with subsequent mutation assays indicating the contribution of positive subsites in modulating exo-hydrolysis and transglycosidic activities. These results enhance our comprehension of laminarin cycling mechanisms by marine Planctomycetota, while also providing essential enzyme components for laminarin hetero-oligosaccharide synthesis.IMPORTANCEThe ubiquitous Planctomycetota, with distinctive physiological traits, exert a significant influence on global carbon and nitrogen fluxes. Their intimate association with algae suggests a propensity for efficient polysaccharide degradation; however, research on glycoside hydrolases derived from Planctomycetota remains scarce. Herein, we unveil the GH16 family laminarinase PtLam from deep-sea Planctomycetota, shedding light on its catalytic mechanisms underlying hydrolysis and transglycosylation. Our findings elucidate the enzymatic pathways governing the marine laminarin cycle orchestrated by Planctomycetota, thereby fostering the exploration of novel polysaccharide hydrolases with promising practical implications.

4.
Angew Chem Int Ed Engl ; : e202412821, 2024 Aug 06.
Artículo en Inglés | MEDLINE | ID: mdl-39105426

RESUMEN

The rational manipulation of the surface reconstruction of catalysts is a key factor in achieving highly efficient water oxidation, but it is a challenge due to the complex reaction conditions. Herein, we introduce a novel in situ reconstruction strategy under a gradient magnetic field to form highly catalytically active species on the surface of ferromagnetic/paramagnetic CoFe2O4@CoBDC core-shell structure for electrochemical oxygen evolution reaction (OER). We demonstrate that the Kelvin force from the cores' local gradient magnetic field modulates the shells' surface reconstruction, leading to a higher proportion of Co2+ as active sites. These Co sites with optimized electronic configuration exhibit more favorable adsorption energy for oxygen-containing intermediates and lower the activation energy of the overall catalytic reaction. As a result, a significant enhancement in OER performance is achieved with a large current density increment about 128 % at 1.63 V and an overpotential reduction by 28 mV at 10 mA cm-2 after reconstruction. Interestingly, after removing the external magnetic field, the activity could persist for over 100 h. This work showcases the directional surface reconstruction of catalysts under a gradient magnetic field for enhanced water oxidation.

5.
ACS Appl Mater Interfaces ; 16(21): 27813-27820, 2024 May 29.
Artículo en Inglés | MEDLINE | ID: mdl-38603540

RESUMEN

Solar-blind photodetectors based on wide bandgap semiconductors have recently attracted a lot of interest. Nickel-containing spinel phase oxides, such as NiAl2O4, are stable p-type semiconductors. This paper describes a multifunctional solar-blind photodetector based on a NiAl2O4/4H-SiC heterojunction that utilizes photovoltaic effects. The position sensitivity reaches a value of 1589.7 mV/mm under 405 nm laser illumination, while the relaxation times of vertical photovoltaic (VPV) effect and lateral photovoltaic (LPV) effect under 266 nm laser illumination are only 0.32 and 0.42 µs, respectively. This junction was used to create a space optical communication system with sunlight having little effect on its optoelectronic properties. The ultrafast photovoltaic relaxation time makes NiAl2O4/4H-SiC a promising candidate for self-powered high-performance solar-blind detectors.

6.
Environ Sci Ecotechnol ; 20: 100405, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38544949

RESUMEN

The ubiquity of refractory organic matter in aquatic environments necessitates innovative removal strategies. Sulfate radical-based advanced oxidation has emerged as an attractive solution, offering high selectivity, enduring efficacy, and anti-interference ability. Among many technologies, sulfite activation, leveraging its cost-effectiveness and lower toxicity compared to conventional persulfates, stands out. Yet, the activation process often relies on transition metals, suffering from low atom utilization. Here we introduce a series of single-atom catalysts (SACs) employing transition metals on g-C3N4 substrates, effectively activating sulfite for acetaminophen degradation. We highlight the superior performance of Fe/CN, which demonstrates a degradation rate constant significantly surpassing those of Ni/CN and Cu/CN. Our investigation into the electronic and spin polarization characteristics of these catalysts reveals their critical role in catalytic efficiency, with oxysulfur radical-mediated reactions predominating. Notably, under visible light, the catalytic activity is enhanced, attributed to an increased generation of oxysulfur radicals and a strengthened electron donation-back donation dynamic. The proximity of Fe/CN's d-band center to the Fermi level, alongside its high spin polarization, is shown to improve sulfite adsorption and reduce the HOMO-LUMO gap, thereby accelerating photo-assisted sulfite activation. This work advances the understanding of SACs in environmental applications and lays the groundwork for future water treatment technologies.

