Unleashing the versatility of porous nanoarchitectures: A voyage for sustainable electrocatalytic water splitting

doi:10.1016/S1872-2067(23)64581-4

Chinese Journal of Catalysis ›› 2024, Vol. 58: 37-85.DOI: 10.1016/S1872-2067(23)64581-4

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Unleashing the versatility of porous nanoarchitectures: A voyage for sustainable electrocatalytic water splitting

Jian Yiing Loh^a^,^b, Joel Jie Foo^a^,^b, Feng Ming Yap^a^,^b, Hanfeng Liang^c, Wee-Jun Ong^a^,^b^,^c^,^d^,^e,*()

^aSchool of Energy and Chemical Engineering, Xiamen University Malaysia, Selangor Darul Ehsan 43900, Malaysia
^bCenter of Excellence for NaNo Energy & Catalysis Technology (CONNECT), Xiamen University Malaysia, Selangor Darul Ehsan 43900, Malaysia
^cState Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China
^dGulei Innovation Institute, Xiamen University, Zhangzhou 363200, Fujian, China
^eShenzhen Research Institute of Xiamen University, Shenzhen 518057, Guangdong, China

Received:2023-08-24 Accepted:2023-11-13 Online:2024-03-18 Published:2024-03-28
Contact: *E-mail: weejun.ong@xmu.edu.my (W.-J. Ong).
About author:Wee-Jun Ong received his B.Eng. and Ph.D. in chemical engineering from Monash University. He is a Professor and Assistant Dean in School of Energy and Chemical Engineering at Xiamen University Malaysia. Starting from 2021, he serves as the Director of Center of Excellence for NaNo Energy & Catalysis Technology (CONNECT). Previously, he was a scientist at Agency for Science, Technology and Research (A*STAR), Singapore. In 2019, he was a visiting scientist at Technische Universität Dresden and a visiting professor at Lawrence Berkeley National Laboratory. His research interests include nanomaterials for energy storage devices, photocatalytic, photoelectrocatalytic, and electrochemical H₂O splitting, CO₂ reduction and N₂ fixation. For more details, refer to https://sites.google.com/site/wjongresearch/.
Supported by:
National Natural Science Foundation of China(22202168);Guangdong Basic and Applied Basic Research Foundation(2021A1515111019);State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University(2023X11);Xiamen University Malaysia Investigatorship(IENG/0038);Xiamen University Malaysia Research Fund(ICOE/0001);Xiamen University Malaysia Research Fund(XMUMRF/2021-C8/IENG/0041)

Abstract

Abstract:

Electrochemical overall water splitting (OWS) has drawn much research fascination as a promising technology for energy conversion to produce clean hydrogen fuel as sustainable chemical resources. However, half reaction of the water splitting reaction, which is oxygen evolution reaction (OER) is the main challenge due to the sluggish kinetics and large thermodynamic barrier. Porous-based materials can markedly enhance the accessibility of active sites, increase specific surface area and optimize the adsorption/desorption of reactants. The enhanced activity arising from the porous materials is attributed to the increase in active sites and improved mass transfer. Herein, the recent research advances made in porous electrocatalysts for hydrogen evolution reaction (HER), oxygen evolution reaction (OER) and OWS are reviewed. This review focuses on the recent advancements in the synthesis strategies, incorporated with the unique roles of porous structure in electrocatalysts are discussed. For boosting the activity, various emerging modification strategies on porous electrocatalysts, covering structure engineering, phase engineering, defect engineering and strain engineering are presented. This review emphasizes on the synthesis methods, how porous materials improve the performance, mechanistic understanding, integrated experiments, theoretical studies in water splitting, advanced modification strategies and proposed synthesis processes. Specially, the structural-activity relationship gives insights into designing and modifying the porous-based materials with unique properties. Finally, the current science challenges and direction for the future development of porous electrocatalysts are highlighted.

Key words: Porous materials, Electrocatalysis, Hydrogen evolution reaction, Oxygen evolution reaction, Water splitting

Jian Yiing Loh, Joel Jie Foo, Feng Ming Yap, Hanfeng Liang, Wee-Jun Ong. Unleashing the versatility of porous nanoarchitectures: A voyage for sustainable electrocatalytic water splitting[J]. Chinese Journal of Catalysis, 2024, 58: 37-85.

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Figures/Tables 37

Fig. 1. Schematic illustration of process of reaction occurs over the catalyst surface (a) and porous electrocatalyst (b).

Fig. 2. Number of annual publications and citations since 2015, sourced from the Web of Science database with the topic keyword “porous” and “electrocatalyst*” and “hydrogen evolution reaction” or “oxygen evolution reaction” or “water splitting” dated on 15th May 2023.

Fig. 3. Timeline of recent advancement of porous electrocatalysts in overall water splitting from 2015 to the present year: 2015. Reproduced with permission from Ref. [43]. Copyright 2015, American Chemical Society; 2016. Reproduced with permission from Ref. [44]. Copyright 2016, Wiley; 2018. Reproduced with permission from Ref. [45]. Copyright 2018, Wiley.; 2019. Reproduced with permission from Ref. [46]. Copyright 2019, Wiley.; 2020. Reproduced with permission from Ref. [47]. Copyright 2020, Wiley.; 2021. Reproduced with permission from Ref. [48]. Copyright 2021, Elsevier.; 2022. Reproduced with permission from Ref. [49]. Copyright 2022, Wiley.; 2023. Reproduced with permission from Ref. [50]. Copyright 2023, Royal Society of Chemistry.

