Catalysis for CO2 conversion: a key technology for rapid introduction of renewable energy in the value chain of chemical industries

Centi, Gabriele; Quadrelli, Elsje Alessandra; Perathoner, Siglinda

doi:10.1039/c3ee00056g

Cited by 1,123 publications

(769 citation statements)

References 186 publications

(137 reference statements)

Supporting

Mentioning

754

Contrasting

Unclassified

Order By: Relevance

“…ΔG°∼ 665 n kJ=mol ðARCÞ [4] combustion and, as generally proposed, would be carried out as separate unit operations, each with its attendant efficiency losses and capital and operating costs (19,20). We report here a photothermochemical process for driving the alkane reverse combustion (ARC) reaction (reaction 4) to produce C 1 to C 13 hydrocarbons in a single operation unit.…”

mentioning

confidence: 99%

RETRACTED: Solar photothermochemical alkane reverse combustion

Chanmanee

Islam

Dennis

et al. 2016

Proc. Natl. Acad. Sci. U.S.A.

View full text Add to dashboard Cite

A one-step, gas-phase photothermocatalytic process for the synthesis of hydrocarbons, including liquid alkanes, aromatics, and oxygenates, with carbon numbers (Cn) up to C13, from CO2 and water is demonstrated in a flow photoreactor operating at elevated temperatures (180–200 °C) and pressures (1–6 bar) using a 5% cobalt on TiO2 catalyst and under UV irradiation. A parametric study of temperature, pressure, and partial pressure ratio revealed that temperatures in excess of 160 °C are needed to obtain the higher Cn products in quantity and that the product distribution shifts toward higher Cn products with increasing pressure. In the best run so far, over 13% by mass of the products were C5+ hydrocarbons and some of these, i.e., octane, are drop-in replacements for existing liquid hydrocarbons fuels. Dioxygen was detected in yields ranging between 64% and 150%. In principle, this tandem photochemical–thermochemical process, fitted with a photocatalyst better matched to the solar spectrum, could provide a cheap and direct method to produce liquid hydrocarbons from CO2 and water via a solar process which uses concentrated sunlight for both photochemical excitation to generate high-energy intermediates and heat to drive important thermochemical carbon-chain-forming reactions.

show abstract

mentioning

confidence: 99%

RETRACTED: Solar photothermochemical alkane reverse combustion

Chanmanee

Islam

Dennis

et al. 2016

Proc. Natl. Acad. Sci. U.S.A.

View full text Add to dashboard Cite

show abstract

“…[7,8] This paper,h owever, focusesonthe combination of the reverse water-gas shift reaction (RWGS) and the Fischer-Tropsch (FT) process, ar oute which has attracted ag reat deal of attention in the literature. [2,[9][10][11][12][13][14][15][16] The majority of studies in the area, though, have focusedo n 'traditional" Fischer-Tropsch catalysts with iron-and cobaltbased systemsr epresenting as ignificant portion of the work. [1,2] Generally,cobalt-based catalysts give ahigh selectivity to methane, most likely due to their poor water-gas shift activity.…”

Section: Introductionmentioning

confidence: 99%

Kinetics of CO₂ Hydrogenation to Hydrocarbons over Iron–Silica Catalysts

et al. 2017

View full text Add to dashboard Cite

The conversion of CO2 to hydrocarbons is increasingly seen as a potential alternative source of fuel and chemicals, while at the same time contributing to addressing global warming effects. An understanding of kinetics and mass transfer limitations is vital to both optimise catalyst performance and to scale up the whole process. In this work we report on a systematic investigation of the influence of the different process parameters, including pore size, catalyst support particle diameter, reaction temperature, pressure and reactant flow rate on conversion and selectivity of iron nanoparticle ‐silica catalysts. The results provided on activation energy and mass transfer limitations represent the basis to fully design a reactor system for the effective catalytic conversion of CO2 to hydrocarbons.

show abstract

“…An important challenge associated with using renewable energy sources, such as solar, is their inherent intermittent nature (4)(5)(6). The emerging field of solar fuels seeks to address this issue by storing radiant solar energy in chemical bonds, which can then be released on demand and act as a drop-in replacement for traditional fossil fuels (7)(8)(9)(10)(11).…”

mentioning

confidence: 99%

Carrier dynamics and the role of surface defects: Designing a photocatalyst for gas-phase CO ₂ reduction

Hoch

Szymanski

Ghuman

et al. 2016

Proc. Natl. Acad. Sci. U.S.A.

