Ethanol-to-butadiene: the reaction and its catalysts

Pomalaza, Guillaume; Ponton, Paola Arango; Capron, Mickäel; Dumeignil, Franck

doi:10.1039/d0cy00784f

Cited by 115 publications

(128 citation statements)

References 252 publications

(863 reference statements)

Supporting

Mentioning

107

Contrasting

Order By: Relevance

“…Nevertheless, acid-base pair concept should not be confused with the coexistence on a same material of acidic and basic phases. For example, in the case of MgO-SiO2 system that was extensively studied for bio-ethanol cascade reaction conversion into butadiene and recently reviewed by Pomalaza et al [175], it was shown that acidic sites (on silica or on magnesium silicates) are involved in the dehydration steps whereas the basic ones (on MgO) catalyse the dehydrogenation and condensation steps. In this case, the catalyst is bifunctional, the two properties are independently characterized and the optimal balance between acid and base phases is defined.…”

Section: Acid-base Pairs and Their Characterizationmentioning

confidence: 99%

Characterisation and reactivity of oxygen species at the surface of metal oxides

Anpo

Costentin

Giamello

et al. 2021

Journal of Catalysis

View full text Add to dashboard Cite

HAL is a multi-disciplinary open access archive for the deposit and dissemination of scientific research documents, whether they are published or not. The documents may come from teaching and research institutions in France or abroad, or from public or private research centers. L'archive ouverte pluridisciplinaire HAL, est destinée au dépôt et à la diffusion de documents scientifiques de niveau recherche, publiés ou non, émanant des établissements d'enseignement et de recherche français ou étrangers, des laboratoires publics ou privés.

show abstract

Section: Acid-base Pairs and Their Characterizationmentioning

confidence: 99%

Characterisation and reactivity of oxygen species at the surface of metal oxides

Anpo

Costentin

Giamello

et al. 2021

Journal of Catalysis

View full text Add to dashboard Cite

show abstract

“…Reducing the ethanol partial pressure appeared to increase the selectivity, which has been observed previously. 9 Da Ros et al 31 obtained a butadiene yield of around 20 % at 723 K on 95:5 MgO-SiO 2 and Taifan et al 26 reported up to 30 % selectivity for butadiene under similar conditions, but with significantly more ethylene formation.…”

Section: Microkinetic Analysismentioning

confidence: 96%

First-principles-informed energy span and microkinetic analysis of ethanol catalytic conversion to 1,3-butadiene on MgO

Boje¹,

Taifan²,

Ström³

et al. 2021

Preprint

View full text Add to dashboard Cite

Kinetic modeling of single-step catalytic conversion of ethanol to 1,3-butadiene is necessary to inform accurate process design. This paper uses first-principles-informed energy span and microkinetic analysis to explore the reaction free energy landscapes and kinetic limitations of competing reaction pathways on a MgO (100) step-edge. Previous studies suggested mechanisms proceeding via both dehydrogenation and dehydration of ethanol, and highlighted sensitivity to conditions and catalyst composition. Here, we use the energy span concept to characterize the theoretical maximum turnover and degree of turnover frequency control for states in each reaction pathway, finding the dehydration route to be less active for 1,3-butadiene, and suggesting rate-determining states in the dehydrogenation, dehydration, and condensation steps. The influence of temperature on the relative rate contribution of each state is quantified and explained through the varying temperature sensitivity of the free energy landscape. A microkinetic model is developed to explore competition between pathways, interaction with gas-phase species, and surface coverage limitations. This suggests that the turnover may be significantly lower than predicted solely based on energetics. Turnover frequency determining states found to have high surface coverage include adsorbed ethanol and two longer, oxygenated hydrocarbons. The combined energy span and microkinetic analysis permits investigation of a complex system from two perspectives and helps elucidate conflicting observations of rate determining steps and product distribution by considering both energetic and kinetic limitations. The impact of uncertainty in the energy landscape is quantified using a correlated error model. While the range of predictions is large, the average performance and trends are similar.

show abstract

“…of sugars, [27,90] wood pyrolysis with addition of calcium carbonate [65] S HO OH OH glycerol byproduct of biodiesel production (50 wt%) [91][92] S OH Me Me O acetoin fmt. of sugars (>40 g/L) [93] P 1,3-butadiene (grain or potato) catalytic gas phase synthesis from ethanol [94] S Me HO 1-butanol ABE-fmt. of sugars (34 wt%) [27,74]…”

Section: P Me Mementioning

confidence: 99%

Xylochemicals and where to find them

et al. 2021

View full text Add to dashboard Cite

show abstract

Ethanol-to-butadiene: the reaction and its catalysts

Abstract: Catalytic conversion of ethanol is a promising technology for producing sustainable butadiene. This paper reviews the reaction and its catalysts, and discusses the challenges their development faces.

Cited by 115 publications

References 252 publications

Characterisation and reactivity of oxygen species at the surface of metal oxides

Characterisation and reactivity of oxygen species at the surface of metal oxides

First-principles-informed energy span and microkinetic analysis of ethanol catalytic conversion to 1,3-butadiene on MgO

Xylochemicals and where to find them

Contact Info

Product

Resources

About