Mn3O4 based materials for electrochemical supercapacitors: Basic principles, charge storage mechanism, progress, and perspectives

doi:10.1016/j.jmst.2022.03.036

Abstract

Abstract:

The captivating properties of supercapacitors (SCs) such as high power and reasonably high energy densities made them stand up as a versatile solution to emerging energy storage applications. Thus, everyone is in pursuit of improvisation of the energy storage characteristics of SCs. Hausmannite or manganese oxide (Mn₃O₄) is a widely studied electrode material considering its fascinating features such as high theoretical capacitance (1370 F/g), variable oxidization states, prominent Jahn-Teller effect, broad potential window, environmentally benign and cost-effectiveness. A lot of research has been carried out on this material to unfold and improve its electrochemical aspects. In this review, comprehensive knowledge and innovative attempts taken to improve its energy storage of Mn₃O₄ material are discussed. Firstly, the basic properties concerned with electrochemical charge storage such as valance states, crystal structure, band diagram and energy storage mechanism are discussed, followed by putting forth the limitations of Mn₃O₄. Later on, various strategies adopted to improve the electrochemical attributes of Mn₃O₄ such as making composite with carbon-based materials, metal-based materials, polymers or doping metal atoms are thorough. Finally, remarks on key scientific points and perspectives for further development of energy storage in Mn₃O₄ conclude this review.

Key words: Supercapacitors, Nanostructures, Mn₃O₄ based composites

S.A. Beknalkar, A.M. Teli, T.S. Bhat, K.K. Pawar, S.S. Patil, N.S. Harale, J.C. Shin, P.S. Patil. Mn₃O₄ based materials for electrochemical supercapacitors: Basic principles, charge storage mechanism, progress, and perspectives[J]. J. Mater. Sci. Technol., 2022, 130: 227-248.

Figures/Tables 17

Fig. 1. Ragone plot showing the specific power vs specific energy of various energy storage devices Reproduced with permissions. American Chemical Society Copyright (2014) [6].

Fig. 2. Schematic illustration of various strategies adopted to improve electrochemical attributes of Mn3O4.

Fig. 3. Research papers based on Manganese oxide as supercapacitor (a) number of papers published on different phases of manganese oxide and (b) year-wise published number of research papers on Mn3O4.

Fig. 4. (a) Pourbaix diagram of manganese. Reproduced with permission. Copyright (2019), MDPI, Basel, Switzerland [27]. (b) Hausmannite cell unit with 28 atoms, Mn2+ tetrahedral and Mn3+ octahedral sites (c). Detailed structure of different Mn sites [32]. (d) Schematic view of the energy diagram of Mn and O for both phases in Mn3O4 if Mn 3d orbitals pointing toward the O atom are t2g and the rest are eg: (i) An extracted diagram for Mn 4s, Mn 4p, and O 2p, (ii) An extracted diagram for Mn 3d and O 2p. Reproduced with permission. Copyright 2015, The Physical Society of Japan [34]. (e) Model of the band formation of an oxide semiconductor. Reproduced with permission. Copyright 2015, The Royal Society of Chemistry[35]. Ex-situ high-resolution XAS spectra after (f) the 1st charge of the manganese oxide electrodes compared with the Mn standard compounds Reproduced with permission. Copyright 2017, The Royal Society of Chemistry [39]. (g) Band diagram and charge-switching alignment of an electrochemical supercapacitor electrode [40]. (h) SEM image of the Mn3O4 nanooctahedrons Reproduced with permission. Copyright 2010, The Royal Society of Chemistry [45].

Table 1. Comparison of electrical parameters of tetragonal and cubic phase of Mn3O4.

Phases		Eμ	EA	C	νo(10¹³/s)	Μ (cm²/(V s))
Tetragonal	Melt-grown	0.38	1.04	350	2.4	5.3 × 10⁻³
Tetragonal	Sintered	0.28	1.17	1200	1.4	8.1 × 10⁻³
Cubic		0.52	0.26	2	23	1.3 × 10⁻³

Table 2. Comparison of electrochemical parameters of pristine Mn3O4.

