Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Liu Tao,Lan Cheng,Tang Min,Li Mengxin,Xu Yitao,Yang Hangrui,Deng Qingyue,Jiang Wenchuan,Zhao Zhiyu,Wu Yifan,Xie Heping
Seawater direct electrolysis (SDE) using renewable energy provides a sustainable pathway to harness abundant oceanic hydrogen resources. However, the side-reaction of the chlorine electro-oxidation reaction (ClOR) severely decreased direct electrolysis efficiency of seawater and gradually corrodes the anode. In this study, a redox-mediated strategy is introduced to suppress the ClOR, and a decoupled seawater direct electrolysis (DSDE) system incorporating a separate O 2 evolution reactor is established. Ferricyanide/ferrocyanide ([Fe(CN) 6 ] 3−/4− ) serves as an electron-mediator between the cell and the reactor, thereby enabling a more dynamically favorable half-reaction to supplant the traditional oxygen evolution reaction (OER). This alteration involves a straightforward, single-electron-transfer anodic reaction without gas precipitation and effectively eliminates the generation of chlorine-containing byproducts. By operating at low voltages (~1.37 V at 10 mA cm −2 and ~1.57 V at 100 mA cm −2 ) and maintaining stability even in a Cl − -saturated seawater electrolyte, this system has the potential of undergoing decoupled seawater electrolysis with zero chlorine emissions. Further improvements in the high-performance redox-mediators and catalysts can provide enhanced cost-effectiveness and sustainability of the DSDE system.
研究领域:
能源科学
·
环境科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
Journal of Cleaner Production
·
2023
·
IF 11.1
Kang Li,Junjie Xie,Zhuonan Shi,Changli Min,Zichen Yin,Ruixin Ma,Shina Li
Rubidium and cesium are highly-priced and important rare alkali elements but they always co-exist with large amount of sodium and potassium in a complex system resulting very difficult and expensive to recover. Hexacyanoferrates (MHCFs) is one of the most efficient methods to separate Rb + and Cs + if we don't consider certain drawbacks such as too small particle size and too viscous liquids to be precipitated. In this study, a new kind of hexacyanoferrate, magnesium (II) hexacyanoferrate (RbCs–MgHCF) has been fabricated at room temperature and applied for the first time to recover Rb + and Cs + from high-salty solutions. Compared with traditional divalent transition elements, such as CuHCFs, ZnHCFs, NiHCFs, CoHCFs or FeHCFs, RbCs–MgHCF had excellent precipitation property and large particle size of about 300 nm. The structure, morphology and composition were characterized by Fourier transform infrared (FTIR), X-ray diffraction (XRD), Scanning electron microscopy (SEM), Inductively coupled plasma (ICP), and Energy dispersive spectroscopy (EDS). The effects of various factors (divalent metal cations, surfactant, Mg 2+ /(Rb + +Cs + ) mole ratio, pH value and titration rate) on the recovery of Rb + and Cs + were explored in 50 mL batch experiments. Scale-up experiment were conducted in 6 and 18 L. Results identified that deposition ratio for Cs + and Rb + were 99% and 95% among pH ranges of 4.0–11.0. The composition of RbCs–MgHCF was confirmed to be Rb 0.61 Cs 1.20 K 0.17 Mg 1.01 Fe(CN) 6 by ICP and EDS and the synthesis mechanism of RbCs–MgHCF is proposed.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ChemistrySelect
·
2025
·Vol. 10
·期 8
·e202406007
·
IF 2
Chenxi Li,Kang Li,Shina Li,Ruixin Ma
Graphical In this study, copper hexacyanoferrate (CsRb–CuHCF) was used as a precipitant. Results demonstrated that CsRb–CuHCF can efficiently separate Rb + and Cs + from the high-salty solutions. The enrichment factor was up to 384 before and after precipitation. The precipitant reacts first with Cs + and then gradually with Rb + and can be used for the separation of Cs + and Rb + from each other. Cesium (Cs) and rubidium (Rb) are important rare alkali metal elements that are scarce and dispersed in nature. They often coexist with high amounts of Na + and K + . In this study, copper hexacyanoferrate (CuHCF) was used as a co-precipitant to enrich Cs + and Rb + in a high-salt solution. The effect of parameters, such as type and dose of divalent metal ions, solution pH, material dropping speed, reaction time, and temperature, was investigated for the recovery rate of Cs + and Rb + . Results showed that the recovery rates of Cs + and Rb + were 99.78% and 88.84% at the optimal Cu 2+ /(Cs + +Rb + ) molar ratio of 0.5, respectively. The reaction could be completed within 10 min in pH 3–8. The detailed characterization of the Cs + and Rb + containing co-precipitants, CsRb–CuHCF, confirm a general formula of Cs 1.09 Rb 0.81 K 0.16 Cu 0.97 Fe(CN) 6 . The (Cs + +Rb + )/(Na + +K + ) increased significantly from 0.074 to 28.47 before and after precipitation, which realized the effective enrichment of Cs + and Rb + . Studies of the precipitation reaction mechanism showed that the precipitant reacted first with Cs + and then with Rb + . This process offers a promising avenue for the enrichment and separation of Cs + and Rb + from high-salty solutions.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Mining Metallurgy & Exploration
