COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
Caifeng Wei,Zujing Yang,Jianyong Zhang,Hongbing Ji
In this paper, imidazolium-functionalized porous organic polymers (IM-Br-2OH) are prepared successfully via a quaternization reaction of tetrakis[4-(1-imidazolyl)phenyl]methane (TIPM) and 1,4-dibromo-2,3-butanediol (2,3-BDO). The as-synthesized IM-Br-2OH are characterized by various tools such as Fourier transform infrared spectroscopy (FTIR), Scanning electron microscope and energy dispersive spectrum (SEM-EDS mapping), Thermogravimetric analysis (TGA), N 2 adsorption-desorption isotherms, X-ray photoelectron spectroscopy (XPS) and solid-state 13 C CP/MAS NMR spectroscopy. The IM-Br-2OH exhibits the maximum adsorption capacity of perrhenate (ReO 4 - ) was 658.4 mg/g with removal efficiency of 98.0 ± 0.2% at 35 ºC. Experimental results showed that the IM-Br-2OH presents a higher adsorption capacity for ReO 4 - than the previously reported adsorbents. In addition, excellent adsorption selectivity of IM-Br-2OH for ReO 4 - was observed in the presence of competing anions such as CO 3 2- , Cl - , SO 4 2- , NO 3 - , and PO 4 3- . Adsorption process of ReO 4 - from solutions onto IM-Br-2OH follows a pseudo-second-order mode well and the adsorption data are in accordance well with the Langmuir isotherm equations. Adsorption mechanism is confirmed with the help of Zeta potentials , FTIR and XPS, indicating that anion-exchange interactions between N + and ReO 4 - contribute to the ReO 4 - adsorption from aqueous solution. The conclusions imply that IM-Br-2OH has potential application in the removal of radioactive pollutants from effluents.
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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高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2023
·Vol. 140
·期 40
·1-18
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IF 3
Wan Xu,Shengyuan Zhao,Huijuan Zhang,Fangfang Niu,Xingsheng Liu,Zhenbin Chen,Yuan Sun
With the continuous depletion of global rhenium resources, the separation and purification of rhenium (Re) from secondary resources became very important. Herein, an imprinted composite membrane with “flexible chain” thermo-responsive imprinted separation layer structure (Re-TIICM) was prepared to achieve selective separation and recovery of Re from secondary resources with complex composition. Re-TIICM's thermo-responsive imprinted separation layer occurred sol/gel phase transition by adjusting the temperature, which effectively mitigated the trade-off between selectivity and desorption. The structure and performance of Re-TIICM under optimum process conditions were tested and evaluated. The results showed that Re-TIICM exhibited a maximum adsorption capacity of 0.1036 mmol/g at 35°C, a separation degree of 4.37 (MnO 4 − as disturbing ions), and remained good adsorption capacity and selectivity after 9 adsorption/desorption cycles. When Re-TIICM was applied in secondary resources, the purity of Re increased from 35.412% to 70.208% after one adsorption/desorption cycle, showing a great potential for industrial applications.
