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1.
Small ; 20(24): e2309769, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38155589

RESUMO

Complicated oxygen evolution reaction (OER) poses the bottleneck in improving the efficiency of hydrogen production through water electrolysis. Herein, an integrated strategy to modulate the electronic structure of NiFe layered double hydroxide (NiFe-LDH) is reported by constructing Ag-incorporated NiCo-PBA@NiFe-LDH heterojunction with a hierarchical hollow structure. This "double heterojunction" facilitates local charge polarization at the interface, thereby promoting electron transfer and reducing the adsorption energy of intermediates, ultimately enhancing the intrinsic activity of the catalyst. It is noteworthy that an exchange bias field is observed between NiCo-PBA and NiFe-LDH, which will be conducive to regulating the electron spin states of metals and facilitating the production of triplet oxygen. Additionally, the unique hierarchical nanoboxes provide a large specific surface area that ensures adequate exposure to adsorption sites and active sites. Profiting from the synergistic advantages, the overpotential is as low as 190 mV at a current density of 10 mA cm-2, with a low Tafel slope of 21 mV dec-1. Moreover, density functional theory (DFT) calculation further substantiated that the incorporation of Ag in the heterojunction can effectively reduce the adsorption energy of reactant intermediates and enhance the conductivity.

2.
Small ; 20(40): e2403435, 2024 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-38874079

RESUMO

The cycling lifespan of Li-metal batteries is compromised by the unstable solid electrolyte interphase (SEI) and the continuous Li dendrites, restricting their practical implementations. Given these challenges, establishing an artificial SEI holds promise. Herein, a trinitarian gradient interphase is innovatively designed through composite coatings of magnesium fluoride (MgF2), N-hexadecyltrimethylammonium chloride (CTAC), and polyvinylidene fluoride-hexafluoropropylene copolymer (PVDF-HFP) on Li-metal anode (LMA). Specifically, the MgF2/CTAC/PVDF-HFP SEI spontaneously forms a lithium fluoride (LiF)-rich PVDF-HFP-based SEI, along with lithium-magnesium (Li-Mg) alloy substrate as lithiophilic electronic conductor and positively charged CTAC during plating. Noticeably, the Li-Mg alloy homogenizes the distribution of electric field and reduce the internal resistance, while the electronically insulated LiF/PVDF-HFP composite SEI offers fast ion-conducting and mechanical flexibility, accommodating the volumetric expansion and ensuring stable Li-ion flux. Additionally, CTAC at the dendritic tip is pivotal for mitigating dendrites through its electrostatic shield mechanism. Innovatively, this trinitarian synergistic mechanism, which facilitates colossal granular Li deposits, constructs a dendrite-free LMA, leading to stable cycling performances in practical Li||LFP, popular Li||NCM811, and promising Li||S full cells. This work demonstrates the design of multifunctional composite SEI for comprehensive Li protection, thereby inspiring further advancements in artificial SEI engineering for alkali-metal batteries.

3.
Chemistry ; 30(2): e202302867, 2024 Jan 08.
Artigo em Inglês | MEDLINE | ID: mdl-37885053

RESUMO

Lithium metal batteries are deemed as an optimal candidate for the next generation of durable energy storage devices. However, the growth of lithium dendrite and significant volume expansion pose as obstacles that impede the application of lithium metal batteries. In this work, a functional copper current collector was designed by coating it with Co-doped ZnO (Co/ZnO) to enhance the lithiophilicity through local electric fields and built-in magnetic fields induced by the ferromagnetic material. The incorporation of Co not only induces a local electric field and thus accelerating electron transfer, but also imparts the ferromagnetic behavior to ZnO, resulting in an internal magnetic field to regulate the dynamic trajectory. Profiting from the above advantages, the symmetric cells have excellent cycle stability in 1 mA cm-2 and 1 mAh cm-2 , maintaining ultra-low voltage for over 2000 h. This study provides a realizable pathway for next-generation current collector of copper modification.

