Generalized Synthesis of Highly Heteroatom Doped Ordered Mesoporous Carbons for Energy Storage

Heteroatom doped carbon materials represent one of the most common materials for energy applications, such as fuel cells, batteries, hydrogen storage or supercapacitors. For Li+ batteries, the lithium-ion storage capacity for heteroatom doped carbon largely depends on the heteroatom doping level. Similarly for Li/Na-S batteries, heteroatom doping can decrease polysulfide shuttling through the favorable interaction between polysulfides and the polarized carbon matrix. One challenge to inhibit shuttling is achieving high heteroatoms doping in the carbon, while maintaining porosity for transport. Here we demonstrate a generalized synthesis for highly doped ordered mesoporous carbons through infiltration of molten dopants in silica reinforced mesoporous crosslinked polymer (resol) and subsequent carbonization. This method is demonstrated to generate ordered mesoporous carbons with high heteroatom content (up to 26 at% N, 15 at% B, 7 at% P, or 4 at% S) for a wide variety of elements through melt infusion of the appropriate heteroatom precursor (melamine, boric anhydride, ammonium dihydrogenphosphate or dibenzyl sulphide).We demonstrate that the high doping content can nearly fully inhibit polysulfide shuttling in Na-S batteries.