研究领域:
材料科学
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环境工程
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冶金工程
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DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2024
·Vol. 141
·期 42
·e56095
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IF 2.7
Xianhang Bu,Zhengcan Chen,Xiaoyu Lin,Wan Xu,Yuanjun Sun,Xiaojian Ou,Yuan Sun,Zhenbin Chen
In this study, we combined the imprinting technique, temperature-sensitive polymer, and Pickering emulsion polymerization to prepare a temperature-sensitive porous imprinted polymer. First, the temperature-sensitive block polymer PDEA-b-P (DEA-co-AM) was prepared by reversible-addition fragmentation chain transfer polymerization, and then a temperature-sensitive porous ReO 4 − imprinted polymer (ReO 4 − -TPIP) was prepared using the Pickering-like polymerization technique, which was introduced to the preparation of the imprinted polymer. The structure and morphology of the polymer were characterized by FTIR, SEM-EDS, and BET. The adsorption experiments showed that the maximum adsorption (Q), separation (R), and desorption (D) of ReO 4 − -TPIP were 0.1568 mmol/g, 3.41, and 85.22%, respectively, and the adsorption equilibrium could be reached after 120 min, which decreased to 0.1212 mmol/g, 1.23, and 70.01% after repeated use for 11 times. These results indicate that ReO 4 − -TPIP has good adsorption and reusability properties. The adsorption studies showed that ReO 4 − -TPIP conformed to the zero-level kinetic model in the pre-adsorption stage, the quasi-one-level kinetic model in the late stage, and the isothermal adsorption process conformed more to the Langmuir model. In addition, in the secondary leach solution of high-temperature alloys, the purity of rhenium in the solution increased from 35.4119% to 53.4812% after one adsorption/desorption cycle. The prepared ReO 4 − -TPIP provides a new material and strategy for the selective separation and purification of rhenium in complex rhenium-containing solutions for the industry.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
Environmental Chemistry Letters
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2020
·Vol. 18
·期 4
·1379-1388
·
IF 5.922
Zhang Hao,Yang Fan,Lu Chuan,Du Chang,Bai Ruixi,Zeng Xian,Zhao Zhigang,Cai Chunqing,Li Jianguo
Treatment and recycling of radioactive waste are major challenges for the nuclear energy sector. Pertechnetate anions, 99 TcO 4 − , occur in nuclear waste and are formed mainly during nuclear fission. 99 TcO 4 − is a very hazardous contaminant due to its long half-life and high solubility and mobility in water. The effective capture of 99 Tc contamination at legacy nuclear sites remains a serious and unsolved environmental issue. In this work, 99 TcO 4 − /ReO 4 − was adsorbed by compressible graphene–chitosan sponges with grafted tertiary amine groups. Moreover, the hydrophobic branched chains strongly reduced the interference of competitive anions during adsorption. Results show that 99 TcO 4 − /ReO 4 − can be effectively removed even under highly acidic conditions and in the presence of competing anions. More than 98% of 99 TcO 4 − /ReO 4 − was removed using simulated nuclear wastes.
研究领域:
环境科学
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核能工程
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材料科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
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IF 5.774
Jun Zhang,Runtian Wang,Xiaojian Ou,Xiaoyan Zhang,Pu Liu,Zhengcan Chen,Boyuan Zhang,Chunli Liu,Shengyuan Zhao,Zhenbin Chen,Jinian Zhu,Sujun Lu,Peng Zhang
A novel thermo-sensitive imprinted composite membranes (TSICMs) was developed. Different from other TSICMs, poly N,N-diethylacrylamide (PDEA) as a block part was grafted onto the imprinted polymeric separation layer matrix to obtain highly adjustable imprinted site, which could ensure imprinted site more excellent selectivity and separation performance. The morphology and structure of this polymer membrane were characterized by scanning electron microscope (SEM), Fourier Transform Infrared Spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). The results showed that TSICMs of ReO 4 − (Re-TSICMs) possessed Thermo-responsive recognition sites and exhibited excellent performance for selective separation and purification of the ReO 4 − through adjusting the structure of imprinted cavities under different temperature. The maximum adsorption capacity was 0.1163 mmol/g at 35 °C, and the adsorption equilibrium was reached in 2 h. Meanwhile, the Re-TSICMs could not only presented an outstanding selectivity (adsorption selectivity coefficient ReO 4 − /MnO 4 − was 19.3), but also showed excellent desorption property (the desorption rate was 78.3%). What’s more, excellent cyclic adsorption-desorption performance was also observed. Conducting the adsorption at 35 °C and desorption at 25 °C aqueous solution, it could still remained 61.3% of the original adsorption capacity with the adsorption selectivity coefficient of 13.3 after ten adsorption/desorption cycles.
