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Internal macropores in silicon/graphene/graphene nanoribbon (Si/Gr/GNR) hybrid anodes by facile thermal removal of sacrificial polymer, polyvinyl alcohol (PVA), are incorporated, to mitigate the volume expansion of silicon and to increase the silicon utilization and rate capability of the anode. The resulting Si/Gr/GNR hybrid anodes give a high capacity of 1874 mAh g⁻¹at 0.1 C, based on total weight of the electrode including binder and carbon, as well as great capacity retention of above 800 mAh g⁻¹after 350 cycles at 0.3 C. The mitigation of volume expansion by carrying out in situ thickness change measurements of small pouch cells via a dilatometer is further demonstrated, exhibiting the saturation of volume expansion below 40% after 100 cycles due to the incorporation of the macropores. Moreover, Si/Gr/GNR anodes with pores exhibit superior rate capability, yielding 1,250 mAh g⁻¹at 2 C rate due to the effective network of graphene sheets and GNRs. 

Abstract Smart materials are versatile material systems which exhibit a measurable response to external stimuli. Recently, smart material systems have been developed which incorporate graphene in order to share on its various advantageous properties, such as mechanical strength, electrical conductivity, and thermal conductivity as well as to achieve unique stimuli‐dependent responses. Here, a graphene fiber‐based smart material that exhibits reversible electrical conductivity switching at a relatively low temperature (60 °C), is reported. Using molecular dynamics (MD) simulation and density functional theory‐based non‐equilibrium Green's function (DFT‐NEGF) approach, it is revealed that this thermo‐response behavior is due to the change in configuration of amphiphilic triblock dispersant molecules occurring in the graphene fiber during heating or cooling. These conformational changes alter the total number of graphene‐graphene contacts within the composite material system, and thus the electrical conductivity as well. Additionally, this graphene fiber fabrication approach uses a scalable, facile, water‐based method, that makes it easy to modify material composition ratios. In all, this work represents an important step forward to enable complete functional tuning of graphene‐based smart materials at the nanoscale while increasing commercialization viability.