• <tr id="yyy80"></tr>
  • <sup id="yyy80"></sup>
  • <tfoot id="yyy80"><noscript id="yyy80"></noscript></tfoot>
  • 99热精品在线国产_美女午夜性视频免费_国产精品国产高清国产av_av欧美777_自拍偷自拍亚洲精品老妇_亚洲熟女精品中文字幕_www日本黄色视频网_国产精品野战在线观看 ?

    New insight into polystyrene ion exchange resin for efficient cesium sequestration: The synergistic role of confined zirconium phosphate nanocrystalline

    2023-02-18 01:55:32MengzhouWngMingynFuJunfengLiYihuiNiuQingruiZhngQinSun
    Chinese Chemical Letters 2023年12期

    Mengzhou Wng ,Mingyn Fu ,Junfeng Li ,Yihui Niu ,Qingrui Zhng,? ,Qin Sun,?

    a Hebei Key Laboratory of Heavy Metal Deep-Remediation in Water and Resource Reuse,School of Environmental and Chemical Engineering,Yanshan University,Qinhuangdao 066004,China

    b Laboratory of Environmental Technology,INET,Tsinghua University,Beijing 100084,China

    Keywords:Zirconium phosphate Nanocrystalline Polystyrene resin Cesium Removal

    ABSTRACT Polystyrene resins (PS) have been practical ion exchangers for radionuclides removal from water.However,nonspecific effects of ion exchange groups continue to be a major obstacle for emergency treatment with coexisting ions of high concentrations.The selectivity for Cs+ enables zirconium phosphate (ZrP)to be the most promising inorganic sorbent for radioactive cesium extraction,despite being difficult to synthesize and causing excessive pressure loss in fixed-bed reactors due to fine powder.Herein,through facile confined crystallization in host macropores,we prepared PS confined α-ZrP nanocrystalline(ZrP-PS).Size-screen sorption of layered α-ZrP and sulfonic acid group preconcentration of PS synergistically enable a considerably higher Cs+ affinity of ZrP-PS than PS,as confirmed by X-ray photoelectron spectroscopy (XPS) analysis.ZrP-PS demonstrated remarkable cesium sequestration performance in both batch and continuous experiments,with a high adsorption capacity of 269.58 mg/g,a rapid equilibrium within 80 min,and a continuous effluent volume of 2300 L/kg sorbents.Given the excellent selectivity for Cs+ and flexibility to separate from treated water,ZrP-PS holds great promise as purification packages for the emergency treatment of radioactively contaminated water.

    In the last 50 years,severe nuclear reactor accidents in Europe,Asia,and North America have caused local radiation to rise above natural background levels in the short term,as well as chronic contamination exceeding prescribed standards in different parts of the world [1–3].The total discharges of radioactive cesium (mostly137Cs and134Cs) after the Fukushima accident were estimated at 27.1 PBq,the most massive amount of artificial radioactive material ever released into the sea [4].As an alkali metal,radioactive cesium exists mainly as the cation of Cs+in water,migrates easily and eventually enters the human body through the food chain,increasing the risk of developing tumors through external and internal exposure [5–7].Therefore,it is of imperative interests to sequestrate cesium from aqueous environments in nuclear emergency treatment.

    Many separation technologies have been used to remove radioisotopes from wastewater in nuclear power plants,including Cs+,such as precipitation,solvent extraction,evaporation concentration,membrane and ion exchange [8–10].Ion exchange technology benefits from flexible operations,adaptability to various scenarios,easy integration of devices and recycling,especially from reducing the amount of final solid waste generated effectively by avoiding large amounts of radioactive sludge or organic solvents[11].However,studies are inadequate on removing radioactive alkaline and alkaline earth metal cations by ion exchange resins when coexisting with cations of high concentration [12,13].As a common feature of ionic pollutants purification by ion exchange resins,the nonspecific effect between ion exchange groups and ions may cause the competitive exchange of coexisting cations and reduce Cs+removal efficiency [14–17].This low Cs+selectivity is the main limitation of ion exchange technology for emergency treatment in real waters.

    Unlike ion exchange resins,inorganic ion exchangers such as zirconium compounds,metal hexacyanoferrates (MHCF),ammonium molybdophosphate (AMP),and clay minerals allow selective enrichment of alkaline metals and alkaline earth metals cations and halide anions [14,18–27].For sequestrating cesium,the performances of Prussian blue,zeolite,and AMP still need to be improved regarding adsorption equilibrium time,adsorption capacity,and stability [14,18].At the same time,zirconium phosphate (ZrP) has received much interest in recent decades on its excellent performance [23–27].Since Clearfield and Alberti pioneered the synthesis and structural description of layered ZrP,analogous layered semicrystalline phosphates have been actively researched for solid acid catalysis,adsorption and drug delivery basing on their similar layered structures [23,24].These semicrystalline ZrP are cationic layered compounds with a permanent surface charge and flexible layered structures bound by van der Waals forces,in which the Zr atoms connectedviathe HPO42?groups with the pristine exchangeable counter-ions located within the interlayer space [25].For the separation and extraction of fission products from high-level liquid wastes (HLLWs),ZrP and its derivatives exhibited remarkable Cs selectivity,very sparing aqueous solubility,and excellent radiation resistance,making them the most promising inorganic ion exchangers in Cs extraction [26].However,it is still a problem for ZrP to be directly employed in flow-through treatment systems due to the excessive pressure drop from the fine powder,which greatly limits the practical engineering application of ZrP as the Cs-selective ion exchangers.

