Key Laboratory of Colloid and Interface Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shandong University, Jinan, 250100, China.
Collaborate Innovat Ctr Chem Energy Storage & Nove, Shandong Prov Key Lab, Liaocheng University, Liaocheng, 252000, China.
Adv Mater. 2022 Dec;34(50):e2204403. doi: 10.1002/adma.202204403. Epub 2022 Nov 7.
Developing a conductive catalyst with high catalytic activity is considered to be an effective strategy for improving cathode kinetics of lithium-sulfur batteries, especially at large current density and with lean electrolytes. Lattice-strain engineering has been a strategy to tune the local structure of catalysts and to help understand the structure-activity relationship between strain and catalyst performance. Here, Co Zn Te @NC is constructed after zinc atoms are uniformly doped into the CoTe lattice. The experimental/theoretical results indicate that a change of the coordination environment for the cobalt atom by the lattice strain modulates the d-band center with more electrons occupied in antibonding orbitals, thus balancing the adsorption of polysulfides and the intrinsic catalytic effect, thereby activating the intrinsic activity of the catalyst. Benefiting from the merits, with only 4 wt% dosages of catalyst in the cathode, an initial discharge capacity of 1030 mAh g can be achieved at 1 C and stable cycling performances are achieved for 1500/2500 cycles at 1 C/2 C. Upon sulfur loading of 7.7 mg cm , the areal capacity can reach 12.8 mAh cm . This work provides a guiding methodology for the design of catalytic materials and refinement of adsorption-catalysis strategies for the rational design of cathode in lithium-sulfur batteries.
开发具有高催化活性的导电催化剂被认为是提高锂硫电池阴极动力学性能的有效策略,特别是在大电流密度和贫电解液的情况下。晶格应变工程是一种调节催化剂局部结构的策略,可以帮助理解应变与催化剂性能之间的结构-活性关系。在这里,锌原子均匀掺杂到 CoTe 晶格中后,合成了 CoZnTe@NC。实验/理论结果表明,晶格应变引起钴原子配位环境的变化,从而调节 d 带中心,使更多的电子占据反键轨道,从而平衡多硫化物的吸附和内在的催化作用,从而激活催化剂的内在活性。得益于这些优点,在阴极中仅添加 4wt%的催化剂,在 1C 时可以实现 1030mAh g 的初始放电容量,在 1C/2C 下循环 1500/2500 次后仍能保持稳定的循环性能。在硫负载量为 7.7mg cm 的情况下,面积容量可达 12.8 mAh cm。这项工作为催化材料的设计和吸附-催化策略的优化提供了一种指导方法,有助于合理设计锂硫电池的阴极。