4.
Chemistry ; 30(8): e202303507, 2024 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-37994505

RESUMO

The Sabatier principle suggests that an excessive adsorption of lithium polysulfides (LiPSs) by metal compounds may hinder their conversion in the absence of a conversion module. Therefore, it is imperative to establish a synergetic effect mechanism between "strong adsorption" and "rapid conversion" for LiPSs. To achieve this coexistence, a molybdenum-doped MnS/MnO@C porous structure is designed as a multifunctional coating on the polypropylene (PP) separator. The incorporation of MnS/MnO@C enhances the adsorption capacity towards LiPSs, while molybdenum facilitates subsequent conversion. Benefiting from the synergistic effect of each component and its large specific surface area, the cell with Mo-doped MnS/MnO@C coating achieves smooth adsorption-diffusion-conversion processes and exhibits an appreciable rate performance with outstanding cycling stability. Even when sulfur loading increases to 9.68 mg cm-2 , the modified battery delivers an excellent initial areal capacity of 11.69 mAh cm-2 and maintains 6.97 mAh cm-2 after 50 cycles at 0.1 C. This study presents a promising approach to simultaneously accomplish "strong adsorption" and "rapid conversion" of polysulfides, offering novel perspectives for devising dual-functional modified separators.

5.
FASEB J ; 37(4): e22880, 2023 04.
Artigo em Inglês | MEDLINE | ID: mdl-36943407

RESUMO

Shp2 is a nonreceptor protein tyrosine phosphatase that is overexpressed in cervical cancer. However, the role of Shp2 in the regulation of cervical cancer metabolism and tumorigenesis is unclear. EGFR signaling pathways are commonly dysregulated in cervical cancer. We showed that Shp2 knockout in cervical cancer cells decreased EGFR expression and downregulated downstream RAS-ERK activation. Although AKT was activated in Shp2 knockout cells, inhibition of AKT activation could not make cells more sensitive to death. Shp2 depletion inhibited cervical cancer cell proliferation and reduced tumor growth in a xenograft mouse model. 1 H NMR spectroscopic analysis showed that glutamine, glutamate, succinate, creatine, glutathione, and UDP-GlcNAc were significantly changed in Shp2 knockout cells. The intracellular glutamine level was higher in Shp2 knockout cells than in control cells. Further analysis demonstrated that Shp2 knockout promoted glutaminolysis and glutathione production by up-regulating the glutamine metabolism-related genes such as glutaminase (GLS). However, inhibition of GLS did not always make cells sensitive to death, which was dependent on glucose concentration. The level of oxidative phosphorylation was significantly increased, accompanied by an increased generation of reactive oxygen species in Shp2 knockout cells. Shp2 deficiency increased c-Myc and c-Jun expression, which may be related to the upregulation of glutamine metabolism. These findings suggested that Shp2 regulates cervical cancer proliferation, glutamine metabolism, and tumorigenicity.


Assuntos
Glutamina , Neoplasias do Colo do Útero , Feminino , Humanos , Animais , Camundongos , Neoplasias do Colo do Útero/genética , Proteínas Proto-Oncogênicas c-akt/metabolismo , Receptores ErbB/genética , Tirosina/metabolismo , Monoéster Fosfórico Hidrolases , Proteína Tirosina Fosfatase não Receptora Tipo 11/genética , Proteína Tirosina Fosfatase não Receptora Tipo 11/metabolismo
6.
Crit Care ; 28(1): 274, 2024 Aug 17.
Artigo em Inglês | MEDLINE | ID: mdl-39154185

