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1.
Anim Nutr ; 18: 257-271, 2024 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-39281054

RESUMEN

This study investigated the impact of different ratios of soluble to insoluble dietary fiber (SDF:IDF) formulations by sugar beet pulp (SBP) supplementation on piglet growth performance, nutrient digestibility, immune function, intestinal morphology, intestinal microbiota and intestinal health. A total of 60 crossbred piglets (Duroc × [Landrace × Yorkshire]) at 40 d old with body weight of 10.0 ± 0.3 kg were randomly assigned to 5 treatments with 6 replicates per treatment and 2 piglets per replicate in a 21-d trial. The dietary treatments included a corn-soybean meal diet (0% SBP supplementation; CON), and diets supplemented with 2%, 4%, 6%, and 8% SBP, representing different SDF:IDF ratios at 10.16%, 13.53%, 16.79%, 19.86%, and 24.81%, respectively. The results indicated that the 8% SBP treatment had a negative effect on feed-to-gain ratio (linear, P = 0.009) compared with the CON treatment (P = 0.021). The apparent total tract digestibility (ATTD) of crude protein was lower in treatments supplemented with SBP (P = 0.002) and showed a linear decrease (P = 0.001), while the ATTD of IDF showed a linear increase (P = 0.037) in four SBP treatments compared to the CON treatment. The 4% SBP treatment increased serum concentrations of triglyceride (quadratic, P = 0.019) and K (linear, P < 0.0037), and decreased alanine transaminase concentration (quadratic, P = 0.015) compared with the CON treatment. The concentrations of Cit, Cys, Ile, Leu, Orn, Arg, taurine, urea, 1-methylhistidine, α-aminoadipic acid, α-aminobutyric acid and cystathionine in the 4% SBP treatment were highest among all treatments (P < 0.05). The serum concentrations of interleukin-6, interleukin-8, interleukin-10, transforming growth factor-ß, and tumor necrosis factor-α in the 6% SBP treatment were higher than those in the CON treatment (P < 0.05), which also increased mucin-2 and G protein-coupled receptor 41 mRNA expression (P < 0.05) in colonic mucosa compared with the CON treatment and improved the intestinal barrier function. Diets containing more than 19.86% SDF:IDF could impair the intestinal health in piglets when SBP was used as the SDF source. Supplementing nursery piglet diets with 16.79% to 19.86% SDF:IDF is recommended for improving intestinal barrier function, increasing short-chain fatty acids concentrations, and improving intestinal microbiota composition.

2.
RSC Adv ; 14(33): 23930-23942, 2024 Jul 26.
Artículo en Inglés | MEDLINE | ID: mdl-39086527

RESUMEN

Magnesium hydroxide (MgH2) has a broad application prospect in solid hydrogen storage, but the associated higher dehydrogenation temperature and undesirable cycling capacity limit its large-scale application. In this study, a BaCrO4 nanocatalyst prepared via a wet chemistry method was added to MgH2 to achieve better kinetic and thermodynamic performances. Kinetic tests suggested that the onset hydrogen desorption temperature was decreased for milled MgH2 from 390 °C to below 280 °C after the introduction of a 5 wt% BaCrO4 nanocatalyst and the maximum dehydrogenation amount was up to 6.32 wt%. With regard to hydrogen absorption, MgH2 incorporated with 10 wt% BaCrO4 could fully absorb 5.78 wt% H2 within 10 min at 300 °C and recharge 3.1 wt% H2 at a low temperature of 250 °C. In comparison, the hydrogen uptake amounts for MgH2 under the same conditions were only 3.98 wt% and 1.52 wt%. With regard to hydrogen desorption, 5 wt% BaCrO4-modified MgH2 could discharge 4.25 wt% H2 within 10 min at 325 °C and 4.81 wt% H2 at 300 °C, while MgH2 could not dehydrogenate at 300 °C. Meanwhile, only 5% of the performance decayed for 5 wt% BaCrO4-modified MgH2 during ten cycles. Dehydrogenation E a reduced to 106.75 kJ mol-1 in contrast to 156.55 kJ mol-1 for MgH2. In addition, DFT results verified that the BaCrO4 nanocatalyst reduced the band gap from 2.78 eV to 2.16 eV to improve the thermodynamic property of MgH2 and contributed to the decrease in the dehydrogenation energy barrier from 2.27 eV to 1.54 eV. This work provides an insight into the performance of ternary transition metal nanocatalysts for MgH2 hydrogen storage systems.

