Basics of Research Progress for Urea Electrolysis for Hydrogen Generation and Urea Fuel Cells

doi:10.19894/j.issn.1000-0518.230131

Chinese Journal of Applied Chemistry ›› 2023, Vol. 40 ›› Issue (8): 1158-1174.DOI: 10.19894/j.issn.1000-0518.230131

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Basics of Research Progress for Urea Electrolysis for Hydrogen Generation and Urea Fuel Cells

Chun YIN, Jia-Xin LI, Li-Gang FENG()

School of Chemistry and Chemical Engineering，Yangzhou University，Yangzhou 225002，China

Received:2023-05-04 Accepted:2023-07-06 Published:2023-08-01 Online:2023-08-24
Contact: Li-Gang FENG
About author:ligang.feng@yzu.edu.cn
Supported by:
the National Natural Science Foundation of China(22272148)

Abstract

Abstract:

Urea as an effective hydrogen carrier can be used in urea electrolysis （UE） for hydrogen production and direct urea fuel cells （DUFC）. In urea electrolysis， the coupling of urea oxidation reaction （UOR） at the anode and hydrogen evolution reaction （HER） at the cathode to produce hydrogen is more cost-effective than water electrolysis， with energy consumption reduced by about 30% and economic cost reduced by about 36%. In the direct urea fuel cells， urea as fuel at the anode and coupled with oxygen reduction at the cathode can convert chemical energy directly into electrical energy. As the basis of these two energy conversion technologies， UOR has received more and more attention. This review discusses the reaction principle and performance description parameters of UOR in alkaline electrolytes and introduces the application of UOR in UE and DUFC. Attention is also given to the principles of UE and DUFC and the development status of some catalysts， and finally， the challenges faced in the development of UE and DUFC are also commented. Hopefully， this review will be helpful for understanding the basics of UE and DUFC.

Key words: Urea, Electrolysis, Fuel cell, Hydrogen, Electrochemistry

CLC Number:

O646

Chun YIN, Jia-Xin LI, Li-Gang FENG. Basics of Research Progress for Urea Electrolysis for Hydrogen Generation and Urea Fuel Cells[J]. Chinese Journal of Applied Chemistry, 2023, 40(8): 1158-1174.

Figures/Tables 11

References 122

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118	YOON J， LEE D， LEE Y N， et al. Solid solution palladium-nickel bimetallic anode catalysts by co-sputtering for direct urea fuel cells （DUFC）［J］. J Power Sources， 2019， 431： 259-264.
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122	PEI C， CHEN S， ZHOU M， et al. Direct urea/H₂O₂ fuel cell with a hierarchical porous nanoglass anode for high-efficiency energy conversion［J］. ACS Appl Mater Interfaces， 2023， 15（20）： 24319-24328.

Hydrogen carrier	w（H element）/%	Melting point/℃， boiling point/℃	Lower/upper explosive limit	Toxicity threshold limit value/（mg·L^-1）	Energy density/（MJ·kg^-1）	Cost/（＄·kg^-1）
Hydrogen	100	-259， -253	4%/75%	Nontoxic	142.0	0.79
Ammonia	17.6	-78， -33	15%/28%	25/35	22.5	0.39
Ethanol	13.1	-117， 79	3.3%/19%	1 000	26.8	0.64
Methanol	12.6	-98， 65	6.7%/36%	200/250	15.2	0.49
Urea	6.7	132.7， 196.6	Low-vapor-pressure solid	Nontoxic	15.66	0.24

Hydrogen carrier	w（H element）/%	Melting point/℃， boiling point/℃	Lower/upper explosive limit	Toxicity threshold limit value/（mg·L^-1）	Energy density/（MJ·kg^-1）	Cost/（＄·kg^-1）
Hydrogen	100	-259， -253	4%/75%	Nontoxic	142.0	0.79
Ammonia	17.6	-78， -33	15%/28%	25/35	22.5	0.39
Ethanol	13.1	-117， 79	3.3%/19%	1 000	26.8	0.64
Methanol	12.6	-98， 65	6.7%/36%	200/250	15.2	0.49
Urea	6.7	132.7， 196.6	Low-vapor-pressure solid	Nontoxic	15.66	0.24

