Molecular Engineering of N-heteroaromatic Organic Cathode for High-Voltage and Highly Stable Zinc Batteries

Yichao Yan; Pei Li; Yiqiao Wang; Leyu Bi; Ting Wai Lau; Mulin Miao; Shuo Yang; Qi Xiong; Francis R Lin; Hin-Lap Yip; Jun Yin; Chunyi Zhi; Alex K.-Y. Jen

doi:10.1002/adfm.202312332

Molecular Engineering of N-heteroaromatic Organic Cathode for High-Voltage and Highly Stable Zinc Batteries

Yichao Yan (Co-first Author), Pei Li (Co-first Author), Yiqiao Wang, Leyu Bi, Ting Wai Lau, Mulin Miao, Shuo Yang, Qi Xiong, Francis R Lin, Hin-Lap Yip, Jun Yin^*, Chunyi Zhi^*, Alex K.-Y. Jen^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

10 Citations (Scopus)

Abstract

Zinc batteries hold promise for grid-scale energy storage due to their safety and low cost. A key challenge for the field is identifying cathode materials that can undergo reversible redox reactions at the extreme potentials required for realizing high energy density devices. While organic materials have been extensively explored as cathode materials due to their structural tunability and eco-friendliness, most reported zinc-organic batteries exhibit a voltage lower than 1.2 V. In this report, by employing rational molecular design and synthesis, computational analysis, and electrochemical evaluation, the well-studied neutral p-type N-centered is redesigned, triphenylamine organic cathode by replacing three phenyl rings with the smallest aromatic system – cationic cyclopropenium. This results in a novel class of cathode materials with simultaneously enhanced potential, capacity, and stability. The resultant full battery exhibits a high discharge voltage of 1.7 V and an outstanding capacity retention of 95% after 10000 cycles at a discharge capacity of 157.5 mAh g⁻¹cation (103.9 mAh g⁻¹salt).

Original language	English
Article number	2312332
Journal	Advanced Functional Materials
Volume	35
Issue number	2
Online published	2 Jan 2024
DOIs	https://doi.org/10.1002/adfm.202312332
Publication status	Published - 22 May 2025

Funding

Y.Y and P.L. contributed equally to this work. The work described in this paper was partially supported by a fellowship award from the Research Grants Council of the Hong Kong Special Administrative Region, China (Project No. CityU PDFS2223-1S08). A.K.-Y.J. is thankful for the sponsorship of the Lee Shau-Kee Chair Professor (Materials Science) and the support from the APRC Grant of the City University of Hong Kong (9380086), the TCFS Grant (GHP/018/20SZ), the MRP Grant (MRP/040/21X) from the Innovation and the Technology Commission of Hong Kong, the Green Tech Fund (202020164) from the Environment and Ecology Bureau of Hong Kong, and the Guangdong Major Project of Basic and the Applied Basic Research (2019B030302007). This research was also supported by the National Key R&D Program of China under Project 2019YFA0705104, Guangzhou Huangpu Technology Bureau (2022GH02) and partially supported by the GRF under Project City U11212920 and ITC of Hong Kong. J.Y. acknowledges the financial support from the Hong Kong Polytechnic University (Grant no. P0042930).

Research Keywords

cyclopropenium
high-voltage
organic cathode
zinc batteries

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title = "Molecular Engineering of N-heteroaromatic Organic Cathode for High-Voltage and Highly Stable Zinc Batteries",

abstract = "Zinc batteries hold promise for grid-scale energy storage due to their safety and low cost. A key challenge for the field is identifying cathode materials that can undergo reversible redox reactions at the extreme potentials required for realizing high energy density devices. While organic materials have been extensively explored as cathode materials due to their structural tunability and eco-friendliness, most reported zinc-organic batteries exhibit a voltage lower than 1.2 V. In this report, by employing rational molecular design and synthesis, computational analysis, and electrochemical evaluation, the well-studied neutral p-type N-centered is redesigned, triphenylamine organic cathode by replacing three phenyl rings with the smallest aromatic system – cationic cyclopropenium. This results in a novel class of cathode materials with simultaneously enhanced potential, capacity, and stability. The resultant full battery exhibits a high discharge voltage of 1.7 V and an outstanding capacity retention of 95% after 10000 cycles at a discharge capacity of 157.5 mAh g−1cation (103.9 mAh g−1salt).",

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Molecular Engineering of N-heteroaromatic Organic Cathode for High-Voltage and Highly Stable Zinc Batteries. / Yan, Yichao (Co-first Author); Li, Pei (Co-first Author); Wang, Yiqiao et al.
In: Advanced Functional Materials, Vol. 35, No. 2, 2312332, 22.05.2025.

