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1.
J Am Chem Soc ; 2024 Jun 06.
Artigo em Inglês | MEDLINE | ID: mdl-38842530

RESUMO

Photocatalytic C2H6-to-C2H4 conversion is very promising, yet it remains a long-lasting challenge due to the high C-H bond dissociation energy of 420 kJ mol-1. Herein, partially oxidized Pdδ+ species anchored on ZnO nanosheets are designed to weaken the C-H bond by the electron interaction between Pdδ+ species and H atoms, with efforts to achieve high-rate and selective C2H6-to-C2H4 conversion. X-ray photoelectron spectra, Bader charge calculations, and electronic localization function demonstrate the presence of partially oxidized Pdδ+ sites, while quasi-in situ X-ray photoelectron spectra disclose the Pdδ+ sites initially adopt and then donate the photoexcited electrons for C2H6 dehydrogenation. In situ electron paramagnetic resonance spectra, in situ Fourier transform infrared spectra, and trapping agent experiments verify C2H6 initially converts to CH3CH2OH via ·OH radicals, then dehydroxylates to CH3CH2· and finally to C2H4, accompanied by H2 production. Density-functional theory calculations elucidate that loading Pd site can lengthen the C-H bond of C2H6 from 1.10 to 1.12 Å, which favors the C-H bond breakage, affirmed by a lowered energy barrier of 0.04 eV. As a result, the optimized 5.87% Pd-ZnO nanosheets achieve a high C2H4 yield of 16.32 mmol g-1 with a 94.83% selectivity as well as a H2 yield of 14.49 mmol g-1 from C2H6 dehydrogenation in 4 h, outperforming all the previously reported photocatalysts under similar conditions.

2.
Nano Lett ; 24(15): 4610-4617, 2024 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-38564191

RESUMO

The intricate protonation process in carbon dioxide reduction usually makes the product unpredictable. Thus, it is significant to control the reactive intermediates to manipulate the reaction steps. Here, we propose that the synergistic La-Ti active sites in the N-La2Ti2O7 nanosheets enable the highly selective carbon dioxide photoreduction into methane. In the photoreduction of CO2 over N-La2Ti2O7 nanosheets, in situ Fourier transform infrared spectra are utilized to monitor the *CH3O intermediate, pivotal for methane production, whereas such monitoring is not conducted for La2Ti2O7 nanosheets. Also, theoretical calculations testify to the increased charge densities on the Ti and La atoms and the regulated formation energy barrier of *CO and *CH3O intermediates by the constructed synergistic active sites. Accordingly, the methane formation rate of 7.97 µL h-1 exhibited by the N-La2Ti2O7 nanosheets, along with an electron selectivity of 96.6%, exceeds that of most previously reported catalysts under similar conditions.

3.
J Am Chem Soc ; 146(17): 12233-12242, 2024 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-38626786

RESUMO

Photocatalytic conversion of methane (CH4) to ethane (C2H6) has attracted extensive attention from academia and industry. Typically, the traditional oxidative coupling of CH4 (OCM) reaches a high C2H6 productivity, yet the inevitable overoxidation limits the target product selectivity. Although the traditional nonoxidative coupling of CH4 (NOCM) can improve the product selectivity, it still encounters unsatisfied activity, arising from being thermodynamically unfavorable. To break the activity-selectivity trade-off, we propose a conceptually new mechanism of H2O2-triggered CH4 coupling, where the H2O2-derived ·OH radicals are rapidly consumed for activating CH4 into ·CH3 radicals exothermically, which bypasses the endothermic steps of the direct CH4 activation by photoholes and the interaction between ·CH3 and ·OH radicals, affirmed by in situ characterization techniques, femtosecond transient absorption spectroscopy, and density-functional theory calculation. By this pathway, the designed Au-WO3 nanosheets achieve unprecedented C2H6 productivity of 76.3 mol molAu-1 h-1 with 95.2% selectivity, and TON of 1542.7 (TOF = 77.1 h-1) in a self-designed flow reactor, outperforming previously reported photocatalysts regardless of OCM and NOCM pathways. Also, under outdoor natural sunlight irradiation, the Au-WO3 nanosheets exhibit similar activity and selectivity toward C2H6 production, showing the possibility for practical applications. Interestingly, this strategy can be applied to other various photocatalysts (Au-WO3, Au-TiO2, Au-CeO2, Pd-WO3, and Ag-WO3), showing a certain universality. It is expected that the proposed mechanism adds another layer to our understanding of CH4-to-C2H6 conversion.

