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1.
Chem Rev ; 124(11): 7045-7105, 2024 Jun 12.
Artículo en Inglés | MEDLINE | ID: mdl-38754042

RESUMEN

Ferroelectrics have become indispensable components in various application fields, including information processing, energy harvesting, and electromechanical conversion, owing to their unique ability to exhibit electrically or mechanically switchable polarization. The distinct polar noncentrosymmetric lattices of ferroelectrics make them highly responsive to specific crystal structures. Even slight changes in the lattice can alter the polarization configuration and response to external fields. In this regard, strain engineering has emerged as a prevalent regulation approach that not only offers a versatile platform for structural and performance optimization within ferroelectrics but also unlocks boundless potential in various functional materials. In this review, we systematically summarize the breakthroughs in ferroelectric-based functional materials achieved through strain engineering and progress in method development. We cover research activities ranging from fundamental attributes to wide-ranging applications and novel functionalities ranging from electromechanical transformation in sensors and actuators to tunable dielectric materials and information technologies, such as transistors and nonvolatile memories. Building upon these achievements, we also explore the endeavors to uncover the unprecedented properties through strain engineering in related chemical functionalities, such as ferromagnetism, multiferroicity, and photoelectricity. Finally, through discussions on the prospects and challenges associated with strain engineering in the materials, this review aims to stimulate the development of new methods for strain regulation and performance boosting in functional materials, transcending the boundaries of ferroelectrics.

2.
Nano Lett ; 24(10): 3118-3124, 2024 Mar 13.
Artículo en Inglés | MEDLINE | ID: mdl-38421801

RESUMEN

The magnetic and electric dipoles of ferroics play a central role in their fascinating properties. In particular, topological configurations have shown promising potential for use in novel electromechanical and electronic devices. Magnetic configurations from simple collinear to complex topological are well-documented. In contrast, many complex topological features in the electric counterpart remain unexplored. Here, we report the first example of three-dimensional electric dipole sinewave topological structure in a PbZrO3-based bulk perovskite, which presents an interesting triple-hysteresis loop macroscopically. This polar configuration consists of two orthogonal sinewave electric dipole modulations decoded from a polar incommensurate phase by advanced diffraction and atomic-resolution imaging techniques. The resulting topology is unraveled to be the competition between the antiferroelectric and ferroelectric states, stabilized by the modulation of the Pb 6s2 lone pair and the antiferrodistortive effect. These findings further reinforce the similarity of the magnetic and electric topologies.

3.
J Am Chem Soc ; 146(3): 1926-1934, 2024 Jan 24.
Artículo en Inglés | MEDLINE | ID: mdl-38193748

RESUMEN

Dielectric capacitors are highly desired in modern electronic devices and power systems to store and recycle electric energy. However, achieving simultaneous high energy density and efficiency remains a challenge. Here, guided by theoretical and phase-field simulations, we are able to achieve a superior comprehensive property of ultrahigh efficiency of 90-94% and high energy density of 85-90 J cm-3 remarkably in strontium titanate (SrTiO3), a linear dielectric of a simple chemical composition, by manipulating local symmetry breaking through introducing Ti/O defects. Atomic-scale characterizations confirm that these Ti/O defects lead to local symmetry breaking and local lattice strains, thus leading to the formation of the isolated ultrafine polar nanoclusters with varying sizes from 2 to 8 nm. These nanoclusters account for both considerable dielectric polarization and negligible polarization hysteresis. The present study opens a new realm of designing high-performance dielectric capacitors utilizing a large family of readily available linear dielectrics with very simple chemistry.

