Disclosing the superior lithium storage of double-shelled Si@N-doped carbon: a synergic combination of experiment and theory

• Published in: Sustainable energy & fuels 2023-02, Vol.7 (4), p.184-192
• Main Authors: Majeed, Muhammad K, Iqbal, Rashid, Hussain, Arshad, Lotfi, Mina, Majeed, M. Umar, Ashfaq, M. Zeeshan, Javed, M. Sufyan, Ahmad, Muhammad, Saleem, Adil
• Format: Article
• Language: English
• Subjects: Anodes; Batteries; Carbon; Cycles; Density functional theory; Electrical conductivity; Electrical resistivity; Electrochemical analysis; Electrochemistry; Electrode materials; Lithium; Lithium-ion batteries; Mathematical analysis; Photoelectron spectroscopy; Photoelectrons; Raman spectroscopy; Rechargeable batteries; Silicon; Spectroscopy; Spectrum analysis; X ray photoelectron spectroscopy; X-ray diffraction
• ISSN: 2398-4902; 2398-4902
• DOI: 10.1039/d2se01571d

Through collective use of experimental investigation and theoretical approaches, i.e. , X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, microscopic properties and density functional theory (DFT) calculations, we comprehensively characterize the structural, morphological, and lithium (Li) storage performance of double-shelled silicon@ZIF-8@ZIF-67 (Si@DNC). The unique architectures not only absorb the huge volume variation stress of Si during cycling but also provide enhanced electrical conductivity and manipulate the stability and integrity of a well-wrapped double-shelled framework. Additionally, N-doped carbon can also enhance the conductivity of electrodes. The superior Li storage performance in double-shelled structures is refined via an interactive lithiation/delithiation approach and validated using DFT calculations. Typically, the as-prepared Si@DNC delivered enhanced cycling stability with a high discharge capacity of 2537.8 mA h g −1 in the first cycle and 1285 mA h g −1 after 200 cycles at 200 mA g −1 . Therefore, the double-shelled structure reflected outstanding electrochemical performance and is expected to be a forthcoming candidate for anode materials in next-generation lithium-ion batteries (LIBs). Si@DNC having dual stabilized architecture with a mesoporous structure is synthesized which consists of interconnected channels presenting exceptional Li storage. The relation between experimental investigation and theoretical approach is clarified.