The gas-phase self-assembly of Sn-SnO 2 @hollow carbon nanospheres (HCNSs) synthesized by floating catalytic chemical vapor deposition, as a new, facile, and scalable method, was performed, and the resultant nanospheres displayed an enhanced lithium storage performance. Freshly synthesized Sn nanoparticles [ % 25 nm in equivalent mobility diameter (EMD)] were incorporated quantitatively with dimethyl sulfide (DMS)-ethanol (EtOH) droplets ( % 45 nm in EMD) in the form of Sn/ DMS-EtOH hybrid droplets ( % 42 nm in EMD). The hybrid droplets were employed to perform catalytic chemical vapor synthesis in a heated tubular reactor. It was observed that SnSnO 2 particles with sizes between 3-6 nm were dispersed in the HCNSs ( % 25 nm in lateral dimension), and no bulky aggregates were visible. Its reversible capacity even increased up to % 870 mA h g À1 after 50 cycles, which is much higher than the conventional theoretical capacity of SnO 2 (782 mA h g
À1).Nanostructured materials have received much attention because of their new electronic, optical, and catalytic properties. [1,2] One category of such materials, Sn-C hybrid nanostructures, are ideal active materials for high energy and power density Li ion batteries (LIBs).[3] Sn-based materials deserve special attention as they offer a promising alternative to graphite because of their high theoretical capacity (Sn: 990 mA h g À1 , SnO 2 : 790 mA h g À1 , compared with 372 mA h g À1 for graphite).[4] However, it is a significant challenge to control the Sn particle size and the uniformity of Sn particle dispersion in the carbon matrix using current synthesis technology because of the low melting point of Sn and the tendency of particle growth, especially during high-temperature carbonization. [5] Despite the urgent need of these kinds of hybrid nanostructures, there are few well-established facile and scalable methods to synthesize these advanced nanostructures. Usually, the multistep coating, currently used for this kind of nanostructured electrode, is time consuming and tedious, which hinders the scale-up of the process significantly. [6,7] The present work introduces a continuous gas-phase self-assembly of Sn-SnO 2 @hollow carbon nanospheres (HCNSs) through a new floating catalytic chemical vapor deposition (CCVD) [8] method for the enhancement of Li storage. HCNSs usually have a porous shell and a protected inner cavity, which endow them with wide potential applications in LIBs, fuel cells, energy storage, catalysis, and drug delivery.[9] The successful key to this method is rooted in the deagglomerated Sn particles within precursor droplets, which allow the dispersion of ultrafine Sn particles in the carbon matrix. A catalytic formation of the carbon network is another factor that prevents Sn particles from growing bigger during the high-temperature process.A spark discharge [10] produced Sn nanoparticles, and the particle-laden flow passed over the Collison atomizer orifice in which they mix with the atomized dimethyl sulfide (DMS)-ethanol (EtOH) solution to form...