Progress in Chemistry

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Applications of Graphene in Hydrogen Evolution Electrocatalyst

Yiming Zhang, Jianping Guo, Jiale Zhang, Aowen Zheng, Yanyan Wang, Guangke Tian

Progress in Chemistry, 2024, 36(5): 633-644. DOI: 10.7536/PC230905

Type		Material	Electrolyte	Initial overpotential(mV)	10 mA/cm² overpotential (mV)	Tafel slope (mV/dec)	Ref
HER electrocatalyst supported by graphene	Supporting metals	Disperse the cobalt onto nitrogen-doped graphene	0.5 M H₂SO₄	30	147	82	51
		Single-atom Ni catalysts anchored to nanoporous graphene	0.5 M H₂SO₄	50	—	45	24
		Mo₂TiC₂ MXene nanosheets with Ni single atoms loaded on the Mo vacancy sites	0.5 M H₂SO₄	—	78	56.7	85
		MoS₂/graphene composite catalyst	0.5 M H₂SO₄	100	183	43.3	86
		MoS₂+graphene mixture		201	365	57.5
		Pure MoS₂		293	>400	114.4
	Supporting nonprecious metal compounds	Vertical MoS₂ nanosheets on graphene	0.5 M H₂SO₄	188	—	84	27
		MoSe₂/rGO hybrid nanostructures	0.5 M H₂SO₄	125	195	67	33
		MoSe₂	0.5 M H₂SO₄	223	390	103	33
		N,S co-doped carbon dots intercalated few-layer MoS₂/graphene nanosheets	0.5 M H₂SO₄	37	98	53	87
Catalytically activated-graphene based HER electrocatalyst	Doping-induced electrocatalytic activity	S,N-doped graphene	0.5 M H₂SO₄	—	280	80.5	10
		B-substituted graphene	0.5 M H₂SO₄	200	440	99	47
		Defective graphene	0.5 M H₂SO₄	300	—	130	47
		N-doped mesoporous graphene	0.5 M H₂SO₄	—	239	109	48
		Ni heterolayer N-doped graphene composite MoS₂	0.5 M H₂SO₄	60	270	56	57
		Nickel heterolayer MoS₂	0.5 M H₂SO₄	285	460	78	57
		Graphene based six membered C-ring dual N-doping	0.5 M H₂SO₄	—	57	44.6	58
		Ultrafine cobalt-ruthenium alloy on nitrogen and phosphorus co-doped graphene	0.5 M H₂SO₄	—	52	38	88
	Strain-induced electrocatalytic activity	Mechanical strain and interfacial-chemical interaction for 1T Co-doped WSe₂/carbon nanotubes	0.5 M H₂SO₄	—	147	33	89
	Strain-induced electrocatalytic activity	Tuning surface lattice strain towards CoPt₂/C truncated octahedron	0.5 M H₂SO₄	—	17	35	90
	Defect-induced electrocatalytic activity	Double defect N-doped graphene	0.5 M H₂SO₄	—	245	141	91
		Single atom S vacancy defect WS₂ nanosheets	0.5 M H₂SO₄	—	137	53.9	92
		Single atom S vacancy defect WS₂ nanosheets loaded on defective graphene	0.5 M H₂SO₄	—	108	48.3	92
Heterogeneous graphene-based HER electrocatalyst		CoFeP/graphene heterostructure	0.5 M H₂SO₄	—	76	—	67
		graphene /CoMo₃S₁₃ sulfur gel heterostructure	0.5 M H₂SO₄	—	130	40.1	68
		MoS₂/ graphene heterostructure	0.5 M H₂SO₄	—	120	72	69
Graphene with different morphologies based-HER electrocatalyst	Zero-dimensional graphene	Coral-shaped MoS₂ decorated with graphene quantum dots	0.5 M H₂SO₄	95	120	40	75
		Coral-shaped MoS₂	0.5 M H₂SO₄	124	173	63	75
		Synthesis of CoP nanoparticles supported on pristine graphene by graphene quantum dots	0.5 M H₂SO₄	7	91.3	42.6	77
		CoP nanoparticles supported on pristine graphene	0.5 M H₂SO₄	118.9	156.89	70.22	77
		graphene quantum dots /MoS₂ microsheets	0.5 M H₂SO₄	—	160	56.9	93
		MoS₂ microsheets	0.5 M H₂SO₄	—	340	93.6	93
		Ultrafine graphene like C₃N₄ quantum dots	0.5 M H₂SO₄	—	208	52	94
	Three-dimensional skeleton graphene	loading of vertical graphene sheets on SiO_x nanowires	0.5 M H₂SO₄	18	107	64	78
		3D interweaved MXene/graphitic carbon nitride nanosheets/graphene nanoarchitectures	0.5 M H₂SO₄	38	—	76	82
		Three-dimensional foliated MoS₂/rGO composite aerogel	0.5 M H₂SO₄	105	—	51	95
		MoS₂	0.5 M H₂SO₄	216	—	89	95
	Encapsulated graphene	Ultrathin graphene shell encapsulated CoNi nanoalloy	0.5 M H₂SO₄	Almost 0	142	104	83
		N-doped graphene encapsulated Ni₃Cu₁ nanoflower	0.5 M H₂SO₄	—	95	77.1	84
		N-doped carbon encapsulated CoP nanoparticles	0.5 M H₂SO₄	—	135	59.3	96
		CoP	0.5 M H₂SO₄	—	231	85.8	96

