SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Haotian Liu,Chuang Wang,Yi Yang,Minghui Gao,Aifang Xue,Hao Chen,Xing Ding
The preferential degradation of specific harmful organic pollutants in photocatalytic processes is critically important, yet remains a significant challenge due to the uncontrolled nature of reactive species, particularly those with high oxidation potentials such as •OH and h + . In this work, we designed an iodine-doped Bi 2 MoO 6 semiconductor to establish a system for photo-induced H 2 O 2 generation. The incorporation of iodine led to a steady enhancement in the selective photo-degradation of para -substituted phenolic pollutants, known precursors to carcinogenic p-benzoquinones, facilitated by the activation of iodine radicals through H 2 O 2 . This system exhibited impressive photo-degradation (96 %) and mineralization efficiency for acetaminophen (APAP), along with superior environmental applicability. It also demonstrated selectivity in degrading phenols with para -substitutions. The in-situ generation and activation of H 2 O 2 and •I were identified as the crucial pathways in this photocatalytic system. This work provides a novel modification path to accomplish the simultaneous generation and utilization of H 2 O 2 in the photocatalytic system and ultimately makes a remarkable performance for the targeted remediation of environmental pollutants.
研究领域:
环境科学
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光催化材料
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污染治理
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DOI
高影响因子
Science China-Chemistry
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2024
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IF 10.4
Tai Bo,Li Baoyu,He Linwei,Ma Zhonglin,Lin Shujing,Zhang Mingxing,Chen Junchang,Wu Fuqi,Chen Long,Dai Xing,Ma Fuyin,Chai Zhifang,Wang Shuao
The development of adsorbent materials for effective capture of radioactive iodomethane (CH 3 I) from the off-gas of used nuclear fuel reprocessing, remains a significant and challenging line of research because currently state-of-art adsorbents still suffer from low binding affinity with CH 3 I. Here, we proposed a brand-new adsorption topological structure by developing a 2D interdigitated layered framework, named SCU-20, featuring slide-like channel with multiple active sites for CH 3 I capture. The responsive rotating-adaptive aperture of SCU-20 enables the optimal utilization of all active sites within the pore for highly selective recognition and capture of CH 3 I. A record-breaking CH 3 I uptake capacity of 1.84 g/g was achieved under static sorption conditions with saturated CH 3 I vapor. Both experimental and theoretical findings demonstrated that the exceptional uptake of SCU-20 towards CH 3 I can be attributed to the confined physical electrostatic adsorption of F sites, coupled with the chemical nitrogen methylation reaction with uncoordinated N atoms of pyrazine. Moreover, dynamic CH 3 I uptake capacity potentially allows for the capture of CH 3 I in simulated real-world off gas reprocessing conditions. This study highlights the potential of SCU-20 as a promising candidate for efficient capture of iodine species and contributes to the development of effective solutions for radioactive iodine remediation.
研究领域:
化学
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环境科学
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核能工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Xin Wu,Xue Yang,Le Yu,Xiao Chun Chen
Aqueous zinc (Zn)-iodine (I 2 ) batteries (ZIBs) are promising large-scale energy storage systems with high safety and low cost. However, the practical application of ZIBs is hindered by the dissolution of I 3 - ions, which leads to the shuttle effect and the loss of active iodine. Herein, we adopt an electrolyte modification strategy using two imidazolium-based ionic liquids (1-butyl-3-methylimidazolium iodide ([BMIM]I) and 1-ethyl-3-methylimidazolium iodide ([EMIM]I)) as electrolyte additives to restrain the dissolution of I 3 - ions and enhance the performance of ZIBs. To be specific, the imidazole rings in [BMIM] + and [EMIM] + can be used as the proton sources, promoting the conversion of imine to protonated amines –NH + = in the polyaniline and subsequent adsorption of I 3 - ions. Therefore, the dissolution of I 3 - ions and shuttle effect are prevented, facilitating the reaction kinetics of cathode. As a proof of concept, the ZIB using [BMIM]I and [EMIM]I as electrolyte additives demonstrates remarkable cycling performance (72.2 % capacity retention after 1000 cycles) at a high current density of 20 mA cm −2 .
