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1.
BMC Genomics ; 25(1): 327, 2024 Apr 02.
Artigo em Inglês | MEDLINE | ID: mdl-38565997

RESUMO

Food security is important for the ever-growing global population. Soybean, Glycine max (L.) Merr., is cultivated worldwide providing a key source of food, protein and oil. Hence, it is imperative to maintain or to increase its yield under different conditions including challenges caused by abiotic and biotic stresses. In recent years, the soybean pod-sucking stinkbug Riptortus pedestris has emerged as an important agricultural insect pest in East, South and Southeast Asia. Here, we present a genomics resource for R. pedestris including its genome assembly, messenger RNA (mRNA) and microRNA (miRNA) transcriptomes at different developmental stages and from different organs. As insect hormone biosynthesis genes (genes involved in metamorphosis) and their regulators such as miRNAs are potential targets for pest control, we analyzed the sesquiterpenoid (juvenile) and ecdysteroid (molting) hormone biosynthesis pathway genes including their miRNAs and relevant neuropeptides. Temporal gene expression changes of these insect hormone biosynthesis pathways were observed at different developmental stages. Similarly, a diet-specific response in gene expression was also observed in both head and salivary glands. Furthermore, we observed that microRNAs (bantam, miR-14, miR-316, and miR-263) of R. pedestris fed with different types of soybeans were differentially expressed in the salivary glands indicating a diet-specific response. Interestingly, the opposite arms of miR-281 (-5p and -3p), a miRNA involved in regulating development, were predicted to target Hmgs genes of R. pedestris and soybean, respectively. These observations among others highlight stinkbug's responses as a function of its interaction with soybean. In brief, the results of this study not only present salient findings that could be of potential use in pest management and mitigation but also provide an invaluable resource for R. pedestris as an insect model to facilitate studies on plant-pest interactions.


Assuntos
Heterópteros , Hormônios de Inseto , MicroRNAs , Animais , Glycine max/genética , Heterópteros/genética , Transcriptoma , MicroRNAs/genética , Perfilação da Expressão Gênica
2.
Angew Chem Int Ed Engl ; : e202405438, 2024 Apr 29.
Artigo em Inglês | MEDLINE | ID: mdl-38682249

RESUMO

The alkaline oxygen evolution reaction (OER) is a promising avenue for producing clean fuels and storing intermittent energy. However, challenges such as excessive OH- consumption and strong adsorption of oxygen-containing intermediates hinder the development of alkaline OER. In this study, we propose a cooperative strategy by leveraging both nano-scale and atomically local electric fields for alkaline OER, demonstrated through the synthesis of Mn single atom doped CoP nanoneedles (Mn SA-CoP NNs). Finite element method simulations and density functional theory calculations predict that the nano-scale local electric field enriches OH- around the catalyst surface, while the atomically local electric field improves *O desorption. Experimental validation using in situ attenuated total reflection infrared and Raman spectroscopy confirms the effectiveness of the nano-scale and atomically electric fields. Mn SA-CoP NNs exhibit an ultra-low overpotential of 189 mV at 10 mA cm-2 and stable operation over 100 hours at ~100 mA cm-2 during alkaline OER. This innovative strategy provides new insights for enhancing catalyst performance in energy conversion reactions.

