Noble-metal-free catalytic nanoparticles hold the promise being abundant, low-cost materials having a small environmental footprint and excellent performance, albeit inferior to that of noble metal counterparts. Several materials have a long-standing history of success in photocatalysis, in particular titanium dioxide, and in recent years more complex oxides and added functionality have emerged with enhanced performance. We will discuss different approaches related to the use of non-centrosymmetric and polar oxide nanoparticles and how the bulk photovoltaic effect, piezoelectricity, and pyroelectricity add to photocatalysis and tribocatalysis. We pay special attention to discriminate between the role of free versus that of bound charges within the catalyst, which is crucial to disentangle the different contributions to the catalytic reaction for the benefit of the overall enhanced catalytic performance in e.g. wastewater treatment and ultimately water-splitting.
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http://dx.doi.org/10.1002/anie.202207975 | DOI Listing |
Anal Chem
January 2025
School of Chemistry and Life Sciences, Jiangsu Key Laboratory for Environmental Functional Materials, Suzhou University of Science and Technology, Suzhou, Jiangsu 215009, China.
Pneumonia is a prevalent acute respiratory infection and a major cause of mortality and hospitalization, and the urgent demand for a rapid, direct, and highly accurate diagnostic method capable of detecting both () and () arises from their prominent roles as the primary pathogens responsible for pneumonia. Herein, two luminescent iridium complexes with nonoverlapping photoluminescence spectra, iridium(III)-bis [4,6-(difluorophenyl)-pyridinato-N,C'] picolinate (abbreviated as Ir-B) and bis (2-(3,5- dimethylphenyl) quinoline-C2,N') (acetylacetonato) iridium(III)) (abbreviated as Ir-R), were unprecedently proposed to construct a novel wavelength-resolved magnetic multiplex biosensor for simultaneous detection of and based on catalytic hairpin assembly (CHA) signal amplification strategy combined with dye-doped silica nanoparticles. Notably, the proposed wavelength-resolved multiplex biosensor not only exhibits a broad linear range from 50 pM to 10 nM but also demonstrates excellent recovery rates for (96.
View Article and Find Full Text PDFACS Nano
January 2025
State Key Laboratory of Physical Chemistry of Solid Surface, Key Laboratory of Chemical Biology of Fujian Province, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, P. R. China.
The assembly of peptides is generally mediated by liquid-liquid phase separation, which enables control over assembly kinetics, final structure, and functions of peptide-based supramolecular materials. Modulating phase separation can alter the assembly kinetics of peptides by changing solvents or introducing external fields. Herein, we demonstrate that the assembly of peptides can be effectively catalyzed by complex coacervates.
View Article and Find Full Text PDFPLoS Genet
January 2025
Epigenetics & Neurobiology Unit, EMBL Rome, European Molecular Biology Laboratory, Italy.
The reversible glycosylation of nuclear and cytoplasmic proteins (O-GlcNAcylation) is catalyzed by a single enzyme, namely O-GlcNAc transferase (OGT). The mammalian Ogt gene is X-linked, and it is essential for embryonic development and for the viability of proliferating cells. We perturbed OGT's function in vivo by creating a murine allelic series of four single amino acid substitutions, reducing OGT's catalytic activity to a range of degrees.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Max-Planck-Institut fur Kohlenforschung, Organometallic Chemistry, Kaiser-Wilhelm-Platz 1, 45470, Mülheim/Ruhr, GERMANY.
Ynamides, when reacted with H2 or HBpin in the presence of [Cp*RuCl]4, convert into chiral-at-metal Fischer carbenes by regioselective gem-hydrogenation or gem-hydroboration of the polarized triple bond, respectively. gem-Hydroboration concomitantly affords a carbogenic borylated stereocenter adjacent to the ruthenium carbene unit, the configuration of which can be controlled using an Evans auxiliary. These are the first examples of asymmetric gem-addition reactions to alkynes known in the literature; representative pianostool ruthenium carbene complexes formed by this unconventional route were characterized by crystallographic and spectroscopic means.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
January 2025
Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA 02138.
Despite the broad catalytic relevance of metal-support interfaces, controlling their chemical nature, the interfacial contact perimeter (exposed to reactants), and consequently, their contributions to overall catalytic reactivity, remains challenging, as the nanoparticle and support characteristics are interdependent when catalysts are prepared by impregnation. Here, we decoupled both characteristics by using a raspberry-colloid-templating strategy that yields partially embedded PdAu nanoparticles within well-defined SiO or TiO supports, thereby increasing the metal-support interfacial contact compared to nonembedded catalysts that we prepared by attaching the same nanoparticles onto support surfaces. Between nonembedded PdAu/SiO and PdAu/TiO, we identified a support effect resulting in a 1.
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