Molybdenum disulfide promoted co-catalyzed alkoxycarbonylation

Zheng, Zhaohui; Zhou, Hao; Deng, Li; Jia, Xiaofei; Li, Yuehui

doi:10.1016/j.jcat.2024.115349

Cited by 3 publications

(3 citation statements)

References 38 publications

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“…Traditionally, Co 2 (CO) 8 is quite unstable, and its synthesis requires either harsh reaction conditions (i.e., 140-230 • C, 10-70 MPa) or stoichiometric reducing reagents (such as metal powders, NaBH 4 , or Na 2 S 2 SO 3 ) or phosphine oxide promoters. Li and coworkers recently reported that Co 2 (CO) 8 could be formed in situ from Co/MoS 2 under conditions of 6 MPa CO, 140 • C, and 15 h, and MoS 2 was claimed to be critical for this process [28]. This work demonstrated that when using conventional SiO 2 as a support material, Co 2 (CO) 8 could also be generated in situ under conditions of 4 MPa CO, 1 MPa H 2 , 160 • C, and 1 h, thus providing a facile, straightforward approach to prepare Co 2 (CO) 8 for Reppe carbonylation reactions.…”

Section: Resultsmentioning

confidence: 99%

“…Cobalt is also the metal of choice for Reppe carbonylation reactions due to its earth abundance and high catalytic activity [25][26][27]. Pyridine-promoted cobalt carbonyls demonstrated high efficiency in converting butadiene to adipic acid in a pilot-scale process developed by BASF [28,29]. Cobalt carbonyls were also competent catalysts in the alkoxycarbonylation reactions of alkenes [30].…”

Section: Introductionmentioning

confidence: 99%

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Co/SiO2 Catalyst for Methoxycarbonylation of Acetylene: On Catalytic Performance and Active Species

Wang,

Cao,

Zhang

et al. 2024

Molecules

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Reppe carbonylation of acetylene is an atom-economic and non-petroleum approach to synthesize acrylic acid and acrylate esters, which are key intermediates in the textile, leather finishing, and polymer industries. In the present work, a noble metal-free Co@SiO2 catalyst was prepared and evaluated in the methoxycarbonylation reaction of acetylene. It was discovered that pretreatment of the catalyst by different reductants (i.e., C2H2, CO, H2, and syngas) greatly improved the catalytic activity, of which Co/SiO2-H2 demonstrated the best performance under conditions of 160 °C, 0.05 MPa C2H2, 4 MPa CO, and 1 h, affording a production rate of 4.38 gMA+MP gcat−1 h−1 for methyl acrylate (MA) and methyl propionate (MP) and 0.91 gDMS gcat−1 h−1 for dimethyl succinate (DMS), respectively. Transmission electron microscopy (TEM), X-ray diffraction (XRD), and diffuse reflectance infrared Fourier transform spectra of CO adsorption (CO-DRIFTS) measurements revealed that an H2 reduction decreased the size of the Co nanoparticles and promoted the formation of hollow architectures, leading to an increase in the metal surface area and CO adsorption on the catalyst. The hot filtration experiment confirmed that Co2(CO)8 was generated in situ during the reaction or at the pre-activation stage, which served as the genuine active species. Our work provides a facile and convenient approach to the in situ synthetization of Co2(CO)8 for a Reppe carbonylation reaction.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Co/SiO2 Catalyst for Methoxycarbonylation of Acetylene: On Catalytic Performance and Active Species

Wang,

Cao,

Zhang

et al. 2024

Molecules

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“…The hot filtration experiment was carried out on the homemade apparatus comprising two 25 mL stainless steel autoclaves connected together, with autoclave-1 being equipped with a filter tube (Figure S1). 54 100 mg of Rh 1 @S-1, 1.48 mL of dodecane, 16 mL of cyclohexane with 1.28 mL of 1-hexene (0.65 mol/L) under low alkene conditions, or 16 mL of pure 1-hexene under pure alkene conditions, were introduced in autoclave-1. Both autoclaves were then purged with N 2 gas three times.…”

Section: Catalytic Activity Measurementmentioning

confidence: 99%

Suppressing Metal Leaching and Sintering in Hydroformylation Reaction by Modulating the Coordination of Rh Single Atoms with Reactants

