Constructing molecule-metal relay catalysis over heterophase metallene for high-performance rechargeable zinc-nitrate/ethanol batteries

Constructing molecule-metal relay catalysis over heterophase metallene for high-performance rechargeable zinc-nitrate/ethanol batteries

Proceedings of the National Academy of Sciences

10.1073/pnas.2311149120

https://doi.org/10.1073/pnas.2311149120

Jingwen Zhou, Yuecheng Xiong, Mingzi Sun, Zhihang Xu, Yunhao Wang, Pengyi Lu, Fu Liu, Fengkun Hao, Tianyi Feng, Yangbo Ma, Jinwen Yin, Chenliang Ye, Biao Chen, Shibo Xi, Ye Zhu, Bolong Huang, Zhanxi Fan

08 December 2023

Zhou, J., Xiong, Y., Sun, M., Xu, Z., Wang, Y., Lu, P., Liu, F., Hao, F., Feng, T., Ma, Y., Yin, J., Ye, C., Chen, B., Xi, S., Zhu, Y., Huang, B., & Fan, Z. (2023). Constructing molecule-metal relay catalysis over heterophase metallene for high-performance rechargeable zinc-nitrate/ethanol batteries. Proceedings of the National Academy of Sciences, 120(50). https://doi.org/10.1073/pnas.2311149120

Zinc-nitrate batteries can integrate energy supply, ammonia electrosynthesis, and sewage disposal into one electrochemical device. However, current zinc-nitrate batteries still severely suffer from the limited energy density and poor rechargeability. Here, we report the synthesis of tetraphenylporphyrin (tpp)-modified heterophase (amorphous/crystalline) rhodium-copper alloy metallenes (RhCu M-tpp). Using RhCu M-tpp as a bifunctional catalyst for nitrate reduction reaction (NO3RR) and ethanol oxidation reaction in neutral solution, a highly rechargeable and low-overpotential zinc-nitrate/ethanol battery is successfully constructed, which exhibits outstanding energy density of 117364.6 Wh kg−1 cat, superior rate capability, excellent cycling stability of ~400 cycles, and potential ammonium acetate production. Ex/in situ experimental studies and theoretical calculations reveal that there is a molecule-metal relay catalysis in NO3RR over RhCu M-tpp that significantly facilitates the ammonia selectivity and reaction kinetics via a low energy barrier pathway. This work provides an effective design strategy of multifunctional metal-based catalysts toward the high-performance zinc-based hybrid energy systems.

Attribution-NonCommercial-NoDerivatives 4.0 International (CC BY-NC-ND 4.0)

This research / project is supported by the Agency for Science, Technology and Research (A*STAR) - Low Carbon Energy Research Finding Initiative (LCERFI01-0033 | U2102d2006)
Grant Reference no. : U2102d2006

https://oar.a-star.edu.sg/communities-collections/articles/22698

0027-8424
1091-6490

Institute of Sustainability for Chemicals, Energy and Environment

https://doi.org/10.1073/pnas.2311149120