Prediction of a low-temperature N2 dissociation catalyst exploiting near-IR–to–visible light nanoplasmonics
نویسندگان
چکیده
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 production. We predict that this can be achieved through Mo doping of the Au surface based on embedded multireference correlated wave function calculations. The Au component serves as a light-harvesting antenna funneling energy onto the Mo active site, whereby excited-state channels (requiring 1.4 to 1.45 eV, near-infrared-to-visible plasmon resonances) may be accessed. This effectively lowers the energy barriers to 0.44 to 0.77 eV/N2 (43 to 74 kJ/mol N2) from 3.5 eV/N2 (335 kJ/mol N2) in the ground state. The overall process requires three successive surface excitation events, which could be facilitated by amplified resonance energy transfer due to plasmon local field enhancement.
منابع مشابه
Preparation of Pt/Al2O3-Cl Catalyst and Investigation of Operating Variables Effects on Isomerization Reaction
A high chlorinated alumina catalyst obtained by treating Pt/γ-Al2O3 (0.25 wt. % Pt) samples with two mixtures of CCl4/N2 and CCl4/N2/H2 was tested for the hydroisomerization of C6 alkane. The conversion of n-hexane feed was diluted with hydrogen performed with different H2/HC ratios at various temperatures, liquid hourly space velocities (LHSVs) and 3MPa total pressure. The catalyst introduced ...
متن کاملLow Temperature Catalytic Cracking of Heavy Feedstock Optimized by Response Surface Method
Upgrading of cracked PFO (Pyrolysis fuel oil) for production of fuels, such as gasoline and light gasoil, was carried out in a semi batch reactor. Two different kinds of mesoporous and microporous catalysts, MCM-41 and ZSM-5, were used. Modification methods, such as ion exchange and impregnation with Fe and Ti, were done for tuning the acidity of the catalyst. XRD, FT-IR, and XRF analyzes were ...
متن کاملPhotocatalytic degradation of methyl orange using TiO2:Mg2+/zeolite composite under visible light irradiation
Photodegradation of methyl orange was investigated using synthesized TiO2:Mg2+/zeolite as the photocatalyst. The photocatalyst was characterized by X-ray, XRF, FT-IR, and SEM. The photocatalytic activities of TiO2:Mg2+/zeolite samples were evaluated in the degradation of methyl orange under visible light irradiation. The appropriate content of Mg in the composite was obtained as 4.711 wt% with ...
متن کاملTwo-directional N2 desorption in thermal dissociation of N2O on Rh„110..., Ir„110..., and Pd„110... at low temperatures
متن کامل
N1,N1,N2,N2-tetramethyl-N1,N2-bis(sulfo)ethane-1,2-diaminium Chloride ([TMBSED][Cl]2): An Efficient Ionic Liquid Catalyst for the One-pot Synthesis of Dihydropyrrol-2-ones and Tetrahydropyridines
N1,N1,N2,N2-tetramethyl-N1,N2-bis(sulfo)ethane-1,2-diaminium chloride ([TMBSED][Cl]2) was synthesized as an acidic ionic liquid and characterized using FT-IR, 1H and 13C NMR, mass spectroscopy, TG, DTG and DTA techniques. This ionic liquid was employed as efficient catalyst for the extremely facile and efficient synthesis of dihydropyrrol-2-ones and functionalized tetrahydropyridines. One-pot f...
متن کامل