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Solid–liquid interfaces are ubiquitous in scientifically and technologically important systems, and they govern complex chemophysical processes such as those in electrochemistry and heterogeneous catalysis. Atomic‐level elucidation of interfacial structures has been extensively pursued; however, related research is still limited. A major obstacle lies in the intrinsic character of interfaces: they are located between two bulk phases that make the application of spectroscopic or surface‐science techniques be difficult. Although this suggests the possibility of employing computational approaches to explore interfacial structures, modern molecular simulation methods suffer from an inability to simulate large interfacial systems in a sufficient time scale at the all‐atom resolution. To develop a method capable of simulating solid–liquid interfaces, we have been developing a mean‐field quantum mechanics/molecular mechanics (QM/MM) method. This Review briefly summarizes the theoretical background of mean‐field QM/MM, as well as recent efforts to advance it. Furthermore, we summarize several studies performed based on this method. [ABSTRACT FROM AUTHOR]

Conductive 2D nanosheets have evoked tremendous scientific efforts because of their high efficiency as hybridization matrices for improving diverse functionalities of nanostructured materials. To address the problems posed by previously reported conductive nanosheets like poorly-interacting graphene and cost-ineffective RuO 2 nanosheets, economically feasible noble-metal-free conductive [Mn x Co 1-2x Ni x ]O 2 oxide nanosheets are synthesized with outstanding interfacial interaction capability. The surface-optimized [Mn 1/4 Co 1/2 Ni 1/4 ]O 2 nanosheets outperformed RuO 2 /graphene nanosheets as hybridization matrices in exploring high-performance visible-light-active (λ >420 nm) photocatalysts. The most efficient g-C 3 N 4 -[Mn 1/4 Co 1/2 Ni 1/4 ]O 2 nanohybrid exhibited unusually high photocatalytic activity (NH 4 + formation rate: 1.2 mmol g -1 h -1 ), i.e., one of the highest N 2 reduction efficiencies. The outstanding hybridization effect of the defective [Mn 1/4 Co 1/2 Ni 1/4 ]O 2 nanosheets is attributed to the optimization of surface bonding character and electronic structure, allowing for improved interfacial coordination bonding with g-C 3 N 4 at the defect sites. Results from spectroscopic measurements and theoretical calculations reveal that hybridization helps optimize the bandgap energy, and improves charge separation, N 2 adsorptivity, and surface reactivity. The universality of the [Mn 1/4 Co 1/2 Ni 1/4 ]O 2 nanosheet as versatile hybridization matrices is corroborated by the improvement in the electrocatalytic activity of hybridized Co-Fe-LDH as well as the photocatalytic hydrogen production ability of hybridized CdS., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)