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Progress in Chemistry 2021, Vol. 33 Issue (9): 1598-1613 DOI: 10.7536/PC200817 Previous Articles   Next Articles

• Review •

Application of Element-Doped Carbonaceous Materials in Lithium-Sulfur Batteries

Yun Lu1,2(), Hongjuan Shi1,2, Yuefeng Su1,2(), Shuangyi Zhao1, Lai Chen1,2, Feng Wu1,2,3   

  1. 1 Beijing Key Laboratory, Department of Energy and Environmental Materials, School of Materials Science and Engineering, Beijing Institute of Technology,Beijing 100081, China
    2 Academician's Workshop of New Materials Technology, Chongqing Innovation Center, Beijing Institute of Technology,Chongqing 401135, China
    3 Collaborative Innovation Center for Electric Vehicles in Beijing, Beijing 100081, China
  • Received: Revised: Online: Published:
  • Contact: Yun Lu, Yuefeng Su
  • About author:
    † Yun Lu and Hongjuan Shi contributed equally to this work.
  • Supported by:
    National Natural Science Foundation of China(51802019)
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The blossoming of mobile electronic devices, plug-in electric vehicles and stationary energy storage have triggered the urgent demand for the exploration of the energy storage systems with high energy density and long cycle life. Lithium-sulfur battery is regarded as one of the most promising candidates of the next-generation rechargeable batteries, since the active substance sulfur is low cost and possesses high theoretical energy density of 2600 Wh·kg-1. However, the practical applications of lithium-sulfur battery are hindered by a series of severe problems, which are caused by the insulative nature of sulfur and its discharge products, and the dissolution and shuttling of polysulfides. Carbonaceous materials are generally used as sulfur hosts to improve the conductivity of the cathode. Regrettably, due to the weak interaction between non-polar carbonaceous materials and polar polysulfides, the carbonaceous materials can inhibit polysulfides only by limited physical adsorption and restrictions, thus the dramatic capacity decline derived from the notorious “shuttling effect” remains insufficiently resolved. Introducing polar or chemical adsorption sites to carbonaceous materials by element doping, such as N, S, Co and B doping, can greatly enhance the adsorption capacity of carbonaceous materials to polysulfides, so as to sufficiently improve the cycling stability of the cell. Moreover, element doping may improve the electronic conductivity of carbonaceous materials by changing their electronic structure, thus effectively increasing the utilization ratio of the active materials. This article reviews the elements doping commonly applied in carbonaceous materials such as porous carbon, carbon nanotubes and graphene for lithium-sulfur batteries, wherein single-element doping, dual-element doping, and multi-element doping are introduced separately. The effects of different doping elements on performance of carbonaceous materials are analyzed. And the development direction of element-doped carbonaceous materials in lithium-sulfur batteries are prospected.

