New insights into structure–activity relationships for propane hydrogenolysis over Ni–Cu bimetallic catalysts

Yao, Yunxi; Goodman, D. W.

doi:10.1039/c5ra07433a

Cited by 15 publications

(9 citation statements)

References 41 publications

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“…Single-atom alloy (SAA) catalysts have been shown to be active for a variety of processes, including selective hydrogenation reactions [127][128][129][130], dehydrogenation reactions [131][132][133],oxidation reactions [134,135], hydrogenolysis [136] and coupling reactions [137] and have generated significant interest in recent years. Here, the creation of SAA catalysts is based on the deposition of isolated reactive metal adatoms into host metal surfaces (of a relatively inert metal).…”

Section: Single-atom Alloysmentioning

confidence: 99%

Single-Atom Catalysts: From Design to Application

Cheng

Zhang

Doyle

et al. 2019

Electrochem. Energ. Rev.

427

270

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Single-atom catalysis is a powerful and attractive technique with exceptional performance, drastic cost reduction and notable catalytic activity and selectivity. In single-atom catalysis, supported single-atom catalysts contain isolated individual atoms dispersed on, and/or coordinated with, surface atoms of appropriate supports, which not only maximize the atomic efficiency of metals, but also provide an alternative strategy to tune the activity and selectivity of catalytic reactions. This review will highlight the attributes of single-atom catalysis and summarize the most recent advancements in single-atom catalysts with a focus on the design of highly active and stable single atoms. In addition, new research directions and future trends will also be discussed.

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Section: Single-atom Alloysmentioning

confidence: 99%

Single-Atom Catalysts: From Design to Application

Cheng

Zhang

Doyle

et al. 2019

Electrochem. Energ. Rev.

427

270

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show abstract

“…Ni supported on alumina or magnesium oxide, for example, is the current standard catalyst in steam reforming of methane. − This major industrial process produces synthesis gas, which in turn fuels other large-scale reactions including Fischer–Tropsch synthesis and methanol synthesis. , Single atom alloys (SAAs), isolated reactive metal adatoms dispersed in the surface layer of a more inert host metal, have generated significant interest as catalysts in recent years. Numerous studies so far have demonstrated the capability of SAAs to catalyze hydrogenations, − dehydrogenations, oxidations, , hydrogenolysis, and coupling reactions . While Cu is a somewhat catalytically inert metal, for example, Pd–Cu SAAs can enable the facile activation of H 2 , spillover of hydrogen atoms onto Cu, and subsequent hydrogenation of styrene and acetylene .…”

Section: Introductionmentioning

confidence: 99%

“…16,17 Single atom alloys (SAAs), isolated reactive metal adatoms dispersed in the surface layer of a more inert host metal, have generated significant interest as catalysts in recent years. Numerous studies so far have demonstrated the capability of SAAs to catalyze hydrogenations, 19−22 dehydrogenations, 23 oxidations, 24,25 hydrogenolysis, 26 and coupling reactions. 27 While Cu is a somewhat catalytically inert metal, for example, Pd−Cu SAAs can enable the facile activation of H 2 , spillover of hydrogen atoms onto Cu, and subsequent hydrogenation of styrene and acetylene.…”

Section: Introductionmentioning

confidence: 99%

Preparation, Structure, and Surface Chemistry of Ni–Au Single Atom Alloys

et al. 2016

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Ni/Au is an alloy combination that while, immiscible in the bulk, exhibits a rich array of surface geometries that may offer improved catalytic properties. It has been demonstrated that the addition of small amounts of Au to Ni tempers its reactivity and reduces coking during the steam reforming of methane. Herein, we report the first successful preparation of dilute Ni−Au alloys (up to 0.04 ML) in which small amounts of Ni are deposited on, and alloyed into, Au(111) using physical vapor deposition. We find that the surface structure can be tuned during deposition via control of the substrate temperature. By adjusting the surface temperature in the 300−650 K range, we are able to produce first Ni islands, then mixtures of Ni islands and Ni−Au surface alloys, and finally, when above 550 K, predominantly island-free Ni−Au single atom alloys (SAAs). Low-temperature scanning tunneling microscopy (STM) combined with density functional theory calculations confirm that the Ni−Au SAAs formed at high temperature correspond to Ni atoms exchanged with surface Au atoms. Ni−Au SAAs form preferentially at the elbow regions of the Au(111) herringbone reconstruction, but at high coverage also appear over the whole surface. To investigate the adsorption properties of Ni−Au SAAs, we studied the adsorption and desorption of CO using STM which allowed us to determine at which atomic sites the CO adsorbs on these heterogeneous alloys. We find that small amounts of Ni in the form of single atoms increases the reactivity of the substrate by creating single Ni sites in the Au surface to which CO binds significantly more strongly than Au. These results serve as a guide in the design of surface architectures that combine Au's weak binding and selective chemistry with localized, strong binding Ni atom sites that serve to increase reactivity.

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“…In contrast to Ni metal, Cu species show selective hydrogenation activity for C−O and C=O bonds, but they are relatively inactive for the hydrogenation of C−C bonds [15] As previously reported, the interaction between Ni and Cu plays an important role in enhancing the catalytic performance for hydrogenation/hydrogenolysis [20,43,62–64] . Previous studies have shown that Cu 0 is not the only active site for GVL conversion, and that the distribution of active Cu species with different chemical valences on the surface of Cu‐based catalysts is usually important for C=O/C−O hydrogenation [37,65] .…”

Section: Resultsmentioning

confidence: 92%

Layered Double Hydroxide‐Derived Bimetallic Ni−Cu Catalysts Prompted the Efficient Conversion of γ‐Valerolactone to 2‐Methyltetrahydrofuran

Wang

et al. 2021

ChemCatChem

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The catalytic upgrading of γ‐valerolactone (GVL) to liquid biofuel, which is of great importance to the development of new types of high‐performance heterogeneous catalysts, is regarded as a technically difficult task because of the thermal stability of GVL. Consequently, in this study, a series of nanocatalysts NixCu3‐x/Al2O3 (x=0, 1, 1.5, 2, and 3) derived from layered double hydroxide (LDH) precursors were prepared for the hydrogenation of biomass‐derived GVL to 2‐methyltetrahydrofuran (2‐MTHF). The optimal bimetallic Ni2Cu1/Al2O3 catalyst showed high 2‐MTHF selectivity with complete GVL conversion. Detailed characterization revealed cooperation between the acid sites and Ni−Cu alloy in the bimetallic catalysts, which was responsible for their high activities. More importantly, the strong interaction between Ni and Cu changed the surface chemical environment, which generated different copper species and enhanced the H2 activation ability. The reusability of the Ni2Cu1/Al2O3 catalyst and the effect of the reaction conditions, such as temperature, H2 pressure, and solvent, were also investigated.

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New insights into structure–activity relationships for propane hydrogenolysis over Ni–Cu bimetallic catalysts

Abstract: The structure–activity relationships of Cu–Ni bimetallic catalysts in propane hydrogenolysis reactions were investigated by using model catalyst systems.

Cited by 15 publications

References 41 publications

Single-Atom Catalysts: From Design to Application

Single-Atom Catalysts: From Design to Application

Preparation, Structure, and Surface Chemistry of Ni–Au Single Atom Alloys

Layered Double Hydroxide‐Derived Bimetallic Ni−Cu Catalysts Prompted the Efficient Conversion of γ‐Valerolactone to 2‐Methyltetrahydrofuran

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