Highly Reversible Aqueous Zinc Batteries enabled by Zincophilic–Zincophobic Interfacial Layers and Interrupted Hydrogen‐Bond Electrolytes

Aqueous Zn batteries promise high energy density but suffer from Zn dendritic growth and poor low‐temperature performance. Here, we overcome both challenges by using an eutectic 7.6 m ZnCl2 aqueous electrolyte with 0.05 m SnCl2 additive, which in situ forms a zincophilic/zincophobic Sn/Zn5(OH)8Cl2⋅H...

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Published in:	Angewandte Chemie (International ed.) Vol. 60; no. 34; pp. 18845 - 18851
Main Authors:	Cao, Longsheng, Li, Dan, Soto, Fernando A., Ponce, Victor, Zhang, Bao, Ma, Lu, Deng, Tao, Seminario, Jorge M., Hu, Enyuan, Yang, Xiao‐Qing, Balbuena, Perla B., Wang, Chunsheng
Format:	Journal Article
Language:	English
Published:	Weinheim Wiley Subscription Services, Inc 16.08.2021 Wiley
Edition:	International ed. in English
Subjects:	Aqueous electrolytes aqueous zinc batteries Dendritic structure Electrolytes ENERGY STORAGE Eutectics Flux density hydrogen bond Hydrogen bonds Ion currents Low temperature MATERIALS SCIENCE Plating salt precipitation Zinc Zinc chloride zincophilic-zincophobic interfacial bilayer
ISSN:	1433-7851, 1521-3773, 1521-3773
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Abstract	Aqueous Zn batteries promise high energy density but suffer from Zn dendritic growth and poor low‐temperature performance. Here, we overcome both challenges by using an eutectic 7.6 m ZnCl2 aqueous electrolyte with 0.05 m SnCl2 additive, which in situ forms a zincophilic/zincophobic Sn/Zn5(OH)8Cl2⋅H2O bilayer interphase and enables low temperature operation. Zincophilic Sn decreases Zn plating/stripping overpotential and promotes uniform Zn plating, while zincophobic Zn5(OH)8Cl2⋅H2O top‐layer suppresses Zn dendrite growth. The eutectic electrolyte has a high ionic conductivity of ≈0.8 mS cm−1 even at −70 °C due to the distortion of hydrogen bond network by solvated Zn2+ and Cl−. The eutectic electrolyte enables Zn∥Ti half‐cell a high Coulombic efficiency (CE) of >99.7 % for 200 cycles and Zn∥Zn cell steady charge/discharge for 500 h with a low overpotential of 8 mV at 3 mA cm−2. Practically, Zn∥VOPO4 batteries maintain >95 % capacity with a CE of >99.9 % for 200 cycles at −50 °C, and retain ≈30 % capacity at −70 °C of that at 20 °C. A highly reversible Zn anode working at low temperature is achieved by introducing SnCl2 into eutectic ZnCl2 aqueous electrolyte to form a zincophilic–zincophobic interfacial layer on the Zn anode in situ. The bottom layer of Sn facilitates uniform Zn deposition, while the top layer of zincophobic Zn5(OH)8Cl2 H2O facilitates Zn2+ diffusion and avoids Zn dendrites. The eutectic composition enhances the low temperature conductivity.