4.
Adv Mater ; 36(23): e2314209, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38331431

RESUMO

Electrochemically reconstructed Cu-based catalysts always exhibit enhanced CO2 electroreduction performance; however, it still remains ambiguous whether the reconstructed Cu vacancies have a substantial impact on CO2-to-C2+ reactivity. Herein, Cu vacancies are first constructed through electrochemical reduction of Cu-based nanowires, in which high-angle annular dark-field scanning transmission electron microscopy image manifests the formation of triple-copper-vacancy associates with different concentrations, confirmed by positron annihilation lifetime spectroscopy. In situ attenuated total reflection-surface enhanced infrared absorption spectroscopy discloses the triple-copper-vacancy associates favor *CO adsorption and fast *CO dimerization. Moreover, density-functional-theory calculations unravel the triple-copper-vacancy associates endow the nearby Cu sites with enriched and disparate local charge density, which enhances the *CO adsorption and reduces the CO-CO coupling barrier, affirmed by the decreased *CO dimerization energy barrier by 0.4 eV. As a result, the triple-copper-vacancy associates confined in Cu nanowires achieve a high Faradaic efficiency of over 80% for C2+ products in a wide current density range of 400-800 mA cm-2, outperforming most reported Cu-based electrocatalysts.

5.
Front Psychol ; 15: 1354820, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-38371706

RESUMO

Given the growing incidence rates of suicide among college students and the potential lifelong consequences of suicide, it is imperative to better understand the factors that reduce the rates at which college students in a clinical sample engage in suicide. This study examines the relationship between social exclusion and suicide intention, the mediating effect of depression, and the moderating effect of meaning in life. Two hundred and ninety-nine Chinese college students, aged from 18 to 22 years (56.86% female, M age = 20.14, SD = 1.27) completed questionnaires assessing their social exclusion, suicide intention, depression, and meaning in life. The result revealed that social exclusion was positively associated with suicide intention, and depression mediated this relationship. In addition, this mediating effect of depression was moderated by meaning in life. That is, the mediation effect was stronger for students with a higher level of meaning in life. These findings provide educational suggestions for preventing and intervening in suicide intention among college students.

6.
Angew Chem Int Ed Engl ; 63(13): e202400828, 2024 Mar 22.
Artigo em Inglês | MEDLINE | ID: mdl-38326235

RESUMO

Targeted synthesis of acetic acid (CH3 COOH) from CO2 photoreduction under mild conditions mainly limits by the kinetic challenge of the C-C coupling. Herein, we utilized doping engineering to build charge-asymmetrical metal pair sites for boosted C-C coupling, enhancing the activity and selectivity of CO2 photoreduction towards CH3 COOH. As a prototype, the Pd doped Co3 O4 atomic layers are synthesized, where the established charge-asymmetrical cobalt pair sites are verified by X-ray photoelectron spectroscopy and X-ray absorption near edge spectroscopy spectra. Theoretical calculations not only reveal the charge-asymmetrical cobalt pair sites caused by Pd atom doping, but also manifest the promoted C-C coupling of double *COOH intermediates through shortening of the coupled C-C bond distance from 1.54 to 1.52 Å and lowering their formation energy barrier from 0.77 to 0.33 eV. Importantly, the decreased reaction energy barrier from the protonation of two*COOH into *CO intermediates for the Pd-Co3 O4 atomic layer slab is 0.49 eV, higher than that of the Co3 O4 atomic layer slab (0.41 eV). Therefore, the Pd-Co3 O4 atomic layers exhibit the CH3 COOH evolution rate of ca. 13.8 µmol g-1 h-1 with near 100% selectivity, both of which outperform all previously reported single photocatalysts for CO2 photoreduction towards CH3 COOH under similar conditions.

