Synthesis of Ordered Mesoporous Molecular Sieve-Supported Cobalt Catalyst via Organometallic Complexation for Propane Non-Oxidative Dehydrogenation.

Co-based catalysts have shown great promise for propane dehydrogenation (PDH) reactions due to their merits of environmental friendliness and low cost. In this study, ordered mesoporous molecular sieve-supported CoOx species (CoOx/Al-SBA-15 catalyst) were prepared by one-step organometallic complexation. The catalysts show worm-like morphology with regular straight-through mesoporous pores and high external specific surface area. These typical features can substantially enhance the dispersion of CoOx species and mass transfer of reactants and products. Compared with the conventional impregnation method, the 10CSOC (10 wt.% Co/Al-SBA-15 prepared by the organometallic complexation method) sample presents a smaller CoOx size and higher Co2+/Co3+ ratio. When applied to PDH reaction, the 10CSOC delivers higher propane conversion and propylene selectivity. Under the optimal conditions (625 °C and 4500 h-1), 10CSOC achieves high propane conversion (43%) and propylene selectivity (83%). This is attributed to the smaller and better dispersion of CoOx nanoparticles, more suitable acid properties, and higher content of Co2+ species. This work paves the way for the rational design of high-performance catalysts for industrially important reactions.

Dual-Active-Sites Single-Atom Catalysts for Advanced Applications.

Dual-Active-Sites Single-Atom catalysts (DASs SACs) are not only the improvement of SACs but also the expansion of dual-atom catalysts. The DASs SACs contains dual active sites, one of which is a single atomic active site, and the other active site can be a single atom or other type of active site, endowing DASs SACs with excellent catalytic performance and a wide range of applications. The DASs SACs are categorized into seven types, including the neighboring mono metallic DASs SACs, bonded DASs SACs, non-bonded DASs SACs, bridged DASs SACs, asymmetric DASs SACs, metal and nonmetal combined DASs SACs and space separated DASs SACs. Based on the above classification, the general methods for the preparation of DASs SACs are comprehensively described, especially their structural characteristics are discussed in detail. Meanwhile, the in-depth assessments of DASs SACs for variety applications including electrocatalysis, thermocatalysis and photocatalysis are provided, as well as their unique catalytic mechanism are addressed. Moreover, the prospects and challenges for DASs SACs and related applications are highlighted. The authors believe the great expectations for DASs SACs, and this review will provide novel conceptual and methodological perspectives and exciting opportunities for further development and application of DASs SACs.

Isolated Single-Atom Ni-N5 Catalytic Site in Hollow Porous Carbon Capsules for Efficient Lithium-Sulfur Batteries.

Lithium-sulfur (Li-S) batteries suffer from multiple complex and often interwoven issues, such as the low electronic conductivity of sulfur and Li2S/Li2S2, shuttle effect, and sluggish electrochemical kinetics of lithium polysulfides (LiPSs). Guided by theoretical calculations, a multifunctional catalyst of isolated single-atom nickel in an optimal Ni-N5 active moiety incorporated in hollow nitrogen-doped porous carbon (Ni-N5/HNPC) is constructed and acts as an ideal host for a sulfur cathode. The host improved electrical conductivity, enhanced physical-chemical dual restricting capability toward LiPSs, and, more importantly, boosted the redox reaction kinetics by the Ni-N5 active moiety. Therefore, the Ni-N5/HNPC/S cathode exhibits superior rate performance, long-term cycling stability, and good areal capacity at high sulfur loading. This work highlights the important role of the coordination number of active centers in single-atom catalysts and provides a strategy to design a hollow nanoarchitecture with single-atom active sites for high-performance Li-S batteries.

ZIF-derived porous carbon supported Pd nanoparticles within mesoporous silica shells: sintering- and leaching-resistant core-shell nanocatalysts.

A facile strategy to prepare sintering- and leaching-resistant core-shell nanocatalysts is reported. ZIF-derived porous carbon supported Pd nanoparticles are coated with a mesoporous silica shell, preventing Pd nanoparticles from sintering at high temperature and leaching in a catalytic process. This nanocatalyst exhibits excellent catalytic activity and recyclability for the oxidation of benzyl alcohol.