Synthesis of Vinyl Chloride Monomer over Carbon-Supported Tris-(Triphenylphosphine) Ruthenium Dichloride Catalysts

Li, Xing; Zhang, Haiyang; Man, Baochang; Zhang, Chuanming; Ding, Hui; Dai, Bin; Zhang, Jinli

doi:10.3390/catal8070276

Cited by 11 publications

(4 citation statements)

References 40 publications

(51 reference statements)

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“…The extra peaks at 558.7 and 1430.2 cm −1 could be attributed to Co−P and P−C vibrations, respectively. 40 The FT-IR spectra show an intense band around ∼2356 cm −1 (Figure S2, SI), which could be assigned to the vibrations of double bonds between carbon and nitrogen resulting from conjugation in the polymeric framework, and this similar observation has been identified by Pieczynśka et al 41 The corresponding peak intensity is decreased for Co 3 O 4 @POP and Co x P@POP, which may be due to the interaction between POP support and Co 3 O 4 and Co x P, respectively, in accordance with the previous report by Li et al 42 In another way, this peak could also be attributed to the adsorbed atmospheric CO 2 (or an artifact), which is not under consideration in our present investigation. 43 Electron Microscopy Analysis.…”

Section: ■ Experimental Sectionsupporting

confidence: 90%

Porous Organic Polymer-Driven Evolution of High-Performance Cobalt Phosphide Hybrid Nanosheets as Vanillin Hydrodeoxygenation Catalyst

Shit

Koley

Joseph

et al. 2019

ACS Appl. Mater. Interfaces

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Hydrodeoxygenation (HDO) is a promising route for the upgrading of bio-oils to eco-friendly biofuel produced from lignocellulose. Herein, we report the sequential synthesis of a hybrid nanocatalyst Co x P@POP, where substoichiometric Co x P nanoparticles are distributed in a porous organic polymer (POP) via solid-state phosphidation of the Co 3 O 4 @POP nanohybrid system. We also explored the catalytic activity of the above two nanohybrids toward the HDO of vanillin, a typical compound of lignin-derived bio-oil to 2-methoxy-4-methylphenol, which is a promising future biofuel. The Co x P@POP exhibited superior catalytic activity and selectivity toward desired product with improved stability compared to the Co 3 O 4 @POP. Based on advanced sample characterization results, the extraordinary selectivity of Co x P@POP is attributed to the strong interaction of the cation of the Co x P nanoparticle with the POP matrix and the consequent modifications of the electronic states. Through attenuated total reflectance-infrared spectroscopy, we have also observed different interaction strengths between vanillin and the two catalysts. The decreased catalytic activity of Co 3 O 4 @POP compared to Co x P@POP catalyst could be attributed to the stronger adsorption of vanillin over the Co 3 O 4 @POP catalyst. Also from kinetic investigation, it is clearly demonstrated that the Co 3 O 4 @POP has higher activation energy barrier than the Co x P@POP, which also reflects to the reduction of the overall efficiency of the Co 3 O 4 @POP catalyst. To the best of our knowledge, this is the first approach in POP-encapsulated cobalt phosphide catalyst synthesis and comprehensive study in establishing the structure− activity relationship in significant step-forwarding in promoting biomass refining.

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Section: ■ Experimental Sectionsupporting

confidence: 90%

Porous Organic Polymer-Driven Evolution of High-Performance Cobalt Phosphide Hybrid Nanosheets as Vanillin Hydrodeoxygenation Catalyst

Shit

Koley

Joseph

et al. 2019

ACS Appl. Mater. Interfaces

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“…Finally, the Ru 3p photoelectron lines of Ru 3p 3/2 and Ru 3p 1/2 had values of 464.6 and 486.8 eV, respectively (Figure D). Compared with previous literature, these values align strongly with the presence of Ru 4+ ions and RuO 2 . − This was unexpected as ruthenium was initially added in its Ru 3+ form as ruthenium nitrosyl nitrate, suggesting that it was oxidized in solution to its higher +4 oxidation state. Ruthenium is known to behave in a complex manner; therefore, it is not necessarily unexpected in the acidic medium .…”

Section: Surface Contamination Speciationsupporting

confidence: 81%

Development of a Multi-technique Characterization Portfolio for Stainless Steels Exposed to Magnox Reprocessing Liquors