7.
Carbohydr Polym ; 327: 121647, 2024 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-38171672

RESUMO

Polyethylene glycol (PEG) is a flexible, water-soluble, non-immunogenic, as well as biocompatible polymer, and it could synergize with polysaccharides for food applications. The molecular modification strategies, including covalent bond interactions (amino groups, carboxyl groups, aldehyde groups, tosylate groups, etc.), and non-covalent bond interactions (hydrogen bonding, electrostatic interactions, etc.) on PEG molecular chains are discussed. Its versatile structure, group modifiability, and amphiphilic block buildability could improve the functions of polysaccharides (e.g., chitosan, cellulose, starch, alginate, etc.) and adjust the properties of combined PEG/polysaccharides with outstanding chain tunability and matrix processability owing to plasticizing effects, compatibilizing effects, steric stabilizing effects and excluded volume effects by PEG, for achieving the diverse performance targets. The synergetic properties of PEG/polysaccharides with remarkable architecture were summarized, including mechanical properties, antibacterial activity, antioxidant performance, self-healing properties, carrier and delivery characteristics. The PEG/polysaccharides with excellent combined properties and embeddable merits illustrate potential applications including food packaging, food intelligent indication/detection, food 3D printing and nutraceutical food absorption. Additionally, prospects (like food innovation and preferable nutrient utilization) and key challenges (like structure-effectiveness-applicability relationship) for PEG/polysaccharides are proposed and addressed for food fields.


Assuntos
Polietilenoglicóis , Polissacarídeos , Polietilenoglicóis/química , Polissacarídeos/farmacologia , Polissacarídeos/química , Polímeros/química , Celulose/química , Alginatos/química
8.
Chemphyschem ; 25(5): e202300368, 2024 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-38193665

RESUMO

The goal of photocatalytic CO2 reduction system is to achieve near 100 % selectivity for the desirable product with reasonably high yield and stability. Here, two-dimensional metal-organic frameworks are constructed with abundant and uniform monometallic active sites, aiming to be an emerged platform for efficient and selective CO2 reduction. As an example, water-stable Cu-based metal-organic framework nanoribbons with coordinatively unsaturated single CuII sites are first fabricated, evidenced by X-ray diffraction patterns and X-ray absorption spectroscopy. In situ Fourier-transform infrared spectra and Gibbs free energy calculations unravel the formation of the key intermediate COOH* and CO* is an exothermic and spontaneous process, whereas the competitive hydrogen evolution reaction is endothermic and non-spontaneous, which accounts for the selective CO2 reduction. As a result, in an aqueous solution containing 1 mol L-1 KHCO3 and without any sacrifice reagent, the water-stable Cu-based metal-organic framework nanoribbons exhibited an average CO yield of 82 µmol g-1 h-1 with the selectivity up to 97 % during 72 h cycling test, which is comparable to other reported photocatalysts under similar conditions.

