Research progress on design strategies and reaction mechanisms of photo-assisted Li-CO2 battery catalysts

doi:10.11949/0438-1157.20240091

Abstract

Abstract:

Photo-assisted Li-CO₂ batteries have the characteristics of high theoretical energy density and environmental friendliness, which are important development direction for the next generation of high specific energy battery systems. However, the CO₂ reduction/evolution reaction at the positive electrode has problems such as slow kinetics, which limits the development of Li-CO₂ batteries. Photo-assisted technology utilizes the photocatalyst loaded on the positive electrode to absorb light energy, generate electrons and holes to drive chemical reactions, which is beneficial for improving battery performance. This review summarizes the photochemical principles and charge-discharge reaction mechanism of photo-assisted Li-CO₂ batteries, lists design strategies and specific examples of cathode photocatalysts. The impact of photocatalyst structure on battery performance is further understood through in-depth exploration of the photocatalytic reaction mechanism of Li-CO₂ batteries. In addition, the basic understanding of photo-assisted Li-CO₂ batteries, current challenges, and prospects for the development of photocatalysts were discussed, providing an important reference for technical research in the field of new energy materials and helps to promote the practical process of Li-CO₂ batteries.

Key words: Li-CO₂ batteries, cathode photocatalyst, reaction mechanism, design strategy

摘要：

光辅助Li-CO₂电池具有理论能量密度高、环境友好等特点，是下一代高比能电池系统的重要发展方向。然而，正极处CO₂还原/析出反应存在动力学缓慢等问题，限制了Li-CO₂电池发展。光辅助技术利用正极负载的光催化剂吸收光能，产生电子和空穴以驱动化学反应，有利于提升电池性能。本文阐述了光辅助Li-CO₂电池的光化学原理及充放电反应机制，详细列举了正极光催化剂的设计策略及具体实例。通过深入探讨Li-CO₂电池的光催化反应机理，进一步理解了光催化剂结构对电池性能的影响机制。此外，还讨论了光辅助Li-CO₂电池的基本认识、当前面临的挑战以及对光催化剂发展前景的展望，可为新能源材料领域的技术研究提供参考，有助于推动Li-CO₂电池的实用化进程。

关键词: Li-CO₂电池, 正极光催化剂, 反应机理, 设计策略

CLC Number:

O 646

Tingting ZHAO, Lixiang YAN, Fuli TANG, Minzhi XIAO, Ye TAN, Liubin SONG, Zhongliang XIAO, Lingjun LI. Research progress on design strategies and reaction mechanisms of photo-assisted Li-CO₂ battery catalysts[J]. CIESC Journal, 2024, 75(5): 1750-1764.

赵亭亭, 鄢立祥, 唐福利, 肖敏之, 谭烨, 宋刘斌, 肖忠良, 李灵均. 光辅助锂-二氧化碳电池催化剂的设计策略与反应机理研究进展[J]. 化工学报, 2024, 75(5): 1750-1764.

Figures/Tables 11

Fig.1 Timeline of design strategies and mechanism development of photocatalysts for Li-CO2 batteries[36,38-40]

Fig.2 Schematic diagram of the photocatalytic reaction process of photo-assisted Li-CO2 batteries[26]

Fig.3 Possible pathway for the formation of Li2CO3 discharge products in photo-assisted Li-CO2 batteries[40]

Fig.4 The working mechanism for the light-induced discharging process (a); Band diagram of the In2S3@CNT/SS (b); Photocurrent response to UV light of ICS, In2S3NS/SS, and CNT (c)[40]

Fig.5 Optimized structures and adsorption energy of intermediate LiCO2 molecules on the TNAs (a); Optimized structures and adsorption energy of intermediate LiCO2 molecules on the TNAs@AgNPs (b); Gibbs free energy of battery surface and solution-mediated reaction pathways (c)[39]