3.
Nanomaterials (Basel) ; 14(15)2024 Jul 30.
Artículo en Inglés | MEDLINE | ID: mdl-39120384

RESUMEN

Mechanoluminescent (ML) materials can exhibit visible-to-near-infrared mechanoluminescence when responding to the fracture or deformation of a solid under mechanical stimulation. Transforming mechanical energy into light demonstrates promising applications in terms of visual mechanical sensing. In this work, we synthesized the phosphor CaZnOS:Tb3+, Sm3+, which exhibited intense and tunable multicolor mechanoluminescence without pre-irradiation. Intense green ML materials were obtained by doping Tb3+ with different concentrations. Tunable multicolor mechanoluminescence (such as green, yellow-green, and orange-red) could be realized by combining green emission (about 542 nm), attributed to Tb3+, and red emission (about 600 nm) generated from the Sm3+ in the CaZnOS substrate. The tunable multicolor ML materials CaZnOS:Tb3+, Sm3+ exhibited intense luminance and recoverable mechanoluminescence when responding to mechanical stimulation. Benefiting from the excellent ML performance and multicolor tunability in CaZnOS:Tb3+, Sm3+, we mixed the phosphor with PDMS and a curing agent to explore its practical application. An application for visual mechanical sensing was designed for handwriting identification. By taking a time-lapsed shot while writing, we easily obtained images of the writer's handwriting. The images of the ML intensity were acquired by using specific software to transform the shooting data. We could easily distinguish people's handwriting through analyzing the different ML performances.

4.
ACS Catal ; 14(13): 9877-9886, 2024 Jul 05.
Artículo en Inglés | MEDLINE | ID: mdl-38988656

RESUMEN

Antimony selenide (Sb2Se3) has recently been intensively investigated and has achieved significant advancement in photoelectrochemical (PEC) water splitting. In this work, a facile one-step hydrothermal method for the preparation of Sn-doped Sb2Se3 photocathodes with improved PEC performance was investigated. We present an in-depth study of the performance enhancement in Sn-doped Sb2Se3 photocathodes using capacitance-voltage (CV), drive-level capacitance profiling (DLCP), and electrochemical impedance spectroscopy (EIS) techniques. The incorporation of Sn2+ into the Sb2Se3 results in increased carrier density, reduced surface defects, and improved charge separation, thereby leading to improved PEC performance. With a thin Sb2Se3 absorber layer (270 nm thickness), the Sn-doped Sb2Se3 photocathode exhibits an improved photocurrent density of 17.1 mA cm-2 at 0 V versus RHE (V RHE) compared to that of the undoped Sb2Se3 photocathode (14.4 mA cm-2). This work not only highlights the positive influence of Sn doping on Sb2Se3 photocathodes but also showcases a one-step method to synthesize doped Sb2Se3 with improved optoelectronic properties.

5.
Small ; : e2404019, 2024 Jul 24.
Artículo en Inglés | MEDLINE | ID: mdl-39045905

RESUMEN

Developing electrocatalysts with excellent activity and stability for water splitting in acidic media remains a formidable challenge due to the sluggish kinetics and severe dissolution. As a solution, a multi-component doped RuO2 prepared through a process of dealloying-annealing is presented. The resulting multi-doped RuO2 possesses a nanoporous structure, ensuring a high utilization efficiency of Ru. Furthermore, the dopants can regulate the electronic structure, causing electron aggregation around unsaturated Ru sites, which mitigates Ru dissolution and significantly enhances the catalytic stability/activity. The representative catalyst (FeCoNiCrTi-RuO2) shows an overpotential of 167 mV at 10 mA cm-2 for oxygen evolution reaction (OER) in 0.5 m H2SO4 solution with a Tafel slope of 53.1 mV dec-1, which is among the highest performance reported. Moreover, it remains stable for over 200 h at a current density of 10 mA cm-2. This work presents a promising approach for improving RuO2-based electrocatalysts, offering a crucial advancement for electrochemical water splitting.

