迈向实用的锂-二氧化碳电池:机理、催化剂和前景

IF 14 Q1 CHEMISTRY, MULTIDISCIPLINARY
Xiaowei Mu, Ping He* and Haoshen Zhou, 
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引用次数: 0

摘要

在温室气体排放威胁迫在眉睫的今天,实现碳中和目标已成为全球的当务之急。金属二氧化碳电池具有二氧化碳利用和电能储存的双重功能,被认为是前景广阔的减排战略之一。在各种金属-CO2 电池中,锂-CO2 电池具有最高的热力学平衡电位(∼2.80 V)和最大的理论比能量(∼1880 Wh kg-1),使其成为研究工作的中心和潜在的变革性储能技术。然而,二氧化碳锂电池的开发仍处于早期阶段。人们对复杂的二氧化碳还原和演化机制尚未完全了解。被广泛接受的二氧化碳还原产物是 Li2CO3 和碳。根据阴极催化剂对中间产物的吸附能和中间产物在电解质中的溶解度,这些产物会通过表面介导或溶液介导的放电途径产生。在充电过程中,使用不同的催化剂可能会发生 Li2CO3 的自分解或 Li2CO3 和碳的可逆编解。除了催化剂的选择外,电解质成分的改变和操作条件的控制也会影响反应过程,从而产生多种还原产物,包括 Li2C2O4、Li2CO3 和 CO 以及 Li2O 和碳。然而,控制反应路线的确切决定因素尚无定论。此外,由于 CO2 反应物和还原产物的固有特性以及多相界面反应动力学的迟缓,锂-CO2 电池面临着较大的过电位和不良的寄生反应。要推动实用锂-CO2 电池的发展,就必须进一步提高电池性能,尤其是能量效率和循环寿命。在本报告中,我们将总结我们和社会各界在研究锂-CO2 电池方面所做的努力,将其作为实现碳中和的一个极具吸引力的途径。我们首先简要介绍了二氧化碳的物理化学特性,并深入讨论了跨多相界面的基本二氧化碳还原和进化反应。然后,重点介绍了涉及催化剂、电解质和操作条件的各种反应途径和基本影响因素。此外,我们还根据近期的研究成果,从催化剂设计、电解质改性、阳极保护和外场辅助四个方面介绍了锂-CO2 电池的增强策略。最后,我们提出了一些潜在的方向,以加深对锂-CO2 电池的理解,优化电池性能,并将其应用拓展到未来的碳中和技术中。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Toward Practical Li–CO2 Batteries: Mechanisms, Catalysts, and Perspectives

Toward Practical Li–CO2 Batteries: Mechanisms, Catalysts, and Perspectives

Toward Practical Li–CO2 Batteries: Mechanisms, Catalysts, and Perspectives

Achieving the target of carbon neutrality has become a pressing global imperative in the world where the imminent threat of greenhouse gas emissions looms large. Metal–CO2 batteries, which possess dual functions of CO2 utilization and electrical energy storage, are considered as one of the promising emission reduction strategies. Among varieties of metal–CO2 batteries, Li–CO2 batteries have the highest thermodynamic equilibrium potential (∼2.80 V) and the largest theoretical specific energy (∼1880 Wh kg–1), making them the center of research efforts and potentially transformational energy storage technologies. However, the development of Li–CO2 batteries is still in its early stages. The complicated CO2 reduction and evolution mechanisms have not been fully understood. Widely accepted CO2 reduction products are Li2CO3 and carbon. These products are produced following a surface-mediated or solution-mediated discharge pathway depending on the adsorption energy of cathode catalysts to intermediates and the solubility of intermediates in electrolytes. During charging, the self-decomposition of Li2CO3 or the reversible codecomposition of Li2CO3 and carbon could occur while applying different catalysts. In addition to the selection of catalysts, the modification of electrolyte components and the control of operation conditions can also affect the reaction processes, contributing to diverse reduction products including Li2C2O4, Li2CO3 and CO, as well as Li2O and carbon. Nonetheless, the exact determining factors of controlling reaction routes have been inconclusive. Besides, owing to the intrinsic properties of CO2 reactants and reduction products as well as the sluggish reaction kinetics at multiphase interfaces, Li–CO2 batteries are confronted with large overpotentials and undesirable parasitic reactions. Further improvement in battery performance, especially the energy efficiency and cyclic life, is necessary to propel the development of practical Li–CO2 batteries. In this Account, we summarize our and the community’s efforts on the investigation of Li–CO2 batteries as an attractive avenue toward carbon neutrality. We start with a brief introduction of the physicochemical properties of CO2 and an in-depth discussion about the fundamental CO2 reduction and evolution reactions across multiphase interfaces. Then, diverse reaction pathways and underlying affecting factors involving catalysts, electrolytes, and operation conditions are highlighted. Furthermore, enhancement strategies for Li–CO2 batteries from four aspects of catalyst design, electrolyte modification, anode protection, and external field assistance are presented based on our recent works. At the end of the Account, we provide some potential directions in deepening the understanding of Li–CO2 batteries, optimizing battery performance, and broadening their application toward future carbon-neutral technologies.

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