    Despite its low selectivity of Cs+,commercial resins have been proposed to be an ideal host for incorporating inorganic particles as an engineering application solution,notably polystyrene ion change resins (PS).In previous studies,PS-hosted nanoparticles were proved efficient in purifying trace heavy metal cations,oxyanions,and halide anions [28–31].PS host primarily provides three benefits.Firstly,immobilize charged groups of the polymeric PS,namely the sulfonic acid group or quaternary ammonium group,permeate and preconcentration target ions by ‘Donnan membrane effect’before surface bonding,enhancing final capacity of target ions [32].Secondly,charged groups facilitate dispersion of small-size particles,providing greater adsorption capacities and/or faster adsorption rates [33].Thirdly,millimeter-scale PS beads are appropriate for continuous flow systems for satisfactory hydrodynamic performance in typical water purification units like continuous packed columns.Thus,we speculate that PS-hosted ZrP exhibits efficient cesium sequestration and is feasible for continuous packed columns.Moreover,universal purification components for emergency treatment could be fabricated based on cesium sequestration behavior and mechanism by PS-hosted ZrP from complex aqueous environments.However,to the best of our knowledge,such research has not been reported.

    Herein,we aim to sequestrate cesium using PS-hosted ZrP and investigate the behavior and mechanism of cesium sequestration.Through facile confined crystallization in the host macropores,we prepared the PS-confinedα-ZrP nanocrystalline,noted as ZrP-PS.Batch sorption runs were performed to examine the adsorption performance of ZrP-PS on simulated radioactive cesium,including the effects of solution pH,coexisting ions,reaction temperature and time.A series of characterizations revealed the mechanism of cesium sequestration.Byin-situcrystalline growth in macropores,nanoα-ZrP was embedded in the porous inner surface of PS.The specific affinity between layeredα-ZrP nanocrystalline and Cs+synergized the Donnan film effect of PS,which allowed cesium to be efficiently separated from water coexisting with highconcentration cations.The continuous packed column assessment predicted ZrP-PS to be an excellent solution for cesium sequestration in emergency treatment applications.

    A polystyrene macroporous cation exchange resin charged with sulfonic acid groups (-SO3–) was used as host.Detailed materials,synthesis and characterization of ZrP-PS and Cs+adsorption experiment sections were in Support Information (Texts S1-S5 in Supporting information).

    By a facile process similar to amorphous ZrP synthesis,nanocrystallineα-ZrP was dispersed in PS and confined in macropores of the host.ZrP-PS was shown with uniformly distributed ZrP particles of diameters of 200–400 nm without aggregation (Fig.1a).In contrast,nano ZrP synthesized without PS host aggregated severely only showing ~50 nm particles at the edges (Fig.1b).For the N2sorption isotherms (Fig.1c),macropores in PS exhibited a type II isotherm with a steep increase in adsorption volume atP/P0=0.95–1.00,while the hysteresis loop of ZrP-PS appeared in the lower relative pressure range reflecting the decreased pore size distribution [34].Also,the pore volume and average pore size of ZrP-PS both decreased (Fig.1c,insert).The atomic force microscope (AFM) 3D analysis in Fig.S1a (Supporting information)showed that the vertical height approximate 200 nm of the central cross-section of ZrP-PS was smoother than that of PS.Both the N2sorption isotherms and the AFM images indicated pore confined ZrP blocked some macropores.Pore-confinement is also demonstrated by the gradually growth of ZrP from the outer surface to the inner part of PS (Text S6 and Fig.S1b in Supporting information).The confined ZrP exhibits the characteristic diffraction peaks at 2θof 11.6,20.3,and 24.9° in the X-ray powder diffractometer(XRD) pattern (Fig.1d),which correspond to the crystal planes(002),(110),and (112) of crystallineα-Zr(HPO4)2·H2O (α-ZrP,JCPDS No.22–1022).The (002) crystal plane spacing was 7.6 ?A calculated from Bragg’s law (Text S7 in Supporting information),indicating the PS-confined ZrP was layeredα-ZrP crystalline [35–38].

    Fig.1. Characterization of ZrP-PS and ZrP: (a) the TEM image of ZrP-PS and (b)the TEM images of ZrP powder,(c) nitrogen adsorption-desorption isotherms (inset:pore size distribution) of PS and ZrP-PS,and (d) XRD patterns of ZrP powder,ZrP-PS and Cs-sequestrated ZrP-PS (ZrP-PS-Cs),and the standard pattern of Zr(HPO4)2·H2O(top to bottom).

    The typical synthesis of layered structural ZrP involves hightemperature calcination [24,38–40].In this study,Zr4+,as the ZrP precursor,dispersed throughout macropores of the PS host due to negative charges of -SO3–,which significantly altered the crystallization behavior of ZrP.Confined formation of the crystalline phase is possible because of altered crystallization kinetics and thermodynamics in PS pores [30,41].Without pore-confinement,ZrP was mainly amorphous and showed broad diffraction peaks in XRD pattern (Fig.1d).Accordingly,through porous and crosslinking matrix and ample surface charge of PS,α-ZrP was confined in the host,which was presumed to facilitate good cesium sequestration in addition to -SO3–groups.

    Cesium sequestration of ZrP-PS demonstrated removal efficiencies higher than 95.2% in the wide pH range of 3.27–10.93 (Fig.2a).This performance benefited from the stably negative zeta potentials of ZrP-PS due to permanently negatively charged -SO3–in PS[42].H+release was observed in cesium sequestration by ZrP-PS(Fig.S2 in Supporting information),suggesting similar proton-Cs+exchange to that of amorphous ZrP,and thus an excess of H+ions inhibited the Cs+removal at pH values 0.84 and 1.91.Furthermore,surface protonation of ZrP-PS at high acidity resulted in the most positive zeta potential at pH around 1.0,which weakened nonspecific electrostatic interaction of ZrP-PS toward Cs+,thereby affecting cesium sequestration.

    Fig.2. (a) Solution pH effects on Cs+ removal (ZrP-PS dose: 1.0 g/L,initial Cs+=50 mg/L,298 K for 24 h) and zeta potentials of ZrP-PS,(b) effects of competing cations Na+and Ca2+ on Cs+ removal (sorbent dose 1.0 g/L,initial Cs+=50 mg/L,298 K for 24 h,pH 6.5–7.0),(c) kinetic models fitting results,inset: intraparticle diffusion model fitting(ZrP-PS dose: 0.4 g/L,initial Cs+=80 mg/L,298 K,pH 6.5–7.0),and (d) adsorption isotherm curves fitted by Langmuir and Freundlich models (ZrP-PS dose: 1.0 g/L,24 h,pH 6.5–7.0).

