Catalysis by Gold: Isolated Surface Au<sup>3+</sup> Ions are Active Sites for Selective Hydrogenation of 1,3‐Butadiene over Au/ZrO<sub>2</sub> Catalysts

Zhang, Xin; Shi, Hui; Xu, Bin

doi:10.1002/anie.200502101

Cited by 325 publications

(279 citation statements)

References 28 publications

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“…These results are in good agreement with the results of Zhang et al [45,46]. This group used Au/ZrO 2 to investigate the effects of Au 3+ /Au 0 ratio on 1,3-butadiene hydrogenation.…”

Section: The Nature Of Au Activation In Nio/au Clusterssupporting

confidence: 91%

“…This group used Au/ZrO 2 to investigate the effects of Au 3+ /Au 0 ratio on 1,3-butadiene hydrogenation. It was reported that metallic Au 0 atoms at the surface of the gold particles were not the only active catalytic sites and that isolated Au 3+ ions were the most active [45,46]. The enhanced activation of H 2 on charged gold could be explained by mechanism of Au n -H 2 formation.…”

Section: The Nature Of Au Activation In Nio/au Clustersmentioning

confidence: 98%

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Sites for the selective hydrogenation of ethyne to ethene on supported NiO/Au catalysts

2012

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Au, NiO, and NiO/Au clusters of 2.5-16 nm, supported on Al 2 O 3 , ZrO 2 , TiO 2 , and ZnO, were studied in the purification of ethene feedstock from ethyne by hydrogenation at 357 K. The Au, NiO, and NiO/Au catalysts possessed 100 % selectivity to ethene. As the size of NiO clusters decreased from 7 to 3 nm, the turnover frequency (TOF) decreased from 812-1,023 to 276 h −1 . In contrast with NiO, Au activity increased with decreasing particle size. NiO/Au catalysts possessed higher stability and activity in comparison with Au and NiO catalysts. The synergistic gain on NiO/Au clusters (SG) calculated as TOF NiO/Au -TOF Au -TOF NiO was 1,466; 1,147; 563; and 569 h −1 for NiO/Au/Al 2 O 3, NiO/Au/TiO 2 , NiO/Au/ZnO, and NiO/Au/ ZrO 2 , respectively. The reasons of the observed catalytic trends and the origin of the most active and selective sites are discussed.

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“…These results are in good agreement with the results of Zhang et al [45,46]. This group used Au/ZrO 2 to investigate the effects of Au 3+ /Au 0 ratio on 1,3-butadiene hydrogenation.…”

Section: The Nature Of Au Activation In Nio/au Clusterssupporting

confidence: 91%

Section: The Nature Of Au Activation In Nio/au Clustersmentioning

confidence: 98%

Sites for the selective hydrogenation of ethyne to ethene on supported NiO/Au catalysts

2012

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“…For the WGS reaction, isolated gold cations have been claimed as the active sites [12], although more recently there appears to be consensus that metallic gold cluster are the active sites [13,14]. A similar debate is apparent about the active sites in alkene hydrogenation [11,[15][16][17].…”

Section: Introductionmentioning

confidence: 99%

Gold Stabilized by Nanostructured Ceria Supports: Nature of the Active Sites and Catalytic Performance

et al. 2011

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The interaction of gold atoms with CeO 2 nanocrystals having rod and cube shapes has been examined by cyanide leaching, TEM, TPR, CO IR and X-ray absorption spectroscopy. After deposition-precipitation and calcination of gold, these surfaces contain gold nanoparticles in the range 2-6 nm. For the ceria nanorods, a substantial amount of gold is present as cations that replace Ce ions in the surface as follows from their first and second coordination shells of oxygen and cerium by EXAFS analysis. These cations are stable against cyanide leaching in contrast to gold nanoparticles. Upon reduction the isolated Au atoms form finely dispersed metal clusters with a high activity in CO oxidation, the WGS reaction and 1,3-butadiene hydrogenation. By analogy with the very low activity of reduced gold nanoparticles on ceria nanocubes exposing the {100} surface plane, it is inferred that the gold nanoparticles on the ceria nanorod surface also have a low activity in such reactions. Although the finely dispersed Au clusters are thermally stable up to quite high temperature in line with earlier findings (Y. Guan and E. J. M. Hensen, Phys Chem Chem Phys 11:9578, 2009), the presence of gold nanoparticles results in their more facile agglomeration, especially in the presence of water (e.g., WGS conditions). For liquid phase alcohol oxidation, metallic gold nanoparticles are the active sites. In the absence of a base, the O-H bond cleavage appears to be rate limiting, while this shifts to C-H bond activation after addition of NaOH. In the latter case, the gold nanoparticles on the surface of ceria nanocubes are much more active than those on the surface of nanorod ceria.

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“…136 In addition, it was claimed that isolated surface Au 3+ ions are active sites for selective hydrogenation of 1,3-butadiene on Au/ZrO 2 . 137 Hensen and co-workers showed that the cationic gold in leached Au/CeO 2 could be partially reduced to metallic gold clusters active for hydrogenation of 1,3-butadiene, CO oxidation, and WGSR. 81,138 Rodriguez and co-workers studied Au/Ce(Gd)O 2 and Au/ CeO x /TiO 2 using in situ time-resolved X-ray absorption spectroscopy (TR-XAS).…”

Section: Nature Of Active Sitesmentioning

confidence: 99%

Water–gas shift on gold catalysts: catalyst systems and fundamental studies

Tao¹,

Ma²

2013

Phys. Chem. Chem. Phys.

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Since the pioneering finding by Haruta et al. that small gold nanoparticles on reducible supports can be highly active for low-temperature CO oxidation, the synthesis, characterization, and application of supported gold catalysts have attracted much attention. The water-gas shift reaction (WGSR: CO + H 2 O = CO 2 + H 2 ) is important for removing CO and upgrading the purity of H 2 for fuel cell applications, ammonia synthesis, and selective hydrogenation processes. In recent years, much attention has been paid to exploration the possibility of using supported gold nanocatalysts for WGSR and understanding the fundamental aspects related to catalyst deactivation mechanisms, nature of active sites, and reaction mechanisms. Here we summarize recent advances in the development of supported gold catalysts for this reaction and fundamental insights that can be gained, and furnish our assessment on the status of research progress.

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Catalysis by Gold: Isolated Surface Au³⁺ Ions are Active Sites for Selective Hydrogenation of 1,3‐Butadiene over Au/ZrO₂ Catalysts

Cited by 325 publications

References 28 publications

Sites for the selective hydrogenation of ethyne to ethene on supported NiO/Au catalysts

Sites for the selective hydrogenation of ethyne to ethene on supported NiO/Au catalysts

Gold Stabilized by Nanostructured Ceria Supports: Nature of the Active Sites and Catalytic Performance

Water–gas shift on gold catalysts: catalyst systems and fundamental studies

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Catalysis by Gold: Isolated Surface Au3+ Ions are Active Sites for Selective Hydrogenation of 1,3‐Butadiene over Au/ZrO2 Catalysts

Cited by 325 publications

References 28 publications

Sites for the selective hydrogenation of ethyne to ethene on supported NiO/Au catalysts

Sites for the selective hydrogenation of ethyne to ethene on supported NiO/Au catalysts

Gold Stabilized by Nanostructured Ceria Supports: Nature of the Active Sites and Catalytic Performance

Water–gas shift on gold catalysts: catalyst systems and fundamental studies

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Product

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Catalysis by Gold: Isolated Surface Au³⁺ Ions are Active Sites for Selective Hydrogenation of 1,3‐Butadiene over Au/ZrO₂ Catalysts