Single-atom catalysts have been proved to be an effective material for the removal of organic pollutants from water and wastewater, and yet, the relationship between their internal structures and their roles still remains elusive. In this work, a catalyst Fe (MIL)-SAC with single-atom Fe-N active site was prepared. Fe (MIL)-SAC/Peroxydisulfate (PDS) system was able to achieve complete degrade of the Sulfamethoxazole (SMX) with k at 0.466 min, which was faster than the Fenton system under the same conditions (k = 0.422 min) and 16 times faster than Fe (MIL) (k = 0.029 min). Density functional calculations reveal that the Fe-N structure will affect the electron transport path and lead to selective generation of O by triggering S-O breakage and O-O polarization in PDS. Furthermore, Fe (MIL)-SAC/PDS system exhibits strong resistance to common influencing factors and has good application prospects. This work provides a new approach for the selectively generation of O for the efficient treatment of organic pollutants in aqueous environment.
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http://dx.doi.org/10.1016/j.chemosphere.2023.140331 | DOI Listing |
Angew Chem Int Ed Engl
January 2025
Tianjin University, School of Materials science and engineering, School of Materials Science and Engineering, Tianjin University, 300072, Tianjin, CHINA.
Fe-N-C catalyst is the most promising alternative to platinum catalyst for proton-exchange membrane fuel cells (PEMFCs), however its high performance cannot be maintained for a long enough time in device. The construction of a new Fe coordination environment that is different from the square-planar Fe-N 4 configuration in Fe-N-C catalyst is expected to break current stability limits, which however remains unexplored. Here, we report the conversion of Fe-N-C to a new FeNxSey catalyst, where the Fe sites are three-dimensionally (3D) co-coordinated by N and Se atoms.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Xiamen University, College of Chemistry and Chemical Engineering, Siming streat, Xiamen, CHINA.
Learning from nature has garnered significant attention in the scientific community for its potential to inspire creative solutions in material or catalyst design. The study reports a biomimetic single selenium (Se) site-modified carbon (C) moiety that retains the unique reactivity of selenoenzyme with peroxides, aiming to selectively catalyze the oxygen reduction reaction (ORR). The as-designed Se-C demonstrates nearly 100% 4-electron selectivity, evidenced by 0.
View Article and Find Full Text PDFSmall
January 2025
Key Lab of Bamboo and Rattan Science & Technology, International Center for Bamboo and Rattan, Beijing, 100102, P. R. China.
A nitrogen-coordinated Fe single-atom catalyst (SA Fe-N/C) is synthesized using a homogeneous ethanol-based dissolution system with bamboo kraft lignin serving as the carbon source. Uniformly dispersed Fe atoms with an interatomic distance of less than 2 Å throughout the SA Fe-N/C structure are revealed through X-ray absorption spectral analysis and HAADF-STEM images, which possessed a high Fe loading of 2.69%.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Department of Chemistry and Guangdong Provincial Key Laboratory of Catalysis, Southern University of Science and Technology, Shenzhen 518055, Guangdong, China.
Single-atom catalysts (SACs) have attracted widespread attention due to their potential to replace platinum-based catalysts in achieving efficient oxygen reduction reaction (ORR), yet the rational optimization of SACs remains challenging due to their elusive reaction mechanisms. Herein, by employing ab initio molecular dynamics simulations and a thermodynamic integration method, we have constructed the potential-dependent free energetics of ORR on a single iron atom catalyst dispersed on nitrogen-doped graphene (Fe-N/C) and further integrated these parameters into a microkinetic model. We demonstrate that the rate-determining step (RDS) of the ORR on SACs is potential-dependent rather than invariant within the operative potential range.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
Center of Nanomaterials for Renewable Energy (CNRE), State Key Laboratory of Electrical Insulation and Power Equipment, School of Electrical Engineering, Xi'an Jiaotong University, Xi'an 710049, P. R. China.
The Fe-N-C catalyst, featuring a single-atom Fe-N configuration, is regarded as one of the most promising catalytic materials for the oxygen reduction reaction (ORR). However, the significant activity difference under acidic and alkaline conditions of Fe-N-C remains a long-standing puzzle. In this work, using extensive ab initio molecular dynamics (AIMD) simulations, we revealed that pH conditions influence ORR activity by tuning the surface charge density of the Fe-N-C surface, rather than through the direct involvement of HO or OH ions.
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