    It is essential for emergency treatment to investigate the selectivity of Cs+under coexistence of competing cations.Both ZrP-PS and PS were affected to some extent with increasing concentrations of Na+and Ca2+(Fig.2b).When Na+/Cs+(mol/mol)was increased from 0 to 16,the Cs+removal efficiency by ZrP-PS remained greater than 90.0%;in contrast,that by PS decreased dramatically from 94.6% to 72.8% and was only 44.8% at Na+/Cs+(mol/mol)=64.When Ca2+/Cs+(mol/mol) was increased from 0 to 32,the removal efficiency of Cs+by ZrP-PS decreased from 97.0% to 40.2%,while that of PS from 94.6% to 16.2%.However,with the further increase of Ca2+/Cs+,the removal efficiency of ZrP-PS stabilized.The solid-liquid distribution ratioKdof ZrP-PS(310 mL/g) was about 24 times greater than that of PS (Text S8 in Supporting information).ZrP-PS is expected to sequestrate Cs+viaproton exchange by ZrP [43] in addition to the nonspecific interaction of -SO3–groups,with the latter to be a main interaction of PS.The proton-exchange sites onα-ZrP provide a specific affinity and high selectivity for Cs+,while the selectivity by PS with coexisting cations was inferior because cations competed the nonspecific sites of -SO3–.In addition,effects of Mg2+,typical coexisting anions (Cl?,NO3?,SO42?),humic acid and salinity on Cs+selectivity supported the benefits of ZrP-PS for emergency treatment in natural waters (Text S9,Fig.S3 in Supporting information).

    The adsorption kinetics and isotherm experiments were conducted through batch adsorption tests to investigate further the cesium sequestration performance of ZrP-PS (Text S10 in Supporting information).Fig.2c shows the adsorption kinetics of Cs+on ZrP-PS,with PS as the reference in Fig.S4a (Supporting information).Cs+uptake equilibriums reached within ~80 min for both ZrP-PS and PS;however,ZrP-PS exhibited a faster kinetic process.Cs+removal efficiencies by ZrP-PS at 30 and 80 min were 55.1% and 84.5%,respectively.Thepseudo-first-order,pseudosecond-order,and intraparticle diffusion models fitted the kinetic data of ZrP-PS well,with higher rate constantsK1,K2andKintrepresenting the faster kinetic rate than PS (Table S1 in Supporting information).The intraparticle diffusion model exhibited a higher correlation to ZrP-PS (R2=0.9825) than PS (R2=0.8393),inferring that decreased average pore size in ZrP-PS affected intraparticle diffusion of Cs+.The isothermal adsorption data of Cs+on PS and ZrP-PS were fitted well by Langmuir and Freundlich models(Fig.2d,Fig.S4b and Table S2 in Supporting information).According to the Langmuir model,the adsorption capacity of Cs+on PS was 230.61 mg/g and did not change much at the experimental temperatures.The adsorption capacity of Cs+by ZrP-PS increased with decreasing temperatures,indicating the exothermic nature of cation exchange ofα-ZrP [44].The maximum adsorption capacity of Cs+on ZrP-PS was 269.85 mg/g at 293 K,greater than that on PS and an almost unmatched maximum capacity for Cs+adsorption compared with the literature in the last ten years [45–54] (Table 1).In addition,when ZrP-PS was used in simulated radioactive wastewater (Table S3 in Supporting information),removal efficiency was not significantly influenced by high Cs+concentrations of 50 and 200 mg/L (Fig.S5 in Supporting information),further demonstrating efficient cesium sequestration performance of ZrP-PS.

    Table 1 Comparison of Cs adsorption capacities and kinetics by adsorbents in literatures in the last ten years.

    To disclose the mechanism of efficient Cs+sequestration by ZrP-PS,XRD,Fourier transform infrared (FT-IR) spectra and X-ray photoelectron spectroscopy (XPS) analysis of different samples was performed,and the results are depicted in Figs.1d and 3,Figs.S6 and S7 (Supporting information).By XPS analysis,differences of P 2p,Zr 3d and O 1s binding energies between PS-confinedα-ZrP nanocrystalline and amorphous ZrP further approved the structural characteristics ZrP-PS and ZrP shown in the XRD patterns(Text S11 in Supporting information).After Cs+adsorption on ZrPPS,cesium was detected in the ZrP-PS-Cs sample both in the XRD and XPS analyses,as the characteristic peaks of Cs+solid solutions(Cs2Zr(PO4)2and CsZrH(PO4)2·xH2O) in Fig.1d and Cs 3d bonding energies at 725.0–740.0 eV in the full XPS spectrum shown in Fig.3b.XRD characteristic peaks ofα-ZrP were observed without position variation.FT-IR spectra comparison of ZrP-PS and ZrP-PS-Cs in Fig.3a presents that most functional groups remained before and after Cs+adsorption,confirming the stable chemical composite of ZrP-PS.Weak bands at 1410 cm?1of ZrP-PS are attributed to the presence ofδ(POH),indicating the existence of structural hydroxyl as exchangeable proton sites in confinedα-ZrP.This involvement of proton exchange in phosphate groups during Cs+adsorption could also be inferred from the notable reduction of the (002) peak intensity of ZrP-PS in Fig.1d and the intensity changes of bands at 1035 and 670 cm?1in Fig.S6 (Text S12 in Supporting information).More information on the mechanism of Cs+sequestration is revealed in the XPS spectra.In the high-resolution analysis,Cs 3d5/2binding energy of ZrP-PS-Cs shifted 0.4 eV compared to the standard peak of CsNO3located at 724.2 eV (Fig.3c) [55],and P 2p binding energy shifted from 134.2 eV of ZrP-Cs to 133.8 eV of ZrP-PS-Cs (Fig.S7d in Supporting information).These bonding energies shifts hint the strong interaction between Cs+and ZrP-PS.In addition,as shown in Fig.S7e (Supporting information),the Cs 3d5/2peak around 723.8 eV is attributable to the electrostatic interaction of -SO3–toward Cs+(noted as -SO3–Cs+),whereas the one around 724.1 eV is attributable to the ion exchange between Cs+and protons of P-O-H inα-ZrP (noted as P-O-Cs) [56].The O 1s of ZrP-PS-Cs shows a broad peak which could correspond to O atoms bonded to Cs atoms in addition to those in Zr-O,P-O andS-O (Fig.3d).The shift of O 1s from 532.2 eV to 531.8 eV after Cs+adsorption also suggests an interaction between Cs+and ZrP-PS using oxygen atoms as bridges,forming the P-O-Cs and lowering the O 1s binding energy [57].Thus,proton exchange by P-OH and electrostatic interaction by -SO3H are associated mechanisms of Cs sequestration by ZrP-PS.