7.
ACS Appl Mater Interfaces ; 16(8): 10138-10147, 2024 Feb 28.
Artículo en Inglés | MEDLINE | ID: mdl-38364211

RESUMEN

Enhancing the reaction selectivity for multicarbon products (C2+) is an important goal for the electrochemical CO(2) reduction (ECO(2)R) process. Cuprous compounds have demonstrated promising C2+ selectivity in the ECO(2)R process, but further investigation is necessary to thoroughly elucidate their catalytic behavior toward C2+ oxygenate production. In this study, copper nitride-based materials with varying reduction rates were employed as precatalysts. Consequently, a relationship between the selectivity toward C2+ oxygenates and the Cu oxidation state during the ECOR process is established. Results of theoretical and experimental analyses reveal that the Cu0/Cu+ interface plays a key role in enhancing *CO adsorption while lowering the formation energy of *CH2CO, thereby promoting acetate production. This work highlights the significance of the Cu0/Cu+ interface in the regulation of C2+ oxygenate production and paves the way for the development of highly selective catalysts in the future.

8.
Inorg Chem ; 63(9): 4312-4327, 2024 Mar 04.
Artículo en Inglés | MEDLINE | ID: mdl-38354197

RESUMEN

It is crucial to eliminate CO emissions using non-noble catalysts. Cu-based catalysts have been widely applied in CO oxidation, but their activity and stability at low temperatures are still challenging. This study reports the preparation and application of an efficient copper-doped ceria electrospun fiber catalyst prepared by a facile electrospinning method. The obtained 10Cu-Ce fiber catalyst achieved complete CO oxidation at a temperature as low as 90 °C. However, a reference 10Cu/Ce catalyst prepared by the impregnation method needed 110 °C to achieve complete CO oxidation under identical reaction conditions. Asymmetric oxygen vacancies (ASOV) at the interface between copper and cerium were constructed, to effectively absorb gas molecules involved in the reaction, leading to the enhanced oxidation of CO. The exceptional ability of the 10Cu-Ce catalyst to adsorb CO is attributed to its unique structure and surface interaction phase Cu+-Ov-Ce3+, as demonstrated by a series of characterizations and DFT calculations. This novel approach of using electrospinning offers a promising technique for developing low-temperature and non-noble metal-based catalysts.

9.
Appl Opt ; 62(24): 6528-6533, 2023 Aug 20.
Artículo en Inglés | MEDLINE | ID: mdl-37706847

RESUMEN

A large lateral photovoltaic effect (LPE) with a fast optical response time is necessary to develop high-performance position-sensitive detectors. In this paper, we report an LPE with a high self-powered position sensitivity and ultrafast optical relaxation time in S n S 2/n-S i junctions prepared using pulsed laser deposition. A large built-in electric field was generated at the S n S 2/S i interface, which resulted in a large LPE with a positional sensitivity of up to 116 mV/mm. Furthermore, the measurement circuit with multiple parallel resistors had a strong influence on the ultrafast optical response time of the LPE and the fastest optical relaxation time observed was ∼0.44µs. Our results suggest that the S n S 2/S i junction would be a promising candidate for a wide range of optoelectronic device applications.