Contents

1 Introduction

2 Rational design of element-doped carbon-based materials

3 Single element doping

3.1 Nitrogen-doped

3.2 Boron-doped

3.3 Cobalt-doped

3.4 Others

4 Double element co-doping

4.1 Nitrogen and sulfur co-doped

4.2 Nitrogen and boron co-doped

4.3 Nitrogen and cobalt co-doped

4.4 Nitrogen and nickel co-doped

4.5 Others

5 Multi-element doped carbonaceous materials

6 Conclusions and outlook

Key words: lithium-sulfur battery, element doping, carbonaceous materials, adsorption, shuttle effect
Table 1 Performances of LSBs prepared with mono-doped carbonaceous materials
Material Doping element Element content Sulfur loading
(wt%)		 Initial discharge
capacity / mAh·g-1		 Cycles Capacity retention Binding energy with Li2S4
N-IOP[57] N 3.0 wt% 80% 1162, 0.2 C 150 64% -
NPCMs[58] N 8.9 wt% 65% 1132, 0.1 A·g-1 100 91% -
HNCM[59] N 12.43 at% 1.5 mg·cm-2 902, 0.5 C 1000 89% -
N-CNT[60] N - 61% 1267, 0.2 C 100 64% -
NG[61] N 3.9 wt% 60% 1030, 0.5 C 300 73% 1.48 eV
3DG@NPC[62] N 18 at% 70% 1280, 0.2 C 100 81% -
BMC[64] B 0.78 wt% 59% 750, 3.2 A·g-1 500 74.96% 0.0803 Ha
BUCNTs[65] B 2.1 wt% 70% 1251, 0.2 C 400 60% -
BGA[66] B 1.76 at% 3 mg· cm - 2 1290, 0.2 C 100 77.05% -
B-G/AC[67] B 3.01 wt% 0.7 mg· cm - 2 1387, 0.1 C 100 76.57% -
SC-Co[75] Co 0.7 wt% 63% 1130, 0.5 C 300 74.1% -
Co-CNF[76] Co 9.1 wt% 70% 820, 0.5 C 300 85.36% -
hSCNC[77] S 3.1 at% 77% ~1075, 0.5 A·g-1 100 ~63% 1.1 eV
Fig. 1 Four forms of N doping in graphene[51]. Copyright 2015, Elsevier
Fig. 2 Schematic diagram for preparation of N doped graphene with different N states[56]. Copyright 2012, The Royal Society of Chemistry
Fig. 3 Cycle performance of HNCM700-S, HNCM800-S, and HNCM900-S cathodes for 1000 cycles at 0.5 C[59]. Copyright 2019, WILEY-VCH
Fig. 4 Cyclic voltammogram of SC and SC-Co electrodes at a scan rate of 100 mV·s-1[74]. Copyright 2019, WILEY-VCH
Table 2 Performances of LSBs prepared with dual-element doped carbonaceous materials
Material Doping element Element content Sulfur content
(wt%)		 Initial discharge
capacity/mAh·g-1		 Cycles Capacity retention Binding energy
with Li2S2
NSC[82] N、S - 70% 1280, 0.2 C 100 84.37% 2.59 eV
CNSMC[81] N、S N 5.0 wt%, S 4.6 wt% 54% 1120, 1 C 100 ~71% -
NSHPC[83] N、S N 3.47 wt%, S 4.03 wt% 80% 1549, 0.1 C 100 61.14% -
SN-PCNF[84] N、S - 80% 1133, 0.1 C 150 75% 2.55 eV
N,S-codoped graphene[85] N、S N 5.4 at%, S 3.9 at% 4.6 mg·cm-2 925, 0.5 C 200 72.4% 2.06 eV
N,S-CDs/
rGO[86]		 N、S N 2.9 wt%, S 3.8 wt% 76% 1296, 0.5 C 150 ~69% -
SNGE[87] N、S N 6.01 at%, S 1.15 at% 42.1% 770, 2 C 250 79.48% -
NB-PPCA[88] N、B N 3.64 wt%, B 6.89 wt% 56% 988, 1 C 500 59.4% -
G-NBCL[89] N、B N 5.3 wt%, B 2.9 wt% 70% 829, 2 C 300 82% N=B/N-B, 5.15 eV
NBCGNs[90] N、B N 6.6 at%, B 7.0 at% 65% 977, 0.2 C 300 76% 2.65 eV
C-Co-N[91] N、Co - 56% 917, 0.5 C 500 50.2% -
Co@NHCRs[92] N、Co Co 0.53 at% 60% 971, 0.5 C 100 73% -
MC-NS[93] N、Co N 2.18 wt%, Co 3.88 wt% 86% 1172, 0.2 C 100 77.4% 1.35 eV
Co-N-CNTA[94] N、Co N 8.6 at% 40% 1045, 1 C 1000 77.89% 1.79 eV
CoSA-N-C[95] N、Co N 16.3 at % 74% 1038, 1 C 1000 65% Li2S6, 0.5 eV
Co-N/G[96] N、Co N 7.25 at %, Co 0.77 at % 67% 861, 1 C 500 79% -
Co-N-C/rGO[97] N、Co - 63% 865, 0.5 C 500 71.2% -
MFCH[100] N、Ni N 9.8 wt % 50% 1150, 0.84 A·g-1 100 79% -
Ni@NG[101] N、Ni - 1 mg·c m - 2 826.2, 1 C 500 78% 1.98 eV
N,P-C[102] N、P N 3.6 at %, P 3.2 at % - 1000, 0.1 C 100 70% -
NOPC/S[103] N、O N 2.02 at%, O 8.04 at% 51.6% 1185, 0.2 C 100 64% -
NONPCM[104] N、O N 4.5 wt%, O 9.43 wt% 70% 690, 800 mA·g-1 180 91.7% N-LiSx, 2.52 eV,
MPNC[105] N、O N 6.2 wt%, O 6.89 wt% 70% ~800, 0.35 mA·cm-2 100 95% ＝O-LiSx, 1.47 eV
Fig. 5 The SNGE intercalation schematic diagram[84]. Copyright 2016, Royal Society of Chemistry
Fig. 6 Calculation of the binding energy of Li2S and Li2S4 with the matrix. (a) Binding energy of Li2S on pristine graphene. (b) Binding energy of Li2S at a pyridinic N site. (c) Binding energy of Li2S at a pyrrolic N site. (d) Binding energy of Li2S at an N=B/N-B site. (e) Binding energy of Li2S4 on pristine graphene. (f) Binding energy of Li2S4 at a pyridinic N site. (g) Binding energy of Li2S4 at a pyrrolic N site. (h) Binding energy of Li2S4 at an N=B/N-B site[86]. Copyright 2016, WILEY-VCH
Fig. 7 (a) Electrostatic potential maps of C, N-C, and Co@N-C; (b) DFT calculations showing the interaction between Li-S and various carbon substrates. Gray, blue, celadon, pink, yellow, and white denote C, N, Co, Li, S, and H atoms, respectively[89]. Copyright 2016, Elsevier
Fig. 8 (a~c) The voltage-time profiles of MC-NS/S, C-NS/S, and C-NP/S cathode at 0.1 C for the in situ Raman test. (d~f) Selected original Raman spectra of MC-NS/S, C-NS/S, and C-NP/S for (dis)charge processes[90]. Copyright 2019, WILEY-VCH
Fig. 9 Schematic illustration of the effect of CoSA-N-C in improving the conversion kinetics between the solid (S, Li2S) and liquid (LiPSs), and mediating the deposition of lithium sulfide nanoparticles[92]. Copyright 2020, Elsevier
Fig. 10 Energy profiles for Li sulfides on N/G and Co-N/G[93]. Copyright 2019, American Chemical Society
Fig. 11 Related performance characterization of Ni@NG. (a) Binding energies between the LiPSs and the Ni@NG or NG. (b) The catalytic mechanism of the LiPSs on the surface of Ni@NG in electrochemical process[98]. Copyright 2019, WILEY-VCH
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