biostudies-literatureUnknown2(2)Dwivedi ISoft graphitizable carbon-based multifunctional nanomaterials have found versatile applications ranging from energy storage to quantum computing. In contrast, their hard-carbon analogues have been poorly investigated from both fundamental and application-oriented perspectives. The predominant challenges have been (a) the lack of approaches to fabricate porous hard-carbons and (b) their thermally nongraphitizable nature, leading to inaccessibility for several potential applications. In this direction, we present design principles for fabrication of porous hard-carbon-based nanostructured carbon florets (NCFs) with a highly accessible surface area (∼936 m²/g), rivalling their soft-carbon counterparts. Subjecting such thermally stable hard-carbons to a synergistic combination of an electric field and Joule heating drives their transformation to free-standing macroscopic monoliths composed of onion-like carbons (OLCMs). This represents the first such structural transformation observed in sp²-based hard-carbon NCFs to sp²-networked OLCMs. Micro-Raman spectroscopy establishes the simultaneous increase in the intensity of D-, 2D-, and D + G-bands at 1341, 2712, and 2936 cm^-1 and is correlated to the reorganization in the disordered graphitic domains of NCFs to curved concentric nested spheres in OLCMs. This therefore completely precludes the formation of a nanodiamond core that has been consistently observed in all previously reported OLCs. The Joule heating-driven formation of OLCMs is accompanied by ∼5700% enhancement in electrical conductivity that is brought about by the fusion of outermost graphitic shells of OLCs to result in monolithic OLC structures (OLCMs). The porous and inter-networked OLCMs exhibit an excellent adsorption-based capture of volatile organic compounds such as toluene at high efficiencies (∼99%) over a concentration range (0.22-1.86 ppm) that is relevant for direct applications such as smoke filters in cigarettes.ACS materials Au154-162https://www.ebi.ac.uk/biostudies/studies/S-EPMC9888654biostudies-literatureJoule Heating-Driven Transformation of Hard-Carbons to Onion-like Carbon Monoliths for Efficient Capture of Volatile Organic Compounds.PMC9888654Dwivedi ISubramaniam CfalseJoule Heating-Driven Transformation of Hard-Carbons to Onion-like Carbon Monoliths for Efficient Capture of Volatile Organic Compounds.Soft graphitizable carbon-based multifunctional nanomaterials have found versatile applications ranging from energy storage to quantum computing. In contrast, their hard-carbon analogues have been poorly investigated from both fundamental and application-oriented perspectives. The predominant challenges have been (a) the lack of approaches to fabricate porous hard-carbons and (b) their thermally nongraphitizable nature, leading to inaccessibility for several potential applications. In this direction, we present design principles for fabrication of porous hard-carbon-based nanostructured carbon florets (NCFs) with a highly accessible surface area (∼936 m²/g), rivalling their soft-carbon counterparts. Subjecting such thermally stable hard-carbons to a synergistic combination of an electric field and Joule heating drives their transformation to free-standing macroscopic monoliths composed of onion-like carbons (OLCMs). This represents the first such structural transformation observed in sp²-based hard-carbon NCFs to sp²-networked OLCMs. Micro-Raman spectroscopy establishes the simultaneous increase in the intensity of D-, 2D-, and D + G-bands at 1341, 2712, and 2936 cm^-1 and is correlated to the reorganization in the disordered graphitic domains of NCFs to curved concentric nested spheres in OLCMs. This therefore completely precludes the formation of a nanodiamond core that has been consistently observed in all previously reported OLCs. The Joule heating-driven formation of OLCMs is accompanied by ∼5700% enhancement in electrical conductivity that is brought about by the fusion of outermost graphitic shells of OLCs to result in monolithic OLC structures (OLCMs). The porous and inter-networked OLCMs exhibit an excellent adsorption-based capture of volatile organic compounds such as toluene at high efficiencies (∼99%) over a concentration range (0.22-1.86 ppm) that is relevant for direct applications such as smoke filters in cigarettes.2022-01-01T00:00:00Z2022 Mar2025-04-04T21:48:09.165Z2025-04-04T21:48:09.165ZS-EPMC98886543685576210.1021/acsmaterialsau.1c00062