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| Design Principles and Mechanistic Understandings of Non-Noble-Metal Bifunctional Electrocatalysts for Zinc-Air Batteries |
Yunnan Gao1, Ling Liu1, Yi Jiang1( ), Dexin Yu1, Xiaomei Zheng4, Jiayi Wang3, Jingwei Liu1, Dan Luo1, Yongguang Zhang1(), Zhenjia Shi1, Xin Wang3, Ya-Ping Deng2(), Zhongwei Chen1() |
1 Power Battery and Systems Research Center, State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, People’s Republic of China
2 Department of Chemical Engineering, University of Waterloo, Waterloo, ON, N2L 3G1, Canada
3 Institute of Carbon Neutrality, Zhejiang Wanli University, Ningbo, 315100, People’s Republic of China
4 College of Materials and Chemistry, China Jiliang University, Hangzhou, 310018, People’s Republic of China |
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Abstract Zinc-air batteries (ZABs) are promising energy storage systems because of high theoretical energy density, safety, low cost, and abundance of zinc. However, the slow multi-step reaction of oxygen and heavy reliance on noble-metal catalysts hinder the practical applications of ZABs. Therefore, feasible and advanced non-noble-metal electrocatalysts for air cathodes need to be identified to promote the oxygen catalytic reaction. In this review, we initially introduced the advancement of ZABs in the past two decades and provided an overview of key developments in this field. Then, we discussed the working mechanism and the design of bifunctional electrocatalysts from the perspective of morphology design, crystal structure tuning, interface strategy, and atomic engineering. We also included theoretical studies, machine learning, and advanced characterization technologies to provide a comprehensive understanding of the structure-performance relationship of electrocatalysts and the reaction pathways of the oxygen redox reactions. Finally, we discussed the challenges and prospects related to designing advanced non-noble-metal bifunctional electrocatalysts for ZABs.
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Received: 08 October 2023
Published: 26 March 2024
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Corresponding Authors:
Yi Jiang, Yongguang Zhang, Ya-Ping Deng, Zhongwei Chen
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About author:: Yunnan Gao, Ling Liu and Yi Jiang have contributed equally to this work. |
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Table 1 Comparison of various metal air batteries | Battery type | Cell voltage (V) | Specific energy (Wh kg−1) | Cost ($ per kg) | Electrolyte | Rechargeable | Advantage | Disadvantage | | Li-O2 | 2.96 | 5930 | 185.1 | Aprotic | Yes | High energy density | Unsafe operation, poor reversibility, poor cycle life | | Na-O2 | 2.3 | 1680 | 2.7 | Aprotic | Yes | | K-O2 | 2.37 | 1190 | 22.6 | Aprotic | Yes | | Zn-air | 1.65 | 1220 | 2.9 | Aqueous | Yes | Suitable theoretical energy density, nontoxicity, low cost, safety | Lack of active and durable bifunction-al electrocatalysts on the cathode | | Mg-air | 3.09 | 5240 | 3.0 | Aqueous | No | High theoretical energy density and discharge voltage | Poor rechargeability and practical values | | Al-air | 2.71 | 5780 | 2.6 | Aqueous | No | | Fe-air | 1.28 | 1080 | 0.5 | Aqueous | Yes | Low cost, good cyclability | Evolution of hydrogen and electrode passivation |
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Table 1 Comparison of various metal air batteries
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Fig. 1 The scope of this review, which covers three aspects in the sequence of catalysts and analytical engineering
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43,44,46,47,48,49,50]">
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Fig. 2 Schematic illustration of the progress of zinc-air batteries. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b43">43</xref>,<xref ref-type="bibr" rid="b44">44</xref>,<xref ref-type="bibr" rid="b46">46</xref>,<xref ref-type="bibr" rid="b47">47</xref>,<xref ref-type="bibr" rid="b48">48</xref>,<xref ref-type="bibr" rid="b49">49</xref>,<xref ref-type="bibr" rid="b50">50</xref>]
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Fig. 3 The distribution of the performance of the reported bifunctional electrocatalysts in recent three years
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68]. c TEM and d HRTEM of 1D La0.8Sr0.2Mn0.95Co0.05O3 nanowires. Reprinted with permission from Ref. [75]. e AFM image and f the corresponding height profiles of CoO nanosheets. Reprinted with permission from Ref. [63]. g Schematic illustration and h STEM image, and i elemental mapping (Ti, Co, O, N, and C) of 3DOM titanium oxynitride. Reprinted with permission from Ref. [87]">
