Acceleration of the semi-hydrogenation of alkynes over an N-doped porous carbon sphere-confined ultrafine PdCu bimetallic nanoparticle catalyst.

Selective hydrogenation of alkynes to obtain alkenes is a key reaction in petrochemical and fine chemical industries. However, the development of stable and highly selective catalysts with uniformly dispersed active sites is still immensely challenging for the semi-hydrogenation of alkynes. In this study, N-doped porous carbon nanospheres (NPCNs) were synthesized by the nanoemulsion self-assembly and subsequently carbonization method. Ultrafine PdCu bimetallic nanoparticles (NPs) were uniformly dispersed and immobilized on NPCNs. The obtained PdCu/NPCNs catalyst exhibited an open framework and abundant active sites originating from ultrafine PdCu NPs. In the semi-hydrogenation of alkynes, the PdCu/NPCNs catalyst exhibited a remarkable performance and stability, outperforming most of the classical catalysts. The excellent performance was related to the introduction of a secondary metal Cu, which can regulate the electronic state of Pd active sites to further enhance the hydrogenation activity and selectivity. Hence, the facile approach reported herein may be useful for constructing highly dispersed bimetallic NP-based catalysts for selective hydrogenation of alkynes in the petrochemical industry.

Platinum clusters anchored on sulfur-doped ordered mesoporous carbon for chemoselective hydrogenation of halogenated nitroarenes.

Chemoselective hydrogenation of unsaturated organic compounds is a significant research topic in the catalysis field. Herein, a sulfur-doped ordered mesoporous carbon (SMC) material was prepared to anchor ultrafine platinum (Pt) clusters for the chemoselective hydrogenation of halogenated nitroarenes. The confinement effect of the ordered pores and the strong metal-support interaction caused by Pt clusters and sulfur atoms, efficiently suppress the aggregation and regulate the electronic states of the ultrafine Pt clusters. Thus, the hydrogenation of parachloronitrobenzene (p-CNB) shows high selectivity catalyzed by the ultrafine Pt clusters with electron-rich states. Meanwhile, the catalytic performance of the hydrogenation reaction catalyzed by Pt/SMC is capable of being maintained after at least 5 cycles, and the catalytic universality can also be applied to different halogenated nitroarenes hydrogenation. Therefore, this study may promote the research into the construction of noble metal-based catalysts for chemoselective hydrogenation reactions in green and sustainable chemical processes.

Facile preparation of ultrafine Pd nanoparticles anchored on covalent triazine frameworks catalysts for efficient N-alkylation.

The fabrication of stable and efficient catalysts for green and economic catalytic transformation is significant. Here, highly stable covalent triazine frameworks (CTF-1) were used as the supporting material for anchoring ultrafine Pd nanoparticles (NPs) via a facile impregnation process and a one-pot calcination-reduction strategy. The widespread dispersion of ultrafine Pd NPs was a result of the abundant high nitrogen-content triazine groups of CTF-1 that endowed the catalyst Pd@CTF-1 with high catalytic activity. The catalytic performance of Pd@CTF-1 was demonstrated by the one-pot N-alkylation of benzaldehyde with aniline (or nitrobenzene) under mild reaction conditions, and Pd@CTF-1 exhibited a wide range of general applicability for N-alkylation reactions. The reaction mechanism for the N-alkylation reaction was also studied in detail. In addition, the Pd@CTF-1 catalyst exhibited high thermal and chemical stability, maintaining good catalytic efficiency after multiple reaction cycles. This study provides new insights for the fabrication of organic supporting materials with highly dispersed active catalytic sites that can lead to excellent catalytic performance for efficient, economical, and green reactions.

Construction of a sandwich-like UiO-66-NH2@Pt@mSiO2 catalyst for one-pot cascade reductive amination of nitrobenzene with benzaldehyde.

Heterogeneous noble metal-based catalysts with stable, precise structures and high catalytic performance are of great research interest for sustainable catalysis. Herein, we designed the novel sandwich-like metal-organic-framework composite nanocatalyst UiO-66-NH2@Pt@mSiO2 using UiO-66-NH2@Pt as the core, and mesoporous SiO2 as the shell. The obtained UiO-66-NH2@Pt@mSiO2 catalyst shows a well-defined structure and interface, and the protection of the mSiO2 shell can efficiently prevent Pt NPs from aggregating and leaching in the reaction process. In the one-pot cascade reaction of nitroarenes and aromatic aldehydes to secondary amines, UiO-66-NH2@Pt@mSiO2 shows excellent catalytic performance due to acid catalytic sites provided by UiO-66-NH2 and Pt hydrogenation catalytic sites. Furthermore, the porous structure of the UiO-66-NH2@Pt@mSiO2 catalyst also enhances reactant diffusion and improves the reaction efficiency. This work provides a new avenue to meticulously design well-defined nanocatalysts with superior catalytic performance and stability for challenging reactions.