研究领域:
材料科学
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环境工程
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化学工程
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
Fangfang Niu,Gang Wu,Siyuan Lu,Xu Wan,Zhengcan Chen,Hongyi Tu,Zhenbin Chen,Xuxu Wei,Xinyu Zhao
In this study, an intelligent block temperature-sensitive PDEA- b -P (DEA- co -AM) was prepared by RAFT polymerization first. Subsequently, it was introduced into the preparation process of ReO 4 - -TPIP to investigate its effect on selective separation performance. ReO 4 - -TPIP was prepared by Pickering-like HIPE polymerization, which could form a porous interoperable network structure and further accelerate the mass transfer rate of ReO 4 - significantly. The structure and morphology of ReO 4 - -TPIP were characterized by FTIR, SEM-EDS, BET, and ICP-AES. Results documented that ReO 4 - -TPIP could reach adsorption equilibrium at 31 °C after 120 min, the maximum adsorption capacity ( Q ) was 0.16 mmol/g, and the desorption efficiency ( D ) arrived at 82.21%, with 3.26 of selective adsorption coefficients in equal molar concentration solution of ReO 4 - and MnO 4 - . After 11 repeated adsorption-desorption recycles, the adsorption capacity and desorption efficiency remained at 79.10% and 71.01% of their initial value, respectively. More surprisingly, the purity of Re in solution rose from 35.41% to 62.82% after 1 adsorption-desorption recycle of ReO 4 - -TPIP in the secondary leaching solution of high-temperature alloys. This demonstrates the promising development of this material for the industrial separation and purification of Re.
研究领域:
材料科学
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环境化学
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工业化学
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高影响因子
Advanced Science
·
2019
·Vol. 6
·期 17
·1900381
·
IF 15.804
Jian Lin,Lin Zhu,Zenghui Yue,Chuang Yang,Wei Liu,Thomas E. Albrecht-Schmitt,Jian-Qiang Wang,Shuao Wang
Various types of polyoxometalates (POMs) have been synthesized since the 19th century, but their assortment has been mostly limited to Groups 5 and 6 metals. Herein, a new family of POMs composed of a carbon group element as the addenda atoms with two distinct phases, LnPbOClO 4 -1 (Ln = Sm to Ho, Y) and LnPbOClO 4 -2 (Ln = Er and Tm) is reported. Both structures are built from [Ln 6 O 8 ] rare-earth metal hexamers being incorporated in [Pb 18 O 32 ]/[Pb 12 O 24 ] polyplumbites, and unbound perchlorates as charge-balancing anions. Impressively, YPbOClO 4 -1 and ErPbOClO 4 -2 exhibit exceptional uptake capacities (434.7 and 427.7 mg g −1 ) toward ReO 4 − , a chemical surrogate for the key radioactive fission product in the nuclear fuel cycle 99 TcO 4 − , which are the highest values among all inorganic anion-exchange materials reported until now. The sorption mechanism is clearly elucidated and visualized by single-crystal-to-single-crystal structural transformation from ErPbOClO 4 -2 to a perrhenate-containing complex ErPbOReO 4 , revealing a unique ReO 4 − uptake selectivity driven by specific interaction within Pb···O-ReO 3 − bonds.
研究领域:
无机化学
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放射化学
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环境化学
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材料科学
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核燃料循环
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DOI
高影响因子
ACS Applied Polymer Materials
·
2026
·
IF 5.2
Zhifeng Nie,Hongxing He,Yi Zhang,Xiaodong Zhuang,Xiaoying Li,Ni Yang
Abstract Given the highly dispersed occurrence of rhenium in the natural environment, it is commonly encountered in conjunction with other minerals and primarily occurs as perrhenate ions (ReO4–) in the acidic waste solutions produced by nonferrous metallurgical operations. The advancement of techniques for the efficient, economical, and selective extraction of rhenium from metallurgical waste acids holds significant socio-economic value. In the present study, a functional polymer designated CY-PPZ, characterized by a conjugated amine structure, was synthesized via a one-pot reaction employing cyanuric chloride and piperazine as monomeric precursors, designed for the targeted adsorption of ReO4– ions. Experimental investigations revealed that CY-PPZ exhibited superior adsorption performance for ReO4– across a broad pH range (2–8), achieving adsorption equilibrium within 480 min and demonstrating a maximum adsorption capacity of 350.92 mg/g. The polymer also displayed remarkable selectivity and resistance to interference from competing ions, as evidenced by a distribution coefficient (Kd) of 14.34 L/g. Notably, in simulated metallurgical waste acid solutions characterized by elevated concentrations of competing anions, specifically with a molar ratio of ReO4– to NO3–, SO42–, and Cl– of 1:3000, the removal efficiency of ReO4– consistently exceeded 88.52%. Additionally, CY-PPZ exhibited excellent recyclability, retaining a removal efficiency of 90.20% after 8 successive adsorption–desorption cycles. Economic analysis indicated that each gram of CY-PPZ could yield an approximate socio-economic value of $26.866. Mechanistic insights obtained from XPS and DFT calculations confirmed that the primary adsorption mechanisms involved synergistic electrostatic interactions and chemical coordination between CY-PPZ and ReO4– ions. In summary, CY-PPZ emerges as a highly promising material for the selective, efficient, and cost-effective extraction of rhenium from metallurgical waste acid streams.
