Hydrochlorination of acetylene catalyzed by an activated carbon supported chlorotriphenylphosphine gold complex

Dong, Yanzhao; Li, Wei; Yan, Zheng; Zhang, Jinli

doi:10.1039/c6cy01241h

Cited by 40 publications

(23 citation statements)

References 60 publications

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“…The Au 4 f spectrum recorded for each catalyst involved three kinds of species -Au 0 , Au + , and Au 3 + at ca. 84.2 eV, 85.1 eV, and 86.7 eV respectively [48,57] (Figure S2). Interestingly, apart from Au 0 , only the peak of Au + appears in the fresh AuÀ L/AC catalysts after the introduction of ligands, which is in line with the best ratio of 1 : 1 between the Au and the ligand.…”

Section: Valence Changes Of the Active Speciesmentioning

confidence: 99%

“…[4,[36][37][38][39] The coking deposition and the agglomeration or the reduction of active species are the main reasons for the deactivation of Au-based catalyst, which have been briefly introduced in the previous literatures. [3,40] Consequently, researchers strive to design and regulate the Aubased catalyst by modifying the carrier, [11,41,42,43,44] adding additives [9,40,45,46] and ligand coordination, [47,48] so as to inhibit the deactivation of Au-based catalysts, and enhance the activity and stability. Considering that high-valence state gold species are easily reduced by the carrier or acetylene, researchers sought different ligands and prepared precursors containing high-valence state gold by coordination between the ligands and the gold cations to improve the catalytic performance of gold-based catalysts.…”

Section: Introductionmentioning

confidence: 99%

“…This proved that ligand coordination can effectively retard the reduction of Au 3 + due to the increase in the redox potential of the Au species by complexation with the Schiff base. [48,49] In our previous work, chlorotriphenylphosphine gold (AuPPh 3 Cl) was synthesized using chloroauric acid and triphenylphosphine (TPP) as precursors. This was followed by the preparation of the AuPPh 3 Cl/AC catalyst for acetylene hydrochlorination.…”

Section: Introductionmentioning

confidence: 99%

“…It also demonstrated that the TPP likely improves the stability of the Au + species and retards the reduction of Au n + (n = 1, 3) species to Au 0 species, thereby improving the catalytic activity and the stability of the AuPPh 3 Cl/AC catalyst. [48] G. J. Hutchings et al [50] designed a Na 3 Au(S 2 O 3 ) 2 precursor through ligand coordination, and prepared an Au-based catalyst with an Au loading of 0.1 wt %. The results indicated that the sulfurcontaining Au complex could be formed in situ by adding the scontaining precursor to HAuCl 4 solution before being deposited on AC.…”

Section: Introductionmentioning

confidence: 99%

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Hydrochlorination of Acetylene Over the Activated‐Carbon‐Supported Au Catalysts Modified by N−P−O‐Containing Ligand

Zhang

et al. 2019

ChemCatChem

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Etidronic acid (HEDP) and Nitrilotri(methylphosphonic acid) (ATMP) were selected as heteroatoms-containing ligands to modify Au catalysts for acetylene hydrochlorination. Results from several analytical methods reveal an optimal mole ratio of Au/ligand (L) of 1 : 1, with obvious increments over the Au 1 -L 1 / AC catalyst. The coordination between the Au and the heteroatoms, especially the collocative presence of N, P, and O promoted electron transfer from the heteroatoms to the Au n + and increased the density of the electron cloud around active centers. This stabilized the Au n + and increased the difficulty in the reduction of Au species, and re-oxidized the Au 0 to active Au n + species. Moreover, the coordination inhibited the migration of active components. The increased density of the electron cloud around active centers also weakens the adsorption capacity for C 2 H 2 and strengthens the adsorption ability for HCl of the catalysts, which is conductive for constructing the micro-environment favorable to the reaction. DFT calculations proved the stabilization effect of the heteroatoms-containing ligands, and the energy sequence of the transition states supported the experimental results.

