Aerogels are highly porous bulk materials assembled chemically or physically with various nanoscale building blocks and thus hold promise for numerous applications including energy storage and conversion. Assembling of hollow or porous particles with the diameter larger than 100 nm into hierarchically porous aerogels is efficient but challenging for achieving a high specific surface of aerogel. In this regard, submicron-sized carbon spheres with hollow cores and microporous shells are assembled into bulk aerogels, for the first time, in the presence of twodimensional graphene sheets as special cross-linkers. The resulting bead-to-sheet polylithic aerogels show ultra-low density (51-67 mg·cm -3 ), high conductivity (263-695 S·m -1 ) and high specific surface area (569-609 m 2 ·g -1 ). An application of thermocells is demonstrated with maximum output power of 1.05 W·m -2 and maximum energy conversion efficiency of 1.4 % relative to Carnot engine, outperforming the current simple U-shaped thermocells reported elsewhere.3
1.IntroductionGradual exhaustion of fossil fuels and rapid increase of energy demand may cause a serious energy crisis in the very near future [1]. Either exploiting the new energy options or developing energy recycling is a highly efficient way to overcome increasingly grim energy crisis [2][3][4][5][6].However, both technologies face the challenge of finding and integrating new materials to meet the demanding performance [7,8]. This constantly motivates scientists to develop novel energy materials [9][10][11][12].An aerogel is a kind of highly porous nanomaterial [13] with many intriguing properties such as the high specific surface area (more than several hundred m 2 ·g -1 ), ultra-low density (as low as 3 mg·cm -3 ), large pore volume (several cm 3 ·g -1 ), low dielectric constant (approaching that of air), superior thermal-insulating behavior (< 0.015 W·m -1 ·K -1 ), outstanding sound-proofing property (> 100 kg·m -2 ·s -1 ), etc. [14,15]. In recent years, intensive studies and exploitations have been carried out across many fields including environmental remediation, thermal insulation, energy storage and conversion, detection, adsorption, catalysis, and so on [16][17][18]. From the perspective of chemistry, aerogels are the sol-gel derivatives made via supercritical fluid drying (or other special drying) of various gel precursors, while from the perspective of structure, aerogels are the of the building blocks play important roles in determining structure and function of the resulting aerogel monoliths [24]. In the case of aerogels assembled with spherical particles, the specific surface area is inversely proportional to both the diameter and density of the individual solid particles under the assumption of no surface overlapping of the particles as shown in Figure 1a. It is desirable to obtain large specific areas of the aerogel with small diameter and/or low density particles [25]. However, only a small range of diameters of the building blocks, from a few to several tens of nanom...