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Fig. 4 a TEM and b HRTEM images of the graphene quantum dots. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b68">68</xref>]. c TEM and d HRTEM of 1D La<sub>0.8</sub>Sr<sub>0.2</sub>Mn<sub>0.9</sub>5Co<sub>0.05</sub>O<sub>3</sub> nanowires. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b75">75</xref>]. e AFM image and f the corresponding height profiles of CoO nanosheets. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b63">63</xref>]. g Schematic illustration and h STEM image, and i elemental mapping (Ti, Co, O, N, and C) of 3DOM titanium oxynitride. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b87">87</xref>]
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100]. c Schematic illustration of 2D BP-CN-c. Reprinted with permission from Ref. [99]. d A diagrammatic representation of electrolyte diffusion state on hollow CoFe-NC-x. Reprinted with permission from Ref. [102]. e-g CoO and Ni-Fe-layered double hydroxide with CNT hybrids for the electrocatalysis of ORR and OER. Reprinted with permission from Ref. [47]">
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Fig. 5 a, b HRTEM images of Ni<sub>3</sub>S<sub>2</sub> quantum dots. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b100">100</xref>]. c Schematic illustration of 2D BP-CN-c. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b99">99</xref>]. d A diagrammatic representation of electrolyte diffusion state on hollow CoFe-NC-x. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b102">102</xref>]. e-g CoO and Ni-Fe-layered double hydroxide with CNT hybrids for the electrocatalysis of ORR and OER. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b47">47</xref>]
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113]. c-e The Co2+/Co3+ surface atomic configurations and the corresponding side views of calculated O2-adsorption matter on different planes. Reprinted with permission from Ref. [116]. f, g Gibbs free energy and processes related to the ORR steps on the (111) and (200) facets of Ni0.8Fe0.2. Reprinted with permission from Ref. [117]. h TEM and HRTEM images of crystalline W2CoB2 with amorphous CoOOH layer. Reprinted with permission from Ref. [133]">
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Fig. 6 a The BET surface areas and b LSV curves of ORR of FeCoNC with star-like and dodecahedron-like structures. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b113">113</xref>]. c-e The Co<sup>2+</sup>/Co<sup>3+</sup> surface atomic configurations and the corresponding side views of calculated O<sub>2</sub>-adsorption matter on different planes. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b116">116</xref>]. f, g Gibbs free energy and processes related to the ORR steps on the (111) and (200) facets of Ni<sub>0.8</sub>Fe<sub>0.2</sub>. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b117">117</xref>]. h TEM and HRTEM images of crystalline W<sub>2</sub>CoB<sub>2</sub> with amorphous CoOOH layer. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b133">133</xref>]
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139]. Energy band of CoFe alloy and CoFe2O4 c before and d after Mott-Schottky contact. Reprinted with permission from Ref. [140]. e Schematic illustration of electron and mass transport during the OER process on FC-Ni3N (left), Ni3N/NCNT (middle) and FC-Ni3N/NCNT (right). Reprinted with permission from Ref. [144]. f AIMD simulations of water layers on CoS and Fe3S4. Reprinted with permission from Ref. [146]">
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Fig. 7 a, b HRTEM images of the interface between Co and Co<sub>3</sub>O<sub>4</sub>. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b139">139</xref>]. Energy band of CoFe alloy and CoFe<sub>2</sub>O<sub>4</sub> c before and d after Mott-Schottky contact. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b140">140</xref>]. e Schematic illustration of electron and mass transport during the OER process on FC-Ni<sub>3</sub>N (left), Ni<sub>3</sub>N/NCNT (middle) and FC-Ni<sub>3</sub>N/NCNT (right). Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b144">144</xref>]. f AIMD simulations of water layers on CoS and Fe<sub>3</sub>S<sub>4</sub>. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b146">146</xref>]
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151]. c ORR and OER mechanisms over Co3O4-x/NG. d The calculated free energy diagram of ORR/OER for three different Co sites. Reprinted with permission from Ref. [152]. e Raman and f ESR spectra of different NiFe samples. Reprinted with permission from Ref. [154]">
