• <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 ?

    Efficient Fe(III)/Fe(II) cycling triggered by MoO2 in Fenton reaction for the degradation of dye molecules and the reduction of Cr(VI)

    2020-01-14 07:55:02BinShenChenchengDongJiahuiJiMingyangXingJinlongZhang
    Chinese Chemical Letters 2019年12期
    關(guān)鍵詞:萊陽市蜜露白粉

    Bin Shen,Chencheng Dong,Jiahui Ji,Mingyang Xing,Jinlong Zhang

    Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, China

    Keywords:

    Fenton reaction

    Co-catalytic

    Molybdenum dioxide

    Fe3+/Fe2+conversion

    Dye wastewater

    ABSTRACT

    There is a relatively low efficiency of Fe(III)/Fe(II) conversion cycle and H2O2 decomposition (<30%) in conventional Fenton process, which further results in a low production efficiency of· OH and seriously restricts the application of Fenton.Herein, we report that the commercial MoO2 can be used as the cocatalyst in Fenton process to dramatically accelerate the oxidation of Lissamine rhodamine B(L-RhB),where the efficiency of Fe(III)/Fe(II)cycling is greatly enhanced in the Fenton reaction meanwhile.And the L-RhB solution could be degraded nearly 100%in 1 min in the MoO2 cocatalytic Fenton system under the optimal reaction condition,which is apparently better than that of the conventional Fenton system(~50%).Different from the conventional Fenton reaction where the· OH plays an important role in the oxidation process,it shows that 1O2 contributes most in the MoO2 cocatalytic Fenton reaction.However,it is found that the exposed Mo4+active sites on the surface of MoO2 powders can greatly promote the rate-limiting step of Fe3+/Fe2+cycle conversion,thus minimizing the dosage of H2O2(0.400 mmol/L)and Fe2+ (0.105 mmol/L).Interestingly, the MoO2 cocatalytic Fenton system also exhibits a good ability for reducing Cr(VI)ions,where the reduction ability for Cr(VI)reaches almost 100%within 2 h.In short,this work shows a new discovery for MoO2 cocatalytic advanced oxidation processes(AOPs),which devotes a lot to the practical water remediation application.

    In recent years,the excessive wastewater discharge containing organic and inorganic pollution from different industry like textiles, printing, leather and cosmetics, is endangering the environment and ecology, and reversely limited the industry development [1-4].To deal with the problem, some strategies were adopted usually, such as membrane technology [5,6],biodegradation [7,8]and physicochemical processes [9-11].So far, there is no single method is as effective as the method we mentioned above to reasonably handle wastewater composed of mixture toxic chemicals (phenols, dyes, pesticides, organic solvents, etc.).Up to now, advanced oxidation processes (AOPs)are chosen as an effective solution with gentle operation condition of room temperature and pressure.Different from the conventional wastewater remediation methods,the in situ generated hydroxyl radicals(·OH)counts in the AOPs strategy,which owns a relatively strong oxidation potential of 2.80 V[12,13].Fenton process is used as a kind of conventional AOPs, where the hydrogen peroxide(H2O2)plays as the oxidant and meanwhile the Fe2+ion plays as the catalyst,involving a redox reaction along with releasing enormous amount of·OH in a while [14-16].And the main active species generation mechanism in the Fenton process can be divided and reduced into three steps, as shown in Eqs.(1-3).

    Research on the Number of Mill in 660 MW Super-critical Unit of “W” Flame Furnace DUAN Yuyan,LI Weike,FAN Xiaoru,WU Afeng,HUO Peiqiang(127)

    According to Eq.(2),it can be known that the mainly efficiency limitation in the Fe(II)/H2O2system is the comparatively low constant of k2corresponding to the step of Fe3+/Fe2+cycle.Besides,it is also is confronted with some trouble in practical application,for instance, the high cost, the limited pH range, the sustainably produced iron sludge,and challenges in reusing the homogeneous catalyst(Fe2+).Even worse,a high concentration of Fe3+ions would lead to a reaction poisoning in conventional Fenton process.Thus,it does call for a valid solution to accelerate the reaction of the ratelimiting step of Eq.(2) to promote the Fe3+/Fe2+cycle process.On one hand,it can help produce more Fe2+ions.On the other hand,it can also reduce the generation of iron sludge.

    Based on our previous work, it was found that metal sulfides(MoS2, WS2, CoS2, etc.) could greatly promote Fenton reaction as cocatalysts, because of the exposed reductive metal sites on the surface of cocatalysts [4,17].However, it makes a potential secondary contamination risk to the environment for the release of hydrogen sulphide.Herein,we employed MoO2instead of MoS2as a cocatalyst to increase the H2O2decomposition efficiency and decrease the consumption of H2O2and Fe2+in AOPs for the remediation of Lissamine rhodamine B (L-RhB).Generally,·OH radicals are considered as the main reactive oxygen species(ROS)for oxidation of organic pollutants in Fenton Process.Interestingly,in the MoO2co-catalytic system,it is found that the singlet oxygen(1O2)acts as the main ROS for the oxidation,which is demonstrated to be involved with the transformation from·OH radicals to singlet oxygen (1O2) on the surface of MoO2.Meanwhile, it can also achieve the goal of reducing of Cr(VI)in suspension,which shows a synchronous REDOX activity over Fenton reaction.

