We developed a tandem electrocatalyst for CO -to-CO conversion comprising the single Cu site co-coordinated with N and S anchored carbon matrix (Cu-S N ) and atomically dispersed Cu clusters (Cu ), denoted as Cu-S N /Cu . The as-prepared Cu-S N /Cu composite presents a 100 % Faradaic efficiency towards CO generation (FE ) at -0.65 V vs. RHE and high FE over 90 % from -0.55 to -0.75 V, outperforming the analogues with Cu-N (FE only 54 % at -0.7 V) and Cu-S N (FE 70 % at -0.7 V) configurations. The unsymmetrical Cu-S N atomic interface in the carbon basal plane possesses an optimized binding energy for the key intermediate *COOH compared with Cu-N site. At the same time, the adjacent Cu effectively promotes the protonation of *CO by accelerating water dissociation and offering *H to the Cu-S N active sites. This work provides a tandem strategy for facilitating proton-coupled electron transfer over the atomic-level catalytic sites.
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http://dx.doi.org/10.1002/anie.202109579 | DOI Listing |
Health Aff (Millwood)
January 2025
David J. Meyers, Brown University.
Under the current Medicare Advantage (MA) risk-adjustment system, plans are incentivized to report diagnosis codes on enrollees' medical claims reflecting additional and more severe health conditions to increase enrollees' risk scores and corresponding plan payments. To improve the integrity of risk adjustment, researchers have proposed four alternative methods to construct risk scores: calculate Hierarchical Condition Categories (HCC) scores excluding diagnosis codes from health risk assessments and chart reviews, calculate HCC scores excluding diagnosis codes most subject to score inflation, use pharmaceutical claims alone, and use self-reported survey responses alone or in combination with diagnosis codes. Using 2016-19 medical and pharmaceutical claims linked to Consumer Assessment of Healthcare Providers and Systems survey responses from 151,432 MA enrollees, we compared the predictive accuracy of each alternative strategy with the standard HCC approach.
View Article and Find Full Text PDFAIDS
January 2025
Hypertension in Africa Research Team (HART), North-West University, Potchefstroom, South Africa.
HIV-1 remains a global challenge, especially in high-prevalence areas like South Africa. This study explores the relationship between inflammation and metabolism in people with HIV, focusing on immune markers and the tryptophan-kynurenine (Trp-Kyn) pathway. We examined immune markers (hsCRP, suPAR, IL-6, NGAL, and sCD163) and Trp-Kyn metabolites (QUIN, Trp, Kyn, Trp/Kyn ratio, and kynurenic acid) in n = 69 treatment-naive South African people with HIV.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
EPFL: Ecole Polytechnique Federale de Lausanne, Institute of Chemical Sciences and Engineering, EPFL-ISIC-LSCI, BCH 3305, 1015, Lausanne, SWITZERLAND.
Artificial metalloenzymes (ArMs) enable the integration of abiotic cofactors within a native protein scaffold, allowing for non-natural catalytic activities. Previous ArMs, however, have primarily relied on single cofactor systems, limiting them to only one catalytic function. Here we present an approach to construct ArMs embedding two catalytic cofactors based on the biotin-streptavidin technology.
View Article and Find Full Text PDFChem Sci
December 2024
Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials, Ministry of Education Key Laboratory for the Synthesis and Application of Organic Functional Molecules, College of Chemistry and Chemical Engineering, Hubei University Wuhan 430062 P. R. China
The prevalence of naphthalene compounds in biologically active natural products, organic ligands and approved drugs has motivated investigators to develop efficient strategies for their selective synthesis. C-H functionalization of naphthalene has been frequently deployed, but mainly involves two-component reactions, while multiple-component C-H functionalization for the synthesis of naphthalene compounds has thus far proven elusive. Herein, we disclose a versatile three-component protocol for the modular synthesis of multifunctional naphthalenes from readily available simple naphthalenes, olefins and alkyl bromides P(iii)-assisted ruthenium-catalyzed remote C-H functionalization.
View Article and Find Full Text PDFEnviron Sci (Camb)
December 2024
Department of Computer Science, Virginia Tech Blacksburg VA 24061 USA
The persistence of pharmaceuticals and personal care products (PPCPs) through wastewater treatment and resulting contamination of aquatic environments and drinking water is a pervasive concern, necessitating means of identifying effective treatment strategies for PPCP removal. In this study, we employed machine learning (ML) models to classify 149 PPCPs based on their chemical properties and predict their removal wastewater and water reuse treatment trains. We evaluated two distinct clustering approaches: C1 (clustering based on the most efficient individual treatment process) and C2 (clustering based on the removal pattern of PPCPs across treatments).
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