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Fig. 8 a O 1s spectra and b O K-edge XANES spectra for NiCo<sub>2.148</sub>O<sub>4</sub>, NiCo<sub>2.150</sub>O<sub>4</sub>, and NiCo<sub>2.137</sub>O<sub>4</sub> PNSs. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b151">151</xref>]. c ORR and OER mechanisms over Co<sub>3</sub>O<sub>4</sub>-x/NG. d The calculated free energy diagram of ORR/OER for three different Co sites. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b152">152</xref>]. e Raman and f ESR spectra of different NiFe samples. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b154">154</xref>]
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158]. b, c XRD patterns, d FFT image of D-CMO. Reprinted with permission from Ref. [159]. Schematic diagram of the e intact ZIFs and f linker-deficient ZIFs. Reprinted with permission from Ref. [160]">
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Fig. 9 a Schematic illustration of the synthesis of CoO<sub>0.87</sub>S<sub>0.13</sub>/GN. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b158">158</xref>]. b, c XRD patterns, d FFT image of D-CMO. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b159">159</xref>]. Schematic diagram of the e intact ZIFs and f linker-deficient ZIFs. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b160">160</xref>]
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174]. d Schematic illustration of the polymerization/crystallization of the COF-F and its subsequent carbonization for preparing NFPC. Reprinted with permission from Ref. [175]. e Schematic diagram of P/Fe-N-C catalyst. f Contour plot of OER overpotential as a function of Gibbs adsorption energies. Reprinted with permission from Ref. [179]">
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Fig. 10 a XPS spectra of N1s for the samples after calcination in different temperatures. b Diagram of different configuration of N doping. c ORR and OER performance of four catalysts compared with commercial Pt/C and IrO<sub>2</sub>. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b174">174</xref>]. d Schematic illustration of the polymerization/crystallization of the COF-F and its subsequent carbonization for preparing NFPC. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b175">175</xref>]. e Schematic diagram of P/Fe-N-C catalyst. f Contour plot of OER overpotential as a function of Gibbs adsorption energies. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b179">179</xref>]
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209]. c Schematic illustration of the preparation of atomically dispersed Mn catalysts. Reprinted with permission from Ref. [212]. d A schematic diagram of a Zn-air battery assembled with Ni-N4/GHSs/Fe-N4. e Free energies of OER and f PDOS of the single-atom sites of Fe-N4 and Ni-N4. Reprinted with permission from Ref. [214]">
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Fig. 11 a LSV curves and Tafel plots of the CoNC@LDH and Pt/C + Ir/C for ORR and OER, respectively. b Descriptor of ORR and OER activity among CoNC@LDH and other reported bifunctional electrocatalysts. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b209">209</xref>]. c Schematic illustration of the preparation of atomically dispersed Mn catalysts. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b212">212</xref>]. d A schematic diagram of a Zn-air battery assembled with Ni-N<sub>4</sub>/GHSs/Fe-N<sub>4</sub>. e Free energies of OER and f PDOS of the single-atom sites of Fe-N<sub>4</sub> and Ni-N<sub>4</sub>. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b214">214</xref>]
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24]. Free energy diagram of various Co9S8 for c ORR and d OER pathways. Reprinted with permission from Ref. [199]. The HOMO of D-CMO (121) with e OH* absorption and f OOH* absorption, respectively. Reprinted with permission from Ref. [159]. FEM multiphysics modeling of O2 diffusion and O2 concentration contour near g the CoS/Fe3S4@SNCP and h CoS@SNCP air cathodes. i Three representative structures during AIMD simulations. Reprinted with permission from Ref. [146]">
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Fig. 12 a The calculated d band density of state for the transition metal atoms in ZnHZ, CoHZ, and BHZ-48. b Schematic illustration explaining change of metal adsorbate interaction by altering the metal d band center (ε<sub>d</sub>). Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b24">24</xref>]. Free energy diagram of various Co<sub>9</sub>S<sub>8</sub> for c ORR and d OER pathways. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b199">199</xref>]. The HOMO of D-CMO (121) with e OH* absorption and f OOH* absorption, respectively. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b159">159</xref>]. FEM multiphysics modeling of O<sub>2</sub> diffusion and O<sub>2</sub> concentration contour near g the CoS/Fe<sub>3</sub>S<sub>4</sub>@SNCP and h CoS@SNCP air cathodes. i Three representative structures during AIMD simulations. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b146">146</xref>]