6.
Inorg Chem ; 63(29): 13474-13483, 2024 Jul 22.
Artículo en Inglés | MEDLINE | ID: mdl-38976574

RESUMEN

Traditional information encryption materials that rely on fluorescent/phosphorescent molecules are facing an increasing risk of counterfeiting or tampering due to their static reading mode and advances in counterfeiting technology. In this study, a series of Mg2-xZnxSnO4 (x = 0.55, 0.6, 0.65, 0.7 0.75, 0.8) that realizes the writing, reading, and erasing of dynamic information is developed. When heated to 90 °C, the materials exhibit a variety of dynamic emission changes with the concentration of Zn2+ ions. As the doping concentration increased, the ratio of the shallow trap to deep trap changed from 7.77 to 20.86. When x = 0.55, the proportion of deep traps is relatively large, resulting in a higher temperature and longer time required to read the information. When x = 0.80, the proportion of shallow traps is larger and the encrypted information is easier to read. Based on the above features, encryption binary codes device was designed, displaying dynamic writing, reading, and erasing of information under daylight and heating conditions. Accordingly, this work provides reliable guidance on advanced dynamic information encryption.

7.
Medicine (Baltimore) ; 103(26): e38535, 2024 Jun 28.
Artículo en Inglés | MEDLINE | ID: mdl-38941431

RESUMEN

OBJECTIVE: To investigate causal associations between diabetes, insulin treatment and osteoporosis using LDSC analysis with a 2-way Mendelian randomization study. METHODS: LDSC analysis was used to estimate the likelihood-scale heritability of the genome-wide association study used with genetic correlation between the 2 genome-wide association study used. Then a 2-sample Mendelian randomization study was performed using 3 methods including inverse variance weighted, MR Egger, and weighted median. RESULTS: The genetic correlation between diabetes, insulin treatment (h2_Z = 3.70, P = 2.16e-4), osteoporosis (h2_Z = 4.93, h2_p = 8.13e-7) and genes was significant. There was a significant genetic correlation (rg = 0.122, P = 0.0211). There was a causal association between diabetes, insulin treatment and osteoporosis [P = 0.003754, OR (95%CI) = 0.998876 (0.998116-0.999636)], while no causal association existed between osteoporosis and insulin use (P = 0.998116-0.999636) causal association existed (P = 0.333244). CONCLUSION: There was a strong genetic correlation between diabetes, insulin treatment and osteoporosis, a causal association between diabetes, insulin treatment and osteoporosis, and no causal association between osteoporosis and diabetes, insulin treatment.


Asunto(s)
Estudio de Asociación del Genoma Completo , Insulina , Análisis de la Aleatorización Mendeliana , Osteoporosis , Humanos , Insulina/uso terapéutico , Insulina/efectos adversos , Osteoporosis/genética , Osteoporosis/epidemiología , Diabetes Mellitus/genética , Diabetes Mellitus/epidemiología , Polimorfismo de Nucleótido Simple
8.
Cell Death Dis ; 14(10): 675, 2023 10 13.
Artículo en Inglés | MEDLINE | ID: mdl-37833248

RESUMEN

Myoepithelium plays an important role in mammary gland development, but less is known about the molecular mechanism underlying how myoepithelium controls acinus differentiation during gestation. Herein, we found that loss of Kindlin-2 in myoepithelial cells impaired mammary morphogenesis, alveologenesis, and lactation. Using five genetically modified mouse lines combined with single-cell RNA sequencing, we found a Kindlin-2-Stat3-Dll1 signaling cascade in myoepithelial cells that inactivates Notch signaling in luminal cells and consequently drives luminal progenitor commitment to alveolar cells identity. Single-cell profiling revealed that Kindlin-2 loss significantly reduces the proportion of matured alveolar cells. Mechanistically, Kindlin-2 depletion in myoepithelial cells promotes Stat3 activation and upregulates Dll1, which activates the Notch pathway in luminal cells and inhibits luminal progenitor differentiation and maturation during gestation. Inhibition of Notch1 with tangeretin allowed luminal progenitors to regain commitment ability in the pregnant mice with Kindlin-2 depletion in myoepithelium. Taken together, we demonstrated that Kindlin-2 is essential to myoepithelium-controlled luminal progenitors to alveoli transition during gestation.


