Porous polyisothiocyanurates for selective palladium recovery and heterogeneous catalysis

Song, Kyung Seob; Ashirov, Timur; Talapaneni, Siddulu Naidu; Clark, Adam H.; Yakimov, Alexander V.; Nachtegaal, Maarten; Copéret, Christophe; Coskun, Ali

doi:10.1016/j.chempr.2022.05.009

Cited by 52 publications

(24 citation statements)

References 55 publications

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“…We recently reported the synthesis of CITCFs bearing in situ formed isothiocyanurate linkages through the trimerization of 1,4-phenylene diisothiocyanate under ionothermal conditions using ZnCl 2 at 500 °C . The resulting CITCF showed a high BET surface area of 1589 m 2 g –1 with hierarchical porosity and a high Pd(II) adsorption capacity of 909 mg g –1 under wastewater conditions . Subsequent reduction of captured Pd(II) within the polymer network led to the formation of Pd NPs within the CITCF, PdNP-CITCF.…”

Section: Resultsmentioning

confidence: 99%

Boosting Polysulfide Conversion in Lithium–Sulfur Batteries via Palladium-Based Environmentally Friendly Porous Catalyst

et al. 2023

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Lithium−sulfur (Li−S) batteries offer a great potential as nextgeneration energy storage systems. However, the shuttling effect and the sluggish reaction kinetics of lithium polysulfides (LiPS) result in a low specific capacity and poor rate performance. In an effort to address these challenges, here, we demonstrate the use of captured Pd from wastewater conditions using porous polyisocyanurates, named covalent isothiocyanurate frameworks (CITCFs), bearing homogeneously distributed sulfur binding sites as a sustainable and environmentally friendly electrocatalyst to suppress the shuttling effect while promoting the kinetics of sulfur redox reactions. The designed electrocatalyst endows Li−S batteries with a high initial specific capacity of 907 mAh g −1 at 1 C, stable capacity of 450 mAh g −1 after 500 cycles at 1 C, and excellent rate performance with a capacity of 681 mAh g −1 at 2 C, thus offering a new perspective for the sustainable development of electrocatalysts toward the realization of practical Li−S batteries.

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Section: Resultsmentioning

confidence: 99%

Boosting Polysulfide Conversion in Lithium–Sulfur Batteries via Palladium-Based Environmentally Friendly Porous Catalyst

et al. 2023

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“…Fe(III), Ni(II), Pb(II), Zn(II), and Cd(II) ions prevalent in waste products often coexist with Pd(II), which may affect the adsorption of Pd(II). , Therefore, we investigated the adsorption selectivity of PAF-1-N 4 for Pd(II). From Figure a, PAF-1-N 4 exhibited the recovery rates for Fe(III) and Zn(II) at 13.44 and 13.23%, respectively.…”

Section: Resultsmentioning

confidence: 99%

Nanoporous Aromatic Framework with Bulky Binding Groups for Palladium Recovery

Zhao

et al. 2022

ACS Appl. Nano Mater.

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Effective extraction of palladium from secondary resources is a promising solution for the sustainable utilization of precious metals. A cyclic molecule containing four N atoms was modified on a nanoporous aromatic framework (PAF) to give PAF-1-N 4 , which provided a meaningful route to introduce bulky molecules with multiple coordination sites into the PAF materials. Through the interaction of multiple binding sites to Pd(II), PAF-1-N 4 showed rapid and deep adsorption of Pd(II) at a low initial concentration. The maximum Pd(II) adsorption capacity of PAF-1-N 4 reached 299.4 mg g −1 , and PAF-1-N 4 reduced the concentration of Pd(II) from 5.35 ppm to 84 ppb within 5 min and finally to 42 ppb within 60 min. After the in situ reduction, the obtained Pd@ PAF-1-N 4 exhibited good catalytic activity and reusability for the Suzuki−Miyaura coupling reaction in five-cycle catalytic experiments, thus realizing its sustainable utilization of palladium extracted from secondary resources.

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“…1 These features endow palladium with indispensable functions in numerous fields including catalysis, hydrogen storage, jewelry, corrosion protection, etc. 2 However, the concentration of palladium in the earth's crust is extremely low (∼10 −6 %). With the ever-increasing industrial demands for this precious metal, the already rare terrestrial ores call for efficient recovery and separation of palladium from secondary resources.…”

Section: Introductionmentioning

confidence: 99%

Complexation and Separation of Palladium with Tridentate 2,6-Bis-triazolyl-pyridine Ligands: Synthesis, Solvent Extraction, Spectroscopy, Crystallography, and DFT Calculations

et al. 2023

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Selective extraction of palladium from high-level liquid waste (HLLW) is desirable for the sustainable development of nuclear energy and resource recovery. In this work, three tridentate 2,6-bis-triazolyl-pyridine ligands (L-I, L-II, and L-III) bearing different alkyl side chains were synthesized and systematically studied for the complexation and extraction of palladium. Altering the alkyl side chains of the ligands led to pronounced differences in extraction performance. Among the three ligands, L-II decorated with two noctyl groups exhibited the highest Pd(II) extraction efficiency at acidity levels of 1−5 M HNO 3 and outstanding selectivity over 13 coexisting competing metal ions. Results from UV−vis titration experiments and theoretical calculations suggested that the differentiated extraction abilities of the ligands could be because of their different hydrophilicity rather than electron-donating effects. Slope analyses and electrospray ionization-high resolution mass spectrometry (ESI-HRMS) experiments revealed the formation of both L/ Pd 1:1 and 2:1 species during the extraction process. These stoichiometries were further confirmed by job plots and NMR titration experiments. The ligands were found to aggregate slightly, especially at higher concentrations, which could result from multiple intermolecular hydrogen bonds as illustrated by X-ray crystallography. The configurations of PdL and PdL 2 were further elucidated by analysis of single crystal structure and density-functional theory (DFT) calculations, respectively, where the first coordination sphere of Pd(II) was surrounded by four nitrogen or oxygen atoms in a quadrangular manner. This study provides an alternative method to separate palladium from HLLW and brings a new understanding of the coordination and complexation behaviors of Pd(II) with tridentate nitrogen ligands.

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Porous polyisothiocyanurates for selective palladium recovery and heterogeneous catalysis

Cited by 52 publications

References 55 publications

Boosting Polysulfide Conversion in Lithium–Sulfur Batteries via Palladium-Based Environmentally Friendly Porous Catalyst

Boosting Polysulfide Conversion in Lithium–Sulfur Batteries via Palladium-Based Environmentally Friendly Porous Catalyst

Nanoporous Aromatic Framework with Bulky Binding Groups for Palladium Recovery

Complexation and Separation of Palladium with Tridentate 2,6-Bis-triazolyl-pyridine Ligands: Synthesis, Solvent Extraction, Spectroscopy, Crystallography, and DFT Calculations

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