Catalyst	Electrolyte	Scan rate/（mV·s^-1）	Peak current density （mA·cm^-2） at （@） specific potential	Potential/V （i=10 mA/cm²）	Ref.
Ni-MOF-0.5	1 mol/L KOH+0.5 mol/L urea	5	—	1.38 V（vs.RHE）	［6］
C@NiO	1 mol/L KOH+0.33 mol/L urea	10	25@1.46 V（vs.RHE）	1.36 V（vs.RHE）	［14］
Ni（OH）₂@NF	1 mol/L KOH+0.33 mol/L urea	5	—	1.35 V（vs.RHE）	［60］
V-Ni₃N/NF	1 mol/L KOH+0.5 mol/L urea	2	—	1.361 V（vs.RHE）	［61］
Ni@NCNT-3	1 mol/L KOH+0.5 mol/L urea	10	45.8@1.5 V（vs.RHE）	1.38 V（vs.RHE）	［62］
Ni/SiO _x /N-C	1 mol/L KOH+0.33 mol/L urea	5	—	1.384 V（vs.RHE）	［63］
NiFe/N-C	1 mol/L KOH+1 mol/L urea	5	100@1.37 V（vs.RHE）	1.37 V（vs.RHE）（at 100 mA/cm²）	［64］
NP-Ni_0.7Fe_0.3NF	1 mol/L KOH+0.33 mol/L urea	5	—	1.33 V（vs.RHE）	［65］
NiFeMo	1 mol/L KOH+0.33 mol/L urea	5	152@1.5 V（vs.RHE）	1.38 V（vs.RHE）	［66］
Ni₃N-350/NF	1 mol/L KOH+0.5 mol/L urea	5	—	1.34 V（vs.RHE）	［67］
a-Ni₂P/G	1 mol/L KOH+0.5 mol/L urea	5	209.1@1.7 V（vs.RHE）	1.28 V（vs.RHE）	［68］
Ni₃S₂/MWCNTs/NF	1 mol/L KOH+0.5 mol/L urea	5	—	1.338 V（vs.RHE）	［69］
β-NiS	1 mol/L KOH+0.33 mol/L urea	5	—	1.4 V（vs.RHE）	［70］
Ni_0.85Se/rGO	1 mol/L KOH+0.5 mol/L urea	5	—	1.36 V（vs.RHE）	［71］
Ni/NiO@NC	1 mol/L KOH+0.33 mol/L urea	5	—	1.35 V（vs.RHE）	［72］
Ni@C-V₂O₃/NF	1 mol/L KOH+0.5 mol/L urea	5	—	1.32 V（vs.RHE）	［73］
NiSe₂-NiO 350	1 mol/L KOH+0.33 mol/L urea	10		1.33 V（vs.RHE）	［74］
NiF₃/Ni₂P@CC-2	1 mol/L KOH+0.33 mol/L urea	10	122@1.6 V（vs.RHE）	1.36 V（vs.RHE）	［37］
MNPBA-P	1 mol/L KOH+0.5 mol/L urea	20	—	1.344 V（vs.RHE）	［75］
Rh-Ni	1 mol/L KOH+0.33 mol/L urea	10	82@0.7 V（vs.Hg/HgO）	1.4 V（vs.RHE）（at 50 mA/cm²）	［76］
Ni/Rh	5 mol/L KOH+0.33 mol/L urea	5	45@0.65 V（vs. Ag/AgCl）	—	［77］
PtIr	5 mol/L KOH+0.33 mol/L urea	10	125@0.8 V（vs.Hg/HgO）	—	［8］
Rh-NCs/NiO-NSs	1 mol/L KOH+0.33 mol/L urea	50	616@1.55V（vs.RHE）	—	［53］