Asunto(s)
Células Epiteliales , Glándulas Mamarias Animales , Animales , Femenino , Ratones , Embarazo , Diferenciación Celular , Células Epiteliales/metabolismo , Epitelio , Lactancia
9.
Dalton Trans ; 52(39): 14132-14141, 2023 Oct 10.
Artículo en Inglés | MEDLINE | ID: mdl-37747221

RESUMEN

The optical characteristics of multimode luminescent materials like multimode luminescence (photoluminescence, afterglow, thermoluminescence) and a multi-excitation source (light, thermal, mechanical force) play crucial roles in optical data storage and readout, document security and anticounterfeiting. A higher level of advanced anticounterfeiting may rely on multimode anticounterfeiting materials that can realize multicolor luminescence. Here, a highly integrated multimode and multicolor Y7O6F9:Er3+,Eu3+ material is developed through multiplexing of dual lanthanides in fluorine oxide particles. In photoluminescence and photoluminescence/up-conversion luminescence modes, the material Y7O6F9:Er3+,Eu3+ has the characteristic of excitation wavelength and power dependence. In the photoluminescence mode, under excitation at 254 nm and 365 nm, Y7O6F9:Er3+ and Y7O6F9:Eu3+ showed bright red and green emissions, respectively. In the photoluminescence/up-conversion mode, under the increased excitation power from 0.2 to 2.0 W cm-2, the color of luminescence emission can be finely tuned from red to orange, yellow and green. Taking this unique excitation wavelength-power-dependent luminescence property into account, a multilevel anticounterfeiting device with the Lily pattern was designed. The device readily integrates the advantages of the excitation wavelength-dependent photoluminescence emissions and excitation power-dependent photoluminescence emissions in one overall device. These findings offer unique insight for designing highly integrated multimode, multicolor luminescence materials and advanced anticounterfeiting technology toward a wide variety of applications, particularly multilevel anticounterfeiting devices.

10.
J Fluoresc ; 2023 Sep 18.
Artículo en Inglés | MEDLINE | ID: mdl-37721706

RESUMEN

The development of portable and cost-effective sensing system for Hg2+ quantitation is highly demanded for environmental monitoring. Herein, an on-site, rapid and portable smartphone readout device based Hg2+ sensing system integrating nitrogen-doped carbon quantum dots (NCDs) modified paper strip was proposed, and the physicochemical properties of NCDs were characterized by high resolution TEM, FTIR, UV-vis absorption spectrum and fluorescence spectral analysis. The modified paper strip was prepared via "ink-jet" printing technology and exhibits sensitive fluorescence response to Hg2+ with fluorescence color of bright blue (at the excitation/emission wavelength of 365/440 nm). This portable smartphone-based sensing platform is highly selective and sensitive to Hg2+ with the limit of detection (LOD) of 10.6 nM and the concentration range of 0-130 nM. In addition, the recoveries of tap water and local lake water were in the range of 89.4% to 109%. The cost-effective sensing system based on smartphone shows a great potential for trace amounts of Hg2+ monitoring in environmental water samples.

