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Position-specific isotope effects during alkaline hydrolysis of 2,4-dinitroanisole resolved by compound-specific isotope analysis, 13 C NMR, and density-functional theory
Compound-specific isotope analysis (CSIA), position-specific isotope analysis (PSIA), and computational modeling (e.g., quantum mechanical models; reactive-transport models) are increasingly being used to monitor and predict biotic and abiotic transformations of organic contaminants in the field. However, identifying the isotope effect(s) associated with a specific transformation remains challenging in many cases. We describe and interpret the position-specific isotope effects of C and N associated with a SN 2 Ar reaction mechanism by a combination of CSIA and PSIA using quantitative 13 C nuclear magnetic resonance spectrometry, and density-functional theory, using 2,4-dinitroanisole (DNAN) as a model compound. The position-specific 13 C enrichment factor of O–C 1 bond at the methoxy group attachment site (ε C1 ) was found to be approximately -41‰, a diagnostic value for transformation of DNAN to its reaction products 2,4-dinitrophenol and methanol. Theoretical kinetic isotope effects calculated for DNAN isotopologues agreed well with the position-specific isotope effects measured by CSIA and PSIA. This combination of measurements and theoretical predictions demonstrates a useful tool for evaluating degradation efficiencies and/or mechanisms of organic contaminants and may promote new and improved applications of isotope analysis in laboratory and field investigations.
Uranium(VI) hydrolysis up to 250 °C and its geological implications
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Local interactions with the Glu166 base and the conformation of an active site loop play key roles in carbapenem hydrolysis by the KPC-2 β-lactamase
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Conformational flexibility in carbapenem hydrolysis drives substrate specificity of the class D carb
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Flash hydrolysis of yeast (Saccharomyces cerevisiae) for protein recovery
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Insights into Ubiquitin Product Release in Hydrolysis Catalyzed by the Bacterial Deubiquitinase SdeA
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Surface Sn(IV) Hydrolysis Improves Inorganic Sn–Pb Perovskite Solar Cells
Cesium tin-lead (Sn-Pb) perovskites are exceptional for their combined capabilities in unlocking ideal bandgaps for solar cells and mitigating the stability issue faced by their hybrid organic-inorganic counterparts. But the development of high-performance solar cells using these materials is retarded by their inherent high density of detrimental Sn(IV) defects. Herein, we demonstrate a sequential surface treatment method, which entails a Sn(II) halide treatment to displace the buried Sn(IV) ions underneath the film surface, followed by a H 2 O treatment to hydrolyze the displaced Sn(IV) ions. The surface treatment induces chemical and microstructural reconstructions that significantly improve the optoelectronic properties and stability of perovskites. As a result, a power conversion efficiency of 16.79% and a T 90 stability of 958 h are achieved, topping all previously reported performance parameters for inorganic Sn-Pb PSCs. This achievement further shortens the performance gap between all-inorganic and hybrid organic- inorganic Sn-Pb PSCs with sub-1.4 eV bandgaps.
Polyene-Free Photoluminescent Polymers via Hydrothermal Hydrolysis of Polyacrylonitrile in Neutral Water
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