9.
Int J Biol Macromol ; 261(Pt 1): 129749, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38281522

RESUMO

Natural polychromatic biomaterials (like carminic acid and gardenia yellow) possess coloring merits and functionality, but are instable under light and heat. Self-assembly of gelatin and polychromatic materials could be induced by carnosic acid inclusions, illustrating great potential in food application. Antioxidant properties, pigment retention rates, UV irradiation stability, rheological properties, and physical resistances (oil, ethanol, heat and microwave) of samples were improved by carnosic acid inclusions, owing to the newly formed hydrogen bonding and electrostatic interactions (UV spectrum, particle size, zeta potential, FTIR, XPS and SEM). The improved properties contributed to the 2D printed pattern stability and the applicability for producing specialized products with high printability and fastness. On the basis of Subtractive Color-Mixing Principle, further three-dimensional dyeing microgel systems were built and modulated; it could functionalize bean paste/carboxymethyl-cellulose food systems, maintain the excellent self-supporting ability & mechanical strength, and promote single/dual-nozzle 3D printing application. Therefore, the self-assembled gelatin/polychromatic materials/carnosic acid microgel samples could not only achieve outstanding 2D printed pattern stability, and could be also promisingly applied in single/dual-nozzle 3D printing for modern innovative, creative food fields.


Assuntos
Abietanos , Microgéis , Gelatina , Materiais Biocompatíveis , Impressão Tridimensional
10.
Int J Biol Macromol ; 261(Pt 2): 129380, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38244745

RESUMO

Carboxymethyl starch (CST) was introduced to improve gelatin films and its practical application as edible high-performance films for food packaging and cooking was also investigated. The gelatin films modified by carboxymethyl starch exhibited the transparent appearance, tensile strength, barrier properties (oxygen, water vapor and UV light), and thermal performance (TGA, thermal shrinkage and heat-sealing strength). Resulting from the effect of electrostatic interaction modes on the properties of films, electrostatic repulsion could surpass electrostatic attraction in improving the tensile strength, oxygen barrier property and thermal stability of the films probably due to extensive physical entanglement without aggregation. Analysis of FTIR, zeta potential, interfacial dilatational rheology, shear rheological properties, XRD, Raman, SEM and AFM suggested that hydrogen bonding and electrostatic repulsion contributed to the excellent performance. The packaged food could also be cooked with the prepared film for porridge; and the film slightly influenced the shear rheological properties of porridge and imposed little effect on the odors (Electronic-Nose) of porridge. Hence, the gelatin films modified by carboxymethyl starch could potentially work as the edible inner packaging or the edible quantitative packaging for food, offer convenience for consumers, reduce the packaging waste and avoid an extra burden on environment.


Assuntos
Gelatina , Amido/análogos & derivados , Eletricidade Estática , Embalagem de Alimentos/métodos , Resistência à Tração , Culinária , Oxigênio , Permeabilidade
11.
Nano Lett ; 24(2): 696-702, 2024 Jan 17.
Artigo em Inglês | MEDLINE | ID: mdl-38175193

RESUMO

Selectively achieving the photoreduction of carbon dioxide (CO2) to methane (CH4) remains a significant challenge, which primarily arises from the complexity of the protonation process. In this work, we designed metal-vacancy pair sites in defective metal oxide semiconductors, which anchor the reactive intermediates with a bridged linkage for the selective protonation to produce CH4. As an example, oxygen-deficient Nb2O5 nanosheets are synthesized, in which the niobium-oxygen vacancy pair sites are demonstrated by X-ray photoelectron spectroscopy and electron paramagnetic resonance spectra. In situ Fourier transform infrared spectroscopy monitors the *CH3O intermediate, a key intermediate for CH4 production, during the CO2 photoreduction in oxygen-deficient Nb2O5 nanosheets. Importantly, the built metal-vacancy pair sites regulate the *CH3O formation step as a spontaneous process, making the reduction of CO2 to CH4 the preferred method. Therefore, the oxygen-deficient Nb2O5 nanosheets exhibit a CH4 formation rate of 19.14 µmol g-1 h-1, with an electron selectivity of ∼94.1%.

