Pichaimuthu Karthika, Jena Anirudha, Chang Ho, Su Chaochin, Hu Shu-Fen, Liu Ru-Shi
Department of Chemistry, National Taiwan University, Taipei 106, Taiwan.
Institute of Organic and Polymeric Materials, Research and Development Centre for Smart Textile, National Taipei University of Technology, Taipei 106, Taiwan.
ACS Appl Mater Interfaces. 2022 Feb 2;14(4):5834-5842. doi: 10.1021/acsami.1c22435. Epub 2022 Jan 21.
Metal-CO rechargeable batteries are of great importance due to their higher energy density and carbon capture capability. In particular, Na-CO batteries are potential energy-storage devices that can replace Li-based batteries due to their lower cost and abundance. However, because of the slow electrochemical processes owing to the carbonated discharge products, the cell shows a high overpotential. The charge overpotential of the Na-CO battery increases because of the cathode catalyst's inability to break down the insulating discharge product NaCO, thereby resulting in poor cycle performance. Herein, we develop an ultrathin nanosheet MoS/SnS cathode composite catalyst for Na-CO battery application. Insertion of SnS reduces the overpotential and improves the cyclic stability compared to pristine MoS. As shown by a cycle test with a restricted capacity of 500 mAh/g at 50 mA/g, the battery is stable up to 100 discharge-charge cycles as the prepared catalyst successfully decomposes NaCO. Furthermore, the battery with the MoS/SnS cathode catalyst has a discharge capacity of 35 889 mAh/g. The reasons for improvements in the cycle performance and overpotential of the MoS/SnS composite cathode catalyst are examined by a combination of Raman, X-ray photoelectron spectroscopy, and extended X-ray absorption fine structure analysis, which reveals an underneath phase transformation and changes in the local atomic environment to be responsible. SnS incorporation induces S-vacancies in the basal plane and 1T character in 2H MoS. This combined impact of SnS incorporation results in undercoordinated Mo atoms. Such a change in the electronic structure and the phase of the MoS/SnS composite cathode catalyst results in higher catalytic activity and reduces the cell overpotential.
金属-CO可充电电池因其较高的能量密度和碳捕获能力而具有重要意义。特别是,Na-CO电池是具有潜力的储能装置,由于其成本较低且储量丰富,有望取代锂基电池。然而,由于碳酸化放电产物导致的电化学过程缓慢,电池表现出较高的过电位。Na-CO电池的充电过电位增加,是因为阴极催化剂无法分解绝缘的放电产物NaCO,从而导致循环性能较差。在此,我们开发了一种用于Na-CO电池的超薄纳米片MoS/SnS阴极复合催化剂。与原始MoS相比,SnS的引入降低了过电位并提高了循环稳定性。在50 mA/g的受限容量为500 mAh/g的循环测试中表明,由于制备的催化剂成功分解了NaCO,电池在100次充放电循环内保持稳定。此外,具有MoS/SnS阴极催化剂的电池放电容量为35889 mAh/g。通过拉曼光谱、X射线光电子能谱和扩展X射线吸收精细结构分析相结合的方法,研究了MoS/SnS复合阴极催化剂循环性能和过电位改善的原因,结果表明其底层相变和局部原子环境变化是造成这种情况的原因。SnS的掺入在基面诱导了S空位,并在2H MoS中引入了1T特性。SnS掺入的这种综合影响导致Mo原子配位不足。MoS/SnS复合阴极催化剂的电子结构和相的这种变化导致更高的催化活性并降低了电池过电位。