    Fig.3. (a) FT-IR spectra of ZrP-PS,ZrP-PS-Cs and ZrP-PS-Cs/Ca samples,(b) XPS survey spectra of PS-Cs,ZrP-Cs,ZrP-PS,and ZrP-PS-Cs,(c) Cs 3d5/2 XPS spectra of CsNO3,ZrP-PS-Cs,and ZrP-PS-Cs/Ca (Ca:Cs=1) samples,(d) O 1s XPS spectra of Zr-PS and ZrP-PS-Cs,and (e) the illustration of synergistic role of confined α-ZrP on cesium sequestration.

    Furthermore,the synergy ofα-ZrP is emphasized by characterizing the competing adsorption of Ca2+on different materials.When Cs+and Ca2+co-existed,the FT-IR peak of -SO3H at 1035 cm?1blue-shifted by 6.75 cm?1,more than just 1.84 cm?1without Ca2+,suggesting nonspecific interaction of -SO3H with both cations.Compared to fresh ZrP-PS,the POH peaks blue-shifted for 4 cm?1after Cs sequestration without and with Ca2+competitive adsorption,which implies specific interaction of P-O-H and Cs+.In high-resolution XPS analysis of Cs 3d5/2in Fig.S7e and Fig.3c,negligible shift on Cs 3d5/2binding energy could be observed from PS-Cs to ZrP-PS-Cs,but a–0.7 eV positive shift exhibited for ZrPPS-Cs/Ca compared to PS-Cs.This is because of different deconvoluted peaks area portions with and without Ca2+coexistence.In both cases,the Cs 3d5/2spectra were divided into two peaks corresponding to P-O-Cs and -SO3–Cs+.The area fractions of P-O-Cs and-SO3?Cs+of ZrP-PS-Cs were 18.2% and 81.8%,respectively.However,as for ZrP-PS-Cs/Ca,peak fractions varied distinguishably with 60.2% P-O-Cs and 39.8% -SO3–Cs+.Such results certify that with high concentration Ca2+coexistence,Cs sequestration by -SO3–Cs+path abated while P-O-Cs dominated and contributed high selectivity of Cs+by ZrP-PS.

    Based on the removal performance and characteristic results,the mechanism of efficient Cs+sequestration by ZrP-PS was elucidated,as illustrated in Fig.3e.Cs+sequestration by ZrP-PS is attributed to the synergistic effect of confined nanocrystallineα-ZrP and -SO3–groups covalently binding in the PS polymer host.

    Firstly,negatively charged -SO3–groups enrich Cs+viaelectrostatic interaction,a fundamental effect of cation exchange resins,to a concentration higher than in the bulk solution by the Donnan membrane effect.This widely verified effect [28–32,34] promotes Cs+diffusion to interaction sites.Secondly,confinedα-ZrP absorb Cs+through interlayer proton exchange.Inα-ZrP,Zr atoms planes severe as the basic layered structure,with -HPO4groups attached by three O atoms coordinating to Zr.While the fourth O of -HPO4,bearing a proton,points toward the interlayer space as a potential cation exchange site [37].The maximum opening to the interlayer space expands to adequate for Cs+(radius 1.69 ?A) to diffuse into interlayers and exchange with the proton in P-O-H [26,58-60],then the accessibility of Cs is constrained by crystal lattice match and restraint,shown as Eq.1.

    Thirdly,with the presence of monovalent alkali metal and divalent alkali earth metal cations that lacking outermost electron distinction from Cs+,confinedα-ZrP plays a vital role in selective adsorption toward Cs+.Competitive Na/Ca/Mg cations occupied the nonspecific adsorption sites of -SO3–,which somewhat reduced Cs+adsorption capacity of ZrP-PS.However,different radius and dehydration enthalpy of hydrated Cs+and competitive cations determine the approachability toα-ZrP interlayers for these cations.The dehydration enthalpy for alkali metal and alkali earth metal ions increases with hydration radius,in the order of Cs+(3.29 ?A)<Na+(3.58 ?A)<Ca2+(4.12 ?A)<Mg2+(4.28 ?A) [61–64].This order indicates that it is more facile for hydrated Cs+to dehydrate than hydrated Na+,Ca2+,and Mg2+.Cs+enter the interlayers ofα-ZrP and exchange with protons,however,hydrated Na+,Ca2+and Mg2+are too large to fit the interlayer channels.Therefore,Na+,Ca2+and Mg2+demonstrate little competition onto the interlayer proton exchange sites.Nanocrystalline and porous structures with particular channel or ring window sizes are also reported in other studies for selectively removing Cs+or Sr2+from aqueous solutions [19,20,65].In all,the synergy of size-screen assisted ion exchange of confinedα-ZrP and -SO3–preconcentration of PS contributes to the efficient sequestration of cesium.