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219]. d Brief description of the ML process, divided into three parts, the data from DFT calculation, the ML model, and the feature importance analysis. e Calculated DFT ΔG *OH vs. ΔG *OH value obtained from ML by the GBR algorithm. f Feature importance of each descriptor with the corresponding proportion. Reprinted with permission from Ref. [220]">
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Fig. 13 a Heat map visualization of the OER activity of double perovskites as a function of A-site/B-site cations in terms of the OER overpotentials and cubic phase probability. The red/blue color bar represent the overpotentials, and the purple bar represents the tolerance factor. b Parity plot for DFT-calculated vs. Gaussian process model prediction of descriptor adsorption free energies on candidate perovskite structures. c Polar distribution plots of the most informatic descriptors (KL entropy index > 0.4). Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b219">219</xref>]. d Brief description of the ML process, divided into three parts, the data from DFT calculation, the ML model, and the feature importance analysis. e Calculated DFT ΔG *OH vs. ΔG *OH value obtained from ML by the GBR algorithm. f Feature importance of each descriptor with the corresponding proportion. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b220">220</xref>]
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221]. b AFM image and c the corresponding height profiles of Cu/Fe-NG. Reprinted with permission from Ref. [82]. d, e HAADF-STEM image and corresponding EDS mapping images on N, Co, Ni, Fe, and O elements of CoNC@LDH. Reprinted with permission from Ref. [209]. f Comparative testing of the contact angles at air-water-solid catalyst interfaces. Reprinted with permission from Ref. [222]">
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Fig. 14 a (Top) A heatmap of the summed scale factors for Zn and ZnO. (Middle) wt% Zn heatmap showing the reaction front of the Zn/ZnO phase transformation. (Bottom) voltage profile over time, shown with the corrected scale factor for Zn and ZnO. (Right) A close-up of the anode subdivided in 0.2 mm × 1 mm segments and schematic diagram showing the capillary-based ZAB. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b221">221</xref>]. b AFM image and c the corresponding height profiles of Cu/Fe-NG. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b82">82</xref>]. d, e HAADF-STEM image and corresponding EDS mapping images on N, Co, Ni, Fe, and O elements of CoNC@LDH. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b209">209</xref>]. f Comparative testing of the contact angles at air-water-solid catalyst interfaces. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b222">222</xref>]
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223]. c Cu K-edge XANES, d FT k3-weighted Cu K-edge EXAFS, and e WT-EXAFS spectra of Cu-SAs@N-CNS and Reference samples. f, g FT-EXAFS fitting curves for Cu-SAs@N-CNS in R and K spaces. Reprinted with permission from Ref. [211]">
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Fig. 15 In situ Raman spectra collected on CoNi-CoN<sub>4</sub>-HPC-900 for a the ORR process and b the OER process in 0.1 M KOH solution. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b223">223</xref>]. c Cu K-edge XANES, d FT k<sup>3</sup>-weighted Cu K-edge EXAFS, and e WT-EXAFS spectra of Cu-SAs@N-CNS and Reference samples. f, g FT-EXAFS fitting curves for Cu-SAs@N-CNS in R and K spaces. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b211">211</xref>]
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230]. b, c The operando XANES spectra of Co. Reprinted with permission from Ref. [192]. d Operando 2D HEXRD contour map of (Fe, Ni)Se2 in a Zn-air battery. e Schematic demonstration of the Se-driven reconstruction mechanism. Reprinted with permission from Ref. [231]">
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Fig. 16 a Illustration of operando XAS set up for ZAB under realistic device working conditions. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b230">230</xref>]. b, c The operando XANES spectra of Co. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b192">192</xref>]. d Operando 2D HEXRD contour map of (Fe, Ni)Se<sub>2</sub> in a Zn-air battery. e Schematic demonstration of the Se-driven reconstruction mechanism. Reprinted with permission from Ref. [<xref ref-type="bibr" rid="b231">231</xref>]
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