Mn₃O₄ nanostructures
Sr. No.	Morphology	Method of preparation	Electrolyte	Specific capacitance	Capacitive retention (%)	Cycles	Refs.
1	Nanoparticles	Hydrothermal	1 M Li₂SO₄	198 F/g at 0.5 mA/cm²	70	1000	[110]
2	Porous nanostructures	hydrothermal	1 M Na₂SO₄	232 F/g at 0.5 A/g	78	5000	[111]
3	Porous nanospheres	Cathodic electrodeposition	0.5 M Na₂SO₄	253 F/g at 10 mV/s	90	1000	[47]
4	Flowers	e-beam evaporation	1 M Na₂SO₄	568 F/g at 1 A/g	93	5000	[46]
5	Pyramidal grains	e-beam evaporation	1 M Na₂SO₄	754 F/g at 1 A/g	89	4000	[54]
6	Nanograins	SILAR	1 M Na₂SO₄	375 F/g at 5 mV/s	94	4500	[112]
7	Stacked nanosheets	CBD	1 M Na₂SO₄	398 F/g at 5 mV/s	82	2000	[113]
8	Microspheres	Modified solvothermal	1 M Na₂SO₄	302 F/g at 0.5 A/g	89	5000	[48]
9	Nanoparticles	simple chemical precipitation	1 M Na₂SO₄	322 F/g at 0.5 mA/cm²	77	1000	[51]
10	Nanoparticles	microwave assisted reflux method	1 M Na₂SO₄	135 F/g at 2 mV/s	-	-	[114]
11	Nanorods	cathodic electrodeposition	1 M Na₂SO₄	321F/g at 2 mV/s	91	1000	[43]
12	Nano-octahedrons	Hydrothermal synthesis	1 M Na₂SO₄	322 F/g at 5 mV/s	-	-	[45]
13	Porous plates	Cathodic electrodeposition	1 M Na₂SO₄	341F/g at 2 mV/s	6	1000	[44]
14	Porous cauliflowers	Hydrothermal treatment	1 M Na₂SO₄	401 F/g at 10 mV/s	91	1000	[115]

Fig. 5. Survey about different strategies developed by researchers to improve the performance of pristine Mn3O4. (*note- M-carbon- Mn3O4/carbon-based composite; M-oxide- Mn3O4/oxide-based composite; M-Polymer- Mn3O4/polymer hybrid composite; M-doping- Doping of metal atoms in Mn3O4; M-Mn3O4; CNT-carbon nanotube, G- graphene, rGO- reduced graphene oxide, CNF-carbon nanofibers, OCa- other carbon-based; BO- binary oxide, OH- Hydroxide, MS- Metal sulphides).

Fig. 6. (a) TEM images of Mn3O4/MWCNT Reproduced with permission. Copyright 2014, Korean Chemical Society [68]. (b) Cycling behavior of 25 MWCNT/Mn3O4 composite and Mn3O4 nanomaterial measured at 1 A/g current density. (c) A plot of energy density Vs power density for MWCNT/Mn3O4 composite and Mn3O4 nanomaterial. Reproduced with permission. Copyright 2015, The Royal Society of Chemistry [69]. (d) Schematic illustration and (i-iv) FE-SEM images of Mn3O4@CNT nano-clusters, and (i) EDX spectrum and (ii-iv) elemental mapping of Mn3O4@CNT nano-clusters. Reproduced with permission. Copyright (2018), The Royal Society of Chemistry and the Center National de la Recherche Scientifique [70]. (e) Schematic illustration of CNT-Fe3O4//CNT- Mn3O4 ASC device. (f) A single ASC powering a Red LED, while shows the tandem ASC device lighting a Blue LED and demonstrates three series-connected ASC devices employed for charging a Samsung mobile phone. Reproduced with permission. Copyright (2018), American Chemical Society [71]. (g, h) Porous graphene@Mn3O4. Reproduced with permission. Copyright (2018), American Chemical Society [72]. (i) Galvanostatic charge-discharge curves at a current density of 0.5 A/g. (j) Specific capacitance from capacitive charge and Faradaic charge and corresponding Faradaic capacitance ratio. (k) Variations of the peak intensity ratio of IC-O-Mn/IMn-O and Faradaic contribution ratio vs. rGO content (l). The power density vs. energy density curves of as-prepared M/rGO-2//AC asymmetric supercapacitor compared to the data for other devices (The inset illustrates the prepared M/rGO-2//AC asymmetric supercapacitor lighting the LED). Reproduced with permission. Copyright (2019), American Chemical Society [73].