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
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IF 7.139
Ke Zhang,Xiaoling Li,Liping Chang,Weiren Bao,Hui Wang
Hydrogen sulfide (H 2 S) emitted from oil industry's hydrotreating processes can be converted into hydrogen and used back to the same processes through a H 2 S splitting cycle, where the Bunsen reaction and HI decomposition are two participating reactions. To overcome the difficulties and complications posted in the scaling up of the cycle, direct electrolysis of the Bunsen reaction product solution was proposed and has been studied in a batch electrolysis cell in our earlier work. This paper studies the direct electrolysis using a customer-made, continuous-flow electrolysis cell. The effects of the operating parameters including the current density , the entering HI concentration and flow rate of the anolyte, the toluene to aqueous phase ratio and stirring speed in anolyte cell, the H 2 SO 4 concentration and circulation rate of the catholyte on the performing parameters such as the conversion of iodide ions, the yield of iodine transferred to toluene, and the anodic and cathodic current efficiencies for iodide conversion and hydrogen production were carefully investigated. The results show that the cathodic current efficiency for hydrogen production is nearly 100% for all the runs and that the anodic current efficiency for iodide ion conversion to iodine is relatively low (20%–70%) and varies with the changes in operating parameters. Running at high levels of the current density, the volumetric ratio of toluene to aqueous phase in anolyte, or the stirring speed in anolyte, and low levels of the entering concentration of I − in anolyte or the flow rate of anolyte in electrolysis operation are in favor of having a high iodide conversion and high I 2 -toluene yield. Iodide anions at a few mmol L −1 level (a few thousandths of the entering concentration) are found in the cathodic chamber caused by its diffuse against the electric field and the proton exchange membrane . The continuous, direct electrolysis of the Bunsen product solution can be considered being adapted in the sulfur-iodine (S–I) water splitting cycle for hydrogen production.
研究领域:
化学工程
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能源科学
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DOI
高影响因子
Journal of Flow Chemistry
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2021
·Vol. 12
·期 1
·41-49
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IF 2.786
Lan Zhou,Lu Yangcheng
Benzyl iodide, an important organic synthesis intermediate, has high reaction activity as well as high commercial value due to its weakest carbon-halogen bond. However, the development of direct iodination of toluene for benzyl iodide is limited by the fact that the C-I bond is easily decomposed under heat or light. In this work, the photoiodination of toluene to synthesize benzyl iodide in the I 2 /PhI(OAc) 2 / t BuOH system was carefully investigated in the flow photoreactor under LEDs irradiation. The reaction window suitable for the reaction kinetic characteristics recognition was revealed with the considerations of the effects of various parameters including light color, light intensity, reaction temperature, residence time, and usage of each substrate. And an optimized result is to achieve 95.83 % of yield and over 99 % of selectivity under a red light with 2.05 mW/cm 2 of light intensity at 80 o C after 15 min reaction. The reaction kinetic model coupling the iodination reaction (photo and thermal reaction) with the decomposition reaction is established, which fits well the experimental results and provides fundamentals for process design and optimization. Graphical abstract
研究领域:
有机化学
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化学工程
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DOI
高影响因子
RSC Advances
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2020
·Vol. 10
·期 24
·14360-14367
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IF 3.119
Trinh Dinh Dinh,Dongxiang Zhang,Vu Ngoc Tuan
The effective adsorption of radioactive iodine is greatly desirable, but is still a significant challenge. In this manuscript, we report the synthesis of a bismuth-modified zinc aluminium layered double hydroxide (BiZnAl-LDH) via a co-precipitation method for the highly efficient absorption of iodine. Based on the robust chemical attraction between Bi and I2, BiZnAl-LDH exhibited highly effective iodine capture. Furthermore, to evaluate BiZnAl-LDH as an effective sorbent, it was characterized via X-ray powder diffraction (XRD), scanning electron microscopy-energy dispersion spectroscopy (SEM-EDS), and Fourier-transform infrared spectroscopy (FITR). In addition, to determine the morphology and iodine adsorption properties of BiZnAl-LDH, several studies were conducted. Through experiments, its elemental composition and vibration before and after iodine adsorption were analyzed via EDS and X-ray photoelectron spectroscopy (XPS). During the capture process, I2 is reduced to I− by the intercalated Bi3+ via chemical adsorption, and the maximum adsorption capacity of BiZnAl-LDH for iodine reached up to 433 mg g−1, which had a surface area, average pore diameter, and pore volume of 36.259 m2 g−1, 2.374 nm, and 0.128 m3 g−1, respectively. Compared with several previous sorbents for iodine adsorption, BiZnAl-LDH exhibited an iodine adsorption of approximately two times that of the commercial Ag-exchange zeolite X, and furthermore BiZnAl-LDH is cost-effective. Thus, the substantial iodine capture by BiZnAl-LDH indicates that it is a capable sorbent for the effective elimination of radioactive iodine from reprocessing plant emissions.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
