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Progress in Chemistry 2020, Vol. 32 Issue (6): 836-850 DOI: 10.7536/PC190924 Previous Articles   Next Articles

• Review •

Progress for Metal-CO2 Batteries: Mechanism and Advanced Materials

Changfan Xu1, Xin Fang1, Jing Zhan1,**(), Jiaxi Chen1, Feng Liang2,**()   

  1. 1. School of Metallurgy and Environment, National Engineering Laboratory for High Efficiency Recovery of Refractory Nonferrous Metals, Central South University, Changsha 410083, China
    2. Faculty of Metallurgy and Energy Engineering, Kunming University of Science and Technology, Kunming 650093, China
  • Received: Revised: Online: Published:
  • Contact: Jing Zhan, Feng Liang
  • Supported by:
    the National Natural Science Foundation of China(51704136); the National Natural Science Foundation of China(11765010); the National Natural Science Foundation of China(51974378); the Scientific and Technological Breakthrough and Major Achievements Transformation of Strategic Emerging Industries of Hunan Province(2018GK4001); the Fundamental Research Funds for the Central Universities of Central South University(2019zzts502)
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Metal-carbon dioxide(Me-CO2) batteries can not only fix carbon dioxide effectively, but also serve as clean energy storage devices, which are considered as potential candidates for the next generation of energy conversion and storage, as well as carbon dioxide capture and utilization. However, due to the slow electrochemical reaction of the cathode, the instability of the electrolyte, and the difficult reversible conversion of the discharge product, the current Me-CO2 batteries are impeded by low capacity and rate capability, high polarizability, low energy conversion efficiency, and short cycle life. In this paper, we provide insights on the current main research progress of Me-CO2 batteries based on metal(lithium, sodium, aluminum, zinc, potassium) anodes, including discharge/charging mechanism, CO2 electrode and electrocatalysts, electrolyte materials and metal electrodes, etc. Considerable emphasis is placed on the effects of function material on the stability and rate of electrode reaction. In addition, the prospects and directions for the rational construction of materials are prospected to improve the electrochemical performance of Me-CO2 batteries and provide guidance for the development of Me-CO2 batteries.