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DOI
高影响因子
ACS Applied Polymer Materials
·
2023
·
IF 5
Xingsheng Liu,Shengyuan Zhao,Wan Xu,Huijuan Zhang,Siyuan Lu,Zhenbin Chen,Fangfang Niu,Gang Wu
With decreasing global rhenium resources, it has become important to separate and purify rhenium in secondary resources, so a preparation strategy for a chitosan-comodified surface-grafted thermosensitive ion-imprinted composite membrane (CS-Re-TIICM) was developed in this work. The key of this design was that the two ends of a poly(N,N-diethylacrylamide) (PDEA) chain were grafted onto the imprinted polymer separating the layer matrix and the surface of the membrane, respectively, which aimed to improve the selectivity and desorption ratio of this material simultaneously. The structure and morphology of this material were characterized by FTIR and SEM, respectively. In addition, CS-Re-TIICM was applied to the secondary leaching solution of the high-temperature alloy to test the actual separation effect, and results showed that CS-Re-TIICM, possessing thermoresponsive recognition sites, and the structure of the imprinting cavity could be adjusted by temperature, which helped this material achieve good selective separation and purification performance for ReO4–. The maximum adsorption capacity was 0.1071 mmol/g at 35 °C. CS-Re-TIICM not only showed an excellent selectivity (separation ReO4–/MnO4– of 3.90 in the presence of interfering ion MnO4–) but also presented an excellent desorption performance (desorption ratio of 68.94%) and good reusability (adsorption capacity of 0.0425 mmol/g, desorption ratio of 59.13%, and separation degree of 1.24). When CS-Re-TIICM was applied to the secondary leaching solution of high-temperature alloys, the purity of Re was increased from 35.41% to 65.10% after one adsorption/desorption cycle, which depicted a prospective application in the industrialized separation of ReO4– from a complex environment.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2025
·
IF 3.7
Tangzheng Lu,Jiayi Feng,Yong Kang
The design of highly stable and efficient porous materials is crucial for physisorption-based separation of radioactive species ( 99 TcO 4 - /ReO 4 - ), serving as an alternative to current concentrate-storage-solidification treatment technologies. Herein, employing a covalent-ionic dual-crosslinking strategy with economical ionic compounds as reactive monomers, a novel cationic organic polymer (TJU-COP-1) was synthesized for the first time via facile radical polymerization for 99 TcO 4 - /ReO 4 - sequestration. TJU-COP-1 demonstrates exceptional adsorption capacity, kinetics and selectivity ( K d ) for 99 TcO 4 - /ReO 4 - (861.87 mg·g –1 , K d = 5.0 × 10 5 ml·g -1 ), achieving adsorption equilibrium within merely 1 min. Notably, TJU-COP-1 maintains adsorption efficiency as high as 96.25% after five adsorption-desorption cycles. The TJU-COP-1 showed high stability after acid (3 mol·L –1 HNO 3 ), alkali (3 mol·L –1 NaOH) and radiation (200 kGy 60 Co γ) treatment. More significantly, TJU-COP-1 demonstrated robust and promising removal performance in complex solution, achieving 98.55% efficiency for 99 TcO 4 - /ReO 4 - amid high concentrations of competing anions and an excellent 72.11% removal in simulated Hanford LAW waste solution. Combined experimental characterization and density functional theory theoretical validation confirmed that the adsorption mechanism involves a synergistic combination of electrostatic interactions and anion exchange. This study illustrates that TJU-COP-1 has great potential for practical application in the capture of 99 TcO 4 - /ReO 4 - , and provides a new approach to the design of high-performance adsorbents for the treatment of nuclear wastewater.