3.
ACS Nano ; 18(17): 11474-11486, 2024 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-38632861

RESUMO

Cobalt-nitrogen-carbon (Co-N-C) catalysts with a CoN4 structure exhibit great potential for oxygen reduction reaction (ORR), but the imperfect adsorption energy toward oxygen species greatly limits their reduction efficiency and practical application potential. Here, F-coordinated Co-N-C catalysts with square-pyramidal CoN4-F1 configuration are successfully synthesized using F atoms to regulate the axial coordination of Co centers via hydrothermal and chemical vapor deposition methods. During the synthesis process, the geometry structure of the Co atom converts from six-coordinated Co-F6 to square-pyramidal CoN4-F1 in the coordinatively unsaturated state, which provides an open binding site for the O2. The introduction of axial F atoms into the CoN4 plane alters the local atomic environment around Co, significantly improving the ORR activity and Zn-air batteries performance. In situ spectroscopy proves that CoN4-F1 sites strongly combine with the OOH* intermediate and facilitate the splitting of O-O bond, making OOH* readily decompose into O* and OH* via a dissociative pathway. Theoretical calculations confirm that the axial F atom effectively reduces the electronic density of the Co centers and facilitates the desorption of the OH* intermediate, efficiently accelerating the overall ORR kinetics. This work advances a feasible synthesis mechanism of axial ligands and provides a route to construct efficient high-coordination catalysts.

4.
Sci Adv ; 10(13): eadl1598, 2024 Mar 29.
Artigo em Inglês | MEDLINE | ID: mdl-38552023

RESUMO

Heatwaves are consecutive hot days with devastating impacts on human health and the environment. These events may evolve across both space and time, characterizing a spatiotemporally contiguous propagation pattern that has not been fully understood. Here, we track the spatiotemporally contiguous heatwaves in both reanalysis datasets and model simulations and examine their moving patterns (i.e., moving distance, speed, and direction) in different continents and periods. Substantial changes in contiguous heatwaves have been identified from 1979 to 2020, with longer persistence, longer traveling distance, and slower propagation. These changes have been amplified since 1997, probably due to the weakening of eddy kinetic energy, zonal wind, and anthropogenic forcing. The results suggest that longer-lived, longer-traveling, and slower-moving contiguous heatwaves will cause more devastating impacts on human health and the environment in the future if greenhouse gas emissions keep rising and no effective measures are taken immediately. Our findings provide important implications for the adaption and mitigation of globally connected extreme heatwaves.

5.
Nat Commun ; 15(1): 1097, 2024 Feb 06.
Artigo em Inglês | MEDLINE | ID: mdl-38321034

RESUMO

Bimetallic PtRu are promising electrocatalysts for hydrogen oxidation reaction in anion exchange membrane fuel cell, where the activity and stability are still unsatisfying. Here, PtRu nanowires were implanted with a series of oxophilic metal atoms (named as i-M-PR), significantly enhancing alkaline hydrogen oxidation reaction (HOR) activity and stability. With the dual doping of In and Zn atoms, the i-ZnIn-PR/C shows mass activity of 10.2 A mgPt+Ru-1 at 50 mV, largely surpassing that of commercial Pt/C (0.27 A mgPt-1) and PtRu/C (1.24 A mgPt+Ru-1). More importantly, the peak power density and specific power density are as high as 1.84 W cm-2 and 18.4 W mgPt+Ru-1 with a low loading (0.1 mg cm-2) anion exchange membrane fuel cell. Advanced experimental characterizations and theoretical calculations collectively suggest that dual doping with In and Zn atoms optimizes the binding strengths of intermediates and promotes CO oxidation, enhancing the HOR performances. This work deepens the understanding of developing novel alloy catalysts, which will attract immediate interest in materials, chemistry, energy and beyond.

6.
Nat Commun ; 15(1): 1264, 2024 Feb 10.
Artigo em Inglês | MEDLINE | ID: mdl-38341446

RESUMO

Nitrate (NO3‒) pollution poses significant threats to water quality and global nitrogen cycles. Alkaline electrocatalytic NO3‒ reduction reaction (NO3RR) emerges as an attractive route for enabling NO3‒ removal and sustainable ammonia (NH3) synthesis. However, it suffers from insufficient proton (H+) supply in high pH conditions, restricting NO3‒-to-NH3 activity. Herein, we propose a halogen-mediated H+ feeding strategy to enhance the alkaline NO3RR performance. Our platform achieves near-100% NH3 Faradaic efficiency (pH = 14) with a current density of 2 A cm-2 and enables an over 99% NO3--to-NH3 conversion efficiency. We also convert NO3‒ to high-purity NH4Cl with near-unity efficiency, suggesting a practical approach to valorizing pollutants into valuable ammonia products. Theoretical simulations and in situ experiments reveal that Cl-coordination endows a shifted d-band center of Pd atoms to construct local H+-abundant environments, through arousing dangling O-H water dissociation and fast *H desorption, for *NO intermediate hydrogenation and finally effective NO3‒-to-NH3 conversion.

