Sun Yafei, Wang Jingyi, Shang Tongxin, Li Zejian, Li Kanghui, Wang Xianwei, Luo Huarui, Lv Wei, Jiang Lilong, Wan Ying
State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, 200237, Shanghai, China.
The Education Ministry Key Laboratory of Resource Chemistry, Joint International Research Laboratory of Resource Chemistry of Ministry of Education, Shanghai Key Laboratory of Rare Earth Functional Materials, Shanghai Normal University, 200234, Shanghai, China.
Angew Chem Int Ed Engl. 2023 Nov 13;62(46):e202306791. doi: 10.1002/anie.202306791. Epub 2023 Oct 13.
The electrocatalytic sulfur reduction reaction (SRR) would allow the production of renewable high-capacity rechargeable lithium-sulfur (Li-S) batteries using sustainable and nontoxic elemental sulfur as a cathode material, but its slow reaction rate causes a serious shuttle effect and dramatically reduces the capacity. We found that a catalyst composed of Pd nanoparticles supported by ordered mesoporous carbon (Pd/OMC) had a high reaction rate in the SRR, and a Li-S battery assembled with this catalyst had a low shuttle constant of 0.031 h and a high-rate performance with a specific capacity of 1527 mAh g at 0.1 C which is close to the theoretical value. The high activity of Pd/OMC with a d-orbital vacancy of 0.87 e was predicted from a volcano relationship between the d charge for the metal and the adsorption activation entropy and reaction rate for the SRR by examining Pd, Au, Pt, Rh, and Ru transition-metal nanocatalysts. The strategy of using a single electronic structure descriptor to design high-efficiency SRR catalysts has suggested a way to produce practical Li-S batteries.
电催化硫还原反应（SRR）将允许使用可持续且无毒的元素硫作为阴极材料来生产可再生的高容量可充电锂硫（Li-S）电池，但其缓慢的反应速率会导致严重的穿梭效应，并显著降低电池容量。我们发现，由有序介孔碳负载的钯纳米颗粒（Pd/OMC）组成的催化剂在SRR中具有较高的反应速率，用这种催化剂组装的锂硫电池具有0.031 h的低穿梭常数，并且在0.1 C下具有1527 mAh g的高倍率性能，接近理论值。通过研究Pd、Au、Pt、Rh和Ru过渡金属纳米催化剂，从金属的d电荷与吸附活化熵以及SRR反应速率之间的火山关系预测，具有0.87 e的d轨道空位的Pd/OMC具有高活性。使用单一电子结构描述符设计高效SRR催化剂的策略为生产实用的锂硫电池提供了一条途径。