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Section: Valence Changes Of the Active Speciesmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Hydrochlorination of Acetylene Over the Activated‐Carbon‐Supported Au Catalysts Modified by N−P−O‐Containing Ligand

Zhang

et al. 2019

ChemCatChem

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“…When the temperature exceeds 360 • C, there is a rapid mass loss for all Ru-based catalysts owing to the burning of activated carbon. The amount of coke deposition is determined together by the mass loss of the fresh and the used catalysts in the temperature range of 150-360 • C and calculated using our previous method [33]. For the fresh and used RuCl 3 /AC catalysts, in the range of 150-360 • C, the mass losses are 2.7% and 16.4%, respectively, ( Table S1).…”

Section: Catalyst Texture Propertiesmentioning

confidence: 99%

Hydrochlorination of Acetylene Catalyzed by an Activated Carbon-Supported Ammonium Hexachlororuthenate Complex

Gao

Zhang

et al. 2017

Catalysts

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Ammonium hexachlororuthenate ((NH 4 ) 2 RuCl 6 ) complex was used as a catalyst precursor and coconut activated carbon (AC) was used as the support in the preparation process of the Ru-based catalyst. (NH 4 ) 2 RuCl 6 /AC catalyst was prepared via an incipient wetness impregnation method and assessed in an acetylene hydrochlorination reaction. Meanwhile, the (NH 4 ) 2 RuCl 6 /AC catalyst was analyzed with low-temperature N 2 adsorption/desorption, thermogravimetry (TG), transmission electron microscopy (TEM), temperature programmed reduction (TPR), X-ray photoelectron spectra (XPS), and temperature programmed desorption (TPD) techniques. Catalytic performance test results show that the (NH 4 ) 2 RuCl 6 /AC catalyst exhibits a superior catalytic activity with the highest acetylene conversion of 90.5% under the conditions of 170 • C and an acetylene gas hourly space velocity of 180 h −1 . The characterization results illustrate that the presence of the NH 4 + cation can inhibit coke deposition as well as the agglomeration of ruthenium particles, and it can also enhance the adsorption ability for reactant HCl, hence improving the catalytic activity and stability.

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Pyrrolidone ligand improved Cu‐based catalysts with high performance for acetylene hydrochlorination

Han

Wang

et al. 2020

Applied Organom Chemis

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A series of Cu-pyrrolidone/spherical activated carbon (SAC) catalysts were prepared via a simple incipient wetness impregnation method and then assessed in acetylene hydrochlorination, and the catalytic evaluation result indicated that the 1-methyl-2-pyrrolidinone (NMP) ligand was found to be the most effective one to significantly improve the activity and stability of Cu catalyst. The catalyst with the optimal molar ratio of NMP/Cu = 0.25 showed 94.2% acetylene conversion at 180 C and an acetylene gas hourly space velocity of 180 h −1. Moreover, the acetylene conversion of Cu-0.25NMP/SAC remained stable over 99.1% for about 220 h under the industrial condition. Transmission electron microscopy (TEM) analyses proved that NMP ligand improved the dispersion of Cu species. In addition, hydrogen temperature-programmed reduction (H 2-TPR), X-ray photoelectron spectra (XPS), thermogravimetric analysis (TGA), and Brunner-Emmet-Teller (BET) indicated that the additive of NMP was preferential to stabilize the catalytic active Cu + and Cu 2+ species and inhibit the reduction of Cu α+ to Cu 0 during the preparation process and reaction, hence restraining the coke deposition. Furthermore, the steady coordination structure between Cu and NMP was confirmed by Fourier-transform infrared spectra (FT-IR) and Raman combining with density functional theory (DFT) calculation, which could effectively lower the adsorption energy of catalyst for C 2 H 2 and inhibit the serious carbon deposition caused by excessive acetylene self-accumulation. Our findings suggest that the efficient, well-stabilized cost-effective, and environmentally friendly Cu catalyst has great potential in acetylene hydrochlorination.

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Hydrochlorination of acetylene catalyzed by an activated carbon supported chlorotriphenylphosphine gold complex

Abstract: The presence of triphenylphosphine ligand inhibits the agglomeration of gold particles during acetylene hydrochlorination, thereby improving the catalytic performance of the Au-based catalyst.

Cited by 40 publications

References 60 publications

Hydrochlorination of Acetylene Over the Activated‐Carbon‐Supported Au Catalysts Modified by N−P−O‐Containing Ligand

Hydrochlorination of Acetylene Over the Activated‐Carbon‐Supported Au Catalysts Modified by N−P−O‐Containing Ligand

Hydrochlorination of Acetylene Catalyzed by an Activated Carbon-Supported Ammonium Hexachlororuthenate Complex

Pyrrolidone ligand improved Cu‐based catalysts with high performance for acetylene hydrochlorination

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