Catalyst	Electrolyte	Scan rate/（mV·s^-1）	Peak current density （mA·cm^-2） at （@） specific potential	Potential/V （i=10 mA/cm²）	Ref.
Ni-MOF-0.5	1 mol/L KOH+0.5 mol/L urea	5	—	1.38 V（vs.RHE）	［6］
C@NiO	1 mol/L KOH+0.33 mol/L urea	10	25@1.46 V（vs.RHE）	1.36 V（vs.RHE）	［14］
Ni（OH）₂@NF	1 mol/L KOH+0.33 mol/L urea	5	—	1.35 V（vs.RHE）	［60］
V-Ni₃N/NF	1 mol/L KOH+0.5 mol/L urea	2	—	1.361 V（vs.RHE）	［61］
Ni@NCNT-3	1 mol/L KOH+0.5 mol/L urea	10	45.8@1.5 V（vs.RHE）	1.38 V（vs.RHE）	［62］
Ni/SiO _x /N-C	1 mol/L KOH+0.33 mol/L urea	5	—	1.384 V（vs.RHE）	［63］
NiFe/N-C	1 mol/L KOH+1 mol/L urea	5	100@1.37 V（vs.RHE）	1.37 V（vs.RHE）（at 100 mA/cm²）	［64］
NP-Ni_0.7Fe_0.3NF	1 mol/L KOH+0.33 mol/L urea	5	—	1.33 V（vs.RHE）	［65］
NiFeMo	1 mol/L KOH+0.33 mol/L urea	5	152@1.5 V（vs.RHE）	1.38 V（vs.RHE）	［66］
Ni₃N-350/NF	1 mol/L KOH+0.5 mol/L urea	5	—	1.34 V（vs.RHE）	［67］
a-Ni₂P/G	1 mol/L KOH+0.5 mol/L urea	5	209.1@1.7 V（vs.RHE）	1.28 V（vs.RHE）	［68］
Ni₃S₂/MWCNTs/NF	1 mol/L KOH+0.5 mol/L urea	5	—	1.338 V（vs.RHE）	［69］
β-NiS	1 mol/L KOH+0.33 mol/L urea	5	—	1.4 V（vs.RHE）	［70］
Ni_0.85Se/rGO	1 mol/L KOH+0.5 mol/L urea	5	—	1.36 V（vs.RHE）	［71］
Ni/NiO@NC	1 mol/L KOH+0.33 mol/L urea	5	—	1.35 V（vs.RHE）	［72］
Ni@C-V₂O₃/NF	1 mol/L KOH+0.5 mol/L urea	5	—	1.32 V（vs.RHE）	［73］
NiSe₂-NiO 350	1 mol/L KOH+0.33 mol/L urea	10		1.33 V（vs.RHE）	［74］
NiF₃/Ni₂P@CC-2	1 mol/L KOH+0.33 mol/L urea	10	122@1.6 V（vs.RHE）	1.36 V（vs.RHE）	［37］
MNPBA-P	1 mol/L KOH+0.5 mol/L urea	20	—	1.344 V（vs.RHE）	［75］
Rh-Ni	1 mol/L KOH+0.33 mol/L urea	10	82@0.7 V（vs.Hg/HgO）	1.4 V（vs.RHE）（at 50 mA/cm²）	［76］
Ni/Rh	5 mol/L KOH+0.33 mol/L urea	5	45@0.65 V（vs. Ag/AgCl）	—	［77］
PtIr	5 mol/L KOH+0.33 mol/L urea	10	125@0.8 V（vs.Hg/HgO）	—	［8］
Rh-NCs/NiO-NSs	1 mol/L KOH+0.33 mol/L urea	50	616@1.55V（vs.RHE）	—	［53］

Anode catalyst	Cathode catalyst	Electrolyte	Cell voltage （V） at （@）specific current density （mA/cm²） for UE	Cell voltage （V） at （@） specific current density （mA/cm²） for WS/V	Ref.
P-CoNi₂S₄	P-CoNi₂S₄	1 mol/L KOH+0.33 mol/L urea	1.402@10	1.544@10	［15］
NiFeRh-LDH	NiFeRh-LDH	1 mol/L KOH+0.33 mol/L urea	1.346@10	1.455@10	［78］
Ni-S-Se/NF	Ni-S-Se/NF	1 mol/L KOH+0.5 mol/L urea	1.47@10	1.57@10	［47］
Ni-NiO-Mo_0.84Ni_0.16/NF	Ni-NiO-Mo_0.84Ni_0.16/NF	1 mol/L KOH+0.5 mol/L urea	1.37@10	1.52@10	［79］
MoP@NiCo-LDH/NF-20	MoP@NiCo-LDH/NF-20	1 mol/L KOH+0.5 mol/L urea	1.405@100	1.697@100	［80］
Fe₂P@Ni _x P/NF	Fe₂P@Ni _x P/NF	1 mol/L KOH+0.5 mol/L urea	1.538@100	1.705@100	［81］
Ni₃N/Ni_0.2Mo_0.8N/NF	Ni₃N/Ni_0.2Mo_0.8N/NF	1 mol/L KOH+0.5 mol/L urea	1.348@10	1.487@10	［82］
NiFeMo	NiFeMo	1 mol/L KOH+0.33 mol/L urea	1.46@10	1.60@10	［66］
NiCoFe-LTH	NiCoFe-LTH	1 mol/L KOH+0.33 mol/L urea	1.49@10	1.65@10	［83］
NC-FNCP	NC-FNCP	1 mol/L KOH+0.5 mol/L urea	1.52@10	1.63@10	［84］
Ni-CoP/HPFs	Ni-CoP/HPFs	1 mol/L KOH+0.5 mol/L urea	1.43@10	1.68@10	［85］
Ni-Mo	Ni-Mo	1 mol/L KOH+0.1 mol/L urea	1.43@10	1.59@10	［86］
Co-Z/Se-2	Co-Z/Se-2	1 mol/L KOH+0.5 mol/L urea	1.49@10	1.678@10	［87］
NF/CoMoS/NiFeOOH	NF/CoMoS/NiFeOOH	1 mol/L KOH+0.5 mol/L urea	1.66@100	1.732@100	［16］
V-FeNi₃N/Ni₃N	V-FeNi₃N/Ni₃N	1 mol/L KOH+0.33 mol/L urea	1.46@10	1.54@10	［88］
Ru-NiFe-③/NF	Ru-NiFe-③/NF	1 mol/L KOH+0.33 mol/L urea	1.47@100	1.63@100	［89］
Co（OH）F/NF	Co–P/NF	1 mol/L KOH+0.7 mol/L urea	1.42@10	1.65@10	［90］
NiO-NiPi	NiP/NiO-NiPi	1 mol/L KOH+0.5 mol/L urea	1.585@100	1.876@100	［91］
Ni/Ni₂P/CNF	Pt/C	1 mol/L KOH+0.33 mol/L urea	1.40@10	1.58@10	［92］