AbstractList	Aqueous Zn batteries promise high energy density but suffer from Zn dendritic growth and poor low-temperature performance. Here, we overcome both challenges by using an eutectic 7.6 m ZnCl2 aqueous electrolyte with 0.05 m SnCl2 additive, which in situ forms a zincophilic/zincophobic Sn/Zn5 (OH)8 Cl2 ⋅H2 O bilayer interphase and enables low temperature operation. Zincophilic Sn decreases Zn plating/stripping overpotential and promotes uniform Zn plating, while zincophobic Zn5 (OH)8 Cl2 ⋅H2 O top-layer suppresses Zn dendrite growth. The eutectic electrolyte has a high ionic conductivity of ≈0.8 mS cm-1 even at -70 °C due to the distortion of hydrogen bond network by solvated Zn2+ and Cl- . The eutectic electrolyte enables Zn∥Ti half-cell a high Coulombic efficiency (CE) of >99.7 % for 200 cycles and Zn∥Zn cell steady charge/discharge for 500 h with a low overpotential of 8 mV at 3 mA cm-2 . Practically, Zn∥VOPO4 batteries maintain >95 % capacity with a CE of >99.9 % for 200 cycles at -50 °C, and retain ≈30 % capacity at -70 °C of that at 20 °C.Aqueous Zn batteries promise high energy density but suffer from Zn dendritic growth and poor low-temperature performance. Here, we overcome both challenges by using an eutectic 7.6 m ZnCl2 aqueous electrolyte with 0.05 m SnCl2 additive, which in situ forms a zincophilic/zincophobic Sn/Zn5 (OH)8 Cl2 ⋅H2 O bilayer interphase and enables low temperature operation. Zincophilic Sn decreases Zn plating/stripping overpotential and promotes uniform Zn plating, while zincophobic Zn5 (OH)8 Cl2 ⋅H2 O top-layer suppresses Zn dendrite growth. The eutectic electrolyte has a high ionic conductivity of ≈0.8 mS cm-1 even at -70 °C due to the distortion of hydrogen bond network by solvated Zn2+ and Cl- . The eutectic electrolyte enables Zn∥Ti half-cell a high Coulombic efficiency (CE) of >99.7 % for 200 cycles and Zn∥Zn cell steady charge/discharge for 500 h with a low overpotential of 8 mV at 3 mA cm-2 . Practically, Zn∥VOPO4 batteries maintain >95 % capacity with a CE of >99.9 % for 200 cycles at -50 °C, and retain ≈30 % capacity at -70 °C of that at 20 °C. Aqueous Zn batteries promise high energy density but suffer from Zn dendritic growth and poor low‐temperature performance. Here, we overcome both challenges by using an eutectic 7.6 m ZnCl2 aqueous electrolyte with 0.05 m SnCl2 additive, which in situ forms a zincophilic/zincophobic Sn/Zn5(OH)8Cl2⋅H2O bilayer interphase and enables low temperature operation. Zincophilic Sn decreases Zn plating/stripping overpotential and promotes uniform Zn plating, while zincophobic Zn5(OH)8Cl2⋅H2O top‐layer suppresses Zn dendrite growth. The eutectic electrolyte has a high ionic conductivity of ≈0.8 mS cm−1 even at −70 °C due to the distortion of hydrogen bond network by solvated Zn2+ and Cl−. The eutectic electrolyte enables Zn∥Ti half‐cell a high Coulombic efficiency (CE) of >99.7 % for 200 cycles and Zn∥Zn cell steady charge/discharge for 500 h with a low overpotential of 8 mV at 3 mA cm−2. Practically, Zn∥VOPO4 batteries maintain >95 % capacity with a CE of >99.9 % for 200 cycles at −50 °C, and retain ≈30 % capacity at −70 °C of that at 20 °C. Aqueous Zn batteries promise high energy density but suffer from Zn dendritic growth and poor low‐temperature performance. Here, we overcome both challenges by using an eutectic 7.6 m ZnCl 2 aqueous electrolyte with 0.05 m SnCl 2 additive, which in situ forms a zincophilic/zincophobic Sn/Zn 5 (OH) 8 Cl 2 ⋅H 2 O bilayer interphase and enables low temperature operation. Zincophilic Sn decreases Zn plating/stripping overpotential and promotes uniform Zn plating, while zincophobic Zn 5 (OH) 8 Cl 2 ⋅H 2 O top‐layer suppresses Zn dendrite growth. The eutectic electrolyte has a high ionic conductivity of ≈0.8 mS cm −1 even at −70 °C due to the distortion of hydrogen bond network by solvated Zn 2+ and Cl − . The eutectic electrolyte enables Zn∥Ti half‐cell a high Coulombic efficiency (CE) of >99.7 % for 200 cycles and Zn∥Zn cell steady charge/discharge for 500 h with a low overpotential of 8 mV at 3 mA cm −2 . Practically, Zn∥VOPO 4 batteries maintain >95 % capacity with a CE of >99.9 % for 200 cycles at −50 °C, and retain ≈30 % capacity at −70 °C of that