Fig. 4. Overview of synthesis, modification strategies and electrocatalytic applications of porous electrocatalysts.

Fig. 5. (a) Trasatti volcano plot for HER in acid solutions. Reproduced with permission from Ref. [65]. Copyright 2014, Beilstein Institute for the Advancement of Chemical Sciences. (b) DFT derived “volcano” plot for HER provided by N?rskov group. Reproduced with permission from Ref. [61]. Copyright 2016, Wiley. (c) Schematic illustration of d-band center theory model. Reproduced with permission from Ref. [63]. Copyright 2011, National Academy of Sciences.

Fig. 6. Mechanisms of HER (a) and Mechanisms of OER (b) on the surface of electrocatalysts in alkaline and acidic medium. (c) Volcano plot of ηthe against standard free energy of ΔGMO?ΔGMOH. Reproduced with permission from Ref. [70]. Copyright 2021, Elsevier.

Fig. 7. Schematic illustration of desired electrocatalysts with highly active catalytic sites.

Fig. 8. (a) Schematic diagram of the in situ XRD cell and detection principle. Reproduced with permission from Ref. [84]. Copyright 2020, Wiley. (b) In situ XRD discharging and charging intensity map. Reproduced with permission from Ref. [91]. Copyright 2022, Elsevier. (c) Schematic diagram of in situ Raman cell. (d) In situ Raman spectra for NiFe foam. Reproduced with permission from Ref. [85]. Copyright 2021, Elsevier. (e) Free energy diagram from DFT calculations. Reproduced with permission from Ref. [88]. Copyright 2023, Elsevier.

Fig. 9. (a) Schematic synthesis progress of vertically aligned nanosized MoS2/N-rGO catalysts. (b) SEM image of MoS2/N-rGO catalyst. (c) SEM images of MoS2/N-rGO composites with different amounts of NH3H2O: 0.25 mL. Reproduced with permission from Ref. [107]. Copyright 2017, Elsevier. (d) Schematic illustration of the synthesis of (MoS2/NiS2/CC). Reproduced with permission from Ref. [106]. Copyright 2021, Elsevier.

Fig. 10. (a) Illustration of the fabrication procedure of (Ni0.33Co0.67) S2 NWs/CC. Reproduced with permission from Ref. [114]. Copyright 2018, American Chemical Society. (b) Synthesis illustration of Co-NiSe/NF nanoflower. Reproduced with permission from Ref. [116]. Copyright 2020, Elsevier. FESEM (c) and TEM (d) image of nickel telluride. Reproduced with permission from Ref. [118]. Copyright 2017, Elsevier.

Fig. 11. Synthesis process (a) and SEM image (b) of Mo0.84Ni0.16-Mo2C@NC nanosphere. Reproduced with permission from Ref. [121]. Copyright 2021, Elsevier. Schematic diagram (c) and TEM image (d) of N-Mo2C@C. Reproduced with permission from Ref. [122]. Copyright 2022, Elsevier.

Fig. 12. (a) Schematic Illustration of the hydrothermal synthesis of a self-supported, flexible composite electrode. (b) SEM image of the 3D electrode. Reproduced with permission from Ref. [125]. Copyright 2017, Royal Society of Chemistry. (c) Schematic diagram of the process and (d) SEM image of urchin-like peapod NiCo2O4@C. Reproduced with permission from Ref. [127]. Copyright 2017, Elsevier. Schematic diagram of the preparation process (e) and SEM image for CoP@NCNFs (f). Reproduced with permission from Ref. [128]. Copyright 2022, Elsevier.

Fig. 13. (a) Schematic illustration for the fabrication of Co3O4/Co-NPC hybrid. (b) SEM image of Co3O4/Co-NPC hybrid. Reproduced with permission from Ref. [133]. Copyright 2018, Elsevier. (c) Schematic illustration of the preparation of porous nanoscale NiO/NiCo2O4 heterostructure. (d) SEM image of NiO/NiCo2O4 heterostructure. Reproduced with permission from Ref. [135]. Copyright 2019, Elsevier. (e) Brief synthesis process of CS-Co/Cs. Reproduced with permission from Ref. [136]. Copyright 2017, American Chemical Society.

Fig. 14. (a) Schematic Illustration of the synthesis process. SEM (b) and TEM (c) images of CoP/NCNHP catalyst. Reproduced with permission from Ref. [139]. Copyright 2018, American Chemical Society. (d) Schematic illustration of the synthesis and structure. TEM (e), SEM (f), and HRTEM (g) images of Fe-Ni5P4/NiFeOH-350. Reproduced with permission from Ref. [140]. Copyright 2021, Elsevier.

Fig. 15. (a) Schematic illustration of the fabrication process. SEM (b) and TEM (c) images of Cu@NiFe LDH. Reproduced with permission from Ref. [141]. Copyright 2017, Royal Society of Chemistry. (d) Schematic illustration for the synthetic process. SEM images of CoNi@CF (e) and CoNI@CF (f) with the molar ratio of Co2+ to Ni2+ at 3:7. Reproduced with permission from Ref. [142]. Copyright 2019, Elsevier.