Fig. 7. (a) TEM image of Mn3O4-GO, The inset is a magnified image of one double-shell hollow sphere. (b) CV curves of Mn3O4-GO double shells hollow spheres and the pure Mn3O4 nanoparticles at a scan rate of 50 mV/s. (c) The plot of the relationship between the specific capacitance and scan rate. Reproduced with permission. Copyright 2016, Elsevier Ltd. [79]. SEM images of Mn3O4 NWs grown on CF at (d) 20 μm (e) 200 nm magnification. (f) Capacitance retention at different bending angles of the supercapacitor [inset digital images of supercapacitor (i) bend at 180° (scale bar = 2 cm), (ii) twisted on a finger (scale bar = 2 cm), and (iii) weaved on a textile fabric glove (scale bar = 2 cm)) Reproduced with permission. Copyright (2019), American Chemical Society [82]. (g) Cyclic voltammetry (CV) curves at a scan rate of 80 mV/s. (h) Galvanostatic charge-discharge (GCD) curves at 0.5 A/g of Mn3O4/PCM and bare Mn3O4. (i) Nyquist plots of Mn3O4/PCM and bare Mn3O4. Reproduced with permission. Copyright (2018), MDPI, Basel, Switzerland [84].

Fig. 8. (a) SEM images of Mn3O4 TB/NHPC composite. (b) TEM images of Mn3O4 TB/NHPC composite Reproduced with permission. Copyright (2020), Elsevier B.V. [85]. (c) Illustration of the fabrication of ordered porous Mn3O4@N-doped carbon/graphene hybrids. (d) Galvanostatic charge-discharge curves of MCG-2 at different current densities from 1 to 20 A/g. (e) Nyquist plots for MCG-2 and Mn3O4. Inset shows the magnified view of the Warburg semicircles in the spectra. Reproduced with permission. Copyright 2016, Springer Nature [86]. (f) Schematic illustration of the fabrication processes for NPCM/Mn3O4. (g) SEM morphologies of the NPCM/ Mn3O4 sample. Reproduced with permission. Copyright (2019), Elsevier Ltd. [87].

Table 3. Comparison of electrochemical parameters of Mn3O4/carbon-based composite.

