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Constructing High‐Performance Cobalt‐Based Environmental Catalysts from Spent Lithium‐Ion Batteries: Unveiling Overlooked Roles of Copper and Aluminum from Current Collectors

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Angewandte Chemie International Edition
Authors:
Jianxing Liang at Shanghai Jiao Tong University
Jianxing Liang
Kan Li at Shanghai Jiao Tong University
Kan Li
Feng Shi
Feng Shi
Feng Shi
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Jingdong Li
Jingdong Li
Jingdong Li
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Abstract and Figures

Converting spent lithium‐ion batteries (LIBs) cathode materials into environmental catalysts has drawn more and more attention. Herein, we fabricated a Co3O4‐based catalyst from spent LiCoO2 LIBs (Co3O4‐LIBs) and found that the role of Al and Cu from current collectors on its performance is nonnegligible. The density functional theory calculations confirmed that the doping of Al and/or Cu upshifts the d‐band center of Co. A Fenton‐like reaction based on peroxymonosulfate (PMS) activation was adopted to evaluate its activity. Interestingly, Al doping strengthened chemisorption for PMS (from −2.615 eV to −2.623 eV) and shortened Co−O bond length (from 2.540 Å to 2.344 Å) between them, whereas Cu doping reduced interfacial charge‐transfer resistance (from 28.347 kΩ to 6.689 kΩ) excepting for the enhancement of the above characteristics. As expected, the degradation activity toward bisphenol A of Co3O4‐LIBs (0.523 min⁻¹) was superior to that of Co3O4 prepared from commercial CoC2O4 (0.287 min⁻¹). Simultaneously, the reasons for improved activity were further verified by comparing activity with catalysts doped Al and/or Cu into Co3O4. This work reveals the role of elements from current collectors on the performance of functional materials from spent LIBs, which is beneficial to the sustainable utilization of spent LIBs.
(A) XRD patterns, (B) FTIR spectra, (C) Raman spectra and (D) Co 2p3/2 XPS spectra of Co3O4 and Co3O4‐LIBs. (E) Cu 2p XPS spectrum of Co3O4‐LIBs. (F) Al 2p and Li 1s XPS spectra of Co3O4‐LIBs. (G) Co K‐edge XANES spectra of Co foil, CoO, Co3O4 and Co3O4‐LIBs. (H) Co K‐edge FT‐EXAFS spectra of Co foil, Co3O4 and Co3O4‐LIBs. (I) Cu K‐edge FT‐EXAFS spectra of Cu foil, CuO and Co3O4‐LIBs.
(A) XRD patterns, (B) FTIR spectra, (C) Raman spectra and (D) Co 2p3/2 XPS spectra of Co3O4 and Co3O4‐LIBs. (E) Cu 2p XPS spectrum of Co3O4‐LIBs. (F) Al 2p and Li 1s XPS spectra of Co3O4‐LIBs. (G) Co K‐edge XANES spectra of Co foil, CoO, Co3O4 and Co3O4‐LIBs. (H) Co K‐edge FT‐EXAFS spectra of Co foil, Co3O4 and Co3O4‐LIBs. (I) Cu K‐edge FT‐EXAFS spectra of Cu foil, CuO and Co3O4‐LIBs.
… 
(A and B) SEM, (C and D) TEM images and (inset) HR‐TEM images of Co3O4 and Co3O4‐LIBs. Elemental mapping of (E) Co, (F) Cu, (G) Al and (H) O in the Co3O4‐LIBs.
(A and B) SEM, (C and D) TEM images and (inset) HR‐TEM images of Co3O4 and Co3O4‐LIBs. Elemental mapping of (E) Co, (F) Cu, (G) Al and (H) O in the Co3O4‐LIBs.
… 
(A) The optimal configurations, (B) PDOS, (C) d‐band center and (D)  electrochemical impedance spectroscopy Nyquist plots of Co3O4, Al−Co3O4, Cu−Co3O4 and Cu/Al−Co3O4.
