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1.
Front Neurorobot ; 18: 1368243, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-38559491

RESUMO

Traditional trajectory learning methods based on Imitation Learning (IL) only learn the existing trajectory knowledge from human demonstration. In this way, it can not adapt the trajectory knowledge to the task environment by interacting with the environment and fine-tuning the policy. To address this problem, a global trajectory learning method which combinines IL with Reinforcement Learning (RL) to adapt the knowledge policy to the environment is proposed. In this paper, IL is proposed to acquire basic trajectory skills, and then learns the agent will explore and exploit more policy which is applicable to the current environment by RL. The basic trajectory skills include the knowledge policy and the time stage information in the whole task space to help learn the time series of the trajectory, and are used to guide the subsequent RL process. Notably, neural networks are not used to model the action policy and the Q value of RL during the RL process. Instead, they are sampled and updated in the whole task space and then transferred to the networks after the RL process through Behavior Cloning (BC) to get continuous and smooth global trajectory policy. The feasibility and the effectiveness of the method was validated in a custom Gym environment of a flower drawing task. And then, we executed the learned policy in the real-world robot drawing experiment.

2.
Angew Chem Int Ed Engl ; : e202319470, 2024 Apr 02.
Artigo em Inglês | MEDLINE | ID: mdl-38566301

RESUMO

Two-electron oxygen reduction reaction (2e- ORR) is a promising method for the synthesis of hydrogen peroxide (H2O2). However, high energy barriers for the generation of key *OOH intermediates hinder the process of 2e- ORR. Herein, we prepared a copper-supported indium selenide catalyst (Cu/In2Se3) to enhance the selectivity and yield of 2e- ORR by employing an electronic metal-support interactions (EMSIs) strategy. EMSIs-induced charge rearrangement between metallic Cu and In2Se3 is conducive to *OOH intermediate generation, promoting H2O2 production. Theoretical investigations reveal that the inclusion of Cu significantly lowers the energy barrier of the 2e- ORR intermediate and impedes the 4e- ORR pathway, thus favoring the formation of H2O2. The concentration of H2O2 produced by Cu/In2Se3 is ~2 times than In2Se3, and Cu/In2Se3 shows promising applications in antibiotic degradation. This research presents a valuable approach for the future utilization of EMSIs in 2e- ORR.

3.
J Virol ; : e0035024, 2024 Apr 09.
Artigo em Inglês | MEDLINE | ID: mdl-38591900

RESUMO

Feline calicivirus (FCV) is one of the few members of the Caliciviridae family that grows well in cell lines and, therefore, serves as a surrogate to study the biology of other viruses in the family. Conley et al. (14) demonstrated that upon the receptor engagement to the capsid, FCV VP2 forms a portal-like assembly, which might provide a channel for RNA release. However, the process of calicivirus RNA release is not yet fully understood. Our findings suggest that the separation of the FCV capsid from its genome RNA (gRNA) occurs rapidly in the early endosomes of infected cells. Using a liposome model decorated with the FCV cell receptor fJAM-A, we demonstrate that FCV releases its gRNA into the liposomes by penetrating membranes under low pH conditions. Furthermore, we found that VP2, which is rich in hydrophobic residues at its N-terminus, functions as the pore-forming protein. When we substituted the VP2 N-terminal hydrophobic residues, the gRNA release efficacy of the FCV mutants decreased. In conclusion, our results suggest that in the acidic environment of early endosomes, FCV VP2 functions as the pore-forming protein to mediate gRNA release into the cytoplasm of infected cells. This provides insight into the mechanism of calicivirus genome release.IMPORTANCEResearch on the biology and pathogenicity of certain caliciviruses, such as Norovirus and Sapovirus, is hindered by the lack of easy-to-use cell culture system. Feline calicivirus (FCV), which grows effectively in cell lines, is used as a substitute. At present, there is limited understanding of the genome release mechanism in caliciviruses. Our findings suggest that FCV uses VP2 to pierce the endosome membrane for genome release and provide new insights into the calicivirus gRNA release mechanism.

