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1.
J Hazard Mater ; 475: 134880, 2024 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-38889464

RESUMO

The efficient recovery of nickel from chloride systems has long presented a challenge in the field. While solvent extraction is a viable approach, conventional extractants have been associated with drawbacks such as a high requirement for chloride ions and substantial consumption of acids and alkalis. In response to these challenges, this investigation developed and synthesized a novel thiazole-based extractant, N, N-Bis(4-thiazolylmethyl)octylamine (NNBT), tailored for the selective extraction of nickel from chloride systems. Findings from the study indicate that the nitrogen atom situated on the benzylamine framework within NNBT can interact synergistically with the chelating thiazole ring, facilitating effective nickel extraction and notably reducing the need for chloride ions. Furthermore, the extractant can be regenerated using deionized water, thereby obviating the necessity for additional consumption of acids and alkalis. Following the validation of NNBT as an environmentally sustainable and efficient nickel extractant within the chloride ion system, it was successfully employed to selectively and effectively extract nickel from the nickel-aluminum slag of spent HDP catalyst. The extracted nickel and aluminum were subsequently processed into electroplated nickel chloride and polyaluminum chloride, respectively, meeting the national standards of China. These outcomes underscore the eco-friendliness and promise of NNBT for nickel extraction from chloride systems.

2.
J Environ Manage ; 322: 116055, 2022 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-36041303

RESUMO

The conventional hydrometallurgical methods for recycling refinery spent hydroprocessing catalysts are ineffective in simultaneously removing all metals (Ni, V, and Mo) in a single-stage operation. In this study, a novel octadentate chelating agent, diethylenetriaminepentaacetic acid (DTPA-C14H23N3O10), has been proposed for the first time to remove toxic metals (Ni, V, and Mo) in a single stage of operation from an industrial spent atmospheric residue desulfurization (ARDS) catalysts. It was discovered that the efficient formation of metal-DTPA complexes was attained under the optimum experimental conditions (60 °C, stirring - 150 rpm, S/L ration (w/v) of 2.5%, 7.5% DTPA, and medium pH-9) that resulted in the high removal of Mo (83.6%), V (81.3%) and Ni (64.1%) from the spent ARDS catalyst. Kinetic studies suggest that the leaching process followed a semi-empirical Avrami equation (R2 > 0.92), which predicted that the diffusion control reaction controlled the leaching. Species distribution and ecological risk analysis of the remaining metals in the insoluble residue (mostly Al2O3) indicated that the potential bioavailability of the remaining metals (except Ni) was significantly decreased, and residue poses a low ecological and contamination risk (individual contamination factor <1). Furthermore, the textural properties of the residue (BET surface area-103 m2/g and pore volume- 0.49 ml/g) were dramatically improved, suggesting that fresh hydroprocessing catalyst support can be synthesized using the leached residue. Compared to the conventional processes, the proposed chelating process is highly selective, closed-loop, and achieved high metal recovery in a single-stage operation while decreasing the environmental risks of the hazardous spent catalysts.


Assuntos
Petróleo , Síndrome do Desconforto Respiratório , Catálise , Quelantes , Descontaminação , Humanos , Cinética , Metais/química , Ácido Pentético , Reciclagem
3.
J Hazard Mater ; 436: 129187, 2022 08 15.
Artigo em Inglês | MEDLINE | ID: mdl-35739717

RESUMO

Concerning the emissions of hydrogen cyanide (HCN) and other N-bearing air pollutants from the fluid catalytic cracking (FCC) regeneration units, this paper has conducted a comprehensive testing and surface characterisation of four industrial spent catalysts, aged catalysts and hard coke sample in three different schemes, Ar-TPD, O2 -TPO and rapid heating to elaborate the transformation of N upon the influence of the heterogeneity of coke and N speciation. In the Ar-TPD scheme, the surface N is responsive for the emission of gaseous NH3 from pyrrolic N-5 and HCN from both pyridinic N-6 and quaternary N-Q. The removal of soft coke is beneficial in promoting the surface exposure of hard coke, thereby increasing the HCN emission dramatically. In the O2-TPO scheme, the oxygen accessibility is the principal factor governing the emission of HCN. The external soft coke is able to access the bulk O2 firstly, the combustion of which in turn provides heat back to promote the cracking of internal hard coke from the same and neighbouring particles to release more HCN. The induction effect of bulk O2 is also superior over the spent catalyst properties in formulating a nearly identical trend of HCN emission for all the four spent catalysts tested. Finally, for the use of rapid heating scheme that is typical in a commercial FCC regenerator, it is effective in accelerating the volatilisation of soft coke quickly, thereby promoting the oxygen accessibility to hard coke and the internal N-bearing precursors so as to mitigate the emission of HCN effectively. The use of a large superficial velocity of gas is further effective in sweeping the volatiles including HCN away from the catalyst, promoting their oxidation extent accordingly.


Assuntos
Poluentes Atmosféricos , Coque , Catálise , Gases , Oxigênio
4.
J Hazard Mater ; 318: 723-731, 2016 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-27484947

RESUMO

Deoiling process is a key issue for recovering metal values from spent hydrotreating catalysts. The oils can be removed with organic solvents, but the industrialized application of this method is greatly hampered by the high cost and complex processes. Despite the roasting method is simple and low-cost, it generates hardest-to-recycle impurities (CoMoO4 or NiMoO4) and enormous toxic gases. In this study, a novel and facile approach to remove oils from the spent hydrotreating catalysts is developed. Firstly, surface properties of spent catalysts are characterized to reveal the possibility of oil removal. And then, oils are removed with water solution under the conditions of 90°C, 0.1wt% SDS, 2.0wt% NaOH and 10ml/gL/S ratio for 4h. Finally, thermal treatment and leaching tests are carried out to further explore the advantages of oil removal. The results show that no hardest-to-recycle impurity CoMoO4 is found in XPS spectra of thermally treated samples after deoiling and molybdenum is leached completely with sodium carbonate solution. It means that the proposed deoiling method can not only remove oils simply and without enormous harmful gases generating, but also avoid the generation of detrimental impurity and promote recycling of valuable metals from spent hydrotreating catalysts.

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