The objective of this research is to develop a scalable manufacturing process for high-volume production of low-cost graphene materials from lignin. The process includes preparation of catalyst-lignin precursors, pretreatment of precursors, and catalytic graphitization of kraft lignin to graphene materials. A growth concept, “catalytic thermal molecular welding (CTMW)” technique is proposed and validated to produce graphene materials from solid carbon resources. CTMW technique is a single process with two stages, i.e., the carbon-encapsulated metal nanostructures are first prepared. Then in the second stage these core-shell structures are opened by “scissoring molecules”, the cracked carbon shell units are welded and reconstructed to multilayer graphene materials under high temperature with selected “welding reagent gases” like light hydrocarbons (methane, natural gas, etc.) and hydrogen. Multi-layer nano-shell structure-based graphene materials, such as fluffy graphene, graphene chains, multi-layer graphene nanoplatelets, flatten or curved sheet-like graphene can be produced through altering fabrication conditions. The effects of transitional metal catalysts (Ni, Cu, Fe, and Mo) on the yields and structures of multi-layer nano-shell structure-based graphene materials from lignin are compared. The effects of the iron chemical resources (Fe(NO3)3, FeCl2, FeCl3, and Fe2O3 (nano)), iron loading on the yields and structures of multi-layer graphene materials from lignin are also examined. The influences of temperature, heating rate, heating time, metal-lignin precursor particle size, and welding reagent gas types on the yield of multi-layer graphene materials from lignin resources are investigated. Welding temperatures are optimized as1,000°C or above, with heating rates of 10°C or above. Welding gases including, argon (Ar), hydrogen (H2), methane (CH4), natural gas (NG), and mixed of these gases, are used at flow rates from 20 to 300 mL/min. Heating time is controlled between 0 to 5 hours. The effect of precursor particle size on final products is examined between 44 to 426 microns (Delta-m).

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