# Fileset

[DQ221014-PILZ@Zn-supporting.docx](https://mdr.nims.go.jp/filesets/536e5fe5-4877-4285-bbd9-148bb09a74c9/download)

## Creator

Qiaohui Duan, Kaiming Xue, Xin Yin, [Denis Y.W. Yu](https://orcid.org/0000-0002-5883-7087)

## Rights

[Creative Commons BY-NC-ND Attribution-NonCommercial-NoDerivs 4.0 International](https://creativecommons.org/licenses/by-nc-nd/4.0/)

## Other metadata

[A cationic polymeric interface enabling dendrite-free and highly stable aqueous Zn-metal batteries](https://mdr.nims.go.jp/datasets/10c28506-8d1e-4b83-b926-83657dfb4e7b)

## Fulltext

A Cationic Polymeric Interface Enabling Dendrite-free and Highly Stable Aqueous Zn-metal Batteries Qiaohui Duana, Kaiming Xuea, Xin Yina, Denis Y. W. Yua,b,*a School of Energy and Environment, City University of Hong Kong, 83 Tat Chee Avenue, Kowloon, Hong Kong S.A.Rb Center of Super-Diamond and Advanced Films (COSDAF), City University of Hong Kong, 83 Tat Chee Avenue, Kowloon, Hong Kong S.A.R.* Corresponding authorEmail: denisyu@cityu.edu.hkAddress: YEUNG G5702, Tat Chee Ave, Kowloon, Hong Kong SAR, People’s Republic of ChinaFigure S1. (a) SEM of bare Zn foil; (b) EDX spectrum of PILZ@Zn. Figure S2. Plot of apparent tracer mobility vs. displacement from the surface in surface zeta potential tests and the linear fitting. Figure S3. Symmetrical Zn-Zn stripping-plating of PILZ@Zn electrodes with different PILZ coating thicknesses.Figure S4. Cross-section SEM images of the bare Zn, PVDF@Zn and PILZ@Zn electrodes after symmetrical Zn-Zn stripping-plating for 100 h.  Figure S5. Surface zeta potential of PILZ@Zn electrode upon symmetrical Zn-Zn stripping-plating tests after different number of hours.Figure S6. (a) SEM, (b) XRD of the ball-milled commercial MnO2.  Bare Zn PVDF@Zn PILZ@Zn Tracer zeta potential (mV) 6.1 -22.8 50.2 Intercept of fitting curve (mV) 6.0 20 21.7 Surface zeta potential (mV) +0.1 -42.8 +28.5 Fitting R2 0.87 0.99 0.98Table S1. Calculation of surface zeta potential of the electrodes.*Surface zeta potential = - intercept + tracer zeta potentialTable S2. Comparison of this work with other previously reported cycling performance of symmetrical cells with Zn electrodes. Cell configurations Electrolyte Current density (mA cm-2) Areal capacity (mAh cm-2) Cycle life (h) Reference Cu mesh substrate + PAM electrolyte additive 1 M ZnSO4 + 0.5 M Na2SO4 + 1 g L−1 polyacrylamide 1 1 180 [1] Ce3+ and La3+ electrolyte additive 1M ZnSO4 + 0.01 M Ce2(SO4)3  1 1 400 [2] PAN coating on Zn 2M Zn(OTf)2 1 1 1100 [3] Bis-tris electrolyte additive 2 M ZnSO4 + 0.1M Bis-tris 1 1 1200 [4] Zn-Al alloy 2M ZnSO4 0.5 0.5 2000 [5] Eutectic Zn(ClO4)2-MSM electrolyte Zn(ClO4)2·6H2O-MSM (1:2 in mol)  1 0.25 2000 [6] PILZ coating on Zn 1M ZnSO4 1 1 2000 This workTable S3. Comparison of this work with other previously reported uniform Zn deposition. Cell configuration Testing condition Uniform Zn deposition (mAh cm-2) Reference PA layer on Ti 0.2 mA cm-2, 15 h 3 [7] Zn(H2PO4)2 electrolyte additive 1 mA cm-2, 3 h 3 [8] ZIF layer on Zn 5 mA cm-2, 1 h 5 [9] MGA layer on Zn N/A 5 [10] Glucose electrolyte additive 5 mA cm-2, 80 min 6.7 [11] PILZ layer on Cu 10 mA cm-2, 2 h  20 This work*N/A: not mentioned Reference:[1] Q. Zhang, J. Luan, L. Fu, S. Wu, Y. Tang, X. Ji, H. Wang, The three‐dimensional dendrite‐free zinc anode on a copper mesh with a zinc‐oriented polyacrylamide electrolyte additive, Angewandte Chemie, 131 (2019) 15988-15994.