J. Semicond. > 2020, Volume 41 > Issue 9 > 091705
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REVIEWS

Recent progress on nanostructured bimetallic electrocatalysts for water splitting and electroreduction of carbon dioxide

Can Cui1, Xiaosong Hu2 and Liaoyong Wen2,

+ Author Affiliations

 Corresponding author: Liaoyong Wen, wenliaoyong@westlake.edu.cn

DOI: 10.1088/1674-4926/41/9/091705

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Abstract: The exploitation of renewable energy as well as the elimination of the harmful impact of excessive carbon emission are worldwide concerns for sustainable development of the ecological environment on earth. To address that, the technologies regarding energy conversion systems, such as water splitting and electroreduction of carbon dioxide, have attracted significant attention for a few decades. Yet, to date, the production of green fuels and/or high energy density chemicals like hydrogen, methane, and ethanol, are still suffering from many drawbacks including high energy consumption, low selectivity, and sluggish reaction rate. In this regard, nanostructured bimetallic materials that is capable of taking the full benefits of the coupling effects between different elements/components with structure modification in nanoscale are considered as a promising strategy for high-performance electrocatalysts. Herein, this review aims to outline the important progress of these nanostructured bimetallic electrocatalysts. It starts with the introduction of some important fundamental background knowledge about the reaction mechanism to understand how these reactions happen. Subsequently, we summarize the most recent progress regarding how the nanostructured bimetallic electrocatalysts manipulate the activity and selectivity of catalytic reactions in the order of bimetallic alloying effect, interface/substrate effect of bi-component electrocatalyst, and nanostructuring effect.

Key words: bimetallic electrocatalysts, nanostructures, water splitting, electroreduction of carbon dioxide



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Fig. 1.  (a) Volcano plot for the HER on metal electrodes in acidic media[20]. Reprinted with permission, Copyright 2010, American Chemical Society. (b) Activity trends for OER as a function of $ \mathrm{\Delta }{G}_{{\mathrm{O}}^{{*}}}-\mathrm{\Delta }{G}_{\mathrm{O}{\mathrm{H}}^{{*}}} $ for rutile and anatase oxides. The activity is expressed by the value of overpotential to achieve a certain value of current density[17]. Reprinted with permission, Copyright 2011, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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Fig. 2.  (Color online) (a) Microstructure and interfaces of the molybdenum sulfide@NPG. (b) HER polarization curves of NPG, MoS2@GCE, and MoS2@NPG[50]. Reprinted with permission, Copyright 2014, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (c) Cross-sectional SEM image of the NiCeOx–Au film. (d) Activity difference between NiCeO x supported on either Au-coated or bare GC disk, as well as OER performance of NiCeOx–Au compared to those benchmarking catalysts reported. (e) Representation of the theoretical overpotential as a function of the difference in O* and HO* adsorption Gibbs energies. (f) DFT+U calculations illustrates the support effects on modifying performance of NiCeOx–Au[52]. Reprinted with permission, Copyright 2016, Springer Nature. (g) Comparison of activity and (h) impedance spectra for Ni-based electrodes with various mass loading and composition. (i) In situ XAS of NiOOH and NiCeOOH on GC and Au substrates[53]. Reprinted with permission, Copyright 2017, American Chemical Society. (j) Adsorption sites and adsorption energies of OH on FeNi LDH and FeNi LDH with hydroxide interfacial layer, respectively. (k) Mass activity and (l) stability test of the FeNi LDH on foils at 1.5 V vs RHE for 10 h[49]. Reprinted with permission, Copyright 2018, American Chemical Society.

