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Transition-metal single-atom catalysts present extraordinary activity per metal atomic site, but suffer from low metal-atom densities (typically less than 5 wt% or 1 at.%), which limits their overall catalytic performance. Here we report a general method for the synthesis of single-atom catalysts with high transition-metal-atom loadings of up to 40 wt% or 3.8 at.%, representing several-fold improvements compared to benchmarks in the literature. Graphene quantum dots, later interweaved into a carbon matrix, were used as a support, providing numerous anchoring sites and thus facilitating the generation of high densities of transition-metal atoms with sufficient spacing between the metal atoms to avoid aggregation. A significant increase in activity in electrochemical CO reduction (used as a representative reaction) was demonstrated on a Ni single-atom catalyst with increased Ni loading.
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http://dx.doi.org/10.1038/s41557-021-00734-x | DOI Listing |
Environ Sci Technol
December 2024
CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science & Technology of China, Hefei 230026, China.
Organic pollutants removal via a polymerization transfer (PT) pathway based on the use of single-atom catalysts (SACs) promises efficient water purification with minimal energy/chemical inputs. However, the precise engineering of such catalytic systems toward PT decontamination is still challenging, and the conventional SACs are plagued by low structural stability of carbon material support. Here, we adopted magnesium oxide (MgO) as a structurally stable alternative for loading single copper (Cu) atoms to drive peroxymonosulfate-based Fenton-like reactions.
View Article and Find Full Text PDFSmall
December 2024
Yangtze Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, Huzhou, 313001, P. R. China.
In recent years, single-atom catalysts (SACs) with separated active centers and high atom utilization have grown significantly as a significant area of catalytic research. In catalytic applications, SACs of various kinds have demonstrated exceptional performance, so the study of the catalytic mechanism of SACs provides a clearer direction for the preparation of catalysts with high performance. Strong linkages between the single atoms and the support are necessary to overcome the tendency of single atoms to aggregate into clusters, which is called metal-support interaction (MSI).
View Article and Find Full Text PDFAnal Chem
December 2024
Key Laboratory of Optic-Electric Sensing and Analytical Chemistry for Life Science, MOE, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, P. R. China.
The classical electrochemiluminescence (ECL) reagent Ru(bpy) was first doped into CdSe QDs to prepare novel dual-potential color-resolved luminophore Ru-CdSe QDs. Ru-CdSe QDs emitted a strong red ECL signal at a positive potential with coreactant TPrA and a strong green ECL signal at a negative potential with coreactant KSO. As a proof-of-concept application, this work introduced Ru-CdSe QDs into a dual-channel closed bipolar electrode (CBPE) system to construct an ECL biosensor for simultaneous detection of chloramphenicol (CAP) and kanamycin (KAN).
View Article and Find Full Text PDFLangmuir
December 2024
Department of Chemistry, School of Physical Chemical and Applied Sciences, Pondicherry University, Puducherry 605014, India.
The electrochemical CO reduction reaction (CORR) is a promising approach to alleviating global warming and emerging energy crises. Yet, the CORR efficiency is impeded by the need for electrocatalysts with good selectivity and efficiency. Recently, single-atom catalysts (SACs) have attracted much attention in electrocatalysis and are more efficient than traditional metal-based catalysts.
View Article and Find Full Text PDFAdv Mater
December 2024
School of Materials Science and Engineering, Tianjin Key Laboratory of Composite and Functional Materials, Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education, Tianjin University, Tianjin, 300350, P. R. China.
Atomically dispersed transition metal (ADTM) catalysts are widely implemented in energy conversion reactions, while the similar properties of TMs make it difficult to continuously improve the activity of ADTMs via tuning the composition of metals. Introducing nonmetal sites into ADTMs may help to effectively modulate the electronic structure of metals and significantly improve the activity. However, it is difficult to achieve the co-existence of ADTMs with nonmetal atoms and clarify their synergistic effect on the catalytic mechanism.
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