11.
Dalton Trans ; 52(33): 11649-11657, 2023 Aug 22.
Artículo en Inglés | MEDLINE | ID: mdl-37552091

RESUMEN

In recent years, a series of persistent luminescence materials excitable by blue light have been developed and widely used in many fields such as optical information storage, AC-LEDs, anti-counterfeiting and bio-imaging. However, it is still a long-standing challenge to develop a superior red-emitting persistent phosphor that can be efficiently excited by blue light. In this work, a novel blue-light excited red-emitting persistent phosphor CaCd2Ga2Ge3O12:Pr3+ was successfully synthesized by using a solid-state method, showing excellent luminescence properties. Moreover, the phase purity, crystal structure, photoluminescence spectra, afterglow emission spectra, and three-dimensional thermoluminescence spectrum were successfully investigated. Under 294 nm excitation, photoluminescence spectra show a single orange emission and a series of peaks centered at 492, 537, 568, 614 and 664 nm, which correspond to the 3P0 → 3H4, 3P0 → 3H5, 3P2 → 3H6, 1D2 → 3H4, and 3P0 → 3F2 transitions of Pr3+, respectively. Interestingly, after blue light excitation, the afterglow luminescence exhibits red long emission, which is attributed to the 1D2 → 3H4 transition of Pr3+. Through thermoluminescence spectra and three-dimensional thermoluminescence spectra, we analyze the reasons for the different colors of photoluminescence and afterglow luminescence. The results imply that there are two types of traps, and the depth of shallow traps and deep traps is calculated to be 0.684 and 0.776 eV, respectively. It is worth noting that the photoluminescence is attributed to the 4f2 → 4f5d and f → f transitions of Pr3+, and the afterglow luminescence is ascribed to a tunneling-related process and the transition of electrons from the valence band to the conduction band. The obtained red-emitting persistent phosphors provide a promising pathway toward AC-LEDs, multi-cycle bio-imaging and other fields.

12.
Cell Rep ; 42(8): 112886, 2023 08 29.
Artículo en Inglés | MEDLINE | ID: mdl-37527040

RESUMEN

Cyclin-dependent kinase 4 (CDK4) and retinoblastoma protein (RB) are both important cell-cycle regulators that function in different scenarios. Here, we report that FERM domain-containing 8 (FRMD8) inhibits CDK4 activation and stabilizes RB, thereby causing cell-cycle arrest and inhibiting colorectal cancer (CRC) cell growth. FRMD8 interacts separately with CDK7 and CDK4, and it disrupts the interaction of CDK7 with CDK4, subsequently inhibiting CDK4 activation. FRMD8 competes with MDM2 to bind RB and attenuates MDM2-mediated RB degradation. Frmd8 deficiency in mice accelerates azoxymethane/dextran-sodium-sulfate-induced colorectal adenoma formation. The FRMD8 promoter is hypermethylated, and low expression of FRMD8 predicts poor prognosis in CRC patients. Further, we identify an LKCHE-containing FRMD8 peptide that blocks MDM2 binding to RB and stabilizes RB. Combined application of the CDK4 inhibitor and FRMD8 peptide leads to marked suppression of CRC cell growth. Therefore, using an LKCHE-containing peptide to interfere with the MDM2-RB interaction may have therapeutic value in CDK4/6 inhibitor-resistant patients.


Asunto(s)
Neoplasias del Colon , Quinasas Ciclina-Dependientes , Animales , Ratones , Neoplasias del Colon/genética , Quinasa 4 Dependiente de la Ciclina/metabolismo , Quinasas Ciclina-Dependientes/metabolismo , Fosforilación , Proteína de Retinoblastoma/metabolismo
13.
Dalton Trans ; 52(7): 2145-2156, 2023 Feb 14.
Artículo en Inglés | MEDLINE | ID: mdl-36722897

RESUMEN

Luminescent anti-counterfeiting materials have drawn much attention in anti-counterfeiting applications due to their photochemical stability and emission patterns. However, conventional materials majorly use single-mode luminescence, leaving a growing demand for new materials to prevent counterfeiting. In this work, multi-mode anti-counterfeiting is guaranteed from a single luminescent material CaCd2Ga2Ge3O12:Tb3+,Yb3+via a high-temperature solid-state reaction. The experimental result showed that this single material features green luminescence with excellent photoluminescence, afterglow, thermoluminescence, and up-conversion luminescence, which are ascribed to Tb3+ transitions. Upon co-doping with Yb3+ as a sensitiser, the photo-stimuli responsiveness was achieved at 254 and 980 nm excitation sources, respectively, and the thermo-stimuli responsiveness was realised after exposure to UV of 254 nm for 10 s and heating at 45 °C, respectively. The band structure calculation, trap distribution, and effective trap depths were used to explain the luminescence mechanism. Based on the two-stimuli responsiveness and four-state emission performance, we prepared images of optical devices using silk screen printing technology. It was found that the images displayed green emission under different luminescence modes. The results prove that we successfully constructed an advanced luminescence anti-counterfeiting material.