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Fig. 3.  (Color online) (a) SEM image of an α-Ni(OH)2 hollow sphere and a digital photo of the nanosheet-assembled α-Ni(OH)2 hollow spheres deposited on glassy carbon. (b) Comparison of CVs recorded at 100th cycle for bare GC electrode and modified GC electrodes comprising the α- and β-Ni(OH)2 nanocrystals, RuO2, and 20 wt% Pt/C and the corresponding Tafel slope[74]. Reprinted with permission, Copyright 2014, American Chemical Society. (c) SEM and TEM images for Cu@NiFe LDH for morphology characterization[60]. Reprinted with permission, Copyright 2017, Royal Society of Chemistry. (d) Polarization curves of CoS2 film and CoS2 nanowire/microwire array towards the morphology-dependent enhancement of both performance and stability. Bottom sketch describe the effect of morphology changing of CoS2 towards the bubble evolution[68]. Reprinted with permission, Copyright 2014, American Chemical Society. (e) Illustration of 3D-nanomesh nickel electrode and the long-term stability tests of Ni foam, the 3D-nanomesh Ni electrode and the 3D-nanomesh NiFe electrode[75]. Reprinted with permission, Copyright 2018, Elsevier.

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Fig. 4.  (Color online) (a) SEM image of the large area SP superlattices and inserted photograph of the SP superlattices with dimensions 0.7 × 0.7 cm2. (b) High-magnification SEM image of the long-rang-ordered Pt nanocrystals and TEM image of the nanocrystal superlattice. (c) Polarization curves of Pt SP5, Pt SP10, Pt SP20, Pt SP50, Pt NP film, Pt/C film and Pt foil electrocatalysts, the current density was normalized by geometry area. (d) Stability testing on Pt SP5 for 11 h. (e) Stability testing on Pt NP films. (f) Schematic illustration of the growth of gas bubbles on a flat film electrode. (g) Schematic illustration of the stability difference between flat film and SP electrode. (h–j) Snapshots of digital videos taken during electrolysis at 10 mA/cm2, magnified observations and schematic illustration of single bubble behavior on (h) Pt SP5, (i) Pt SP20 and (j) Pt NP film. (k) i–t curves with a stable and straight curve in the case of Pt SP5 and serrated curves on the Pt SP20 and Pt NP films[37]. Reprinted with permission, Copyright 2019, American Chemical Society.

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Fig. 5.  (Color online) Possible mechanistic pathways of CO2 reduction to C1 and C2 products[12]. Reprinted with permission, Copyright 2019, American Chemical Society.

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Fig. 6.  (Color online) (a) Microstructural analysis and bulk compositions of the catalysts. (b) Calculated reaction energy profiles for CO2 electroreduction to form CO (top) and HCOOH (bottom) on the PdSnO2 surface[113]. Reprinted with permission, Copyright 2019, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (c) Surface valence band photoemission spectra of Au–Cu bimetallic nanoparticles. (d) Schematic showing the proposed mechanism for CO2 reduction on the catalyst surface of Au–Cu bimetallic nanoparticles[120]. Reprinted with permission, Copyright 2014, Springer Nature. (e) The sketch of atomic ordering transformation of AuCu nanoparticles and the corresponding structural investigation. (f) Computational results of CO2 reduction on AuCu surfaces. (g) The illustration of CuPd nanoalloys with different structures and the corresponding comparison of FE[125]. Reprinted with permission, Copyright 2017, American Chemical Society. (h) The SEM image of NixGay alloying and the terminal products[95]. Reprinted with permission, Copyright 2016, American Chemical Society.

