Carbon-supported ruthenium catalysts prepared by a coordination strategy for acetylene hydrochlorination

Wang, Xiaolong; Lan, Guojun; Cheng, Zaizhe; Han, Wenfeng; Tang, Haodong; Liu, Huazhang; Liu, Ying

doi:10.1016/s1872-2067(20)63616-6

Cited by 28 publications

(11 citation statements)

References 44 publications

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“…This is understandable NH 3 as a probe molecule, the alkalinity is stronger than that of acetylene, so it is impossible to distinguish the acid adsorption sites of acetylene with different acid strengths. 8 The areas of the NH 3 desorption peak are in the order of RuCl 3 /AC-O > RuCl 3 /AC > RuCl 3 /AC-D (Fig. S8 † shows that the interference of water desorption in the catalyst structure has been eliminated).…”

Section: 2mentioning

confidence: 98%

“…Our previous research shows that the catalytic activity of the ruthenium catalyst for acetylene hydrochlorination is positively correlated with the electron density of the ruthenium catalyst. 8 Regrettably, there is currently no correlation between the electron density and catalytic stability of ruthenium catalysts. Thus, the relationship between the deactivation rate, coke deposition and the acidity of the ruthenium catalyst was investigated.…”

Section: The Catalytic Performance Of Ruthenium Catalysts For Acetylene Hydrochlorinationmentioning

confidence: 99%

“…[4][5][6][7] In our previous work, we regulated the electronic structure of ruthenium ions by a coordination strategy and found that the turnover frequencies (TOFs) and apparent activation energies for acetylene hydrochlorination are positively correlated with the electron density of ruthenium ions. 8 As is known, the adsorption behavior of reactants is greatly affected by the electronic structure of metal ions for supported catalysts, which greatly affects the catalytic performance. [9][10][11] Thus, it is an effective strategy to regulate the electronic structure of metal ions to obtain catalysts with high catalytic performance.…”

Section: Introductionmentioning

confidence: 99%

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The reaction mechanism of acetylene hydrochlorination on defective carbon supported ruthenium catalysts identified by DFT calculations and experimental approaches

Wang

Fan

Lan

et al. 2022

Inorg. Chem. Front.

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Section: 2mentioning

confidence: 98%

Section: The Catalytic Performance Of Ruthenium Catalysts For Acetylene Hydrochlorinationmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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The reaction mechanism of acetylene hydrochlorination on defective carbon supported ruthenium catalysts identified by DFT calculations and experimental approaches

Wang

Fan

Lan

et al. 2022

Inorg. Chem. Front.

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“…Therefore, the Minamata Convention on Mercury enlightened the people on the necessity of considering green and efficient catalysts as alternatives to Hg-based ones for the hydrochlorination of acetylene. [2] Thus, many metal-based catalysts, including Au, [3] Ru, [4] Pd, [5] Cu, [6] Sn, [7] Bi, [8] had been investigated. Further, to improve their performances, it was overwhelmingly paramount to probe the catalytic and deactivation mechanisms of these catalysts.…”

Section: Introductionmentioning

confidence: 99%

Effect of the Transforming Ag into an Active Species (Silver Chloride) for the Acetylene Hydrochlorination

Liu

Song

et al. 2021

ChemCatChem

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Effective approaches are desired to improve catalytic performances for the hydrochlorination of acetylene. Crucially, the systematic explorations of catalytic and deactivation mechanisms are prerequisites to the implementation of such approaches. Ag has been scarcely researched for acetylene hydrochlorination reaction because it is easily poisoned by Cl, which inactivates it. However, this challenge must be further verified.Here, the active species and causes of the deactivation of Ag/ activated carbon (AC) were discussed in detail. The results indicated that Ag/AC exhibited excellent catalytic performance in the acetylene hydrochlorination. Specifically, X-ray photoelectron spectroscopy (XPS) analysis revealed that AgCl was the main active site, which was almost transformed from Ag 0 after the activation with HCl for 0.5 h. Moreover, inductively coupled plasma optical emission spectrometer (ICP-OES) and transmission electron microscopy (TEM) results confirmed that the deactivation of the catalyst was justified by the loss of Ag and particle aggregation. Thus, the conversion of acetylene of the small-sized AgCl nanoparticles were significantly enhanced, and these inhibited the agglomeration of the particles, thereby further verifying that AgCl was the active site. This perspective offered a suitable insight for the subsequent research on Agbased catalysts.

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“…Although there have been many studies on phosphorus doping, it has not been investigated that which of the different phosphorus species produced during the preparation process can be the most suitable anchoring sites for metal coordination [31][32][33][34][35][36] to play a key role in acetylene hydrochlorination and how it interacts with copper species. In order to solve this problem, in this study, non-toxic and low-cost 1hydroxyethylidene-1,1-diphosphonic acid (HEDP) is used as phosphorus source to prepare copper catalysts supported on phosphorus-doped activated carbon calcined at different temperatures.…”

Section: Introductionmentioning

confidence: 99%

Isolated Single-Atomic Cu Catalyst Supported on P-doped Carbon for Hydrochlorination of Acetylene

Wang

Jiang

Tang

et al. 2021

Preprint

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As an environmentally friendly non-mercury catalyst for the hydrochlorination of acetylene, Cu-based catalysts have always attracted attention. In this study, a series of phosphorus-doped Cu-based catalysts supported on activated carbon were prepared by the wet impregnation method, the difference of them is that the calcination temperature of phosphorus-doped carrier is 200 ℃, 400 ℃, 600 ℃ and 800 ℃ respectively. In the test conditions of T = 150℃, GHSV(C2H2) = 90 h− 1 and V(HCl): V(C2H2) = 1.2, the highest acetylene conversion was 83.1%. The type of phosphorus configuration and the distribution on the surface of the carrier can be adjusted by changing the calcination temperature. Among the different phosphorus species formed by the phosphorus doping treatment at different temperatures, the P-C bond formed after the phosphorus element is incorporated into the carbon lattice also accounts for an increasing proportion with the increase of the calcination temperature,which is accompanied by a higher and higher acetylene conversion. It can be seen that the P-C bond plays a key role in the acetylene hydrochlorination reaction in this system. Meanwhile, Cu2+ was identified as the main active component in the catalyst by XPS. The representative HAADF-STEM image shows isolated copper species, confirming that the single-center copper species supported on the carbon support is the active center of the acetylene hydrochlorination reaction. The coordination structure formed by the interaction between the P-C bond and the atomically dispersed Cu2+ species is an effective and stable active site in the reaction. Density functional theory calculations indicate that the reaction is proposed to proceed according to the Langmuir-Hinshelwood (L-H) mechanism. This work is the first to identify which phosphorus species plays a role in the hydrochlorination of acetylene, which may provide some ideas for the design and optimization of phosphorus doping catalysts in the future.

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Carbon-supported ruthenium catalysts prepared by a coordination strategy for acetylene hydrochlorination

Cited by 28 publications

References 44 publications

The reaction mechanism of acetylene hydrochlorination on defective carbon supported ruthenium catalysts identified by DFT calculations and experimental approaches

The reaction mechanism of acetylene hydrochlorination on defective carbon supported ruthenium catalysts identified by DFT calculations and experimental approaches

Effect of the Transforming Ag into an Active Species (Silver Chloride) for the Acetylene Hydrochlorination

Isolated Single-Atomic Cu Catalyst Supported on P-doped Carbon for Hydrochlorination of Acetylene

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