(A) The optimal configurations, (B) PDOS, (C) d‐band center and (D)  electrochemical impedance spectroscopy Nyquist plots of Co3O4, Al−Co3O4, Cu−Co3O4 and Cu/Al−Co3O4.
… 
(A) Degradation of BPA and (B) the corresponding k in different systems. (C) Normalization based on k and BET specific surface area of Co3O4, Co3O4‐LIBs, and Cu/Al−Co3O4, respectively. (D) k of Co3O4/PMS, Cu−Co3O4/PMS, Al−Co3O4/PMS and Cu/Al−Co3O4/PMS systems for the degradation of BPA. Reaction conditions: [BPA]0=20 mg ⋅ L⁻¹, [catalyst]=0.2 g ⋅ L⁻¹, [PMS]=0.1 g ⋅ L⁻¹, initial pH=7.2, T=25 °C.
(A) Degradation of BPA and (B) the corresponding k in different systems. (C) Normalization based on k and BET specific surface area of Co3O4, Co3O4‐LIBs, and Cu/Al−Co3O4, respectively. (D) k of Co3O4/PMS, Cu−Co3O4/PMS, Al−Co3O4/PMS and Cu/Al−Co3O4/PMS systems for the degradation of BPA. Reaction conditions: [BPA]0=20 mg ⋅ L⁻¹, [catalyst]=0.2 g ⋅ L⁻¹, [PMS]=0.1 g ⋅ L⁻¹, initial pH=7.2, T=25 °C.
… 
Effect of scavengers on the degradation of BPA in (A) Co3O4‐LIBs/PMS and (B) Co3O4/PMS systems. Reaction conditions: [BPA]0=20 mg ⋅ L⁻¹, [catalyst]=0.2 g ⋅ L⁻¹, [PMS]=0.1 g ⋅ L⁻¹, initial pH=7.2, T=25 °C, [TBA]=[MeOH]=[NBA]=200 mM, [BQ]=20 mM, [CHCl3]=10 mM, [FFA]=20 mM, [L‐histidine]=10 mM, [β‐carotene]=0.5 mM, [Phenol]=20 mM, [DMSO]=5 mM. EPR spectra of (C) Co3O4‐LIBs/PMS and (D) Co3O4/PMS systems with/without NaF. Reaction conditions: [NaF]0=1 mM (if need), [catalyst]=0.2 g ⋅ L⁻¹, [PMS]=0.1 g ⋅ L⁻¹, T=25 °C.
+3
Effect of scavengers on the degradation of BPA in (A) Co3O4‐LIBs/PMS and (B) Co3O4/PMS systems. Reaction conditions: [BPA]0=20 mg ⋅ L⁻¹, [catalyst]=0.2 g ⋅ L⁻¹, [PMS]=0.1 g ⋅ L⁻¹, initial pH=7.2, T=25 °C, [TBA]=[MeOH]=[NBA]=200 mM, [BQ]=20 mM, [CHCl3]=10 mM, [FFA]=20 mM, [L‐histidine]=10 mM, [β‐carotene]=0.5 mM, [Phenol]=20 mM, [DMSO]=5 mM. EPR spectra of (C) Co3O4‐LIBs/PMS and (D) Co3O4/PMS systems with/without NaF. Reaction conditions: [NaF]0=1 mM (if need), [catalyst]=0.2 g ⋅ L⁻¹, [PMS]=0.1 g ⋅ L⁻¹, T=25 °C.
… 
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Heterogeneous Catalysis
Constructing High-Performance Cobalt-Based Environmental
Catalysts from Spent Lithium-Ion Batteries: Unveiling Overlooked
Roles of Copper and Aluminum from Current Collectors
Jianxing Liang, Kan Li,* Feng Shi, Jingdong Li, Jia-nan Gu, Yixin Xue, Chenyu Bao,
Mingming Guo, Jinping Jia, Maohong Fan,* and Tonghua Sun*
Abstract: Converting spent lithium-ion batteries (LIBs)
cathode materials into environmental catalysts has
drawn more and more attention. Herein, we fabricated a
Co3O4-based catalyst from spent LiCoO2LIBs
(Co3O4-LIBs) and found that the role of Al and Cu from
current collectors on its performance is nonnegligible.
