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1.
Small ; : e2406075, 2024 Sep 23.
Artículo en Inglés | MEDLINE | ID: mdl-39314014

RESUMEN

Alkaline electrolysis plays a crucial role in sustainable energy solutions by utilizing electrolytic cells to produce hydrogen gas, providing a clean and efficient method for energy storage and conversion. Efficient, stable, and low-cost electrocatalysts for the oxygen evolution reaction (OER) are essential to facilitate alkaline water electrolysis on a commercial scale. Nickel-iron-based (NiFe-based) transition metal electrocatalysts are considered the most promising non-precious metal catalysts for alkaline OER due to their low cost, abundance, and tunable catalytic properties. Nevertheless, the majority of existing NiFe-based catalysts suffer from limited activity and poor stability, posing a significant challenge in meeting industrial applications. This also highlights a common situation where the emphasis on material activity receives significant attention, while the equally critical stability aspect is often underemphasized. Initiating with a comprehensive exploration of the stability of NiFe-based OER materials, this article first summarizes the debate surrounding the determination of active sites in NiFe-based OER electrocatalysts. Subsequently, the degradation mechanisms of recently reported NiFe-based electrocatalysts are outlined, encompassing assessments of both chemical and mechanical endurance, along with essential approaches for enhancing their stability. Finally, suggestions are put forth regarding the essential considerations for the design of NiFe-based OER electrocatalysts, with a focus on heightened stability.

2.
Behav Brain Res ; : 115268, 2024 Sep 23.
Artículo en Inglés | MEDLINE | ID: mdl-39322063

RESUMEN

OBJECTIVE: Remimazolam, a novel benzodiazepine, is widely used as an anesthetic in endoscopic procedures; however, its effects on cognitive function remain unclear, limiting its broader application in general anaesthesia. Neuroinflammation is a well-established key factor in the etiology and progression of cognitive dysfunction, including conditions such as Alzheimer's disease, Parkinson's disease, postoperative delirium, and postoperative cognitive dysfunction. Preclinical studies have demonstrated that remimazolam exerts anti-inflammatory and neuroprotective effects, and clinical reports indicate a reduced incidence of postoperative delirium in patients treated with remimazolam. Nevertheless, whether remimazolam improves cognitive function through its anti-inflammatory properties remains uncertain. This study aimed to investigate the neuroprotective effects of remimazolam and its underlying mechanism in a lipopolysaccharide (LPS)-induced model of neuroinflammation, neuronal injury, and cognitive dysfunction METHODS: C57BL/6J male mice were administered LPS intraperitoneally to establish a model of neuroinflammation-induced cognitive impairment. A subset of mice received remimazolam via intraperitoneal injection 30minutes prior to LPS administration. Cognitive performance was evaluated using behavioural tests, including the Morris Water Maze (MWM), Novel Object Recognition (NOR) test, and Open Field Test (OFT). Hippocampal tissues were analyzed by haematoxylin-eosin (HE) staining to assess structural changes. Inflammatory markers, including Interleukin (IL)-6, IL-1ß, and tumor necrosis factor-α, were quantified using enzyme-linked immunosorbent assay (ELISA) and real-time quantitative PCR. Immunofluorescence was used to detect translocator protein (TSPO) and markers of microglia activation (IBA-1, CD16/32, and CD206). RESULTS: (1) Remimazolam reversed LPS-induced cognitive deficits, as evidenced by shorter spatial exploration latency and increased platform crossings in the MWM, and an elevated recognition index in the NOR test. (2) Remimazolam improved hippocampal morphology, reducing LPS-induced neuronal damage. (3) Remimazolam significantly decreased levels of hippocampal inflammatory cytokines, inhibited microglial activation, promoted M2-type microglia polarization, and increased TSPO expression. CONCLUSION: Remimazolam demonstrated neuroprotective and anti-neuroinflammatory effects in a mouse model of LPS-induced cognitive impairment. These effects are likely mediated through the regulation of TSPO, which inhibits microglial activation and promotes the polarization of microglia from the pro-inflammatory M1 phenotype to the anti-inflammatory M2 phenotype.

