Recent Progress in Carbon-based Materials of Non-Noble Metal Catalysts for ORR in Acidic Environment

doi:10.1007/s40195-021-01229-x

Abstract

Abstract:

Proton exchange membrane fuel cell (PEMFC) has important implications for the success of clean transportation in the future. One of the key factors affecting the cost and performance of PEMFC is the cathode electrocatalyst for the oxygen reduction reaction (ORR) to overcome sluggish kinetics and instability in an acidic environment. As an essential component of the electrocatalyst, the support material largely determines the activity, mass transfer, charge transfer, and durability of the electrocatalyst. Thereby, the support material plays a critical role in the overall performance of the electrocatalyst. Carbon-based materials are widely used as electrocatalyst supports because of their high porosity, conductivity, chemical stability, and tunable morphology. Recently, some new carbon-based materials with excellent structure have been introduced, such as carbon nanotubes, carbon nanowires, graphene, metal-organic framework (MOF)-derived carbon, and biomass-derived carbon materials. Combined with a variety of strategies, such as controllable construction of porous structures and surface defects, proper doping heteroatoms, the ingenious design of model electrocatalysts, and predictive theoretical calculation, a new reliable path was provided for further improving the performance of electrocatalysts and exploring the catalytic mechanism. Based on the topic of carbon-based materials for ORR in acidic medium, this review summarizes the up-to-date progress and breakthroughs, highlights the factors affecting the catalytic activity and stability of ORR electrocatalysts in acids, and discusses their future application and development.

Key words: Carbon-based materials, Non-noble metal electrocatalysts, Acidic environment, Oxygen reduction reaction, Proton exchange membrane fuel cell

Jie Lian, Jin-Yu Zhao, Xiao-Min Wang. Recent Progress in Carbon-based Materials of Non-Noble Metal Catalysts for ORR in Acidic Environment[J]. Acta Metallurgica Sinica (English Letters), 2021, 34(7): 885-899.

Figures/Tables 7

Fig. 1 a Schematic representation of the formation of porous CNT structure. b The as-formed CNT sponge bearing a large extent of deformation without fracture. c Scanning electron microscopy (SEM) image of Fe-CNT sponges (scale bar: 1 μm). The rotating disk electrode (RDE) polarization curves in O2-saturated 0.5 M H2SO4 of d CNT, Fe-CNT, Fe-CNT-ox, Fe-CNT-Py, CNT-PA, Fe-CNT-PA, and Pt/C (20 wt% Pt); and e Fe-CNT-PA compared with commercial Pt/C before and after 10, 000, 20, 000 cyclic voltammetry (CV) cycles. Reproduced with permission from Ref. [52]. Copyright 2015, The Royal Society of Chemistry

Fig. 2 a Schematic representation of the synthesis procedure, b X-ray diffraction (XRD) patterns, c transmission electron microscopy (TEM) image, dhigh-resolution TEM (HRTEM) image, e aberration-corrected high-angle annular dark-field scanning transmission electron microscope (HADDF-STEM) image of Fe1-N-NG/RGO. Reproduced with permission from Ref. [56]. Copyright 2019, Elsevier Ltd.

Fig. 3 a Schematic illustration of creating Fe/N/C model catalysts in MLG. b Atomic force microscopy (AFM) image and corresponding height profile at the folded FeN-MLG marked by the black lines 1 and 2, respectively, c Raman spectra of FeN-MLG with different defect densities, normalized by the G band. d Correlation graph between the mean distance of defects (LD) and the ORR current. e Correlation graph between the percentage of Nx-Fe moiety and the ORR current. Reproduced with permission from Ref. [57]. Copyright 2017, American Chemical Society

Fig. 4 a Schematic representation of the synthesis process of GNR@CNT and the application as ORR catalyst in a PEMFC. b SEM image of GNR@CNT (scale bar: 100 nm). c Linear sweep voltammetry (LSV) curves of GNR@CNT, N-doped GNR@CNT (N-GNR@CNT), and N-doped graphene nanoribbons (N-GNR) for ORR activity in 0.5 M H2SO4. Reproduced with permission from Ref. [35]. Copyright 2018, Springer Nature

Fig. 5 a Schematic illustration of the synthesis, b, c SEM images, d aberration corrected scanning transmission electron microscopy (AC-STEM) image, and e electron energy loss spectrometer (EELS) mapping of FeN4/HOPC-c-1000. Reproduced with permission from Ref. [81]. Copyright 2019, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

Fig. 6 Reproduced with permission from Ref. [102] Copyright 2018, Elsevier Ltd Inner structure of N/Fe-CG a Schematic, b SEM images. Electrochemical characterizations of N-CGFe in 0.1 M HClO4. cRDE polarization curves of N/Fe-CG at different rotating speeds. The inset shows the corresponding Koutecky-Levich (K-L) plots at different potentials. d RDE polarization curves e Tafel plots of C, CG, Fe-CG, N-CG, N/Fe-CG, and Pt/C at 1600 rpm.