Fig. 16. Schematic illustration of the synthesis (a) and SEM image (b) of p-CoSe2/CC. Reproduced with permission from Ref. [146]. Copyright 2018, American Chemical Society. SEM image (c) and schematic diagram (d) of CoFe-LDH with electrodeposition time of 200 s. Reproduced with permission from Ref. [147]. Copyright 2019, Elsevier. (e) SEM image of Co-Fe-P foam prepared by electrodeposition. Reproduced with permission from Ref. [149]. Copyright 2018, American Chemical Society.

Fig. 17. (a) Schematic illustration of the fabrication process for Co9S8/WS2 composites with different arrays. Reproduced with permission from Ref. [153]. Copyright 2021, Royal Society of Chemistry. (b) Schematic illustration of the preparation of the nanoframes composed of Co0.6Fe0.4P NPs coated with the carbon matrix. Reproduced with permission from Ref. [157]. Copyright 2019, Royal Society of Chemistry. (c) SEM image of NiCoP@Cu3P/CF. (d) TEM image of NiCoP@Cu3P. Reproduced with permission from Ref. [158]. Copyright 2018, Royal Society of Chemistry. (e) SEM top-view image of porous MoO2 nanosheets synthesized on nickel foam. (f) Synthesis steps of porous MoO2 nanosheets on nickel foam. Reproduced with permission from Ref. [44]. Copyright 2016, Wiley.

Fig. 18. (a) Schematic illustration of the fabrication process of NiFeOx/IF and NiFe-P/IF electrodes. (b) SEM image of NiFeOx/IF electrode. (c) TEM image of NiFeOx nanosheets scrapped from NiFeOx/IF electrode. Reproduced with permission from Ref. [160]. Copyright 2017, Wiley. (d) Illustration of the galvanic replacement reaction for Cu wire and AgNO3. Reproduced with permission Ref. [161]. Copyright 2013 Wiley.

Fig. 19. (a) TEM image of N-Mo2C NSs. Reproduced with permission from Ref. [164]. Copyright 2017, American Chemical Society. SEM (b) and TEM (c) image of CoPS samples. Reproduced with permission from Ref. [165]. Copyright 2021, American Chemical Society. (d) Schematic illustration for synthesis of porous g-C3N4, (e,f) SEM images of g-C3N4 with different melamine to NaCl ratio. Reproduced with permission from Ref. [162]. Copyright 2019, American Chemical Society. (g) Schematic illustration of the preparation of Co12@Ni3S2/NF. FE-SEM images of Co12@Ni3S2 nanocones (h) and Co12@Ni3S2/NF (i) after the long-time test. Reproduced with permission from Ref. [168]. Copyright 2021, Elsevier.

Fig. 20. (a) SEM image of 2D porous CoPo nanosheets. (b) Steady-state polarization curves in 1 mol L?1 KOH for HER and OER. HER (c), OER (d) Tafel plots and steady-state polarization curves (e) for overall water splitting of Ni foam. Reproduced with permission from Ref. [174]. Copyright 2018, Wiley. (f) TEM image of Ni@CoO@Co-MOFC. HER (g) and OER (h) LSV curves. Reproduced with permission from Ref. [175]. Copyright 2021, Royal Society of Chemistry.

Fig. 21. (a) Chronopotentiometry durability test at a constant current density of 100 mA cm?2. (b) Potential shift and corresponding potential loss and retention during 285 h durability test. Reproduced with permission from Ref. [76]. Copyright 2017, Elsevier. SEM (c) and TEM (d) images of NISe2/NF. (e) LSV plot for water splitting systems in 1.0 mol L?1 KOH at a scan rate of 5 mV s?1. (f) Long-term stability measurement of the NiSe2/Ni-based electrolyzer at 10 mA cm?2. Reproduced with permission from Ref. [177]. Copyright 2018, American Chemical Society.

Fig. 22. (a) CV curves of OER with iR-correction. (b) LSV curves of HER with iR correction. (c) Long-term chronopotetiometric measurement for 35 h of OER (black line) and HER (red line). Reproduced with permission from Ref. [181]. Copyright 2018, American Chemical Society. Polarization curves (d) and Tafel plots (e) of MoS2 before and after exfoliation in 2 mol L?1 H2SO4 at a scan rate of 5 mV. (f) EIS plots of 2H MoS2 and C-1T MoS2. Reproduced with permission from Ref. [36]. Copyright 2017, Royal Society of Chemistry.

Fig. 23. (a,b) SEM images of 3D printing graphene-CNT electrode. (c) SEM image of 3D printing GC/NiFeP electrode. HER (d) and OER (e) polarization curves. (f) Two electrode polarization curves for water splitting. Reproduced with permission from Ref. [189]. Copyright 2020, Wiley.

Fig. 24. OER (a) and HER (b) polarization curves with iR correction. (c) Tafel plots for electrodes in 1 mol L?1 KOH. (d) Polarization curve of water electrolysis. Chronoamperometric response curve (e) and HER polarization curves (f) of N-Ni3S2/NF after and before 5000 CV tests. Reproduced with permission from Ref. [197]. Copyright 2017, Wiley. Tafel slope for HER (g), LSV curves (h) and Tafel slope (i) for OER. Reproduced with permission from Ref. [199]. Copyright 2019, Elsevier.

