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Boosting C-O Bond Cleavage and Reverse Water-Gas Shift Activity via Enriched in-plane Sulfur Vacancies in Single-Layer Molybdenum Disulfide.
Angew Chem Int Ed Engl
January 2025
Chinese Academy of Sciences Dalian Institute of Chemical Physics, State Key Laboratory of Catalysis, 457 Zhongshan Road, 116023, Dalian, CHINA.
The reduction of CO2 to CO provides a promising approach to the production of valuable chemicals through CO2 utilization. However, challenges persist with the rapid deactivation and insufficient activity of catalysts. Herein, we developed a soft-hard dual-template method to synthesize layered MoS2 using inexpensive and scalable templates, enabling facile regulation of sulfur vacancies by controlling the number of layers.
View Article and Find Full Text PDFAnti-correlation of LacI association and dissociation rates observed in living cells.
Nat Commun
January 2025
Science for Life Laboratory, Department of Cell and Molecular Biology, Uppsala University, Uppsala, Sweden.
The rate at which transcription factors (TFs) bind their cognate sites has long been assumed to be limited by diffusion, and thus independent of binding site sequence. Here, we systematically test this assumption using cell-to-cell variability in gene expression as a window into the in vivo association and dissociation kinetics of the model transcription factor LacI. Using a stochastic model of the relationship between gene expression variability and binding kinetics, we performed single-cell gene expression measurements to infer association and dissociation rates for a set of 35 different LacI binding sites.
View Article and Find Full Text PDFSAMHD1 shapes deoxynucleotide triphosphate homeostasis by interconnecting the depletion and biosynthesis of different dNTPs.
Nat Commun
January 2025
Department of Biochemistry and Structural Biology, UT Health San Antonio, San Antonio, TX, USA.
SAMHD1 is a dNTPase that impedes replication of HIV-1 in myeloid cells and resting T lymphocytes. Here we elucidate the substrate activation mechanism of SAMHD1, which involves dNTP binding at allosteric sites and transient tetramerization. Our findings reveal that tetramerization alone is insufficient to promote dNTP hydrolysis; instead, the activation mechanism requires an inactive tetrameric intermediate with partially occupied allosteric sites.
View Article and Find Full Text PDFEnhanced sampling of protein conformational changes via true reaction coordinates from energy relaxation.
Nat Commun
January 2025
Center for Bioinformatics and Quantitative Biology, Richard and Loan Hill Department of Biomedical Engineering, The University of Illinois Chicago, 851 South Morgan Street, Chicago, IL, 60607, USA.
The bottleneck in enhanced sampling lies in finding collective variables that effectively accelerate protein conformational changes; true reaction coordinates that accurately predict the committor are the well-recognized optimal choice. However, identifying them requires unbiased natural reactive trajectories, which, paradoxically, require effective enhanced sampling. Using the generalized work functional method, we uncover that true reaction coordinates control both conformational changes and energy relaxation, enabling us to compute them from energy relaxation simulations.
View Article and Find Full Text PDFOn-Surface Synthesis and Characterization of Pentadecacene and Its Gold Complexes.
J Am Chem Soc
January 2025
Philipps-Universität Marburg, Fachbereich Chemie, Hans-Meerwein-Str. 4, 35032 Marburg, Germany.
Acenes are an important class of polycyclic aromatic hydrocarbons that have gained considerable attention from chemists, physicists, and material scientists, due to their exceptional potential for organic electronics. They serve as an ideal platform for studying the physical and chemical properties of sp carbon frameworks in the one-dimensional limit and also provide a fertile playground to explore magnetism in graphenic nanostructures due to their zigzag edge topology. While higher acenes up to tridecacene have been successfully generated by means of on-surface synthesis, it is imperative to extend their synthesis toward even longer homologues to comprehensively understand the evolution of their electronic ground state.
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