Electron-Transfer-Induced Dissociation of H2 on Gold Nanoparticles: Excited-State Potential Energy Surfaces via Embedded Correlated Wavefunction Theory
نویسندگان
چکیده
By Florian Libisch, Jin Cheng, and Emily A. Carter3,∗ 1 Department for Mechanical and Aerospace Engineering, Princeton University, Engineering Quadrangle, Olden Street, NJ, 08540 Princeton, USA 2 Department of Chemistry, Princeton University, Washington Road, NJ, 08544 Princeton, USA 3 Department for Mechanical and Aerospace Engineering, Program in Applied and Computational Mathematics, and Andlinger Center for Energy and the Environment, Princeton University, Engineering Quadrangle, Olden Street, NJ, 08540 Princeton, USA
منابع مشابه
Embedded correlated wavefunction schemes: theory and applications.
Conspectus Ab initio modeling of matter has become a pillar of chemical research: with ever-increasing computational power, simulations can be used to accurately predict, for example, chemical reaction rates, electronic and mechanical properties of materials, and dynamical properties of liquids. Many competing quantum mechanical methods have been developed over the years that vary in computatio...
متن کاملEmbedding potentials for excited states of embedded species.
Frozen-Density-Embedding Theory (FDET) is a formalism to obtain the upper bound of the ground-state energy of the total system and the corresponding embedded wavefunction by means of Euler-Lagrange equations [T. A. Wesolowski, Phys. Rev. A 77(1), 012504 (2008)]. FDET provides the expression for the embedding potential as a functional of the electron density of the embedded species, electron den...
متن کاملHot electrons do the impossible: plasmon-induced dissociation of H2 on Au.
Heterogeneous catalysis is of paramount importance in chemistry and energy applications. Catalysts that couple light energy into chemical reactions in a directed, orbital-specific manner would greatly reduce the energy input requirements of chemical transformations, revolutionizing catalysis-driven chemistry. Here we report the room temperature dissociation of H(2) on gold nanoparticles using v...
متن کاملPrediction of a low-temperature N2 dissociation catalyst exploiting near-IR–to–visible light nanoplasmonics
Despite more than a century of advances in catalyst and production plant design, the Haber-Bosch process for industrial ammonia (NH3) synthesis still requires energy-intensive high temperatures and pressures. We propose taking advantage of sunlight conversion into surface plasmon resonances in Au nanoparticles to enhance the rate of the N2 dissociation reaction, which is the bottleneck in NH3 p...
متن کاملA density functional theory study of the dissociation of H2 on gold clusters: importance of fluxionality and ensemble effects.
Density functional theory was employed to calculate the adsorption/dissociation of H2 on gold surfaces, Au(111) and Au(100), and on gold particles from 0.7 (Au14) to 1.2 nm (Au29). Flat surfaces of the bulk metal were not active towards H2, but a different effect was observed in gold nanoclusters, where the hydrogen was adsorbed through a dissociative pathway. Several parameters such as the coo...
متن کامل