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1.
J Org Chem ; 89(13): 9654-9660, 2024 Jul 05.
Article in English | MEDLINE | ID: mdl-38900965

ABSTRACT

We report the first example of copper-catalyzed α-alkylation of acetamides with alcohols via a borrowing hydrogen strategy. Catalyzed by the in situ-generated copper particles, acetamides and various substituted benzyl or alkyl alcohols were transformed into functionalized amides in good yields with excellent selectivity. Compared with previous work, this process is simple using commercially available Cu(OAc)2 as a precatalyst, without an additional ligand or a metal complex, and easier. Mechanistic studies revealed that aldehyde and α,ß-unsaturated amides were the intermediates of this reaction and also disclosed the role of copper in alcohol dehydrogenation and C═C bond hydrogenation.

2.
Adv Mater ; : e2311355, 2024 Feb 20.
Article in English | MEDLINE | ID: mdl-38374727

ABSTRACT

Liquid organic hydrogen carriers (LOHCs) have gained significant attention for large-scale hydrogen storage due to their remarkable gravimetric hydrogen storage capacity (HSC) and compatibility with existing oil and gas transportation networks for long-distance transport. However, the practical application of reversible LOHC systems has been constrained by the intrinsic thermodynamic properties of hydrogen carriers and the performances of associated catalysts in the (de)hydrogenation cycles. To overcome these challenges, thermodynamically favored carriers, high-performance catalysts, and catalytic procedures need to be developed. Here, significant advances in recent years have been summarized, primarily centered on regular LOHC systems catalyzed by homogeneous and heterogeneous catalysts, including dehydrogenative aromatization of cycloalkanes to arenes and N-heterocyclics to N-heteroarenes, as well as reverse hydrogenation processes. Furthermore, with the development of metal complexes for dehydrogenative coupling, a new family of reversible LOHC systems based on alcohols is described that can release H2 under relatively mild conditions. Finally, views on the next steps and challenges in the field of LOHC technology are provided, emphasizing new resources for low-cost hydrogen carriers, high-performance catalysts, catalytic technologies, and application scenarios.

3.
Org Lett ; 25(17): 3066-3071, 2023 May 05.
Article in English | MEDLINE | ID: mdl-37088958

ABSTRACT

We report the first heterogeneous catalytic hydrogenation of N-substituted imides and polyimide to generate primary amines, diols, and lactones. Catalyzed by Ag/TiO2, this reaction proceeded smoothly in high yields and selectivities for N-alkyl and N-aryl phthalimides and N-aryl succinimides, which also had activity for the degradation of waste polyimide plastics. In contrast to the typical Gabriel process, this reaction does not need any toxic reagent, and the byproducts are also very useful. Recycling experiments showed that the catalyst Ag/TiO2 could be easily recovered without a decrease in catalytic activity.

4.
J Hazard Mater ; 407: 124761, 2021 04 05.
Article in English | MEDLINE | ID: mdl-33316687

ABSTRACT

Consecutive microwave sintering is a method proposed in this study to dispose soil contaminated by Sr during a nuclear accident by rapidly solidifying the contaminated soil. The results show that soil contaminated with 20 wt% SrSO4 and 30 wt% SrSO4 can be completely solidified by microwave sintering at 1100-1200 and 1300 â„ƒ, respectively, for 30 min. Sr was found to be cured into slawsonite (SrAl2Si2O8) and glass structures. Moreover, soil sintered at 1300 â„ƒ has large cured solubility (30 wt.%), good uniformity, and excellent hardness (6.9-7.2 GPa) and chemical durability (below 1.46 × 10-5 g m-2 d-1 at 28 d). Thus, consecutive microwave sintering technology may provide a new method for treating Sr-contaminated soil in case of a nuclear accident emergency.

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