12.
Small ; 20(1): e2304502, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37649185

RESUMO

Reduced graphene oxide (rGO) has garnered extensive attention as electrodes, sensors, and membranes, necessitating the efficient reduction of graphene oxide (GO) for optimal performance. In this work, a swift reduction of GO that involves bringing GO foam in contact with semi-molten metals like tin (Sn) and lithium (Li) is presented. These findings reveal that the electrical resistance of GO foam is significantly diminished by its interaction with these metals, even in dry air. Taking inspiration from this technique, Sn foil is employed to encase the GO foam, followed by a calcination in 15 vol% H2 /Ar environment at 235 °C to fabricate the rGO, which demonstrates a remarkably lower electrical resistivity of 0.42 Ω cm when compared to the chemically reduced GO via hydrazine hydrate (650 Ω cm). The reduction mechanism entails the migration of Sn on GO and its subsequent reaction with oxygen functional groups. SnO/Sn(OH)2 formed from the reaction can be subsequently reversed through reduction by H2 to Sn. Utilizing this rGO as the host material for a sulfur cathode, a lithium-sulfur battery is constructed that displays a specific capacity of 1146 mAh g-1 and maintains a capacity retention of 68.4% after 300 cycles at a rate of 0.2 C.

13.
Food Chem ; 438: 137964, 2024 Apr 16.
Artigo em Inglês | MEDLINE | ID: mdl-37976879

RESUMO

Silk fibroin materials are emergingly explored for food applications due to their inherent properties including safe oral consumption, biocompatibility, gelatinization, antioxidant performance, and mechanical properties. However, silk fibroin possesses drawbacks like brittleness owing to its inherent specific composition and structure, which limit their applications in this field. This review discusses current progress about molecular modification methods on silk fibroin such as extraction, blending, self-assembly, enzymatic catalysis, etc., to address these limitations and improve their physical/chemical properties. It also summarizes matrix enhancement strategies including freeze drying, spray drying, electrospinning/electrospraying, microfluidic spinning/wheel spinning, desolvation and supercritical fluid, to generate nano-, submicron-, micron-, or bulk-scale materials. It finally highlights the food applications of silk fibroin materials, including nutraceutical improvement, emulsions, enzyme immobilization and 3D/4D printing. This review also provides insights on potential opportunities (like safe modification, toxicity risk evaluation, and digestion conditions) and possibilities (like digital additive manufacturing) in functional food industry.


Assuntos
Fibroínas , Fibroínas/química , Alimento Funcional , Materiais Biocompatíveis/química
14.
Food Res Int ; 173(Pt 2): 113392, 2023 11.
Artigo em Inglês | MEDLINE | ID: mdl-37803730

RESUMO

Lutein could be stabilized in gelatin type A/B-chitosan systems by different polyoxyethylene sorbitan fatty acid esters (tweens) via tunable chains and bonds, and the homogeneous system held potential in food 2D/3D printing. During encapsulation of lutein in gelatin-chitosan matrix complexes, tween 40, tween 60 and tween 80 assisted in the excellent centrifugation stability, freeze-thaw stability, chemical stability as well as thermal stability. The tweens contained systems also possessed excellent rheological properties, including shearing thinning property, self-supporting characteristics, and favorable thixotropy. Especially, tween 80 performed well in facilitating the stability and rheological properties of systems with uniform micromorphology due to its long alkyl chains and carbon-carbon double bonds (two sp2 hybridized C-atoms) (from FTIR, XRD, SEM, etc.); and gelatin type B illustrated higher protection effects on lutein because of its strong electrostatic interaction with chitosan. The optimal systems could work as edible ink for 2D/3D printing on food with great UV-irradiation stability and high definition. Surimi could be modified by the optimal complex and possessed excellent shear-thinning property, proper yield stress, low dependence on frequency and stable structure, which was successfully applied for innovative 3D printing with sophisticated shapes. The practical food 2D/3D printing (like bread and surimi) demonstrated high potential in food creation and food innovation.