RESUMO

OBJECTIVE: Our study aimed to investigate the effects of different extracorporeal membrane oxygenation (ECMO) blood flow rates on lung perfusion assessment using the saline bolus-based electrical impedance tomography (EIT) technique in patients on veno-venous (VV) ECMO. METHODS: In this single-centered prospective physiological study, patients on VV ECMO who met the ECMO weaning criteria were assessed for lung perfusion using saline bolus-based EIT at various ECMO blood flow rates (gradually decreased from 4.5 L/min to 3.5 L/min, 2.5 L/min, 1.5 L/min, and finally to 0 L/min). Lung perfusion distribution, dead space, shunt, ventilation/perfusion matching, and recirculation fraction at different flow rates were compared. RESULTS: Fifteen patients were included. As the ECMO blood flow rate decreased from 4.5 L/min to 0 L/min, the recirculation fraction decreased significantly. The main EIT-based findings were as follows. (1) Median lung perfusion significantly increased in region-of-interest (ROI) 2 and the ventral region [38.21 (34.93-42.16)% to 41.29 (35.32-43.75)%, p = 0.003, and 48.86 (45.53-58.96)% to 54.12 (45.07-61.16)%, p = 0.037, respectively], whereas it significantly decreased in ROI 4 and the dorsal region [7.87 (5.42-9.78)% to 6.08 (5.27-9.34)%, p = 0.049, and 51.14 (41.04-54.47)% to 45.88 (38.84-54.93)%, p = 0.037, respectively]. (2) Dead space significantly decreased, and ventilation/perfusion matching significantly increased in both the ventral and global regions. (3) No significant variations were observed in regional and global shunt. CONCLUSIONS: During VV ECMO, the ECMO blood flow rate, closely linked to recirculation fraction, could affect the accuracy of lung perfusion assessment using hypertonic saline bolus-based EIT.


Assuntos
Impedância Elétrica , Oxigenação por Membrana Extracorpórea , Pulmão , Tomografia , Humanos , Oxigenação por Membrana Extracorpórea/métodos , Masculino , Feminino , Estudos Prospectivos , Impedância Elétrica/uso terapêutico , Pessoa de Meia-Idade , Adulto , Tomografia/métodos , Pulmão/irrigação sanguínea , Pulmão/fisiopatologia , Pulmão/diagnóstico por imagem , Solução Salina Hipertônica/uso terapêutico , Idoso , Velocidade do Fluxo Sanguíneo/fisiologia
7.
Crit Care ; 27(1): 474, 2023 12 04.
Artigo em Inglês | MEDLINE | ID: mdl-38049909

RESUMO

OBJECTIVE: To compare the efficacy and safety of remimazolam besylate and propofol for deep sedation in critically ill patients. METHODS: In this single-center, prospective, randomized, controlled pilot study, patients in the intensive care unit (ICU) requiring deep sedation were randomized to receive remimazolam besylate or propofol intravenously. Deep sedation was defined as a Richmond Agitation and Sedation Scale (RASS) score of - 4 or - 5. Sedation depth was monitored using RASS and Narcotrend Index (NI). The primary outcome was the percentage of time within the target sedation range without rescue sedation. The secondary outcomes included ventilator-free hours within 7 days, successful extubation, length of ICU stay, and 28-day mortality. Adverse events during the interventional period were also recorded. RESULTS: Thirty patients were assigned to each group. The median (IQR) RASS score was - 5.0 (- 5.0, - 4.0), and the median (IQR) NI value was 29.0 (21.0, 37.0) during the intervention period. Target RASS was reached a median of 100% of the sedation time in the two groups. No significant differences were observed in ventilator-free hours within 7 days, successful extubation, length of ICU stay, or 28-day mortality among groups. Hypotension occurred in 16 (53.3%) patients of remimazolam group and 18 (60.0%) patients of propofol group (p > 0.05). No patient experienced bradycardia. CONCLUSIONS: Remimazolam besylate appears to be an effective and safe agent for short-term deep sedation in critically ill patients. Our findings warrant large sample-sized randomized clinical trials.


Assuntos
Sedação Profunda , Propofol , Humanos , Estado Terminal/terapia , Hipnóticos e Sedativos/farmacologia , Hipnóticos e Sedativos/uso terapêutico , Projetos Piloto , Propofol/farmacologia , Propofol/uso terapêutico , Estudos Prospectivos , Respiração Artificial
8.
BMC Pulm Med ; 22(1): 52, 2022 Feb 05.
Artigo em Inglês | MEDLINE | ID: mdl-35123448

RESUMO

COVID-19 has inflicted the world for over two years. The recent mutant virus strains pose greater challenges to disease prevention and treatment. COVID-19 can cause acute respiratory distress syndrome (ARDS) and extrapulmonary injury. Dynamic monitoring of each patient's condition is necessary to timely tailor treatments, improve prognosis and reduce mortality. Point-of-care ultrasound (POCUS) is broadly used in patients with ARDS. POCUS is recommended to be performed regularly in COVID-19 patients for respiratory failure management. In this review, we summarized the ultrasound characteristics of COVID-19 patients, mainly focusing on lung ultrasound and echocardiography. Furthermore, we also provided the experience of using POCUS to manage COVID-19-related ARDS.