    The practicality of ZrP-PS for cesium sequestration was evaluated by a simulated emergency treatment test using flow-through columns packed with ZrP-PS and PS,respectively,with the results shown in Fig.4.As expected,ZrP-PS demonstrated a considerable improvement in Cs+removal efficiency over PS.After a continuous run of approximately 2300 liters per kilo sorbents,Cs+concentration in the effluent from the ZrP-PS column rose,reaching the breakthrough at ~3200 liters per kilo sorbents.In contrast,the effluent was only approximately 208 liters per kilo sorbents at the breakthrough of PS.It is noteworthy that for PS,the concentration of Cs+in the effluent around 300 L/kg sorbent was higher than 2 mg/L,which can be explained by the elution effect in continuous sorption [66,67].Some Cs+initially sorbed by PS was replaced by competing cations Na+,Ca2+,and Mg2+because of the nonspecific effect of -SO3–on these cations.Due to the specific affinity ofα-ZrP for Cs+,the elution effect in Cs+adsorption by ZrPPS was suppressed,and therefore a larger treatment capacity was obtained.The amount of water treated by ZrP-PS was more than ten times that of PS,indicating the promising application of PSconfinedα-ZrP nanocrystalline.

    Fig.4. Assessment of continuous sorption performances of ZrP-PS and PS (SLV:0.3 m/h,EBCT: 6 min,Cs+: 2 mg/L,Ca2+: 100 mg/L,Mg2+: 100 mg/L,Na+: 100 mg/L).

    In summary,we developed efficient cesium sequestration using the PS confinedα-ZrP nanocrystalline.Macropores and -SO3–in the PS host permitted uniform dispersion ofα-ZrP,whose interlayer spacing screened competitive hydrated cations out and allowed Cs+retention on interlayer ion exchange sites.The specific ion exchange and nonspecific electrostatic reaction synergistically prompted a high Cs+adsorption capacity of 269.58 mg/g and a quick equilibrium within 80 min.The continuous treatment exhibited a remarkable capacity of approximately 2300 L water/kg ZrPPS.Given its efficient cesium sequestration and flexibility to separate from treated water,ZrP-PS has excellent potential for emergency treatment and deep purification of radioactively contaminated water.

    Declaration of competing interest

    The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

    Acknowledgments

    This work was financially supported by NSFC (Nos.U22A20403,21301151 and 52070115),Natural Science Foundation of Hebei Province (Nos.B2021203036 and E2022203011),and Key Project of the Hebei Education Department (No.ZD2021103).

    Supplementary materials

    Supplementary material associated with this article can be found,in the online version,at doi:10.1016/j.cclet.2023.108442.

