journal article·2022-04-27

Homogenizing Li2CO3 Nucleation and Growth through High-Density Single-Atomic Ru Loading toward Reversible Li-CO2 Reaction

Jian Cheng, Yuqing Bai, Yuebin Lian, Yong Ma, Zi Yin, Le Wei, Hao Sun, Yanhui Su, Yuting Gu, Peng Kuang, Jun Zhong, Yang Peng, Haibo Wang, Zhao Deng

ACS Applied Materials & Interfaces· Volume 14· Issue 16
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Abstract

The high activation barrier and sluggish kinetics of Li2CO3 decomposition impose a severe challenge on the development of a Li-CO2 battery with high Coulombic efficiency. To tackle this issue, herein we devise a novel synthetic tactic by combining electrostatic assembly with in situ polycondensation to obtain a single-atomic Ru catalyst of high density up to ∼5 wt %. When deployed to the CO2 cathode, the catalyst delivered an extraordinary capacity of 44.7 Ah g–1, an ultralow charge/discharge polarization of 0.97 V at 0.1 A g–1 (1.90 V at 2 A g–1), and a long-term cycling stability up to 367 cycles at 1 Ah g–1 (196 cycles at 2 Ah g–1), outshining most of the state-of-the-art CO2 cathode catalysts reported today. Further through extensive in situ and ex situ electroanalytical, spectroscopic, and microscopic characterizations, we attribute the superb battery performance mainly to the highly reversible Li2CO3 formation/decomposition, facilitated by the homogenized and downsized Li2CO3 nucleation and growth on account of the high density single-atomic Ru loading. This work not only offers a facile method to fabricate single-atom catalysts with high mass loading but also sheds light on promoting the reversible Li-CO2 reaction by mediating product morphology.
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Research context

OpenAlex topics: Advancements in Battery Materials · Advanced Battery Materials and Technologies · Advanced battery technologies research

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou 215006, P. R. China

Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Suzhou 215006, P. R. China

School of Photoelectric Engineering, Changzhou Institute of Technology, Changzhou 213032, People’s Republic of China

Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, People’s Republic of China

University of Chinese Academy of Sciences, Beijing 100049, People’s Republic of China

Institute of Functional Nano and Soft Materials Laboratory (FUNSOM), Soochow University, Suzhou 215123, China

Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou 215123, China

Funding

Six Talent Peaks Project in Jiangsu Province · National Natural Science Foundation of China · Priority Academic Program Development of Jiangsu Higher Education Institutions · Key Technology Initiative of Suzhou Municipal Science and Technology Bureau · Natural Science Research Project of Jiangsu Higher Education Institutions of China

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