Yu,

Zhang,

Zhang

et al. 2024

J. Am. Chem. Soc.

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Hydroformylation reaction is one of the largest homogeneously catalyzed industrial processes yet suffers from difficulty and high cost in catalyst separation and recovery. Heterogeneous single-atom catalysts (SACs), on the other hand, have emerged as a promising alternative due to their high initial activity and reasonable regioselectivity. Nevertheless, the stability of SACs against metal aggregation and leaching during the reaction has rarely been addressed. Herein, we elucidate the mechanism of Rh aggregation and leaching by investigating the structural evolution of Rh 1 @silicalite-1 SAC in response to different adsorbates (CO, H 2 , alkene, and aldehydes) by using diffuse reflectance infrared Fourier transform spectroscopy, X-ray adsorption fine structure, and scanning transmission electron microscopy techniques and kinetic studies. It is discovered that the aggregation and leaching of Rh are induced by the strong adsorption of CO and aldehydes on Rh, as well as the reduction of Rh 3+ by CO/ H 2 which weakens the binding of Rh with support. In contrast, alkene effectively counteracts this effect by the competitive adsorption on Rh atoms with CO/aldehyde, and the disintegration of Rh clusters. Based on these results, we propose a strategy to conduct the reaction under conditions of high alkene concentration, which proves to be able to stabilize Rh single atom against aggregation and/or leaching for more than 100 h time-on-stream.

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Recycling Cobalt in Spent Lithium-Ion Batteries to Design Two-Dimensional Porous CoO_x/CoN_x Nanosheets for Full Water Splitting and Nonenzymatic Glucose Detection

Wang,

Li,

Cao

et al. 2024

ACS Appl. Nano Mater.

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Enhancing catalytic efficiency, achieving controlled synthesis, and lowering production costs are crucial for promoting the use of cobalt oxide (CoO x )/cobalt nitride (CoN x ) composites in full water splitting and electrochemical sensing. In this study, a three-dimensional (3D) hierarchically porous material composed of numerous two-dimensional (2D) porous CoO x /CoN x nanosheets (denoted as CoO x /CoN x NSs) was synthesized by using cobalt oxalates (COs) recycled from spent lithium-ion batteries. In a 1.0 M KOH solution, the 2D porous CoO x /CoN x NSs exhibited higher oxygen evolution reaction (OER) electrocatalytic activity than commercial ruthenium oxide (RuO 2 ). Meanwhile, the CoO x / CoN x NSs exhibited a slightly lower hydrogen evolution reaction (HER) electrocatalytic activity than 20 wt % platinum/carbon (Pt/ C). Moreover, the CoO x /CoN x NS-based full water-splitting electrolyzer achieved a current density of 10 mA cm −2 at 1.562 V, which was 49 mV more positive than the 1.489 V of the Pt/C||RuO 2 benchmark. Furthermore, the 2D porous CoO x /CoN x NSs featured significantly higher HER, OER, and full water-splitting catalytic stability than Pt/C/RuO 2 . Moreover, the CoO x /CoN x NSbased nonenzymatic electrochemical sensor exhibited advanced glucose detection performance. Particularly, the sensor had a wide linear range of 1.0−10.5 mM), a low detection limit of 5.0 μM), and a fast response time of 0.6 s. The 2D porous CoO x /CoN x NSs exhibited excellent catalytic activity owing to their 3D hierarchically porous architectures, large surface area, good conductivity, uniformly dispersed active sites, and synergistic effects of CoN x and CoO. This study presents an advanced model for recycling Co metal from spent devices and designing advanced Co-based electrocatalysts for water splitting and electrochemical sensing.

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Molybdenum disulfide promoted co-catalyzed alkoxycarbonylation

Cited by 3 publications

References 38 publications

Co/SiO2 Catalyst for Methoxycarbonylation of Acetylene: On Catalytic Performance and Active Species

Co/SiO2 Catalyst for Methoxycarbonylation of Acetylene: On Catalytic Performance and Active Species

Suppressing Metal Leaching and Sintering in Hydroformylation Reaction by Modulating the Coordination of Rh Single Atoms with Reactants

Recycling Cobalt in Spent Lithium-Ion Batteries to Design Two-Dimensional Porous CoO_x/CoN_x Nanosheets for Full Water Splitting and Nonenzymatic Glucose Detection

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Molybdenum disulfide promoted co-catalyzed alkoxycarbonylation

Cited by 3 publications

References 38 publications

Co/SiO2 Catalyst for Methoxycarbonylation of Acetylene: On Catalytic Performance and Active Species

Co/SiO2 Catalyst for Methoxycarbonylation of Acetylene: On Catalytic Performance and Active Species

Suppressing Metal Leaching and Sintering in Hydroformylation Reaction by Modulating the Coordination of Rh Single Atoms with Reactants

Recycling Cobalt in Spent Lithium-Ion Batteries to Design Two-Dimensional Porous CoOx/CoNx Nanosheets for Full Water Splitting and Nonenzymatic Glucose Detection

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About

Recycling Cobalt in Spent Lithium-Ion Batteries to Design Two-Dimensional Porous CoO_x/CoN_x Nanosheets for Full Water Splitting and Nonenzymatic Glucose Detection