Fig. 25. HER (a), OER (b) and overall water splitting polarization curves (c) for Co-doped NiO/NiFe2O4. Reproduced with permission from Ref. [208]. Copyright 2018, Royal Society of Chemistry. HER (d), OER (e) and overall water splitting LSV curves (f) for Co2P/CoNPC. Reproduced with permission from Ref. [211]. Copyright 2020, Wiley. (g) CV curves of NF/N-CoMoO4 catalyst. Reproduced with permission from Ref. [212]. Copyright 2020, Elsevier. HER (h) and OER (i) LSV curves of NF/T(Ni3S2/MnS-O). Reproduced with permission from Ref. [101]. Copyright 2019, Elsevier.

Fig. 26. (a) Polarization curve with iR correction. (b) Tafel slopes for HER. (c) Plots showing the extraction of Cdl. Reproduced with permission from Ref. [218]. Copyright 2016, American Chemical Society. (d) SEM image of Cu@MoS2. Polarization curve (e) and Tafel slope (f) of HER for Cu@MoS2. Reproduced with permission from Ref. [219]. Copyright 2019, Elsevier. (g) HRTEM image of Co3S4 PNSvac. Polarization curves with iR correction (h) and Tafel slope (i) of HER. Reproduced with permission from Ref. [220]. Copyright 2018, American Chemical Society.

Fig. 27. (a) Standard free energy diagram for HER and (b) OER process. Reproduced with permission from Ref. [224]. Copyright 2018, Wiley. (c) Schematic illustration of porous monolayer NIFe-LDH, (d) H2O adsorption energies and (e) OH* bonding energies on different active sites with various vacancies. Reproduced with permission from Ref. [225]. Copyright 2019, Wiley. (f) Polarization curve for overall water splitting. (g) Partial density of states (PDOS) for dual-vacancy MnO2. (h) Bandgap and possible band edge position for MnO2. Reproduced with permission from Ref. [226]. Copyright 2021, Wiley.

Fig. 28. (a) Nyquist plot under a fixed current density of 10 mA cm?2. (b) Polarization curves for overall water splitting. (c) Time-dependent current density curve for CoMoS4/Ni3S2 hybrid electrodes. Reproduced with permission from Ref. [232]. Copyright 2019, Elsevier. HER (d) and OER (e) polarization curves for different samples. (f) Polarization curves of IP/NP-NF as electrodes for OWS. Reproduced with permission from Ref. [233]. Copyright 2019, Elsevier.

Fig. 29. (a) EIS Nyquist plots of CoO/CoN4 and other samples. (b) Polarization curves of CoO/Co4N/NF as electrodes for OWS. Reproduced with permission from Ref. [234]. Copyright 2018, Royal of Society Chemistry. HER (c) and OER (d) polarization curves for NF/Co5.0Mo1P/NiFe-LDH and other samples. Polarization curves (e) of NF/Co5.0Mo1P/NiFe-LDH as electrodes for OWS and long-term stability test (f) at constant current densities of 100 mA cm?2. Reproduced with permission from Ref. [236]. Copyright 2020, American Chemical Society.

Fig. 30. (a) Merits of 3D MXene architecture. (b) EIS patterns of CoP@3D Ti3C2 MXene and other samples. Reproduced with permission from Ref. [242]. Copyright 2018, American Chemical Society. (c) Overpotentials for HER at different current densities. (d) Overpotentials for OER at different current densities. (e) Charge density difference isosurfaces for Co3Mo/CoMoO3 heterostructure from DFT calculations. Reproduced with permission from Ref. [245]. Copyright 2023, Elsevier.

Fig. 31. (a) Schematic illustration of HER reaction catalyzed by atomically strained MoS2 on curved NPG substrate. (b) Polarization curves of Pt, pure NPG, and MoS2@NPG for HER. Reproduced with permission from Ref. [250]. Copyright 2014, Wiley. HER (c) and OER (d) processes Gibbs free energy diagram for NiSxSe1?x. HER (e), OER (f) and overall water splitting polarization curves (g). Reproduced with permission from Ref. [251]. Copyright 2020, Wiley. (h) Overall water splitting polarization curves for Co2P/Ni2P-2%Mo electrodes. Reproduced with permission from Ref. [252]. Copyright 2020, Elsevier.

Table 1 Summary table for electrocatalytic overall water splitting system with modified porous electrocatalysts.

