Hydrogenolysis of methyl glycolate to ethanol over a Pt–Cu/SiO<sub>2</sub>single-atom alloy catalyst: a further step from cellulose to ethanol

Yang, Chun‐Feng; Miao, Zhili; Zhang, Fan; Li, Lin; Liu, Yanting; Wang, Aiqin; Zhang, Tao

doi:10.1039/c8gc00309b

Cited by 92 publications

(68 citation statements)

References 41 publications

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“…280 Alongside ethylbenzene, relevant amounts of methyl-cyclohexane, benzene, and cyclohexane were also observed. These products may result either from hydrogenation of the reactant or from the hydrogenolysis process 281 In the latter study, several loadings of Pt single atoms alloyed with Cu were prepared and tested for hydrogenolysis of MG. The single atom alloys of Pt−Cu/SiO 2 were prepared stepwise; in the first step, silica-supported Cu was prepared via urea assisted gelation (UAG) method using a literature procedure.…”

Section: Chemical Reviewsmentioning

confidence: 99%

“…MG conversion reached 100% above 473 K, whereas the highest selectivity for ethanol (69%) was observed at 523 K. Above this temperature, side products such as (Figure 37). 281 The other SAAC (0.3Pt−Cu/SiO 2 and 0.06Pt−Cu/SiO 2 ) produced mostly ethylene glycol, 2-propanol, propanol, and butanol (Scheme 16 and Figure 37). 281 Characterization of Pt SAA reveals that the dispersion of Cu was highest at the Pt content of 0.1 wt % and improved the Cu + /Cu 0 ratio; on the other hand, the single atoms of Pt promoted the activation of H 2 while minimizing the C−C cleavage reaction, hence improving the ethanol selectivity.…”

Section: Chemical Reviewsmentioning

confidence: 99%

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The Comparison between Single Atom Catalysis and Surface Organometallic Catalysis

et al. 2019

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Single atom catalysis (SAC) is a recent discipline of heterogeneous catalysis for which a single atom on a surface is able to carry out various catalytic reactions. A kind of revolution in heterogeneous catalysis by metals for which it was assumed that specific sites or defects of a nanoparticle were necessary to activate substrates in catalytic reactions. In another extreme of the spectrum, surface organometallic chemistry (SOMC), and, by extension, surface organometallic catalysis (SOMCat), have demonstrated that single atoms on a surface, but this time with specific ligands, could lead to a more predictive approach in heterogeneous catalysis. The predictive character of SOMCat was just the result of intuitive mechanisms derived from the elementary steps of molecular chemistry. This review article will compare the aspects of single atom catalysis and surface organometallic catalysis by considering several specific catalytic reactions, some of which exist for both fields, whereas others might see mutual overlap in the future. After a definition of both domains, a detailed approach of the methods, mostly modeling and spectroscopy, will be followed by a detailed analysis of catalytic reactions: hydrogenation, dehydrogenation, hydrogenolysis, oxidative dehydrogenation, alkane and cycloalkane metathesis, methane activation, metathetic oxidation, CO 2 activation to cyclic carbonates, imine metathesis, and selective catalytic reduction (SCR) reactions. A prospective resulting from present knowledge is showing the emergence of a new discipline from the overlap between the two areas.

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Section: Chemical Reviewsmentioning

confidence: 99%

Section: Chemical Reviewsmentioning

confidence: 99%

The Comparison between Single Atom Catalysis and Surface Organometallic Catalysis

et al. 2019

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“…Moreover, they show high resistance to CO poisoning, 14 and have successfully catalysed reactions of practical interest, including hydrogenations, 15 dehydrogenations, 16 C-H activation, 17 hydrosilylations 18 and hydrogenolysis. 19 Though SAAs are extremely promising new catalysts, their isolated single atoms are sometime unable to activate chemical bonds that can otherwise be broken by small ensembles of PGMs such as dimers, trimers and islands. [20][21][22] Therefore in these cases the formation of surface aggregates in highly dilute alloy surfaces may be necessary in order to achieve reasonable catalytic rates.…”

Section: Introductionmentioning

confidence: 99%

CO-Induced Aggregation and Segregation of Highly Dilute Alloys: A Density Functional Theory Study

2019

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Highly dilute binary alloys composed of an active platinum group metal (PGM) and a more inert coinage metal are important in the field of catalysis, as they function as active and selective catalysts. Their catalytic properties depend on the surface "ensemble" of PGM atoms, whose size may be altered under reactive conditions. We use density functional theory and investigate the interaction of CO, a molecule common in numerous industrially important chemistries, with alloys that are composed of a PGM (Pt, Pd, Rh, Ir, Ni) doped in coinage metal hosts (Cu, Au, Ag). We study the adsorption of CO on the (211) step and (100) facet and compare our results to those previously obtained on the (111) facet. We determine strong correlations between the adsorption energies of CO across the facets and highlight the corresponding thermochemical scaling relations. Finally, we study the stability of isolated surface dopant atoms with respect to aggregation into clusters and segregation into the bulk, both in the presence and absence of CO. We find that strong COdopant interactions significantly influence the morphology of the catalyst surface, suggesting that it may be possible to establish control over the ensemble size of the dopant by tuning PCO.

