Rational Catalyst Structural Design to Facilitate Reversible Li-CO2 Batteries with Boosted CO2 Conversion Kinetics
Rational Catalyst Structural Design to Facilitate Reversible Li-CO2 Batteries with Boosted CO2 Conversion Kinetics
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DOI：
10.1016/j.nanoen.2023.108872
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发表时间：
2023-09
期刊：
影响因子：
17.6
通讯作者：
Shiming Chen;Kai Yang;Hengyao Zhu;Jianan Wang;Yi Gong;Huanxin Li;Manman Wang;Wenguang Zhao-Wenguang-Z
中科院分区：
文献类型：
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作者：
Shiming Chen;Kai Yang;Hengyao Zhu;Jianan Wang;Yi Gong;Huanxin Li;Manman Wang;Wenguang Zhao-Wenguang-Z
锂-二氧化碳电池（lcb）作为一种具有二氧化碳减排和储能能力的能源系统，在碳中和和社会可持续发展方面引起了广泛的关注。然而，它们的实际应用受到催化反应动力学缓慢和li2co3产物可逆性差的限制，这导致了过电位大、能量效率低和可逆性差的问题。本文提出了一种有效的催化剂设计和合成策略来克服上述瓶颈。通过电焦耳加热过程，具有随机晶体取向的Pt在几秒钟内转化为具有优选（111）晶体取向的3D多孔Pt催化剂，表现出增强的co2转化动力学和优异的电化学性能。这包括超低过电位（0.45 V），快速充电（高达160 μ A cm - 2）和高稳定性（在40 μ A cm - 2下超过200次循环）。在实际电流密度下，展示了一种具有稳定运行性能的堆叠式锂二氧化碳袋电池的概念验证，表明了大规模操作的巨大潜力。这种自下而上的高效催化剂和合成策略设计提供了一种快速且经济高效的方法，可以在限制催化剂负载的情况下最大化二氧化碳转化的催化位点，展示了其在广泛的基于催化剂的能量转换和存储系统中的多功能性。
Lithium-CO2batteries (LCBs) are regarded as a promising energy system for CO2drawdown and energy storage capability which has attracted widespread interest in carbon neutrality and sustainable societal development. However, their practical application has been limited by slow kinetics in catalytic reactions and poor reversibility of Li2CO3products which leads to the issue of a large overpotential, low energy efficiency and poor reversibility. Herein, an efficient catalyst design and synthesis strategy is proposed to overcome the abovementioned bottleneck. Through an electrical joule heating procedure, Pt with random crystal orientations is converted into a 3D porous Pt catalyst with preferred (111) crystal orientation within seconds, exhibiting enhanced CO2conversion kinetics with superior electrochemical performance. This includes ultralow overpotential (0.45 V), fast rate charging (up to 160 µA cm−2) and high stability (over 200 cycles under 40 µA cm−2). A proof-of-concept stacked Li-CO2pouch cell, with stable operation under practical current density is demonstrated, indicating significant potential for large-scale operations. This bottom-up design of efficient catalysts and synthesis strategy offers a rapid and cost-effective approach to maximizing catalytic sites for CO2conversion under restricted catalyst loading, showcasing its versatility across a broad spectrum of catalyst-based energy conversion and storage systems.