Ketone Skeletal Modification via a Metallaphotoredox-Catalyzed Deacylation and Acylation Strategy.

Herein, we describe a dual catalytic strategy that employs dihydroquinazolinones, derived from ketone analogs, as versatile intermediates for acylation via α C-C cleavage with 2-pyridyl esters, facilitating the efficient synthesis of a variety of ketones. The reaction accommodates a wide range of ketones and carboxylic acids, showing tolerance to various functional groups. The versatility of this synthetic technique is further highlighted through its application in the late-stage modification of pharmaceuticals and biologically active natural products.

Lipid-conjugated nucleoside monophosphate and monophosphonate prodrugs: A versatile drug delivery paradigm.

Integrating lipid conjugation strategies into the design of nucleoside monophosphate and monophosphonate prodrugs is a well-established approach for discovering potential therapeutics. The unique prodrug design endows nucleoside analogues with strong lipophilicity and structures resembling lysoglycerophospholipids, which improve cellular uptake, oral bioavailability and pharmacological activity. In addition, the metabolic stability, pharmacological activity, pharmacokinetic profiles and biodistribution of lipid prodrugs can be finely optimized by adding biostable caps, incorporating transporter-targeted groups, inserting stimulus-responsive bonds, adjusting chain lengths, and applying proper isosteric replacements.

Visible light-promoted difluoromethylthiolation of cycloalkanols by C-C bond cleavage.

A mild and general methodology for the difluoromethylthiolation of cycloalkanols has been developed by employing -difluoromethylthiophthalimide as the SCFH radical source, in combination with an acridinium-derived organo-photosensitizer, under redox-neutral conditions. This reaction protocol demonstrates high efficiency, scalability, and mild reaction conditions, thus presenting a green approach for the rapid synthesis of distal difluoromethylthiolated alkyl ketones that are challenging to be synthesized through alternative means.

The 2023 report of the Lancet Countdown on health and climate change: the imperative for a health-centred response in a world facing irreversible harms.

Unlabelled: The Countdown is an international research collaboration that independently monitors the evolving impacts of climate change on health, and the emerging health opportunities of climate action. In its eighth iteration, this 2023 report draws on the expertise of 114 scientists and health practitioners from 52 research institutions and UN agencies worldwide to provide its most comprehensive assessment yet. In 2022, the Countdown warned that people’s health is at the mercy of fossil fuels and stressed the transformative opportunity of jointly tackling the concurrent climate change, energy, cost-of-living, and health crises for human health and wellbeing.

Base-Mediated α--Difluoroalkenylations of Aldehydes and Ketones.

Herein, we present a base-mediated nucleophilic substitution reaction of α-trifluoromethylstyrenes with simple silyl enol ethers, enabling the efficient synthesis of carbonyl-substituted -difluoroalkenes. The merit of this protocol is exhibited by its mild reaction conditions, broad substrate scope, and scalable preparation. Notably, this method demonstrates its applicability for late-stage functionalization of structurally complex molecules.

The Polarizing Trend of Regional CO Emissions in China and Its Implications.

CO emissions are unevenly distributed both globally and regionally within nation-states. Given China's entrance into the new stage of economic development, an updated study on the largest CO emitter's domestic emission distribution is needed for effective and coordinated global CO mitigation planning. We discovered that domestic CO emissions in China are increasingly polarized for the 2007-2017 period.

The 2022 report of the Lancet Countdown on health and climate change: health at the mercy of fossil fuels.

Unlabelled: The 2022 report of the Countdown is published as the world confronts profound and concurrent systemic shocks. Countries and health systems continue to contend with the health, social, and economic impacts of the COVID-19 pandemic, while Russia’s invasion of Ukraine and a persistent fossil fuel overdependence has pushed the world into global energy and cost-of-living crises. As these crises unfold, climate change escalates unabated.

An Update Mini-Review on the Progress of Azanucleoside Analogues.

The development of structurally novel nucleoside analogues is an active area in medicinal chemistry, since these drugs have proven clinical efficacy for decades. Azanucleosides are nucleoside analogues in which the sugar moieties are composed of nitrogen-containing rings or chains. In recent years, many azanucleosides have demonstrated therapeutic potential.

Palladium-Catalyzed Regio- and Diastereoselective Olefinic C-H Difluoromethylthiolation at Room Temperature.

Herein, we developed palladium-catalyzed regio- and diastereoselective difluoromethylthiolation of acrylamides to form the -isomer product at room temperature. Using 8-aminoquinoline as a directing group, this protocol resulted in a high efficiency under mild reaction conditions and showed good functional group tolerances, which opens a novel synthetic methodology for accessing SCFH-containing skeletons. Moreover, mechanistic studies were conducted to obtain insights into the reaction mechanism, and post-functionalization of the product reactions was performed.

The 2021 report of the Lancet Countdown on health and climate change: code red for a healthy future.