10.
Small ; 19(15): e2206940, 2023 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-36604989

RESUMEN

It is indispensable to develop and design high capacity, high rate performance, long cycling life, and low-cost electrodes materials for lithium-ion batteries (LIBs) and sodium-ion batteries (SIBs). Herein, MoO2 /MoS2 /C, with dual heterogeneous interfaces, is designed to induce a built-in electric field, which has been proved by experiments and theoretical calculation can accelerate electrochemical reaction kinetics and generate interfacial interactions to strengthen structural stability. The carbon foam serves as a conductive frame to assist the movement of electrons/ions, as well as forms heterogeneous interfaces with MoO2 /MoS2 through CS and CO bonds, maintaining structural integrity and enhancing electronic transport. Thanks to these unique characteristics, the MoO2 /MoS2 /C renders a significantly enhanced electrochemical performance (324 mAh g-1 at 1 A g-1 after 1000 cycles for SIB and 500 mAh g-1 at 1 A g-1 after 500 cycles for LIBs). The current work presents a simple, useful and cost-effective route to design high-quality electrodes via interfacial engineering.

11.
ACS Appl Mater Interfaces ; 15(1): 1505-1512, 2023 Jan 11.
Artículo en Inglés | MEDLINE | ID: mdl-36548398

RESUMEN

CsPbBr3, an inorganic halide perovskite, has attracted great interest in recent years due to its excellent photoelectric properties. In this paper, we report a high-performance position-sensitive detector and laser communication sensor based on a CsPbBr3/4H-SiC heterojunction that effectively exploits the lateral photovoltaic (LPV) effect. The X-ray diffraction, X-ray photoelectron spectra, and photoluminescence data indicate that a high-quality CsPbBr3 film has been successfully obtained using pulsed laser deposition. The thickness of the CsPbBr3 film is shown to play a key role in the open-circuit voltage and linear LPV. A large position sensitivity (up to 827 mV/mm) of the LPV with a fast relaxation time is observed. Moreover, the shortest relaxation time of only 0.34 µs for 532 nm laser irradiation among counterparts is achieved in the detector under consideration. Furthermore, the position sensitivity and relaxation time of the LPV in the CsPbBr3/4H-SiC heterojunction show a weak dependence on the laser wavelength from 266 to 532 nm. The robust characteristics of fast relaxation time and high position sensitivity of the LPV make the CsPbBr3 junction a promising candidate for both laser communication sensors and self-powered high-performance position-sensitive detectors.

12.
Rev. bras. med. esporte ; 29: e2022_0734, 2023. tab, graf
Artículo en Inglés | LILACS-Express | LILACS | ID: biblio-1423510

RESUMEN

ABSTRACT Introduction: The stroke in tennis is a closed chain kinetic energy transfer starting from the lower limbs, through the trunk, to the upper limbs, and finally to the ball, requiring an upward coordinated muscular explosion. Due to its complex nature, it is believed that technical training can improve stability and accuracy in its players. Objective: Analyze the impacts of technical training on the physical fitness of college tennis players. Methods: Twenty tennis players from a tennis team at a university were selected and divided into an experimental group and a control group. The experiment lasted eight weeks. The experimental group received a technical training protocol on tennis strokes, while the control group received traditional physical training. Results: The hand-striking ability of the experimental group increased from 6.47 ± 2.02 to 8.67 ± 1.39 after four weeks and 10.56 ± 2.03 after eight weeks of training, while the control group increased from 4.42 ± 1.08 to 5.02 ± 0.59 in 4 weeks and 6.82 ± 1.46 after eight weeks of training. Conclusion: The application of technical movement training associated with traditional protocols is recommended to improve the physical fitness of athletes. Level of evidence II; Therapeutic studies - investigation of treatment outcomes.