Assuntos
COVID-19/diagnóstico por imagem , Ecocardiografia , Pulmão/diagnóstico por imagem , Testes Imediatos , Síndrome do Desconforto Respiratório/diagnóstico por imagem , Terapia Respiratória/métodos , COVID-19/terapia , Humanos , Síndrome do Desconforto Respiratório/terapia , Síndrome do Desconforto Respiratório/virologia
9.
Mediators Inflamm ; 2022: 1474891, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-35125962

RESUMO

BACKGROUND: The cholinergic anti-inflammatory pathway connects the immune response system and the nervous system via the vagus nerve. The key regulatory receptor is the α7-subtype of the nicotinic acetylcholine receptor (α7nAChR). Cholinergic anti-inflammatory pathway has been proved to be effective in suppressing the inflammation responses in acute lung injury (ALI). Dendritic cells (DCs), the important antigen-presenting cells, also express the α7nAChR. Past studies have indicated that reducing the quantity of mature conventional DCs and inhibiting the maturation of pulmonary DCs may prove effective for the treatment of ALI. However, the effects of cholinergic anti-inflammatory pathway on maturation, function, and quantity of DCs and conventional DCs in ALI remain unclear. OBJECTIVE: It was hypothesized that cholinergic anti-inflammatory pathway may inhibit the inflammatory response of ALI by regulating maturation, phenotype, and quantity of DCs and conventional DCs. METHODS: GTS-21 (GTS-21 dihydrochloride), an α7nAchR agonist, was prophylactically administered in sepsis-induced ALI mouse model and LPS-primed bone marrow-derived dendritic cells. The effects of GTS-21 were observed with respect to maturation, phenotype, and quantity of DCs, conventional DCs, and conventional DCs2 (type 2 conventional DCs) and the release of DC-related proinflammatory cytokines in vivo and in vitro. RESULTS: The results of the present study revealed that GTS-21 treatment decreased the maturation of DCs and the production of DC-related proinflammatory cytokines in vitro and in sepsis-induced ALI mouse model; it reduced the quantity of CD11c+MHCII+ conventional DCs and CD11c+CD11b+ conventional DCs2 in vivo experiment. CONCLUSIONS: Cholinergic anti-inflammatory pathway contributes to the reduction in the inflammatory response in ALI by regulating maturation, phenotype, and quantity of DCs, conventional DCs, and conventional DCs2.


Assuntos
Lesão Pulmonar Aguda , Sepse , Lesão Pulmonar Aguda/metabolismo , Animais , Células Dendríticas/metabolismo , Lipopolissacarídeos/metabolismo , Lipopolissacarídeos/farmacologia , Camundongos , Neuroimunomodulação , Sepse/metabolismo
10.
Chemistry ; 25(63): 14358-14363, 2019 Nov 13.
Artigo em Inglês | MEDLINE | ID: mdl-31423674

RESUMO

The development of sodium-ion batteries (SIBs) is hindered by the rapid reduction in reversible capacity of carbon-based anode materials. Outside-in doping of carbon-based anodes has been extensively explored. Nickel and NiS2 particles embedded in nitrogen and sulfur codoped porous graphene can significantly improve the electrochemical performance. Herein a built-in heteroatom "self-doping" of albumen-derived graphene for sodium storage is reported. The built-in sulfur and nitrogen in albumen act as the doping source during the carbonization of proteins. The sulfur-rich proteins in albumen can also guide the doping and nucleation of nickel sulfide nanoparticles. Additionally, the porous architecture of the carbonized proteins is achieved through removable KCl/NaCl salts (medium) under high-temperature melting conditions. During the carbonization process, nitrogen can also reduce the carbonization temperature of thermally stable carbon materials. In this work, the NS-graphene delivered a specific capacity of 108.3 mAh g-1 after 800 cycles under a constant current density of 500 mA g-1 . In contrast, the Ni/NiS2 /NS-graphene maintained a specific capacity of 134.4 mAh g-1 ; thus the presence of Ni/NiS2 particles improved the electrochemical performance of the whole composite.