4.
J Am Chem Soc ; 146(1): 460-467, 2024 Jan 10.
Artículo en Inglés | MEDLINE | ID: mdl-38109256

RESUMEN

Dielectric ceramic capacitors with high recoverable energy density (Wrec) and efficiency (η) are of great significance in advanced electronic devices. However, it remains a challenge to achieve high Wrec and η parameters simultaneously. Herein, based on density functional theory calculations and local structure analysis, the feasibility of developing the aforementioned capacitors is demonstrated by considering Bi0.25Na0.25Ba0.5TiO3 (BNT-50BT) as a matrix material with large local polarization and structural distortion. Remarkable Wrec and η of 16.21 J/cm3 and 90.5% have been achieved in Bi0.25Na0.25Ba0.5Ti0.92Hf0.08O3 via simple chemical modification, which is the highest Wrec value among reported bulk ceramics with η greater than 90%. The examination results of local structures at lattice and atomic scales indicate that the disorderly polarization distribution and small nanoregion (∼3 nm) lead to low hysteresis and high efficiency. In turn, the drastic increase in local polarization activated via the ultrahigh electric field (80 kV/mm) leads to large polarization and superior energy storage density. Therefore, this study emphasizes that chemical design should be established on a clear understanding of the performance-related local structure to enable a targeted regulation of high-performance systems.

5.
Int Microbiol ; 2024 Jan 09.
Artículo en Inglés | MEDLINE | ID: mdl-38196020

RESUMEN

Sun-drying is a traditional process for preparing dried shrimp in coastal area of South China, but its impacts on nutrition and the formation of flavor-contributory substances in dried shrimp remain largely unknown. This study aimed to examine the effects of the production process on the microbiota and metabolites in dried shrimp. 16S rDNA amplicon sequencing was employed to identify 170 operational taxonomic units (OTUs), with Vibrio, Photobacterium, and Shewanella emerging as the primary pathogenic bacteria in shrimp samples. Lactococcus lactis was identified as the principal potential beneficial microorganism to accrue during the dried shrimp production process and found to contribute significantly to the development of desirable shrimp flavors. LC-MS-based analyses of dried shrimp sample metabolomes revealed a notable increase in compounds associated with unsaturated fatty acid biosynthesis, arachidonic acid metabolism, amino acid biosynthesis, and flavonoid and flavanol biosynthesis throughout the drying process. Subsequent exploration of the relationship between metabolites and bacterial communities highlighted the predominant coexistence of Bifidobacterium, Clostridium, and Photobacterium contributing heterocyclic compounds and metabolites of organic acids and their derivatives. Conversely, Arthrobacter and Staphylococcus were found to inhibit each other, primarily in the presence of heterocyclic compounds. This comprehensive investigation provides valuable insights into the dynamic changes in the microbiota and metabolites of dried shrimps spanning different drying periods, which we expect to contribute to enhancing production techniques and safety measures for dried shrimp processing.

6.
World J Surg Oncol ; 22(1): 38, 2024 Jan 30.
Artículo en Inglés | MEDLINE | ID: mdl-38287345

RESUMEN

BACKGROUND: Sarcopenia is associated with poor outcomes in many malignancies. However, the relationship between sarcopenia and the prognosis of pancreatic cancer has not been well understood. The aim of this meta-analysis was to identify the prognostic value of preoperative sarcopenia in patients with pancreatic cancer after curative-intent surgery. METHODS: Database from PubMed, Embase, and Web of Science were searched from its inception to July 2023. The primary outcomes were overall survival (OS), progression-free survival (PFS), and the incidence of major complications. The hazard ratio (HR), odds ratio (OR), and 95% confidence intervals (CIs) were used to assess the relationship between preoperative sarcopenia and the prognosis of patients with pancreatic cancer. All statistical analyses were conducted by Review Manager 5.3 and STATA 17.0 software. RESULTS: A total of 23 retrospective studies involving 5888 patients were included in this meta-analysis. The pooled results demonstrated that sarcopenia was significantly associated with worse OS (HR = 1.53, P < 0.00001) and PFS (HR = 1.55, P < 0.00001). However, this association was not obvious in regard to the incidence of major complications (OR = 1.33, P = 0.11). CONCLUSION: Preoperative sarcopenia was preliminarily proved to be associated with the terrible prognosis of pancreatic cancer after surgery. However, this relationship needs to be further validated in more prospective studies.


