CHEMICAL ENGINEERING RESEARCH & DESIGN
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2024
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IF 3.7
Yan Li,Sisi Tang,Hang Lei,Yuxia Zhong,Yue-Fei Zhang
In this paper, two adsorbents based on hydrophilic and hydrophobic fumed silica carriers for efficient recovery of palladium were prepared using 1,4,7,10-tetraazacyclododecane as a functional group. These functional adsorbents were characterized by FT-IR, SEM and BET. The effects of pH (2-6), contact time (1-480 min), and temperature (25-55℃) on the adsorption performance were investigated. The concentration of palladium(II) after adsorption was determined by flame atomic absorption spectrometry and the data were analyzed by kinetic, thermodynamic and isotherm fitting. At pH = 4, the adsorption conformed to Pseudo-second-order kinetic model, with rapid adsorption within 2 h and able to reach equilibrium within 5 h. Meanwhile, the Langmuir model was able to better describe the isotherm data, with the maximum adsorption exceeding 140 mg·g -1 . Moreover, the thermodynamic analysis indicated that the adsorption was a heat-absorbing spontaneous process. The combination of XPS and DFT calculations elucidated the adsorption and desorption mechanisms, emphasized the potential of these adsorbents for the recovery of Pd(II) from aqueous solutions, and contributed to the development of sustainable and effective adsorption technologies.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Abdul Haleem,Fan Wu,Mohib Ullah,Tooba Saeed,Hao Li,Jianmimg Pan
Retrieving valuable metals like palladium, gold, and platinum from electronic waste poses significant challenges. In this study, we developed highly macroporous and flexible antibacterial chitosan-based cryogel through rapid cryopolymerization induced by ultraviolet exposure. This designed cryogel exhibited exceptional palladium adsorption capabilities within an acidic environment, demonstrating swift and efficient adsorption. Remarkably, the chitosan-based cryogel showed an impressive palladium adsorption capacity, reaching 184.93 mg g −1 as Langmuir isotherm model, thus highlighting its promising potential for palladium recovery. The adsorption efficiency and concentration examination was conducted using an Inductively Coupled Plasma Optical Emission Spectrometer in the presence of multiple coexisting ions. Various factors and parameters, including pH, contact time, temperature, concentration, and selectivity, were investigated to assess the effectiveness of the biopolymeric cryogel in palladium adsorption. Additionally, the thermal stability of the developed cryogel was explored within the temperature range of 25-100˚C, revealing a commendable palladium adsorption capacity even at 100˚C. This finding underscores the material's potential for application under challenging conditions. The cryogel that was synthesized exhibits an extended shelf-life of up to six months and can be reused without any discernible alteration in its adsorption efficiency. Furthermore, the palladium adsorption capacity was evaluated in a real-world sample, demonstrating commendable adsorption capabilities. Remarkably, the biosorbent displayed a higher selectivity of 91% for palladium, even in the competing ions presence. In summary, biosorbent offers superior adsorption performance and remarkable stability, making it a valuable contribution to polymer chemistry and environmental science. Its potential for recovering precious metals from wastewater is indeed noteworthy.
研究领域:
环境科学
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高分子化学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Yilong Zhu,Huifang Xing,Shan Ni,Ke Xu,ZhaoXiang Zhong,Liangrong Yang
The recycling of precious materials, such as palladium (Pd), was repeatedly documented as essential for a sustainable future with respect to the environment and energy production. However, high-efficiency extraction presented significant challenges. In this work, a surface hydroxyl regulation strategy was used to prepare a defective carbon nitride (CN) with a high specific surface area and hierarchical porosity through cobalt (Co)-doping. Characterization confirmed the successful synthesis of the adsorbent. The results indicated that the optimal pH for the adsorption process was 5.5, adsorption kinetics and isotherms of Pd on the adsorbent suggested that the adsorption followed a pseudo-second-order model and the Langmuir model, respectively. The maximum adsorption capacity reached up to 529.1 mg·g –1 . In addition, it showed high affinity for Pd ions, the K d value was 4.1 × 10 4 ml·g –1 . After Pd adsorption, due to the presence of abundant and uniformly dispersed Pd and Co particles which further facilitated cooperative catalysis on the surface of adsorbent, As a result, the Co-CN-Pd was reused as a catalyst for p-nitrophenol hydrogenation. It achieved a turnover frequency (TOF) as high as 1032.6 h –1 , significantly surpassing other catalysts reported in the literature. Overall, this novel adsorbent presented broad application prospects in the field of Pd recovery and reuse.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2024
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IF 12.2
Fan Wu,Abdul Haleem,Mohib Ullah,Li Chen,Hao Li,Jianming Pan
Recovering precious metals such as palladium from secondary resources faces significant challenges, including the scarcity of efficient adsorbents capable of withstanding harsh acidic conditions and needing materials with high selectivity, mechanical stability, and scalability. In response to these challenges, we developed highly porous cryogels functionalized with sulfonic and amidoxime groups, achieving a unique combination of hydrophilicity, flexibility, and selectivity for Pd(II) ions. Using a redox cryopolymerization method, these cryogels attained a gel fraction of 100 % and a maximum adsorption capacity of 425.3 mg g −1 at 318 K, as the Langmuir isotherm model fitted. This work also combined 3D printing technology with cryopolymerization to create a highly selective, high mechanical strength and customizable shape adsorption material, overcoming traditional adsorption materials' limitations in acid conditions. This innovative combination fills the gap in selective palladium recovery in customizable super macroporous materials, offering a sustainable solution for precious metal recovery and setting a foundation for broader applications in adsorption separation.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Hao Li,Fan Wu,Yang Pan,Yuting Zhang,Roser Pleixats,Jianming Pan