Contents

1 Introduction
2 Mechanism for metal-CO2 batteries

2.1 Li-CO2 batteries

2.2 Na-CO2 batteries

2.3 Al-CO2 batteries

2.4 Zn-CO2 batteries

2.5 K-CO2 batteries

3 CO2 electrode/catalysts

3.1 Carbon/heteroatom doped carbon catalysts

3.2 Precious catalysts

3.2 Non-Precious catalysts

4 Electrolytes

4.1 Non-aqueous electrolytes

4.2 Quasi-solid/solid electrolytes

4.3 Hybrid electrolytes

5 Metal anode
6 Conclusion and outlook
Key words: metal-carbon dioxide batteries, reaction mechanism, electrocatalysis, electrolyte, reaction kinetics
Table 1 Possible reactions of the decomposition of Li2CO3 and the reversible potential of the corresponding reactions[19]
No. Possible reactions Erev/V vs. Li
1 Li2CO3 → CO2+1/2 O2+Li++2e- 3.82
2 Li2CO3 → CO2+2Li+ + O2·-
O2·- → O2
O2·- → O2 + electrolyte → uncertain product
3 2Li2CO3 + C → 3CO2+4Li++4e- 2.80
Fig. 1 Schematic illustration of a reversible Me-CO2 battery
Fig. 2 (a) The schematic representation of Li-CO2 battery with a BN-hG cathode.(b) Full discharge/charge curves,(c) discharge end voltage and (d) polarization curves at different current densities,(e) long-term cycling performance[38]
Fig. 3 Schematic diagram of the (a) reaction mechanism of the charging process of the Li-CO2 battery without the Ru catalyst, (b) possible charging mechanism of the Li-CO2 battery with the Ru catalyst and (c) discharging process of the Li-CO2 battery[22];(d) Discharge-charge voltage profiles and (e) Cyclability of two Al-CO2 batteries with NPG@Pd or NPG as cathodes, in which the current density was fixed at 333 mA·g-1[30]
Fig. 4 Rechargeable aqueous Zn-CO2 batteries with NiPG catalyst cathode.(a) The LSV curves for CO2 reduction reaction.(b) CO and H2 Faradaic efficiency at several discharge currents.(c) Galvanostatic discharge and charge potentials at 1.5 and 0.5 mA, respectively.(d) Galvanostatic discharge-charge cycling curves with 0.5 mA of discharge and 0.25 mA of charge[53]
Fig. 5 (a) The effect of dielectric constant of electrolyte solvent on the reaction pathway of Li-O2/CO2 battery[37];(b) Schematic illustrations of the formation mechanism of final discharge product(Li2CO3) in dilute LiTFSI-DMSO electrolyte;(c) Schematic illustrations of the formation mechanism of final discharge product(C2O62-) in super-concentrated LiTFSI-DMSO electrolyte[14]
Fig. 6 (a) Schematic illustration of the proposed hybrid Na-CO2 battery with N-SWCNH as a catalyst.(b) Discharge-charge voltage curves,(c) discharge capacities curves,(d) the cycling performance of hybrid Na-CO2 battery with N-SWCNH as catalyst at a current density of 0.1 mA·cm-2,(e) In-situ Raman characterization of the hybrid Na-CO2 battery during discharge and recharge,(f) Ex-situ XRD pattern of the CO2 electrode after discharge and charge[76]
Fig. 7 Design and characterization of rGO-Na anode(A~C) SEM images with corresponding inset photographs of GO foam(A), rGO foam reduced by molten Na(B), and rGO-Na anode surface(C).(D) FTIR of GO foam and rGO foam. a.u., arbitrary units. XPS spectra of O 1 s(E) and C 1 s(F) of GO foam and rGO foam.(G) XRD of rGO and rGO-Na anode.(H) Cyclic voltammograms of Na+ plating/stripping in a rGO-Na or Na/CPE/stainless steel cell with a sweep speed of 0.5 V·s-1.(I) Fast discharge/charge profiles of quasi-solid state Na-CO2 batteries in Ar atmosphere using rGO-Na and pure Na anodes. Rate, 0.3 mA·cm-2; voltage range, 1 to 4 V. Inset: SEM images of rGO-Na and pure Na anode surfaces after 450 cycles[71]