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Fig. 7.  (Color online) (a) A schematic illustration of the Ag3Sn core-shell structure. (b) CO2 reduction Faradaic efficiencies of AgSn/SnOx. (c) The most favorable free energy pathways of CO and HCOOH formation on SnO with Ov and –(O)H*, respectively[112]. Reprinted with permission, Copyright 2017, American Chemical Society. (d) Schematic and TEM characterization of the three types of Ag/Cu nanocrystals. (e) The schematic illustration and activity comparison of Ag NPs, Cu NPs, and AgCu alloy with various composition ratio[137]. Reprinted with permission, Copyright 2019, American Chemical Society. (f) Interaction between CeOx/Au(111) and CO2 (g) DFT calculations of CO2RR at 0 V vs RHE on Au(111) and Ce3O7H7/Au(111) surfaces[134]. Reprinted with permission, Copyright 2017, American Chemical Society. (h) Schematic illustration of the synthesis process and the corresponding morphology and composition characterization of the Ag@Al-PMOF. (i) FEs and total current densities for Ag NCs and Ag@Al-PMOF hybrids with different MOF thicknesses[138]. Reprinted with permission, Copyright 2017, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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Fig. 8.  (Color online) (a) Schematic illustration of the structure of Cu nanofoams and the terminal products. (b) Product distribution as a function of applied potential during the electrochemical reduction of CO2[145]. Reprinted with permission, Copyright 2014, American Chemical Society. (c) SEM images of the Cu cube surface and cyclic voltammograms of Cu cube and polycrystalline cupper surface towards formation of H2, methane and ethylene[146]. Reprinted with permission, Copyright 2015, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (d) Schematic showing the Cu overlayer structure-dependency over the formation of hydrocarbons. (e) Ratios of RFSs for CH4/C2H4 on different thicknesses of the Cu layer deposited on a pure Pt substrate obtained from the CO2 reduction experiments[147]. Reprinted with permission, Copyright 2013, American Chemical Society.

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Fig. 9.  (Color online) (a) This is illustrated on a diving bell spider for subaquatic breathing. (b) A hydrophobic dendritic Cu surface for aqueous CO2 reduction. (c) The contact angle measurements of the wettable and hydrophobic dendrite. (d) SEM image of the hydrophobic dendrite. (e) Illustration of the hydrophobic dendrite gaining a solid–liquid interface on the application of a negative potential. (f) CPE product FEs from the wettable and hydrophobic dendrite at various potentials. (g) The proposed role of hydrophobicity in promoting CO2 reduction over proton reduction[140]. Reprinted with permission, Copyright 2019, Springer Nature. (h) SEM images of EDTA modified porous hollow cupper sphere. (i) FE of all the reduction products for H-Cu MPs at various potentials. (j) Free energy profiles for the CO dimerization reaction on surfaces with or without EDTA modification[149]. Reprinted with permission, Copyright 2020, American Chemical Society.

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    Received: 01 July 2020 Revised: 13 July 2020 Online: Accepted Manuscript: 19 August 2020Uncorrected proof: 21 August 2020Published: 04 September 2020

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      Article Navigation >  Journal of Semiconductors  > 2020  >  41(9): 091705
      Can Cui, Xiaosong Hu, Liaoyong Wen. Recent progress on nanostructured bimetallic electrocatalysts for water splitting and electroreduction of carbon dioxide[J]. Journal of Semiconductors, 2020, 41(9): 091705. doi: 10.1088/1674-4926/41/9/091705 ****C Cui, X S Hu, L Y Wen, Recent progress on nanostructured bimetallic electrocatalysts for water splitting and electroreduction of carbon dioxide[J]. J. Semicond., 2020, 41(9): 091705. doi: 10.1088/1674-4926/41/9/091705.
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      Can Cui, Xiaosong Hu, Liaoyong Wen. Recent progress on nanostructured bimetallic electrocatalysts for water splitting and electroreduction of carbon dioxide[J]. Journal of Semiconductors, 2020, 41(9): 091705. doi: 10.1088/1674-4926/41/9/091705 ****
      C Cui, X S Hu, L Y Wen, Recent progress on nanostructured bimetallic electrocatalysts for water splitting and electroreduction of carbon dioxide[J]. J. Semicond., 2020, 41(9): 091705. doi: 10.1088/1674-4926/41/9/091705.
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      Recent progress on nanostructured bimetallic electrocatalysts for water splitting and electroreduction of carbon dioxide

      DOI: 10.1088/1674-4926/41/9/091705
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        Department of Materials Science and Engineering & Institute of Materials Science, University of Connecticut, Storrs, Connecticut, 06269-3136, United States of America

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        Key Laboratory of 3D Micro/Nano Fabrication and Characterization of Zhejiang Province, School of Engineering, Westlake University, Hangzhou 310024, China

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