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Carbon Nanotube‐Encapsulated Noble Metal Nanoparticle Hybrid as a Cathode Material for Li‐Oxygen Batteries
Authors:Xin Huang  Hong Yu  Huiteng Tan  Jixin Zhu  Wenyu Zhang  Chengyuan Wang  Jun Zhang  Yuxi Wang  Yunbo Lv  Zhi Zeng  Dayong Liu  Jun Ding  Qichun Zhang  Madhavi Srinivasan  Pulickel M Ajayan  Huey Hoon Hng  Qingyu Yan
Affiliation:1. Department of Biomass and Chemical Engineering, Sichuan University, Chengdu, PR China;2. National Engineering Laboratory for Clean Technology of Leather Manufacture, Sichuan University, Chengdu, PR China;3. School of Materials Science and Engineering, Nanyang Technological University, Singapore;4. Institute of Solid State Physics, Chinese Academy of Sciences, Hefei, Anhui, PR China;5. CREATE, Singapore;6. Department of Materials Science & Engineering, National University of Singapore, Singapore;7. Department of Mechanical Engineering & Materials Science, Rice University, Houston, Texas, USA;8. Energy Research Institute @ Nanyang Technological University, Nanyang Technological University, Singapore
Abstract:Although Li‐oxygen batteries offer extremely high theoretical specific energy, their practical application still faces critical challenges. One of the main obstacles is the high charge overpotential caused by sluggish kinetics of charge transfer that is closely related to the morphology of discharge products and their distribution on the cathode. Here, a series of noble metal nanoparticles (Pd, Pt, Ru and Au) are encapsulated inside end‐opened carbon nanotubes (CNTs) by wet impregnation followed by thermal annealing. The resultant cathode materials exhibit a dramatic reduction of charge overpotentials compared to their counterparts with nanoparticles supported on CNT surface. Notably, the charge overpotential can be as low as 0.3 V when CNT‐encapsulated Pd nanoparticles are used on the cathode. The cathode also shows good stability during discharge–charge cycling. Density functional theory (DFT) calculations reveal that encapsulation of “guest” noble metal nanoparticles in “host” CNTs is able to strengthen the electron density on CNT surfaces, and to avoid the regional enrichment of electron density caused by the direct exposure of nanoparticles on CNT surface. These unique properties ensure the uniform coverage of Li2O2 nanocrystals on CNT surfaces instead of localized distribution of Li2O2 aggregation, thus providing efficient charge transfer for the decomposition of Li2O2.
Keywords:carbon nanotubes  cathode materials  encapsulation  surface electron distribution  Li‐oxygen batteries  charge overpotential
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