12.
Molecules ; 23(9)2018 Aug 29.
Artigo em Inglês | MEDLINE | ID: mdl-30158429

RESUMO

A method for the rapid determination of 4-hexylresorcinol (4-HR) residue in shrimp by solid phase extraction (SPE) ultra-high performance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS) was established. 4-HR was extracted twice with methanol, and the extract was formulated into methanol-water solution (1:1). After being cleaned up and concentrated by a PRIME HLB solid phase extraction column, the sample was analyzed by UPLC-MS/MS and quantitatively determined by an external standard method. The separation was performed with a gradient system consisting of water and acetonitrile as the mobile phase. Monitoring was performed by electrospray ionization (ESI) in negative ion mode using multiple ion reaction monitoring (MRM). Good linearity was obtained in the concentration range of 1.0⁻100.0 µg/L, with correlation coefficients larger than 0.999. The limit of detection (LOD) was 0.25 µg/kg and the limit of quantification (LOQ) was 0.80 µg/kg. The average recoveries of 4-HR at spiked concentrations of 2.40, 6.40 and 16 µg/kg ranged from 81.35% to 94.68% with the relative standard deviations (n = 6) from 3.57% to 6.86%. The results showed that the method is simple, fast, sensitive, reliable, and reproducible; thus, it could be used as a rapid confirmation and quantitative analysis method of 4-HR residue in aquatic products.


Assuntos
Anti-Helmínticos/análise , Crustáceos/química , Hexilresorcinol/análise , Animais , Anti-Helmínticos/química , Cromatografia Líquida de Alta Pressão , Monitoramento Ambiental , Hexilresorcinol/química , Limite de Detecção , Extração em Fase Sólida , Espectrometria de Massas em Tandem
13.
Angew Chem Int Ed Engl ; 55(21): 6290-4, 2016 05 17.
Artigo em Inglês | MEDLINE | ID: mdl-27061909

RESUMO

Bifunctional electrocatalysts for the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in alkaline electrolyte may improve the efficiency of overall water splitting. Nickel cobaltite (NiCo2 O4 ) has been considered a promising electrode material for the OER. However, NiCo2 O4 that can be used as an electrocatalyst in HER has not been studied yet. Herein, we report self-assembled hierarchical NiCo2 O4 hollow microcuboids for overall water splitting including both the HER and OER reactions. The NiCo2 O4 electrode shows excellent activity toward overall water splitting, with 10 mA cm(-2) water-splitting current reached by applying just 1.65 V and 20 mA cm(-2) by applying just 1.74 V across the two electrodes. The synthesis of NiCo2 O4 microflowers confirms the importance of structural features for high-performance overall water splitting.

14.
Angew Chem Int Ed Engl ; 54(48): 14331-5, 2015 Nov 23.
Artigo em Inglês | MEDLINE | ID: mdl-26429596

RESUMO

Titanium dioxide (TiO2) is considered a promising anode material for high-power lithium ion batteries (LIBs) because of its low cost, high thermal/chemical stability, and good safety performance without solid electrolyte interface formation. However, the poor electronic conductivity and low lithium ion diffusivity of TiO2 result in poor cyclability and lithium ion depletion at high current rates, which hinder them from practical applications. Herein we demonstrate that hierarchically structured TiO2 microboxes with controlled internal porosity can address the aforementioned problems for high-power, long-life LIB anodes. A self-templating method for the synthesis of mesoporous microboxes was developed through Na2 EDTA-assisted ion exchange of CaTiO3 microcubes. The resulting TiO2 nanorods were organized into microboxes that resemble the microcube precursors. This nanostructured TiO2 material has superior lithium storage properties with a capacity of 187 mAh g(-1) after 300 cycles at 1 C and good rate capabilities up to 20 C.