Asunto(s)
Neoplasias Pancreáticas , Sarcopenia , Humanos , Sarcopenia/complicaciones , Sarcopenia/diagnóstico , Estudios Prospectivos , Estudios Retrospectivos , Pronóstico , Neoplasias Pancreáticas/complicaciones , Neoplasias Pancreáticas/cirugía
7.
Nano Lett ; 23(3): 948-953, 2023 Feb 08.
Artículo en Inglés | MEDLINE | ID: mdl-36716221

RESUMEN

Electric-field-induced antiferroelectric-ferroelectric (AFE-FE) phase transition is a prominent feature of antiferroelectric (AFE) materials. The critical electric field of this phase transition is crucial for the device performance of AEFs in many applications, but the determining factor of the critical electric field is still unclear. Here, we have established the correlation between the underlying structure and the critical electric field by using in situ synchrotron X-ray diffraction and high-resolution neutron diffraction in Pb(Zr,Sn,Ti)O3-based antiferroelectrics. It is found that the critical electric field is determined by the angle between the average polarization vector in the incommensurate AFE state and the [111]P polarization direction in the rhombohedral FE state. A large polarization rotation angle gives rise to a large critical electric field. Further, density functional theory (DFT) calculations corroborate that the lower energy is required for driving a smaller angle polarization rotation. Our discovery will offer guidance to optimize the performance of AFE materials.

8.
Nano Lett ; 23(4): 1273-1279, 2023 Feb 22.
Artículo en Inglés | MEDLINE | ID: mdl-36729943

RESUMEN

Regulating the magnetic properties of multiferroics lays the foundation for their prospective application in spintronic devices. Single-phase multiferroics, such as rare-earth ferrites, are promising candidates; however, they typically exhibit weak magnetism at room temperature (RT). Here, we significantly boosted the RT ferromagnetism of a representative ferrite, EuFeO3, by oxygen defect engineering. Polarized neutron reflectometry and magnetometry measurements reveal that saturation magnetization reaches 0.04 µB/Fe, which is approximately 5 times higher than its bulk phase. Combining the annular bright-field images with theoretical assessment, we unravel the underlying mechanism for magnetic enhancement, in which the decrease in Fe-O-Fe bond angles caused by oxygen vacancies (VO) strengthens magnetic interactions and tilts Fe spins. Furthermore, the internal relationship between magnetism and VO was established by illustrating how the magnetic structure and magnitude change with VO configuration and concentration. Our strategy for regulating magnetic properties can be applied to numerous functional oxide materials.

9.
J Am Chem Soc ; 145(25): 13623-13631, 2023 Jun 28.
Artículo en Inglés | MEDLINE | ID: mdl-37327186

RESUMEN

Owing to their wide application in oxide-based electrochemical and energy devices, ion conductors have attracted considerable attention. However, the ionic conductivity of the developed systems is still too low to satisfy the low-temperature application. In this study, by developing the emergent interphase strain engineering method, we achieve a colossal ionic conductivity in SrZrO3-xMgO nanocomposite films, which is over one order of magnitude higher than that of the currently widely used yttria-stabilized zirconia below 673 K. Atomic-scale electron microscopy studies ascribe this superior ionic conductivity to the periodically well-aligned SrZrO3 and MgO nanopillars that feature coherent interfaces. Wherein, a tensile strain as large as +1.7% is introduced into SrZrO3, expanding the c-lattice and distorting the oxygen octahedra to decrease the oxygen migration energy. Combining with theoretical assessments, we clarify the strain-dependent oxygen migration path and energy and unravel the mechanisms for strain-tuned ionic conductivity. This study provides a new scope for the property improvement of wide-range ion conductors by strain engineering.