RESUMO Introdução: O golpe no tênis é uma transferência de energia cinética em cadeia fechada partindo dos membros inferiores, através do tronco, para os membros superiores e finalmente para a bola, exigindo uma explosão muscular coordenada ascendente. Devido a sua natureza complexa, acredita-se que um treinamento técnico possa melhorar a estabilidade e precisão em seus jogadores. Objetivo: Analisar os impactos do treino técnico sobre a aptidão física de tenistas universitários. Métodos: Foram selecionados 20 tenistas de uma equipe de tênis em uma universidade, divididos em grupo experimental e grupo de controle. O experimento durou 8 semanas. O grupo experimental recebeu um protocolo de treinamento técnico em golpes de tênis, enquanto o grupo de controle recebeu o treinamento físico tradicional. Resultados: A habilidade de golpe manual do grupo experimental aumentou de 6,47 ± 2,02 para 8,67 ± 1,39 após 4 semanas e 10,56 ± 2,03 após 8 semanas de treinamento; enquanto o grupo controle aumentou de 4,42 ± 1,08 para 5,02 ± 0,59 em 4 semanas e 6,82 ± 1,46 após 8 semanas de treinamento. Conclusão: Recomenda-se a aplicação do treinamento de movimentos técnicos associados aos protocolos tradicionais, a fim de melhorar a aptidão física dos atletas. Nível de evidência II; Estudos terapêuticos - investigação dos resultados do tratamento.


RESUMEN Introducción: El golpe en el tenis es una transferencia de energía cinética en cadena cerrada que parte de los miembros inferiores, pasa por el tronco, llega a los miembros superiores y finalmente a la pelota, lo que requiere una explosión muscular coordinada ascendente. Debido a su naturaleza compleja, se cree que el entrenamiento técnico puede mejorar la estabilidad y la precisión de sus jugadores. Objetivo: Analizar las repercusiones del entrenamiento técnico en la aptitud física de los tenistas universitarios. Métodos: Se seleccionaron 20 tenistas de un equipo de tenis de una universidad y se dividieron en un grupo experimental y un grupo de control. El experimento duró 8 semanas. El grupo experimental recibió un protocolo de entrenamiento técnico sobre golpes de tenis, mientras que el grupo de control recibió entrenamiento físico tradicional. Resultados: La capacidad de golpeo con las manos del grupo experimental aumentó de 6,47 ± 2,02 a 8,67 ± 1,39 tras 4 semanas y a 10,56 ± 2,03 tras 8 semanas de entrenamiento; mientras que la del grupo de control aumentó de 4,42 ± 1,08 a 5,02 ± 0,59 en 4 semanas y a 6,82 ± 1,46 tras 8 semanas de entrenamiento. Conclusión: Se recomienda la aplicación del entrenamiento técnico del movimiento asociado a protocolos tradicionales para mejorar la aptitud física de los deportistas. Nivel de evidencia II; Estudios terapéuticos - investigación de los resultados del tratamiento.

13.
Front Chem ; 10: 1021394, 2022.
Artículo en Inglés | MEDLINE | ID: mdl-36277343

RESUMEN

Contamination of phenolic compounds has devastating effects on the environment. Therefore, its harmless treatment and recycling have received extensive attention. Herein, a novel method for preparing N-S doped phenolic resin (NSPR) from phenols, N and S groups in semi-coking wastewater, and formaldehyde are developed. The KOH is consequently incorporated into the NSPR through simultaneous carbonization and activation in a single step to produce porous carbon material (NSPC). The as-obtained NSPC exhibits a high specific capacitance of 182 F g-1 at 0.5 A g-1, a high energy density of 9.1 Wh kg-1 at a power density of 0.15 kW kg-1, and remarkable cycling stability in aqueous KOH electrolyte. This outstanding electrochemical performance is attributed to its ultrahigh specific surface area (SSA, 2,523 m2 g-1), enormous total pore volume (Vt, 1.30 cm3 g-1), rational pore structure, and N-S heteroatom self-doping (0.76 at% N and 0.914 at% S), which ensures adequate charge storage, rapid electrolyte ion diffusion, and contributed pseudo-capacitance. This work not only provides a facile method for transforming phenolic wastewater into high-value products but also offers a cost-effective and high-performance porous carbon material for supercapacitors.

