Significant impact of γ-Al2O3 facet structure on the character and performance of surface Co-Mo sulfides for CO removal in H2 fuel via water gas shift

Wang, Pengcheng; Li, Jun; Xu, Peiwen; Feng, Xinzhen; Ji, Weijie

doi:10.1016/j.apsusc.2020.148230

Cited by 6 publications

(5 citation statements)

References 70 publications

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“…The selected area electron diffraction (SAED) patterns of Al 2 O 3 -HP and Al 2 O 3 -SHP (not shown) verify the high sample crystallinity and major exposed facet(s) of (110) or (111)/(100), respectively. According to our previous study, the areal fraction of the (110) facet is about 90% on Al 2 O 3 -HP, whereas the areal fraction of the (111)/(100) facet is approximately 59% Figure d–f shows the SEM images of the three supported trimetallic catalysts.…”

Section: Resultssupporting

confidence: 86%

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Selective Hydrogenation of Polyenes in Biomass-Derived Cardanol over the Trimetallic Ni–Co–Cu Catalyst Supported on Morphologically Controlled Alumina

Ding,

Xu,

Fang

et al. 2023

Ind. Eng. Chem. Res.

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The aim of this study is to achieve a high fraction of monoene in biomass-derived cardanol to manipulate a well-balanced potential of cross-linking and coupling between resin and curing agent for heavy-duty coating. We reported a heterogeneous nonprecious trimetallic catalyst for selective hydrogenation of polyenes in cardanol for the first time. By cointroducing the second and third metal constituents (Cu and Co), and particularly facet controlling as well as Zn doping of Al2O3 substrate, we can accomplish the highly selective hydrogenation of triene/diene into monoene with variable ratio. The larger sized Ni entities with higher electron density on the Al2O3 hexagonal plates are more favorable for activating triene/diene responsible for a high potential of selective hydrogenation. On the other hand, the Ni0 fraction is comparatively lower, while the mean particle size of Ni0 is the smallest with lower electron density on the commercially obtained γ-Al2O3 spherules. The latter kind of Ni entities is more favorable for activating hydrogen to generate highly reactive H species accounting for a strong potential of full hydrogenation. Over a fine-tuned 10% Ni-5% Co-3% Cu/3% Zn-Al2O3-hexagonal plate under the optimized conditions (7.5% cardanol in n-butanol, 2.5 MPa H2, 80 °C, and 3.5 h), as high as 76% monoene can be obtainable. It is worth noting that not only the current catalyst system is more economic but also the reaction becomes kinetically much faster (within 3.5 h). This catalyst system is operational to a large-scale application in the modification of cardanol via selective hydrogenation. Ni–Co–Cu synergism and low-content Zn modification of the Al2O3 (110) facet are essential to achieve the aim of this study.

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Section: Resultssupporting

confidence: 86%

“…(1) Synthesis of Al 2 O 3 hexagonal plates (Al 2 O 3 -HP): The procedure was in reference to that previously reported by us . Briefly, AlCl 3 ·6H 2 O (0.483 g) was dissolved in 4.62 mL deionized water and stirred at room temperature (RT) for 30 min.…”

Section: Methodsmentioning

confidence: 99%

Selective Hydrogenation of Polyenes in Biomass-Derived Cardanol over the Trimetallic Ni–Co–Cu Catalyst Supported on Morphologically Controlled Alumina

Ding,

Xu,

Fang

et al. 2023

Ind. Eng. Chem. Res.

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“…It was found out that the Pt/(110) interface significantly outperforms the other interfaces for WGS (Figure S7). Our previous studies also demonstrated that the sulfide/Al 2 O 3 (110) interface is superior to the sulfide/Al 2 O 3 (111) & (100) interfaces for the hydrodesulfurization of dibenzothiophene and water gas shift . On the (110) facet of γ-Al 2 O 3 , more active MoS 2 and Co 9 S 8 /Co–Mo–S species are favorably formed while less active CoMoO x S 2 and SO x 2– species are constrainedly produced.…”

Section: Resultsmentioning

confidence: 89%

“…Our previous studies also demonstrated that the sulfide/Al 2 O 3 (110) interface is superior to the sulfide/Al 2 O 3 (111) & (100) interfaces for the hydrodesulfurization of dibenzothiophene 89 and water gas shift. 90 Comparing the behaviors of the two reactions over the same catalyst series looks interesting. In the WGS reaction, the CO conversion could be very high at 200 °C, while the H 2 (CO 2 ) yield appears relatively low at the corresponding temperature, which implies that, at a relatively lower temperature (200 °C), the adsorbed CO reacting with the activated water (or surface OH group) to develop the critical intermediate such as COOH is kinetically sluggish (the rate-limiting step), which is confirmed by the following DFT simulation results.…”

Section: Theoretical Calculations/computationalmentioning

confidence: 99%

Atomic-Layer-Deposition Derived Pt subnano Clusters on the (110) Facet of Hexagonal Al₂O₃ Plates: Efficient for Formic Acid Decomposition and Water Gas Shift

Chen

et al. 2022

ACS Catal.