Table 2 Summary of Metal-CO2 batteries and their performances
Battery type Cathode Electrolyte Full discharge capacity
(mAh·g-1)		 Cyclability/
cycles		 Voltage
gap/V		 ref
Li-CO2/O2 (1∶1) Ketjen Black 1 M LiTFSI/EC:DEC(3∶7 v/v) 6750(0.1 mA·cm-2) - - 13
Li-CO2 Ketjen Black 1 M LiTFSI/EC:DEC(3∶7 v/v) 66(0.2 mA·cm-2) - - 13
Li-CO2/O2(2∶1) Ketjen Black LiCF3SO3/TEGDME(1∶4) 1808(30 mA·g-1) 10(30 mA·g-1) ~1.6 16
Li-CO2 Ketjen Black LiCF3SO3/TEGDME(1∶4) 1032(30 mA·g-1) 7(30 mA·g-1) ~1.6 16
Li-CO2 Ketjen black 1 M LiTFSI/TEGDME+LiBr 11 500(50 mA·g-1) 38(50 mA·g-1) ~1.4 83
Li-CO2 Super P 1 M LiTFSI/([bmim][Tf2N]) ~0(0.05 mA·cm-1) - - 15
Li-CO2 Super P LiCF3SO3/TEGDME(1∶4) 6062(100 mA·g-1) 20(100 mA·g-1) ~2 22
Li-CO2 high surface area carbon 1 M LiTFSI/([bmim][Tf2N]) ~750(0.05 mA·cm-1) - - 15
Li-CO2 CNTs Composite polymer electrolyte 993.2 mAh(2.5 mA) 100(100 mA·g-1) ~2.1 73
Li-CO2 CNTs Gel Polymer Electrolyte 8536(50 mA·g-1) 60(100 mA·g-1) ~1.65 72
Li-CO2 CNTs Polymer electrolyte 12 000(100 mA·g-1) 60(100 mA·g-1) ~1.65 84
Li-CO2 CNTs 1 M LiTFSI/TEGDME 8379(50 mA·g-1) 29(50 mA·g-1) ~1.5 17
Li-CO2 CNT 1 M LiCF3SO3/TEGDME ~2850 μAh/20 uA - ~1.4 18
Li-CO2 Graphene 1 M LiTFSI/TEGDME 14 722(50 mA·g-1) 20(50 mA·g-1) ~1.23 17
Li-CO2 pencil-trace Bi-CoPc-GPE 27 196(100 mA·g-1) 120(200 mA·g-1) 1.14 85
Li-CO2 B,N-hG 1 M LiTFSI/TEGDME 14 996(300 mA·g-1) 200(1.0 A g-1) ~1.0 38
Li-CO2 CQD/hG 1 M LiTFSI+0.3 M LiNO3/DMSO 12 300(500 mA·g-1) 235(1.0 A g-1) ~1.02 42
Li-CO2 Ru@super P LiCF3SO3/TEGDME(1∶4) 8229(100 mA·g-1) 70(100 mA·g-1) ~1.71 22
Li-CO2/2% O2 Ru@GNSs 0.1 M LiClO4/DMSO 4742(0.08 mA·cm-2) 67(0.16 mA·cm-2) ~1.3 43
Li-CO2 Ru-Cu-G 1 M LiTFSI/TEGDME 13 698(200 mA·g-1) 100(100 mA·g-1) ~0.88 86
Li-CO2 RuO2/LDO 1 M LiTFSI/TEGDME 5455(100 mA·g-1) 60(166 mA·g-1) ~0.6 44
Li-CO2 /O2 (4∶1) Ru/N-CNT 1 M LITFSI/TEGDME 10 200(100 mA·g-1) 184(100 mA·g-1) ~1.2 87
Li-CO2 /O2 (2∶1) Ru/N-CNT 1 M LITFSI/TEGDME 12 000(100 mA·g-1) 190(100 mA·g-1) ~1.2 87
Li-CO2 Ru/N-CNT 1 M LITFSI/TEGDME 9300(100 mA·g-1) 150(100 mA·g-1) ~1.8 87
Li-CO2 Ru/ACNF 1 M LITFSI/TEGDME 11 495(200 mA·g-1) 50(100 mA·g-1) ~1.43 88
Li-CO2 Ru nanosheet 1 M LiTFSI/TEGDME 9502(100 mA·g-1) 100(200 mA·g-1) ~1.2 89
Li-CO2 RuP2-NPCF 1 M LiTFSI/TEGDME 11 951(100 mA·g-1) 200(200 mA·g-1) ~1.77 21
Li-CO2 CNT@RuO2 LiCF3SO3/TEGDME(1∶4) 2187(50 mA·g-1) 30(50 mA·g-1) ~1.4 90
Li-CO2 Ir-NSs-CNFs 1 M LITFSI/TEGDME 7666.7(166.7 mA·g-1) 400(500 mA·g-1) ~1.05 48
Li-CO2 IrO2/δ-MnO2 1 M LiClO4/TEGDME 6604(100 mA·g-1) 378(400 mA·g-1) ~1.3 47
Li-CO2/O2 (1∶1) Au NPs LiTFSI/DMSO(1∶3) 753(400 mA·g-1) 100(100 mA·g-1) ~0.6 14
Li-CO2 Ru/CNT flexible wood 1 M LiTFSI/TEGDME 11 mAh·cm-2 200(100 mA·g-1) ~1.5 66
Li-CO2 Ir/CNFs 1 M LiTFSI/TEGDME 21 528(50 mA·g-1) 45(50 mA·g-1) ~1.4 67
Li-CO2 Mn2(dobdc) 1 M LiTFSI/TEGDME 18 022(50 mA·g-1) 50(200 mA·g-1) ~1.35 20
Li-CO2 Mn(HCOO)2 1 M LiTFSI/TEGDME 15 510(50 mA·g-1) 50(200 mA·g-1) ~1.4 20