    亚洲综合色网址| 亚洲少妇的诱惑av| 91精品一卡2卡3卡4卡| 插逼视频在线观看| 欧美日韩在线观看h| 18禁裸乳无遮挡动漫免费视频| 亚洲情色 制服丝袜| 久久久久网色| 国产日韩欧美在线精品| 欧美日韩一区二区视频在线观看视频在线| 九九久久精品国产亚洲av麻豆| 国产精品女同一区二区软件| 99热全是精品| 国产又色又爽无遮挡免| 亚洲激情五月婷婷啪啪| 免费av中文字幕在线| 久久 成人 亚洲| 狂野欧美激情性bbbbbb| av专区在线播放| 精品国产一区二区三区久久久樱花| 亚洲精品日韩av片在线观看| 精品少妇久久久久久888优播| 亚洲国产精品成人久久小说| 夜夜爽夜夜爽视频| 成年美女黄网站色视频大全免费 | 精品亚洲成国产av| 久久国产精品大桥未久av| 制服诱惑二区| 人人妻人人添人人爽欧美一区卜| 久久久精品区二区三区| 亚洲久久久国产精品| 美女大奶头黄色视频| 亚洲精品乱久久久久久| 国内精品宾馆在线| 亚洲第一av免费看| 两个人的视频大全免费| 2018国产大陆天天弄谢| 国产精品嫩草影院av在线观看| 高清在线视频一区二区三区| 九九在线视频观看精品| 桃花免费在线播放| 高清欧美精品videossex| 中文字幕免费在线视频6| 99re6热这里在线精品视频| 日韩av不卡免费在线播放| 在线观看三级黄色| 国产片特级美女逼逼视频| 久久久国产欧美日韩av| 久久精品人人爽人人爽视色| 精品久久国产蜜桃| 人妻人人澡人人爽人人| 极品少妇高潮喷水抽搐| 国产精品麻豆人妻色哟哟久久| 少妇精品久久久久久久| 免费看不卡的av| 国产精品一区二区三区四区免费观看| 蜜臀久久99精品久久宅男| 国产男女内射视频| 91在线精品国自产拍蜜月| 精品国产国语对白av| 久久久久久人妻| 国产在线视频一区二区| 搡女人真爽免费视频火全软件| 美女xxoo啪啪120秒动态图| 九色亚洲精品在线播放| kizo精华| 亚洲av国产av综合av卡| 精品午夜福利在线看| videossex国产| 丝袜在线中文字幕| 人人妻人人爽人人添夜夜欢视频| av福利片在线| 亚洲成人手机| 久久久国产欧美日韩av| 天天操日日干夜夜撸| 五月玫瑰六月丁香| 日韩 亚洲 欧美在线| 秋霞伦理黄片| 欧美亚洲 丝袜 人妻 在线| 男女国产视频网站| 91精品国产九色| 在线精品无人区一区二区三| 成人国产麻豆网| 免费观看无遮挡的男女| 一个人免费看片子| 久久免费观看电影| 91在线精品国自产拍蜜月| 纯流量卡能插随身wifi吗| 国产成人精品福利久久| 十分钟在线观看高清视频www| 好男人视频免费观看在线| 久久精品国产鲁丝片午夜精品| 色94色欧美一区二区| 国产精品秋霞免费鲁丝片| av卡一久久| 99热这里只有精品一区| 大话2 男鬼变身卡| 亚洲精品国产色婷婷电影| 国产黄色视频一区二区在线观看| 国产成人一区二区在线| 日韩精品有码人妻一区| 我要看黄色一级片免费的| 91成人精品电影| 日本黄大片高清| 一级片'在线观看视频| 免费日韩欧美在线观看| 午夜视频国产福利| 日韩中字成人| 中文字幕精品免费在线观看视频 | 肉色欧美久久久久久久蜜桃| 精品久久国产蜜桃| 性色av一级| 亚洲性久久影院| 免费人妻精品一区二区三区视频| 91在线精品国自产拍蜜月| 久久精品夜色国产| 男人爽女人下面视频在线观看| 国产 精品1| 中文字幕人妻熟人妻熟丝袜美| 国产精品99久久久久久久久| 高清黄色对白视频在线免费看| 男女啪啪激烈高潮av片| 99热国产这里只有精品6| 免费观看性生交大片5| 少妇 在线观看| 少妇精品久久久久久久| 人妻夜夜爽99麻豆av| 国产国语露脸激情在线看| 国产视频首页在线观看| a级毛片黄视频| 精品人妻在线不人妻| 大陆偷拍与自拍| av免费观看日本| 成人18禁高潮啪啪吃奶动态图 | 国产日韩欧美在线精品| 亚洲成人av在线免费| 在线观看免费日韩欧美大片 | 国产淫语在线视频| 午夜福利在线观看免费完整高清在| 日本wwww免费看| 久久影院123| 国产黄色视频一区二区在线观看| 亚洲,欧美,日韩| a级毛片在线看网站| 日韩三级伦理在线观看| 嘟嘟电影网在线观看| 尾随美女入室| 国产一区二区在线观看av| 国产精品久久久久久av不卡| 亚洲av综合色区一区| 岛国毛片在线播放| 视频区图区小说| 春色校园在线视频观看| 国产日韩欧美在线精品| 国产女主播在线喷水免费视频网站| 夫妻午夜视频| 午夜激情福利司机影院| 久久精品人人爽人人爽视色| 制服诱惑二区| 久久精品久久久久久噜噜老黄| 又大又黄又爽视频免费| 日日撸夜夜添| 一级毛片我不卡| 亚洲人成网站在线播| 人妻一区二区av| 日本黄色日本黄色录像| 精品午夜福利在线看| 亚洲精品国产av成人精品| 精品亚洲成a人片在线观看| av有码第一页| 国产欧美日韩综合在线一区二区| 少妇猛男粗大的猛烈进出视频| 免费看av在线观看网站| 热re99久久精品国产66热6| 亚洲精品乱码久久久v下载方式| 欧美激情极品国产一区二区三区 | 国产黄频视频在线观看| 97超视频在线观看视频| 成人影院久久| 免费不卡的大黄色大毛片视频在线观看| xxxhd国产人妻xxx| 麻豆精品久久久久久蜜桃| 精品人妻在线不人妻| 制服丝袜香蕉在线| 自拍欧美九色日韩亚洲蝌蚪91| 狂野欧美激情性bbbbbb| 国产成人精品一,二区| 免费观看av网站的网址| 2018国产大陆天天弄谢| 在线 av 中文字幕| 精品视频人人做人人爽| 又大又黄又爽视频免费| 久久青草综合色| 久久精品久久精品一区二区三区| 性色avwww在线观看| 午夜福利影视在线免费观看| 国产在线一区二区三区精| 国产精品麻豆人妻色哟哟久久| 精品一品国产午夜福利视频| 亚洲av成人精品一区久久| 特大巨黑吊av在线直播| 久久久欧美国产精品| 五月开心婷婷网| 