Local structural environment of single-atom catalysts
Zheng Chen,
Lili Han
Abstract:Single-atom catalysts (SACs) provide opportunities for bridging the gap between homogeneous and heterogeneous catalysis, facilitating the precise structure identification of the catalytic active sites, and offering new opportunities for interpreting...
“…In the last decade, single-atom catalysts (SACs) have received wide research interest because of their unique electronic effects, the uniform distribution of active centers, and the highest atom use efficiency. [16][17][18] Numerous results have suggested that SACs provide identifiable active sites and a perfect model for both experimental and theoretical studies. 19 In the case of electrocatalysts for ORR, the catalytic efficiency largely depends on two factors, i.e.…”
Atomically iron-nitrogen coordinated active sites on carbon (Fe-N-C) are considered to be absorbing materials to alternate Pt-based catalysts for the electrochemical oxygen reduction reaction (ORR). However, Fe-N-C catalysts suffer from...
“…In the last decade, single-atom catalysts (SACs) have received wide research interest because of their unique electronic effects, the uniform distribution of active centers, and the highest atom use efficiency. [16][17][18] Numerous results have suggested that SACs provide identifiable active sites and a perfect model for both experimental and theoretical studies. 19 In the case of electrocatalysts for ORR, the catalytic efficiency largely depends on two factors, i.e.…”
Atomically iron-nitrogen coordinated active sites on carbon (Fe-N-C) are considered to be absorbing materials to alternate Pt-based catalysts for the electrochemical oxygen reduction reaction (ORR). However, Fe-N-C catalysts suffer from...
“…Single-atom catalysts (SACs) have attracted considerable attention in recent years due to their ability to maximize atom utilization, exhibit distinctive electronic properties, and provide uniform and adjustable active sites. 14–30 SACs’ well-defined active sites also serve as an ideal model to gain comprehensive insights into catalytic reaction mechanisms at an atomic scale. 24–27 From a coordination chemistry perspective, the catalytic activity of SACs is closely related to their local coordination microenvironment.…”
The Zn–N2P site, engineered with optimal electron density, demonstrates superior performance and enhanced reaction kinetics in the intramolecular hydroamination of o-alkynylaniline, outperforming current heterogeneous transition metal catalysts.
Mg and its related solid base catalysts have always been thought of with weak or medium basicity. Herein, we present the synthesis of Mg single atom catalyst (Mg1/NPC) with strong basicity by tuning its coordination environment, which shows unusual activity in strong‐base‐catalyzed transesterification reaction. Mg1/NPC were obtained through impregnation‐pyrolysis method, results manifest Mg single atoms are embedded in nitrogen doped carbon in penta‐coordination (Mg‐C3N2) which endows Mg single atoms with strong basicity and is in contrast to traditional alkaline‐earth metal oxides. The novel Mg1/NPC exhibits excellent activity (40.2%) and stability in transesterification of methanol and ethylene carbonate to produce dimethyl carbonate (DMC), outperforming all state‐of‐the‐art Mg‐based solid base catalysts thus far reported as well as Ca, Na, and K‐based catalysts with superbasicity (2.5%–39.2%). This work might pave the way for the advancement of novel solid base catalysts with extraordinary sources of basicity for multifarious applications.
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