Mn₃O₄-Carbon based nanocomposites
Sr. No.	Material	Electrolyte	Specific capacitance	Capacitive retention (%)	Cycles	Energy density	Power density	Refs.
1	Mn₃O₄@MWCNT	1 M Na₂SO₄	257 F/g at 5 mV/s	85	1000	-	-	[68]
2	Mn₃O₄@MWCNT		441 F/g at 2 mV/s	98	1000	54.95 Wh/kg	500 W/kg	[69]
3	Mn₃O₄@CNT	1 M Na₂SO₄	81.9 F/g at 0.6 A/g	87	1000	-	-	[70]
4	Mn₃O₄- CNT (cathode) Fe₃O₄- CNT (anode)	1 M Na₂SO₄	135.2 F/g at 10 mV/s	100	15,000	31.4 Wh/kg	10.3 kW/kg	[71]
5	Mn₃O₄@MWCNT	0.5 M Na₂SO₄	2.8 F/cm² at 2 mV/s	-	-	29 Wh/kg	159 W/kg	[74]
6	Mn₃O₄- rGO	1 M Na₂SO₄	228 F/g at 5 A/g	95	500	82 Wh/kg	7097 W/ kg	[116]
7	Mn₃O₄-G	1 M Na₂SO₄	270.6 F/g at 0.2 A/g	91	1500	-	-	[117]
8	Mn₃O₄-G	1 M Na₂SO₄	312 F/g at 0.5 mA/cm²	76	1000	-	-	[118]
9	Mn₃O₄-G	1 M Na₂SO₄	271.5 F/g at 0.1 A/g	100	20,000	-	-	[119]
10	Mn₃O₄-G	6 M KOH	256 F/g at 5 mV/s	-		-	-	[120]
11	Mn₃O₄- rGO	1 M Na₂SO₄	351 F/g at 0.5 A/g	80.1	10,000	36.76 Wh/kg	0.5 kW/ kg	[121]
12	Mn₃O₄-G	1 M Na₂SO₄	22.5 F/g at 5 A/g	100	1000	-	-	[122]
13	Mn₃O₄-G	1 M Na₂SO₄	317 F/g at 10 mV/s	100	4000	-	-	[123]
14	Mn₃O₄-G	1 M Na₂SO₄	208 F/g at 0.5 A/g	86	2000	30.1 Wh/kg	9500 W/kg	[72]
15	Mn₃O₄-G	-	315 F/g at 0.5 A/g	105	5000	-	-	[73]
16	Mn₃O₄-G	1 M K₂SO₄	260 F/g at 50A/g	92-94	1000	6.4 Wh/ kg	0.4 kW/ kg	[75]
17	Mn₃O₄- rGO	6 M KOH	409 F/g at 0.5 A/g,	92	3000	-	-	[76]
18	Mn₃O₄- rGO	PVA/H₃PO₄	311 F/cm³ at 300 mA/ cm³	85	10,000	4.05 mWh/cm³	268 mW/ cm³	[77]
19	Mn₃O₄/CNT/G/	]−CH₂−CH(CO₂K)−]_n./KCl	220F/g at 10 A/g	86	10,000	32.7 Wh/kg)	-	[78]
20	Mn₃O₄-CNF	1 M Na₂SO₄	300.7 F/g	100	7500	-	-	[82]
21	Mn₃O₄-CNF	1 M Na₂SO₄	313 F/g at 0.5 A/g	94	5000	18 Wh/kg	-	[83]
22	Mn₃O₄-CNF	1 M Na₂SO₄	140.5 F/g at 0.25 A/g	90.3	5000	27.13 Wh/Kg	0.41 kW/Kg	[84]
23	Mn₃O₄-PC	1 M Na₂SO₄	366 F/g at 0.5 A/g	97	10,000	34.7 Wh/Kg	450 W/Kg	[85]
24	Mn₃O₄/N-C/G/	1 M Na₂SO₄	456 F/g at 1 A/g	98.1	2000	-	-	[86]
25	Mn₃O₄-C	1 M Na₂SO₄	384 F/g at 0.5 A/g	99	5000	16 Wh/Kg	207 W/Kg	[87]
26	Mn₃O₄-C	1 M Na₂SO₄	522 F/g at 1 A/g	100	1400	58.72 W h/kg	451.6 W/kg	[88]
27	Mn₃O₄-C	5 M LiCl	430 F/g at 1 mV/s	93.15	10,000	13.5 Wh /kg	0.3 kW/kg	[124]
28	Mn₃O₄-G	0.5 M Na₂SO₄	225 F/g at 5 mV/s	99.5	6000	34.1 Wh/kg	251 W/kg	[79]

Table 3. Comparison of electrochemical parameters of Mn3O4/carbon-based composite.

