The electrochemical nitrogen reduction reaction (NRR) offers a sustainable solution towards ammonia production but suffers poor reaction performance owing to preferential catalyst–H formation and the ...consequential hydrogen evolution reaction (HER). Now, the Pt/Au electrocatalyst d‐band structure is electronically modified using zeolitic imidazole framework (ZIF) to achieve a Faradaic efficiency (FE) of >44 % with high ammonia yield rate of >161 μg mgcat−1 h−1 under ambient conditions. The strategy lowers electrocatalyst d‐band position to weaken H adsorption and concurrently creates electron‐deficient sites to kinetically drive NRR by promoting catalyst–N2 interaction. The ZIF coating on the electrocatalyst doubles as a hydrophobic layer to suppress HER, further improving FE by >44‐fold compared to without ZIF (ca. 1 %). The Pt/Au‐NZIF interaction is key to enable strong N2 adsorption over H atom.
A kinetically driven ambient nitrogen reduction reaction has a Faradaic efficiency of over 44 % and an ammonia yield rate of over 161 μg mgcat−1 h−1. It employs a zeolitic imidazole framework to induce electron‐deficient sites on the catalyst and a lower d‐band to weaken catalyst–H interactions whilst promoting the catalyst–N2 interaction.
Photothermal materials are crucial for diverse heating applications, but it remains challenging to achieve high energy conversion efficiency due to the difficulty to concurrently improve light ...absorbance and suppress heat loss. Herein, a zeolitic imidazolate framework‐isolated graphene (G@ZIF) nanohybrid is demonstrated that utilizes ultrathin, heat‐insulating ZIF layers, and G@ZIF interfacial nanocavity to synergistically intensify light absorbance and heat localization. Under artificial sunlight illumination (≈1 kW m−2), the G@ZIF film attains a maximum temperature of 120 °C in an open environment with a 98% solar‐to‐thermal conversion efficiency. Importantly, the porous ZIF layer allows small molecules/media to enter and access the embedded hot graphene surface for targeted heat transfer in practical applications. As a proof‐of‐concept, the G@ZIF‐based steam generator realizes 96% energy conversion from light to vapor with near‐perfect desalination and water purification efficiencies (>99.9%). This design is generic and can be extended to other photothermal systems for advanced solar‐thermal applications, including catalysis, water treatments, sterilization, and mechanical actuation.
MOF‐isolated graphene (G@ZIF) nanohybrids demonstrate strong solar light absorbance and a 98% solar‐to‐thermal conversion efficiency, owing to its ultrathin, heat‐insulating ZIF layers, and G@ZIF interfacial nanocavity to synergistically intensify light absorbance and minimize heat loss. The maximum surface temperature reaches 120 °C under simulated one‐sun illumination, enabling efficient interfacial water evaporation for desalination.
We comprehensively analyzed clinical, genomic, and transcriptomic data of a cohort of 465 primary triple-negative breast cancer (TNBC). PIK3CA mutations and copy-number gains of chromosome 22q11 were ...more frequent in our Chinese cohort than in The Cancer Genome Atlas. We classified TNBCs into four transcriptome-based subtypes: (1) luminal androgen receptor (LAR), (2) immunomodulatory, (3) basal-like immune-suppressed, and (4) mesenchymal-like. Putative therapeutic targets or biomarkers were identified among each subtype. Importantly, the LAR subtype showed more ERBB2 somatic mutations, infrequent mutational signature 3 and frequent CDKN2A loss. The comprehensive profile of TNBCs provided here will serve as a reference to further advance the understanding and precision treatment of TNBC.
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•We build the genomic and transcriptomic landscape of 465 primary TNBCs•Chinese TNBC cases demonstrate more PIK3CA mutations and LAR subtype•Transcriptomic data classify TNBCs into four subtypes•Multi-omics profiling identifies potential targets within specific TNBC subtypes
Jiang et al. characterize primary Chinese triple-negative breast cancer (TNBC) and classify it into four subtypes. They find that these TNBCs have more frequent PIK3CA mutations and chromosome 22q11 copy-number gains than non-Asian TNBCs and that the LAR subtype has more ERBB2 somatic mutations and CDKN2A loss.
We demonstrate the fabrication of graphene liquid marbles as photothermal miniature reactors with precise temperature control for reaction kinetics modulation. Graphene liquid marbles show rapid and ...highly reproducible photothermal behavior while maintaining their excellent mechanical robustness. By tuning the applied laser power, swift regulation of graphene liquid marble’s surface temperature between 21–135 °C and its encapsulated water temperature between 21–74 °C are demonstrated. The temperature regulation modulates the reaction kinetics in our graphene liquid marble, achieving a 12‐fold superior reaction rate constant for methylene blue degradation than at room temperature.
