Breakdown of Native Oxide Enables Multifunctional, Free-Form Carbon Nanotube–Metal Hierarchical Architectures

Passive oxide layers on metal substrates impose remarkable interfacial resistance for electron and phonon transport. Here, a scalable surface activation process is presented for the breakdown of the passive oxide layer and the formation of nanowire/nanopyramid structured surfaces on metal substrates, which enables high-efficiency catalysis of high-crystallinity carbon nanotubes (CNTs) and the direct integration of the CNT–metal hierarchical architectures with flexible free-form configurations. The CNT–metal hierarchical architecture facilitates a dielectric free-energy-carrier transport pathway and blocks the reformation of passive oxide layer, and thus demonstrates a 5-fold decrease in interfacial electrical resistance with 66% increase in specific surface area compared with those without surface activation. Moreover, the CNT–metal hierarchical architectures demonstrate omnidirectional blackbody photoabsorption with the reflectance of 1 × 10 –5 over the range from ultraviolet to terahertz region, which is 1 order of magnitude lower than that of any previously reported broadband absorber material. The synergistically incorporated CNT–metal hierarchical architectures offer record-high broadband optical absorption with excellent electrical and structural properties as well as industrial-scale producibility.