The density functional theory calculations confirmed
that the doping of Al and/or Cu upshifts the d-band
center of Co. A Fenton-like reaction based on perox-
ymonosulfate (PMS) activation was adopted to evaluate
its activity. Interestingly, Al doping strengthened chem-
isorption for PMS (from 2.615 eV to 2.623 eV) and
shortened CoO bond length (from 2.540 Å to 2.344 Å)
between them, whereas Cu doping reduced interfacial
charge-transfer resistance (from 28.347 kΩ to 6.689 kΩ)
excepting for the enhancement of the above character-
istics. As expected, the degradation activity toward
bisphenol A of Co3O4-LIBs (0.523 min1) was superior
to that of Co3O4prepared from commercial CoC2O4
(0.287 min1). Simultaneously, the reasons for improved
activity were further verified by comparing activity with
catalysts doped Al and/or Cu into Co3O4. This work
reveals the role of elements from current collectors on
the performance of functional materials from spent
LIBs, which is beneficial to the sustainable utilization of
spent LIBs.
Introduction
To realize carbon neutrality, the development of electric
vehicles (EVs), using lithium-ion batteries (LIBs) as the
power source, has been propelled due to the vital way to
reduce carbon emissions in the transportation industry
effectively.[1] According to the estimation from The Interna-
tional Energy Agency, global EVs sales will increase from
4 million in 2020 to 21.5 million in 2030, meaning that the
demand for LIBs will be increased substantially.[2] Owing to
the limited lifespan of LIBs, the production of spent LIBs
rises greatly.[3] Nevertheless, spent LIBs contain massive
toxic electrolytes and transition metals, which could lead to
serious environmental pollution without proper treatment.[4]
More importantly, the content of valuable metals (e.g., Li)
in spent LIBs is richer than in natural ores.[3] Therefore,
recycling spent LIBs, especially cathode, is necessary, as it
not only alleviates environmental pollution but also reduces
the waste of resources.
At present, pyrometallurgy and hydrometallurgy are
routine processes to recycle spent LIBs.[1a,c] However, the
former requires massive energy consumption and causes an
amount of carbon dioxide emission, whereas the latter needs
multiple steps accompanying the significant discharge of
wastewater during the separation-purification process.[1a,3]
Recently, directly converting spent LIBs cathodes into
functional materials has seemed like a promising route for
recycling spent LIBs.[5] Cheng et al. successfully synthesized
high-efficiency NiMnCo-based catalysts for zinc-air bat-
teries, using spent LiNi1xyMnxCoyO2cathodes as raw
material by the acid leaching-radiative heating process.[6]
[*] J. Liang, Dr. K. Li, J. Li, J.-n. Gu, Y. Xue, C. Bao, M. Guo,
Prof. Dr. J. Jia, Prof. Dr. T. Sun
School of Environmental Science and Engineering
Shanghai Jiao Tong University
800 Dong Chuan Road, 200240 Shanghai, P. R. China
E-mail: likan@sjtu.edu.cn
sunth@sjtu.edu.cn
Dr. F. Shi
School of Chemistry and Chemical Engineering
Shanghai University of Engineering Science
333 Longteng Rd., 201620 Shanghai, P. R. China
Prof. Dr. M. Fan
College of Engineering and Physical Sciences, and School of Energy
Resources
University of Wyoming
82071 Laramie, WY, USA
E-mail: mfan@uwyo.edu
Prof. Dr. M. Fan
College of Engineering
Georgia Institute of Technology
30332 Atlanta, GA, USA
Prof. Dr. T. Sun
Shanghai Engineering Research Center of Solid Waste Treatment
and Resource Recovery
Shanghai Jiao Tong University
800 Dong Chuan Road, 200240 Shanghai, P. R. China
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How to cite: Angew. Chem. Int. Ed. 2024, e202407870
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