With the rapid development of the automobile industry and increasingly strict regulations on automobile exhaust emissions around the world, the production of waste purification catalysts for automobile exhaust will increase, leading to an increasing demand for palladium . Recycling waste three-way catalysts (TWCs) is an important way to obtain palladium resources. However, it is still a challenge to obtain highly selective adsorbents for palladium. Herein, we successfully fabricated two different kinds of Pd 2+ selective composite adsorbents ( PVA@MSNs and PVA@MONs ) through covalent attachment of a proline-valinol amide ( PVA ) as the ligand on silica nanoparticles. The as-prepared adsorbents were characterized by TEM , SEM, elemental analysis , 29 Si and 13 C CP MAS NMR, N 2 -adsorption-desorption isotherm analysis, DLS, zeta-potential, p -XRD and FT-IR, revealing their high loading rate, and the mesoporous structure in the case of PVA@MSNs . In order to evaluate the ability of these two sorbents to selectively capture palladium(II), a series of sequential adsorption experiments were performed. The results showed that 56.35 mg and 67.74 mg of Pd 2+ could be captured per gram by PVA@MSNs and PVA@MONs, respectively. Furthermore, they had a stronger selectivity towards Pd 2+ than other cations (i.e . Co 2+ , Ni 2+ , Zn 2+ , Pb 2+ , Fe 2+ ,) present in the simulated sample. Both sorbents were able to remain stable and show consistent performance in cyclic adsorption-desorption runs. Interestingly, the adsorbents realized for the first time the enrichment and recovery of palladium from organic solvents , offering a potential application in palladium catalyst-loaded industrial waste liquid processes.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Rui Zhang,Yahong Li,Bo Meng,Yuan Liu,Jianxian Zeng,Guangyong Weng,Houchao Shan,Di Cai,Xiaoping Huang,Lin Jin
Palladium (Pd) recovery from secondary resources is urgently needed to meet the rising demands for precious metals for sustainable development and environmental protection. To achieve the goal of simple, efficient, and selective recovery of precious metal Pd, we reported an innovative strategy that utilized a double-layer adsorptive membrane based on polydopamine (PDA) modification and polymethacryloxyethyltrimethyl ammonium chloride (PDMC) grafting. The adsorption results suggested that the adsorptive membrane exhibited an excellent adsorption capacity of 61.5 mg g −1 towards Pd(II) at pH 2.0 and the adsorption capacity remained stable after six cycles. Moreover, the adsorption processes of Pd(II) were fitted to pseudo second-order kinetic models and the Langmuir isotherm models. Density functional theory (DFT) simulation, and FTIR, XPS analysis indicated the adsorption mechanisms were ion exchange from the PDMC layer and chelation and ion exchange from the PDA layer. In the presence of other metal ions (Ni(II), Cu(II), Zn(II), Ca(II), Mg(II), K(I) and Na(I)), the separation factor of adsorptive membrane for Pd(II) was in the range of 50–529. The remarkable selectivity was due to the mechanism of the combination of electrostatic attraction and coordination interaction to Pd(II) while the electrostatic repulsion to other metal cations. Furthermore, membrane filtration results suggested that Pd(II) was effectively adsorbed and rejected and the leakage risk could be reduced by dual adsorption from the double-layer membrane. This study not only offers an innovative strategy to precisely and effectively recover Pd(II) and other platinum group metals, but also provides valuable insights for the future implementation of adsorptive membranes in recycling low-concentration wastewater in an efficient and friendly way.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
DESALINATION
·
2025
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IF 9.8
Shunyan Ning,Sizhi Xu,Jiaxu Zheng,Shichang Zhang,Xiangbiao Yin,WenLong Li,Yuezhou Wei,Lifeng Chen
Spent fuel reprocessing typically produces high-level liquid waste (HLLW), where lots of palladium and other radioactive nuclides exist. Palladium recovery from HLLW contributes to not only increasing the palladium supply but also addressing the issue of furnace clogging during the vitrification of HLLW. To achieve this, several aminopyridine-functionalized silica-based resins (SiPAc-NH-Pys) were prepared in this study through in-situ polymerization and post-synthetic modification, and the adsorption behaviors and mechanisms toward palladium were systematically studied by batch experiment and spectroscopy. The results showed that aminopyridine-functionalized SiPAc-NH-Pys with porous structure and uniform shapes were successfully prepared. These SiPAc-NH-Pys exhibited high selectivity for palladium in simulative HLLW, with almost no affinity for lanthanides or alkaline metal ions. In addition, SiPAc-NH-Pys exhibited fast adsorption and desorption kinetics, with equilibrium reached within 10 min. The adsorption kinetics were fitted well by the pseudo-second-order kinetic model, and the adsorption isotherm was well described by the Langmuir model. Spectroscopy experiments suggested that the nitrogen atom in the pyridine ring was the main active site for palladium adsorption and that nitrate anions were involved in palladium coordination; thus, they were co-adsorbed. The direct and selective recovery of palladium from simulative HLLW was finally realized in column mode, with the recovery rate close to 100 %. Overall, this work provides excellent functional material candidates for the separation of rare metal palladium from HLLW, showing significant potential.