4.
J Gastrointest Surg ; 28(4): 375-380, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38583886

RESUMO

PURPOSE: This study aimed to investigate the correlation between sarcopenia and adverse events (AEs) of postoperative imatinib therapy through computed tomography (CT) quantitative body composition for intermediate- and high-risk gastrointestinal stromal tumors (GISTs). METHODS: The study retrospectively analyzed the clinical data of 208 patients with intermediate- and high-risk GIST treated surgically and treated with imatinib afterward at the First Affiliated Hospital of Wenzhou Medical University between October 2011 and October 2021. Images of preoperative CT scans within 1 month were used to determine the body composition of the patients. On the basis of the L3 skeletal muscle index, patients were classified into sarcopenia and nonsarcopenia groups. In 2 groups, AEs related to imatinib were analyzed. RESULTS: The proportion of AEs related to imatinib in the sarcopenia group was higher, and this disparity had a significant statistical significance (P = .013). Sarcopenia was significantly associated with hemoglobin reduction compared with nonsarcopenia (P = .015). There was a significant difference between the sarcopenia group and the nonsarcopenia group in the ratio of severe AEs (grades 3-4). Hemoglobin content (odds ratio [OR], 0.981; 95% CI, 0.963-1.000; P = .045), sex (OR, 0.416; 95% CI, 0.192-0.904; P = .027), and sarcopenia (OR, 5.631; 95% CI, 2.262-14.014; P < .001) were the influential factors of imatinib severe AEs in patients with intermediate- and high-risk GIST within 1 year after imatinib treatment. CONCLUSION: Patients with preoperative sarcopenia have a higher incidence and severity of AEs during adjuvant imatinib therapy.


Assuntos
Antineoplásicos , Tumores do Estroma Gastrointestinal , Sarcopenia , Humanos , Mesilato de Imatinib/efeitos adversos , Tumores do Estroma Gastrointestinal/diagnóstico por imagem , Tumores do Estroma Gastrointestinal/tratamento farmacológico , Tumores do Estroma Gastrointestinal/cirurgia , Estudos Retrospectivos , Sarcopenia/induzido quimicamente , Sarcopenia/diagnóstico por imagem , Quimioterapia Adjuvante , Hemoglobinas , Tomografia , Antineoplásicos/efeitos adversos
5.
Adv Sci (Weinh) ; : e2401404, 2024 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-38622875

RESUMO

The development of membranes with rapid and selective ionic transport is imperative for diverse electrochemical energy conversion and storage systems, including fuel cells and flow batteries. However, the practical application of membranes is significantly hindered by their limited conductivity and stability under strong alkaline conditions. Herein, a unique composite membrane decorated with functional Cu2+ cross-linked chitosan (Cts-Cu-M) is reported and their high hydroxide ion conductivity and stability in alkaline flow batteries are demonstrated. The underlying hydroxide ions transport of the membrane through Cu2+ coordinated nano-confined channels with abundant hydrogen bonding network via Grotthuss (proton hopping) mechanism is proposed. Consequently, the Cts-Cu-M membrane achieves high hydroxide ion conductivity with an area resistance of 0.17 Ω cm2 and enables an alkaline zinc-based flow battery to operate at 320 mA cm-2, along with an energy efficiency of ≈80%. Furthermore, the membrane enables the battery for 200 cycles of long-cycle stability at a current density of 200 mA cm-2. This study offers an in-depth understanding of ion transport for the design and preparation of high-performance membranes for energy storage devices and beyond.

6.
Adv Healthc Mater ; : e2304485, 2024 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-38567748

RESUMO

Ferroptosis is identified as a potential target for anticancer therapy. However, most conventional ferroptosis inducers not only fail to trigger intracellular lipid peroxidation storm, but are also prone to cause ferroptosis-related toxicity through off-target destruction of intracellular antioxidant defense systems. Therefore, a potent and highly tumor-specific ferroptosis induction modality is desired. Herein, a self-cooperative nanomedicine for imaging-guided photothermal ferrotherapy, which is fabricated based on molecular nanoassembly (NA) of DiR (a photothermal probe) and ferrocene (Fc, a reactant of the Fenton reaction), is elaborately exploited. DiR-elicited hyperthermia induces both photothermal therapy (PTT) and a significant acceleration of the kinetics of the Fc-involved Fenton reaction, collaboratively causing a lipid peroxidation storm in tumor cells. In turn, plenty of lipid peroxides boost PTT through the downregulation of heat shock protein 90. As expected, such a self-cooperative NA demonstrates synergetic tumor eradication in the 4T1 breast tumor-bearing mice xenograft model. This study offers a novel nanotherapeutic paradigm for precise multimodal cancer therapy.