14.
ACS Appl Mater Interfaces ; 14(32): 36688-36699, 2022 Aug 17.
Artículo en Inglés | MEDLINE | ID: mdl-35930060

RESUMEN

Precious metals (Pt, Ir, Ru, and so on) and related compounds usually demonstrate superb catalytic activity for electrochemical hydrogen production. However, scarcity and stability are still challenges for hydrogen evolution reaction, even for single-atomic-site electrocatalysts. Herein, a fluorine (F) doping strategy is proposed to enhance the strong metal-support interaction between the F-doped Ni3N support and the loaded ruthenium (Ru) species. Via synergistically modulating both the Ru loading amount and F doping concentration, outstanding HER activity was achieved in Ru@F-Ni3N with an overpotential (η) of 115 mV at 100 mA cm-2, superior to the benchmark Pt/C (η = 201 mV). Density functional theory simulation in combination with X-ray photoelectron spectra and X-ray absorption spectroscopy characterizations convincingly demonstrate that, with the strongest electronegativity, F doping could effectively stabilize Ru atoms doped in the F-Ni3N substrate and simultaneously reduce the H bonding strength, which accelerated the desorption of H2. These findings provide a facile strategy to modulate both catalytic activities and stabilities of heteroatom-loaded catalytic materials.

15.
J Phys Chem Lett ; 13(32): 7476-7482, 2022 Aug 18.
Artículo en Inglés | MEDLINE | ID: mdl-35939648

RESUMEN

Spin polarization modulation in ferromagnetic materials has become an effective way to promote the electrocatalytic oxygen evolution reaction (OER). Herein, to reveal the coercivity-related OER performance, single-domain ferromagnetic CoFe2O4 (CFO) nanocrystals with different coercivities are synthesized and subjected to OER under an in situ tunable magnetic field. As the more ordered spin polarization state of CFO with a higher coercivity can afford a facilitated electron transfer process, the magnetic field-assisted OER activity can be more improved with an increase in coercivity. Specifically, the decreased magnitudes of the overpotential, Tafel slope, and charge transfer resistance increase on the samples with higher coercivity. The CFO with the largest coercivity (7500 Oe) shows the best OER performance with an overpotential of 350 mV at a current density of 10 mA cm-2 under a magnetic field of 14000 G. In addition, a hysteresis effect that maintains enhanced OER current density after the magnetic field has been withdrawn is observed, where higher coercivity affords a longer hysteresis period. The exploration of coercivity-related OER enhancement may provide new insights into the design and synthesis of promising "magnetic effect" catalysts.

16.
Materials (Basel) ; 15(11)2022 May 29.
Artículo en Inglés | MEDLINE | ID: mdl-35683174

RESUMEN

Designing a high-strength node is significant for space structures. Topological optimization can optimally allocate the material distribution of components to meet performance requirements. Although the material distribution after topology optimization is optimum, the structure becomes complicated to manufacture. By using additive manufacturing technology, this problem can be well solved. At present, both topology optimization technology and additive manufacturing technology are quite mature, but their application in the design of spatial nodes is very recent and less researched. This paper involves the study and improvement of the node optimization design-manufacturing integrated method. This study used the BESO optimization algorithm as the research algorithm. Through a reasonable improvement of the material interpolation method, the algorithm's dependence on the experience of selecting the material penalty index P was reduced. On this basis, the secondary development was carried out, and a multisoftware integration was carried out for optimization and manufacturing. The spatial node was taken as the research object, and the calculation results of the commercial finite element software were compared. The comparison showed that the algorithm used in this paper was better. Not only was it not trapped in a local optimum, but the maximum stress was also lower. In addition, this paper proposed a practical finite element geometric model extraction method and smoothing of the optimized nodes, completing the experiment of the additive manufacturing forming of the nodes. It provides ideas for processing jagged edges brought by the BESO algorithm. This paper verified the feasibility of the multisoftware integration method of optimized manufacturing.