at 20 °C. Aqueous Zn batteries promise high energy density but suffer from Zn dendritic growth and poor low‐temperature performance. Here, we overcome both challenges by using an eutectic 7.6 m ZnCl2 aqueous electrolyte with 0.05 m SnCl2 additive, which in situ forms a zincophilic/zincophobic Sn/Zn5(OH)8Cl2⋅H2O bilayer interphase and enables low temperature operation. Zincophilic Sn decreases Zn plating/stripping overpotential and promotes uniform Zn plating, while zincophobic Zn5(OH)8Cl2⋅H2O top‐layer suppresses Zn dendrite growth. The eutectic electrolyte has a high ionic conductivity of ≈0.8 mS cm−1 even at −70 °C due to the distortion of hydrogen bond network by solvated Zn2+ and Cl−. The eutectic electrolyte enables Zn∥Ti half‐cell a high Coulombic efficiency (CE) of >99.7 % for 200 cycles and Zn∥Zn cell steady charge/discharge for 500 h with a low overpotential of 8 mV at 3 mA cm−2. Practically, Zn∥VOPO4 batteries maintain >95 % capacity with a CE of >99.9 % for 200 cycles at −50 °C, and retain ≈30 % capacity at −70 °C of that at 20 °C. A highly reversible Zn anode working at low temperature is achieved by introducing SnCl2 into eutectic ZnCl2 aqueous electrolyte to form a zincophilic–zincophobic interfacial layer on the Zn anode in situ. The bottom layer of Sn facilitates uniform Zn deposition, while the top layer of zincophobic Zn5(OH)8Cl2 H2O facilitates Zn2+ diffusion and avoids Zn dendrites. The eutectic composition enhances the low temperature conductivity.
Author	Wang, Chunsheng Ma, Lu Li, Dan Balbuena, Perla B. Deng, Tao Cao, Longsheng Yang, Xiao‐Qing Soto, Fernando A. Ponce, Victor Zhang, Bao Hu, Enyuan Seminario, Jorge M.
Author_xml	– sequence: 1 givenname: Longsheng orcidid: 0000-0002-2917-6523 surname: Cao fullname: Cao, Longsheng organization: University of Maryland – sequence: 2 givenname: Dan orcidid: 0000-0003-3097-9363 surname: Li fullname: Li, Dan organization: University of Maryland – sequence: 3 givenname: Fernando A. surname: Soto fullname: Soto, Fernando A. organization: Texas A&M University – sequence: 4 givenname: Victor surname: Ponce fullname: Ponce, Victor organization: Texas A&M University – sequence: 5 givenname: Bao surname: Zhang fullname: Zhang, Bao organization: University of Maryland – sequence: 6 givenname: Lu surname: Ma fullname: Ma, Lu organization: Brookhaven National Laboratory – sequence: 7 givenname: Tao surname: Deng fullname: Deng, Tao organization: University of Maryland – sequence: 8 givenname: Jorge M. surname: Seminario fullname: Seminario, Jorge M. organization: Texas A&M University – sequence: 9 givenname: Enyuan surname: Hu fullname: Hu, Enyuan organization: Brookhaven National Laboratory – sequence: 10 givenname: Xiao‐Qing surname: Yang fullname: Yang, Xiao‐Qing organization: Brookhaven National Laboratory – sequence: 11 givenname: Perla B. surname: Balbuena fullname: Balbuena, Perla B. email: balbuena@tamu.edu organization: Texas A&M University – sequence: 12 givenname: Chunsheng orcidid: 0000-0002-8626-6381 surname: Wang fullname: Wang, Chunsheng email: cswang@umd.edu organization: University of Maryland
BackLink	https://www.osti.gov/servlets/purl/1807958$$D View this record in Osti.gov
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Copyright	2021 Wiley‐VCH GmbH 2021 Wiley-VCH GmbH.
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Snippet	Aqueous Zn batteries promise high energy density but suffer from Zn dendritic growth and poor low‐temperature performance. Here, we overcome both challenges by... Aqueous Zn batteries promise high energy density but suffer from Zn dendritic growth and poor low-temperature performance. Here, we overcome both challenges by...
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SubjectTerms	Aqueous electrolytes aqueous zinc batteries Dendritic structure Electrolytes ENERGY STORAGE Eutectics Flux density hydrogen bond Hydrogen bonds Ion currents Low temperature MATERIALS SCIENCE Plating salt precipitation Zinc Zinc chloride zincophilic-zincophobic interfacial bilayer
Title	Highly Reversible Aqueous Zinc Batteries enabled by Zincophilic–Zincophobic Interfacial Layers and Interrupted Hydrogen‐Bond Electrolytes
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