The botryoid hybrid nano-carbon materials were incorporated into cementitious materials to develop a new type of self-sensing cementitious composites, and then the mechanical, electrically conductive, and piezoresistive behaviors of the developed self-sensing cementitious composites with botryoid hybrid nano-carbon materials were comprehensively investigated. Moreover, the modification mechanisms of botryoid hybrid nano-carbon materials to cementitious materials were also explored. The experimental results show that the compressive strength and the elasticity modulus of the self-sensing cementitious composites botryoid hybrid nano-carbon materials decrease with the increase in the botryoid hybrid nano-carbon material content, while the Poisson’s ratio does the opposite. The percolation threshold zone of the self-sensing cementitious composites botryoid hybrid nano-carbon materials is from 2.28 to 3.85 vol.%. The optimal content of botryoid hybrid nano-carbon materials is 3.38 vol.% for piezoresistivity of the self-sensing cementitious composites botryoid hybrid nano-carbon materials. The amplitude of fractional change in resistivity goes up to 70.4% and 28.9%, respectively, under the monotonic compressive loading to failure and under the repeated compressive loading within elastic regime. The piezoresistive stress/strain sensitivity reaches (3.04%/MPa)/354.28 within elastic regime. The effective modification of botryoid hybrid nano-carbon materials to electrically conductive and piezoresistive properties of cementitious materials at such low content is attributed to their botryoid structures, which are beneficial for the dispersion of botryoid hybrid nano-carbon materials and the formation of conductive network in cementitious materials. The use of botryoid hybrid nano-carbon materials provides a new bottom–up design and fabrication approach for nano-engineering multifunctional cementitious composites.

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The production of effective loading and direct deposition of Pt nanoparticles on graphene is difficult because this intriguing carbon material has highly hydrophobic surface properties. In this work, Pt/graphene sheet (GS) composites were successfully synthesized via a simple, effective, and environmentally benign one-pot supercritical carbon dioxide deposition route using dimethyl (1,5-cyclooctadiene) platinum(II) (PtMe 2 COD) as a soluble organometallic precursor. The preparation process obviates the need for solvents, which are often volatile and toxic. No post-treatment processes such as washing and drying are needed. Transmission electron microscopy shows that ultrafine metal nanoparticles with an average size as small as ∼2 nm are densely and evenly decorated on the hydrophobic surfaces of GS at Pt loadings up to 80 wt %. Electrochemical studies reveal that the prepared Pt/ GS composites possess notably higher catalytic activity and better stability toward methanol electrooxidation in comparison with Pt/multiwalled carbon nanotube and Pt/carbon black composites. The supercritical carbon dioxide deposition method could be easily extended to the fabrication of other graphene-based metal composites with desirable properties by selecting suitable organometallic precursors.