·
2024
·Vol. 41
·期 2
·1089-1097
·
IF 1.5
Junjie Xie,Kang Li,Zhuonan Shi,Changli Min,Shina Li,Zichen Yin,Ruixin Ma
Cesium and rubidium were effectively separated by zinc ferrocyanide coprecipitation method, and the effect of precipitant addition amount on the separation of cesium and rubidium was studied. Under the conditions of Zn/Cs molar ratio of 0.45 and Zn/Fe molar ratio of 1, the precipitation rate of cesium is 84.01% and the separation factor of Cs/Rb is 164.65. The thermogravimetric curves of the sediment were measured, and the effects of roasting temperature, roasting time, and leaching liquid/solid ratio on the extraction of cesium were studied. Almost all of the cesium was extracted under optimal conditions: roasting temperature of 600 °C, roasting time of 3 h, leaching temperature of 25 °C, leaching time of 0.5 h, and liquid/solid ratio of 5:1 mL/g. After the leaching process, the leach liquor with high concentration of cesium of 80.17 g/L was obtained. Finally, the leach liquor was further purified by solvent extraction, and the purity of the cesium chloride product reached 99.66%. Graphical Abstract
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2022
·Vol. 331
·期 6
·2655-2665
·
IF 1.754
Li Tingting,Wang Fang,Xia Liangshu
Uranium, as a highly toxic radioactive contaminant existing in mine wastewater and contaminated groundwater, has sparked widespread alarm in recent years. This work demonstrates the technological possibility of recovering uranium from aqueous solutions using potassium titanium ferrocyanide (KTiFC). The adsorption behavior, kinetics, isotherms, and thermodynamic investigations were systematically examined. The maximum capacities were achieved at pH3.8, and KTiFC was proven to be stable across a wide pH range. The adsorption process was best represented by a pseudo-second order rate equation and the Langmuir isotherm model, with 90% of the uranium eliminated in 60 min. The adsorption process was endothermic and spontaneous, adsorption efficiency of uranium is highly related to water temperature. The integrated analysis of EDS, ICP-OES, FTIR and XPS suggested that chemisorption combined with ion exchange between K and U can describe the adsorption mechanism of uranium sorption on KTiFC. This study points the way toward developing effective and low-cost materials with practical functionality for uranium extraction from polluted water.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Hao Fang,Lu Yang,Jie Ni,Shanshan Feng,Wenhao Jia,Na Li,Xiaoyi Ma,Zhengwei Zhou,Yao Zhang,Sheng Feng
This study developed an innovative adsorbent—cobalt ferrocyanide/ZIF-67/aged garbage humus soil aerogel (PBA/ZIF-67/AARH aerogel)—specifically designed for the effective removal of cesium ions (Cs) from radioactive wastewater. The aerogel exhibited a maximum adsorption capacity of up to 51.92 mg/g, maintaining excellent Cs adsorption performance even in complex aquatic environments that contain other ions and dissolved organic matter (DOM). The experimental results showed that the adsorption effect of PBA/ZIF-67/AARH aerogel was the best when the dosage of PBA/ZIF-67/AARH aerogel was 0.01 g and pH value was 5. The adsorption capacity was 29.75 ± 0.5 mg/g. At the same time, PBA/ZIF-67/AARH aerogel has good regeneration stability. After five sorption-desorption cycles, the adsorption capacity is 20.1 ± 0.3 mg/g, and the Cs removal rate remains at 84.5 ± 0.5%. The PBA/ZIF-67/AARH aerogel also has a large specific surface area, reaching 30.7950 m 2 /g. Experimental analyses indicated that the Cs removal process aligns with both the Langmuir adsorption model and pseudo-second-order kinetics, revealing key mechanisms for adsorption efficiency, including ion exchange, functional group complexation, and the synergistic effects of cross-linking. This research provides a novel solution for the efficient removal of Cs, establishing a solid theoretical and practical foundation for future applications in pollution water treatment technologies. It holds significant potential for environmental protection and profound implications for human health.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Yaqin Rong,Shuai Li,Junjian Niu,Zhongde Wang,Xiaogang Hao,Chengwen Song,Tonghua Wang,Guoqing Guan