3.
Angew Chem Int Ed Engl ; : e202411591, 2024 Aug 13.
Artículo en Inglés | MEDLINE | ID: mdl-39136330

RESUMEN

Deeply electrolytic reduction of carbon dioxide (CO2) to high-value ethylene (C2H4) is very attractive. However, the sluggish kinetics of C-C coupling seriously results in the low selectivity of CO2 electroreduction to C2H4. Herein, we report a copper-based polyhedron (Cu2) that features uniformly distributed and atomically precise bi-Cu units, which can stabilize *OCCO dipole to facilitate the C-C coupling for high selective C2H4 production. The C2H4 faradaic efficiency (FE) reaches 51% with a current density of 469.4 mA cm-2, much superior to the Cu single site catalyst (Cu SAC) (~0%). Moreover, the Cu2 catalyst has a higher turnover frequency (TOF, ~520 h-1) compared to Cu nanoparticles (~9.42 h-1) and Cu SAC (~0.87 h-1). In situ characterizations and theoretical calculations revealed that the unique Cu2 structural configuration could optimize the dipole moments and stabilize the *OCCO adsorbate to promote the generation of C2H4.

4.
Am J Otolaryngol ; 45(6): 104475, 2024 Aug 02.
Artículo en Inglés | MEDLINE | ID: mdl-39121639

RESUMEN

OBJECTIVE: The objective of this study was to compare the outcomes of endoscopic cartilage underlay myringoplasty(CNM) with or without balloon Eustachian tuboplasty (BET) for the treatment of chronic perforation with Eustachian tube dysfunction (ETD). MATERIALS AND METHODS: A total of 50 ears diagnosed with chronic perforation and ETD were randomly divided into receiving alone CNM and CNM + BET. During the 12 months follow-up, the Eustachian tube score (ETS), Eustachian Tube Dysfunction Questionnaire-7 (ETDQ-7), ET inflammation scale, hearing results and graft success rate of the patients were recorded and analyzed. RESULTS: The improvement in the ETDQ-7 score was 6.23 ± 2.51 in the CNM + BET group, which was significantly higher than that in the CNM group (4.22 ± 3.85, P < 0.01) at postoperative 3 months, however, no significant between-group difference was found at post-12 months.The graft success rate was 88.0 % in the CNM group and 92.0 % in the CNM + BET group at postoperative 3 months (P > 0.05). Also, no significant difference was found among two groups (84.0 % vs 88.0 %, P > 0.05).The ABG improvement was 13.16 ± 3.19 dB in the CNM + BET group and 9.74 ± 2.56 dB in the CNM group, with a statistically significant between-group difference (P < 0.01)at postoperative 3 months. However, no significant between-group difference was found at postoperative 12 months. During followup process, neither complications nor patulous symptoms were noted. No patients developted atelectasis or otitis media with effusion. However, myringitis was seen in 8 % patients in the CNM group and 12 % patients in the CNM + BET group. CONCLUSIONS: Although BET combined with endoscopic cartilage myringoplasty had better short-term improvement of hearing and ETDQ-7 scores compared with endoscopic cartilage myringoplasty for the treatment of chronic large perforation with ETD, the long-term outcomes was not satisfactory. Also, BET did not improve the 3-and 12 months graft success rate.

5.
J Am Chem Soc ; 146(29): 20530-20538, 2024 Jul 24.
Artículo en Inglés | MEDLINE | ID: mdl-38991189

RESUMEN

The electrochemical reduction reaction of carbon dioxide (CO2RR) into valuable products offers notable economic benefits and contributes to environmental sustainability. However, precisely controlling the reaction pathways and selectively converting key intermediates pose considerable challenges. In this study, our theoretical calculations reveal that the active sites with different states of copper atoms (1-3-5-7-9) play a pivotal role in the adsorption behavior of the *CHO critical intermediate. This behavior dictates the subsequent hydrogenation and coupling steps, ultimately influencing the formation of the desired products. Consequently, we designed two model electrocatalysts comprising Cu single atoms and particles supported on CeO2. This design enables controlled *CHO intermediate transformation through either hydrogenation with *H or coupling with *CO, leading to a highly selective CO2RR. Notably, our selective control strategy tunes the Faradaic efficiency from 61.1% for ethylene (C2H4) to 61.2% for methane (CH4). Additionally, the catalyst demonstrated a high current density and remarkable stability, exceeding 500 h of operation. This work not only provides efficient catalysts for selective CO2RR but also offers valuable insights into tailoring surface chemistry and designing catalysts for precise control over catalytic processes to achieve targeted product generation in CO2RR technology.