7.
Bioresour Technol ; 401: 130709, 2024 Apr 16.
Artigo em Inglês | MEDLINE | ID: mdl-38636877

RESUMO

Low-temperature could inhibit the performance of anaerobic granular sludge (AnGS). Quorum sensing (QS), as a communication mode between microorganisms, can effectively regulate AnGS. In this study, a kind of embedded particles (PVA/SA@Serratia) based on signal molecule secreting bacteria was prepared by microbial immobilization technology based on polyvinyl alcohol and sodium alginate to accelerate the recovery of AnGS system after low temperature. Low-temperature shock experiment verified the positive effect of PVA/SA@Serratia on restoring the COD removal rate and methanogenesis capacity of AnGS. Further analysis by metagenomics analysis showed that PVA/SA@Serratia stimulated higher QS activity and promoted the secretion of extracellular polymeric substance (EPS) in AnGS. The rapid construction of EPS protective layer effectively accelerated the establishment of a robust microbial community structure. PVA/SA@Serratia also enhanced multiple methanogenic pathways, including direct interspecies electron transfer. In conclusion, this study demonstrated that PVA/SA@Serratia could effectively strengthen AnGS after low-temperature shock.

8.
World J Gastroenterol ; 30(9): 1164-1176, 2024 Mar 07.
Artigo em Inglês | MEDLINE | ID: mdl-38577177

RESUMO

BACKGROUND: Diffusion-weighted imaging (DWI) has been developed to stage liver fibrosis. However, its diagnostic performance is inconsistent among studies. Therefore, it is worth studying the diagnostic value of various diffusion models for liver fibrosis in one cohort. AIM: To evaluate the clinical potential of six diffusion-weighted models in liver fibrosis staging and compare their diagnostic performances. METHODS: This prospective study enrolled 59 patients suspected of liver disease and scheduled for liver biopsy and 17 healthy participants. All participants underwent multi-b value DWI. The main DWI-derived parameters included Mono-apparent diffusion coefficient (ADC) from mono-exponential DWI, intravoxel incoherent motion model-derived true diffusion coefficient (IVIM-D), diffusion kurtosis imaging-derived apparent diffusivity (DKI-MD), stretched exponential model-derived distributed diffusion coefficient (SEM-DDC), fractional order calculus (FROC) model-derived diffusion coefficient (FROC-D) and FROC model-derived microstructural quantity (FROC-µ), and continuous-time random-walk (CTRW) model-derived anomalous diffusion coefficient (CTRW-D) and CTRW model-derived temporal diffusion heterogeneity index (CTRW-α). The correlations between DWI-derived parameters and fibrosis stages and the parameters' diagnostic efficacy in detecting significant fibrosis (SF) were assessed and compared. RESULTS: CTRW-D (r = -0.356), CTRW-α (r = -0.297), DKI-MD (r = -0.297), FROC-D (r = -0.350), FROC-µ (r = -0.321), IVIM-D (r = -0.251), Mono-ADC (r = -0.362), and SEM-DDC (r = -0.263) were significantly correlated with fibrosis stages. The areas under the ROC curves (AUCs) of the combined index of the six models for distinguishing SF (0.697-0.747) were higher than each of the parameters alone (0.524-0.719). The DWI models' ability to detect SF was similar. The combined index of CTRW model parameters had the highest AUC (0.747). CONCLUSION: The DWI models were similarly valuable in distinguishing SF in patients with liver disease. The combined index of CTRW parameters had the highest AUC.