Mn₃O₄-Carbon based nanocomposites
Sr. No.	Material	Electrolyte	Specific capacitance	Capacitive retention (%)	Cycles	Energy density	Power density	Refs.
1	Mn₃O₄@MWCNT	1 M Na₂SO₄	257 F/g at 5 mV/s	85	1000	-	-	[68]
2	Mn₃O₄@MWCNT		441 F/g at 2 mV/s	98	1000	54.95 Wh/kg	500 W/kg	[69]
3	Mn₃O₄@CNT	1 M Na₂SO₄	81.9 F/g at 0.6 A/g	87	1000	-	-	[70]
4	Mn₃O₄- CNT (cathode) Fe₃O₄- CNT (anode)	1 M Na₂SO₄	135.2 F/g at 10 mV/s	100	15,000	31.4 Wh/kg	10.3 kW/kg	[71]
5	Mn₃O₄@MWCNT	0.5 M Na₂SO₄	2.8 F/cm² at 2 mV/s	-	-	29 Wh/kg	159 W/kg	[74]
6	Mn₃O₄- rGO	1 M Na₂SO₄	228 F/g at 5 A/g	95	500	82 Wh/kg	7097 W/ kg	[116]
7	Mn₃O₄-G	1 M Na₂SO₄	270.6 F/g at 0.2 A/g	91	1500	-	-	[117]
8	Mn₃O₄-G	1 M Na₂SO₄	312 F/g at 0.5 mA/cm²	76	1000	-	-	[118]
9	Mn₃O₄-G	1 M Na₂SO₄	271.5 F/g at 0.1 A/g	100	20,000	-	-	[119]
10	Mn₃O₄-G	6 M KOH	256 F/g at 5 mV/s	-		-	-	[120]
11	Mn₃O₄- rGO	1 M Na₂SO₄	351 F/g at 0.5 A/g	80.1	10,000	36.76 Wh/kg	0.5 kW/ kg	[121]
12	Mn₃O₄-G	1 M Na₂SO₄	22.5 F/g at 5 A/g	100	1000	-	-	[122]
13	Mn₃O₄-G	1 M Na₂SO₄	317 F/g at 10 mV/s	100	4000	-	-	[123]
14	Mn₃O₄-G	1 M Na₂SO₄	208 F/g at 0.5 A/g	86	2000	30.1 Wh/kg	9500 W/kg	[72]
15	Mn₃O₄-G	-	315 F/g at 0.5 A/g	105	5000	-	-	[73]
16	Mn₃O₄-G	1 M K₂SO₄	260 F/g at 50A/g	92-94	1000	6.4 Wh/ kg	0.4 kW/ kg	[75]
17	Mn₃O₄- rGO	6 M KOH	409 F/g at 0.5 A/g,	92	3000	-	-	[76]
18	Mn₃O₄- rGO	PVA/H₃PO₄	311 F/cm³ at 300 mA/ cm³	85	10,000	4.05 mWh/cm³	268 mW/ cm³	[77]
19	Mn₃O₄/CNT/G/	]−CH₂−CH(CO₂K)−]_n./KCl	220F/g at 10 A/g	86	10,000	32.7 Wh/kg)	-	[78]
20	Mn₃O₄-CNF	1 M Na₂SO₄	300.7 F/g	100	7500	-	-	[82]
21	Mn₃O₄-CNF	1 M Na₂SO₄	313 F/g at 0.5 A/g	94	5000	18 Wh/kg	-	[83]
22	Mn₃O₄-CNF	1 M Na₂SO₄	140.5 F/g at 0.25 A/g	90.3	5000	27.13 Wh/Kg	0.41 kW/Kg	[84]
23	Mn₃O₄-PC	1 M Na₂SO₄	366 F/g at 0.5 A/g	97	10,000	34.7 Wh/Kg	450 W/Kg	[85]
24	Mn₃O₄/N-C/G/	1 M Na₂SO₄	456 F/g at 1 A/g	98.1	2000	-	-	[86]
25	Mn₃O₄-C	1 M Na₂SO₄	384 F/g at 0.5 A/g	99	5000	16 Wh/Kg	207 W/Kg	[87]
26	Mn₃O₄-C	1 M Na₂SO₄	522 F/g at 1 A/g	100	1400	58.72 W h/kg	451.6 W/kg	[88]
27	Mn₃O₄-C	5 M LiCl	430 F/g at 1 mV/s	93.15	10,000	13.5 Wh /kg	0.3 kW/kg	[124]
28	Mn₃O₄-G	0.5 M Na₂SO₄	225 F/g at 5 mV/s	99.5	6000	34.1 Wh/kg	251 W/kg	[79]

Fig. 9. (a) Comparative charge/discharge study of VM-1, VM-2, VM-3, VM-4, V2O5 and Mn3O4 at a current density of 5 A/g. (b) EIS study of VM-1, VM-2, VM-3, VM-4, rGO, V2O5 and Mn3O4. Reproduced with permission. Copyright (2019), Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim [89]. (c) SEM images of the Mn3O4-Co3O4 products after heat treatment at 450 °C for 30 min. (d) TEM images of Mn3O4-Co3O4 Reproduced with permission. Copyright (2012), The Royal Society of Chemistry [92]. (e) Schematic representation for the microwave-assisted formation of Mn3O4-Fe2O3/Fe3O4@rGO ternary hybrids. Reproduced with permission. Copyright (2019), Elsevier B.V. [95]. (f) Low and high magnification SEM images for MNN-12. (g) EDX mapping of Ni, Co, Mn, and O for MNN-12 Reproduced with permission. Copyright (2019), Elsevier Ltd [96]. (h) CV plots at 5 mV/s for Mn-5, Ni-5, MnNi-5, and MnNi-12 in 1 M KOH electrolyte Reproduced with permission. Copyright 2017, Elsevier Ltd [100].