14.
Inorg Chem ; 62(1): 75-86, 2023 Jan 09.
Artículo en Inglés | MEDLINE | ID: mdl-36574356

RESUMEN

The continuously growing significance of information security and authentication has put forward many new requirements and challenges for modern luminescent materials and anti-counterfeiting technologies. Recently, luminescent materials have attracted much attention in this field owing to their legibility, repeatability, multicolor, and multiple stimuli-responsive nature. In this work, the efficient multicolor and multimodal luminescence material CaCd2Ga2Ge3O12:Mn2+ was successfully designed and synthesized using the strategy of single-doped Mn2+ in a single matrix. Also, we combined the morphology, crystal structure, energy band calculation, luminescence properties, and trap analysis to study the optical data storage capacity of CaCd2Ga2Ge3O12:Mn2+. Interestingly, in the presence of the 254 nm UV lamp, the sample can exhibit a tunable emission color from bule to cyan to yellow by increasing the dopant concentration of Mn2+. Also, under the afterglow and thermoluminescence luminescence modes, it presented strong yellow emission centered at 558 nm. Based on the advantage of multiple tunable luminescence, samples were made into anti-counterfeiting ink and were used to print four optical devices through the screen printing technology. The results show that the material has excellent multicolor anti-counterfeiting properties under the three luminescence modes, which has contributed to the development of many kinds of luminescent anti-counterfeiting materials for security purposes.


Asunto(s)
Luminiscencia , Humanos , Manganeso , Germanio , Cadmio , Calcio
15.
Adv Mater ; 34(43): e2205414, 2022 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-36042002

RESUMEN

Electrochemical generation of hydrogen peroxide (H2 O2 ) by two-electron oxygen reduction offers a green method to mitigate the current dependence on the energy-intensive anthraquinone process, promising its on-site applications. Unfortunately, in alkaline environments, H2 O2 is not stable and undergoes rapid decomposition. Making H2 O2 in acidic electrolytes can prevent its decomposition, but choices of active, stable, and selective electrocatalysts are significantly limited. Here, the selective and efficient two-electron reduction of oxygen toward H2 O2 in acid by a composite catalyst that is composed of black phosphorus (BP) nailed chemically on the metallic cobalt diselenide (CoSe2 ) surface is reported. It is found that this catalyst exhibits a 91% Faradic efficiency for H2 O2 product at an overpotential of 300 mV. Moreover, it can mediate oxygen to H2 O2 with a high production rate of ≈1530 mg L-1 h-1 cm-2 in a flow-cell reactor. Spectroscopic and computational studies together uncover a BP-induced surface charge redistribution in CoSe2 , which leads to a favorable surface electronic structure that weakens the HOO* adsorption, thus enhancing the kinetics toward H2 O2 formation.

16.
Cell Rep ; 40(8): 111210, 2022 08 23.
Artículo en Inglés | MEDLINE | ID: mdl-36001969

RESUMEN

HOXB9 is an important transcription factor associated with unfavorable outcomes in patients with lung adenocarcinoma (LUAD). However, its degradation mechanism remains unclear. Here, we show that HOXB9 is a substrate of AMP kinase alpha (AMPKα). AMPK mediates HOXB9 T133 phosphorylation and downregulates the level of HOXB9 in mice and LUAD cells. Mechanistically, phosphorylated HOXB9 promoted E3 ligase Praja2-mediated HOXB9 degradation. Blocking HOXB9 phosphorylation by depleting AMPKα1/2 or employing the HOXB9 T133A mutant promoted tumor cell growth in cell culture and mouse xenografts via upregulation of HOXB9 and KRAS that is herein identified as a target of HOXB9. Clinically, AMPK activation levels in LUAD samples were positively correlated with pHOXB9 levels; higher pHOXB9 levels were associated with better survival of patients with LUAD. We thus present a HOXB9 degradation mechanism and demonstrate an AMPK-HOXB9-KRAS axis linking glucose-level-regulated AMPK activation to HOXB9 stability and KRAS gene expression, ultimately controlling LUAD progression.