Li-CO2 MnCO3 1 M LiTFSI/TEGDME 11 110(50 mA·g-1) 25(200 mA·g-1) ~1.7 20
Li-CO2 MnO@NC-G 1 M LITFSI/TEGDME 25 021(50 mA·g-1) 206(0.1 A g-1) ~0.88 56
Li-CO2 Porous Mn2O3 0.5 M LiClO4/TEGDME 9434(50 mA·g-1) 45(50 mA·g-1) ~1.4 91
Li-CO2 NiO-CNT 1 M LiTFSI/TEGDME 9000(50 mA·g-1) 42(50 mA·g-1) ~1.4 64
Li-CO2 NiO nanofibers 1 M LiCF3SO3/TEGDME 11 288(100 mA·g-1) 134(100 mA·g-1) ~1.6 92
Li-CO2 Ni-NG 1 M LiTFSI/TEGDME 17 625(100 mA·g-1) 100(100 mA·g-1) ~1.6 50
Li-CO2 Ni/r-GO 1 M LiTFSI/TEGDME 8991(0.1 mA·cm-2) 100(100 mA·g-1) ~1.05 65
Li-CO2 NiFe@NC/PPC 1 M LiCF3SO3/TEGDME 6.8 mAh·cm-2(0.05 mA·cm-2) 109(0.05 mA·cm-2) ~1.85 93
Li-CO2 Cu-NG 1 M LiTFSI/TEGDME 14 864(200 mA·g-1) 50(200 mA·g-1) ~1.3 55
Li-CO2 CoPPc 1 M LITFSI/TEGDME 13.6 mAh·cm-2
(0.05 mA·cm-2)		 50(0.05 mA·cm-2) ~1.3 94
Li-CO2 Mo2C/CNT 1 M LiCF3SO3/TEGDME 1150 μAh/20 μA 40(20 μA) ~0.9 18
Li-CO2 CC@Mo2C NPs Gel polymer electrolyte(GPE) 3415 μAh·cm-2(50 μA·cm-2) 40(20 μA·cm-2) ~0.65 54
Li-CO2 /trace O2 MFCN 1 M LiTFSI/TEGDME 8827(100 mA·g-1) 90(100 mA·g-1) ~1.04 95
Li-CO2 N-CNTs@Ti 1 M LiTFSI/TEGDME 9292.3(50 mA·g-1) 25(50 mA·g-1) ~1.51 96
Li-CO2 TiO2-NP/CNT/CNF 1 M LiTFSI/DMSO 1950 μAh·cm-2 20(0.05 mA·cm-2) ~1.4 97
Li-CO2 i-Ru4Cu1/CNFs 1 M LiTFSI/DMSO 15 753(300 mA·g-1) 110(500 mA·g-1) ~ 1.45 98
Li-CO2 Co0.2Mn0.8O2/CC 1 M LiTFSI/TEGDME 8203(100 mA·g-1) 500(100 mA·g-1) ~0.73 99
Li-CO2 MoS2 nanoflakes 0.1 M LiTFSI/EMIM-BF4/DMSO 60 000(100 mA·g-1) 500(500 mA·g-1) ~0.7 100
Li-CO2 ZnS QDs/N-rGO 1 M LiTFSI/TEGDME 10 310(100 mA·g-1) 190(400 mA·g-1) 1.21 101
Li-CO2 B-NCNT 1 M LiTFSI/TEGDME 23 328(50 mA·g-1) 360(1000 mA·g-1) 1.21~1.96 102
Li-CO2 COFs 1 M LiTFSI/TEGDME 27 348(200 mA·g-1) 200(1000 mA·g-1) 1.24 103
Li-CO2 adjacent Co/GO 1 M LiTFSI/TEGDME 17 358(100 mA·g-1) 100(100 mA·g-1) ~1.8 104
Li-CO2 Graphene@COF 1 M LiTFSI/TEGDME 27 833(75 mA·g-1) 56(500 mA·g-1) ~1.08 105
Li-CO2 MoS2-NS 1 M LiTFSI/DMSO 846 μAh·cm-2 50(0.05 mA·cm-2) ~1.0 106
Na-CO2 Super P 1 M NaClO4/TEGDME 173 mAh·g-1 - - 25
Na-CO2/O2 (3∶2) Super P 1 M NaClO4/TEGDME 2882(70 mA·g-1) - - 25
Na-CO2 Super P 0.75 M NaCF3SO3/IL 183 mAh·g-1 - - 25
Na-CO2/O2 (2∶3) Super P 0.75 M NaCF3SO3/IL 3500(70 mA·g-1) - - 25
Na-CO2/O2 (1∶1) porous carbon SiO2-IL-TFSI/PC-NaTFSI - 20(200 mA·g-1) ~2.2 26
Na-CO2 a-MWCNTs 1 M NaClO4/TEGDME 60 000(1000 mA·g-1) 200(1.0 A g-1) 0.6 27
Na-CO2 Na2CO3/CNTs 1 M NaClO4/TEGDME 350 mAh·g-1 100(0.05 mA·cm-2) ~1.7 28
Na-CO2 t-MCNT Composite polymer electrolyte 5000(50 mA·g-1) 400(500 mA·g-1) ~1.75 71
Na-CO2 CMO@CF 1 M NaClO4/TEGDME 8448(200 mA·g-1) 75 ~1.77 58
Na-CO2 CO@CF 1 M NaClO4/TEGDME 7427(200 mA·g-1) ~46 ~1.90 58
Na-CO2 MO@CF 1 M NaClO4/TEGDME 6634(200 mA·g-1) ~44 ~1.85 58
Na-CO2 MWCNTs SN-based electrolyte 7624(50 mA·g-1) 100(200 mA·g-1) ~2.08 107
Na-CO2 Ru@KB 1 M NaClO4/TEGDME 11 537(100 mA·g-1) 130(200 mA·g-1) ~2.0 108
Al-CO2/O2(4∶1) Ketjenblack ([EMIm]Cl/AlCl3 13 000(70 mA·g-1) - - 29
Al-CO2 NPG@Pd AlCl3/([EMim]Cl 26 739.9(333 mA·g-1) 30(333 mA·g-1) 0.091 30
Aqueous Zn-CO2 3D porous Pd double-electrolyte - 100(0.56 mA·cm-2) ~0.19 31
Aqueous Zn-CO2 Ir@Au double-electrolyte - 90(5 mA·cm-2) ~2.2 32
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