Fig. 10. (a) Schematic illustration for the formation of MoS2/Mn3O4 nanostructure. The black sheets represent MoS2 nanosheets and the orange ball represents Mn3O4 nanoparticles. (b) Low TEM image of MoS2 Reproduced with permission. Copyright 2016, Elsevier Ltd. [102]. (c) Schematic illustration for the fabrication of Mn3O4/MnS. (d) TEM image of Mn3O4/MnS heterostructures building multi-shelled hollow microspheres. (e) Electrochemical performance of the samples for supercapacitors. CV curves of all samples at the scan rate of 50 mV/s. (f) Nyquist plots in a frequency range from 0.1 Hz to 100 kHz for Mn2O3, Mn3O4, Mn3O4/MnS, and MnS. (g) Cycling performance at a constant current density of 10 A/g. Reproduced with permission. Copyright (2019), Elsevier B.V [103]. (h) TEM image of AgNW@Mn3O4. (i) CV plots of the AgNW@Mn3O4 and Mn3O4 electrodes at the same scan rate. (j) Capacitance retention of the ASC device with cycle numbers (a red LED powered by the ASC device shown in the inset). Reproduced with permission. Copyright 2017, Wiley‐VCH Verlag GmbH & Co. KGaA, Weinheim [24].

Table 4. Comparison of electrochemical parameters of Mn3O4/metal-based composite.

Mn₃O₄-metal based nanocomposites
Sr. No.	Material	Electrolyte	Specific capacitance	Capacitive retention (%)	Cycles	Energy density (Wh/kg)	Power density (W/kg)	Refs.
1	Mn₃O₄/V₂O₅	-	1008 F/g at 5 A/g	111	5000	44.9	1.76	[89]
2	Mn₃O₄/V₂O₅	1 M Na₂SO₄ -PVA	768 F/g at 2mV/s	-		-	-	[90]
3	Mn₃O₄/TiO₂	1 M Na₂SO₄	570 F/g at 1 A/g	91.8	2000	-	-	[91]
4	Co₃O₄/Mn₃O₄	1 M Na₂SO₄	450 F/g at 2 mV/s	98	2000	85.6	333	[92]
5	Mn₃O₄/Ni(OH)₂	1 M KOH	742 F/g at 1 A/g			15.3	168.8	[99]
6	Mn₃O₄/Fe₃O₄-G	1 M Na₂SO₄	58.46 F/g at 50 mV/s	100	5000	-	-	[93]
7	Mn₃O₄-Au-Fe₂O₃-	0.5 M H₂SO₄	580 F/g at 1 A/g	89	2000	36.12	1994	[94]
8	Mn₃O₄-Fe₂O₃/Fe₃O₄@rGO	1.0 M KOH	590.7 F/g at 5 mV/s	64.5	1000	-	-	[95]
9	NiCo-LDH/Mn₃O₄	3 M KOH	1034.33 C/g at 1 mA/cm²	82	5000	57.03	765.8	[98]
10	Mn₃O₄@NiCo₂O₄@NiO	2 M KOH	1905 F/g at 1 A/g	92	10,000	76.8	800	[96]
11	Mn₃O₄-NiO-Co₃O₄	0.5 M KOH/0.04 M K₃Fe(CN)₆	7404 F/g at 20 A/g	82	1800	1028	99 k	[97]
12	Mn₃O₄/ Cr₂O₃	1 M KOH	494 F/g at 5 mA/cm²	-		-	-	[58]
13	Mn₃O₄-CeO₂	1 M Na₂SO₄	310 F/g at 2 A/g	92	1000	-	-	[125]
14	Mn₃O₄/Ni(OH)₂	1 M KOH	707 F/g at 1 A/g	89	2000	17.8	162	[100]
15	Mn₃O₄/ZnMn₂O₄	1 M Na₂SO₄	321 F/g at 1 mV/s	93	2000	-	-	[25]
5	Mn₃O₄/MnS	2 M KOH	744 F/g at 20 A/g	97.7	10,000	65.8 Wh /kg	16000 W/kg	[126]
17	MoS₂/Mn₃O₄	1 M Na₂SO₄	119 F/g at 1 A/g	69.3	2000	-	-	[102]
18	Ag@Mn₃O₄	0.5 M Na₂SO₄	203 F/g at 0.25 A/g	94	5000	28 Wh/kg	320 W/kg	[24]