6.
Zhonghua Yi Xue Yi Chuan Xue Za Zhi ; 41(7): 803-806, 2024 Jul 10.
Artículo en Chino | MEDLINE | ID: mdl-38946361

RESUMEN

OBJECTIVE: To explore the application of an automatic slide-dropping instrument in bone marrow chromosomal karyotyping. METHODS: The effects of manual and automatic dropping methods under different environmental humidity were retrospectively analyzed, and the repeatability of the automatic dropping method was analyzed. RESULTS: No statistical difference was found between the results of automatic and manual dropping methods under the optimum ambient humidity and high humidity (P > 0.05). At low humidity, there was a statistical difference between the two methods (P < 0.05). With regard to the repeatability, the coefficient of variations of the automatic dropping method for the number of split phases, the rate of good dispersion and the rate of overlap were all lower than those of the manual dropping method. A statistical difference was also found in the number of split phases (P < 0.05) but not in the discrete excellent rate and overlapping rate between the two methods (P > 0.05). CONCLUSION: Better effect can be obtained by the automatic dropping instrument. It is suggested to gradually replace manual work with machine.


Asunto(s)
Cariotipificación , Humanos , Cariotipificación/métodos , Adulto , Femenino , Masculino , Médula Ósea , Persona de Mediana Edad , Estudios Retrospectivos , Adulto Joven , Adolescente , Humedad , Automatización , Niño , Anciano , Preescolar
7.
Acta Pharm Sin B ; 14(5): 2153-2176, 2024 May.
Artículo en Inglés | MEDLINE | ID: mdl-38799623

RESUMEN

Aberrant changes in the gut microbiota are implicated in many diseases, including inflammatory bowel disease (IBD). Gut microbes produce diverse metabolites that can shape the immune system and impact the intestinal barrier integrity, indicating that microbe-mediated modulation may be a promising strategy for preventing and treating IBD. Although fecal microbiota transplantation and probiotic supplementation are well-established IBD therapies, novel chemical agents that are safe and exert strong effects on the gut microbiota are urgently needed. Herein, we report the total synthesis of heudelotinone and the discovery of 5S-heudelotinone (an enantiomer) as a potent agent against experimental colitis that acts by modulating the gut microbiota. 5S-Heudelotinone alters the diversity and composition of the gut microbiota and increases the concentration of short-chain fatty acids (SCFAs); thus, it regulates the intestinal immune system by reducing proinflammatory immune cell numbers, and maintains intestinal mucosal integrity by modulating tight junctions (TJs). Moreover, 5S-heudelotinone (2) ameliorates colitis-associated colorectal cancer (CAC) in an azoxymethane (AOM)/dextran sulfate sodium (DSS)-induced in situ carcinoma model. Together, these findings reveal the potential of a novel natural product, namely, 5S-heudelotinone, to control intestinal inflammation and highlight that this product is a safe and effective candidate for the treatment of IBD and CAC.