17.
Small Methods ; 6(6): e2200084, 2022 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-35460208

RESUMEN

Here, a strategy to regulate the electron density distribution by integrating NiFe layered double hydroxides (NiFe-LDH) nanosheets with Co3 O4 nanowires to construct the NiFe-LDH/Co3 O4 p-n heterojunction supported on nickel foam (NiFe-LDH/Co3 O4 /NF) for electrocatalytic oxygen evolution reaction (OER) is proposed. The p-n heterojunction can induce the charge redistribution in the heterogeneous interface to reach Fermi level alignment, thus modifying the adsorption free energy of *OOH and improving the intrinsic activity of the catalyst. As a result, NiFe-LDH/Co3 O4 /NF exhibits outstanding OER performance with a low overpotential of 274 mV at a current density of 50 mA cm-2 and long-time stability over 90 h. Moreover, NF can serve as a magnetic core that induces the exchange bias effect between the magnetic substrate and the active species under the action of the magnetic field, resulting in decreased magnetoresistance and weakened scattering of spin electrons, which further lowers the OER overpotential by 25 mV @ 50 mA cm-2 under a 10 000 G magnetic field. This work provides a new perspective on the design of p-n heterojunction catalysts and a deeper understanding of the magnetic field-enhanced electrocatalytic reactions.

18.
Molecules ; 28(1)2022 Dec 30.
Artículo en Inglés | MEDLINE | ID: mdl-36615510

RESUMEN

Water electrolysis offers a zero-carbon route to generate renewable energy conversion systems. Herein, a self-supported nickel phosphosulfide nanosheet (NS) electrocatalyst was fabricated at a low temperature on carbon cloth, which was then subjected to Ar etching to enhance its catalytic activity. Etching resulted in better hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) performance than other samples, with overpotentials of 103.1 mV (at 10 mA cm-2) and 278.9 mV (at 50 mA cm-2), respectively. The characterization results confirmed that Ar etching created a thin amorphous layer around the NiPS3 NSs, which increased the number of active sites and modulated their electronic structures. These 3D-structured NiPS3 NSs and their subsequent Ar etching process show promise for applications in overall water splitting in alkaline media.

19.
Nat Commun ; 12(1): 3036, 2021 May 24.
Artículo en Inglés | MEDLINE | ID: mdl-34031417

RESUMEN

Developing efficient and stable earth-abundant electrocatalysts for acidic oxygen evolution reaction is the bottleneck for water splitting using proton exchange membrane electrolyzers. Here, we show that nanocrystalline CeO2 in a Co3O4/CeO2 nanocomposite can modify the redox properties of Co3O4 and enhances its intrinsic oxygen evolution reaction activity, and combine electrochemical and structural characterizations including kinetic isotope effect, pH- and temperature-dependence, in situ Raman and ex situ X-ray absorption spectroscopy analyses to understand the origin. The local bonding environment of Co3O4 can be modified after the introduction of nanocrystalline CeO2, which allows the CoIII species to be easily oxidized into catalytically active CoIV species, bypassing the potential-determining surface reconstruction process. Co3O4/CeO2 displays a comparable stability to Co3O4 thus breaks the activity/stability tradeoff. This work not only establishes an efficient earth-abundant catalysts for acidic oxygen evolution reaction, but also provides strategies for designing more active catalysts for other reactions.

20.
Angew Chem Int Ed Engl ; 60(1): 259-267, 2021 Jan 04.
Artículo en Inglés | MEDLINE | ID: mdl-32964599

RESUMEN

To ensure sustainable hydrogen production by water electrolysis, robust, earth-abundant, and high-efficient electrocatalysts are required. Constructing a hybrid system could lead to further improvement in electrocatalytic activity. Interface engineering in composite catalysts is thus critical to determine the performance, and the phase-junction interface should improve the catalytic activity. Here, we show that nickel diphosphide phase junction (c-NiP2 /m-NiP2 ) is an effective electrocatalyst for hydrogen production in alkaline media. The overpotential (at 10 mA cm-2 ) for NiP2 -650 (c/m) in alkaline media could be significantly reduced by 26 % and 96 % compared with c-NiP2 and m-NiP2 , respectively. The enhancement of catalytic activity should be attributed to the strong water dissociation ability and the rearrangement of electrons around the phase junction, which markedly improved the Volmer step and benefited the reduction process of adsorbed protons.

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