101

View full text Add to dashboard Cite

In 2 O 3-x (OH) y nanoparticles have been shown to function as an effective gas-phase photocatalyst for the reduction of CO 2 to CO via the reverse water-gas shift reaction. Their photocatalytic activity is strongly correlated to the number of oxygen vacancy and hydroxide defects present in the system. To better understand how such defects interact with photogenerated electrons and holes in these materials, we have studied the relaxation dynamics of In 2 O 3-x (OH) y nanoparticles with varying concentration of defects using two different excitation energies corresponding to above-band-gap (318-nm) and near-band-gap (405-nm) excitations. Our results demonstrate that defects play a significant role in the excited-state, charge relaxation pathways. Higher defect concentrations result in longer excited-state lifetimes, which are attributed to improved charge separation. This correlates well with the observed trends in the photocatalytic activity. These results are further supported by density-functional theory calculations, which confirm the positions of oxygen vacancy and hydroxide defect states within the optical band gap of indium oxide. This enhanced understanding of the role these defects play in determining the optoelectronic properties and charge carrier dynamics can provide valuable insight toward the rational development of more efficient photocatalytic materials for CO 2 reduction.indium oxide | solar fuels | CO 2 hydrogenation | transient absorption | surface defects C oncerns over climate change and the projected rise in global energy demand have motivated researchers to develop alternative, more sustainable ways to generate energy from naturally abundant and renewable sources (1-3). An important challenge associated with using renewable energy sources, such as solar, is their inherent intermittent nature (4-6). The emerging field of solar fuels seeks to address this issue by storing radiant solar energy in chemical bonds, which can then be released on demand and act as a drop-in replacement for traditional fossil fuels (7-11). By using the greenhouse gas, CO 2 , currently regarded as a waste product, as a feedstock and converting it into valuable products such as solar fuels or platform chemicals, we could simultaneously address concerns over climate change and energy security while creating significant economic benefits (12)(13)(14). However, despite recent advances in the development of active materials that can drive the photocatalytic reduction of CO 2 into useful chemical species, much remains unknown about the fundamental physical properties that control the activity of a photocatalyst. To facilitate the rational development and improvement of photocatalytic materials, a detailed understanding of the complex interplay between chemical, optical, and electronic processes is needed.Indium oxide has many favorable optical, electronic, and surface properties that make it a compelling choice as a photocatalyst for CO 2 reduction. It has a relatively high conduction band, and common defects such as oxyge...

show abstract

Catalysis for CO2 conversion: a key technology for rapid introduction of renewable energy in the value chain of chemical industries

Cited by 1,123 publications

References 186 publications

RETRACTED: Solar photothermochemical alkane reverse combustion

RETRACTED: Solar photothermochemical alkane reverse combustion

Kinetics of CO₂ Hydrogenation to Hydrocarbons over Iron–Silica Catalysts

Carrier dynamics and the role of surface defects: Designing a photocatalyst for gas-phase CO ₂ reduction

Contact Info

Product

Resources

About

Catalysis for CO2 conversion: a key technology for rapid introduction of renewable energy in the value chain of chemical industries

Cited by 1,123 publications

References 186 publications

RETRACTED: Solar photothermochemical alkane reverse combustion

RETRACTED: Solar photothermochemical alkane reverse combustion

Kinetics of CO2 Hydrogenation to Hydrocarbons over Iron–Silica Catalysts

Carrier dynamics and the role of surface defects: Designing a photocatalyst for gas-phase CO 2 reduction

Contact Info

Product

Resources

About

Kinetics of CO₂ Hydrogenation to Hydrocarbons over Iron–Silica Catalysts

Carrier dynamics and the role of surface defects: Designing a photocatalyst for gas-phase CO ₂ reduction