Radioactive cesium ( 137 Cs) ions exhibit high-energy gamma radiation and long half-life. When they enter water body, serious environmental problems and damage to the human body are always generated. Herein, an electroactive composite membrane was facilely prepared by uniformly deposition of nickel hexacyanoferrate (NiHCF) nanoparticles on the surface and inner wall of coal-based tubular carbon membrane (CTCM) for rapid and selective separation of Cs + from wastewater. This NiHCF incorporated CTCM tube exhibited an extremely high removal rate (over 99.99%) over a long period. Meanwhile, it also demonstrated extreme Cs + selectivities even in the solutions with high coexisting ion concentrations (e.g., Cs + :Na + = 1:99, Cs + :K + = 1:99). The rapid and selective Cs + uptake/release should be attributed to the better dispersion of NiHCF nanoparticles with high selectivity to Cs + in the CTCM tube, which reduced the mass transfer distance, increased fluid turbulence and accelerated mass transfer rate. It is expected that such a NiHCF incorporated CTCM tube could be a promising alternative of conventional materials for the separating of radioactive Cs + ions.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 20
·7147
·
IF 4.6
Xiafei Gao,Mengyue Gao,Xueping Yu,Xiaoyong Jin,Gang Ni,Juan Peng
The very slow anodic oxygen evolution reaction (OER) greatly limits the development of large-scale hydrogen production via water electrolysis. By replacing OER with an easier urea oxidation reaction (UOR), developing an HER/UOR coupling electrolysis system for hydrogen production could save a significant amount of energy and money. An Al-doped cobalt ferrocyanide (Al-Co2Fe(CN)6) nanocube array was in situ grown on nickel foam (Al-Co2Fe(CN)6/NF). Due to the unique nanocube array structure and regulated electronic structure of Al-Co2Fe(CN)6, the as-prepared Al-Co2Fe(CN)6/NF electrode exhibited outstanding catalytic activities and long-term stability to both UOR and HER. The Al-Co2Fe(CN)6/NF electrode needed potentials of 0.169 V and 1.118 V (vs. a reversible hydrogen electrode) to drive 10 mA cm−2for HER and UOR, respectively, in alkaline conditions. Applying the Al-Co2Fe(CN)6/NF to a whole-urea electrolysis system, 10 mA cm−2was achieved at a cell voltage of 1.357 V, which saved 11.2% electricity energy compared to that of traditional water splitting. Density functional theory calculations demonstrated that the boosted UOR activity comes from Co sites with Al-doped electronic environments. This promoted and balanced the adsorption/desorption of the main intermediates in the UOR process. This work indicates that Co-based materials as efficient catalysts have great prospects for application in urea electrolysis systems and are expected to achieve low-cost and energy-saving H2production.Keywords:hydrogen;urea oxidation;electronic structure;energy-saving;cobalt ferrocyanide
研究领域:
电化学
·
材料科学
·
能源工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2015
·
IF 2.729
Xiaoli Luo,Jianbin Pan,Kemei Pan,Yanyan Yu,Anni Zhong,Shanshan Wei,Jin Li,Jiayan Shi,Xinchun Li
Hydrazine and nitrite are well known as carcinogenic substances, which however, are commonly used in chemical industry and food processing. Monitoring of such two species in water and food is necessary. Here, we report a convenient electroanalytical method for detection of hydrazine and nitrite by facile preparation of graphene–cobalt hexacyanoferrate nanocomposite through a two-step electrode surface functionalization. The morphology and constituent of the prepared nanocomposite were characterized by scanning electron microscopy, transmission electron microscopy, and X-ray photoelectron spectroscopy. Cyclic voltammetry was used to profile the electrochemical behaviors of hydrazine and nitrite, revealing the synergetic electrocatalytic function of reduced graphene oxide and cobalt hexacyanoferrate nanoparticles. This was confirmed by the decreased oxidation overpotentials and increased current response of the target analytes, and thus offered a premise for electroanalysis. The quantitative measurements were carried out by amperometry and differential pulse voltammetry, respectively. Moreover, the analytical utility was demonstrated by determination of water samples and pickled food; the average recovery was found to be from 92.2% to 108%, with the relative standard deviation (RSD) less than 7.8%. The present method opens an avenue for detection of potential carcinogens in relation to environment and food territory.