8.
Angew Chem Int Ed Engl ; 63(30): e202316755, 2024 Jul 22.
Artículo en Inglés | MEDLINE | ID: mdl-38739420

RESUMEN

The hydrazine oxidation-assisted H2 evolution method promises low-input and input-free hydrogen production. However, developing high-performance catalysts for hydrazine oxidation (HzOR) and hydrogen evolution (HER) is challenging. Here, we introduce a bifunctional electrocatalyst α-MoC/N-C/RuNSA, merging ruthenium (Ru) nanoclusters (NCs) and single atoms (SA) into cubic α-MoC nanoparticles-decorated N-doped carbon (α-MoC/N-C) nanowires, through electrodeposition. The composite showcases exceptional activity for both HzOR and HER, requiring -80 mV and -9 mV respectively to reach 10 mA cm-2. Theoretical and experimental insights confirm the importance of two Ru species for bifunctionality: NCs enhance the conductivity, and its coexistence with SA balances the H ad/desorption for HER and facilitates the initial dehydrogenation during the HzOR. In the overall hydrazine splitting (OHzS) system, α-MoC/N-C/RuNSA excels as both anode and cathode materials, achieving 10 mA cm-2 at just 64 mV. The zinc hydrazine (Zn-Hz) battery assembled with α-MoC/N-C/RuNSA cathode and Zn foil anode can exhibit 97.3 % energy efficiency, as well as temporary separation of hydrogen gas during the discharge process. Therefore, integrating Zn-Hz with OHzS system enables self-powered H2 evolution, even in hydrazine sewage. Overall, the amalgamation of NCs with SA achieves diverse catalytic activities for yielding multifold hydrogen gas through advanced cell-integrated-electrolyzer system.

9.
BMC Med Imaging ; 24(1): 72, 2024 Mar 26.
Artículo en Inglés | MEDLINE | ID: mdl-38532313

RESUMEN

BACKGROUND: Quantitative determination of the correlation between cognitive ability and functional biomarkers in the older brain is essential. To identify biomarkers associated with cognitive performance in the older, this study combined an index model specific for resting-state functional connectivity (FC) with a supervised machine learning method. METHODS: Performance scores on conventional cognitive test scores and resting-state functional MRI data were obtained for 98 healthy older individuals and 90 healthy youth from two public databases. Based on the test scores, the older cohort was categorized into two groups: excellent and poor. A resting-state FC scores model (rs-FCSM) was constructed for each older individual to determine the relative differences in FC among brain regions compared with that in the youth cohort. Brain areas sensitive to test scores could then be identified using this model. To suggest the effectiveness of constructed model, the scores of these brain areas were used as feature matrix inputs for training an extreme learning machine. classification accuracy (CA) was then tested in separate groups and validated by N-fold cross-validation. RESULTS: This learning study could effectively classify the cognitive status of healthy older individuals according to the model scores of frontal lobe, temporal lobe, and parietal lobe with a mean accuracy of 86.67%, which is higher than that achieved using conventional correlation analysis. CONCLUSION: This classification study of the rs-FCSM may facilitate early detection of age-related cognitive decline as well as help reveal the underlying pathological mechanisms.


Asunto(s)
Encéfalo , Cognición , Adolescente , Humanos , Mapeo Encefálico/métodos , Imagen por Resonancia Magnética/métodos , Biomarcadores
10.
Nat Commun ; 15(1): 1719, 2024 Feb 26.
Artículo en Inglés | MEDLINE | ID: mdl-38409205

RESUMEN

Tuning interfacial electric fields provides a powerful means to control electrocatalyst activity. Importantly, electric fields can modify adsorbate binding energies based on their polarizability and dipole moment, and hence operate independently of scaling relations that fundamentally limit performance. However, implementation of such a strategy remains challenging because typical methods modify the electric field non-uniformly and affects only a minority of active sites. Here we discover that uniformly tunable electric field modulation can be achieved using a model system of single-atom catalysts (SACs). These consist of M-N4 active sites hosted on a series of spherical carbon supports with varying degrees of nanocurvature. Using in-situ Raman spectroscopy with a Stark shift reporter, we demonstrate that a larger nanocurvature induces a stronger electric field. We show that this strategy is effective over a broad range of SAC systems and electrocatalytic reactions. For instance, Ni SACs with optimized nanocurvature achieved a high CO partial current density of ~400 mA cm-2 at >99% Faradaic efficiency for CO2 reduction in acidic media.

