Recently, Professor Zhou Guang Lu from Southern University of Science and Technology published a paper entitled “Cu single atoms regulating nitrogen active-sites of g-C3N4 for sodium” in the internationally renowned journal Energy Storage Materials ion storage “article. In this paper, the regulation of g-C3N4 nitrogen active site by monatomic copper is analyzed, and it is concluded that monatomic copper enhances sodium storage capacity through REDOX mechanism. Dr. Huimin Yuan and Guiyu Liu are the first authors of this paper.
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Research background
The nitrogen-rich material graphite phase carbon nitride (g-C3N4) is regarded as one of the most promising anode materials for sodium-ion batteries (SIBs) because of its low cost and easy availability. However, excessive unstable nitrogen active sites in low-crystallinity carbon nitride can lead to significant irreversible sodium ion adsorption, as well as inadequate electrical conductivity and structural instability, thus limiting its practical application. A novel cryogenic strategy is proposed to stabilize g-C3N4 by using monatomic copper to regulate the nitrogen configuration. Copper single atom as an anchor effectively regulates the coordination environment of nitrogen atoms in carbon nitride, thus constructing a stable active site for Na+ storage and establishing a fast conductive network for Na+ transport. As a result, Cu1.0/NC exhibits excellent capacity (350.4mAhg-1 at a current density of 50 mag-1), excellent magnification performance (252.3mAhg-1 at a current density of 1000 mag-1), and good stability in long cycle tests. In addition, a combination of in situ Raman, in situ XANES and XPS techniques revealed that Cu atoms significantly affect the charge transfer of Na+ through REDOX reaction and change the storage mode of sodium ions during the process of natrization/desodization.
Research questions
Figure 1. Design principles of anode materials for sodium ion batteries
Figure 2.(a)g-C3N4 supported monatomic copper synthesis scheme. (b) TEM and HRTEM images of Cu1.0/NC. (c1-c4) EDS mapping images of all elements in Cu1.0/NC. (d) HAADF-STEM images of Cu1.0/NC. (e) High-resolution Cu2pXPS spectra of all composites. (f) Cuk-side XANES spectra of reference samples (Cu foil and CuPC) and prepared composites (Cu0.5/NC, Cu1.0/NC, and Cu2.0/NC). (g)K3 weighted χ(k) function. (h)EPR spectrum.
Figure 3.(a) N1sXPS spectra of g-C3N4, NC, and Cu1.0/NC. (b) Comparison of pyridine and pyrrole nitrogen content in NC, Cu0.5/NC, Cu1.0/NC and Cu2.0/NC. (c)FTIR spectroscopy. (d) sodium storage configuration. (e) Adsorption energy of pyrrole nitrogen, pyridine nitrogen and graphitized nitrogen with sodium ions.
Figure 4.(a) Charge/discharge curves of NC, Cu0.5/NC, Cu1.0/NC and Cu2.0/NC at a current of 50mAg-1. (b) Comparison of initial Coulomb efficiency (ICE) of each material. (c) magnification properties of different materials. (d) Cyclic stability of NC, Cu0.5/NC, Cu1.0/NC and Cu2.0/NC at current 0.1Ag-1. (e) Long cycle performance of Cu1.0/NC at 5Ag-1.
Figure 5. Sodium storage mechanism of Cu1.0/NC. (a) CV curve of Cu1.0/NC at scan rates ranging from 0.1 to 1.0mVs−1. (b) The corresponding log(i)vslog(ν) diagram (c) compares the B-values calculated from the CV curve. (d) In situ Raman of Cu1.0/NC and corresponding time-voltage curves. (e) Schematic diagram of sodium storage mechanism in Cu1.0/NC. Non-situ XANES of (f)N1s and (g)CuK-edge at different voltages. (h) out-of-situ Na1s spectra of XPS during charging and discharging. (i) Schematic diagram of Cu3d orbital electron evolution. (j) All considered Na adsorption sites and corresponding adsorption energy (Eads) on Cu1.0/NC.
Research summary
The nitrogen configuration in g-C3N4 was successfully regulated by the introduction of monatomic copper. The incorporation of monatomic copper into carbonitrides not only enhances the electrical conductivity of nitrogen-rich carbon materials and promotes effective electron conversion, but also optimizes the electron configuration of nitrogen atoms and establishes a stable active center for sodium storage. Interestingly, the metal copper altered the electronegativity of the coordinated nitrogen atoms by inducing REDOX effects, leading to changes in sodium storage patterns, with significant benefits for long-term cyclic tolerance. Therefore, the modified Cu1.0/NC as a negative electrode material shows excellent magnification performance and long life stability. Manipulating the nitrogen coordination environment by metal single atoms provides a new perspective for the system design of high-performance electrode materials in rechargeable batteries.
The original link: https://doi.org/10.1016/j.ensm.2024.103608
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