研究领域:
环境科学
·
食品安全
·
分析化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Pingping Dong,Xiaoxu Jing,Yungui Li,Yi Shen,Qingqing Li,Qile Fang
Phosphorus (P) discharge is well recognized as the chief culprit of eutrophication and algal blooms. It is of pressing need to remove excessive phosphorus to protect the important watershed. Lanthanum (La) based materials are one type of attention-grabbing adsorbent due to their superior affinity to phosphate. Here, a La-Fe cyanometallate (CM) framework with a novel “twin lotus flower” structure was synthesized and rich hierarchical pores were fabricated via pyrolysis. The resultant “twin lotus flower” oxide of LaFe CM-500 was demonstrated to be a high-performance adsorbent for phosphate removal with a saturated capacity as high as 45.03 mg P/g. It also possessed superior removal ability for the stubborn low concentration of P pollution. The abundant hierarchical pores (from macropore to micropore) render a rapid diffusion of phosphate on the LaFe CM-500. The La components on porous adsorbent were verified to be the key active sites that form stable LaPO 4 via a ligand exchange process. The effects of solution conditions (temperature, pH, co-existing ions, and humic acid) were also investigated, and a high selectivity for phosphate adsorption enables the as-prepared “twin lotus flower” adsorbent to be competitive in practical water body treatment.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROANALYSIS
·
2011
·Vol. 23
·期 12
·2870-2877
·
IF 2.721
Qin Qian,Ping Yu,Hanjun Cheng,Xiang Wang,Lifen Yang,Lanqun Mao
Quantification of hygroscopicity of ionic liquids (ILs) is of great importance in both fundamental studies and practical applications of ILs. This study demonstrates an electrochemical method for effectively quantifying the hygroscopicity of ILs through electrochemically monitoring water contents absorbed into ILs. The measurements of water content absorbed into the ILs are performed with square wave voltammetry (SWV) based on the water-induced enhancement of diffusion of solution-dissolved potassium ferricyanide (K 3 Fe(CN) 6 ) redox probe. For demonstration, two kinds of ILs with different hygroscopicity (i.e., hydrophilic Bmim + Gly − and hydrophobic Bmim + PF 6 − ) are employed in this study. The dissolution of K 3 Fe(CN) 6 redox probe into ILs is found to have little effect on the hygroscopicity of ILs. The hygroscopicity of ILs is thus able to be quantified by monitoring water content absorbed into ILs as a function of time when ILs are stored at room temperature and standard atmospheric pressure under 55 % relative humidity (RH). Under the conditions employed in this study, the hygroscopicity of Bmim + Gly − and Bmim + PF 6 − is determined to be 1.33 M per hour and 0.05 M per hour, respectively, which are almost consistent with those measured with Karl Fischer titration under the same conditions. The electrochemical method demonstrated in this study is experimentally simply and environmentally benign and may be potentially extended for general quantification of hygroscopicity of ILs.
研究领域:
化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Engineering
·
2019
·
IF 4.568
Shiyuan Ding,Lilan Zhang,Yang Li,Li’an Hou
In this study, a copper ferrocyanide/silica/polyvinylidene fluoride (CuFC/SiO 2 /PVDF) hollow-fiber composite membrane was successfully synthesized through a facile and effective crosslinking strategy. The PVDF hollow-fiber membrane with embedded SiO 2 was used to fix the dispersion of CuFC nanoparticles for cesium (Cs) removal. The surface morphology and chemical composition of the composite membrane were analyzed using scanning electron microscopy and X-ray photoelectron spectroscopy (XPS). The composite membrane showed a high Cs rejection rate and membrane flux at the three layers of CuFC and 0.5% SiO 2 , and its Cs rejection rate was not affected by variation in the pH (pH = 4–10). The modified membrane could be effectively regenerated many times using ammonium nitrate (NH 4 NO 3 ). The Cs selectivity performance was verified by an efficient Cs rejection rate (76.25% and 88.67% in 8 h) in a solution of 100 μg·L −1 of Cs with 1 mmol·L −1 of competing cations (K + and Na + ). The CuFC/SiO 2 /PVDF hollow-fiber composite membrane showed a particularly superior removal performance (greater than 90%) in natural surface water and simulated water with a low Cs concentration. Therefore, the CuFC/SiO 2 /PVDF hollow-fiber composite membrane can be used directly in engineering applications for the remediation of radioactive Cs-contaminated water.
研究领域:
环境工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）