研究领域:
环境科学
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材料化学
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核化学
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吸附技术
·
聚合物化学
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DOI
高影响因子
Journal of Physical Chemistry C
·
2024
·
IF 3.3
Tianyao Pei,Zheng Tang,Dequan Jiang,Chen Li,Yingying Ma,En Chen,Binbin Yue,Yonggang Wang
Sr8(Al12O24)(CrO4)2 (SACR) is a kind of aluminate sodalite, which has been found to have a ferroelectric phase transition near room temperature. The main reason for a phase transition is the freezing of anionic group orientation caused by temperature reduction. The β-cage based on the AlO4 framework with abundant vacancies also brings new possibilities for introducing functional ions. For effectively optimizing its properties, chemical doping is a common modification method. In this study, we reported the (Sr1–xCdx)8(Al12O24)(CrO4)2 series doped at the central cationic site of β-cage and the Sr8(Al12O24)(Cr1–xRexO4)2 series doped at the central anionic site of the molecular cage and compared the effect of doping at different point sites on the phase transformation properties of SACR. Among them, the cationic site doping is not complete and does not affect the phase transition temperature, and the phase transitions are still first-order phase transitions with thermal effect. For the doping of the anionic site, a complete doping series is achieved, and the new end compound Sr8(Al12O24)(ReO4)2 is synthesized. Compared with Sr8(Al12O24)(CrO4)2, the phase transition behavior of Sr8(Al12O24)(ReO4)2 is obviously different, and there is no orthorhombic–tetragonal phase transition between 103 and 450 K.
研究领域:
材料科学
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固态化学
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铁电材料
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晶体工程
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DOI
高影响因子
DESALINATION
·
2026
·
IF 9.9
Xiangjun Liao,Huining Zhang,Yuxiao Tian,Guangtai Zheng,Shijian Pan,Jing Chen,Yuri A. Ustynyuk,Valentin G. Nenajdenko,Yuan Liao,Cheng-peng Li
The sustainable and efficient treatment of high-salinity radioactive wastewater containing 99 TcO 4 − represents a critical challenge, driven by the severe environmental risks of 99 TcO 4 − and the inadequacy of existing treatment technologies. Here, we introduced membrane distillation (MD) as a novel approach for such wastewater and developed a robust superhydrophobic membrane (# PVDF-PN ) that simultaneously resisted wetting and scaling while overcoming the conventional selectivity-permeability trade-off. The # PVDF-PN was fabricated through in situ hydrolysis and polymerization of trichloromethylsilane (TCMS) on hydroxylated polyvinylidene fluoride (PVDF), yielding a surface densely covered with low-surface-energy polysiloxane nanofilaments. This unique nanofilament architecture significantly enhanced the gas-liquid interfacial area for vapor evaporation, without compromising pore integrity or permeability due to surface modification. When tested with challenging feeds containing surfactants or supersaturated gypsum, # PVDF-PN maintained a stable flux of ∼33.0 kg·m −2 ·h −1 and near-complete salt rejection (>99.99%), outperforming both unmodified # PVDF and fluorinated silica-coated # PVDF-FS . Its exceptional performance was attributed to a high liquid entry pressure, an elevated energy barrier for crystal nucleation, and reduced liquid-solid contact area and interaction time. Importantly, in long-term MD treatment of simulated 99 TcO 4 − /ReO 4 − -laden high-salinity wastewater, # PVDF-PN achieved non-detectable effluent concentrations of target oxyanions, demonstrating its potential as a reliable and efficient solution for radioactive wastewater management and emergency response.
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高影响因子