Metal ion-induced separation of valuable organic acids from a depolymerized mixture of lignite without using organic solvents

Hao, Jianxiu; Han, Limin; Yang, Keli; Zhao, Hongye; Li, Xiaomin; Ban, Yanpeng; Li, Na; Liu, Quansheng

doi:10.1039/c9ra10542e

Cited by 5 publications

(3 citation statements)

References 26 publications

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“…The real lignite depolymerized mixture (DM) was analyzed by HPLC (Shimadzu LC-20AT) as in our previous report. , A binary gradient elution procedure was used for the HPLC analysis. The mobile phase was acetonitrile and 0.1% (volume fraction) phosphoric acid aqueous solution, and the stationary phase was C18 bonded by silica gel (Shim-pack GIST C18, 5 μm).…”

Section: Methodsmentioning

confidence: 99%

A General Route of Using Lignite Depolymerized Derivatives for Catalyst Construction: Insights into the Effects of the Derivative Structures and Solvents

Hao

Han²,

Yang³

et al. 2021

ACS Omega

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Depolymerization is an emerging and promising route for the value-added utilization of low-rank coal (LRC) resources, and how to use the complex depolymerized mixtures efficiently is of great importance for this route. In this work, we designed the rational route of using depolymerized mixtures from lignite via ruthenium ion-catalyzed oxidation (RICO) depolymerization directly without complex separation to construct a Zr-based hydrogenation catalyst. The prepared catalyst was applied into the catalytic transfer hydrogenation of biomass-derived carbonyl compounds. Meanwhile, a copper-based oxidation catalyst was also constructed via a similar route to investigate the universality of the proposed route. Special insights were given into how the depolymerized components with different structures influenced the performances of the catalysts. The effects of the solvents used during the catalyst preparation (H 2 O and DMF) were also studied. The results showed that the proposed route using the depolymerized mixtures from lignite via RICO to construct catalysts was feasible for both Zr-based and Cu-based catalysts. The two catalysts prepared gave high efficiency for their corresponding reaction, i.e. , the Zr-based catalyst for catalytic transfer hydrogenation of biomass-derived carbonyl compounds and the Cu-based catalyst for selective oxidation of alcohols into aldehydes. Different depolymerized components contributed differently to the activity of the catalyst, and the solvents during the preparation process could also influence the activity of the catalyst. The depolymerized components and the solvents influenced the activities of the Zr-based catalyst mainly via changing the Zr contents, the microenvironment of Zr 4+ , and the specific areas of the catalyst.

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Section: Methodsmentioning

confidence: 99%

A General Route of Using Lignite Depolymerized Derivatives for Catalyst Construction: Insights into the Effects of the Derivative Structures and Solvents

Hao

Han²,

Yang³

et al. 2021

ACS Omega

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“…The structures of the depolymerized products BPCAs were identified by HPLC (SHIMADZU LC-20AT, Japan) and GC-MS (Agilent 7890 series GC with a 5977 MS detector). 44 The depolymerized products have been esterized before GC-MS analysis. Before esterification, the depolymerization product BPCAs and the salt in RICO, the aqueous phase…”

Section: Discussionmentioning

confidence: 99%

Reusability Investigation of a Ruthenium Catalyst during Ruthenium Ion-Catalyzed Oxidative Depolymerization of Lignite for the Production of Valuable Organic Acids

et al. 2021

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A clean and efficient conversion process is essential for the utilization of low-rank coals. Lignite, a typical representative of the low-rank coal family, has huge potential for the production of valuable chemicals via the oxidative depolymerization reaction. Ruthenium ion-catalyzed oxidation (RICO) is an effective route for lignite depolymerization under mild conditions, but the high cost of precious Ru limits the potential large-scale application of RICO. How to recycle and reuse Ru is critical to promote the application of RICO. In this work, a novel and efficient approach for reusing Ru through recycling the solvent mixture containing Ru was established for RICO. First, the influence of different reaction parameters on the depolymerization degree of lignite and benzene polycarboxylic acid (BPCA) yields was investigated. Second, the distribution of Ru in the organic phase (OP), aqueous phase (AP), and residual solid phase (RSP) was analyzed after the RICO reaction. Finally, based on the distribution of Ru in different phases, a novel route of recycling Ru by reusing the Ru-containing solvents was proposed. The results showed that the dosage of RuCl 3 and NaIO 4 had a significant influence on both the depolymerization degree of lignite and BPCA yields. The distribution of Ru had a close relationship with the depolymerization degree of lignite and the dosage of NaIO 4 . After the depolymerization reaction, the CCl 4 phase containing Ru was reused directly as the solvent for the next run, which could fulfill the reuse of both CCl 4 and Ru. The results proved that the Ru-containing CCl 4 phase could maintain catalytic performance for 5 runs. This work provides an efficient route to reuse Ru for the RICO depolymerization of lignite into valuable organic acids. As far as we know, this is the first report concerning the recycling and reuse of Ru during the RICO of lignite. This work is important for the application of RICO in lignite depolymerization.

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“…The BPCAs in the depolymerized product was determined by HPLC(SHIMADZU LC-20AT). 30 A binary gradient elution procedure was used for HPLC analysis. The mobile phase was acetonitrile and 0.1% (volume fraction) phosphoric acid aqueous solution, and the stationary phase was C18 bonded to silica gel (Shim-pack GIST C18, 5 mm).…”

Section: Methodsmentioning

confidence: 99%

Ruthenium ion catalytic oxidation depolymerization of lignite under ultra-low dosage of RuCl₃ catalyst and separation of the organic products with inorganic salts

et al. 2023

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Metal ion-induced separation of valuable organic acids from a depolymerized mixture of lignite without using organic solvents

Abstract: Metal ion-induced separation of valuable organic acids from complex lignite depolymerized mixtures was proposed and proved to be an efficient, green, and facile separation process with easily tunable separation selectivity.

Cited by 5 publications

References 26 publications

A General Route of Using Lignite Depolymerized Derivatives for Catalyst Construction: Insights into the Effects of the Derivative Structures and Solvents

A General Route of Using Lignite Depolymerized Derivatives for Catalyst Construction: Insights into the Effects of the Derivative Structures and Solvents

Reusability Investigation of a Ruthenium Catalyst during Ruthenium Ion-Catalyzed Oxidative Depolymerization of Lignite for the Production of Valuable Organic Acids

Ruthenium ion catalytic oxidation depolymerization of lignite under ultra-low dosage of RuCl₃ catalyst and separation of the organic products with inorganic salts

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Metal ion-induced separation of valuable organic acids from a depolymerized mixture of lignite without using organic solvents

Abstract: Metal ion-induced separation of valuable organic acids from complex lignite depolymerized mixtures was proposed and proved to be an efficient, green, and facile separation process with easily tunable separation selectivity.

Cited by 5 publications

References 26 publications

A General Route of Using Lignite Depolymerized Derivatives for Catalyst Construction: Insights into the Effects of the Derivative Structures and Solvents

A General Route of Using Lignite Depolymerized Derivatives for Catalyst Construction: Insights into the Effects of the Derivative Structures and Solvents

Reusability Investigation of a Ruthenium Catalyst during Ruthenium Ion-Catalyzed Oxidative Depolymerization of Lignite for the Production of Valuable Organic Acids

Ruthenium ion catalytic oxidation depolymerization of lignite under ultra-low dosage of RuCl3 catalyst and separation of the organic products with inorganic salts

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Ruthenium ion catalytic oxidation depolymerization of lignite under ultra-low dosage of RuCl₃ catalyst and separation of the organic products with inorganic salts