Assuntos
Quitosana , Polissorbatos , Adolescente , Criança , Humanos , Gelatina/química , Luteína , Carbono
15.
Materials (Basel) ; 16(20)2023 Oct 16.
Artigo em Inglês | MEDLINE | ID: mdl-37895684

RESUMO

Biomimetic structures are inspired by elegant and complex architectures of natural creatures, drawing inspiration from biological structures to achieve specific functions or improve specific strength and modulus to reduce weight. In particular, the rapid closure of a Venus flytrap leaf is one of the fastest motions in plants, its biomechanics does not rely on muscle tissues to produce rapid shape-changing, which is significant for engineering applications. Composites are ubiquitous in nature and are used for biomimetic design due to their superior overall performance and programmability. Here, we focus on reviewing the most recent progress on biomimetic Venus flytrap structures based on smart composite technology. An overview of the biomechanics of Venus flytrap is first introduced, in order to reveal the underlying mechanisms. The smart composite technology was then discussed by covering mainly the principles and driving mechanics of various types of bistable composite structures, followed by research progress on the smart composite-based biomimetic flytrap structures, with a focus on the bionic strategies in terms of sensing, responding and actuation, as well as the rapid snap-trapping, aiming to enrich the diversities and reveal the fundamentals in order to further advance the multidisciplinary science and technological development into composite bionics.

16.
Carbohydr Polym ; 319: 121209, 2023 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-37567685

RESUMO

This work presented a facile way of stabilizing capsanthin by physically-connected soft hydrogels via utilizing specially-structured polysaccharides, and investigated rheological properties, self-recovering mechanism and 3D printability. The functionalized hydrogels demonstrated excellent color quality including redness, yellowness index and hue with great storage stability and visual perception. The soft hydrogels fabricated with properly sequenced polyglyceryl fatty acid esters, ß-cyclodextrin, chitosan, and low-content capsanthin possessed outstanding extrudability, appropriate yield stress, reasonable mechanical strength, rational elasticity and structure sustainability. Furthermore, the self-recovering properties based on hydrogen bonds, host-guest interactions and electrostatic interactions were revealed and verified by structural, zeta potential, micro-morphological, zeta potential, thixotropic, creep-recovery, and macroscopic/microscopic characterizations. Along with excellent antioxidant performance, the subsequent 3D printing onto bread with complex models elucidated the high geometry accuracy and great sensory characters. The sequenced physically-connected hydrogels incorporated with capsanthin can provide new insights on stabilizing hydrophobic biomaterials and developing the 3D printed exquisite, innovative food.

17.
Int J Mol Med ; 52(1)2023 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-37232353

RESUMO

The side effects of chemotherapy drugs have been hindering the progress of tumor treatment. The liver is the metabolic site of most drugs, which leads to the frequent occurrence of liver injury. Classical chemotherapy drugs such as pirarubicin (THP) can also cause dose­dependent hepatotoxicity, and the related mechanism is closely related to liver inflammation. Scutellarein (Sc) is a potential Chinese herbal monomer exhibiting liver protection activity, which can effectively alleviate the liver inflammation caused by obesity. In the present study, THP was used to establish a rat model of hepatotoxicity, and Sc was used for treatment. The experimental methods used included measuring body weight, detecting serum biomarkers, observing liver morphology with H&E staining, observing cell apoptosis with TUNEL staining, and detecting the expression of PTEN/AKT/NFκB signaling pathways and inflammatory genes with PCR and western blotting. However, whether Sc can inhibit the liver inflammation induced by THP has not been reported. The experimental results showed that THP led to the upregulation of PTEN and the increase of inflammatory factors in rat liver, while Sc effectively alleviated the aforementioned changes. It was further identified in primary hepatocytes that Sc can effectively inhabited PTEN, regulate AKT/NFκB signaling pathway, inhibit liver inflammation and ultimately protect the liver.