7.
Small ; : e2400564, 2024 Feb 17.
Artigo em Inglês | MEDLINE | ID: mdl-38368264

RESUMO

Developing efficient metal-free catalysts to directly synthesize hydrogen peroxide (H2 O2 ) through a 2-electron (2e) oxygen reduction reaction (ORR) is crucial for substituting the traditional energy-intensive anthraquinone process. Here, in-plane topological defects enriched graphene with pentagon-S and pyrrolic-N coordination (SNC) is synthesized via the process of hydrothermal and nitridation. In SNC, pentagon-S and pyrrolic-N originating from thiourea precursor are covalently grafted onto the basal plane of the graphene framework, building unsymmetrical dumbbell-like S─C─N motifs, which effectively modulates atomic and electronic structures of graphene. The SNC catalyst delivers ultrahigh H2 O2 productivity of 8.1, 7.3, and 3.9 mol gcatalyst -1  h-1 in alkaline, neutral, and acidic electrolytes, respectively, together with long-term operational stability in pH-universal electrolytes, outperforming most reported carbon catalysts. Theoretical calculations further unveil that defective S─C─N motifs efficiently optimize the binding strength to OOH* intermediate and substantially diminish the kinetic barrier for reducing O2 to H2 O2 , thereby promoting the intrinsic activity of 2e-ORR.

8.
Genome Biol ; 25(1): 46, 2024 Feb 12.
Artigo em Inglês | MEDLINE | ID: mdl-38347618

RESUMO

Single-strand breaks are the major DNA damage in the genome and serve a crucial role in various biological processes. To reveal the significance of single-strand breaks, multiple sequencing-based single-strand break detection methods have been developed, which are costly and unfeasible for large-scale analysis. Hence, we propose SSBlazer, an explainable and scalable deep learning framework for single-strand break site prediction at the nucleotide level. SSBlazer is a lightweight model with robust generalization capabilities across various species and is capable of numerous unexplored SSB-related applications.


Assuntos
Dano ao DNA , Nucleotídeos , Reparo do DNA
9.
J Leukoc Biol ; 115(1): 164-176, 2024 01 05.
Artigo em Inglês | MEDLINE | ID: mdl-37170891

RESUMO

Asthma is the chronic pulmonary inflammatory response that could lead to respiratory failure when allergic reactions exacerbate. It is featured by type 2 immunity with eosinophilic inflammation, mucus, and IgE production, and Th2 cytokine secretion upon repeated challenge of allergens. The symptom severity of asthma displays an apparent circadian rhythm with aggravated airway resistance in the early morning in patients. Bmal1 is the core regulator of the circadian clock, while the regulatory role of Bmal1 in asthma remains unclear. Here, we investigate whether the myeloid Bmal1 is involved in the pathogenesis of house dust mite (HDM)-induced lung allergy. We found that knockdown of Bmal1 in macrophages suppressed the time-of-day variance of the eosinophil infiltration in the alveolar spaces in chronic asthmatic mice. This was accompanied by decreased bronchial mucus production, collagen deposition, and HDM-specific IgE production. However, the suppression effects of myeloid Bmal1 deletion did not alter the allergic responses in short-term exposure to HDM. The transcriptome profile of alveolar macrophages (AMs) showed that Bmal1-deficient AMs have enhanced phagocytosis and reduced production of allergy-mediating prostanoids thromboxane A2 and prostaglandin F2α synthesis. The attenuated thromboxane A2 and prostaglandin F2α may lead to less induction of the eosinophil chemokine Ccl11 expression in bronchial epithelial cells. In summary, our study demonstrates that Bmal1 ablation in macrophages attenuates eosinophilic inflammation in HDM-induced chronic lung allergy, which involves enhanced phagocytosis and reduced prostanoid secretion.