Catalyst	Fabrication method		Substrates			Electrolyte		HER				OER						Overall water splitting		Ref.
Catalyst	Fabrication method		Substrates			Electrolyte		η_{j = 10} (mV)		Tafel slope (mV dec^-1)		η_{j = 10} (mV)		Tafel slope (mV dec^-1)				E_{j = 10z} (V)		Ref.
Structure engineering (porous structure)
2D CoPo nanosheets	solvothermal and pyrolysis		NF			1 mol L^‒1 KOH		158		101		280				59		1.52		[174]
Ni@CoO@Co-MOFC	pyrolysis		NF			1 mol L^‒1 KOH		138		59		247				51		1.61		[175]
Structure engineering (self-supported)
Ni₃Se₂/NF	hydrothermal		NF			1 mol L^‒1 KOH		—		—		315 @100 mA cm^‒2				40.2		1.58		[76]
NiSe₂/Ni	immersion-selenization		NF			1 mol L^‒1 KOH		166		92.3		235				63.1		1.64		[177]
MoS₂/Ni₃S₂	electrodeposition + solvothermal		NF			1 mol L^‒1 KOH		99		71		185				46		1.50		[181]
MoS₂-CoS₂@PCMT	hydrothermal + thermal reduction + acid treatment		porous carbon microtube textile			1 mol L^‒1 KOH		200		95.2		215				93		1.59		[179]
Structure engineering (3D-printing)
3D P GC/NiFeP	3D printed graphene materials		—			1 mol L^‒1 KOH		133@30 mA cm^-2		97		214@30 mA cm^-2				162		1.58 @30 mA cm^‒2		[189]
Defect-engineering (doping)
N-Ni₃S₂/NF	annealing		NF			1 mol L^‒1 KOH		110		—		330 @100 mA cm^‒2				70		1.48		[197]
N-doped Ni/C	carbonization		—			1 mol L^‒1 KOH		142		52		350				56		1.63		[194]
CoP@NPCSs	coordination- polymerization-pyrolysis		carbon substrate			1 mol L^‒1 KOH		115		109		350				103		1.643		[198]
PrGO/Ni-CoP	hydrothermal + phosphorization		NF			3 mol L^‒1 KOH		106		58.3		281.3				60.1		1.56		[199]
Ni-Mo-P aerogel	induced gelation + in situ doping		carbon cloth			1 mol L^‒1 KOH		69		108.4		235				96.6		1.46		[201]
Fe-Ni₃S₂/AF	surface assisted chemical vapor transport		SCE			1 mol L^‒1 KOH		75		103		267				36		1.5		[204]
Fe-doped NiSe NSs/CNT	thermal treatment + CVD		carbon paper			1 mol L^‒1 KOH		242.3		130		282.7				55		—		[206]
Co-doped NiO/NiFe₂O₄	solvothermal		NF			1 mol L^‒1 KOH		84		53.6		183				38.5		1.583		[208]
Co₂P/CoNPC	phosphidation		SCE			1 mol L^‒1 KOH		130		63		328				78		1.64		[211]
PA-NiO	hydrothermal + phosphorization		NF			1 mol L^‒1 KOH		138		130		310@100 mA cm^‒2				53		1.56		[213]
CoMoP@N,P-C	pyrolysis		carbon cloth			1 mol L^‒1 KOH		152		76.8		296				97		1.62		[215]
N-doped carbon/Co/ CoP	carbonization + partial phosphating		carbon paper			1 mol L^‒1 KOH		208		126		350				94		1.72		[264]
Cu₈S₅/NSC-900	direct pyrolysis		NF			1 mol L^‒1 KOH		137		136.8		313				66.5		1.64		[265]
FeNi/NPC	pyrolysis		GCE			0.1 mol L^‒1 KOH		260		112		0.44 V				62		1.63		[266]
Defect-engineering (vacancy)
Ni₃AlP	solvothermal		NF			1 mol L^‒1 KOH		80		38		242				76		1.55		[223]
d-FeOOH NSs	wet-chemical route		NF			1 mol L^‒1 KOH		108		68		265				36		1.62		[224]
DV-MnO₂	wet-chemical route		—			1 mol L^‒1 KOH		59		63		260				40		1.55		[226]
Hybrid engineering
CoMoS₄/Ni₃S₂		hydrothermal+sulfuration		NF	1 mol L^‒1 KOH		76		169		200		63				1.568		[232]
IP/NP-NF		in situ synthesis + phosphorization		NF	1 mol L^‒1 KOH		63		59		185		47				1.567		[233]
CoO/Co₄N/NF		hydrothermal		NF	neutral electrolyte		145		80		398		83				1.79		[234]
NF/Co_5.0Mo₁P/NiFe-LDH		hydrothermal + electrodeposition		NF	1 mol L^‒1 KOH		98.9		93.3		225@50 mA cm^‒2		55				1.68		[236]
NiFeMoS/NF-P		electrodeposition + hydrothermal		NF	1 mol L^‒1 KOH		100		121		280@150 mA cm^‒2		69				1.52@100 mA cm^‒2		[237]
Ni₅P₄		contact conversion synthesis		NF	1 mol L^‒1 KOH		0.15 V		53		1.25 V		40				< 1.7		[238]
NiFeP_x@NiCo₂P_x		hydrothermal + annealing		NF	1 mol L^‒1 KOH		97		—		230		—				1.56		[240]
CoP@3D Ti₃C		annealing		RDE	1 mol L^‒1 KOH		168		58		298		51				1.565		[242]
CoNiO₂@rGO/NF		hydrothermal + annealing		—	1 mol L^‒1 KOH		126		72		272@100 mA cm^‒2		49				1.56		[244]
Co₃/Mo/CoMoO₃ NPSs		thermal treatment		NF	1 mol L^‒1 KOH		334@1000 mA cm^‒2		46.4		410@500 mA cm^‒2		52.7				1.59@100 mA cm^‒2		[245]
Co(OH)₂/La(OH)₃@ Cu NW		thermal annealing + electrodeposition		Cu nanowires	1 mol L^‒1 KOH		36		22.9		273@100 mA cm^‒2		89				1.56@20 mA cm^‒2		[50]
Strain engineering
NiS_0.5Se_0.5 NNH		solvothermal		NF	1 mol L^‒1 KOH		70		78		257				61		1.55		[251]
Ni₂P/Co₂P		hydrothermal		NF	1 mol L^‒1 KOH		164@100 mA cm^‒2		45.4		357@100 mA cm^‒2				46.1		1.57		[252]

Table 1 Summary table for electrocatalytic overall water splitting system with modified porous electrocatalysts.

