Metal-organic framework (MOF) derived single-atom catalysts (SACs), featured unique active sites and adjustable topological structures, exhibit high electrocatalytic performance on carbon dioxide reduction reactions (CO2RR). By modulating elements and atomic...
Atomically dispersed metal sites (ADMSs) attract immense attention because they can be used in the fields of energy and environmental protection as they are characterized by high atomic utilization efficiency and exhibit high activity. Various supports for anchoring isolated metal atoms are developed to construct ADMSs characterized by highly stable and well‐defined structures. This can be achieved by increasing the number of anchoring sites and reinforcing metal–support interactions. MXenes, a new series of 2D nanomaterials, exhibit promising potential in stabilizing isolated metal atoms because of their large specific surface areas and unique surface properties. The high conductivity and hydrophilicity of MXenes can be attributed to the nature of surface functionalization and the properties of tunable structures of the materials. Benefiting from these excellent properties, MXenes can find their applications in various fields. Herein, the precise characterization methods that can be followed to study ADMSs, the construction of MXene‐supported ADMSs using theoretical predictions, and experimental modulation strategies are summarized, and their corresponding applications in electrocatalysis, organocatalysis, and advanced battery systems are systematically illustrated. It is hoped that this review will provide insights that can be used for the further development of MXene‐supported ADMSs.
The
regulation of the coordination environment of the central metal
atom is considered as an alternative way to enhance the performance
of single-atom catalysts (SACs). Herein, we design an electrocatalyst
with active sites of isolated Co atoms coordinated with four sulfur
atoms supported on N-doped carbon frameworks (Co1-S4/NC), confirmed by high-angle annular dark-field scanning
transmission electron microscope (HADDF-STEM) and synchrotron-radiation-based
X-ray absorption fine structure (XAFS) spectroscopy. The Co1-S4/NC possesses higher hydrogen evolution reaction (HER)
catalytic activity than other Co species and exceptional stability,
which exhibits a small Tafel slope of 60 mV dec–1 and a low overpotential of 114 mV at 10 mA cm–2 during the HER in 0.5 M H2SO4 solution. Furthermore,
through in situ X-ray absorption spectrum tests and density functional
theory (DFT) calculations, we reveal the catalytic mechanism of Co1-S4 moieties and find that the increasing number
of sulfur atoms in the Co coordination environment leads to a substantial
reduction of the theoretical HER overpotential. This work may point
a new direction for the synthesis, performance regulation, and practical
application of single-metal-atom catalysts.
Strain engineering is an attractive strategy for improving the intrinsic catalytic performance of heterogeneous catalysts. Manipulating strain on the short-range atomic scale to the local structure of the catalytic sites is still challenging. Herein, we successfully achieved atomic strain modulation on ultrathin layered vanadium oxide nanoribbons by an ingenious intercalation chemistry method. When trace sodium cations were introduced between the V 2 O 5 layers (Na + -V 2 O 5 ), the V−O bonds were stretched by the atomically strained vanadium sites, redistributing the local charges. The Na + -V 2 O 5 demonstrated excellent photooxidation performance, which was approximately 12 and 14 times higher than that of pristine V 2 O 5 and VO 2 , respectively. Complementary spectroscopy analysis and theoretical calculations confirmed that the atomically strained Na + -V 2 O 5 had a high surficial charge density, improving the activation of oxygen molecules and contributing to the excellent photocatalytic property. This work provides a new approach for the rational design of strain-equipped catalysts for selective photooxidation reactions.
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