Single-atom catalysts (SACs) have been widely recognized as state-of-the-art catalysts in environment remediation because of their exceptional performance, 100% metal atomic utilization, almost no secondary pollution, and robust structures. Most recently, the activation of persulfate with carbon-based SACs in advanced oxidation processes (AOPs) raises tremendous interest in the degradation of emerging contaminants in wastewater, owning to its efficient and versatile reactive oxidant species (ROS) generation. However, the comprehensive and critical review unraveling the underlying relationship between structures of carbon-based SACs and the corresponding generated ROS is still rare. Herein, we systematically summarize the fundamental understandings and intrinsic mechanisms between single metal atom active sites and produced ROS during AOPs. The types of emerging contaminants are firstly elaborated, presenting the prior pollutants that need to be degraded. Then, the preparation and characterization methods of carbon-based SACs are overviewed. The underlying material structure-ROS type relationship in persulfate-based AOPs is discussed in depth to expound the catalytic mechanisms. Finally, we briefly conclude the current development of carbon-based SACs in AOPs and propose the prospects for rational design and synthesis of carbon-based SACs with on-demand catalytic performances in AOPs in future research.
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http://dx.doi.org/10.1016/j.eehl.2023.04.002 | DOI Listing |
Small
January 2025
College of Material Science and Engineering, Hunan University, Changsha, Hunan, 410082, China.
Single-atom catalysts (SACs) with high activity and efficient atom utilization for oxygen reduction reactions (ORRs) are imperative for rechargeable Zinc-air batteries (ZABs). However, it is still a prominent challenge to construct a noble-metal-free SAC with low cost but high efficiency. Herein, a novel nitrogen-doped graphene (NrGO) based SAC, immobilized with atomically dispersed single cobalt (Co) atoms (Co-NrGO-SAC), is reported for ORRs.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
College of Chemistry, Chemical Engineering and Environment, Fujian Provincial Key Laboratory of Modern Analytical Science and Separation Technology, Micro-Nano Organic Optical Materials Laboratory, Minnan Normal University, Zhangzhou 363000, China.
The type of coordinated N atoms in the metal-N coordination structure is of paramount importance to the catalytic property of N-modified carbon-based single-atom catalysts (SACs). Extended X-ray absorption fine structure (EXAFS) spectroscopy is a powerful tool for analyzing the coordination environments of SACs. Despite its efficacy, the limited availability of synchrotron light sources and the complexity of data analysis have constrained its broader application in identifying metal-N coordination types within SACs.
View Article and Find Full Text PDFNanoscale
December 2024
National Key Laboratory of Aerospace Flight Technology, Beijing Aerospace Technology Research Institute, Beijing 100074, China.
Exploiting efficient and inexpensive electrocatalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is of great significance for the rapid development of renewable energy technologies. The embedding of single-atom metals into two-dimensional (2D) carbon-based materials as electrocatalysts for fuel cells and metal-air batteries have become a major research focus. Herein, the catalytic properties of the ORR and OER of partial metal atoms embedded in a two-dimensional h-BCN monolayer were systematically investigated on thermodynamic and kinetic scales using density functional theory calculations.
View Article and Find Full Text PDFJ Colloid Interface Sci
October 2023
College of Chemistry and Chemical Engineering, Ningxia University, Yinchuan, Ningxia 750021, PR China. Electronic address:
Angew Chem Int Ed Engl
January 2025
International Cooperation United Laboratory of Eco-chemical Engineering and Green Manufacturing, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao, 266042, China.
Dimeric metal sites (DiMSs) in carbon-based single atom catalysts (SACs) offer distinct advantages in optimizing the adsorption energies of the catalytic intermediates and reaction pathways over single atom sites, which inspires the investigations on the rational design of DiMSs-based SACs and the accurate discernment of catalytic mechanisms. Here, dimeric Fe sites on carbon blacks (DiFe-N/CBs) are prepared using the precursor of metal-organic complex with a controlled structure, and the rigid ligand confinement secures the preservation of dimeric Fe sites during the thermal treatment. DiFe-N/CBs shows excellent electrocatalytic performance for oxygen reduction reaction (ORR) with a high half-wave potential of 0.
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