Assuntos
Imagem de Difusão por Ressonância Magnética , Hepatopatias , Humanos , Estudos Prospectivos , Imagem de Difusão por Ressonância Magnética/métodos , Cirrose Hepática/diagnóstico por imagem , Cirrose Hepática/patologia , Imagem de Tensor de Difusão/métodos
9.
Materials (Basel) ; 17(7)2024 Apr 07.
Artigo em Inglês | MEDLINE | ID: mdl-38612208

RESUMO

The microstructures and mechanical properties of equiatomic CoCrFeMnNi high-entropy alloys (HEAs) treated with various processing parameters of laser surface heat treatment are studied in this paper. The typical inverse gradient-grained structure, which is composed of a hard central layer and a soft surface layer, can be obtained by laser surface heat treatment. A much narrower gradient layer leads to the highest yield strength by sacrificing ductility when the surface temperature of the laser-irradiated region remains at ~850 °C, whereas the fully recrystallized microstructure, which exists from the top surface layer to the ~1.05 mm depth layer, increases the ductility but decreases the yield strength as the maximum heating temperature rises to ~1050 °C. Significantly, the superior strength-ductility combination can be acquired by controlling the surface temperature of a laser-irradiated surface at ~1000 °C with a scanning speed of ~4 mm/s due to the effect of hetero-deformation-induced strengthening and hardening, as well as the enhanced interaction between dislocation and nanotwins by the hierarchical nanotwins. Therefore, retaining the partial recrystallized microstructure with a relatively high microhardness in the central layer, promoting the generation of hierarchical nanotwins, and increasing the volume proportion of gradient layer can effectively facilitate the inverse gradient-grained CoCrFeMnNi HEAs to exhibit a desirable strength-ductility synergy.

10.
Org Lett ; 26(15): 3279-3283, 2024 Apr 19.
Artigo em Inglês | MEDLINE | ID: mdl-38578864

RESUMO

Chiral spiro-polycyclic oxindoles are valuable heterocyclic ring systems that are widely distributed in natural alkaloids and biologically active compounds. Herein, we reported an asymmetric tandem Michael addition/interrupted Nef reaction of nitromethane with oxindole-derived alkenes catalyzed by a chiral 2-aminobenzimidazole bifunctional organocatalyst. A series of novel enantiomerically enriched spiro-polycyclic oxindole derivatives bearing an oxime group were synthesized in moderate to excellent isolated yields (up to 99%) with an excellent level of enantioselectivities (up to 99% ee). Furthermore, the antiproliferation activity of the resulting oxindoles derivatives were evaluated, and compound 2d demonstrated promising anticancer properties against HCT116 (IC50 = 14.08 µM) and HT29 (IC50 = 15.46 µM) cell lines.

11.
Front Neurol ; 15: 1286079, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-38633532

RESUMO

Introduction: Tirofiban is a non-peptide selective glycoprotein IIb/IIIa receptor inhibitor with a short half-life. The research assesses the efficacy and safety of continuous intravenous tirofiban in patients with acute ischemic stroke (AIS) undergoing endovascular therapy (ET). Methods: A systematic search of Pubmed, Embase, Web of Science, and Cochrane Library databases is conducted from inception until January 26, 2024. Eligible studies are included based on predefined selection criteria. Efficacy outcomes (favorable functional outcome and excellent functional outcome) and safety outcomes (symptomatic intracranial hemorrhage [sICH], any intracranial hemorrhage [ICH], and 90-day mortality) are calculated using odds ratios (OR) and 95% confidence intervals (CI). Results: A total of 4,329 patients from 15 studies are included in the analysis. The results indicate a significant trend toward favorable functional outcomes in the tirofiban group (OR, 1.24; 95% CI, 1.09-1.42; p = 0.001). In terms of safety outcomes, tirofiban does not increase the risk of sICH (OR, 0.90; 95% CI, 0.71-1.13; p = 0.35) or any ICH (OR, 0.97; 95% CI, 0.70-1.34; p = 0.85), but it significantly decreases 90-day mortality (OR, 0.75; 95% CI, 0.64-0.88; p = 0.0006). A subgroup analysis suggests that continuous intravenous tirofiban demonstrates better efficacy (OR, 1.24; 95% CI, 1.09-1.42; p = 0.001) for patients with AIS undergoing rescue ET with even better results when used in combination with intra-arterial and intravenous administration (OR, 1.25; 95% CI, 1.07-1.451; p = 0.005). Conclusion: Continuous intravenous tirofiban is effective and safe for patients with AIS undergoing rescue ET, particularly when combined with intra-arterial tirofiban. Systematic review registration: PROSPERO, identifier CRD42023385695.