Basics of Research Progress for Urea Electrolysis for Hydrogen Generation and Urea Fuel Cells

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Anode	Cathode	Anolyte	Oxidant	Peak power density/ （mW·cm^-2）	Temperature/℃	Ref.
Pt/C	Pt/C	1 mol/L urea	Air	0.55	Room temperature	［10］
Ni/C	Ag/C	1 mol/L urea	Air	0.14	Room temperature
Ni/C	MnO₂/C	1 mol/L urea	Air	1.7	50
Ni@C	Pt/C	1 mol/L KOH+0.33 mol/L urea	Air	13.8	50	［104］
Ni-Cu/ZnO@MWCNT	Pt/C	3 mol/L KOH+0.7 mol/L urea	Air	44.36	50	［94］
h-NiWO₄NPs/rGO	Pt/C	1 mol/L KOH+0.33 mol/L urea	Air	5	Room temperature	［105］
NiCo₂O₄/CC-12	Pt/C	1 mol/L KOH+0.05 mol/L urea	Air	38	80	［106］
Co₃O₄/NiO	Co₃O₄@MnO₂	0.1 mol/L KOH+0.05 mol/L urea	Air	33.8	60	［107］
Ni-Co/MWCNT	Pt/C	3 mol/L KOH+1 mol/L urea	O₂	17.5	60	［108］
Ni/rGO-300	Graphite/Filter paper	6 mol/L KOH+0.33 mol/L urea	30% H₂O₂	0.18	19	［109］
CoNi/rGO@NF	Pd/CFC	5 mol/L KOH+0.33 mol/L urea	0.9 mol/L H₂O₂+2 mol/L H₂SO₄	12.58	60	［110］
NiCo₂S₄@CS	Pd/Ti	5 mol/L KOH+0.2 mol/L urea	1 mol/L H₂O₂+2 mol/L H₂SO₄	10.36	60	［111］
Ni（OH）₂/NF	Pd/C@TiC	5 mol/L KOH+0.6 mol/L urea	2 mol/L H₂O₂+2 mol/L H₂SO₄	19.7	20	［112］
NiCo/NF	Pd/CFC	7 mol/L KOH+0.5 mol/L urea	2 mol/L H₂O₂+2 mol/L H₂SO₄	17.4	20	［113］
Ni-Se/NF	Prussian blue	1 mol/L KOH+0.5 mol/L urea	2 mol/L H₂O₂+2 mol/L H₂SO₄	33	20	［100］
Ni-120/VC	Pt/C	7 mol/L KOH+0.33 mol/L urea	2 mol/L H₂O₂+2 mol/L H₂SO₄	36.4	70	［114］
Ni_0.8Co_0.2（OH）₂	Pt/C	5 mol/L KOH+0.5 mol/L urea	2 mol/L H₂O₂+2 mol/L H₂SO₄	11.2	20	［97］
Ni₆Cr₄-CNT@C	Pt/C	5 mol/L KOH+1 mol/L urea	2 mol/L H₂O₂+2 mol/L H₂SO₄	48.1	80	［115］
Pt	Graphite	1 mol/L KOH+0.3 mol/L urea	0.65 mol/L AgNO₃	0.91	Room temperature	［116］
Ni/CC	CC	Fresh urine	50 mg/L Cr（Ⅵ）+0.25 mol/L H₂SO₄	0.34	20	［117］
Pd-Ni/C	Pd/C	1 mol/L KOH+0.33 mol/L urea	O₂	1.12	Room temperature	［118］
Ni/CNT@sponge	Pt/C	3 mol/L KOH+3 mol/L urea	1.5 mol/L H₂SO₄	6.6	45	［119］
Ni nanorods/NF	Prussian blue	1 mol/L NaOH+0.33 mol/L urea	2 mol/L H₂O₂+2 mol/L KCl+ 2 mol/L H₂SO₄	10.6	20	［120］
Ni-Co NWAs	Pd/CFC	5 mol/L KOH+0.33 mol/L urea	2 mol/L H₂O₂+2 mol/L H₂SO₄	5.03	25	［121］
Ni-P HPNG-40	Pt net	9 mol/L KOH+0.5 mol/L urea	2 mol/L H₂O₂+2 mol/L H₂SO₄	38.15	60	［122］

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