10.
J Am Chem Soc ; 145(35): 19396-19404, 2023 Sep 06.
Artículo en Inglés | MEDLINE | ID: mdl-37606548

RESUMEN

Designing Pb-free relaxors with both a high capacitive energy density (Wrec) and high storage efficiency (η) remains a remarkable challenge for cutting-edge pulsed power technologies. Local compositional heterogeneity is crucial for achieving complex polar structure in solid solution relaxors, but its role in optimizing energy storage properties is often overlooked. Here, we report that an exceptionally high Wrec of 15.2 J cm-3 along with an ultrahigh η of 91% can be achieved through designing local chemical clustering in Bi0.5Na0.5TiO3-BaTiO3-based relaxors. A three-dimensional atomistic model derived from neutron/X-ray total scattering combined with reverse Monte Carlo method reveals the presence of subnanometer scale clustering of Bi, Na, and Ba, which host differentiated polar displacements, and confirming the prediction by density functional theory calculations. This leads to a polar state with small polar clusters and strong length and direction fluctuations in unit-cell polar vectors, thus manifesting improved high-field polarizability, steadily reduced hysteresis, and high breakdown strength macroscopically. The favorable polar structure features also result in a unique field-increased η, excellent stability, and superior discharge capacity. Our work demonstrates that the hidden local chemical order exerts a significant impact on the polarization characteristic of relaxors, and can be exploited for accessing superior energy storage performance.

11.
J Am Chem Soc ; 145(21): 11764-11772, 2023 May 31.
Artículo en Inglés | MEDLINE | ID: mdl-37205832

RESUMEN

Dielectric capacitors have captured substantial attention for advanced electrical and electronic systems. Developing dielectrics with high energy density and high storage efficiency is challenging owing to the high compositional diversity and the lack of general guidelines. Herein, we propose a map that captures the structural distortion (δ) and tolerance factor (t) of perovskites to design Pb-free relaxors with extremely high capacitive energy storage. Our map shows how to select ferroelectric with large δ and paraelectric components to form relaxors with a t value close to 1 and thus obtaining eliminated hysteresis and large polarization under a high electric breakdown. Taking the Bi0.5Na0.5TiO3-based solid solution as an example, we demonstrate that composition-driven predominant order-disorder characteristic of local atomic polar displacements endows the relaxor with a slushlike structure and strong local polar fluctuations at several nanoscale. This leads to a giant recoverable energy density of 13.6 J cm-3, along with an ultrahigh efficiency of 94%, which is far beyond the current performance boundary reported in Pb-free bulk ceramics. Our work provides a solution through rational chemical design for obtaining Pb-free relaxors with outstanding energy-storage properties.

12.
J Am Chem Soc ; 145(11): 6194-6202, 2023 Mar 22.
Artículo en Inglés | MEDLINE | ID: mdl-36892264

RESUMEN

Chemical design of lead-free relaxors with simultaneously high energy density (Wrec) and high efficiency (η) for capacitive energy-storage has been a big challenge for advanced electronic systems. The current situation indicates that realizing such superior energy-storage properties requires highly complex chemical components. Herein, we demonstrate that, via local structure design, an ultrahigh Wrec of 10.1 J/cm3, concurrent with a high η of 90%, as well as excellent thermal and frequency stabilities can be achieved in a relaxor with a very simple chemical composition. By introducing 6s2 lone pair stereochemical active Bi into the classical BaTiO3 ferroelectric to generate a mismatch between A- and B-site polar displacements, a relaxor state with strong local polar fluctuations can be formed. Through advanced atomic-resolution displacement mapping and 3D reconstructing the nanoscale structure from neutron/X-ray total scattering, it is revealed that the localized Bi enhances the polar length largely at several perovskite unit cells and disrupts the long-range coherent Ti polar displacements, resulting in a slush-like structure with extremely small size polar clusters and strong local polar fluctuations. This favorable relaxor state exhibits substantially enhanced polarization, and minimized hysteresis at a high breakdown strength. This work offers a feasible avenue to chemically design new relaxors with a simple composition for high-performance capacitive energy-storage.

