The development of nanotechnology has made it possible to evaluate properties and functions at the nano-level. In order to fulfill this as material chemistry, it is necessary to develop a concept that integrates nanotechnology with existing fields such as supramolecular chemistry. This role is assigned to nanoarchitectonics, which is considered as a post-nanotechnology concept. In this paper, several recent examples related to nanoarchitectonics especially at interfaces are reviewed and discussed. In addition to nontechnology-driven organic reaction at solid surfaces, various nano-films preparation though techniques such as Langmuir-Blodgett (LB) method and layer-by-layer (LbL) assembly were discussed as nanoarchitectonics approaches to create functional materials such as two-dimensional nanocarbons and electroactive ultrathin films at interfaces.

The studies about surface chemistry of formic acid on Cu-based model catalysts including our recent investigation are reviewed from the surface-science point of view. The Cu-based model catalysts including steps and Zn-deposition have been prepared using the well-defined single crystalline Cu surfaces. Formate species are formed by the decomposition from formic acid on the model catalysts surfaces. Various surface spectroscopies have been applied for the assignments of intermediate species, the quantitative estimation of their coverages and the kinetics of adsorbed species. The active sites and reaction mechanisms of the decomposition of formic acid and the hydrogenation of formate species are discussed.

Precious metals, including Rh, are used practically in three-way catalytic converters of automobiles. An important role of Rh is the reduction of NO_x to N₂. Gas-phase clusters are used to study reactions relevant to heterogeneous catalysts because it is possible to define and detect the number of atoms included in the cluster and to obtain atomic-level insights into the reactions. We have studied the adsorption forms of NO molecules on metal clusters by using infrared multiple photon dissociation (IRMPD) spectroscopy. We found that NO molecules adsorb on metal clusters molecularly or dissociatively depending on the element and the size of the clusters. For instance, NO adsorbs on Rh_n^＋ clusters mainly in the molecular form (＞95% on Rh₆^＋), while more NO adsorbs dissociatively on Ir_n^＋ clusters (～50% on Ir₆^＋). In this review, the methodology and results of the identification of NO adsorption forms on Rh and related clusters are presented.

Graphene oxide (GO) causes unique phenomena in the adsorption, structural transformation, and intramembrane domain distribution of lipid bilayer membranes. The amphiphilic surface property of GO because of nanoscale patches of pristine graphene and oxygen-functionalized regions affects the assembly of amphiphilic lipid molecules in the bimolecular membrane. Spherical vesicles of phosphatidylcholine (PC) transformed to a single bilayer, doubly stacking bilayer, or intact vesicles on GO depending on the surrounding condition. In a binary lipid bilayer comprising PC and a lipid tagged with polyethylene glycol (PEG), the domain of the PEG-tagged lipid preferentially localized on GO. The results about the interaction between GO and artificial lipid bilayer membranes provide fundamental information for understanding compatibility and/or toxicity of GO on cells and organelles.

Defective oxide electrocatalysts are gaining attention as a platinum substitute for the hydrogen fuel cell. Oxygen reduction reaction (ORR) catalyzed at the surface is predicted using an exhaustive first-principles approach. After investigating the equilibrium distribution of the oxygen vacancies and nitrogen impurities at a tetragonal ZrO₂(101), adsorption energy of the ORR intermediates was calculated. The free energy profile depends on the defect configuration. The profile obtained for stable configurations showed that the rate-determining step is the removal of OH and the heat of the reaction is comparable to that of the defect-free surface. It is thus suggested that the role of the defects in enhancing the current density observed experimentally is possibly due to enhanced carrier supply through a defect-induced gap state.

The GRRM program is a computational program for automated chemical reaction path search. The Artificial Force Induced Reaction (AFIR) method implemented in the GRRM program enables automatic reaction path searches for gas and liquid phase reactions. Recently, the AFIR method has been extended to solid phase systems such as crystals and surfaces. This article reviews applications of the AFIR method to crystal structure prediction and surface reactions.