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1.
Angew Chem Int Ed Engl ; 62(27): e202304413, 2023 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-37160619

RESUMO

Designing highly efficient and stable electrode-electrolyte interface for hydrogen peroxide (H2 O2 ) electrosynthesis remains challenging. Inhibiting the competitive side reaction, 4 e- oxygen reduction to H2 O, is essential for highly selective H2 O2 electrosynthesis. Instead of hindering excessive hydrogenation of H2 O2 via catalyst modification, we discover that adding a hydrogen-bond acceptor, dimethyl sulfoxide (DMSO), to the KOH electrolyte enables simultaneous improvement of the selectivity and activity of H2 O2 electrosynthesis. Spectral characterization and molecular simulation confirm that the formation of hydrogen bonds between DMSO and water molecules at the electrode-electrolyte interface can reduce the activity of water dissociation into active H* species. The suitable H* supply environment hinders excessive hydrogenation of the oxygen reduction reaction (ORR), thus improving the selectivity of 2 e- ORR and achieving over 90 % selectivity of H2 O2 . This work highlights the importance of regulating the interfacial hydrogen-bond environment by organic molecules as a means of boosting electrochemical performance in aqueous electrosynthesis and beyond.

2.
J Colloid Interface Sci ; 555: 470-479, 2019 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-31400539

RESUMO

Ultrasmall silver nanoclusters (Ag NCs) are one of the emerging and highly efficient antibacterial agents, owing to the unique features of sub-2 nm particle size and the high abundance of the active Ag+ species. However, practical applications of Ag NCs in biological environment are often hampered by silver oxidization, which results in particle aggregation and loss of antibacterial activity. In this study, for the first time, we develop a facile method to synthesize highly dispersed Ag NCs decorated mesoporous silica nanoparticles (Ag NC-MSNs) capable of long-term and efficient release of Ag+ ions. This novel Ag NC-MSNs nanocomposite was demonstrated as an effective antibacterial agent against both Gram-positive and Gram-negative pathogenic bacteria. Compared with the counterparts Ag NCs and silver nanoparticles decorated mesoporous silica nanoparticles (Ag NP-MSNs), Ag NC-MSNs exhibit 17-fold and 27-fold enhancement in antibacterial potency, respectively. The homogeneous distribution of ultrasmall Ag NCs in the mesoporous architecture of supporting MSNs matrix is crucial for the controlled release of Ag+ ions, leading to the superior broad-spectrum antimicrobial activity. Moreover, the cytotoxicity assay indicated that the effective antibacterial concentration of Ag NC-MSNs shows minimum toxicity on mammalian cells. This new Ag nanocomposite developed in this work is promising for practical applications against various microbial infections.


Assuntos
Antibacterianos/farmacologia , Nanopartículas/química , Pseudomonas aeruginosa/efeitos dos fármacos , Dióxido de Silício/farmacologia , Prata/farmacologia , Staphylococcus aureus/efeitos dos fármacos , Antibacterianos/química , Sobrevivência Celular/efeitos dos fármacos , Células HeLa , Humanos , Testes de Sensibilidade Microbiana , Tamanho da Partícula , Porosidade , Espécies Reativas de Oxigênio/análise , Dióxido de Silício/química , Prata/química , Propriedades de Superfície
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