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Catalyst Design and Progresses for Urea Oxidation Electrolysis in Alkaline Media

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Abstract

Urea, as a significant molecule in biology, chemistry and agriculture, is extensively present both in industrial production and daily life. However, its excessively releasing into water and soil could bring about a serious threat to the environment and ecology due to the potential eutrophication. Considering the potential hydrogen content in urea, urea-rich wastewater is also regarded as a strategic energy storage resource. Among all technologies, the electrochemical treatment of urea wastewater behaves superior advantages both on environment protection and energy recovery, causing tremendous attention in recent years. Herein, this review summarized electrochemical methods for urea conversions for pollutant control and energy harvesting. As the kernel role in the electrochemical systems, the latest development of advanced electrodes is presented with the basic design principles described. The relationships between the electrocatalysts and their urea oxidation performance have been discussed thoroughly. Additionally, recent advances about novel applications for energy production and resource recovery are also displayed. Finally, the prospects and challenges are still to be addressed, orienting a clear direction for the electrochemical hydrogen harvesting from urea-containing wastewater in the future.

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Fig. 1

Reproduced with permission from Ref. [26]. b Comparison of urea electrolysis and water splitting from electrochemical reaction and standard potentials required

Fig. 2

Reproduced with permission from Ref. [34]. c Optimized structure for bridge-coordinated urea on nickel oxyhydroxide. (Reproduced with permission from Ref. [35]). d LSV of NiClO-D and NiOH-D catalysts on GCEs in 1 m KOH aqueous electrolyte with 0.33 m urea, and illustration of lattice-oxygen involved mechanism and calculated Gibbs free energy profiles. (Reproduced with permission from Ref. [36])

Fig. 3

Reproduced with permission from Ref. [47]) c Schematic illustration of the metallic sulfur incorporation Ni(OH)2 nanosheets. d Urea oxidation LSV plots of M-Ni(OH)2 electrode (the inset shows the onset potential) and e comparison between M-Ni(OH)2 electrode and the P-Ni(OH)2 electrode. (Reproduced with permission from Ref. [48]). f Open-ended Ni(OH)2 nanotubes grown on 3D nickel foam for enhanced urea electrocatalytic oxidation. (Reproduced with permission from Ref. [49]). g The formation energy calculated from Ni(OH)2 and NiClOH to NiOO models (Reproduced with permission from Ref. [36]). h Schematic illustration of deep reconstruction of Ni-based electrodes by a lithiation-induced strategy. (Reproduced with permission from Ref. [54])

Fig. 4

Reproduced with permission from Ref. [58. c LSV curves of several electrodes in a two-electrode systems in 1 M KOH with and without 0.33 M urea. (Reproduced with permission from Ref. [68]). d The synthesis process for Ni-MOF nanosheets, and e their corresponding SEM (i) and TEM (ii) images. f LSV curves of Ni-MOF, Ni(OH)2 and 20% Pt/C in 1 M KOH electrolyte with and without 0.33 M urea, and g the corresponding Nyquist plots of Ni-MOF and Ni(OH)2. (Reproduced with permission from Ref. [70])

Fig. 5

Reproduced with permission from Ref. [84]) c Illustration of an oxygen vacancy in NiMoO4 structure. d CV curves comparison of several electrodes in 1 M KOH and 0.5 M urea electrolyte and long-time operation of r-NiMoO4/NF. (Reproduced with permission from Ref. [85]) e Chronoamperometry experiments of LaNiO3 and NiO performed at 0.45, 0.50, and 0.58 V in 5 M KOH and 0.33 M urea solution. (Reproduced with permission from Ref. [93]) f Cycling stability tests for La0.5Sr1.5NiO4+δ performed in Ar-saturated 1 M KOH and 1 M urea solution at a scan rate of 10 mV s−1 over a potential window of 0.41 to 0.7 V. (Reproduced with permission from Ref. [94])

Fig. 6

Reproduced with permission from Ref. [118]. b Images of Ni–Fe2O3/rGO/PVA aerogel without (i) and with (ii) a load of 100 g, and the CV plots of NiO/rGO/PVA and c NiO–Fe2O3/rGO/PVA electrodes in absence and presence of 0.33 M urea in 1.0 M KOH electrolyte. (Reproduced with permission from Ref. [121]) d Schematic illustration of the fabrication processof the Ni-WC/C catalyst, and e their corresponding CV in the electrolyte of 1 M KOH and 0.33 M urea. (Reproduced with permission from Ref. [122])

Fig. 7

Reproduced with permission from Ref. [137]) b TEM images of small and large size MnO2 nanolayers with the size distribution histograms inset. The LSV plots of S-MnO2-G-NF in 1 M KOH electrolyte in the absence and presence of 0.5 M urea, and LSV comparison with other electrodes in 1 M KOH with 0.5 M urea. (Reproduced with permission from Ref. [145]) c SEM image (i), cross image (ii) and (iii) EDS mapping of the fabricated Zn0.08Co0.92P/TM electrode. Polarization curves (iv) for Zn0.08Co0.92P/TM||Zn0.08Co0.92P/TM as bifunctional catalysts in overall electrolysis in the presence and absence of 0.5 m urea in 1.0 m KOH. Photograph of overall urea electrolysis driven by a 1.0 V DC power supply (V). (Reproduced with permission from Ref. [147])

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Acknowledgements

This work was supported by grants from the National Key Research and Development Program of China (No. 2019YFC1906700), the National Natural Science Foundation of China (No. 219611322025, 21876049, 91834301), the China Postdoctoral Science Foundation (No. 2019M661412, 2019M661409, 2020T130190), and the Strategic Priority Research Program of the Chinese Academy of Sciences (No. XDA23010400). Liaoning Revitalization Talents Program (No. XLYC1807245) and Dalian High-Level Talent Innovation Program (No. 2017RQ085).

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Authors and Affiliations

  1. National Engineering Laboratory for Industrial Wastewater Treatment, East China University of Science and Technology, Shanghai, 200237, China

    Jianan Li, Jianping Li, Hualin Wang & Xuejing Yang

  2. School of Resources and Environmental Engineering, East China University of Science and Technology, Shanghai, 200237, China

    Jianan Li, Jianping Li, Chong Peng, Hualin Wang & Xuejing Yang

  3. State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China

    Jianan Li, Jianping Li, Hualin Wang & Xuejing Yang

  4. Department of Chemistry, Fudan University, Shanghai, 200433, China

    Ming Gong

  5. Dalian Research Institute of Petroleum and Petrochemicals, SINOPEC, Dalian, 116045, China

    Chong Peng

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  1. Jianan Li
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Li, J., Li, J., Gong, M. et al. Catalyst Design and Progresses for Urea Oxidation Electrolysis in Alkaline Media. Top Catal 64, 532–558 (2021). https://doi.org/10.1007/s11244-021-01453-w

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