Energy input plays a crucial role in the assembling of matter. In our present study, we utilize EDC as a chemical fuel to drive the molecular assembling of POR-COOH. POR-COOH will react with EDC to generate the intermediate POR-COOEDC first, which was well-solvated by solvent molecules. During the subsequent hydrolysis process, EDU and oversaturated POR-COOH molecules at high energy states will be formed and thus allowed the self-assembling of POR-COOH into 2D nanosheets. This chemical energy assisted assembling process could be performed not only under mild conditions with high spatial accuracy but also with high selectivity in complex environments.
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http://dx.doi.org/10.1039/d2sc06621a | DOI Listing |
Proc Natl Acad Sci U S A
January 2025
State Key Laboratory of Superhard Materials, College of Physics, Jilin University, Changchun 130012, China.
The abrupt drop of resistance to zero at a critical temperature is a key signature of the current paradigm of the metal-superconductor transition. However, the emergence of an intermediate bosonic insulating state characterized by a resistance peak preceding the onset of the superconducting transition has challenged this traditional understanding. Notably, this phenomenon has been predominantly observed in disordered or chemically doped low-dimensional systems, raising intriguing questions about the generality of the effect and its underlying fundamental physics.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
January 2025
Department of Chemistry, Chemical Theory Center, University of Minnesota, Minneapolis, MN 55455-0431.
Multiconfiguration pair-density functional theory (MC-PDFT) was proposed a decade ago, but it is still in the early stage of density functional development. MC-PDFT uses functionals that are called on-top functionals; they depend on the density and the on-top pair density. Most MC-PDFT calculations to date have been unoptimized translations of generalized gradient approximations (GGAs) of Kohn-Sham density functional theory (KS-DFT).
View Article and Find Full Text PDFProc Natl Acad Sci U S A
January 2025
Department of Chemistry, State Key Laboratory of Molecular Engineering of Polymers, College of Chemistry and Materials, iChem (Collaborative Innovation Center of Chemistry for Energy Materials), Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200433, China.
Emulsion interface engineering has been widely employed for the synthesis of nanomaterials with various morphologies. However, the instability of the liquid-liquid interface and uncertain interfacial interactions impose significant limitations on controllable fabrications. Here, we developed a liquid-nano-liquid interface-oriented anisotropic encapsulation strategy for fabricating asymmetric nanohybrids.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
January 2025
Department of Mechanical and Aerospace Engineering, Carleton University, Ottawa, ON K1S 5B6, Canada.
Limiting climate change to targets enshrined in the Paris Agreement will require both deep decarbonization of the energy system and the deployment of carbon dioxide removal at potentially large scale (gigatons of annual removal). Nations are pursuing direct air capture to compensate for inertia in the expansion of low-carbon energy systems, decarbonize hard-to-abate sectors, and address legacy emissions. Global assessments of this technology have failed to integrate factors that affect net capture and removal cost, including ambient conditions like temperature and humidity, as well as emission factors of electricity and natural gas systems.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
January 2025
California Institute for Quantitative Biosciences, University of California, Berkeley, CA 94720.
Polysaccharide monooxygenase (PMO) catalysis involves the chemically difficult hydroxylation of unactivated C-H bonds in carbohydrates. The reaction requires reducing equivalents and will utilize either oxygen or hydrogen peroxide as a cosubstrate. Two key mechanistic questions are addressed here: 1) How does the enzyme regulate the timely and tightly controlled electron delivery to the mononuclear copper active site, especially when bound substrate occludes the active site? and 2) How does this electron delivery differ when utilizing oxygen or hydrogen peroxide as a cosubstrate? Using a computational approach, potential paths of electron transfer (ET) to the active site copper ion were identified in a representative AA9 family PMO from (PMO9E).
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