ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Ningning Feng,Bingliang Wang,Zhuo Yu,Yuming Gu,Lili Xu,Jing Ma,Yonggang Wang,Yongyao Xia
Li–CO2 batteries have attracted worldwide attention because of their dual characteristics of high energy density and effective CO2 capture. However, the basic electrochemistry mechanism involved has been unclear, which is mainly confused by the complicated decomposition of organic electrolytes. Herein, water-in-salt (WIS, LiTFSI/H2O 21.0 mol/1 kg) has been explored as a suitable electrolyte for the first time to investigate the reaction mechanism of Li–CO2 batteries with different cathodes (carbon nanotube (CNT) and Mo2C/CNT, respectively). An Mo2C-based Li–CO2 battery with WIS delivers a higher energy efficiency of 83% and a superior cyclability, compared to those of the CNT-based counterpart cell. Through various ex/in situ qualitative/quantitative characterizations, the Mo2C-based Li–CO2 battery with WIS can operate on the reversible conversion of CO2-to-Li2C2O4 ((e–/CO2)ideal = 1) at lower discharge/charge overpotentials, while the CNT-based counterpart cell is based on the formation/decomposition of Li2CO3 ((e–/CO2)ideal ≈ 1.33) at high overpotentials. Such a difference in CO2 reduction products stems from the stronger interaction between Mo2C(101) and Li2C2O4 than that of the CNT and Li2C2O4 based on the density functional theory calculations, resulting in the selective stabilization of the intermediate product Li2C2O4 on the Mo2C surface.
研究领域:
材料科学
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电化学
·
能源存储
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DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2022
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IF 10.383
Li-Na Song,Li-Jun Zheng,Xiao-Xue Wang,Yi-Feng Wang,Yue Wang,Shuang Liang,Ji-Jing Xu
The design of highly efficient electrocatalysts is a promising strategy to improve the electrochemical kinetics of Li–CO2 batteries. However, electrocatalysts usually aim to reduce the energetic barrier for the corresponding electrochemical reactions; little attention has been given to modulating the kinetics that directly determine the local concentration of reaction molecules surrounding catalysts. Herein, we present a systematic study on the role of Li+ reunion on the improvement of reaction kinetics in Li–CO2 batteries with a Cu cone cathode. Specifically, this local, geometry-driven tip effect can enrich the local electron concentration to facilitate Li+ ions diffusion from the bulk electrolyte to the surface of catalyst, leading to boosted catalytic performance. Further studies demonstrate that Cu(II/I) as a solid redox mediator dominates the reversible bulk redox reactions in a Cu cone cathode, which acts as an electron–hole transfer agent and permits the efficient reduction and oxidation of solid Li2CO3, contributing to an accessible theoretical discharge voltage, low charge potential below 3.2 V, impressive rate capability, and a long cycling stability (333 days) for Li–CO2 batteries. The exploitation of the sharp-tip enhancement effect and dynamic creation of catalytic active sites is expected to become routine practice in future mechanistic studies for metal-air batteries.
研究领域:
电化学
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材料科学
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2024
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IF 7.1
Xiaoqi Zhu,Lin Chen,Qisheng Fang,Jianli Cheng,Yuefeng Su,Paula Ratajczak,Francois Beguin,Bin Wang
Li-CO2 batteries with attractive characteristics of high energy density power supply and carbon dioxide fixation have attracted widespread attention. However, the lack of suitable cathode catalysts and their unsatisfactory electrochemical performance have impeded their development as promising Li-CO2 batteries for energy storage. Constructing heterojunctions by interfacial engineering to improve performance is considered one of the effective strategies. Herein, heterostructured CuCo2S4-Co9S8 nanosheets are fabricated by a facile hydrothermal method and employed as efficient cathode catalysts for Li-CO2 batteries. The construction of heterojunctions by interfacial engineering has proved as an effective strategy to enhance the electrochemical performance of the Li-CO2 batteries. The delocalized electrons between CuCo2S4 and Co9S8 contribute to a low median charge potential (∼3.6 V), small polarization (0.62 V), high energy efficiency of up to 83%, and outstanding cycle life (480 h) of the CuCo2S4-Co9S8 cathodes. Meanwhile, as a proof of concept, flexible fiber-shaped Li-CO2 batteries based on these cathodes are fabricated and demonstrate boosted flexibility adaptability and provide a stable power supply at various bending conditions.
研究领域:
材料科学
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电化学
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能源存储
·
纳米技术
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DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
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IF 14.7
Li Wei,Zhang Menghang,Sun Xinyi,Sheng Chuanchao,Mu Xiaowei,Wang Lei,He Ping,Zhou Haoshen
Li-CO 2 batteries offer a promising avenue for converting greenhouse gases into electricity. However, the inherent challenge of direct electrocatalytic reduction of inert CO 2 often results in the formation of Li 2 CO 3 , causing a dip in output voltage and energy efficiency. Our innovative approach involves solid redox mediators, affixed to the cathode via a Cu(II) coordination compound of benzene-1,3,5-tricarboxylic acid. This technique effectively circumvents the shuttle effect and sluggish kinetics associated with soluble redox mediators. Results show that the electrochemically reduced Cu(I) solid redox mediator efficiently captures CO 2 , facilitating Li 2 C 2 O 4 formation through a dimerization reaction involving a dimeric oxalate intermediate. The Li-CO 2 battery employing the Cu(II) solid redox mediator boasts a higher discharge voltage of 2.8 V, a lower charge potential of 3.7 V, and superior cycling performance over 400 cycles. Simultaneously, the successful development of a Li-CO 2 pouch battery propels metal-CO 2 batteries closer to practical application.
研究领域:
电化学
·
材料科学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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