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

TY - JOUR

T1 - Molecular Engineering of N-heteroaromatic Organic Cathode for High-Voltage and Highly Stable Zinc Batteries

AU - Yan, Yichao

AU - Li, Pei

AU - Wang, Yiqiao

AU - Bi, Leyu

AU - Lau, Ting Wai

AU - Miao, Mulin

AU - Yang, Shuo

AU - Xiong, Qi

AU - Lin, Francis R

AU - Yip, Hin-Lap

AU - Yin, Jun

AU - Zhi, Chunyi

AU - Jen, Alex K.-Y.

PY - 2025/5/22

Y1 - 2025/5/22

N2 - Zinc batteries hold promise for grid-scale energy storage due to their safety and low cost. A key challenge for the field is identifying cathode materials that can undergo reversible redox reactions at the extreme potentials required for realizing high energy density devices. While organic materials have been extensively explored as cathode materials due to their structural tunability and eco-friendliness, most reported zinc-organic batteries exhibit a voltage lower than 1.2 V. In this report, by employing rational molecular design and synthesis, computational analysis, and electrochemical evaluation, the well-studied neutral p-type N-centered is redesigned, triphenylamine organic cathode by replacing three phenyl rings with the smallest aromatic system – cationic cyclopropenium. This results in a novel class of cathode materials with simultaneously enhanced potential, capacity, and stability. The resultant full battery exhibits a high discharge voltage of 1.7 V and an outstanding capacity retention of 95% after 10000 cycles at a discharge capacity of 157.5 mAh g−1cation (103.9 mAh g−1salt).

AB - Zinc batteries hold promise for grid-scale energy storage due to their safety and low cost. A key challenge for the field is identifying cathode materials that can undergo reversible redox reactions at the extreme potentials required for realizing high energy density devices. While organic materials have been extensively explored as cathode materials due to their structural tunability and eco-friendliness, most reported zinc-organic batteries exhibit a voltage lower than 1.2 V. In this report, by employing rational molecular design and synthesis, computational analysis, and electrochemical evaluation, the well-studied neutral p-type N-centered is redesigned, triphenylamine organic cathode by replacing three phenyl rings with the smallest aromatic system – cationic cyclopropenium. This results in a novel class of cathode materials with simultaneously enhanced potential, capacity, and stability. The resultant full battery exhibits a high discharge voltage of 1.7 V and an outstanding capacity retention of 95% after 10000 cycles at a discharge capacity of 157.5 mAh g−1cation (103.9 mAh g−1salt).

KW - cyclopropenium

KW - high-voltage

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Molecular Engineering of N-heteroaromatic Organic Cathode for High-Voltage and Highly Stable Zinc Batteries

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GTF_EPD: Development of Printable Perovskite Solar Cells for Transformative Clean Energy and Sustainable Society

ITF: Development of Efficient and Stable Perovskite Solar Cell with Safe-to-Use

ITF: Using High-Throughput Optical Model to Design High Performance Thin Film Structures for Next-Generation Glass Materials and Products

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Molecular Engineering of N-heteroaromatic Organic Cathode for High-Voltage and Highly Stable Zinc Batteries

Abstract

Funding

Research Keywords

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Projects

GTF_EPD: Development of Printable Perovskite Solar Cells for Transformative Clean Energy and Sustainable Society

ITF: Development of Efficient and Stable Perovskite Solar Cell with Safe-to-Use

ITF: Using High-Throughput Optical Model to Design High Performance Thin Film Structures for Next-Generation Glass Materials and Products

Cite this