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The Pt subnano clusters dispersed on the (110) facet of regularly shaped hexagonal Al2O3 plates were fabricated via an atomic layer deposition approach. The resulting material contains Pt loading as low as 0.07 wt %; the interfacial structure exhibits nearly full CO conversion for water gas shift reaction at 210 °C, and the turnover frequency (TOF) of CO is as high as 2.1 s–1, outperforming most of the systems reported. The same interfacial structure was also found to be highly active for catalytic decomposition of formic acid (FA), with full FA conversion (with little CO product) and the TOF being 1.02 s–1. Further characterizations together with density functional theory simulations elucidate that the superior catalytic performances are attributed to the unique interfacial structure and the synergism between the small Pt clusters and the Al2O3 (110) substrate, leading to lower energy barriers for the *COOH intermediate formation over the ultrafine Pt ensembles and the hydroxylation over the Al2O3 (110) substrate close to the Pt entities. Both are favorable for the evolution of *COOH intermediate and the reaction between *COOH and neighbor OH species. The current study provides insights into the effectiveness in generating high-performance catalytic material for clean energy production and modulation through precise control of the metal entity dimension and the oxide substrate engineering to achieve specific facet exposure.

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“…In this way, metal particles with controllable particle sizes can be precisely deposited onto the structurally clear oxide support to establish unique metal–oxide interfaces applied for certain catalytic processes and to achieve a structure–performance correlation in depth. This is the major tactic of the present study, and such tactics have been successfully applied for a variety of catalyst systems and reactions in our lab. − …”

Section: Introductionmentioning

confidence: 99%

Atomic Layer Deposition of Pt Fine Clusters over the Structurally Defined SnO₂ Facets for Efficient Formic Acid Decomposition and H₂ Evolution

Chen,

Wu,

et al. 2023

ACS Sustainable Chem. Eng.

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Significant impact of γ-Al2O3 facet structure on the character and performance of surface Co-Mo sulfides for CO removal in H2 fuel via water gas shift

Cited by 6 publications

References 70 publications

Selective Hydrogenation of Polyenes in Biomass-Derived Cardanol over the Trimetallic Ni–Co–Cu Catalyst Supported on Morphologically Controlled Alumina

Selective Hydrogenation of Polyenes in Biomass-Derived Cardanol over the Trimetallic Ni–Co–Cu Catalyst Supported on Morphologically Controlled Alumina

Atomic-Layer-Deposition Derived Pt subnano Clusters on the (110) Facet of Hexagonal Al₂O₃ Plates: Efficient for Formic Acid Decomposition and Water Gas Shift

Atomic Layer Deposition of Pt Fine Clusters over the Structurally Defined SnO₂ Facets for Efficient Formic Acid Decomposition and H₂ Evolution

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Significant impact of γ-Al2O3 facet structure on the character and performance of surface Co-Mo sulfides for CO removal in H2 fuel via water gas shift

Cited by 6 publications

References 70 publications

Selective Hydrogenation of Polyenes in Biomass-Derived Cardanol over the Trimetallic Ni–Co–Cu Catalyst Supported on Morphologically Controlled Alumina

Selective Hydrogenation of Polyenes in Biomass-Derived Cardanol over the Trimetallic Ni–Co–Cu Catalyst Supported on Morphologically Controlled Alumina

Atomic-Layer-Deposition Derived Pt subnano Clusters on the (110) Facet of Hexagonal Al2O3 Plates: Efficient for Formic Acid Decomposition and Water Gas Shift

Atomic Layer Deposition of Pt Fine Clusters over the Structurally Defined SnO2 Facets for Efficient Formic Acid Decomposition and H2 Evolution

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Atomic-Layer-Deposition Derived Pt subnano Clusters on the (110) Facet of Hexagonal Al₂O₃ Plates: Efficient for Formic Acid Decomposition and Water Gas Shift

Atomic Layer Deposition of Pt Fine Clusters over the Structurally Defined SnO₂ Facets for Efficient Formic Acid Decomposition and H₂ Evolution