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“…Therefore, the providential design of multifunctional and robust catalysts that can regulate all kinds of complex reactions efficiently is paramount. As reported, tungsten-based catalysts and Pt-Cu/SiO 2 single-atom alloy catalyst were successfully applied to the two-step conversion of cellulose to ethanol, methyl glycolate(MG) is easily formed from glycolaldehyde intermediate when the reactions were carried out in methanol solvent, and further hydrogenation is necessary to obtain ethanol after MG hydrogenated to EG (Xu et al, 2017;Yang et al, 2018). Noting that the EG is the precursor of ethanol production and could get a high yield in deionized water which avoids the use of organic solvent, thereby the process that conversion of cellulose to ethanol is thought highly of in aqueous phase.…”

Section: Ethanolmentioning

confidence: 99%

Catalytic Production of Oxygenated and Hydrocarbon Chemicals From Cellulose Hydrogenolysis in Aqueous Phase

Xin

Cai

et al. 2020

Front. Chem.

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As the most abundant polysaccharide in lignocellulosic biomass, a clean and renewable carbon resource, cellulose shows huge capacity and roused much attention on the methodologies of its conversion to downstream products, mainly including platform chemicals and fuel additives. Without appropriate treatments in the processes of cellulose decompose, there are some by-products that may not be chemically valuable or even truly harmful. Therefore, higher selectivity and more economical and greener processes would be favored and serve as criteria in a correlational study. Aqueous phase, an economically accessible and immensely potential reaction system, has been widely studied in the preparation of downstream products of cellulose. Accordingly, this mini-review aims at making a related summary about several conversion pathways of cellulose to target products in aqueous phase. Mainly, there are four categories about the conversion of cellulose to downstream products in the following: (i) cellulose hydrolysis hydrogenation to saccharides and sugar alcohols, like glucose, sorbitol, mannose, etc.; (ii) selective hydrogenolysis leads to the cleavage of the corresponding glucose CC and CO bond, like ethylene glycol (EG), 1,2-propylene glycol (PG), etc.; (iii) dehydration of fructose and further oxidation, like 5-hydroxymethylfurfural (HMF), 2,5-furandicarboxylic acid (FDCA), etc.; and (iv) production of liquid alkanes via hydrogenolysis and hydrodeoxygenation, like pentane, hexane, etc. The representative products were enumerated, and the mechanism and pathway of mentioned reaction are also summarized in a brief description. Ultimately, the remaining challenges and possible further research objects are proposed in perspective to provide researchers with a lucid research direction.

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Hydrogenolysis of methyl glycolate to ethanol over a Pt–Cu/SiO₂single-atom alloy catalyst: a further step from cellulose to ethanol

Abstract: The Pt–Cu single-atom alloy (SAA) catalyst showed significantly enhanced activity, selectivity, and stability for the hydrogenolysis of methyl glycolate to ethanol.

Cited by 92 publications

References 41 publications

The Comparison between Single Atom Catalysis and Surface Organometallic Catalysis

The Comparison between Single Atom Catalysis and Surface Organometallic Catalysis

CO-Induced Aggregation and Segregation of Highly Dilute Alloys: A Density Functional Theory Study

Catalytic Production of Oxygenated and Hydrocarbon Chemicals From Cellulose Hydrogenolysis in Aqueous Phase

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Hydrogenolysis of methyl glycolate to ethanol over a Pt–Cu/SiO2single-atom alloy catalyst: a further step from cellulose to ethanol

Abstract: The Pt–Cu single-atom alloy (SAA) catalyst showed significantly enhanced activity, selectivity, and stability for the hydrogenolysis of methyl glycolate to ethanol.

Cited by 92 publications

References 41 publications

The Comparison between Single Atom Catalysis and Surface Organometallic Catalysis

The Comparison between Single Atom Catalysis and Surface Organometallic Catalysis

CO-Induced Aggregation and Segregation of Highly Dilute Alloys: A Density Functional Theory Study

Catalytic Production of Oxygenated and Hydrocarbon Chemicals From Cellulose Hydrogenolysis in Aqueous Phase

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Hydrogenolysis of methyl glycolate to ethanol over a Pt–Cu/SiO₂single-atom alloy catalyst: a further step from cellulose to ethanol