Controlling the speciation and reactivity of carbon-supported gold nanostructures for catalysed acetylene hydrochlorination

Kaiser, Selina K.; Lin, Rui‐Biao; Mitchell, Sharon; Fako, Edvin; Krumeich, Frank; Hauert, Roland; Safonova, Оlga V.; Kondratenko, Vita A.; Kondratenko, Evgenii V.; Collins, Sean M.; Midgley, Paul A.; López, Núria; Pérez‐Ramírez, Javier

doi:10.1039/c8sc03186j

Cited by 87 publications

(160 citation statements)

References 43 publications

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“…However, it was worth noting that Au/ACF−H 2 O was superior to the typical aqua regia‐treated catalysts in terms of stability over 15 h. The reason for this superior performance was speculatively based on the influence of surface chemistry and could be the presence of SOGs and pyrrolic N species, which may have served as anchoring sites for Au species on the ACF. Recently, Kaiser et al . reported that N species have a stabilizing effect on single Au atoms, which was consistent with our results.…”

Section: Resultssupporting

confidence: 93%

An Alternative Carbon Carrier in Green Preparation of Efficient Gold/Carbon Catalyst for Acetylene Hydrochlorination

et al. 2019

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Au catalysts supported with carbon‐based carriers have been extensively studied for the hydrochlorination of acetylene and expected to replace toxic mercury catalysts. However, removal of the highly corrosive aqua regia used in the preparation of carbon‐based catalysts while maintaining catalytic activity and stability remains a key challenge. Herein, we present a green technology carrier, activated carbon fibers (ACF), to support gold catalysts for the hydrochlorination of acetylene. TPD and XPS analyses confirmed the presence of surface oxygen‐containing functional groups (SOGs) and pyrrolic N species on the ACF. The Au/ACF−H2O catalyst exhibited better catalytic activity and stability than Au/ROX0.8(AQ)−H2O. Characterization results revealed that the catalytic properties of Au/ACF−H2O could be attributed to the anchoring and stabilization of gold active species on the SOGs, leading to atomic dispersion, and to the improvement of HCl adsorption with the synergistic effect of electron‐donating pyrrolic N groups. The results indicated that usage of this green carrier can be considered as the a new approach to reduce or eliminate the use of strong oxidizing reagents in the preparation of Au catalysts.

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Section: Resultssupporting

confidence: 93%

An Alternative Carbon Carrier in Green Preparation of Efficient Gold/Carbon Catalyst for Acetylene Hydrochlorination

et al. 2019

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“…Schematic representation of crucial hydrogen evolution steps in protic acidic medium on an extended (111) surface of an fcc metal (b) and a typical [166] SAHC (Pd atoms supported on heptazinic carbon nitride) (c). Coordination environments of successful single atom HER catalyst described in the literature [167][168][169][170][171][172][173].…”

Section: Her At Single Atom Catalystsmentioning

confidence: 99%

Hydrogen Evolution Reaction - From Single Crystal to Single Atom Catalysts

Gutić¹,

Dobrota²,

Fako³

et al. 2020

Preprint

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Hydrogen evolution reaction (HER) is one of the most important reaction in electrochemistry. This is not only because it is the simplest way to produce high purity hydrogen and the fact that it is the side reaction in many other technologies. HER actually shaped current electrochemistry because it was in focus of active research for so many years (and it still is). The number of catalysts investigated for HER is immense, and it is impossible to overview them all. In fact, it seems that the complexity of the field overcomes the complexity of HER. The aim of this review is to point out some of the latest developments in HER catalysis, current directions and some of the missing links between a single crystal, nanosized supported catalysts and, recently emerging, single atom catalysts for HER.3 of 36 HER at single crystal surfaces and bulk surfacesA crystalline solid can be considered as a series of mutually parallel lattice planes, arranged in a periodic way. Close to the surface, the spatial arrangement of the lattice planes, their crystallographic structure, as well as the dynamics of the constituent atoms may differ from the corresponding features in the bulk [1]. Most clean metals show the tendency to minimize their surface energy. One of the mechanisms is relaxation, the shift of one or more lattice planes located near to the surface, usually perpendicularly to the surface, so that the interlayer distance changes compared to the bulk lattice. The other one is reconstruction -change in equilibrium positions and bonding of surface atoms so that the projection of bulk unit cell to the given surface does not correspond to the surface unit cell. Different crystallographic planes (with different Miller indices) of the same metal exhibit unequal surface densities (number of atoms per surface area), and therefore undergo surface relaxation/reconstruction to different extents [2]. For example, Pt(100) has lower surface density compared to densely packed Pt(111) and therefore has a stronger tendency to relax/reconstruct. Since the main driving force for the mentioned surface modifications is the low coordination number (non-saturation) of surface atoms, it is obvious that atom/molecule adsorption on clean metal surfaces can have a significant effect on its surface structure, inducing relaxation/reconstruction changes. This is of huge importance for HER, as it involves adsorbed atomic hydrogen (Hads) as an intermediate. Additionally, in an electrochemical system, the electrode will be modified by adsorption of "spectator" species (ions/molecules from the electrolyte), so HER will not be taking place on clean metal surfaces, but rather on modified ones. Obviously, there is a complex dynamic interplay between the catalyst surface, reactants, intermediates, and electrolyte.According to the Sabatier principle, the interaction of the reaction reactants/intermediates with the catalyst has to be optimal in strength. If it is too weak, the reactants will not bind to the catalyst and the reaction will not be able to take place. In...

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“…Perez-Ramirez et al found that Au single atoms hosted on N-doped carbon-derived by the controlled pyrolysis of polyaniline exhibited remarkable stability for acetylene hydrochlorination. 6 In our previous work, we reported that metallic Au nanoparticles exhibited considerable catalytic activity for acetylene hydrochlorination, and the aggregation of Au nanoparticles was another reason for the deactivation of the Aubased catalyst in addition to the reduction of Au(III) or Au(I). 7 Therefore, this study used metallic Au as an active site for acetylene hydrochlorination.…”

Section: Introductionmentioning

confidence: 99%

An efficient Au catalyst supported on hollow carbon spheres for acetylene hydrochlorination

Kang

2019

RSC Adv.

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Controlling the speciation and reactivity of carbon-supported gold nanostructures for catalysed acetylene hydrochlorination

Abstract: Distinct gold nanostructures on activated and nitrogen-doped carbons are evaluated in acetylene hydrochlorination.

Cited by 87 publications

References 43 publications

An Alternative Carbon Carrier in Green Preparation of Efficient Gold/Carbon Catalyst for Acetylene Hydrochlorination

An Alternative Carbon Carrier in Green Preparation of Efficient Gold/Carbon Catalyst for Acetylene Hydrochlorination

Hydrogen Evolution Reaction - From Single Crystal to Single Atom Catalysts

An efficient Au catalyst supported on hollow carbon spheres for acetylene hydrochlorination

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