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Role of Dihydride and Dihydrogen Complexes in Hydrogen Evolution Reaction on Single-Atom Catalysts.

Published in Journal of the American Chemical Society

The hydrogen evolution reaction (HER) has a key role in electrochemical water splitting. Recently a lot of attention has been dedicated to HER from single atom catalysts (SACs). The activity of SACs in HER is usually rationalized or predicted using the original model proposed by Nørskov where the free energy of a H atom adsorbed on an extended meta...

Direct SARS-CoV-2 Nucleic Acid Detection by Y-Shaped DNA Dual-Probe Transistor Assay.

Published in Journal of the American Chemical Society

Rapid screening of infected individuals from a large population is an effective means in epidemiology, especially to contain outbreaks such as COVID-19. The gold standard assays for COVID-19 diagnostics are mainly based on the reverse transcription polymerase chain reaction, which mismatches the requirements for wide-population screening due to tim...

Complex Polyheterocycles and the Stereochemical Reassignment of Pileamartine A via Aza-Heck Triggered Aryl C–H Functiona...

Published in Journal of the American Chemical Society

Structurally complex benzo- and spiro-fused N-polyheterocycles can be accessed via intramolecular Pd(0)-catalyzed alkene 1,2-aminoarylation reactions. The method uses N -(pentafluorobenzoyloxy)carbamates as the initiating motif, and this allows aza-Heck-type alkene amino-palladation in advance of C–H palladation of the aromatic component. The chemi...

Confinement-Controlled, Either syn- or anti-Selective Catalytic Asymmetric Mukaiyama Aldolizations of Propionaldehyde En...

Published in Journal of the American Chemical Society

Protected aldols (i.e., true aldols derived from aldehydes) with either syn- or anti- stereochemistry are versatile intermediates in many oligopropionate syntheses. Traditional stereoselective approaches to such aldols typically require several nonstrategic operations. Here we report two highly enantioselective and diastereoselective catalytic Muka...

The Ascent of Alkyne Metathesis to Strategy-Level Status

Published in Journal of the American Chemical Society

For numerous enabling features and strategic virtues, contemporary alkyne metathesis is increasingly recognized as a formidable synthetic tool. Central to this development was the remarkable evolution of the catalysts during the past decades. Molybdenum alkylidynes carrying (tripodal) silanolate ligands currently set the standards; their functional...

Probing Bioelectronic Connections using Streptavidin Molecules with Modified Valency

Published in Journal of the American Chemical Society

Interlayer Interactions as Design Tool for Large-Pore COFs

Published in Journal of the American Chemical Society

Covalent organic frameworks (COFs) with a pore size beyond 5 nm are still rarely seen in this emerging field. Besides obvious complications such as the elaborated synthesis of large linkers with sufficient solubility, more subtle challenges regarding large-pore COF synthesis, including pore occlusion and collapse, prevail. Here we present two isore...

The Unexplored Importance of Fleeting Chiral Intermediates in Enzyme-Catalyzed Reactions

Published in Journal of the American Chemical Society

Decades of extensive research efforts by biochemists, organic chemists, and protein engineers have led to an understanding of the basic mechanisms of essentially all known types of enzymes, but in a formidable number of cases an essential aspect has been overlooked. The occurrence of short-lived chiral intermediates formed by symmetry-breaking of p...

Trivalent Subunit Vaccine Candidates for COVID-19 and Their Delivery Devices

Published in Journal of the American Chemical Society

The COVID-19 pandemic highlights the need for platform technologies enabling rapid development of vaccines for emerging viral diseases. The current vaccines target the SARS-CoV-2 spike (S) protein and thus far have shown tremendous efficacy. However, the need for cold-chain distribution, a prime-boost administration schedule, and the emergence of v...

Molecular Understanding of the Catalytic Consequence of Ketene Intermediates under Confinement

Published in Journal of the American Chemical Society

Neutral ketene is a crucial intermediate during zeolite carbonylation reactions. In this work, the roles of ketene and its derivates (viz., acylium ion and surface acetyl) associated with direct C–C bond coupling during the carbonylation reaction have been theoretically investigated under realistic reaction conditions and further validated by synch...