Novel heterogeneous Rh-incorporated graphitic-carbon nitride for liquid-phase carbonylation of methanol to acetic acid

Nam, Ji Su; Kim, A. Rong; Kim, Da Mi; Chang, Tae‐Sun; Kim, Beom Sik; Bae, Jong Wook

doi:10.1016/j.catcom.2017.06.007

Cited by 28 publications

(17 citation statements)

References 22 publications

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“…Acetic acid is an organic acid containing one carboxylic group with pKa = 4.76. It is largely produced by methanol carbonylation [27], and the price is comparable with that of mineral acids, making it attractive for usage as a leaching agent. In the work of Zanonato et al [28], it was shown that Nd3+ forms at least successive mononuclear complexes according to the following equilibrium:…”

Section: Introductionmentioning

confidence: 99%

Leaching and Recovery of Rare-Earth Elements from Neodymium Magnet Waste Using Organic Acids

Gergorić

Ravaux²,

Steenari

et al. 2018

Metals

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Over the last decade, rare-earth elements (REEs) have become critical in the European Union (EU) in terms of supply risk, and they remain critical to this day. End-of-life electronic scrap (e-scrap) recycling can provide a partial solution to the supply of REEs in the EU. One such product is end-of-life neodymium (NdFeB) magnets, which can be a feasible source of Nd, Dy, and Pr. REEs are normally leached out of NdFeB magnet waste using strong mineral acids, which can have an adverse impact on the environment in case of accidental release. Organic acids can be a solution to this problem due to easier handling, degradability, and less poisonous gas evolution during leaching. However, the literature on leaching NdFeB magnets waste with organic acids is very scarce and poorly investigated. This paper investigates the recovery of Nd, Pr, and Dy from NdFeB magnets waste powder using leaching and solvent extraction. The goal was to determine potential selectivity between the recovery of REEs and other impurities in the material. Citric acid and acetic acid were used as leaching agents, while di-(2-ethylhexyl) phosphoric acid (D2EHPA) was used for preliminary solvent extraction tests. The highest leaching efficiencies were achieved with 1 mol/L citric acid (where almost 100% of the REEs were leached after 24 h) and 1 mol/L acetic acid (where >95% of the REEs were leached). Fe and Co—two major impurities—were co-leached into the solution, and no leaching selectivity was achieved between the impurities and the REEs. The solvent extraction experiments with D2EHPA in Solvent 70 on 1 mol/L leachates of both acetic acid and citric acid showed much higher affinity for Nd than Fe, with better extraction properties observed in acetic acid leachate. The results showed that acetic acid and citric acid are feasible for the recovery of REEs out of NdFeB waste under certain conditions.

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Section: Introductionmentioning

confidence: 99%

Leaching and Recovery of Rare-Earth Elements from Neodymium Magnet Waste Using Organic Acids

Gergorić

Ravaux²,

Steenari

et al. 2018

Metals

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“…12−14 In addition, many interesting and significant works have been reported, such as using iodide compounds and carbonyl complexes to increase the reaction rate, 15 adding -N, -P, and -S organic ligand to improve electronic effect. 14,16−19 Except for the homogeneous system, heterogeneous fixed-bed methanol carbonylation were also explored, such as activated carbon supported Ir catalyst, 20,21 Rh catalyst, 22 Au catalyst, 23 Pt catalyst, 24 and Ni catalyst; 25,26 SiO 2 and Al 2 O 3 supported Rh catalyst, 27 polymer supported Rh or Ir catalyst, 28−31 g-C 3 N 4 supported Rh catalyst, 32 heteropoly acid supported Rh catalyst, 33 ionic liquid supported Rh catalyst, 34,35 as well as other noniodide promoted zeolite supported Cu catalyst. 36,37 These works contributed the advance of methanol carbonylation.…”