研究领域:
核化学与化工
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材料科学
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环境科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Fenglei Liu,Zhihao Li,Fang Xia,Baowei Hu
The efficient recovery of palladium from the spent nuclear fuel was of great significance to the sustainable development of nuclear energy. Herein, the uniform spherical COFs were constructed by a facile approach at room temperature, which were further surface functionalized by a thiol-ene “click” reaction to recover Pd(II). Microscopic and spectroscopic studies manifested that the formation mechanism and size of spherical COFs were greatly affected by the amount of catalyst and solvent type. The TAPB-BPTA-DTT and TAPB-BPTA-S-β-CD exhibited high Pd(II) recovery efficiency due to the introduction of sulfhydryl groups, and the maximum adsorption capacities were 489.3 and 234.3 mg/g, respectively. Meanwhile, the water environmental condition played an important role in the separation process, and the classical adsorption models demonstrated that monolayer chemisorption was the dominant removal mechanism. Mechanism analysis showed that the excellent adsorption performance was mainly attributed to the electrostatic interaction, physical absorption and chelation of N, O, and S groups with Pd(II). Thus, it is expected that this work could provide more insight into COFs materials, thereby promoting palladium removal advancements in the spent nuclear fuel.
研究领域:
材料科学
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环境科学
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核能工程
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Zhiliang Ma,Chao Xie,YueZhou Wei,Xiangbiao Yin,Caiwu Luo,Shunyan Ning,Qiang Wu,Tianjiao Jiang
The efficient separation and recovery of palladium (Pd) from high-level liquid waste (HLLW) are critical for promoting resource sustainability and advancing the nuclear fuel cycle. In this study, a novel silica-based sorbent (HT-paPBI@SiO 2 ) enriched with nitrogen adsorption sites was synthesized via a polymerization–vacuum impregnation–high-temperature optimization strategy to address the challenges of Pd(II) recovery in highly acidic and ionically complex environments. HT‑paPBI@SiO 2 was systematically characterized using SEM, EDS, TG‑DSC, BET, and FT‑IR analyses, which confirmed its rigid framework, abundant porosity, high loading efficiency, and excellent thermal stability. Static batch adsorption experiments demonstrated that HT‑paPBI@SiO 2 efficiently adsorbs Pd(II) over a broad acidity range (0.1–9 M HNO 3 ). In simulated HLLW at 6 M HNO 3 , the material exhibited outstanding selectivity ( SF Pd/other metal ions > 1.05 × 10 3 ) and a high saturation adsorption capacity of 128.2 ± 1.8 mg/g. Furthermore, the adsorption kinetics fit well with a pseudo‑second‑order model, while the equilibrium data conform to the Langmuir isotherm and van’t Hoff thermodynamic models, indicating a spontaneous, endothermic, monolayer chemical adsorption process. Furthermore, dynamic adsorption experiments successfully achieved the selective recovery of Pd(II) from simulated HLLW, highlighting the potential of HT-paPBI@SiO 2 for industrial-scale applications. Mechanistic investigations, supported by FT-IR, XPS, and DFT calculations, revealed that the benzene ring in paPBI was oxidized to a quinone structure under high-temperature treatment. The electron-rich regions resulting from the interaction of the C=O group in quinone with the C=N − C moiety in imidazole enhance the affinity for Pd(II). This interaction facilitates the coordination of nitrogen and oxygen atoms with Pd(II), while NO 3 − ions coordinate to balance the charge.