Table 1 Characterization and performance of carbon-based catalysts for ORR in an acidic environment

Carbon support [precursor]	Type of catalyst [name]	Elemental analysis	T_pyro (°C)	E_onset (V)	E_1/2 (V)	H₂O₂ yield [n_trans]	P_max [backpressure] (mW·cm^-2)	S_BET (m²·g^-1)	References
[Co-ZIF8@F127]	Co-N-C [Co-N-C@F127]	1.0 at% Co 9.1 at% N	900	0.93	0.84	< 2%	870 [1 bar]	825	[80]
[Fe-ZIF8-polystyrene sphere]	Fe-N-C [FeN₄/HOPC-ZIF8]	Fe 0.33 at% N 4.54 at%	1000	0.9	0.8	1.75% [3.97]	420 [1 bar]	1483.2	[81]
[Co/Zn-ZIF67]	Co-N-C [CoN₃@NC-7-1000]	-	1000	0.82	0.72	~ 6%, [3.87-3.91]	160 [ambient pressure]	-	[104]
[TPI@ZIF8(SiO₂)]	Fe-N-C [TPI@Z8[SiO₂]-650-C]	Fe 3.01wt% N 11.98 wt%	1000	-	0.823	0.9% [3.98]	1180 [2.5 bar]	1648	[79]
[Fe-ZIF8]	Fe-N-C [C-FeZIF-1.44-950]	Fe 1 wt% N 5.51 at%	950	-	0.78	2% [3.97]	775 [30 psig]	1255	[105]
[Mn-ZIF8]	Mn-N-C [20Mn-NC-second]	Mn 3.03 wt% (ICP-MS)N 1.3 at%	1100	-	0.8	< 4%	460 [1 bar]	658	[106]
CNT [Fe-ZIF8]	Fe-N-C [Fe-ZIF’/CNT-1]	Fe 0.8 at% N 5.6 at%	900	-	0.77	-	480 [2 bar]	626	[100]
Black Pearls 2000 [cyanamide, PANI]	Fe-N-C [CM + PANI]-Fe-C	Fe 0.3 at% N 5.0 at%	900	-	0.8	< 2.5% [> 3.95]	940 [2 bar]	~ 1500	[107]
Ketjenblack EC 600JD [phen]	Fe-N-C [Fe²[1.5%] - N - C²-900]	Fe 1.5 wt% N 1.55 at%	900	-	0.79	[3.9]	540 [1.5 bar]	-	[108]
CNF [PAN, DMF]	Co-N-C [Co@SACo-N-C-10]	N 4.91 wt% Co 1.95 wt%	900	0.92	0.778	10%, [3.76]	420 [30 psig]	369.29	[109]
[dicyandiamide, ammonium ferric citrate]	Fe-N-C [Fe-N-C/NH₄Cl]	Fe 5.72 wt% N 5.61 wt%	900	0.831	-	-	270 [2 bar]	495	[110]
[Sodium alginate]	Fe-N-C [SA-Fe-N-1.5-800]	Fe 0.23 at% N 3.76 at%	800	0.941	0.812	< 0.8% [~ 3.99]	-	1190	[111]
[Lignin]	N-S-Cl-C [LN-3-1]	N 3.35 at% S 0.80 at% Cl 0.56 at%	1000	0.892	0.792	< 5% [~ 3.93]	779 [30 psi]	1290	[71]
[melamine-diphenylphosphinic acid]	N-C-P [NPC-4-1100-Zn]	N 6.38 at% P 2.54 at%	1100	0.91	0.79	~ 1% [3.95]	579 [20 psig]	2048	[36]
GNR@CNT	N-C [N-GNR@CNT]	N 3.09 at%	800	0.75	-	[3.72-3.92]	241 [2 bar]	-	[35]
[Flower spikes of Typha orientalis]	N-C NCS-800	N 9.1 at%	800	0.725	-	< 5.5% [3.90-3.98]	-	646	[95]
[Black fungus]	Fe-N-S-C [BF-N-950]	Fe 0.13 wt% N 5.14 wt% S 0.17 wt%	950	-	0.77	[3.9]	255 [2 bar]	916	[96]
Carbon Nanocages	Co-Mo-N-C [Co_0.5Mo_0.5N_y/NCNCs]	Co 0.41 at% Mo 0.30 at% N 7.70 at%	700	0.808	-	~ 12.6% [~ 3.75 ± 0.10]	-	843 (NCNC)	[112]
CNF-Graphene	Fe-N-C [N/Fe-CG]	Fe 0.44 at% N 3.94 at%	900	0.93	0.73	[3.99]	-	290	[102]
Grapheme [PEDOT]	Fe-S-C [P12-900]	Fe 5.3 at% S 2.44 at%	900	0.92	0.78	< 3%	345 [ambient pressure]	1684	[113]

