Raman spectra of single-wall carbon nanotubes ͑SWCNTs͒ were measured at different temperatures by varying the incident laser power. The elevated temperature of the SWCNTs and multiwall carbon nanotubes ͑MWCNTs͒ is confirmed to be due to the presence of impurities, defects, and disorder. The temperature coefficient of the frequency of the CC stretching mode E 2g ͑GM͒ and that of the radial breathing mode in the SWCNT were determined to be ϳϪ0.038 and ϳϪ0.013 cm Ϫ1 /K, respectively. It is found that the temperature coefficient of the GM in the SWCNT is larger than that of the MWCNT, highly oriented pyrolytic graphite, and the graphite. This is attributed to the structural characteristic of the SWCNT-a single tubular carbon sheet with smaller diameter.

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Catalysts with designable intelligent nanostructure may potentially drive the changes in chemical reaction techniques. Herein, a multi‐function integrating nanocatalyst, Pt‐containing magnetic yolk‐shell carbonaceous structure, having catalysis function, microenvironment heating, thermal insulation, and elevated pressure into a whole is designed, which induces selective hydrogenation within heating‐constrained nanoreactors surrounded by ambient environment. As a demonstration, carbonyl of α, β‐unsaturated aldehydes/ketones are selectively hydrogenated to unsaturated alcohols with a >98% selectivity at a nearly complete conversion under mild conditions of 40 °C and 3 bar instead of harsh requirements of 120 °C and 30 bar. It is creatively demonstrated that the locally increased temperature and endogenous pressure (estimated as ≈120 °C, 9.7 bar) in the nano‐sized space greatly facilitate the reaction kinetics under an alternating magnetic field. The outward‐diffused products to the “cool environment” remain thermodynamically stable, avoiding the over‐hydrogenation that often occurs under constantly heated conditions of 120 °C. Regulation of the electronic state of Pt by sulfur doping of carbon allows selective chemical adsorption of the CO group and consequently leads to selective hydrogenation. It is expected that such a multi‐function integrated catalyst provides an ideal platform for precisely operating a variety of organic liquid‐phase transformations under mild reaction conditions.

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