研究领域:
核化学与化工
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材料科学
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环境工程
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Hao Liu,Qing-da An,Jeonghun Kim,Lin Guo,Yu-meng Zhao,Zuo-yi Xiao,Shang-ru Zhai
The recovery of noble metals from aqueous systems is of great significance for constructing sustainable framework of modern industry yet remains challenging. Herein, Cu x S y /Carbon composites with superior thermal stability and adsorption capacity were successfully synthesized via one-pot hydrothermal method using lignosulfonate as dual role of raw materials. The optimal synthesis conditions were investigated via tailoring the temperature and the mass ratio of reagents. The morphologies and physical properties of the composites were characterized by scanning electron microscope (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), and thermogravimetric analysis (TGA). The surface chemistry was analyzed by Zeta potential analysis, Brunauer-Emmet-Teller (BET), and X-ray photoelectron spectroscopy (XPS). The Langmuir model and the pseudo-second-order model well described the adsorption of Pd(II) and Pd(IV) delivered by fabricated composites. The adsorption capacity obtained from Langmuir isotherm model towards Pd(IV) was 114 mg/g and Pd(II) was 101 mg/g, respectively. More importantly, the adsorbed palladium species could be desorbed with hydrochloric acid and thiourea, which suggested good durability and recycling performance of the typical composite. This work might provide a new guidance for the utilization of lignin or its derivatives and enriched the research in the field of noble metal recovery.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 48
·27320-27331
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IF 12.732
Pengcheng Wu,Hui Liu,Mengqi Sun,Yaxin Zeng,Jiawei Ye,Song Qin,Yimin Cai,Wen Feng,Lihua Yuan
Efficient palladium recovery from high level liquid wastes (HLLW) is of increasing priority for sustainable development and addressing issues in radioactive waste treatment. However, searching for robust materials for palladium sorption, in the presence of large amounts of competing ions even at rather high acidity still poses a great challenge. Herein we present two novel cationic covalent triazine frameworks (denoted as CTF-S and CTF-L) created by polymerization of monomers IL-S and IL-L for palladium recovery. The resultant CTF-S and CTF-L with respective surface areas of 212.9 m2 g−1 and 342.5 m2 g−1 exhibit excellent sorption ability toward palladium at high acidity. This has been demonstrated by a maximum sorption capacity of 333 mg g−1, which is the highest at 3 M HNO3 among all porous adsorbents reported so far. More importantly, these materials reveal remarkable selectivity toward palladium over other metal ions that are co-existing in simulated HLLW. In addition, thanks to the relatively large π-conjugated structures, no obvious decrease in sorption capability was observed after being exposed to 1000 kGy γ irradiation. Desorption could be easily achieved by a single contact with a mixed solution of 1 M thiourea and 1 M HCl and the sorption performance still remains at the initial level without conspicuous loss after five cycles. The XPS results, anion competitive experiments, and DFT calculations propose a sorption mechanism in which the anion exchange between anionic Pd complexes and chloride, and the chemical coordination between triazine N and Pd(II) work coorperatively to enhance the sorption capacity. This work not only provides a new kind of excellent adsorbent for selective palladium recovery, but also demonstrates a promising approach for constructing robust materials for nuclear waste remediation.
研究领域:
材料科学
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核化学与放射化学
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环境科学
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DOI
高影响因子
Chemical Science
·
2025
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IF 7.4
Yang Liu,Weikang Guo,Jiale Liu,Haijuan Tao,Juan Yang,Qin Shuai,Yusuke Yamauchi,Brian Yuliarto,Yusuke Asakura,Lijin Huang
Palladium (Pd), a rare and precious metal, is highly valued due to its non-renewable nature and significant cost. Therefore, recovering palladium from industrial wastewater is of great importance but remains a challenge. Herein, a composite aerogel adsorbent has been developed by linking a bipyridine covalent organic framework, termed TpBpy, with chitosan (CS) through robust covalent bonds. The resulting TpBpy/CS aerogel is employed for the selective separation and recovery of palladium at low concentrations in real wastewater. Experimental results reveal that the maximum adsorption capacity of the TpBpy/CS aerogel for Pd(II) is 274.4 mg g−1 at pH 1. Additionally, even in the presence of other coexisting ions at concentrations 100 times higher than Pd(II), the adsorption efficiency for Pd(II) remains above 99%. Mechanistic investigations indicate that the adsorption of Pd(II) by the TpBpy/CS aerogels primarily occurs through the coordination between pyridine N and Pd(II), as well as the electrostatic interaction between protonated amino groups and Pd(II). Moreover, the TpBpy/CS aerogel demonstrates exceptional reusability, maintaining an adsorption efficiency for Pd(II) above 99% after nine adsorption–desorption cycles. Overall, the TpBpy/CS aerogel is a promising monolithic adsorbent for the efficient recovery of Pd(II) from acidic industrial wastewater due to its exceptional adsorption capacity and selectivity, demonstrating substantial potential for practical applications.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）