Enhancing electrochemical performance of ultrasmall Fe2O3-embedded carbon nanotubes via combusting-induced high-valence dopants

doi:10.1016/j.jmst.2022.06.040

Abstract

Abstract:

Doping is a reasonable solution to improve the electronic structure and surface properties of nanomaterials. Herein, we propose a rapid and simple methodology, flame synthesis, as an effective preparation strategy for incorporating high-valence metal ions (Ti⁴⁺, Sn⁴⁺, and Zr⁴⁺) into ultrasmall Fe₂O₃ on carbon nanotube support (i.e., M-FeO-CNT). The resulting materials exhibit not only a boosted Na⁺ adsorption as shown by density functional theory (DFT) calculations, but also display an increased oxygen deficiency. The electrochemical activity and charge transfer efficiency of Fe₂O₃ can be improved by reasonably substituting Fe³⁺ with Ti⁴⁺, Sn⁴⁺, and Zr⁴⁺. The electrochemical investigation of Ti-doped Fe₂O₃ (Ti-FeO-CNT) electrode demonstrates a splendid specific capacitance of 1.25 F cm⁻² at 1 mA cm⁻² in 1 M Na₂SO₄. This is significantly higher as compared to the capacitance of 0.48 F cm⁻². Flexible solid-state asymmetric supercapacitor Ti-FeO-CNT//MnO₂ is verified with operating voltage of 2.0 V and stability over 3000 cycles, and delivers a high energy density of 2.14 mWh cm⁻³ at power density of 25 mW cm⁻³. The flame synthesis is expected to be widely applicable for the preparation of high-valence metal ions doped nanosized Fe₂O₃ functionalized materials, thus opening up new avenues for energy and catalysis research.

Key words: Ultrasmall Fe₂O₃ nanoparticles, Doping, Flame synthesis, Flexible supercapacitor, DFT calculations

Yuan Wang, Tao Zhang, Jianfei Xiao, Xiaobao Tian, Shaojun Yuan. Enhancing electrochemical performance of ultrasmall Fe₂O₃-embedded carbon nanotubes via combusting-induced high-valence dopants[J]. J. Mater. Sci. Technol., 2023, 134: 142-150.

Figures/Tables 5

Fig. 1. (a) Schematic illustration of the preparation procedure of M-FeO-CNT/CC electrode (M = Ti, Sn, and Zr). (b) SEM and (c) TEM images of FeO-CNT. (d) SEM images of Ti-FeO-CNT. (e) Elemental mapping images of the Ti-FeO-CNT. (f) TEM images of Ti-FeO-CNT, and (g) corresponding HRTEM image.

Fig. 2. (a) Schematic illustration of atom doped Fe2O3. (b) XRD patterns of Ti doped FeO-CNT at different Ti percentage. The corresponding XPS spectra for (c) Ti 2p, (d) Fe 2p, and (e) O 1 s regions. (f) Contents of OI, OII, and OIII in Ti-FeO-CNT. (g) EPR spectra of the pristine and Ti doped FeO-CNT samples.

Fig. 3. Electrochemical performance of pristine FeO-CNT and M-FeO-CNT (M = Ti, Sn, and Zr) electrodes in a three-electrode system. (a) CV curves at a scan rate of 10 mV s?1 and (b) GCD curves at a current density of 1 mA cm?2. (c) Comparison of the specific capacitance of all samples. (d) Rate performance of Ti doped FeO-CNT based on GCD data. (e) Nyquist plots of the pristine FeO-CNT and M-FeO-CNT electrodes, and (f) the corresponding Bode phase plots. Dashed line points the characteristic frequency f0 (1/τ) at the phase angle of ?45°. (g) Resistance shows of M-FeO-CNT electrodes measured by a multimeter. (h) Dynamic contact angle measurements using 1 M Na2SO4 solution for pristine and M-FeO-CNT electrodes. (i) Randles-Sevcik plots. (j) Diffusion and capacitive contributions at various scan rates.

Fig. 4. The charge density difference of the (a) pure, (b) Ti1, and (c) Ti2 doped Fe2O3(110). (d) The average Na+ adsorption energies and obtained charge of O atom for different system. The isoface value is 0.002 e ?3. Light blue and yellow refer to the charge depletion and charge accumulation, respectively.

Fig. 5. (a) Schematic of the structure of flexible Ti-FeO-CNT//MnO2 ASC with two electrodes separated by the NKK membrane. (b) CV curves tested over the operating voltage windows from 1.4 to 2.0 V. (c) CV curves at different scan rates. (d) Bending test at a scan rate of 100 mV s?1. (e) GCD curves at various current densities. (f) Ragone plots along with other solid-state ASCs for comparison.

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Enhancing electrochemical performance of ultrasmall Fe₂O₃-embedded carbon nanotubes via combusting-induced high-valence dopants

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