Assuntos
Asma , Eosinofilia , Hipersensibilidade , Humanos , Camundongos , Animais , Pyroglyphidae , Dinoprosta/metabolismo , Tromboxano A2/metabolismo , Pulmão , Alérgenos , Eosinofilia/metabolismo , Eosinofilia/patologia , Imunoglobulina E/metabolismo , Inflamação/patologia , Modelos Animais de Doenças
10.
Small ; 20(2): e2305219, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37658514

RESUMO

Materials with negative thermal expansion (NTE) attract significant research attention owing to their unique physical properties and promising applications. Although ferroelectric phase transitions leading to NTE are widely investigated, information on antiferroelectricity-induced NTE remains limited. In this study, single-crystal and polycrystalline Pb2 CoMoO6 samples are prepared at high pressure and temperature conditions. The compound crystallizes into an antiferroelectric Pnma orthorhombic double perovskite structure at room temperature owing to the opposite displacements dominated by Pb2+ ions. With increasing temperature to 400 K, a structural phase transition to cubic Fm-3m paraelectric phase occurs, accompanied by a sharp volume contraction of 0.41%. This is the first report of an antiferroelectric-to-paraelectric transition-induced NTE in Pb2 CoMoO6 . Moreover, the compound also exhibits remarkable NTE with an average volumetric coefficient of thermal expansion αV = -1.33 × 10-5 K-1 in a wide temperature range of 30-420 K. The as-prepared Pb2 CoMoO6 thus serves as a prototype material system for studying antiferroelectricity-induced NTE.

11.
Nat Nanotechnol ; 19(2): 208-218, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-37798568

RESUMO

A critical current challenge in the development of all-solid-state lithium batteries (ASSLBs) is reducing the cost of fabrication without compromising the performance. Here we report a sulfide ASSLB based on a high-energy, Co-free LiNiO2 cathode with a robust outside-in structure. This promising cathode is enabled by the high-pressure O2 synthesis and subsequent atomic layer deposition of a unique ultrathin LixAlyZnzOδ protective layer comprising a LixAlyZnzOδ surface coating region and an Al and Zn near-surface doping region. This high-quality artificial interphase enhances the structural stability and interfacial dynamics of the cathode as it mitigates the contact loss and continuous side reactions at the cathode/solid electrolyte interface. As a result, our ASSLBs exhibit a high areal capacity (4.65 mAh cm-2), a high specific cathode capacity (203 mAh g-1), superior cycling stability (92% capacity retention after 200 cycles) and a good rate capability (93 mAh g-1 at 2C). This work also offers mechanistic insights into how to break through the limitation of using expensive cathodes (for example, Co-based) and coatings (for example, Nb-, Ta-, La- or Zr-based) while still achieving a high-energy ASSLB performance.