15.
Small ; 10(14): 2815-9, 2742, 2014 Jul 23.
Artigo em Inglês | MEDLINE | ID: mdl-24677569

RESUMO

One-dimensional Fe3O4/C composite microrods are synthesized via a facile one-pot solvothermal reaction in the presence of an external magnetic field. When evaluated as an anode material for lithium ion batteries, these Fe3O4/C microrods manifest high specific capacity and excellent cycling performance.

16.
Angew Chem Int Ed Engl ; 53(23): 5917-21, 2014 Jun 02.
Artigo em Inglês | MEDLINE | ID: mdl-24821565

RESUMO

Semiconductor heterostructures are of great interest in a wide range of applications. In this work, we design and synthesize a novel heteronanostructure with controlled relative composition, i.e., BiVO4/Bi2S3 hollow discoid-like particles with mesoporous shell. The synthesis involves a facile anion exchange process by reacting pre-synthesized BiVO4 discoid-like particles with Na2S in an aqueous solution. Benefiting from the unique structural features and the formation of heterostructure, the as-prepared BiVO4/Bi2S3 hollow discoids exhibit significantly enhanced photoelectrochemical current response and photocatalytic activity for reduction of Cr(VI) under visible-light illumination.

17.
Eur J Med Res ; 29(1): 463, 2024 Sep 17.
Artigo em Inglês | MEDLINE | ID: mdl-39289769

RESUMO

BACKGROUND: The epidemiology of fungi identified via next-generation sequencing in bronchoalveolar lavage fluid among patients with COVID-19 is unknown. METHODS: De-identified information, including age, SARS-CoV-2 reads and fungi from bronchoalveolar lavage fluid, were used to analysis. RESULTS: A total of 960 patients with COVID-19 were included. Gender was unknown in 38 patients, and 648 (70.3%) of the rest patients were male. For 876 patients with information on age, their mean ± standard age was 63.4 ± 21.3 years, with the minimum being 0.2 years and the maximum being 101 years. For all the patients, their median [interquartile range] SARS-CoV-2 reads were 26,038 [4421.5, 44,641.5]. The Aspergilli were identified in 159 (16.6%) patients, with Aspergillus fumigatus, Aspergillus flavus and Aspergillus niger in 103 (10.7%), 81 (8.4%) and 17 (1.8%), respectively. The Mucoraceae were identified in 14 (1.5%) patients. Pneumocystis jirovecii was identified in 65 (6.8%) patients, among whom 12 (18.5%) patients also had Aspergilli. The Cryptococcaceae and the Dematiaceae were also identified in some patients, including Cryptococcus in 11 (1.1%) patients. CONCLUSIONS: In bronchoalveolar lavage fluid among patients with COVID-19, the Aspergilli were very commonly identified, as were the Mucoraceae, Pneumocystis jirovecii and Cryptococcus via next-generation sequencing.


Assuntos
Líquido da Lavagem Broncoalveolar , COVID-19 , Sequenciamento de Nucleotídeos em Larga Escala , Humanos , Líquido da Lavagem Broncoalveolar/microbiologia , Líquido da Lavagem Broncoalveolar/virologia , Masculino , COVID-19/diagnóstico , COVID-19/virologia , COVID-19/microbiologia , COVID-19/epidemiologia , Pessoa de Meia-Idade , Feminino , Sequenciamento de Nucleotídeos em Larga Escala/métodos , Idoso , Estudos Retrospectivos , Adulto , Idoso de 80 Anos ou mais , SARS-CoV-2/genética , SARS-CoV-2/isolamento & purificação , Adulto Jovem , Adolescente , Criança , Lactente , Pré-Escolar , Fungos/isolamento & purificação , Fungos/genética , Fungos/classificação
18.
J Colloid Interface Sci ; 674: 677-685, 2024 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-38950466