12.
Opt Lett ; 49(8): 2113-2116, 2024 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-38621089

RESUMO

In this Letter, we report continuous-wave (CW) lasers with wavelengths beyond 3 µm in homemade Ho3+/Pr3+ co-doped AlF3-based glass fibers. The laser cavity was established through the integration of a dichroic mirror (DM, HR@3-3.1 µm) positioned at the pump end and a partial reflectivity (PR) fiber Bragg grating (FBG) situated at the laser emission end. The FBGs in AlF3-based glass fibers were fabricated by a fs laser direct-writing method, and the resonant wavelengths were 3.009, 3.036, and 3.064 µm, respectively. Under the pump of 1.15 µm laser, a maximum unsaturated output power of 1.014 W was obtained at 3.009 µm with an overall laser efficiency of 11.8% and FWHM bandwidth of 0.88 nm. Furthermore, in order to enhance the optical-thermal stability, the FBG was heat-treated at 200°C for 30 min, and a higher output power of 1081 mW (348 mW without heat treatment) at 3.036 µm was achieved. To the best of our knowledge, this is the first demonstration of 3-3.1 µm lasers by using FBGs in Ho3+/Pr3+ co-doped AlF3-based fibers.

13.
J Nat Prod ; 2024 Apr 11.
Artigo em Inglês | MEDLINE | ID: mdl-38603577

RESUMO

Epithelial ovarian cancer is among the deadliest gynecological tumors worldwide. Clinical treatment usually consists of surgery and adjuvant chemo- and radiotherapies. Due to the high rate of recurrence and rapid development of drug resistance, the current focus of research is on finding effective natural products with minimal toxic side effects for treating epithelial ovarian tumors. Cannabidiol is among the most abundant cannabinoids and has a non-psychoactive effect compared to tetrahydrocannabinol, which is a key advantage for clinical application. Studies have shown that cannabidiol has antiproliferative, pro-apoptotic, cytotoxic, antiangiogenic, anti-inflammatory, and immunomodulatory properties. However, its therapeutic value for epithelial ovarian tumors remains unclear. This study aims to investigate the effects of cannabidiol on epithelial ovarian tumors and to elucidate the underlying mechanisms. The results showed that cannabidiol has a significant inhibitory effect on epithelial ovarian tumors. In vivo experiments demonstrated that cannabidiol could inhibit tumor growth by modulating the intestinal microbiome and increasing the abundance of beneficial bacteria. Western blot assays showed that cannabidiol bound to EGFR/AKT/MMPs proteins and suppressed EGFR/AKT/MMPs expression in a dose-dependent manner. Network pharmacology and molecular docking results suggested that cannabidiol could affect the EGFR/AKT/MMPs signaling pathway.

15.
J Colloid Interface Sci ; 667: 607-616, 2024 Apr 21.
Artigo em Inglês | MEDLINE | ID: mdl-38657544

RESUMO

Prussian blue analogues (PBAs) are regarded as promising cathode materials for ammonium-ion batteries (AIBs) because of their low cost and superb theoretical capacity. However, its inherently poor conductivity and structural collapse can significantly limit the enhancement of rate property and cycling stability. In this work, Berlin Green (BG) electrode materials with similar wool-like clusters were constructed by direct precipitation method to accelerate the kinetic, which realizes outstanding cycling stability. Berlin Green with the appropriate amount of iron (BG-2) has a fast ion transport channel, enhanced structure stability, highly reversible insertion/extraction of NH4+, and fine electrochemical reaction activity. Benefiting from the unique architecture and component, the BG-2 electrode shows an excellent rate performance with a discharge/charge specific capacity of 60.1/59.3 mAh g-1 at 5 A g-1. Even at 5 A g-1, BG-2 exhibits remarkable cycling stability with an initial discharge capacity of 59.5 mAh g-1 and a capacity retention rate of approximately 76% after 30,000 cycles. The BG-2 reveals exceedingly good electrochemical reversibility during the process of NH4+ (de)insertion. BG materials indicate huge potential as a cathode material for the next generation of high-performance aqueous batteries.