11.
Adv Mater ; 36(2): e2304713, 2024 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-37439396

RESUMEN

Single-atom catalysts (SACs) have attracted considerable attention in heterogeneous catalysis because of their well-defined active sites, maximum atomic utilization efficiency, and unique unsaturated coordinated structures. However, their effectiveness is limited to reactions requiring active sites containing multiple metal atoms. Furthermore, the loading amounts of single-atom sites must be restricted to prevent aggregation, which can adversely affect the catalytic performance despite the high activity of the individual atoms. The introduction of nanoscale metal particles (NMPs) into SACs (NMP-SACs) has proven to be an efficient approach for improving their catalytic performance. A comprehensive review is urgently needed to systematically introduce the synthesis, characterization, and application of NMP-SACs and the mechanisms behind their superior catalytic performance. This review first presents and classifies the different mechanisms through which NMPs enhance the performance of SACs. It then summarizes the currently reported synthetic strategies and state-of-the-art characterization techniques of NMP-SACs. Moreover, their application in electro/thermo/photocatalysis, and the reasons for their superior performance are discussed. Finally, the challenges and perspectives of NMP-SACs for the future design of advanced catalysts are addressed.

12.
Small ; : e2308530, 2023 Dec 07.
Artículo en Inglés | MEDLINE | ID: mdl-38059871

RESUMEN

Metal single-atom catalysts (M-SACs) attract extraordinary attention for promoting oxygen reduction reaction (ORR) with 100% atomic utilization. However, low metal loading (usually less than 2 wt%) limits their overall catalytic performance. Herein, a hierarchical-structure-stabilization strategy for fabricating high-loading (18.3%) M-SACs with efficient ORR activity is reported. Hierarchical pores structure generated with high N content by SiO2 can provide more coordination sites and facilitate the adsorption of Fe3+ through mesoporous and confinement effect of it stabilizes Fe atoms in micropores on it during pyrolysis. High N content on hierarchical pores structure could provide more anchor sites of Fe atoms during the subsequent secondary pyrolysis and synthesize the dense and accessible Fe-N4 sites after subsequent pyrolysis. In addition, Se power is introduced to modulate the electronic structure of Fe-N4 sites and further decrease the energy barrier of the ORR rate-determining step. As a result, the Fe single atom catalyst delivers unprecedentedly high ORR activity with a half-wave potential of 0.895 V in 0.1 M KOH aqueous solution and 0.791 V in 0.1 M HClO4 aqueous solution. Therefore, a hierarchical-pore-stabilization strategy for boosting the density and accessibility of Fe-N4 species paves a new avenue toward high-loading M-SACs for various applications such as thermocatalysis and photocatalysis.

13.
RSC Adv ; 13(45): 32023-32027, 2023 Oct 26.
Artículo en Inglés | MEDLINE | ID: mdl-37920199

RESUMEN

The energy crisis is a the worldwide problem which needs humans to solve immediately. To solve this problem, it is necessary to develop energy storage batteries. It is worth mentioning the aqueous rechargeable zinc ion batteries (ARZBs) which have some advantages, such as low cost, good safety and no need for an organic electrolyte as in the traditional lithium-ion batteries. However, it is still a challenge to find suitable and reliable electrode materials. In this work, as-prepared H2V3O8 nanorods and MXene composites are used as cathode materials in ARZBs which were designed well using a hydrothermal method after optimizing the reaction time. The results showed that H2V3O8/MXene ARZBs could provide a good transport path for zinc ions, which were based on special 1D H2V3O8 nanorods and 2D multi-layered MXene materials, which exhibited an outstanding initial specific discharge capacity of 373 mA h g-1 at 200 mA g-1, good rate capability and a long lifecycle with only 15.8% capacity decay at 500 mA g-1 after 5000 cycles. The H2V3O8/MXene composites with a good electrochemical performance bring insight into their promising applications for energy storage batteries. They provided enhanced rate performance and excellent cycling stability, which was ascribed to the multi-step and multi-mode zinc ion insertion/extraction process. This was confirmed by the use of the 1D/2D integrated structure of the H2V3O8/MXene composites, which was conductive to zinc ion diffusion.