CATALYSIS LETTERS
·
2024
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IF 2.3
Yu Pengxin,He Jianshen,Du Mingzhi,Lai Ying,Peng Yang,Yu Fuqing,Wang Hongmin,Yang Weiran
Disproportionation of alcohols to the corresponding alkanes and aldehydes/ketones is an important reaction, especially for biomass valorisation. Previously, we reported for the first time that hydroiodic acid can be used as an efficient catalyst for the alcohol disproportionation reaction, and the interconversion between hydroiodic acid and iodine is the key step for hydrogen transfer. As a continuation of our previous work, this work mainly focused on the mechanistic study involved and studied the difference between hydroiodic acid or molecular iodine as the catalyst for the disproportionation of alcohols. Density Functional Theoretical calculation indicated the oxidation step was a synergistic reaction process through the iodine effect on oxygen-hydrogen bond, which was proved by the characteristic oxygen-iodine bond captured by in-situ Attenuated Total Reflectance Fourier Transform Infrared. A non-polar solvent was preferable for the reaction with iodine. Addition of small amount of water was shown to be beneficial for the reaction, because water promoted Brønsted acidity of hydroiodic acid and accelerated the rate-determining step. Finally, we showed that the system was also applicable to various benzyl, allyl alcohols, and some heterocyclic alcohols. Graphical Abstract
研究领域:
化学
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催化反应机制
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Hao Zou,Lei Liao,Gaoling Liang,Wanjiang You,Shilong Song,Ning Pan,Hao Lei,Weimin Li,Xiaoqiang Wang
The silver-based materials are widely used in nuclear fuel reprocessing plant for iodine capture. They are powerful but expensive. In this paper, the mercury-bismuth co-modified silica gel (Hg-Bi-Silica gel) was studied and tried to displace the silver-based materials. Firstly, the Hg-Bi-Silica gel was prepared through activating, impregnating and drying. Mercury and bismuth existed as Hg(OH)NO 3 and [Bi 6 O 5 (OH) 3 ](NO 3 ) 5 ·2H 2 O in Hg-Bi-Silica gel, respectively. Secondly, the iodine adsorption performances of Hg-Bi-Silica gel were investigated. The static trapping capacity of I 2 and CH 3 I was 209.1 ± 1.7 mg/g and 151.0 ± 6.9 mg/g, respectively, which was better than that of the commercial silver-based materials (148.6 ± 3.5 mg/g and 132.7 ± 3.0 mg/g). The dynamic adsorption efficiency of CH 3 131/127 I was 99.996 %, which was closed to that of the commercial silver-based materials (99.990 %). Thirdly, the possible mechanism for iodine capture in the Hg-Bi-Silica gel system was proposed. I 2 was captured by Hg-Bi-Silica gel mainly in the form of HgI 2 and Hg(IO 3 ) 2 , however, CH 3 I was captured by Hg-Bi-Silica gel mainly in the form of HgI 2 . Furthermore, [Bi 6 O 5 (OH) 3 ](NO 3 ) 5 ·2H 2 O was cooperated with Hg(OH)NO 3 on capturing iodine. Finally, the stabilities of Hg-Bi-Silica gel were evaluated. The Hg-Bi-Silica gel showed excellent thermal stability, NO x -corrosion resistance and irradiation resistance. In summary, the more cost-effective Hg-Bi-Silica gel was a potential effective substitution of silver-based materials.
研究领域:
核化学与放射化学
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环境科学
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产品关联
DOI
高影响因子
Water Supply
·
2020
·Vol. 21
·期 3
·1016-1024
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IF 0.9
Dong Zijun,Li Mu,Chen Meifen,Gu Yurong,Jiang Chengchun,Sun Feiyun
The transformation of iodide (I − ) and hypoiodous acid (IO − ) by Fe (II)-activated peroxydisulfate (PDS) in the presence of natural organic matter (NOM) was investigated. In the water of a reservoir in Shenzhen, four kinds of organic matter were detected: iodoform > diiodo-bromomethane > dibromo-iodomethane > dichloromethane. As pH increased from 3 to 10, I − conversion rate decreased from 31.0% to 11.0%. There is basically no iodic acid ( ) generated under alkaline conditions, probably due to these organic matters. When PDS concentration is low, PDS can oxidize part of I − to IO − , and the oxidation of I − into reaction and continued oxidation reaction exist at the same time, so some is generated in the system. As the proportion of Fe (II) increases, the generation rate of gradually increases. When Fe 2+ /PDS is 1:5, 2:5, and 3:5, the conversion rates of are 4.7%, 6.5%, and 8.4%, respectively. There are two main reasons for this: (i) the reaction of IO − produced in the system with humic acid (HA) inhibits the further conversion of IO − to ; (ii) both HA and I- in the system can react with PDS, resulting in a reduction in the oxidation rate of I − . Formation of I-DBPs by Fe (II)/PDS process in real water was evaluated. I-DBPs generation in various reaction conditions was examined. Existence of HA showed apparent inhibition on IO 3 − generation.