16.
Langmuir ; 40(16): 8678-8684, 2024 Apr 23.
Artigo em Inglês | MEDLINE | ID: mdl-38606578

RESUMO

The practical use of lithium-sulfur batteries faces the "shuttle effect" and lithium dendrite growth. Employing SiO instead of Li metal can fundamentally solve the above problems. Nevertheless, selecting a convenient prelithiation method is essential for normal operation of the battery system. Hence, this work proposed a novel SiO-sulfur battery with preloaded Li3N in a cathode as a prelithiation reagent, which can thoroughly solve the dendrite problem and the side reaction with polysulfides of lithium anode. The S@KB-Li3N vs SiO full cell can obtain a high specific capacity of 790 mAh g-1 after the activation process and be maintained at 478 mAh g-1 after 100 cycles. Our design will provide a new prelithiation strategy for a high-specific-energy SiO-sulfur battery system.

17.
Aging (Albany NY) ; 16(7): 5866-5886, 2024 Apr 12.
Artigo em Inglês | MEDLINE | ID: mdl-38613793

RESUMO

NXPH4 promotes cancer proliferation and invasion. However, its specific role and mechanism in cancer remain unclear. Transcriptome and clinical data for pan-cancer were derived from the TCGA database. K-M survival curve and univariate Cox were used for prognostic analysis. CIBERSORT and TIMER algorithms were employed to calculate immune cell infiltration. Gene set enrichment analysis (GSEA) was employed for investigating the function of NXPH4. Western blot verified differential expression of NXPH4 in colon cancer. Functional assays (CCK-8, plate clonogenicity assay, wound healing assay, and Transwell assay) confirmed the impact of NXPH4 on proliferation, invasion, and migration of colon cancer cells. Dysregulation of NXPH4 in pan-cancer suggests its potential as a diagnostic and prognostic marker for certain cancers, including colon and liver cancer. High expression of NXPH4 in pan-cancer might be associated with the increase in copy number and hypomethylation. NXPH4 expression in pan-cancer is substantially linked to immune cell infiltration in the immune microenvironment. NXPH4 expression is associated with the susceptibility to immunotherapy and chemotherapy. Western blot further confirmed the higher expression of NXPH4 in colon cancer. Knockdown of NXPH4 significantly suppresses proliferation, invasion, and migration of colon cancer cell lines HT-29 and HCT116, as validated by functional assays.


Assuntos
Biomarcadores Tumorais , Movimento Celular , Proliferação de Células , Neoplasias do Colo , Humanos , Neoplasias do Colo/genética , Neoplasias do Colo/patologia , Neoplasias do Colo/metabolismo , Biomarcadores Tumorais/metabolismo , Biomarcadores Tumorais/genética , Proliferação de Células/genética , Movimento Celular/genética , Regulação Neoplásica da Expressão Gênica , Progressão da Doença , Células HT29 , Células HCT116 , Prognóstico , Invasividade Neoplásica , Microambiente Tumoral/genética , Microambiente Tumoral/imunologia , Linhagem Celular Tumoral , Proteínas de Ligação a RNA/genética , Proteínas de Ligação a RNA/metabolismo
18.
Angew Chem Int Ed Engl ; : e202403585, 2024 Apr 02.
Artigo em Inglês | MEDLINE | ID: mdl-38565432

