A Strong Support Effect in Selective Propane Dehydrogenation Catalyzed by Ga(i-Bu)3 Grafted onto γ-Alumina and Silica

Szeto, Kai C.; Jones, Zachary R.; Merle, Nicolas; Rios, César; Gallo, Alessandro; Le Quemener, Frederic; Delevoye, Laurent; Gauvin, Régis M.; Scott, Susannah L.; Taoufik, Mostafa

doi:10.1021/acscatal.8b00936

Title: A Strong Support Effect in Selective Propane Dehydrogenation Catalyzed by Ga(i-Bu)₃ Grafted onto γ-Alumina and Silica

Journal Article · Mon Jul 09 00:00:00 EDT 2018 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.8b00936· OSTI ID:1476169

Szeto, Kai C. ^[1]; Jones, Zachary R. ^[2];

^[3]; Rios, César ^[1]; Gallo, Alessandro ^[4]; Le Quemener, Frederic ^[1]; Delevoye, Laurent ^[3];

^[3];

^[2]; Taoufik, Mostafa ^[1]

Univ. Lyon, Villeurbanne Cedex (France)
Univ. of California, Santa Barbara, CA (United States)
Univ. Lille, Lille (France)
Univ. of California, Santa Barbara, CA (United States); Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)

The reactions of Ga(i-Bu)₃ (i-Bu = CH₂CH(CH₃)₂) with the dehydrated and partially dehydroxylated surfaces of alumina (Al₂O_3–500) and silica (SiO_2–700) were studied by IR, high field solid-state NMR and EXAFS spectroscopies, as well as elemental analysis. Grafting onto Al₂O_3–500 occurs selectively by protonolysis at individual surface hydroxyl groups, resulting in the formation of mononuclear [(≡AlO)Ga(i-Bu)₂L] (L = surface oxygen) sites as the major surface organometallic entities. Conversely, grafting on silica affords dinuclear species [(≡SiO)₂Ga₂(i-Bu)₃] by a combination of protonolysis and isobutyl group transfer to Si. Further evidence for the difference in nuclearity was obtained by analysis of the WT-EXAFS. The mononuclear alumina-supported Ga sites show much higher activity in propane dehydrogenation than their dinuclear silica-supported counterparts. The propane dehydrogenation reaction may require the presence of Al–O–Ga bonds to promote heterolytic C–H bond activation. In conclusion, comparisons with benchmark catalysts and related systems show that the effect of the catalyst diluent is significant under the reaction conditions and must be carefully assessed in order to attribute reactivity correctly.

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Research Organization:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-76SF00515; FG02-03ER15467; FR 2638

OSTI ID:: 1476169

Journal Information:: ACS Catalysis, Vol. 8, Issue 8; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 52 works

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Title: A Strong Support Effect in Selective Propane Dehydrogenation Catalyzed by Ga(i-Bu)3 Grafted onto γ-Alumina and Silica

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Title: A Strong Support Effect in Selective Propane Dehydrogenation Catalyzed by Ga(i-Bu)₃ Grafted onto γ-Alumina and Silica