Fig. 11. (a) SEM image of Mn3O4/PANI hydrogel with different Mn3O4/PANi. (b) EIS spectra of Mn3O4, PANi, Mn3O4/PANi-A, and Mn3O4/PANi-B electrodes. (c) Cycling performance of different electrodes measured at 10 A/g for 2000 cycles. Reproduced with permission. Copyright (2018), Springer Nature [104]. (d) A fabrication process for the growth of Mn3O4 nanoparticles on activated carbon via employing polyaniline layer as the structural/interface coupling bridge. Reproduced with permission. Copyright (2021), Elsevier B.V [105]. (e) galvanostatic charge-discharge of Mn3O4-GO, Mn3O4-GO-PANi with stirring, and Mn3O4-GOPANi without stirring (1:0.5) at current density 0.3 A/g Reproduced with permission. Copyright (2019), Springer-Verlag GmbH Germany [107]. (f) SEM image and (g) TEM image of PANI@Mn3O4/GNP-CF after PANI coating. Reproduced with permission. Copyright (2019), Wiley‐VCH Verlag GmbH & Co. KGaA, Weinheim [108].

Table 5. Comparison of electrochemical parameters of Mn3O4/polymer-based hybrid composite and doping of metal atoms in Mn3O4.

Sr. No.	Material	Electrolyte	Specific capacitance	Capacitive Retention (%)	Cycles	Energy density (Wh/kg)	Power density 0 (W/kg)	Refs.
Mn₃O₄-polymer-based hybrid nanocomposites
1	Mn₃O₄/PANI	6 M KOH	422 F/g at 0.5 A/g	89	2000	-	-	[104]
2	Mn₃O₄/G/PANI	1 M H₂SO₄	660 F/g at 0.2 A/g	89	4000	23	600	[106]
3	Mn₃O₄/GO/PANI	1 M H₂SO₄	829.27 F/g at 0.3 A/g	94	1800	121	891	[107]
4	Mn₃O₄/PANI/AC	6 M KOH	352 F/g at 0.5 A/g	90	10,000	33.8	152	[105]
5	Mn₃O₄- G-PANI	1 M H₂SO₄	452 F/g at 1 mV/s	89	1000	-	-	[108]
Doping of metal atoms in Mn₃O₄
6	Cr- Mn₃O₄	1 M Na₂SO₄	272 F/g at 0.5 A/g	70	1000	-	-	[60]
	Co- Mn₃O₄		209 F/g at 0.5 A/g	-	-
	Ni- Mn₃O₄		184 F/g at 0.5 A/g	-	-
	Cu- Mn₃O₄		134 F/g at 0.5 A/g	-	-
7	Sn-Mn₃O₄/G	6 M KOH	216 F/g at 5 A/g	93	10,000	-	-	[109]

Fig. 12. (a) TEM and HRTEM images of pristine Mn3O4 nanocrystals. The insets show the SAED patterns. (b) Representative CV curves of doped Mn3O4 nanocrystals at a scan rate of 10 mV/s. (c) Nyquist plots of pristine and doped Mn3O4 electrodes. Inset is the equivalent circuit. Reproduced with permission. Copyright 2013, American Chemical Society [60]. (d) TEM picture of Sn-Mn3O4/C. (e) Galvanostatic charge/discharge curves of Mn3O4, Sn-Mn3O4, and Sn-Mn3O4/C at 0.5 A/g. Reproduced with permission. Copyright 2013, Elsevier B.V. [109].

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Mn₃O₄ based materials for electrochemical supercapacitors: Basic principles, charge storage mechanism, progress, and perspectives

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