Catalyst	Fabrication method		Substrates			Electrolyte		HER				OER						Overall water splitting		Ref.
Catalyst	Fabrication method		Substrates			Electrolyte		η_{j = 10} (mV)		Tafel slope (mV dec^-1)		η_{j = 10} (mV)		Tafel slope (mV dec^-1)				E_{j = 10z} (V)		Ref.
Structure engineering (porous structure)
2D CoPo nanosheets	solvothermal and pyrolysis		NF			1 mol L^‒1 KOH		158		101		280				59		1.52		[174]
Ni@CoO@Co-MOFC	pyrolysis		NF			1 mol L^‒1 KOH		138		59		247				51		1.61		[175]
Structure engineering (self-supported)
Ni₃Se₂/NF	hydrothermal		NF			1 mol L^‒1 KOH		—		—		315 @100 mA cm^‒2				40.2		1.58		[76]
NiSe₂/Ni	immersion-selenization		NF			1 mol L^‒1 KOH		166		92.3		235				63.1		1.64		[177]
MoS₂/Ni₃S₂	electrodeposition + solvothermal		NF			1 mol L^‒1 KOH		99		71		185				46		1.50		[181]
MoS₂-CoS₂@PCMT	hydrothermal + thermal reduction + acid treatment		porous carbon microtube textile			1 mol L^‒1 KOH		200		95.2		215				93		1.59		[179]
Structure engineering (3D-printing)
3D P GC/NiFeP	3D printed graphene materials		—			1 mol L^‒1 KOH		133@30 mA cm^-2		97		214@30 mA cm^-2				162		1.58 @30 mA cm^‒2		[189]
Defect-engineering (doping)
N-Ni₃S₂/NF	annealing		NF			1 mol L^‒1 KOH		110		—		330 @100 mA cm^‒2				70		1.48		[197]
N-doped Ni/C	carbonization		—			1 mol L^‒1 KOH		142		52		350				56		1.63		[194]
CoP@NPCSs	coordination- polymerization-pyrolysis		carbon substrate			1 mol L^‒1 KOH		115		109		350				103		1.643		[198]
PrGO/Ni-CoP	hydrothermal + phosphorization		NF			3 mol L^‒1 KOH		106		58.3		281.3				60.1		1.56		[199]
Ni-Mo-P aerogel	induced gelation + in situ doping		carbon cloth			1 mol L^‒1 KOH		69		108.4		235				96.6		1.46		[201]
Fe-Ni₃S₂/AF	surface assisted chemical vapor transport		SCE			1 mol L^‒1 KOH		75		103		267				36		1.5		[204]
Fe-doped NiSe NSs/CNT	thermal treatment + CVD		carbon paper			1 mol L^‒1 KOH		242.3		130		282.7				55		—		[206]
Co-doped NiO/NiFe₂O₄	solvothermal		NF			1 mol L^‒1 KOH		84		53.6		183				38.5		1.583		[208]
Co₂P/CoNPC	phosphidation		SCE			1 mol L^‒1 KOH		130		63		328				78		1.64		[211]
PA-NiO	hydrothermal + phosphorization		NF			1 mol L^‒1 KOH		138		130		310@100 mA cm^‒2				53		1.56		[213]
CoMoP@N,P-C	pyrolysis		carbon cloth			1 mol L^‒1 KOH		152		76.8		296				97		1.62		[215]
N-doped carbon/Co/ CoP	carbonization + partial phosphating		carbon paper			1 mol L^‒1 KOH		208		126		350				94		1.72		[264]
Cu₈S₅/NSC-900	direct pyrolysis		NF			1 mol L^‒1 KOH		137		136.8		313				66.5		1.64		[265]
FeNi/NPC	pyrolysis		GCE			0.1 mol L^‒1 KOH		260		112		0.44 V				62		1.63		[266]
Defect-engineering (vacancy)
Ni₃AlP	solvothermal		NF			1 mol L^‒1 KOH		80		38		242				76		1.55		[223]
d-FeOOH NSs	wet-chemical route		NF			1 mol L^‒1 KOH		108		68		265				36		1.62		[224]
DV-MnO₂	wet-chemical route		—			1 mol L^‒1 KOH		59		63		260				40		1.55		[226]
Hybrid engineering
CoMoS₄/Ni₃S₂		hydrothermal+sulfuration		NF	1 mol L^‒1 KOH		76		169		200		63				1.568		[232]
IP/NP-NF		in situ synthesis + phosphorization		NF	1 mol L^‒1 KOH		63		59		185		47				1.567		[233]
CoO/Co₄N/NF		hydrothermal		NF	neutral electrolyte		145		80		398		83				1.79		[234]
NF/Co_5.0Mo₁P/NiFe-LDH		hydrothermal + electrodeposition		NF	1 mol L^‒1 KOH		98.9		93.3		225@50 mA cm^‒2		55				1.68		[236]
NiFeMoS/NF-P		electrodeposition + hydrothermal		NF	1 mol L^‒1 KOH		100		121		280@150 mA cm^‒2		69				1.52@100 mA cm^‒2		[237]
Ni₅P₄		contact conversion synthesis		NF	1 mol L^‒1 KOH		0.15 V		53		1.25 V		40				< 1.7		[238]
NiFeP_x@NiCo₂P_x		hydrothermal + annealing		NF	1 mol L^‒1 KOH		97		—		230		—				1.56		[240]
CoP@3D Ti₃C		annealing		RDE	1 mol L^‒1 KOH		168		58		298		51				1.565		[242]
CoNiO₂@rGO/NF		hydrothermal + annealing		—	1 mol L^‒1 KOH		126		72		272@100 mA cm^‒2		49				1.56		[244]
Co₃/Mo/CoMoO₃ NPSs		thermal treatment		NF	1 mol L^‒1 KOH		334@1000 mA cm^‒2		46.4		410@500 mA cm^‒2		52.7				1.59@100 mA cm^‒2		[245]
Co(OH)₂/La(OH)₃@ Cu NW		thermal annealing + electrodeposition		Cu nanowires	1 mol L^‒1 KOH		36		22.9		273@100 mA cm^‒2		89				1.56@20 mA cm^‒2		[50]
Strain engineering
NiS_0.5Se_0.5 NNH		solvothermal		NF	1 mol L^‒1 KOH		70		78		257				61		1.55		[251]
Ni₂P/Co₂P		hydrothermal		NF	1 mol L^‒1 KOH		164@100 mA cm^‒2		45.4		357@100 mA cm^‒2				46.1		1.57		[252]