Unlabelled: The Countdown is an international collaboration that independently monitors the health consequences of a changing climate. Publishing updated, new, and improved indicators each year, the Countdown represents the consensus of leading researchers from 43 academic institutions and UN agencies. The 44 indicators of this report expose an unabated rise in the health impacts of climate change and the current health consequences of the delayed and inconsistent response of countries around the globe—providing a clear imperative for accelerated action that puts the health of people and planet above all else.

Visible-Light Photoredox-Catalyzed Decarboxylative Alkylation of Heteroarenes Using Carboxylic Acids with Hydrogen Release.

Herein, we have developed visible-light photoredox-catalyzed decarboxylating carboxylic acids for alkylation of heteroarenes under mild conditions. The transformation occurred smoothly without the requirement of stoichiometric oxidants in the presence of 0.3 equiv of base, which benefited from the release of hydrogen (H) and carbon dioxide (CO).

Tracing the Uncertain Chinese Mercury Footprint within the Global Supply Chain Using a Stochastic, Nested Input-Output Model.

A detailed understanding of the mercury footprint at subnational entity levels can facilitate the implementation of the "Minamata Convention on Mercury", especially for China, the largest mercury emitter worldwide. Some provinces of China have more than 100 million people, with economic activities and energy consumption levels comparable to those of smaller G7 countries. We constructed a stochastic, nested multiregion input-output (MRIO) model, which regionalized the China block in the EXIOBASE global-scale MRIO table, to model the mercury footprint associated with global supply chains spanning China's regions and other countries.

Visible-Light Photoredox-Catalyzed Iminyl Radical Formation by N-H Cleavage with Hydrogen Release and Its Application in Synthesis of Isoquinolines.

An unprecedented visible-light photoredox-catalyzed iminyl radical formation by N-H cleavage with H release has been developed. Its application in the synthesis of various isoquinolines and related polyaromatics in high atom economy at ambient temperature by applying a photosensitizer, Acr-Mes ClO, and a new cobalt catalyst, Co(dmgH)(4-CONMePy)Cl is reported. Mechanistic investigations indicated that the generated iminyl radical initiates the cascade C-N/C-C bonds formation and the catalytic cycle occurs by a simultaneous oxidative as well as reductive quenching pathway.

Acceptorless Dehydrogenation of N-Heterocycles by Merging Visible-Light Photoredox Catalysis and Cobalt Catalysis.

Herein, the first acceptorless dehydrogenation of tetrahydroquinolines (THQs), indolines, and other related N-heterocycles, by merging visible-light photoredox catalysis and cobalt catalysis at ambient temperature, is described. The potential applications to organic transformations and hydrogen-storage materials are demonstrated. Primary mechanistic investigations indicate that the catalytic cycle occurs predominantly by an oxidative quenching pathway.

Redox-Divergent Hydrogen-Retentive or Hydrogen-Releasing Synthesis of 3,4-Dihydroisoquinolines or Isoquinolines.

A rare Ru-catalyzed highly selective synthesis of 3,4-dihydroisoquinolines or isoquinolines is accomplished via a redox-divergent hydrogen-retentive or hydrogen-releasing fashion. Notably, high cis-selectivity of 3,4-dihydroisoquinolines is achieved. Potential applications are shown by gram-scale reactions and very concise synthesis of N-containing polycyclic aromatic compounds.

Oxidant-free dehydrogenative coupling reactions via hydrogen evolution.

Oxidant-free dehydrogenative coupling reactions: Recently, coupling reactions have followed a novel strategy for the construction of C==C, C==N, C==P, and S==S bonds by dehydrogenation without using any extra oxidant, via H2 evolution. These breakthroughs inspire a new direction in the construction of chemical bonds, towards more sustainable, highly atom-economical, and environmentally benign synthetic methods.

Synthesis of fluorenone derivatives through Pd-catalyzed dehydrogenative cyclization.

Palladium-catalyzed dual C-H functionalization of benzophenones to form fluorenones by oxidative dehydrogenative cyclization is reported. This method provides a concise and effective route toward the synthesis of fluorenone derivatives, which shows outstanding functional group compatibility.

Straightforward synthesis of phenanthrenes from styrenes and arenes.

Semi-one-pot synthesis of phenanthrenes from styrenes and arenes was developed through cross-dehydrogenative coupling. A sequence of Heck-type coupling and photo-cyclization were involved and a variety of functionalities were tolerated. This method provides an effective and practical protocol towards the synthesis of substituted phenanthrenes.

N-Directing group assisted rhodium-catalyzed aryl C-H addition to aryl aldehydes.

Direct aryl C-H addition to aryl aldehydes to produce biaryl methanols was reported via Rh catalysis with an N-containing directing group. The method is highly atom-, step-, and redox-economic. The procedure is robust, reliable, and compatible with water and air.