The fabrication of graphene liquid marbles as photothermal miniature reactors with high mechanical robustness is demonstrated. The reaction temperature can be precisely controlled between 21 and 135 °C by tuning the laser power applied. This allows their application for the modulation and acceleration of reaction kinetics and overcomes the lack of a heating mechanism in conventional liquid marble reactors.
To control the ongoing COVID‐19 pandemic, a variety of severe acute respiratory syndrome coronavirus 2 (SARS‐CoV‐2) vaccines have been developed. However, the rapid mutations of SARS‐CoV‐2 spike (S) ...protein may reduce the protective efficacy of the existing vaccines which is mainly determined by the level of neutralizing antibodies targeting S. In this study, we screened prevalent S mutations and constructed 124 pseudotyped lentiviral particles carrying these mutants. We challenged these pseudoviruses with sera vaccinated by Sinovac CoronaVac and ZF2001 vaccines, two popular vaccines designed for the initial strain of SARS‐CoV‐2, and then systematically assessed the susceptivity of these SARS‐CoV‐2 variants to the immune sera of vaccines. As a result, 14 S mutants (H146Y, V320I + S477N, V382L, K444R, L455F + S477N, L452M + F486L, F486L, Y508H, P521R, A626S, S477N + S698L, A701V, S477N + T778I, E1144Q) were found to be significantly resistant to neutralization, indicating reduced protective efficacy of the vaccines against these SARS‐CoV‐2 variants. In addition, F486L and Y508H significantly enhanced the utilization of human angiotensin‐converting enzyme 2, suggesting a potentially elevated infectivity of these two mutants. In conclusion, our results show that some prevalent S mutations of SARS‐CoV‐2 reduced the protective efficacy of current vaccines and enhance the infectivity of the virus, indicating the necessity of vaccine renewal and providing direction for the development of new vaccines.
The understanding of the localized surface plasmons (LSPs) that occur at the geometrically bounded surface of metal nanoparticles continues to advance as new and more complex nanostructures are ...found. It has been shown that the oscillation of electrons at the metal dielectric interface is strongly dependent on the size, symmetry, and proximity of nanoparticles. Here, we present a new method to chemically control the shape of silver nanocrystals by using a highly anisotropic etching process. Tuning of the etchant strength and reaction conditions allows the preparation of new nanoparticle shapes in high yield and purity, which cannot be synthesized with conventional nanocrystal growth methods. The etching process produces intraparticle gaps, which introduce modified plasmonic characteristics and significant scattering intensity in the near-infrared. These new silver particles serve as excellent substrates for wavelength-tunable, single-particle surface enhanced Raman spectroscopy (spSERS).
The discovery of the enhancement of Raman scattering by molecules adsorbed on nanostructured metal surfaces is a landmark in the history of spectroscopic and analytical techniques. Significant ...experimental and theoretical effort has been directed toward understanding the surface-enhanced Raman scattering (SERS) effect and demonstrating its potential in various types of ultrasensitive sensing applications in a wide variety of fields. In the 45 years since its discovery, SERS has blossomed into a rich area of research and technology, but additional efforts are still needed before it can be routinely used analytically and in commercial products. In this Review, prominent authors from around the world joined together to summarize the state of the art in understanding and using SERS and to predict what can be expected in the near future in terms of research, applications, and technological development. This Review is dedicated to SERS pioneer and our coauthor, the late Prof. Richard Van Duyne, whom we lost during the preparation of this article.
A novel approach was developed to fabricate a protective superhydrophobic LDH film on a Zn–Al alloyed surface of AZ31 Mg alloy. The alloyed surface layer not only provided essential divalent and ...trivalent cations and a base for the direct growth of a Mg–Zn–Al LDH film in a sodium nitrate hydrothermal solution, but also offered additional corrosion and mechanical protection for the substrate magnesium alloy. Further modification with low surface energy lauric acid (LA) could change the micro/nano hierarchical topographic surface of the LDH film from hydrophilicity to super-hydrophobicity. The long-term anti-corrosion performance, super-hydrophobicity, wear resistance, chemical stability and adhesion strength of the LA-modified LDH film on the surface-alloyed AZ31 were experimentally verified.
•A LDH film is directly grown on a surface-alloyed AZ31.•The alloyed surface layer acts as an internal of feedstock of divalent and trivalent cations for the LDH formation.•The alloyed surface layer provides a good adhesive protective and wear-resistant base for the LDH film.•The LDH film is long-term anti-corrosion resistant.•The LA-modified LDH film is super-hydrophobicity.
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