研究领域:
环境化学
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水处理技术
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高级氧化工艺
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消毒副产物生成
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DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
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IF 14.7
Shen Jiafu,Huang Xi,Dai Yu,Zhang Xiaojin,Xia Fan
Low-grade heat is abundant and ubiquitous, but it is generally discarded due to the lack of cost-effective recovery technologies. Ion thermoelectric cells are an affordable and straightforward approach of converting low-grade heat into usable electricity for sustainable power. Despite their potential, ion thermoelectric cells face challenges such as limited Seebeck coefficient and required series integration. Here, we demonstrate that the N-type and P-type conversion of ion thermoelectric cells can be achieved through the phase transition of temperature-sensitive hydrogel containing the triiodide/iodide redox couple. Through the strong interaction between the hydrophobic region of the hydrogel and triiodide, the hydrophobic side selectively captures triiodide and the hydrophilic side repels triiodide, raising the concentration difference of triiodide and thereby increasing the Seebeck coefficient. Specifically, the Seebeck coefficient of the N-type ion thermoelectric cells is 7.7 mV K −1 , and the Seebeck coefficient of P-type ion thermoelectric cells is −6.3 mV K −1 (Δ T = 15 K). By connecting 10 pairs of the N-type and P-type ion thermoelectric cells, we achieve a voltage of 1.8 V and an output power of 85 μW, surpassing the reported triiodide/iodide-based ion thermoelectric cells. Our work proposes a phase transition strategy for the N-P conversion of ion thermoelectric cells, and highlights the prospect of series integrated hydrogel ion thermoelectric cells for low-grade heat harvesting.
研究领域:
材料科学
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能源技术
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化学工程
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产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2025
·Vol. 49
·期 9
·3536-3544
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IF 2.5
Yang Shen,Jingbo Zhang,Yue Wang,Xuemei Li
The development of covalent organic polymers (COPs) to remove iodine in vapor and from solutions is highly desirable for the sustainable production of nuclear energy. Herein, we reported the successful synthesis of an ionic COP (iCOP) via a post-synthesis functionalization approach. Subsequently, a magnetically responsive iCOP (IMF-COP-Fe) was obtained using a simple double-solvent reduction method to facilitate separation. It is noteworthy that IMF-COP-Fe could rapidly achieve solid–liquid separation under the influence of an external magnetic field, with a magnetic recovery rate of 91.89%. The rational design endowed IMF-COP-Fe with affinity sites for removal of iodine in vapor and from solutions. Experimental findings demonstrated that the adsorption capacity of IMF-COP-Fe towards iodine vapor was 2.46 g g−1 at 75 °C. Concurrently, the iodine removal rate of IMF-COP-Fe in 700 mg L−1 iodine–cyclohexane solution reached 80.56%. Even after four adsorption–desorption experiments, it still maintained good adsorption performance. Furthermore, the maximum adsorption capacity of IMF-COP-Fe for iodide ions was found to be 109.9 mg g−1. The present study proposes original concepts for the rational molecular design of materials for simultaneous removal of various forms of radioactive iodine.
研究领域:
材料科学
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环境科学
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核技术
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产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2024
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IF 5.1
Guoyang Xu,Jing Lin,Xiangqian Gao,Chao Yu,Chengchun Tang,Yang Huang
Development of effective iodine capture materials and techniques is crucial for addressing the diverse applications of iodine and its significance in various contexts, including nuclear pollution control. This study presents the creation of a new 3-Aminopropyltriethoxysilane (APTES)-modified boron nitride (BN) aerogel designed for effective iodine capture. The internal structural units of BN aerogel , specifically the one-dimensional BN fibers, have been successfully functionalized with amine groups, resulting in the formation of an amine-rich SiO x capping layer on the surface of these fibers. The APTES modification not only establishes a stable connection within the internal BN fibers network but also imparts the material with a significant number of iodine capture sites. The resulting aerogel demonstrates an impressive iodine vapor capture capacity of 313.64 wt% at 350 K and atmospheric pressure, and up to 1028.96 mg/g in iodine/n-hexane solution, surpassing the capabilities of pure BN aerogel and most existing iodine capture materials. The excellent iodine capture performance of APTES-modified BN aerogel suggests its promising potential for future applications in iodine capture.
研究领域:
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
危险品化学品经营许可证（带存储）