14.
Angew Chem Int Ed Engl ; 62(50): e202315621, 2023 Dec 11.
Artículo en Inglés | MEDLINE | ID: mdl-37902435

RESUMEN

Electrochemical CO2 reduction reaction (CO2 RR) over Cu catalysts exhibits enormous potential for efficiently converting CO2 to ethylene (C2 H4 ). However, achieving high C2 H4 selectivity remains a considerable challenge due to the propensity of Cu catalysts to undergo structural reconstruction during CO2 RR. Herein, we report an in situ molecule modification strategy that involves tannic acid (TA) molecules adaptive regulating the reconstruction of a Cu-based material to a pathway that facilitates CO2 reduction to C2 H4 products. An excellent Faraday efficiency (FE) of 63.6 % on C2 H4 with a current density of 497.2 mA cm-2 in flow cell was achieved, about 6.5 times higher than the pristine Cu catalyst which mainly produce CH4 . The in situ X-ray absorption spectroscopy and Raman studies reveal that the hydroxyl group in TA stabilizes Cuδ+ during the CO2 RR. Furthermore, theoretical calculations demonstrate that the Cuδ+ /Cu0 interfaces lower the activation energy barrier for *CO dimerization, and hydroxyl species stabilize the *COH intermediate via hydrogen bonding, thereby promoting C2 H4 production. Such molecule engineering modulated electronic structure provides a promising strategy to achieve highly selective CO2 reduction to value-added chemicals.

15.
Sci Adv ; 9(42): eadi8025, 2023 Oct 20.
Artículo en Inglés | MEDLINE | ID: mdl-37851800

RESUMEN

The anode corrosion induced by the harsh acidic and oxidative environment greatly restricts the lifespan of catalysts. Here, we propose an antioxidation strategy to mitigate Ir dissolution by triggering strong electronic interaction via elaborately constructing a heterostructured Ir-Sn pair-site catalyst. The formation of Ir-Sn dual-site at the heterointerface and the resulting strong electronic interactions considerably reduce d-band holes of Ir species during both the synthesis and the oxygen evolution reaction processes and suppress their overoxidation, enabling the catalyst with substantially boosted corrosion resistance. Consequently, the optimized catalyst exhibits a high mass activity of 4.4 A mgIr-1 at an overpotential of 320 mV and outstanding long-term stability. A proton-exchange-membrane water electrolyzer using this catalyst delivers a current density of 2 A cm-2 at 1.711 V and low degradation in an accelerated aging test. Theoretical calculations unravel that the oxygen radicals induced by the π* interaction between Ir 5d-O 2p might be responsible for the boosted activity and durability.

16.
RSC Adv ; 13(33): 22945-22957, 2023 Jul 26.
Artículo en Inglés | MEDLINE | ID: mdl-37529363

RESUMEN

Photocatalytic reactions convert solar energy into chemical energy through a clean and green reaction process. Photocatalytic technology based on semiconductor materials provides us with a new idea in energy utilization and environmental governance. It was found that vanadium pentoxide (V2O5) has a narrow band gap, wide response range in the visible region, high oxygen density in the V2O5 lattice, high oxidation state of V5+, small energy requirement, and superior catalytic activity in partial oxidation. Therefore, the utilization rate of sunlight and photocatalytic oxidation can be greatly improved using V2O5 materials. However, the narrow band gap of V2O5 also makes it easier for the photogenerated electrons and holes to recombine in the excited state, and the stored energy is instantly consumed by carrier recombination. Therefore, how to promote the carrier separation of V2O5 and improve the photocatalytic efficiency are the key problems to be solved. Herein, several methods to improve the photocatalytic performance of V2O5 are reviewed, including metallic ion doping, non-metallic ion doping, semiconductor recombination, and noble metal deposition. Finally, it is suggested that future research directions should focus on a variety of modification methods simultaneously to promote photocatalytic efficiency and lower the cost, which will enable V2O5 to have a broad development prospect in the field of photocatalysis.

