Tatsuhiko Ohto

Ternary NiMoCo hybrid nanowire arrays with modulated electronic states and intermediate adsorption energies as efficient water splitting catalysts.

Interfacial water structures have been studied intensively by probing the O-H stretch mode of water molecules using sum-frequency generation (SFG) spectroscopy. This surface-specific technique is finding increasingly widespread use, and accordingly, computational approaches to calculate SFG spectra using molecular dynamics (MD) trajectories of interfacial water molecules have been developed and employed to correlate specific spectral signatures with distinct interfacial water structures. Such si

Graphene-covering is a promising approach for achieving an acid-stable, non-noble-metal-catalysed hydrogen evolution reaction (HER). Optimization of the number of graphene-covering layers and the density of defects generated by chemical doping is crucial for achieving a balance between corrosion resistance and catalytic activity. Here, we investigate the influence of charge transfer and proton penetration through the graphene layers on the HER mechanisms of the non-noble metals Ni and Cu in an a

The development of noble-metal-free hydrogen evolution reaction (HER) materials for electrochemical water splitting is the key to achieving low-cost and efficient electrocatalysis that drives electrochemical hydrogen evolution. However, the electrocatalytic activities of most non-noble metals decrease in acidic electrolytes. Here, we have fabricated non-noble-metal electrodes using a bicontinuous and open porous NiMo alloy covered by nitrogen-doped (N-doped) graphene with nanometer-sized holes.

Electrochemical water splitting is an ecofriendly technology for generating oxygen and hydrogen from water. The electrode is a key component that controls the efficiency of water splitting. Although noble metals such as Pt, Ru and Ir can achieve high energy efficiencies, their application in water splitting is limited by their high cost. Thus, developing efficient noble-metal-free electrodes is necessary to achieve sustainable hydrogen societies. Here, we report a technique of graphene encapsula

We present a combined experimental sum-frequency generation (SFG) spectroscopy and ab initio molecular dynamics simulations study to clarify the structure and orientation of water at zwitterionic phosphatidylcholine (PC) lipid and amine N-oxide (AO) surfactant monolayers. Simulated O-H stretch SFG spectra of water show good agreement with the experimental data. The SFG response at the PC interface exhibits positive peaks, whereas both negative and positive bands are present for the similar zwitt

Acid-stable, non-noble catalysts are promising for hydrogen evolution reaction (HER); however, they get easily damaged when used in acidic electrolytes, thus reducing the HER lifetimes. Moreover, completely blocking catalysts from acidic electrolytes degrades HER performance. To achieve a balance between the HER lifetime and performance, we vary the number of N-doped graphene layers (1–2, 2–3, and 3–5 layers) encapsulating NiMo nanoparticles as efficient HER catalysts and obtain the optimal numb

We simulate sum-frequency generation (SFG) spectra of isotopically diluted water at the water-graphene and water-hexagonal boron-nitride (hBN) sheet interfaces, using ab initio molecular dynamics simulations. A sharp 'dangling' O-D peak around ∼2640 cm-1 appearing in both simulated SFG spectra evidences that both graphene and hBN are hydrophobic. The dangling O-D peak is 10 cm-1 red-shifted at the water-hBN interface relative to the peak at the water-graphene interface. This frequency difference

Density functional theory-based molecular dynamics simulations are increasingly being used for simulating aqueous interfaces. Nonetheless, the choice of the appropriate density functional, critically affecting the outcome of the simulation, has remained arbitrary. Here, we assess the performance of various exchange-correlation (XC) functionals, based on the metrics relevant to sum-frequency generation spectroscopy. The structure and dynamics of water at the water-air interface are governed by he

The osmolyte molecule trimethylamine-N-oxide (TMAO) stabilizes the structure of proteins. As functional proteins are generally found in aqueous solutions, an important aspect of this stabilization is the interaction of TMAO with water. Here, we review, using vibrational spectroscopy and molecular dynamics simulations, recent studies on the structure and dynamics of TMAO with its surrounding water molecules. This article ends with an outlook on the open questions on TMAO-protein and TMAO-urea int

By combining heterodyne-detected sum-frequency generation (SFG) spectroscopy, ab initio molecular dynamics (AIMD) simulation, and a post-vibrational self-consistent field (VSCF) approach, we reveal the orientation and surface activity of the amphiphile trimethylamine-N-oxide (TMAO) at the water/air interface. Both measured and simulated C–H stretch SFG spectra show a strong negative and a weak positive peak. We attribute these peaks to the symmetric stretch mode/Fermi resonance and antisymmetric

We studied the supramolecular structure between barbituric acid (pyrimidine-2,4,6(1<i>H</i>,3<i>H</i>,5<i>H</i>)-trione, BA) and an amphiphilic melamine derivative at the air/water interface by heterodyne-detected vibrational sum frequency generation (HD-VSFG) spectroscopy. HD-VSFG measurements <i>in situ</i> showed a positive broad band from 2300 to 2950 cm^-1. By comparing the experimental results with <i>ab initio</i> molecular dynamics (AIMD) simulations, we assigned the broad band

We report molecular dynamics (MD) simulations of the water/clean rutile TiO2 (110) interface using polarizable and non-surface polarity force field models. The effect of surface polarity on the water dynamics near the TiO2(110) surface is addressed, specifically by calculating the water hydrogen bond and reorientational dynamics. The hydrogen bond lifetime of interfacial water molecules is several times longer than that of bulk water due to the strong water-TiO2 interactions. A comparison of the

The reaction conditions for the deposition of N-heterocyclic carbene (NHC) on a gold substrate play a crucial role in determining the surface coverage of NHC adsorbates. This, in turn, has a significant impact on the power factor.

Accelerating the CO2-recycling process is crucial for preventing global warming. Electrochemical reduction allows the efficient conversion of CO2 into useful chemical compounds with catalysts. During the electrolytic synthesis of CO2, an increase in voltage accelerates the synthesis of the target product and enhances byproduct formation. Previously investigated electrocatalysts do not increase the formation rate with parameter tuning. Herein, we report the development of a polymer-covered Sn cat