Tandem Oxidation Activation of Carbon for Enhanced Electrochemical Synthesis of H2O2: Unveiling the Role of Quinone Groups and Their Operando Derivatives.

Oxygen-doped carbon materials show great promise to catalyze two-electron oxygen reduction reaction (2e-ORR) for electrochemical synthesis of hydrogen peroxide (H2O2), but the identification of the active sites is the subject of ongoing debate. In this study, a tandem oxidation strategy is developed to activate carbon black for achieving highly efficient electrochemical synthesis of H2O2. Acetylene black (AB) is processed with O2 plasma and subsequent electrochemical oxidation, resulting in a remarkable selectivity of >96% over a wide potential range, and a record-setting high yield of >10 mol gcat -1 h-1 with good durability in gas diffusion electrode. Comprehensive characterizations and calculations revealed that the presence of abundant C═O groups at the edge sites positively correlated to and accounted for the excellent 2e-ORR performance. Notably, the edge hydroquinone group formed from quinone under operando conditions, which is overlooked in previous research, is identified as the most active catalytic site.

Synthesis and Analysis of Natural-Product-Like Macrocycles by Tandem Oxidation/Oxa-Conjugate Addition Reactions.

As traditional small-molecule drug discovery programs focus on a relatively narrow range of chemical space, most human proteins are viewed as unreachable targets. Consequently, there is a strong interest in expanding the chemical space in drug discovery beyond traditional small molecules. Here, a strategy for the preparation of a broad natural-product-like macrocyclic library by using the tandem allylic oxidation/oxa-conjugate addition and macrocyclization reactions is reported. Cheminformatic analyses demonstrate that this tetrahydropyran-containing macrocyclic library shows a significant overlap with natural products in the chemical space. This approach can be used for designing libraries that may probe more deeply into natural-product-like space.

Superparamagnetic Fe(OH)3@Fe3O4 Nanoparticles: An Efficient and Recoverable Catalyst for Tandem Oxidative Amidation of Alcohols with Amine Hydrochloride Salts.

Magnetic Fe(OH)3@Fe3O4 nanoparticles were successfully prepared and characterized. This magnetic nanocomposite was employed as an efficient, reusable, and environmentally benign heterogeneous catalyst for the direct amidation of alcohols with amine hydrochloride salts. Several derivatives of primary, secondary and tertiary amides were synthesized in moderate to good yields in the presence of this catalytic system. The catalyst was successfully recycled and reused up to six times without significant loss of its catalytic activity.

Green oxidations: titanium dioxide induced tandem oxidation coupling reactions.

The application of titanium dioxide as an oxidant in tandem oxidation type processes is described. Under microwave irradiation, quinoxalines have been synthesized in good yields from the corresponding alpha-hydroxyketones.