In-Situ Integration of a Hydrophobic and Fast-Zn2+ -Conductive Inorganic Interphase to Stabilize Zn Metal Anodes

Mengyu Liu; Wentao Yuan; Guoqiang Ma; Kaiyue Qiu; Xueyu Nie; Yongchang Liu; Shigang Shen; Ning Zhang

doi:10.1002/anie.202304444

In-Situ Integration of a Hydrophobic and Fast-Zn²⁺ -Conductive Inorganic Interphase to Stabilize Zn Metal Anodes

Angew Chem Int Ed Engl. 2023 Jul 3;62(27):e202304444. doi: 10.1002/anie.202304444. Epub 2023 May 19.

Authors

Mengyu Liu¹, Wentao Yuan¹, Guoqiang Ma¹, Kaiyue Qiu¹, Xueyu Nie¹, Yongchang Liu², Shigang Shen¹, Ning Zhang¹

Affiliations

¹ College of Chemistry and Materials Science, Key Laboratory of Analytical Science and Technology of Hebei Province, Hebei University, Baoding, 071002, P. R. China.
² Beijing Advanced Innovation Center for Materials Genome Engineering, Institute for Advanced Materials and Technology, State Key Laboratory for Advanced Metals and Materials, University of Science and Technology Beijing, Beijing, 100083, P. R. China.

PMID: 37129439
DOI: 10.1002/anie.202304444

Abstract

The irreversible issues of Zn anode stemming from dendrite growth and water-induced erosion have severely hindered the commercialization of rechargeable aqueous Zn batteries. Herein, a hydrophobic and fast-Zn²⁺ -conductive zinc hexacyanoferrate (HB-ZnHCF) interphase layer is in situ integrated on Zn by a rapid room-temperature wet-chemistry method to address these dilemmas. Different from currently proposed hydrophilic inorganic cases, the hydrophobic and compact HB-ZnHCF interphase effectively prevents the access of water molecules to Zn surface, thus avoiding H₂ evolution and Zn corrosion. Moreover, the HB-ZnHCF with large internal ion channels, strong zincophilicity, and high Zn²⁺ transference number (0.86) permits fast Zn²⁺ transport and enables smooth Zn deposition. Remarkably, the resultant HB-ZnHCF@Zn electrode delivers unprecedented reversibility with 99.88 % Coulombic efficiency over 3000 cycles, realizes long-term cycling over 5800 h (>8 months, 1 mA cm^-2 ) and 1000 h (10 mA cm^-2 ), and assures the stable operation of full Zn battery with both coin- and pouch-type configurations.

Keywords: Aqueous Zn Battery; Hydrophobic Interphase; Inorganic Interphase; Zinc Hexacyanoferrate; Zn Metal Anode.

Abstract

Grants and funding