12.
Clin Gastroenterol Hepatol ; 22(3): 630-641.e4, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-37918685

RESUMO

BACKGROUND: The effect of computer-aided polyp detection (CADe) on adenoma detection rate (ADR) among endoscopists-in-training remains unknown. METHODS: We performed a single-blind, parallel-group, randomized controlled trial in Hong Kong between April 2021 and July 2022 (NCT04838951). Eligible subjects undergoing screening/surveillance/diagnostic colonoscopies were randomized 1:1 to receive colonoscopies with CADe (ENDO-AID[OIP-1]) or not (control) during withdrawal. Procedures were performed by endoscopists-in-training with <500 procedures and <3 years' experience. Randomization was stratified by patient age, sex, and endoscopist experience (beginner vs intermediate level, <200 vs 200-500 procedures). Image enhancement and distal attachment devices were disallowed. Subjects with incomplete colonoscopies or inadequate bowel preparation were excluded. Treatment allocation was blinded to outcome assessors. The primary outcome was ADR. Secondary outcomes were ADR for different adenoma sizes and locations, mean number of adenomas, and non-neoplastic resection rate. RESULTS: A total of 386 and 380 subjects were randomized to CADe and control groups, respectively. The overall ADR was significantly higher in the CADe group than in the control group (57.5% vs 44.5%; adjusted relative risk, 1.41; 95% CI, 1.17-1.72; P < .001). The ADRs for <5 mm (40.4% vs 25.0%) and 5- to 10-mm adenomas (36.8% vs 29.2%) were higher in the CADe group. The ADRs were higher in the CADe group in both the right colon (42.0% vs 30.8%) and left colon (34.5% vs 27.6%), but there was no significant difference in advanced ADR. The ADRs were higher in the CADe group among beginner (60.0% vs 41.9%) and intermediate-level (56.5% vs 45.5%) endoscopists. Mean number of adenomas (1.48 vs 0.86) and non-neoplastic resection rate (52.1% vs 35.0%) were higher in the CADe group. CONCLUSIONS: Among endoscopists-in-training, the use of CADe during colonoscopies was associated with increased overall ADR. (ClinicalTrials.gov, Number: NCT04838951).


Assuntos
Adenoma , Pólipos do Colo , Neoplasias Colorretais , Pólipos , Humanos , Neoplasias Colorretais/diagnóstico , Método Simples-Cego , Colonoscopia/métodos , Adenoma/diagnóstico , Computadores , Pólipos do Colo/diagnóstico
13.
J Am Chem Soc ; 146(1): 468-475, 2024 Jan 10.
Artigo em Inglês | MEDLINE | ID: mdl-38150583

RESUMO

The in-tandem catalyst holds great promise for addressing the limitation of low *CO coverage on Cu-based materials for selective C2H4 generation during CO2 electroreduction. However, the potential mismatch between the CO-formation catalyst and the favorable C-C coupling Cu catalyst represents a bottleneck in these types of electrocatalysts, resulting in low tandem efficiencies. In this study, we propose a robust solution to this problem by introducing a wide-CO generation-potential window nickel single atom catalyst (Ni SAC) supported on a Cu catalyst. The selection of Ni SAC was based on theoretical calculations, and its excellent performance was further confirmed by using in situ IR spectroscopy. The facilitated carbon dimerization in our tandem catalyst led to a ∼370 mA/cm2 partial current density of C2H4, corresponding to a faradic efficiency of ∼62%. This performance remained stable and consistent for at least ∼14 h at a high current density of 500 mA/cm2 in a flow-cell reactor, outperforming most tandem catalysts reported so far.

14.
Nano Lett ; 23(24): 11827-11834, 2023 Dec 27.
Artigo em Inglês | MEDLINE | ID: mdl-38079388

RESUMO

Local electric field induced by the lightning-rod effect attracts great attention for regulating the local microenvironment and electronic properties of active sites. Nevertheless, local electric-field-assisted applications are mainly limited to metals with strong surface plasmonic resonance properties (e.g., Au, Ag, and Cu). Herein, we fabricate RuCu snow-like nanosheets (SNSs) with high-curvature nanotips for enhancing the hydrogen oxidation reaction (HOR) and hydrogen evolution reaction (HER). Theoretical simulations show that RuCu SNSs can induce a strong local electric field around the sharp nanotips, which favors the accumulation of OH- for HOR and H+ for HER. Cu incorporation can modulate the binding strength of OH* and H*, leading to significantly enhanced HOR and HER performance. Impressively, the mass activity of RuCu SNSs for alkaline HOR is 31.3 times higher than that of RuCu nanocrystals without sharp tips. Besides, the required overpotential for reaching 10 mA cm-2 during HER over RuCu SNSs is 14.0 mV.

