To increase the power of X-ray crystallography to determine not only the structures but also the motions of biomolecules, we developed methods to address two classic crystallographic problems: putting electron density maps on the absolute scale of e(-)/Å(3) and calculating the noise at every point in the map. We find that noise varies with position and is often six to eight times lower than thresholds currently used in model building. Analyzing the rescaled electron density maps from 485 representative proteins revealed unmodeled conformations above the estimated noise for 45% of side chains and a previously hidden, low-occupancy inhibitor of HIV capsid protein. Comparing the electron density maps in the free and nucleotide-bound structures of three human protein kinases suggested that substrate binding perturbs distinct intrinsic allosteric networks that link the active site to surfaces that recognize regulatory proteins. These results illustrate general approaches to identify and analyze alternative conformations, low-occupancy small molecules, solvent distributions, communication pathways, and protein motions.
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http://dx.doi.org/10.1073/pnas.1302823110 | DOI Listing |
Chemistry
January 2025
China University of Geosciences, Faculty of Materials Science and Chemistry, CHINA.
Pd cocatalysts show great potential for the photocatalytic production of H2O2. However, the catalytic efficiency of Pd cocatalyst is limited due to the strong adsorption of O2, which promotes O-O bond cleavage and thus reduces selectivity for the two-electron O2 reduction reaction. Considering that adjusting the electron density of Pd can predominately optimize Pd-Oads bond strength, in this work, electron-rich Pd sites are constructed by introducing Bi2Se3 middle layer between Pd cocatalysts and (010) facet of BiVO4 using an in-situ selenization strategy.
View Article and Find Full Text PDFJ Mol Model
January 2025
Departamento de Investigación y Desarrollo, ConsultoresAcademicos SpA, Moneda 1137, 8340457, Santiago, Chile.
Context: This study meticulously examines the criteria for assigning electron rearrangements along the intrinsic reaction coordinate (IRC) leading to bond formation and breaking processes during the pyrolytic isomerization of cubane (CUB) to 1,3,5,7-cyclooctatetraene (COT) from both thermochemical and bonding perspectives. Notably, no cusp-type function was detected in the initial thermal conversion step of CUB to bicyclo[4.2.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
State Key Laboratory of Fine Chemicals, Laboratory of Advanced Materials and Catalytic Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China.
The industrial advancement of downstream products resulting from the directed hydrogenation of maleic anhydride is hindered by the limitations related to the activity and stability of catalysts. The development of nonprecious metal intermetallic compounds, in which active sites are adjustable in the local structures and electronic properties embedded within a distinct framework, holds immense potential in enhancing catalytic efficacy and stability. Herein, we report that nickel-based silicides catalysts, RNiSi (R = Ca, La, and Y), afford high efficiency in the selective hydrogenation of maleic anhydride.
View Article and Find Full Text PDFACS Nano
January 2025
School of Information Science and Technology and Department of Optical Science and Engineering and Key Laboratory of Micro and Nano Photonic Structures (MOE), Fudan University, Shanghai 200433, China.
The formation of large polarons resulting from the Fröhlich coupling of photogenerated carriers with the polarized crystal lattice is considered crucial in shaping the outstanding optoelectronic properties in hybrid organic-inorganic perovskite crystals. Until now, the initial polaron dynamics after photoexcitation have remained elusive in the hybrid perovskite system. Here, based on the terahertz time-domain spectroscopy and optical-pump terahertz probe, we access the nature of interplay between photoexcited unbound charge carriers and optical phonons in MAPbBr within the initial 5 ps after excitation and have demonstrated the simultaneous existence of both electron- and hole-polarons, together with the photogenerated carrier dynamic process.
View Article and Find Full Text PDFACS Nano
January 2025
Department of Physics and Astronomy & Nebraska Center for Materials and Nanoscience, University of Nebraska, Lincoln, Nebraska 68588-0299, United States.
A spin valve represents a well-established device concept in magnetic memory technologies, whose functionality is determined by electron transmission, controlled by the relative alignment of magnetic moments of the two ferromagnetic layers. Recently, the advent of valleytronics has conceptualized a valley spin valve (VSV)─a device that utilizes the valley degree of freedom and spin-valley locking to achieve a similar valve effect without relying on magnetism. In this study, we propose a nonvolatile VSV (-VSV) based on a two-dimensional (2D) ferroelectric semiconductor where resistance of -VSV is controlled by a ferroelectric domain wall between two uniformly polarized domains.
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