Tuning the Selectivity of Catalytic Carbon Dioxide Hydrogenation over Iridium/Cerium Oxide Catalysts with a Strong Metal–Support Interaction

Li, Siwei; Xü, Yao; Chen, Yifu; Li, Weizhen; Lin, Lili; Li, Mengzhu; Deng, Yuchen; Wang, Xiaoping; Ge, Binghui; Yang, Ce; Yao, Siyu; Xie, Jinglin; Li, Yongwang; Liu, Xi; Ma, Ding

doi:10.1002/anie.201705002

Cited by 405 publications

(296 citation statements)

References 47 publications

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“…Recently, Li et al. reported that a strong metal–support interaction between Ir and CeO 2 modulated the chemical state of metal species and changed the selectivity for CO 2 hydrogenation significantly . Similarly, in our case, it is very likely that the metal–support interaction between Ni and the surrounding silica changed the electron density of the Ni surface and consequent CO adsorption behavior.…”

Section: Resultssupporting

confidence: 63%

Sandwich‐Like Silica@Ni@Silica Multicore–Shell Catalyst for the Low‐Temperature Dry Reforming of Methane: Confinement Effect Against Carbon Formation

2017

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We synthesize a new sandwich‐like silica@Ni@silica multicore–shell catalyst. Firstly, Ni phyllosilicate (NiPS) is supported on silica nanospheres by a simple ammonia evaporation method. Then NiPS is coated with a layer of mesoporous silica to obtain a core–shell NiPS@silica structure by the hydrolysis of tetraethylorthosilicate (TEOS). The thickness of the shell can be tuned by varying the amount of TEOS. After calcination and H2 reduction at high temperature, multiple small Ni nanoparticles (≈6 nm) are generated and supported on the inner silica core but also encapsulated within the outer mesoporous silica shell. This silica@Ni@silica multicore–shell catalyst shows a high and stable conversion (≈60 %, gas hourly space velocity=60 000 mL h−1 gcat−1) for the dry reforming of methane (DRM) at 600 °C, whereas pristine NiPS deactivates quickly because of heavy carbon formation. We investigated the spent catalysts by using thermogravimetric analysis and TEM and found that there is almost no carbon formation for this new multicore–shell catalyst. Compared with a conventional Ni@silica core–shell catalyst, our multicore–shell catalyst is much easier to synthesize and the process does not require any toxic organic solvents. We believe that this strategy to make a multicore–shell catalyst can be applied to more nanomaterials and extended to other catalytic reactions besides DRM.

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Section: Resultssupporting

confidence: 63%

Sandwich‐Like Silica@Ni@Silica Multicore–Shell Catalyst for the Low‐Temperature Dry Reforming of Methane: Confinement Effect Against Carbon Formation

2017

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“…Zeolite (HY) behaves as the effective active sites to catalyze the dehydration of fructose to HMF, subsequently, the FOL is selectively produced over Pd‐catalysts under mild reaction conditions. In addition, since the first example associated with strong metal support interaction (SMSI) was reported by S. J. Tauster at 1978, the SMSI is frequently viewed as a crucial issue for supported‐metal catalysts, even the SMSI is identified as a decisive factor for the distribution of products . Interestingly, in the presented work, the SMSI was also observed and it could govern the direction of selectivity.…”

Section: Introductionsupporting

confidence: 51%

One‐step Conversion of Fructose to Furfuryl Alcohol in a Continuous Fixed‐bed Reactor: The Important Role of Supports

et al. 2019

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One‐step catalytic conversion of fructose to furfuryl alcohol (FOL) is not only a challenge task but also to open a new pathway for conversion of hexose into useful chemicals. The favorable yield (41.6 %) of FOL can be directly obtained from fructose over the tandem of HY zeolite and Pd/Al2O3. However, the Pd/montmorillonite (Pd/MMT) was deactivated for production of FOL. The proportion of available Pd active sites (i. e. facets, corners and edges) vary with different supports, and the strong metal support interaction (SMSI) plays the pivotal role on the catalytic performance. For Al2O3 support, exposure of Pd (111) plane allows the hydroxymethylfurfural (HMF) to bind on the Pd (111) surface via planar arrangement. In this stance, the aldehyde group of HMF is readily eliminated by decarbonylation. Conversely, for Pd/MMT, the decarbonylation is completely inhibited due to the HMF absorbs on corner sites in perpendicular orientation. The XPS studies indicate that the density electron of Pd nanoparticles (NPs) could be manipulated by various supports, and the electron‐donating effect of Al2O3 was observed. The collaborative effects between available sites and density electron of Pd are observed with respect to the different binding modes of HMF on the surface of Pd. The electronegative Pd NPs facilitate the decarbonylation of HMF as a consequence of the different adsorption strength between furan ring and aldehyde group.

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“…The high‐resolution C 1s and Ru 3d spectrum (Figure g) can be deconvoluted into five individual peaks, which are attributed to C−C (284.7 eV), C−N (285.8 eV), C=O (288.5 eV), Ru 3d 5/2 (280.7 eV) and Ru 3d 3/2 (283.0 eV), respectively. Additionally, two peaks at 462.3 and 484.7 eV for Ru 3p (Figure h) are attributed to Ru 3p 3/2 and Ru 3p 1/2 (Ru 0 ), respectively …”

Section: Figurementioning

confidence: 97%

Synthesis of Ru‐Doped VN by a Soft‐Urea Pathway as an Efficient Catalyst for Hydrogen Evolution

et al. 2020

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Unraveling the effect of metal doping on the intrinsic activity of metal nitride remains a grand challenge. Herein, Ru (Rh)‐doped vanadium nitride are successfully synthesized via a simple soft‐urea pathway. In comparison, the Ru‐doped VN electrocatalyst exhibits much better HER performance than Rh‐doped VN electrocatalysts. The optimal Ru‐VN catalyst delivers a low overpotential of 134 (144) mV at current density of 10 mA cm−2, and a low Tafel slope of 35 (73) mV dec−1 in acidic (alkaline) condition. Such excellent performance can be attributed to the unique synergetic effect between Ru and VN. Moreover, moderate Ru dopant can effectively promote the HER kinetics of VN, resulting in mechanism transformation of hydrogen evolution from Volmer‐Heyrovsky to Volmer‐Tafel route, especially in acidic condition. This simple and facile strategy can be utilized to fabricate a series of Ru‐doped nitrides, which can be applied in energy conversion fields.

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Tuning the Selectivity of Catalytic Carbon Dioxide Hydrogenation over Iridium/Cerium Oxide Catalysts with a Strong Metal–Support Interaction

Cited by 405 publications

References 47 publications

Sandwich‐Like Silica@Ni@Silica Multicore–Shell Catalyst for the Low‐Temperature Dry Reforming of Methane: Confinement Effect Against Carbon Formation

Sandwich‐Like Silica@Ni@Silica Multicore–Shell Catalyst for the Low‐Temperature Dry Reforming of Methane: Confinement Effect Against Carbon Formation

One‐step Conversion of Fructose to Furfuryl Alcohol in a Continuous Fixed‐bed Reactor: The Important Role of Supports

Synthesis of Ru‐Doped VN by a Soft‐Urea Pathway as an Efficient Catalyst for Hydrogen Evolution

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