Engineered 3D micro-architected carbon structures via conformal deposition of multifunctional transition metal catalysts

Le résumé fourni par la source

Three-dimensional (3D) carbon structures have garnered increasing attention in energy storage and conversion technologies. While conventional porous carbon materials offer high surface areas, their ill-defined structures are replete with closed pores, reducing the effective surface area for electrochemical reactions. . A promising solution is converting 3D polymers into precisely engineered 3D carbon architectures with large accessible surface areas and low tortuosity, thereby facilitating rapid volumetric electrochemical reactions. However, direct pyrolysis of polymers suffers from low carbon yields and significant shrinkage. Herein, we report a method to enhance carbonization yield of 3D-printed polymers while improving dimensional retention using low-cost transition metal salts as catalysts. Facilitated by metal-ester (O–C O) coordination, transition metal salts were conformally deposited onto 3D polymer structures before pyrolysis. During pyrolysis, these metal salts serve two key functions: catalyzing the decomposition of polymer into carbon and graphitization. FeCl 3 demonstrates effective catalysis by increasing yield from 4.2 wt% for neat polymer to 21.4 wt%. In addition to a catalytic interface, the Fe-rich overcoat promotes the preservation of the 3D polymer geometry during pyrolysis. Dense polymer lattices with 50 μm strut diameters, which typically exhibit substantial shrinkage down to 10 μm, were converted into carbon with strut diameters of 43 μm. This high level of dimensional retention enables the creation of high-density carbon struts otherwise unattainable. The ability of this method to tune carbon yield, dimensional retention, graphitization, and porosity enables a pathway for high-throughput manufacturing and offers a toolbox for fabricating highly engineered 3D micro-architected carbon for diverse applications.

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