RESUMO

The construction and regulation of built-in electric field (BIEF) are considered effective strategies for enhancing the oxygen evolution reaction (OER) performance of transition metal-based electrocatalysts. Herein, we present a strategy to regulate the electronic structure of nickel-iron layered double hydroxide (NiFe-LDH) by constructing and enhancing the BIEF induced by in-situ heterojunction transformation. This concept is demonstrated through the design and synthesis of Ag2S@S/NiFe-LDH (p-n heterojunction) and Ag@S/NiFe-LDH (Mott-Schottky heterojunction). Benefiting from the larger BIEF of Mott-Schottky heterojunction, efficient electron transfer occurs at the interface between silver (Ag) and NiFe-LDH. As a result, Ag@S/NiFe-LDH exhibits excellent OER performance, requiring only a 232 mV overpotential at 1 M KOH to achieve a current density of 100 mA cm-2, with a small Tafel slope of 73 mV dec-1, as well as excellent electrocatalytic durability. Density functional theory (DFT) calculations further verified that stronger BIEF in Mott-Schottky heterojunction enhances the electron interaction at the interfaces, reduces the energy barrier for the rate-determining step (RDS), and accelerates the OER kinetics. This work provides an effective strategy for designing catalyst with larger BIEF to enhance electrocatalytic activity.

19.
J Colloid Interface Sci ; 666: 322-330, 2024 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-38603875

RESUMO

The commercial application of lithium-sulfur batteries is primarily impeded by the constant shuttling of soluble polysulfides and sluggish redox kinetics. Nowadays, the discovery of the heterojunction, which combines materials with diverse properties, offers a new perspective for overcoming these obstacles. Herein, a functional coating separator for the lithium-sulfur battery is designed using a MnO2-ZnS p-n heterojunction with a spontaneous built-in electric field (BIEF). The MnO2 nanowire provides suitable adsorption capacity for polysulfides, while the abundant reactive sites brought by ZnS ensure efficient conversion. Moreover, the BIEF significantly facilitates the migration of electrons and polysulfides at the MnO2-ZnS interface, enabling a smooth "adsorption-diffusion-conversion" reaction mechanism. By serving as both the adsorption module and catalytic sites, this BIEF allows batteries utilizing separators modified with MnO2-ZnS heterojunction to achieve an impressive initial capacity of 1511.1 mAh g-1 at 0.1C and maintain a capacity decay rate of merely 0.048% per cycle at 2.0C after 1000 cycles. Even when increasing sulfur loading to 9.4 mg cm-2 in lean electrolyte (5.4 µL mg-1), the battery still exhibits an ultrahigh areal capacity of 6.0 mAh cm-2 after 100 cycles.

20.
ACS Appl Mater Interfaces ; 16(1): 520-529, 2024 Jan 10.
Artigo em Inglês | MEDLINE | ID: mdl-38150322

RESUMO

Pt-based catalysts are regarded as state-of-the-art electrocatalysts for producing clean hydrogen energy; however, their wide application is restricted by their low abundance, high cost, and poor stability. Herein, we report an integrated PtxCoy-hierarchical carbon matrix electrocatalyst (Pt/Co@NCNTs, Pt3Co@NCNTs, PtCo@NCNTs, and PtCo3@NCNTs) that is developed using a thermally driven Co migration strategy forming alloy nanoparticles to achieve efficient hydrogen evolution reaction (HER). Benefiting from its electronic regulation effect and unique hierarchical hollow structure, the Pt3Co@NCNTs catalyst loaded with 11.5 wt % Pt exhibits superior catalytic performance and durability for HER compared with commercial 20 wt % Pt/C. Under both alkaline and acidic conditions, Pt3Co@NCNTs exhibits excellent HER activity with overpotentials of 21 and 45 mV at 10 mA cm-2, respectively. Density functional theory (DFT) results further verify that the interaction between Pt and Co in Pt3Co@NCNTs can modulate electronic rearrangement, optimize the d-band center, and accelerate water dissociation and *H desorption, thereby enhancing HER activity.

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