Assuntos
Doença Hepática Induzida por Substâncias e Drogas , Proteínas Proto-Oncogênicas c-akt , Ratos , Animais , Proteínas Proto-Oncogênicas c-akt/metabolismo , Transdução de Sinais , PTEN Fosfo-Hidrolase/genética , PTEN Fosfo-Hidrolase/metabolismo , NF-kappa B/metabolismo , Apoptose , Inflamação/tratamento farmacológico , Inflamação/prevenção & controle
18.
Front Pediatr ; 11: 1144952, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37152321

RESUMO

Introduction: White matter injury (WMI) is now the major disease that seriously affects the quality of life of preterm infants and causes cerebral palsy of children, which also causes periventricular leuko-malacia (PVL) in severe cases. The study aimed to develop a method based on cranial ultrasound images to evaluate the risk of WMI. Methods: This study proposed an ultrasound radiomics diagnostic system to predict the WMI risk. A multi-task deep learning model was used to segment white matter and predict the WMI risk simultaneously. In total, 158 preterm infants with 807 cranial ultrasound images were enrolled. WMI occurred in 32preterm infants (20.3%, 32/158). Results: Ultrasound radiomics diagnostic system implemented a great result with AUC of 0.845 in the testing set. Meanwhile, multi-task deep learning model preformed a promising result both in segmentation of white matter with a Dice coefficient of 0.78 and prediction of WMI risk with AUC of 0.863 in the testing cohort. Discussion: In this study, we presented a data-driven diagnostic system for white matter injury in preterm infants. The system combined multi-task deep learning and traditional radiomics features to achieve automatic detection of white matter regions on the one hand, and design a fusion strategy of deep learning features and manual radiomics features on the other hand to obtain stable and efficient diagnostic performance.

19.
Small ; 19(36): e2300286, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37162459

RESUMO

Lithium-sulfur (Li-S) battery has been considered as a strong contender for commercial aerospace battery, but the commercialization requires Ah-level pouch cells with both efficient discharge at high rates and ultra-high energy density. In this paper, the application of lithium-sulfur batteries for powering drones by using the cathode of highly dispersed sulfur nanoparticles with well-controlled particle sizes have been realized. The sulfur nanoparticles are prepared by a precipitation method in an eco-friendly and efficient way, and loaded on graphene oxide-cetyltrimethylammonium bromide by molecular grafting to realize a large-scale fabrication of sulfur-based cathodes with superior electrochemical performance. A button cell based on the cathode exhibits an excellent discharge capacity of 62.8 mAh cm-2 at a high sulfur loading of 60 mg cm-2 (i.e., 1046.7 mAh g-1 ). The assembled miniature pouch cell (PCmini) shows a discharge capacity of 130 mAh g-1 , while the formed Ah-level pouch cell (PCAh) achieves energy density of 307 Wh kg-1 at 0.3C and 92 Wh kg-1 at 4C. Especially, a four-axis propeller drone powered by the PC has successfully completed a long flight (>3 min) at high altitudes, demonstrating the practical applicability as aviation batteries.

20.
Angew Chem Int Ed Engl ; 62(15): e202301075, 2023 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-36792533

RESUMO

Selective CO2 photoreduction into C2 fuels under mild conditions suffers from low product yield and poor selectivity owing to the kinetic challenge of C-C coupling. Here, triatomic sites are introduced into bimetallic sulfide to promote C-C coupling for selectively forming C2 products. As an example, FeCoS2 atomic layers with different oxidation degrees are first synthesized, demonstrated by X-ray photoelectron spectroscopy and X-ray absorption near edge spectroscopy spectra. Both experiment and theoretical calculation verify more charges aggregate around the introduced oxygen atom, which enables the original Co-Fe dual sites to turn into Co-O-Fe triatomic sites, thus promoting C-C coupling of double *COOH intermediates. Accordingly, the mildly oxidized FeCoS2 atomic layers exhibit C2 H4 formation rate of 20.1 µmol g-1 h-1 , with the product selectivity and electron selectivity of 82.9 % and 96.7 %, outperforming most previously reported photocatalysts under similar conditions.

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