Asunto(s)
Adenocarcinoma del Pulmón , Adenocarcinoma , Neoplasias Pulmonares , Proteínas Quinasas Activadas por AMP/metabolismo , Adenocarcinoma/patología , Adenocarcinoma del Pulmón/genética , Adenocarcinoma del Pulmón/patología , Animales , Regulación Neoplásica de la Expresión Génica , Proteínas de Homeodominio/genética , Proteínas de Homeodominio/metabolismo , Humanos , Neoplasias Pulmonares/patología , Ratones , Proteínas Proto-Oncogénicas p21(ras)/genética , Proteínas Proto-Oncogénicas p21(ras)/metabolismo
17.
Phys Chem Chem Phys ; 24(28): 17116-17120, 2022 Jul 21.
Artículo en Inglés | MEDLINE | ID: mdl-35791889

RESUMEN

A good oxygen reduction reaction (ORR) catalyst should be stable and active under electrochemical reaction conditions. Niobium pentaoxide (Nb2O5) is known to be stable under ORR conditions. However it has a large band gap, which makes conductivity a challenge during the reaction. In this work, we aim to understand if surface modification of the 110 facet of niobium pentaoxide with transition metal doping has any effect on its ORR activity and conductivity. While the problem of conductivity in the case of transition metal oxides (TMOs) can be partially rectified by transition metal doping, it has negligible influence on the ORR activity of the doped systems.

18.
Adv Sci (Weinh) ; 9(27): e2201916, 2022 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-35869034

RESUMEN

Exploring low cost, highly active, and durable electrocatalysts for oxygen evolution reaction (OER) is of prime importance to boost energy conversion efficiency. Perovskite fluorides are emerging as alternative electrocatalysts for OER, however, their intrinsically active sites during real operation are still elusive. Herein, the self-reconstruction on newly designed NiFe coupled perovskite fluorides during OER process is demonstrated. In situ Raman spectroscopy, ex situ X-ray absorption spectroscopy, and theoretical calculation reveal that Fe incorporation can significantly activate the self-reconstruction of perovskite fluorides and efficiently lower the energy barrier of OER. Benefiting from self-reconstruction and low energy barrier, the KNi0.8 Fe0.2 F3 @nickel foam (KNFF2@NF) electrocatalyst delivers an ultralow overpotential of 258 mV to afford 100 mA cm-2 and an excellent durability for 100 h, favorably rivaling most the state-of-the-art OER electrocatalysts. This protocol provides the fundamental understanding on OER mechanism associated with surface reconstruction for perovskite fluorides.

19.
Nat Commun ; 13(1): 2382, 2022 May 02.
Artículo en Inglés | MEDLINE | ID: mdl-35501341

RESUMEN

The need for efficient ammonia synthesis is as urgent as ever. Over the past two decades, many attempts to find new catalysts for ammonia synthesis at mild conditions have been reported and, in particular, many new promoters of the catalytic rate have been introduced beyond the traditional K and Cs oxides. Herein, we provide an overview of recent experimental results for non-traditional promoters and develop a comprehensive model to explain how they work. The model has two components. First, we establish what is the most likely structure of the active sites in the presence of the different promoters. We then show that there are two effects dictating the catalytic activity. One is an electrostatic interaction between the adsorbed promoter and the N-N dissociation transition state. In addition, we identify a new promoter effect for magnetic catalysts giving rise to an anomalously large lowering of the activation energy opening the possibility of finding new ammonia synthesis catalysts.

20.
Nat Commun ; 13(1): 2294, 2022 Apr 28.
Artículo en Inglés | MEDLINE | ID: mdl-35484271

RESUMEN

Developing non-noble catalysts with superior activity and durability for oxygen evolution reaction (OER) in acidic media is paramount for hydrogen production from water. Still, challenges remain due to the inadequate activity and stability of the OER catalyst. Here, we report a cost-effective and stable manganese oxybromide (Mn7.5O10Br3) catalyst exhibiting an excellent OER activity in acidic electrolytes, with an overpotential of as low as 295 ± 5 mV at a current density of 10 mA cm-2. Mn7.5O10Br3 maintains good stability under operating conditions for at least 500 h. In situ Raman spectroscopy, X ray absorption near edge spectroscopy, and density functional theory calculations confirm that a self-oxidized surface with enhanced electronic transmission capacity forms on Mn7.5O10Br3 and is responsible for both the high catalytic activity and long-term stability during catalysis. The development of Mn7.5O10Br3 as an OER catalyst provides crucial insights into the design of non-noble metal electrocatalysts for water oxidation.

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