制服丝袜香蕉在线| 国产免费福利视频在线观看| 视频在线观看一区二区三区| 亚洲精品,欧美精品| 久久久久久久久大av| 各种免费的搞黄视频| av国产精品久久久久影院| 一本一本综合久久| 秋霞在线观看毛片| 超碰97精品在线观看| 国产深夜福利视频在线观看| 新久久久久国产一级毛片| 国产爽快片一区二区三区| 高清在线视频一区二区三区| 人妻 亚洲 视频| 九草在线视频观看| 欧美xxⅹ黑人| 最新的欧美精品一区二区| 九九在线视频观看精品| 亚洲av欧美aⅴ国产| av免费观看日本| 欧美日韩视频精品一区| 超色免费av| 少妇人妻久久综合中文| 激情五月婷婷亚洲| 日韩欧美精品免费久久| 成年人午夜在线观看视频| 内地一区二区视频在线| h视频一区二区三区| 国产在线视频一区二区| 久久99蜜桃精品久久| 国产精品国产三级专区第一集| 亚洲第一av免费看| 另类亚洲欧美激情| 女性生殖器流出的白浆| 老司机影院毛片| 亚洲av日韩在线播放| 日本午夜av视频| 国产精品国产三级国产av玫瑰| 春色校园在线视频观看| 成年女人在线观看亚洲视频| 国产黄色免费在线视频| 午夜福利视频精品| 亚洲精品一区蜜桃| 一区二区三区精品91| 18禁在线播放成人免费| 18禁动态无遮挡网站| 波野结衣二区三区在线| 亚洲av.av天堂| 一本久久精品| 国产不卡av网站在线观看| 男女边摸边吃奶| 国产精品三级大全| 亚洲少妇的诱惑av| 高清黄色对白视频在线免费看| 一级片'在线观看视频| 欧美精品亚洲一区二区| 日本黄色日本黄色录像| 亚洲欧美成人综合另类久久久| 久久国产亚洲av麻豆专区| 国产69精品久久久久777片| 99国产综合亚洲精品| 欧美精品国产亚洲| 久久久久精品性色| 亚洲三级黄色毛片| 91午夜精品亚洲一区二区三区| 搡老乐熟女国产| 下体分泌物呈黄色| 一本一本久久a久久精品综合妖精 国产伦在线观看视频一区 | 五月开心婷婷网| 菩萨蛮人人尽说江南好唐韦庄| 久久精品国产亚洲网站| 蜜桃在线观看..| 亚洲天堂av无毛| 久久 成人 亚洲| av线在线观看网站| 亚洲一区二区三区欧美精品| 日韩成人av中文字幕在线观看| 人妻 亚洲 视频| 午夜av观看不卡| 热re99久久国产66热| 久久久国产欧美日韩av| 国产精品无大码| 欧美日韩av久久| 午夜福利,免费看| 欧美bdsm另类| 欧美 亚洲 国产 日韩一| 一级毛片aaaaaa免费看小| 久久99精品国语久久久| 精品国产国语对白av| 国产乱人偷精品视频| 69精品国产乱码久久久| a级毛片免费高清观看在线播放| 美女视频免费永久观看网站| 日本av免费视频播放| 亚洲成人手机| 久久狼人影院| 欧美日韩精品成人综合77777| 日韩欧美精品免费久久| 80岁老熟妇乱子伦牲交| 多毛熟女@视频| 飞空精品影院首页| 交换朋友夫妻互换小说| 免费观看性生交大片5| 99热这里只有精品一区| 日韩精品有码人妻一区| 在现免费观看毛片| 蜜桃在线观看..| 免费观看a级毛片全部| 午夜91福利影院| 久久久久久久亚洲中文字幕| 亚洲精品视频女| 中文乱码字字幕精品一区二区三区| 青春草视频在线免费观看| 免费高清在线观看视频在线观看| 精品国产国语对白av| 人妻一区二区av| 少妇人妻 视频| 日日摸夜夜添夜夜爱| 精品一品国产午夜福利视频| 亚洲精品一二三| 黑人猛操日本美女一级片| 中文字幕制服av| 黑丝袜美女国产一区| 免费av中文字幕在线| 国产精品人妻久久久影院| 丰满饥渴人妻一区二区三| 岛国毛片在线播放| 国产精品三级大全| 欧美 日韩 精品 国产| 欧美日韩在线观看h| 亚洲高清免费不卡视频| 考比视频在线观看| 日韩不卡一区二区三区视频在线| 狂野欧美激情性bbbbbb| 国产精品久久久久久精品古装| 国产高清三级在线| 亚洲精品久久久久久婷婷小说| 午夜福利视频精品| 热99久久久久精品小说推荐| 日韩不卡一区二区三区视频在线| 欧美日韩亚洲高清精品| 大话2 男鬼变身卡| 成人漫画全彩无遮挡| 亚洲图色成人| 日韩人妻高清精品专区| 韩国av在线不卡| 岛国毛片在线播放| 黑人猛操日本美女一级片| 国产欧美日韩一区二区三区在线 | 国产亚洲精品久久久com| 少妇被粗大的猛进出69影院 | 80岁老熟妇乱子伦牲交| 少妇人妻 视频| 国产爽快片一区二区三区| 男女啪啪激烈高潮av片| 欧美少妇被猛烈插入视频| 王馨瑶露胸无遮挡在线观看| 久久人人爽人人片av| 热re99久久精品国产66热6| 成人综合一区亚洲| 一区二区日韩欧美中文字幕 | 国产亚洲精品久久久com| 久久精品国产亚洲av天美| 蜜桃在线观看..| 久久综合国产亚洲精品| 婷婷色av中文字幕| 高清视频免费观看一区二区| 免费人妻精品一区二区三区视频| 2018国产大陆天天弄谢| 99久久人妻综合| av国产久精品久网站免费入址| 国产一级毛片在线| 国产免费福利视频在线观看| 久久97久久精品| 国产又色又爽无遮挡免| 国产成人91sexporn| 久久久久国产精品人妻一区二区| 久久毛片免费看一区二区三区| 亚洲内射少妇av| 最近2019中文字幕mv第一页| 国产有黄有色有爽视频| 国产精品久久久久成人av| 亚洲成人手机| 精品99又大又爽又粗少妇毛片| 免费观看的影片在线观看| 亚洲av成人精品一区久久| 免费大片18禁| 在线观看免费高清a一片| 色哟哟·www| 午夜福利影视在线免费观看| 99九九在线精品视频| 亚洲精品国产av成人精品| 婷婷色综合www| 啦啦啦视频在线资源免费观看| 亚洲婷婷狠狠爱综合网| 免费看不卡的av| 成人国产麻豆网| 久久韩国三级中文字幕| 亚洲人成77777在线视频| 国产片内射在线| 欧美 日韩 精品 国产| 欧美xxⅹ黑人| 欧美性感艳星| 久久精品国产鲁丝片午夜精品| 亚洲av成人精品一二三区| 狂野欧美激情性bbbbbb| av有码第一页| 