Table 2 Summary table for electrocatalytic hydrogen evolution system with modified porous electrocatalysts.

Catalyst	Fabrication method	Substrate	Electrolyte	η_{j = 10}(mV)	Tafel slope (mV dec^‒1)	Ref.
Structure engineering (porous structure)
MoO_3‒_x	calcination	CC	0.5 mol L^‒1 H₂SO₄	179	72	[186]
Structure engineering (self-supported)
MoS_x/V₂O₃	annealing	CC	0.5 mol L^‒1 H₂SO₄	146	45	[180]
WC-N/W-1200	phase-inversion tape-casting and pressureless sintering method	ceramic membrane	0.5 mol L^‒1 H₂SO₄	87	44.9	[49]
Structure engineering (phase engineering)
1T/2H MoS₂	hydrothermal	—	0.5 mol L^‒1 H₂SO₄	‒309	89	[267]
1T’ MoS₂-Ti₃C₂	solvothermal	Ti₃C₂	0.5 mol L^‒1 H₂SO₄	98	45	[184]
C-1T MoS₂	hydrothermal + lithium intercalation	—	0.5 mol L^‒1 H₂SO₄	‒156	42.7	[36]
Vertically aligned 2H-1T MoS₂	solvothermal	—	0.5 mol L^‒1 H₂SO₄	116	60	[187]
1T/2H-WS₂/N-rGO/CC	hydrothermal	CC	0.5 mol L^‒1 H₂SO₄	21.13	29.55	[188]
1T/2H-WS₂/N-rGO/CC	hydrothermal	CC	1 mol L^‒1 KOH	80.35	137.02	[188]
1T/2H MoS₂ (25D)/Ti₃C₂T_x-1 (MTC-1)	ultrasonication + mechanical stirring	GCE	0.5 mol L^‒1 H₂SO₄	280	83.8	[183]
1T/2H MoS₂ (25D)/Ti₃C₂T_x-1 (MTC-1)	ultrasonication + mechanical stirring	GCE	1 mol L^‒1 KOH	300	117.2	[183]
Defect engineering (doping)
P-doped MoS₂	hydrothermal	GCE	0.5 mol L^‒1 H₂SO₄	43	34	[200]
Mn-doped CoSe₂	solvothermal	GCE	0.5 mol L^‒1 H₂SO₄	174	36	[202]
Fe-NiS₂	sulfurization	GCE	0.5 mol L^‒1 H₂SO₄	121	37	[205]
Co/β-Mo2C Nps incorporated (N-C/Co/Mo2C) holey nanorods	pyrolysis	GCE	1 mol L^‒1 KOH	142	98.5	[268]
Defect engineering (vacancy)
P-1T-MoS₂	liquid-ammonia-assisted-lithiation	GCE	0.5 mol L^‒1 H₂SO₄	153	43	[218]
Cu@MoS	solvothermal	GCE	0.5 mol L^‒1 H₂SO₄	131	51	[219]
Co₃S₄ PNS_vac	plasma induced dry exfoliation	—	1 mol L^‒1 KOH	63	58	[220]
b-Mo₂C spheres	hydrothermal	—	1 mol L^‒1 KOH	125	70.95	[222]
Strain engineering
3D-MoS₂@NPG	CVD	chemical dealloyed nanoporous gold	0.5 mol L^‒1 H₂SO₄	123	46	[250]
W(Se_xS_1‒_x)₂ NPA	electrochemical anodization + CVD	tungsten substrate	0.5 mol L^‒1 H₂SO₄ bubbled with H₂	45	59	[257]

Table 2 Summary table for electrocatalytic hydrogen evolution system with modified porous electrocatalysts.

