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The precise organization of nano-objects into well-defined patterns at interfaces is an outstanding challenge in the field of nanocomposites toward technologically important materials and devices. Herein, by means of computer simulations we show novel mechanomutable nanocomposites designed by binary mixtures of tethered Janus nanoparticles at the interface of a binary fluid mixture under mechanical pressure. Our simulations demonstrate that the nanoparticle organization in the systems undergo reversible transition between random state and long-ranged intercalation state, controlled by various structural parameters of the tethered chains and the applied pressure. The dynamical mechanism during the transition is explored through examining the diffusion trajectories of the nanoparticles confined at the interfaces. We provide a theoretical analysis of the lateral pressure induced by the tethered chains, which is fully supported by simulation data and reveals that the compression-induced transition is fundamentally attributed to the entropic effect from the tethered chains. Our study leads to a class of interface-reactive nanomaterials in which the transfer and recovery of interfacial nanopatterning presents precise and tunable mechanical responses.

It is of significance to design catalysts for achieving high‐performance electrochemical nitrate reduction to ammonia (NRA) in mild neutral media. However, the faradaic efficiency and selectivity are still far from satisfactory. Here, the fabrication of an efficient catalyst was achieved by rationally doping Fe to Cu into a metasequoia‐like nanocrystal of CuFe for NRA in neutral media. Fe doping was found to deepen energy level of the Cu 3d band, favorably tuning adsorption energies of reaction intermediates to promote the NRA. At an applied potential of −0.7 V vs. the reversible hydrogen electrode, the CuFe with approximately 2 % Fe doping content delivered a catalytic current density of 55.6 mA cm−2, which was 2.1 times that of the Cu material. The CuFe also exhibited a faradaic efficiency up to 94.5 %, and a good selectivity of 86.8 %.

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