男女国产视频网站| 亚洲国产精品国产精品| 91国产中文字幕| 夜夜骑夜夜射夜夜干| 最近中文字幕2019免费版| 黄片播放在线免费| 日本欧美视频一区| 久久精品国产自在天天线| 精品一区二区三区视频在线| 国产免费现黄频在线看| 青春草亚洲视频在线观看| 九九爱精品视频在线观看| 最新的欧美精品一区二区| 久久久久人妻精品一区果冻| 国产爽快片一区二区三区| 色网站视频免费| 久久99热这里只频精品6学生| 亚洲av综合色区一区| 精品久久久久久久久亚洲| 我要看黄色一级片免费的| 亚洲久久久国产精品| 一级毛片 在线播放| 国产成人a∨麻豆精品| 人人妻人人澡人人爽人人夜夜| 免费av中文字幕在线| 亚洲av在线观看美女高潮| 最新的欧美精品一区二区| 国产亚洲精品久久久com| 国产探花极品一区二区| 有码 亚洲区| 在线亚洲精品国产二区图片欧美 | 少妇的逼好多水| 青春草国产在线视频| 久久人人爽人人爽人人片va| av黄色大香蕉| av福利片在线| 亚洲怡红院男人天堂| 免费大片黄手机在线观看| 热re99久久精品国产66热6| 国产亚洲一区二区精品| 亚洲人成网站在线播| 国产精品人妻久久久久久| 纵有疾风起免费观看全集完整版| 一本色道久久久久久精品综合| 国产精品免费大片| 丝袜美足系列| 在线免费观看不下载黄p国产| 亚洲国产色片| 精品亚洲乱码少妇综合久久| 国产又色又爽无遮挡免| 色网站视频免费| 自拍欧美九色日韩亚洲蝌蚪91| 最近中文字幕高清免费大全6| 青春草国产在线视频| 亚洲精品乱码久久久久久按摩| 视频区图区小说| 99九九线精品视频在线观看视频| 蜜桃国产av成人99| 麻豆成人av视频| 免费观看a级毛片全部| 日韩欧美精品免费久久| 亚洲精品乱码久久久v下载方式| 国产成人精品一,二区| 在线播放无遮挡| 高清午夜精品一区二区三区| 大码成人一级视频| 免费观看av网站的网址| 免费播放大片免费观看视频在线观看| 久久久精品94久久精品| 久久人人爽人人片av| 亚洲无线观看免费| 久久久久精品久久久久真实原创| 亚洲欧美清纯卡通| 国产免费又黄又爽又色| 久久久久久久久久久久大奶| 亚洲精品乱久久久久久| 国产精品免费大片| 久久久久久久精品精品| 亚洲精品av麻豆狂野| 久久精品久久久久久久性| 午夜福利网站1000一区二区三区| 午夜日本视频在线| 国产精品一国产av| 69精品国产乱码久久久| 亚洲av中文av极速乱| 我的女老师完整版在线观看| 国产日韩一区二区三区精品不卡 | 国产 精品1| 老女人水多毛片| 亚洲精品中文字幕在线视频| 成人免费观看视频高清| 亚洲伊人久久精品综合| 国产精品久久久久久久久免| 亚洲精品自拍成人| a 毛片基地| 中文字幕人妻丝袜制服| 大片免费播放器 马上看| 免费av不卡在线播放| 免费观看无遮挡的男女| 日本wwww免费看| 热re99久久精品国产66热6| 街头女战士在线观看网站| 中文乱码字字幕精品一区二区三区| 女人久久www免费人成看片| 久久国产亚洲av麻豆专区| av福利片在线| 夫妻午夜视频| 久久狼人影院| 自拍欧美九色日韩亚洲蝌蚪91| 久久久久久久亚洲中文字幕| 最新中文字幕久久久久| 在线亚洲精品国产二区图片欧美 | 午夜福利在线观看免费完整高清在| av一本久久久久| 成年女人在线观看亚洲视频| 在线观看三级黄色| 国产一区有黄有色的免费视频| 成人亚洲欧美一区二区av| 一级片'在线观看视频| 不卡视频在线观看欧美| 国产精品一区二区在线不卡| av专区在线播放| 18禁裸乳无遮挡动漫免费视频| 韩国av在线不卡| 亚洲精品视频女| 狂野欧美白嫩少妇大欣赏| 欧美xxⅹ黑人| 老司机亚洲免费影院| 国产av一区二区精品久久| 久久韩国三级中文字幕| 人人妻人人澡人人爽人人夜夜| 一区二区三区四区激情视频| 黄色一级大片看看| 精品少妇内射三级| 精品人妻熟女毛片av久久网站| 国产精品人妻久久久影院| 国产免费一级a男人的天堂| 国产老妇伦熟女老妇高清| 成年美女黄网站色视频大全免费 | 国产精品不卡视频一区二区| 亚州av有码| 日本黄色日本黄色录像| www.色视频.com| 亚洲图色成人| 成人国产av品久久久| 久久国内精品自在自线图片| 国产男女超爽视频在线观看| 最近手机中文字幕大全| 国产又色又爽无遮挡免| 国产亚洲午夜精品一区二区久久| 80岁老熟妇乱子伦牲交| 国产精品免费大片| 国产不卡av网站在线观看| 一区二区三区免费毛片| 黑丝袜美女国产一区| 一边摸一边做爽爽视频免费| 免费人妻精品一区二区三区视频| 欧美精品高潮呻吟av久久| 制服人妻中文乱码| 欧美激情极品国产一区二区三区 | 女的被弄到高潮叫床怎么办| 久久精品久久久久久噜噜老黄| av专区在线播放| 久久综合国产亚洲精品| 国产免费一级a男人的天堂| 麻豆乱淫一区二区| 日韩制服骚丝袜av| 精品久久久噜噜| 国产男女内射视频| 黄色欧美视频在线观看| 亚洲,一卡二卡三卡| 老司机影院毛片| 午夜老司机福利剧场| 全区人妻精品视频| 在线观看免费高清a一片| 国产av精品麻豆| 狂野欧美激情性xxxx在线观看| 欧美+日韩+精品| 国产黄片视频在线免费观看| 99国产精品免费福利视频| 日韩制服骚丝袜av| 久久久精品区二区三区| 久久女婷五月综合色啪小说| 伦理电影大哥的女人| 97超视频在线观看视频| 久久国内精品自在自线图片| 人妻一区二区av| 婷婷色麻豆天堂久久| 久久久久久久久久久免费av| 激情五月婷婷亚洲| 天堂俺去俺来也www色官网| 高清毛片免费看| 天天操日日干夜夜撸| 国产精品人妻久久久久久| 国产伦精品一区二区三区视频9| 有码 亚洲区| av线在线观看网站| 大香蕉久久成人网| 人人妻人人澡人人看| 国产视频内射| 日韩,欧美,国产一区二区三区| 精品久久久久久久久av| 免费黄网站久久成人精品| 亚洲精品一二三|