Simultaneous CO2 capture and metal purification from waste streams using triple-level dynamic combinatorial chemistry

Abstract

A reduction in CO2 emissions is required to mitigate global warming. Post-combustion carbon capture is one of the most developed technologies that has the potential to meet this goal, but its cost prevents its widespread use. A different approach would be to use CO2 directly as it is captured, before it is stored. Here we explore spontaneous CO2 fixation by industrial polyamines as a strategy to generate dynamic libraries of ligands for metal separation and recovery. We identify the CO2 loadings and solvents promoting the optimal precipitation of each metal from the dynamic libraries of complexes. We demonstrate the separation of lanthanum and nickel using the exhaust gas of an internal combustion engine vehicle, and show that the three metal constituents of the La2Ni9Co alloys used to manufacture the batteries of electric vehicles can be separated and recovered by successive CO2-induced selective precipitations. Beyond the concept of CO2-sourced multi-level dynamic coordination chemistry, this study provides a potential framework for integrated CO2 capture and use through sustainable processes.

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Fig. 1: Simplified virtual triple-level dCLIP dynamic combinatorial system.
Fig. 2: Metal-free dynamic carbamation system dCMeOH.
Fig. 3: Constituent analyses of the dCLIPMeOH–Ln system.
Fig. 4: Selection and amplification of tailored sets of ligands from the dCMeOH–M subsystems (M = Ln, Co or Ni).
Fig. 5: Fraction of components captured into the dCLIPSEtOH–M system from the dCLIPEtOH–M system.
Fig. 6: Flowcharts of individual metal recovery induced by CO2 capture.

Data availability

Crystallographic data for the structures reported in this Article have been deposited at the Cambridge Crystallographic Data Centre, under deposition number CCDC 1951701 (Ni(C0)2Cl2). Copies of the data can be obtained free of charge via https://www.ccdc.cam.ac.uk/structures/. All other data supporting the findings of this study, including synthetic and analytical procedures are available within the Article and its Supplementary Information, or from the corresponding author upon reasonable request.

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Acknowledgements

We thank F. Bosselet, Y. Aizac (powder X-ray diffraction), E. Jeaneau (single-crystal X-ray diffraction), A. Berlioz-Barbier (cold-spray ionization mass spectrometry) and A. Baudouin (diffusion-ordered spectroscopy NMR analyses) for technical support. (We are grateful to O. Tillement for providing access to ICP-OES facilities and to D. J. Heldebrant, L. Vial and F. MacPherson for commenting on drafts of this manuscript. Financial support from Pulsalys to J.S. is gratefully acknowledged. This work was supported by the LABEX iMUST (ANR-10-LABX-0064) of Université de Lyon, within the programme ‘Investissements d’Avenir’ (ANR-11-IDEX-0007) operated by the French National Research Agency (ANR).

Author information

J.L. conceived the idea. J.L. and J.S. designed the experiments. J.S. and C.T. carried out the experimental work. J.S., C.T. and P.J. conducted the analyses. R.G. and C.N. designed and performed the simulations. J.L. and J.S. co-wrote the paper. All authors contributed to revising the paper.

Correspondence to Julien Leclaire.

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Competing interests

The authors have filed patent application WO2014188115 relating to this work.

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Supplementary information

Supplementary Information

The supplementary file contains all synthetic and analytical procedures (including CO2–metal integrated capture analysed in situ and ex situ; metal recovery from La2Ni9Co alloys through CO2 capture; CO2 and metal release; and La/Ni separation using exhaust fumes), data processing methods (including speciation and nonlinear fitting models, statistical repartition in the solid phases and calculation of normalized AFs), supplementary figures and data (DFT calculations and X-ray diffraction images).

Crystallographic data

CIF for Ni(C0)2Cl2; CCDC reference 1951701.

Crystallographic data

Supplementary Video

CO2 and La/Ni separation from exhaust fumes.

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Septavaux, J., Tosi, C., Jame, P. et al. Simultaneous CO2 capture and metal purification from waste streams using triple-level dynamic combinatorial chemistry. Nat. Chem. 12, 202–212 (2020). https://doi.org/10.1038/s41557-019-0388-5

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