RESUMO

In spite of the competitive performance at room temperature, the development of sodium-ion batteries (SIBs) is still hindered by sluggish electrochemical reaction kinetics and unstable electrode/electrolyte interphase under subzero environments. Herein, a low-concentration electrolyte, consisting of 0.5M NaPF6 dissolving in diethylene glycol dimethyl ether solvent, is proposed for SIBs working at low temperature. Such an electrolyte generates a thin, amorphous, and homogeneous cathode/electrolyte interphase at low temperature. The interphase is monolithic and rich in organic components, reducing the limitation of Na+ migration through inorganic crystals, thereby facilitating the interfacial Na+ dynamics at low temperature. Furthermore, it effectively blocks the unfavorable side reactions between active materials and electrolytes, improving the structural stability. Consequently, Na0.7Li0.03Mg0.03Ni0.27Mn0.6Ti0.07O2//Na and hard carbon//Na cells deliver a high capacity retention of 90.8 % after 900 cycles at 1C, a capacity over 310 mAh g-1 under -30 °C, respectively, showing long-term cycling stability and great rate capability at low temperature.

19.
Nanomicro Lett ; 16(1): 161, 2024 Mar 25.
Artigo em Inglês | MEDLINE | ID: mdl-38526682

RESUMO

With the merits of the high energy density of batteries and power density of supercapacitors, the aqueous Zn-ion hybrid supercapacitors emerge as a promising candidate for applications where both rapid energy delivery and moderate energy storage are required. However, the narrow electrochemical window of aqueous electrolytes induces severe side reactions on the Zn metal anode and shortens its lifespan. It also limits the operation voltage and energy density of the Zn-ion hybrid supercapacitors. Using 'water in salt' electrolytes can effectively broaden their electrochemical windows, but this is at the expense of high cost, low ionic conductivity, and narrow temperature compatibility, compromising the electrochemical performance of the Zn-ion hybrid supercapacitors. Thus, designing a new electrolyte to balance these factors towards high-performance Zn-ion hybrid supercapacitors is urgent and necessary. We developed a dilute water/acetonitrile electrolyte (0.5 m Zn(CF3SO3)2 + 1 m LiTFSI-H2O/AN) for Zn-ion hybrid supercapacitors, which simultaneously exhibited expanded electrochemical window, decent ionic conductivity, and broad temperature compatibility. In this electrolyte, the hydration shells and hydrogen bonds are significantly modulated by the acetonitrile and TFSI- anions. As a result, a Zn-ion hybrid supercapacitor with such an electrolyte demonstrates a high operating voltage up to 2.2 V and long lifespan beyond 120,000 cycles.

20.
J Am Chem Soc ; 146(11): 7779-7790, 2024 Mar 20.
Artigo em Inglês | MEDLINE | ID: mdl-38466142

RESUMO

The electrochemical nitrate reduction reaction (NO3RR) holds promise for converting nitrogenous pollutants to valuable ammonia products. However, conventional electrocatalysis faces challenges in effectively driving the complex eight-electron and nine-proton transfer process of the NO3RR while also competing with the hydrogen evolution reaction. In this study, we present the thermally enhanced electrocatalysis of nitrate-to-ammonia conversion over nickel-modified copper oxide single-atom alloy oxide nanowires. The catalyst demonstrates improved ammonia production performance with a Faradaic efficiency of approximately 80% and a yield rate of 9.7 mg h-1 cm-2 at +0.1 V versus a reversible hydrogen electrode at elevated cell temperatures. In addition, this thermally enhanced electrocatalysis system displays impressive stability, interference resistance, and favorable energy consumption and greenhouse gas emissions for the simulated industrial wastewater treatment. Complementary in situ analyses confirm that the significantly superior relay of active hydrogen species formed at Ni sites facilitates the thermal-field-coupled electrocatalysis of Cu surface-adsorbed *NOx hydrogenation. Theoretical calculations further support the thermodynamic and kinetic feasibility of the relay catalysis mechanism for the NO3RR over the Ni1Cu model catalyst. This study introduces a conceptual thermal-electrochemistry approach for the synergistic regulation of complex catalytic processes, highlighting the potential of multifield-coupled catalysis to advance sustainable-energy-powered chemical synthesis technologies.

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