15.
Environ Sci Technol ; 57(51): 21779-21790, 2023 Dec 26.
Artigo em Inglês | MEDLINE | ID: mdl-38091466

RESUMO

Arbuscular mycorrhizal (AM) fungi play an important role in organic matter (OM) stabilization in Fe ore tailings for eco-engineered soil formation. However, little has been understood about the AM fungi-derived organic signature and organo-mineral interactions in situ at the submicron scale. In this study, a compartmentalized cultivation system was used to investigate the role of AM fungi in OM formation and stabilization in tailings. Particularly, microspectroscopic analyses including synchrotron-based transmission Fourier transform infrared (FTIR) and scanning transmission X-ray microspectroscopy combined with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS) were employed to characterize the chemical signatures at the AM fungal-mineral and mineral-OM interfaces at the submicron scale. The results indicated that AM fungal mycelia developed well in the tailings and entangled mineral particles for aggregation. AM fungal colonization enhanced N-rich OM stabilization through organo-mineral association. Bulk spectroscopic analysis together with FTIR mapping revealed that fungi-derived lipids, proteins, and carbohydrates were associated with Fe/Si minerals. Furthermore, STXM-NEXAFS analysis revealed that AM fungi-derived aromatic, aliphatic, and carboxylic/amide compounds were heterogeneously distributed and trapped by Fe(II)/Fe(III)-bearing minerals originating from biotite-like minerals weathering. These findings imply that AM fungi can stimulate mineral weathering and provide organic substances to associate with minerals, contributing to OM stabilization and aggregate formation as key processes for eco-engineered soil formation in tailings.


Assuntos
Compostos Férricos , Micorrizas , Compostos Férricos/química , Espectroscopia de Infravermelho com Transformada de Fourier , Síncrotrons , Análise de Fourier , Minerais/química , Solo/química , Ferro
16.
Environ Sci Technol ; 57(51): 21744-21756, 2023 Dec 26.
Artigo em Inglês | MEDLINE | ID: mdl-38085882

RESUMO

Mineral weathering and alkaline pH neutralization are prerequisites to the ecoengineering of alkaline Fe-ore tailings into soil-like growth media (i.e., Technosols). These processes can be accelerated by the growth and physiological functions of tolerant sulfur oxidizing bacteria (SOB) in tailings. The present study characterized an indigenous SOB community enriched in the tailings, in response to the addition of elemental sulfur (S0) and organic matter (OM), as well as resultant S0oxidation, pH neutralization, and mineral weathering in a glasshouse experiment. The addition of S0 was found to have stimulated the growth of indigenous SOB, such as acidophilic Alicyclobacillaceae, Bacillaceae, and Hydrogenophilaceae in tailings. The OM amendment favored the growth of heterotrophic/mixotrophic SOB (e.g., class Alphaproteobacteria and Gammaproteobacteria). The resultant S0 oxidation neutralized the alkaline pH and enhanced the weathering of biotite-like minerals and formation of secondary minerals, such as ferrihydrite- and jarosite-like minerals. The improved physicochemical properties and secondary mineral formation facilitated organo-mineral associations that are critical to soil aggregate formation. From these findings, co-amendments of S0 and plant biomass (OM) can be applied to enhance the abundance of the indigenous SOB community in tailings and accelerate mineral weathering and geochemical changes for eco-engineered soil formation, as a sustainable option for rehabilitation of Fe ore tailings.