13.
Phys Rev Lett ; 131(24): 246801, 2023 Dec 15.
Artículo en Inglés | MEDLINE | ID: mdl-38181148

RESUMEN

Disordered ferroics hold great promise for next-generation magnetoelectric devices because their lack of symmetry constraints implies negligible hysteresis with low energy costs. However, the transition temperature and the magnitude of polarization and magnetization are still too low to meet application requirements. Here, taking the prototype perovskite of SrTiO_{3} as an instance, we realize a coexisting spin and dipole reentrant glass states in SrTiO_{3} homoepitaxial films via manipulation of local symmetry. Room-temperature saturation magnetization and spontaneous polarization reach ∼ 10 emu/cm^{3} and ∼ 25 µC/cm^{2}, respectively, with high transition temperatures (101 K and 236 K for spin and dipole glass temperatures and 556 K and 1100 K for Curie temperatures, respectively). Our atomic-scale investigation points out an underlying mechanism, where the Ti/O-defective unit cells break the local translational and orbital symmetry to drive the formation of unusual slush states. This study advances our understanding of the nature of the intricate couplings of ferroic glasses. Our approach could be applied to numerous perovskite oxides for the simultaneous control of the local magnetic and polar orderings and for the exploration of the underlying physics.

14.
Angew Chem Int Ed Engl ; 62(15): e202219230, 2023 Apr 03.
Artículo en Inglés | MEDLINE | ID: mdl-36780319

RESUMEN

Manganese-rich layered oxide cathodes of sodium-ion batteries (SIBs) are extremely promising for large-scale energy storage owing to their high capacities and cost effectiveness, while the Jahn-Teller (J-T) distortion and low operating potential of Mn redox largely hinder their practical applications. Herein, we reveal that annealing in argon rather than conventional air is a universal strategy to comprehensively upgrade the Na-storage performance of Mn-based oxide cathodes. Bulk oxygen vacancies are introduced via this method, leading to reduced Mn valence, lowered Mn 3d-orbital energy level, and formation of the new-concept Mn domains. As a result, the energy density of the model P2-Na0.75 Mg0.25 Mn0.75 O2 cathode increases by ≈50 % benefiting from the improved specific capacity and operating potential of Mn redox. The Mn domains can disrupt the cooperative J-T distortion, greatly promoting the cycling stability. This exciting finding opens a new avenue towards high-performance Mn-based oxide cathodes for SIBs.

15.
Nano Lett ; 21(15): 6648-6655, 2021 Aug 11.
Artículo en Inglés | MEDLINE | ID: mdl-34283627

RESUMEN

Understanding how individual dopants or substitutional atoms interact with host lattices enables us to manipulate, control, and improve the functionality of materials. However, because of the intimate coupling among various degrees of freedom in multiferroics, the atomic-scale influence of individual foreign atoms has remained elusive. Here, we unravel the critical roles of individual Sc substitutional atoms in modulating ferroelectricity at the atomic scale of typical multiferroics, Lu1-xScxFeO3, by combining advanced microscopy and theoretical studies. Atomic variations in polar displacement of intriguing topological vortex domains stabilized by Sc substitution are directly correlated with Sc atom-mediated local chemical and electronic fluctuations. The local FeO5 trimerization magnitude and Lu/Sc-O hybridization strength are found to be significantly reinforced by Sc, clarifying the origin of the strong dependence of improper ferroelectricity on Sc content. This study could pave the way for correlating dopant-regulated atomic-scale local structures with global properties to engineer emergent functionalities of numerous chemically doped functional materials.