Table 1 Summary of the HER performance of some graphene-based electrocatalysts

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Fig. 1 Number of SCI papers related to graphene-based hydrogen evolution electrocatalytic materials published from 2018 to 2022
Fig. 2 (A) Schematic illustration of the proposed mechanism for the formation of Pt-CNSs/rGO nanohybrids. (B) TEM image of Pt-CNSs, insets: (a) HRTEM image and (b) FFT pattern of Pt-CNSs. (C) Typical TEM images of Pt-CNSs/rGO nanohybrids. (D) HER polarization curves of Pt-CNSs/rGO nanohybrids and Pt-CNSs in N₂-saturated 0.5 M H₂SO₄ solution at a scan rate of 5 mV/s and rotation rate of 1000 r/min. The top-right inset shows the corresponding Tafel plots for Pt-CNSs/rGO nanohybrids and Pt-CNSs. (E) Electrochemical impedance spectra of Pt-CNSs/rGO nanohybrids and Pt-CNSs^[17]
Fig. 3 (A) Schematic solvothermal synthesis with GO sheets to afford the MoS₂/rGO hybrid. (B) SEM and (inset) TEM images of the MoS₂/RGO hybrid. (C) Schematic solvothermal synthesis without any GO sheets, resulting in large, free MoS₂ particles. (D) SEM and (inset) TEM images of the free particles. (E) TEM image showing folded edges of MoS₂ particles on RGO in the hybrid. The inset shows a magnified image of the folded edge of a MoS₂ nanoparticle. (F) HRTEM image showing nanosized MoS₂ with highly exposed edges stacked on a RGO sheet. Polarization curves (G) and corresponding Tafel plots (H) of different electrocatalysts^[26]
Fig. 4 Low magnification TEM images of N, S co-doped graphene (NSG) (a) and plasma-etched N, S co-doped graphene (P-NSG) (b); high magnification TEM images of NSG (c) and P-NSG (d); SAED patterns of NSG (e) and P-NSG (f); (g) schematic illustration of the synthesis process of P-NSG^[44]
Fig. 5 SEM images of (a) CoFeP and (b) CoFeP/rGO, (d) TEM image and corresponding elemental mapping images (e~i) of CoFeP/rGO. HER performance of CoFeP and CoFeP/rGO composites in the 0.5 M H₂SO₄ solution: (j) HER polarization curves; (k) Overpotentials; (l) Tafel plots; (m) Capacitive current densities; (n) Nyquist plots; (o) i-t curves of CoFeP/rGO at potential of 0.076 V vs RHE^[67]
Fig. 6 LSV curves (A) and Tafel plots (B) of CoP/G⁞GQD, CoP/G, and commercial Pt/C; (C) Nyquist plots of CoP/G⁞GQD and CoP/G measured at an overpotential of 200 mV in a frequency range from 10⁶ to 1 Hz; (D) LSV curves of CoP/G⁞GQD at a scan rate of 2 mV/s before and after 2000 CV cycles at a scan rate of 100 mV/s between -0.17 and +0.01 V. Inset: time dependence of the current density of CoP/ G⁞GQD at an overpotential of 91.3 mV; (E) schematic illustration of the synthesis process of CoP/G⁞GQD^[77]
Fig. 7 Morphological and microstructural analysisof the 3D MX/CN/RGO nanoarchitecture. Representative (a, b) FE-SEM, (c, d) TEM, (e) HAADF-STEM images reveal the successful integration of Ti₃C₂T_x, g-C₃N₄ nanosheets and graphene into a 3D interconnected framework; (f, g) HR-TEM images disclose the lattice fringes of Ti₃C₂T_x and g-C₃N₄ nanosheets; (h) LSV polarization curves and (i) the corresponding Tafel plots^[82]
Fig. 8 (a, b) HRTEM images of CoNi@NC, showing the graphene shells and encapsulated metal nanoparticles. (c) Schematic illustration of the CoNi@NC structure. (d) Statistical analysis of the number of layers in the graphene shells encapsulating the metal nanoparticles in CoNi@NC. (e~h) HAADF-STEM image and corresponding elemental mapping images of CoNi@NC. (i) Gibbs free energy (ΔG) profile of the HER on various catalysts. (j) Volcano plot of the polarized current (i₀) versus ΔG(H^*) for a CoNi cluster, CoNi@C, and an N-doped graphene shell (Ncarbon)^[83]

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