Nanoconfinement in porous catalysts may induce reactant concentration gradients inside the pores due to local conversion. This leads to inefficient active material use since parts of the catalyst may be trapped in an inactive state. Experimentally, these effects remain unstudied due to material complexity and required high spatial resolution. Here, we have nanofabricated quasi-two-dimensional mimics of porous catalysts, which combine the traits of nanofluidics with single particle plasmonics and online mass spectrometry readout. Enabled by single particle resolution at conditions during CO oxidation over a Cu model catalyst, we directly visualize reactant concentration gradient formation due to conversion on single Cu nanoparticles inside the "model pore" and how it dynamically controls oxidation state-and, thus, activity-of particles downstream. Our results provide a general framework for single particle catalysis in the gas phase and highlight the importance of single particle approaches for the understanding of complex catalyst materials.
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http://dx.doi.org/10.1126/sciadv.aba7678 | DOI Listing |
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December 2024
Department of Chemistry, The University of British Columbia, 3247 University Way, Kelowna, BC, V1V 1V7, Canada.
Limitations in solar energy conversion by photocatalysis typically stem from poor underlying charge carrier properties. Transient Absorption (TA) reveals insights on key photocatalytic properties such as charge carrier lifetimes and trapping. However, on the microsecond timescale, these measurements use relatively large probe sizes ranging in millimetres to centimetres which averages the effect of spatial heterogeneity at smaller length scales.
View Article and Find Full Text PDFAdv Mater
December 2024
Department of Material Science and Engineering, University of California, Berkeley, CA, 94706, USA.
Mn-rich disordered rocksalt materials with Li-excess (DRX) materials have emerged as a promising class of earth-abundant and energy-dense next-generation cathode materials for lithium-ion batteries. Recently, an electrochemical transformation to a spinel-like "δ" phase has been reported in Mn-rich DRX materials, with improved capacity, rate capability, and cycling stability compared with previous DRX compositions. However, this transformation unfolds slowly over the course of cycling, complicating the development and understanding of these materials.
View Article and Find Full Text PDFMikrochim Acta
December 2024
Department of Analytical Chemistry and Food Technology, Environmental Sciences Institute (ICAM), University of Castilla-La Mancha, Avda. Carlos III S/N, 45071, Toledo, Spain.
Single particle inductively coupled plasma mass spectrometry (SP-ICP-MS) is a powerful tool for metallic nanoparticle (NP) characterisation in terms of concentration and, taking into account several assumptions, also size. However, this technique faces challenges, such as the intrinsic matrix effect, which significantly impact the results when analysing real complex samples. This issue is critical for the calculations of key SP-ICP-MS parameters ultimately altering the final outcomes.
View Article and Find Full Text PDFJ Struct Biol
December 2024
Program in Cellular and Molecular Medicine, Boston Children's Hospital, 200 Longwood Ave, Boston, MA 02115, USA; Department of Cell Biology, Harvard Medical School, 200 Longwood Ave, Boston, MA 02115, USA; Department of Pediatrics, Harvard Medical School, 200 Longwood Ave, Boston, MA 02115, USA. Electronic address:
Cryogenic electron tomography (cryo-ET) has rapidly advanced as a high-resolution imaging tool for visualizing subcellular structures in 3D with molecular detail. Direct image inspection remains challenging due to inherent low signal-to-noise ratios (SNR). We introduce CryoSamba, a self-supervised deep learning-based model designed for denoising cryo-ET images.
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