16.
Inorg Chem ; 60(5): 3232-3237, 2021 Mar 01.
Artículo en Inglés | MEDLINE | ID: mdl-33560114

RESUMEN

Antiferroelectrics are of great academic and technological interest due to their excellent strain and energy storage properties, while the incommensurate modulation-related complex configuration of polarization remains unclear. In this study, an intriguing polarization configuration of mixed Ising- and Néel-type has been established in the prototype PbZrO3-based antiferroelectric materials via the combination of high-resolution synchrotron X-ray and neutron diffraction investigations. Such unusual polarization configuration of antiferroelectrics shows the internal coupling, which mainly contributes from the displacement of the A-site and the distortion of the AO12 and BO6 polyhedra. The electric dipole oscillates in the (001)P plane, and its magnitude and direction show obvious modulation characteristics resulting in a neither antiparallel nor fully compensated polarization configuration, which is completely different from the traditional view of antiferroelectricity. There is an antiferroelectric feature along the [110]P direction, while there is a ferrielectric one along the [1̅10]P direction in which the net polarization can reach 12 µC/cm2. The maximum local polarization can reach 4.3 µC/cm2 in the [110]P direction and 27.6 µC/cm2 in the [1̅10]P direction. This work will be very helpful for the development of antiferroelectric theories and the design of novel energy storage materials.

17.
Nanotechnology ; 32(24)2021 Mar 24.
Artículo en Inglés | MEDLINE | ID: mdl-33657545

RESUMEN

Three-dimensional (3D) composite polyvinylidene fluoride (PVDF)/polyacrylonitrile (PAN) electrospun nanofibrous membranes combining both thick and thin nanofibers have been fabricated by the method of multi-jet electrospinning with sheath gas to realize high-efficiency air filtration under a low pressure drop. The thin PAN nanofibers form a dense membrane, with a strong capturing ability on the ultra-fine particles, while the thick PVDF nanofibers play a 3D supporting effect on the thin PAN nanofibers. In this case, the combination results in a fluffy membrane with higher porosity, which could achieve the airflow passing through the membrane without the air pressure drop. The effects of the composite manner of thick nanofibers and thin nanofibers are investigated, in order to optimize the air filtration performance of the 3D composite nanofibrous membrane. As a result, the maximum quality factor for air filtration could reach up to 0.398 Pa-1. The particle-fiber interaction model was used to simulate the air filtration process as well, and the simulation results were fairly consistent with the experimental results, providing a guidance method for the optimization of composite nanofibrous membrane for high-efficiency air filtration. More interestingly, a cationic poly[2-(N,N-dimethyl amino) ethyl methacrylate] (PDMAEMA) was added in the PVDF solution to obtain a composite air filtration membrane with excellent antibiosis performance, which achieved the highest inhibition rate of approximately 90%. In short, this work provides an effective way to promote antibiosis air filtration performance by using an electrospun nanofibrous membrane, and might also effectively accelerate the biological protection application of current air filtration membranes.