Assuntos
Compostos de Ferro , Minerais , Bactérias , Enxofre , Oxirredução , Ferro , Solo , Concentração de Íons de Hidrogênio
18.
Plant Genome ; 16(4): e20400, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37940622

RESUMO

Breeding for increased protein without a reduction in oil content in soybeans [Glycine max (L.) Merr.] is a challenge for soybean breeders but an expected goal. Many efforts have been made to develop new soybean varieties with high yield in combination with desirable protein and/or oil traits. An elite line, R05-1415, was reported to be high yielding, high protein, and low oil. Several significant quantitative trait loci (QTL) for protein and oil were reported in this line, but many of them were unstable across environments or genetic backgrounds. Thus, a new study under multiple field environments using the Infinium BARCSoySNP6K BeadChips was conducted to detect and confirm stable genomic loci for these traits. Genetic analyses consistently detected a single major genomic locus conveying these two traits with remarkably high phenotypic variation explained (R2 ), varying between 24.2% and 43.5%. This new genomic locus is located between 25.0 and 26.7 Mb, distant from the previously reported QTL and did not overlap with other commonly reported QTL and the recently cloned gene Glyma.20G085100. Homolog analysis indicated that this QTL did not result from the paracentric chromosome inversion with an adjacent genomic fragment that harbors the reported QTL. The pleiotropic effect of this QTL could be a challenge for improving protein and oil simultaneously; however, a further study of four candidate genes with significant expressions in the seed developmental stages coupled with haplotype analysis may be able to pinpoint causative genes. The functionality and roles of these genes can be determined and characterized, which lay a solid foundation for the improvement of protein and oil content in soybeans.


Assuntos
Glycine max , Melhoramento Vegetal , Mapeamento Cromossômico , Genômica , Glycine max/genética , Sementes/genética , Sementes/metabolismo , Óleos de Plantas
19.
ACS Nano ; 17(22): 22691-22700, 2023 Nov 28.
Artigo em Inglês | MEDLINE | ID: mdl-37926947

RESUMO

High-entropy alloys (HEAs) are significantly promising candidates for heterogeneous catalysis, yet the controllable synthesis of ultrafine HEA nanoparticles (NPs) remains a formidable challenge due to severe thermal sintering during the high-temperature fabrication process. Herein, we report a sulfur-stabilizing strategy to construct ultrafine HEA NPs with an average diameter of 4.02 nm supported on sulfur-modified Ti3C2Tx (S-Ti3C2Tx) MXene, on which the strong interfacial metal-sulfur interactions between HEA NPs and the S-Ti3C2Tx supports significantly increase the interfacial adhesion strength, thus greatly suppressing nanoparticle sintering by retarding both particle migration and metal atom diffusion. The representative quinary PtPdCuNiCo HEA-S-Ti3C2Tx exhibits excellent catalytic performance toward alkaline ethanol oxidation reaction (EOR) with an ultrahigh mass activity of 7.03 A mgPt+Pd-1, which is 4.34 and 5.17 times higher than those of the commercial Pt/C and Pd/C catalysts, respectively. In situ attenuated total reflection-infrared spectroscopy studies reveal that the high intrinsic catalytic activity for the EOR can be ascribed to the synergy of different catalytically active sites of HEA NPs and the well-designed interfacial metal-sulfur interactions.

20.
Nat Commun ; 14(1): 6576, 2023 Oct 18.
Artigo em Inglês | MEDLINE | ID: mdl-37852958

RESUMO

Realizing viable electrocatalytic processes for energy conversion/storage strongly relies on an atomic-level understanding of dynamic configurations on catalyst-electrolyte interface. X-ray absorption spectroscopy (XAS) has become an indispensable tool to in situ investigate dynamic natures of electrocatalysts but still suffers from limited energy resolution, leading to significant electronic transitions poorly resolved. Herein, we highlight advanced X-ray spectroscopies beyond conventional XAS, with emphasis on their unprecedented capabilities of deciphering key configurations of electrocatalysts. The profound complementarities of X-ray spectroscopies from various aspects are established in a probing energy-dependent "in situ spectroscopy map" for comprehensively understanding the solid-liquid interface. This perspective establishes an indispensable in situ research model for future studies and offers exciting research prospects for scientists and spectroscopists.

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