Fig.6 Schematic illustration of different growth mechanisms of Li2CO3 in the Li-CO2 batteries based on TiO2 NAs/CT and RuO2-TiO2 NAs/CT cathodes (a); The optimized structures and the corresponding binding energy of Li2CO3 on TiO2 and RuO2 surfaces (b); The differential charge density Δρ of CO2 or Li2CO3 adsorbed on TiO2 and RuO2 surfaces (c)[38]

Fig.7 Charge curves of Li-CO2 batteries with TiO2/CC cathode with and without illumination (a); LSV curves measured in the CO2ER region of TiO2/CC with and without illumination in 0.5 mol·L-1 CO2-saturated LiTFSI/DME solution at a scan rate of 5 mV·s-1 (b); Corresponding Tafel curves (c); Galvanostatic intermittent titration technique curves obtained from Li-CO2 battery with TiO2/CC cathode with and without illumination (d); Schematic of energy diagrams for the reduced charge voltage of Li-CO2 battery under illumination (e)[36]

Table 1 Structure and performance of photo-assisted Li-CO2 batteries

光催化剂	首次效率/%	电流密度/（mA·cm^-2）	放电比容量/（mAh·cm^-2）	充电/放电电压平台/V	循环次数（圈）	文献
TiO₂/CC	97.2	0.01	0.01	2.82/2.88	30	[36]
RuO₂/TiO₂	95.5	250 mA·g^-1	1000 mAh·g^-1	2.78/2.91	238	[38]
TiO₂@Ag	87.1	0.01	0.1	2.49/2.86	100	[39]
Cu₂O/CNT	85	100 mA·g^-1	100 mAh·g^-1	2.5/4.5	50	[42]
In₂S₃@CNT/SS	98.1	0.01	0.01	3.14/3.2	25	[40]
CNT@C₃N₄	98.8	0.02	0.02	3.24/3.28	100	[34]
SiC/RGO	84.4	20 mA·g^-1	0.01	2.77/3.28	20	[43]
CoPc-Mn-O	98.5	0.02	—	3.20/3.25	30	[35]
Au@TiO₂	92.4	0.01	0.01	2.95/3.49	200	[44]
混合相TiO₂	—	0.025	—	2.2/3.0	52	[45]

Fig.8 Schematic depiction of the solar-spectrum photothermal effect of plasmonic semiconductor nanomaterials via plasmon-and exciton-based approaches (a); On/off response of the surface temperature increase of Au@TiO2 and TiO2 (b); Distribution of the surface temperature increase on TiO2 (c) and Au@TiO2 (d) spheres under the illumination conditions; I-T curves of Au@TiO2 and TiO2 spheres (e); Distribution of the electric near field under the illumination conditions on TiO2 and Au@TiO2 spheres surface (f); LSV curves for the CDR process of TiO2 and Au@TiO2 spheres with and without illumination (g)[44]

Fig.9 Schematic diagram of the synergistic effect of SiC flakes and RGO (a); UV-Vis diffuse reflectance spectra of RGO, SiC/RGO and pure SiC (b); The Tauc plot (c); Mott-Schottky plots (d); Room-temperature PL spectra of SiC and SiC/RGO samples (e); LSV curves of SiC/RGO and SiC cathodes under illumination (f)[43]

Fig.10 Working mechanism of the dual-field assisted Li-CO2 battery (a); Discharge/charge voltage profiles at the first cycle (b); Cycling performance (c); Rate capability of Li-CO2 batteries with TNAs and TNAs@AgNPs cathodes in light or dark (d); Discharge/charge curves of the TNAs@AgNPs cathode in light at 1.0 mAh·cm-2 and 2.0 mA·cm-2 (e); Comparison of cycling stability (f) and rate capability (g) of the dual-field assisted Li-CO2 battery with some representative Li-CO2 batteries based on the electrocatalysis and photo electrocatalysis mechanisms[39]

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Research progress on design strategies and reaction mechanisms of photo-assisted Li-CO₂ battery catalysts

光辅助锂-二氧化碳电池催化剂的设计策略与反应机理研究进展

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