18.
Zhongguo Dang Dai Er Ke Za Zhi ; 22(9): 942-947, 2020 Sep.
Artículo en Zh | MEDLINE | ID: mdl-32933623

RESUMEN

OBJECTIVE: To investigate the clinical features and outcome of neonatal acute respiratory distress syndrome (ARDS) in southwest Hubei, China. METHODS: According to the Montreux definition of neonatal ARDS, a retrospective clinical epidemiological investigation was performed on the medical data of neonates with ARDS who were admitted to Department of Neonatology/Pediatrics in 17 level 2 or level 3 hospitals in southwest Hubei from January to December, 2017. RESULTS: A total of 7 150 neonates were admitted to the 17 hospitals in southwest Hubei during 2017 and 66 (0.92%) were diagnosed with ARDS. Among the 66 neonates with ARDS, 23 (35%) had mild ARDS, 28 (42%) had moderate ARDS, and 15 (23%) had severe ARDS. The main primary diseases for neonatal ARDS were perinatal asphyxia in 23 neonates (35%), pneumonia in 18 neonates (27%), sepsis in 12 neonates (18%), and meconium aspiration syndrome in 10 neonates (15%). Among the 66 neonates with ARDS, 10 neonates (15%) were born to the mothers with an age of ≥35 years, 30 neonates (45%) suffered from intrauterine distress, 32 neonates (49%) had a 1-minute Apgar score of 0 to 7 points, 24 neonates (36%) had abnormal fetal heart monitoring results, and 21 neonates (32%) experienced meconium staining of amniotic fluid. Intraventricular hemorrhage was the most common comorbidity (12 neonates), followed by neonatal shock (9 neonates) and patent ductus arteriosus (8 neonates). All 66 neonates with ARDS were treated with mechanical ventilation in addition to the treatment for primary diseases. Among the 66 neonates with ARDS, 10 died, with a mortality rate of 15% (10/66), and 56 neonates were improved or cured, with a survival rate of 85% (56/66). CONCLUSIONS: Neonatal ARDS in southwest Hubei is mostly mild or moderate. Perinatal asphyxia and infection may be the main causes of neonatal ARDS in this area. Intraventricular hemorrhage is the most common comorbidity. Neonates with ARDS tend to have a high survival rate after multimodality treatment.


Asunto(s)
Síndrome de Dificultad Respiratoria del Recién Nacido , China , Femenino , Humanos , Recién Nacido , Síndrome de Aspiración de Meconio , Embarazo , Estudios Retrospectivos
19.
J Am Chem Soc ; 141(24): 9629-9636, 2019 Jun 19.
Artículo en Inglés | MEDLINE | ID: mdl-31129960

RESUMEN

Understanding the roles of metals and atomic structures in activating various elementary steps of electrocatalytic reactions can help rational design of binary or ternary catalysts for promoting activity toward desirable products via favorable pathways. Here we report on a newly developed ternary Au@PtIr core-shell catalyst for ethanol oxidation reaction (EOR) in alkaline solutions, which exhibits an activity enhancement of 6 orders of magnitude compared to AuPtIr alloy catalysts. Analysis of in situ infrared reflection absorption spectra for Au@PtIr and its bimetallic subsets, Au@Pt and PtIr alloy, found that monatomic steps and Au-induced tensile strain on PtIr facilitate C-C bond splitting via ethanol dissociative adsorption and Ir promotes dehydrogenation at low potentials. As evidenced by the CO band being observed only for the PtIr alloy that is rather inactive for ethanol dissociative adsorption, we propose that splitting the C-C bond at the earliest stage of EOR activates a direct 12-electron full oxidation pathway because hydrogen-rich fragments can be fully oxidized without CO as a poisoning intermediate. The resulting synergy of complementary effects of Au core and surface Ir leads to an outstanding performance of Au@PtIr for EOR as characterized by a low onset potential of 0.3 V and 8.3 A mg-1all-metals peak current with 57% currents generated via full ethanol oxidation.

20.
Phys Rev Lett ; 122(12): 126401, 2019 Mar 29.
Artículo en Inglés | MEDLINE | ID: mdl-30978042

RESUMEN

Understanding singularities in ordered structures, such as dislocations in lattice modulation and solitons in charge ordering, offers great opportunities to disentangle the interactions between the electronic degrees of freedom and the lattice. Specifically, a modulated structure has traditionally been expressed in the form of a discrete Fourier series with a constant phase and amplitude for each component. Here, we report atomic scale observation and analysis of a new modulation wave in hole-doped LuFe_{2}O_{4+δ} that requires significant modifications to the conventional modeling of ordered structures. This new modulation with an unusual quasiperiodic singularity can be accurately described only by introducing a well-defined secondary modulation vector in both the phase and amplitude parameter spaces. Correlated with density-functional-theory (DFT) calculations, our results reveal that those singularities originate from the discontinuity of lattice displacement induced by interstitial oxygen in the system. The approach of our work is applicable to a wide range of ordered systems, advancing our understanding of the nature of singularity and modulation.

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