Barton,

Denman,

Grebennikova

et al. 2023

ACS Omega

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AISI Type 304 stainless steel coupons have been exposed to a simulant aqueous environment representative of the Magnox Reprocessing Plant (MRP) at Sellafield, UK. The experiments were performed for extended time periods (up to 420 days) at elevated temperatures to develop a comprehensive understanding of the extent, nature, and depth of contamination for pipework and vessels in Magnox spent nuclear fuel reprocessing environments. This will inform upcoming decommissioning work which represents a major post-operational challenge. Previous relevant literature has focused on developing fundamental understanding of contamination mechanisms of stainless steels in simplistic, single-element systems, which lack elements of industrial relevance. Contamination behavior is expected to be drastically different in these more complex environments. A characterization portfolio has been developed to enable detailed assessment of corrosion and contamination behavior in acidic reprocessing environments. Solution, surface, and depth analysis determined that uptake was dominated by the elements present in highest concentrations within the environment, namely, Mg, Nd, and Cs. Most contaminants were incorporated into a relatively thin surface oxide layer (<100 nm) in metal oxide form, although there were some exceptions (Cs and Sr). Grain boundary etching was present despite very low corrosion rates (3 μm year −1 ). As a result of this lack of corrosion, diffusion of contaminants beyond the immediate surface (10− 20 nm) did not occur, evidenced through depth profiling. As a result of these findings, surface-based decontamination techniques minimizing excess secondary waste generation can be further developed in order to reduce the environmental and economic burden associated with decommissioning activities.

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“…Such stable catalysis of Ru–NC@MIL in terms of the catalytic time (150 h) and deactivation rate (0.009%/h) was evidently superior in the present study to that of other recently reported Ru-based catalysts under the same reaction conditions ( T = 180 °C, and GHSV (C 2 H 2 ) = 180 h –1 ) (Figure d and Table S8). ,,− …”

Section: Resultsmentioning

confidence: 99%

Metal–Organic Frameworks Encaged Ru Single Atoms for Rapid Acetylene Harvest and Activation in Hydrochlorination

Fan

Liu

Sun

et al. 2023

ACS Appl. Mater. Interfaces

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Ruthenium (Ru)-based catalysts have been candidates in hydrochlorination for vinyl chloride monomer (VCM) production, yet they are limited by efficient acetylene (C2H2) utilization. The strong adsorption performance of HCl can deactivate Ru active sites which resulted in weak C2H2 adsorption and slow activation kinetics. Herein, we designed a channel that employed metal–organic framework (MOF)-encaged Ru single atoms to achieve rapid adsorption and activation of C2H2. Low-Ru (∼0.5 wt %) single-atom catalysts (named Ru–NC@MIL) were assembled by hydrogen-bonding nanotraps (the H–CC–Hδ+···Oδ− interactions between C2H2 and carboxylate groups/furan rings). Results confirmed that C2H2 could easily enter the encapsulation channels in an optimal mode perpendicular to the channel with a potential energy of 42.3 kJ/mol. The harvested C2H2 molecules can be quickly passed to Ru–N4 active sites for activation by stretching the length of carbon–carbon triple bonds (CC) to 1.212 Å. Such a strategy guaranteed >99% C2H2 conversion efficiency and >99% VCM selectivity. Moreover, a stable long-term (>150 h) catalysis with high efficiency (∼0.85 kgvcm/h/kgcat.) and a low deactivation constant (0.001 h–1) was also achieved. This work provides an innovative strategy for precise C2H2 adsorption and activation and guidance for designing multi-functional Ru-based catalysts.

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Synthesis of Vinyl Chloride Monomer over Carbon-Supported Tris-(Triphenylphosphine) Ruthenium Dichloride Catalysts

Cited by 11 publications

References 40 publications

Porous Organic Polymer-Driven Evolution of High-Performance Cobalt Phosphide Hybrid Nanosheets as Vanillin Hydrodeoxygenation Catalyst

Porous Organic Polymer-Driven Evolution of High-Performance Cobalt Phosphide Hybrid Nanosheets as Vanillin Hydrodeoxygenation Catalyst

Development of a Multi-technique Characterization Portfolio for Stainless Steels Exposed to Magnox Reprocessing Liquors

Metal–Organic Frameworks Encaged Ru Single Atoms for Rapid Acetylene Harvest and Activation in Hydrochlorination

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