Catalyst	Fabrication method	Substrate	Electrolyte	η_{j = 10}(mV)	Tafel slope (mV dec^‒1)	Ref.
Structure engineering (porous structure)
MoO_3‒_x	calcination	CC	0.5 mol L^‒1 H₂SO₄	179	72	[186]
Structure engineering (self-supported)
MoS_x/V₂O₃	annealing	CC	0.5 mol L^‒1 H₂SO₄	146	45	[180]
WC-N/W-1200	phase-inversion tape-casting and pressureless sintering method	ceramic membrane	0.5 mol L^‒1 H₂SO₄	87	44.9	[49]
Structure engineering (phase engineering)
1T/2H MoS₂	hydrothermal	—	0.5 mol L^‒1 H₂SO₄	‒309	89	[267]
1T’ MoS₂-Ti₃C₂	solvothermal	Ti₃C₂	0.5 mol L^‒1 H₂SO₄	98	45	[184]
C-1T MoS₂	hydrothermal + lithium intercalation	—	0.5 mol L^‒1 H₂SO₄	‒156	42.7	[36]
Vertically aligned 2H-1T MoS₂	solvothermal	—	0.5 mol L^‒1 H₂SO₄	116	60	[187]
1T/2H-WS₂/N-rGO/CC	hydrothermal	CC	0.5 mol L^‒1 H₂SO₄	21.13	29.55	[188]
1T/2H-WS₂/N-rGO/CC	hydrothermal	CC	1 mol L^‒1 KOH	80.35	137.02	[188]
1T/2H MoS₂ (25D)/Ti₃C₂T_x-1 (MTC-1)	ultrasonication + mechanical stirring	GCE	0.5 mol L^‒1 H₂SO₄	280	83.8	[183]
1T/2H MoS₂ (25D)/Ti₃C₂T_x-1 (MTC-1)	ultrasonication + mechanical stirring	GCE	1 mol L^‒1 KOH	300	117.2	[183]
Defect engineering (doping)
P-doped MoS₂	hydrothermal	GCE	0.5 mol L^‒1 H₂SO₄	43	34	[200]
Mn-doped CoSe₂	solvothermal	GCE	0.5 mol L^‒1 H₂SO₄	174	36	[202]
Fe-NiS₂	sulfurization	GCE	0.5 mol L^‒1 H₂SO₄	121	37	[205]
Co/β-Mo2C Nps incorporated (N-C/Co/Mo2C) holey nanorods	pyrolysis	GCE	1 mol L^‒1 KOH	142	98.5	[268]
Defect engineering (vacancy)
P-1T-MoS₂	liquid-ammonia-assisted-lithiation	GCE	0.5 mol L^‒1 H₂SO₄	153	43	[218]
Cu@MoS	solvothermal	GCE	0.5 mol L^‒1 H₂SO₄	131	51	[219]
Co₃S₄ PNS_vac	plasma induced dry exfoliation	—	1 mol L^‒1 KOH	63	58	[220]
b-Mo₂C spheres	hydrothermal	—	1 mol L^‒1 KOH	125	70.95	[222]
Strain engineering
3D-MoS₂@NPG	CVD	chemical dealloyed nanoporous gold	0.5 mol L^‒1 H₂SO₄	123	46	[250]
W(Se_xS_1‒_x)₂ NPA	electrochemical anodization + CVD	tungsten substrate	0.5 mol L^‒1 H₂SO₄ bubbled with H₂	45	59	[257]

Table 3 Summary table for electrocatalytic oxygen evolution system with modified porous electrocatalysts.

Catalyst	Fabrication method	Substrate	Electrolyte	η_{j = 10} (mV)	Tafel slope (mV dec^-1)	Ref.
Structure engineering (self-supported)
Ni₃Se₂/NF	hydrothermal	NF	1 mol L^‒1 KOH	315	40.2	[76]
NiCo₂S₄/FeOOH nanowires	hydrothermal + anion exchange	carbon cloth	1 mol L^‒1 KOH	200	71	[269]
Defect engineering (vacancy)
H-Vs-Co₃-S₄	calcination + sulfidation + reduction	—	1 mol L^‒1 KOH	270	59	[221]
PM-LDH	coprecipitation	—	1 mol L^‒1 KOH	230	47	[225]
Hybrid engineering
Fe_2‒_xMn_xP	single-pot solution-phase synthesis	GCE	1 mol L^‒1 KOH	480	39	[239]
NiFeP/MXene	hydrothermal + phosphorization	GCE	1 mol L^‒1 KOH	312	68	[270]
NiCo₂S₄/Co₉S₈	hydrothermal	GCE	0.1 mol L^‒1 KOH	0.32 V	72.16	[271]
Strain engineering
NiFe MOF	hydrothermal	RDE	N₂-saturated 0.1 mol L^‒1 KOH	210@200 mA cm^‒2	68	[256]
CoO₃ NWs (PNWs)	thermal oxidation	GCE	1 mol L^‒1 KOH	319	51	[272]

Fig. 32. (a) Schematic illustration of the amorphous SACs. Reproduced with permission from Ref. [258]. Copyright 2021, Wiley. (b) Polarization curves of modified MoS2. Reproduced with permission from Ref. [260]. Copyright 2018, Wiley. (c) OER polarization curves if 2D COFs with carbon nanotube. Reproduced with permission from Ref. [261]. Copyright 2021, American Chemical Society.

Fig. 33. Key points to design porous electrocatalyst.

Fig. 34. Future outlook for porous electrocatalysts for HER, OER and OWS.

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Unleashing the versatility of porous nanoarchitectures: A voyage for sustainable electrocatalytic water splitting

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