Table 1 Characterization and performance of carbon-based catalysts for ORR in an acidic environment

Carbon support [precursor]	Type of catalyst [name]	Elemental analysis	T_pyro (°C)	E_onset (V)	E_1/2 (V)	H₂O₂ yield [n_trans]	P_max [backpressure] (mW·cm^-2)	S_BET (m²·g^-1)	References
[Co-ZIF8@F127]	Co-N-C [Co-N-C@F127]	1.0 at% Co 9.1 at% N	900	0.93	0.84	< 2%	870 [1 bar]	825	[80]
[Fe-ZIF8-polystyrene sphere]	Fe-N-C [FeN₄/HOPC-ZIF8]	Fe 0.33 at% N 4.54 at%	1000	0.9	0.8	1.75% [3.97]	420 [1 bar]	1483.2	[81]
[Co/Zn-ZIF67]	Co-N-C [CoN₃@NC-7-1000]	-	1000	0.82	0.72	~ 6%, [3.87-3.91]	160 [ambient pressure]	-	[104]
[TPI@ZIF8(SiO₂)]	Fe-N-C [TPI@Z8[SiO₂]-650-C]	Fe 3.01wt% N 11.98 wt%	1000	-	0.823	0.9% [3.98]	1180 [2.5 bar]	1648	[79]
[Fe-ZIF8]	Fe-N-C [C-FeZIF-1.44-950]	Fe 1 wt% N 5.51 at%	950	-	0.78	2% [3.97]	775 [30 psig]	1255	[105]
[Mn-ZIF8]	Mn-N-C [20Mn-NC-second]	Mn 3.03 wt% (ICP-MS)N 1.3 at%	1100	-	0.8	< 4%	460 [1 bar]	658	[106]
CNT [Fe-ZIF8]	Fe-N-C [Fe-ZIF’/CNT-1]	Fe 0.8 at% N 5.6 at%	900	-	0.77	-	480 [2 bar]	626	[100]
Black Pearls 2000 [cyanamide, PANI]	Fe-N-C [CM + PANI]-Fe-C	Fe 0.3 at% N 5.0 at%	900	-	0.8	< 2.5% [> 3.95]	940 [2 bar]	~ 1500	[107]
Ketjenblack EC 600JD [phen]	Fe-N-C [Fe²[1.5%] - N - C²-900]	Fe 1.5 wt% N 1.55 at%	900	-	0.79	[3.9]	540 [1.5 bar]	-	[108]
CNF [PAN, DMF]	Co-N-C [Co@SACo-N-C-10]	N 4.91 wt% Co 1.95 wt%	900	0.92	0.778	10%, [3.76]	420 [30 psig]	369.29	[109]
[dicyandiamide, ammonium ferric citrate]	Fe-N-C [Fe-N-C/NH₄Cl]	Fe 5.72 wt% N 5.61 wt%	900	0.831	-	-	270 [2 bar]	495	[110]
[Sodium alginate]	Fe-N-C [SA-Fe-N-1.5-800]	Fe 0.23 at% N 3.76 at%	800	0.941	0.812	< 0.8% [~ 3.99]	-	1190	[111]
[Lignin]	N-S-Cl-C [LN-3-1]	N 3.35 at% S 0.80 at% Cl 0.56 at%	1000	0.892	0.792	< 5% [~ 3.93]	779 [30 psi]	1290	[71]
[melamine-diphenylphosphinic acid]	N-C-P [NPC-4-1100-Zn]	N 6.38 at% P 2.54 at%	1100	0.91	0.79	~ 1% [3.95]	579 [20 psig]	2048	[36]
GNR@CNT	N-C [N-GNR@CNT]	N 3.09 at%	800	0.75	-	[3.72-3.92]	241 [2 bar]	-	[35]
[Flower spikes of Typha orientalis]	N-C NCS-800	N 9.1 at%	800	0.725	-	< 5.5% [3.90-3.98]	-	646	[95]
[Black fungus]	Fe-N-S-C [BF-N-950]	Fe 0.13 wt% N 5.14 wt% S 0.17 wt%	950	-	0.77	[3.9]	255 [2 bar]	916	[96]
Carbon Nanocages	Co-Mo-N-C [Co_0.5Mo_0.5N_y/NCNCs]	Co 0.41 at% Mo 0.30 at% N 7.70 at%	700	0.808	-	~ 12.6% [~ 3.75 ± 0.10]	-	843 (NCNC)	[112]
CNF-Graphene	Fe-N-C [N/Fe-CG]	Fe 0.44 at% N 3.94 at%	900	0.93	0.73	[3.99]	-	290	[102]
Grapheme [PEDOT]	Fe-S-C [P12-900]	Fe 5.3 at% S 2.44 at%	900	0.92	0.78	< 3%	345 [ambient pressure]	1684	[113]

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