17.
Adv Mater ; 35(46): e2305077, 2023 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-37497609

RESUMEN

Recently, single-atom nanozymes have made significant progress in the fields of sterilization and treatment, but their catalytic performance as substitutes for natural enzymes and drugs is far from satisfactory. Here, a method is reported to improve enzyme activity by adjusting the spatial position of a single-atom site on the nanoplatforms. Two types of Cu single-atom site nanozymes are synthesized in the interlayer (CuL /PHI) and in-plane (CuP /PHI) of poly (heptazine imide) (PHI) through different synthesis pathways. Experimental and theoretical analysis indicates that the interlayer position of PHI can effectively adjust the coordination number, coordination bond length, and electronic structure of Cu single atoms compared to the in-plane position, thereby promoting photoinduced electron migration and O2 activation, enabling effective generate reactive oxygen species (ROS). Under visible light irradiation, the photocatalytic bactericidal activity of CuL /PHI against aureus is ≈100%, achieving the same antibacterial effect as antibiotics, after 10 min of low-dose light exposure and 2 h of incubation.


Asunto(s)
Antibacterianos , Electrónica , Antibacterianos/farmacología , Catálisis , Electrones , Imidas
18.
Nano Lett ; 23(6): 2312-2320, 2023 Mar 22.
Artículo en Inglés | MEDLINE | ID: mdl-36861218

RESUMEN

Positively charged Cu sites have been confirmed to significantly promote the production of multicarbon (C2) products from an electrochemical CO2 reduction reaction (CO2RR). However, the positively charged Cu has difficulty in existing under a strong negative bias. In this work, we design a Pdδ--Cu3N catalyst containing charge-separated Pdδ--Cuδ+ atom pair that can stabilize the Cuδ+ sites. In situ characterizations and density functional theory reveal that the first reported negatively charged Pdδ- sites exhibited a superior CO binding capacity together with the adjacent Cuδ+ sites, synergistically promoting the CO dimerization process to produce C2 products. As a result, we achieve a 14-fold increase in the C2 product Faradaic efficiency (FE) on Pdδ--Cu3N, from 5.6% to 78.2%. This work provides a new strategy for synthesizing negative valence atom-pair catalysts and an atomic-level modulation approach of unstable Cuδ+ sites in the CO2RR.

19.
Exp Gerontol ; 174: 112132, 2023 04.
Artículo en Inglés | MEDLINE | ID: mdl-36849001

RESUMEN

Inflammation is believed to play a role in the progression of numerous human diseases. Research has shown that inflammation and telomeres are involved in a feedback regulatory loop: inflammation increases the rate of telomere attrition, leading to telomere dysfunction, while telomere components also participate in regulating the inflammatory response. However, the specific mechanism behind this feedback loop between inflammatory signaling and telomere/telomerase complex dysfunction has yet to be fully understood. This review presents the latest findings on this topic, with a particular focus on the detailed regulation and molecular mechanisms involved in the progression of aging, various chronic inflammatory diseases, cancers, and different stressors. Several feedback loops between inflammatory signaling and telomere/telomerase complex dysfunction, including NF-κB-TERT feedback, NF-κB-RAP1 feedback, NF-κB-TERC feedback, STAT3-TERT feedback, and p38 MAPK-shelterin complex-related gene feedback, are summarized. Understanding the latest discoveries of this feedback regulatory loop can help identify novel potential drug targets for the suppression of various inflammation-associated diseases.


Asunto(s)
Telomerasa , Humanos , Telomerasa/metabolismo , FN-kappa B , Retroalimentación , Telómero , Inflamación
20.
Angew Chem Int Ed Engl ; 62(3): e202215136, 2023 Jan 16.
Artículo en Inglés | MEDLINE | ID: mdl-36399049

RESUMEN

Precise design and tuning of the micro-atomic structure of single atom catalysts (SACs) can help efficiently adapt complex catalytic systems. Herein, we inventively found that when the active center of the main group element gallium (Ga) is downsized to the atomic level, whose characteristic has significant differences from conventional bulk and rigid Ga catalysts. The Ga SACs with a P, S atomic coordination environment display specific flow properties, showing CO products with FE of ≈92 % at -0.3 V vs. RHE in electrochemical CO2 reduction (CO2 RR). Theoretical simulations demonstrate that the adaptive dynamic transition of Ga optimizes the adsorption energy of the *COOH intermediate and renews the active sites in time, leading to excellent CO2 RR selectivity and stability. This liquid single atom catalysts system with dynamic interfaces lays the foundation for future exploration of synthesis and catalysis.

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