[2] Y. Li, P. Wu, W. Zhong, C. Xie, Y. Xie, Q. Zhang, D. Sun, Y. Tang, H. Wang, A progressive nucleation mechanism enables stable zinc stripping–plating behavior, Energy & Environmental Science, 14 (2021) 5563-5571.[3] P. Chen, X. Yuan, Y. Xia, Y. Zhang, L. Fu, L. Liu, N. Yu, Q. Huang, B. Wang, X. Hu, An Artificial Polyacrylonitrile Coating Layer Confining Zinc Dendrite Growth for Highly Reversible Aqueous Zinc‐Based Batteries, Advanced Science, 8 (2021) 2100309.[4] M. Luo, C. Wang, H. Lu, Y. Lu, B.B. Xu, W. Sun, H. Pan, M. Yan, Y. Jiang, Dendrite-free zinc anode enabled by zinc-chelating chemistry, Energy Storage Materials, 41 (2021) 515-521.[5] S.-B. Wang, Q. Ran, R.-Q. Yao, H. Shi, Z. Wen, M. Zhao, X.-Y. Lang, Q. Jiang, Lamella-nanostructured eutectic zinc–aluminum alloys as reversible and dendrite-free anodes for aqueous rechargeable batteries, Nature Communications, 11 (2020) 1-9.[6] M. Han, J. Huang, X. Xie, T.C. Li, J. Huang, S. Liang, J. Zhou, H.J. Fan, Hydrated Eutectic Electrolyte with Ligand‐Oriented Solvation Shell to Boost the Stability of Zinc Battery, Advanced Functional Materials, (2022) 2110957.[7] Z. Zhao, J. Zhao, Z. Hu, J. Li, J. Li, Y. Zhang, C. Wang, G. Cui, Long-life and deeply rechargeable aqueous Zn anodes enabled by a multifunctional brightener-inspired interphase, Energy & Environmental Science, 12 (2019) 1938-1949.[8] X. Zeng, J. Mao, J. Hao, J. Liu, S. Liu, Z. Wang, Y. Wang, S. Zhang, T. Zheng, J. Liu, Electrolyte design for in situ construction of highly Zn2+‐conductive solid electrolyte interphase to enable high‐performance aqueous Zn‐ion batteries under practical conditions, Advanced Materials, 33 (2021) 2007416.[9] X. Liu, F. Yang, W. Xu, Y. Zeng, J. He, X. Lu, Zeolitic imidazolate frameworks as Zn2+ modulation layers to enable dendrite‐free Zn anodes, Advanced Science, 7 (2020) 2002173.[10] J. Zhou, M. Xie, F. Wu, Y. Mei, Y. Hao, L. Li, R. Chen, Encapsulation of Metallic Zn in a Hybrid MXene/Graphene Aerogel as a Stable Zn Anode for Foldable Zn‐Ion Batteries, Advanced Materials, 34 (2022) 2106897.[11] P. Sun, L. Ma, W. Zhou, M. Qiu, Z. Wang, D. Chao, W. Mai, Simultaneous regulation on solvation shell and electrode interface for dendrite‐free Zn ion batteries achieved by a low‐cost glucose additive, Angewandte Chemie, 133 (2021) 18395-18403.image4.emf0 125 250 375 500-40-30-20-100102030PVDF@ZnApparent zeta potential (mV)Surface displacement (mm)image5.emf0 125 250 375 500-20-1001020Apparent zeta potential (mV)Surface displacement (mm)bare Znimage6.emf0 500 1000 1500 2000-0.20-0.15-0.10-0.050.000.050.100.150.20Voltage(V)Time(h) PILZ@Zn-13mm PILZ@Zn-30 µm PILZ@Zn-50 µm1mA cm-21mAh cm-2image7.pngimage8.emf28.527.630.129.2pristine 100 h 200h 500h01020304050Surface zeta potential (mV)PILZ@Zn upon symetrical Zn-Zn stripping-platingimage9.pngimage1.emf0 2 4 6 8 10ZnSFOCIntensity (a.u.)Energy (KeV)Nimage2.pngimage3.emf0 125 250 375 50020253035PILZ@ZnApparent zeta potential (mV)Surface displacement (mm)