Section: Introductionmentioning

confidence: 99%

“…Homogeneous methanol carbonylation emerged as an effective way to produce AA. Many technologies have been developed, such as Monsanto process, BP Cativa process, Celanese & Daidel AO Plus process, Chiyoda & UOP Acetica process. − In addition, many interesting and significant works have been reported, such as using iodide compounds and carbonyl complexes to increase the reaction rate, adding -N, -P, and -S organic ligand to improve electronic effect. ,− Except for the homogeneous system, heterogeneous fixed-bed methanol carbonylation were also explored, such as activated carbon supported Ir catalyst, , Rh catalyst, Au catalyst, Pt catalyst, and Ni catalyst; , SiO 2 and Al 2 O 3 supported Rh catalyst, polymer supported Rh or Ir catalyst, − g-C 3 N 4 supported Rh catalyst, heteropoly acid supported Rh catalyst, ionic liquid supported Rh catalyst, , as well as other noniodide promoted zeolite supported Cu catalyst. , These works contributed the advance of methanol carbonylation. Among the reported catalyst, some of supported Ir, Rh, and Ni catalysts showed relatively high activity, but the most problem is the unsatisfied stability.…”

Section: Introductionmentioning

confidence: 99%

La-Stabilized, Single-Atom Ir/AC Catalyst for Heterogeneous Methanol Carbonylation to Methyl Acetate

Feng

Song

Ren

et al. 2019

Ind. Eng. Chem. Res.

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Although homogeneous methanol carbonylation is industrialized to produce acetic acid, it still suffers from the problems of difficult separation and metal leaching. Here, we report a heterogeneous single atom Ir–La/AC catalyst to produce methyl acetate in a fixed-bed reactor. A high TOF of 2200h–1 and high selectivity over 90% for methyl acetate with space time yield of 8200 g/(kgcat h) were achieved over the Ir–La/AC catalyst. Furthermore, the effects of reaction temperature, partial pressure of CO and CH3OH, weight ratio of CH3I/CH3OH, total LHSV as well as the role of La on the catalytic performance of Ir/AC were tested in this paper. In addition, we proposed a reasonable mechanism for heterogeneous methanol carbonylation over La stabilized single atom Ir/AC catalyst. Our work provides a reference for the further scale-up of the process and a stable, supported, single-atom system as a substitution for other homogeneous catalyst.

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“…Rhodium is a metal that has been widely used in various catalytic reactions in an active phase [1][2][3]. It is characterized by its easy dispersion on the surface of metal oxides [4], its metallic stability in oxidizing atmospheres [5] and the chemical interactions that can occur on its surface [6,7].…”

Section: Introductionmentioning

confidence: 99%

“…shows the TEM images of RhTi1, RhTi2, RhTi3 and RhTi4 catalysts. The average crystallite size (d) was calculated using the equation d = n i d3 i / n i d 2 i . Rh particles on TiO 2 supports can be seen clearly in…”

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confidence: 99%

Correlation of Rh Particle Size with CO Chemisorption: Effect on the Catalytic Oxidation of MTBE

et al. 2019

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This study was conducted to identify the correlation between the CO chemisorption (linear interaction and gem dicarbonyl) and the specific size of rhodium particles, and further to determine the influence of this relationship on the catalytic oxidation reaction of methyl tert-butyl ether (MTBE). During the synthesis, first, TiO2 was developed by the sol-gel method under acidic conditions. Second, Rh was deposited (1 wt %) by the incipient wetness impregnation method. Later, with the aim of controlling the particle size, the Rh/TiO2 materials were crystallized at different reduction conditions during 3 h heat treatment. The results obtained by TEM micrographs indicated that the average particle size varies between 1.0 and 8.1 nm, depending on the conditions of heat treatment. From the histogram analysis of each TEM micrograph, two correlations were made: (i) the gem-dicarbonyl interaction was typical of Rh particles ≤ 1.5 nm, and (ii) a linear interaction, bridged interaction and dentate interaction were observed in particles ≥ 1.6 nm. The gem-dicarbonyl interaction (particle size ≤ 1.5 nm) was the most active in the oxidation reaction of MTBE.

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Novel heterogeneous Rh-incorporated graphitic-carbon nitride for liquid-phase carbonylation of methanol to acetic acid

Cited by 28 publications

References 22 publications

Leaching and Recovery of Rare-Earth Elements from Neodymium Magnet Waste Using Organic Acids

Leaching and Recovery of Rare-Earth Elements from Neodymium Magnet Waste Using Organic Acids

La-Stabilized, Single-Atom Ir/AC Catalyst for Heterogeneous Methanol Carbonylation to Methyl Acetate

Correlation of Rh Particle Size with CO Chemisorption: Effect on the Catalytic Oxidation of MTBE

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