    努力使工程施工形成可視化記錄。對隱蔽工程的每道工序的驗收,進行拍攝,形成圖片檔案;在水泥攪拌樁的施工中,我們分別在鉆機的前后聲安裝了兩個攝像頭,做到了相關(guān)管理人員不在現(xiàn)場就能隨時檢查工程施工情況,以及關(guān)鍵后期的檢查;項目部還利用無人機進行巡航拍攝,以記錄工地當時的整個現(xiàn)場情況。

    First of all,to optimize the reaction conditions,the effects of pH value, Fe2+concentration, hydroxyl peroxide (H2O2) and MoO2powder dosage in the degradation of L-RhB were investigated in Fig.1.In our case, all the Fenton experiments were carried out under dark situation at room temperature.As a result, the optimum condition of MoO2cocatalytic Fenton reaction for the remediation of L-RhB is fixed at: pH~3.4, FeSO4·7H2O dosage of 30 mg/L, H2O2concentration of 0.4 mmol/L and MoO2powder dosage of 30 mg/L.As can be seen in Fig.1a,when pH value is near neutral condition,the efficiency was obviously inhibited,which is ascribed to the loss of dissolution of iron ions.Additionally, in Fig.1b, the activity of degrading L-RhB was not significantly improved with the continuous increase of Fe2+concentration,which indicates that H2O2has achieved a complete decomposition and the excessive iron ions cannot significantly produce more ROS.Moreover, when H2O2added slowly, the Fenton efficacy firstly shows an increasing trend,and then followed by a downward trend because that H2O2possesses both oxidative and reductive ability(Fig.1c).Seen from Fig.1d, as the adding amount of MoO2increased,the Fenton activity tends to increase,indicating that the cocatalyst plays a vital role on reaction kinetics of the Fenton reaction.In addition, we have carried out the apparent kinetic calculation of MoO2cocatalytic Fenton reaction for the remediation of L-RhB, as shown in Fig.S1 (Supporting information).As a result,according to the apparent kinetic equation(Eq.4),the total reaction constant of “a+b+c” equals to 2.229, which implies that the adding of FeSO4·7H2O, H2O2and MoO2are beneficial to improving the efficiency of Fenton process.

    Although it has been proved that the MoO2can promote the conversion from Fe3+to Fe2+during the Fenton reaction,it cannot determine whether the reduction process occurs in solution or on the surface of MoO2.Thus, the coumarin and benzoic acid are employed as the trapping agents for the trapping of ROS in the solution and on the surface of MoO2,respectively.Coumarin has a weak polarity, and it is not easily soluble in water, thus cannot adsorb on the surface of MoO2to capture·OH.However, benzoic acid is negatively charged in aqueous solution and easily adsorbed on MoO2(When pH value is 3.4, the MoO2surface is positively charged,as shown in Fig.S8 in Supporting information).It can be seen that the “Coumarin+H2O2+Fe2++MoO2” shows an obvious decrease signal for the trapping of·OH in the solution, compared with that of“Coumarin+H2O2+Fe2+”(Fig.3a).On the contrary,the“Fe2++H2O2+MoO2+C6H5COOH”shows a significant increase signal for the trapping of·OH, compared with that of “Fe2++H2O2+C6H5-COOH” (Fig.3b).Hence, we can conclude that the cocatalytic reaction mainly occurs on the surface of MoO2.Although·OH radicals are detected on the surface of MoO2in the cocatalytic Fenton system, it does not mean that·OH play a direct role in the oxidation reaction.Since·OH radicals have a relatively short lifetime(<2 ns),it is reasonable to believe that·OH radicals are the main precursors for the formation of1O2.1O2has a relatively long lifetime (2~3.5 μs) and can be diffused into aqueous solution to oxidize and degrade the organic pollutants.It is also worth mentioning that we cannot rule out that·O2-can also be converted to1O2in the presence of Mo6+[21].

    where V is the reaction rate of the Fenton degradation reaction;c is the concentration of Lissamine rhodamine B; t is time.

    Fig.1.Fenton degradation performance of L-RhB (20 mg/L) by adding cocatalyst of MoO2 at different conditions: (a) different pH value; (b) different FeSO4·7H2O concentration;(c) different H2O2 dosage;(d)different MoO2 concentration.(e)Degradation of L-RhB (20 mg/L) over different Fenton systems.(f)Cycling test of the MoO2 cocatalytic Fenton reaction for the degradation of L-RhB (20 mg/L).(g) XRD patterns of co-catalyst of MoO2 before and after cycle test.(h) High performance liquid chromatography (HPLC) spectra of different reaction products for the L-RhB (20 mg/L) degradation over different Fenton systems.

    In summary, we have developed an inorganic catalytic system by MoO2in Fenton process.With the aid of Mo4+active metallic sites exposed on MoO2's surface,the efficiency of Fe(III)/Fe(II)cycle and the precipitation of iron sludge can be significantly enhanced and inhibited, respectively.Noticeably, it is found that1O2is responsible for the degradation of L-RhB by the cocatalytic effect of commercial MoO2in Fenton reaction.Simultaneously, MoO2cocatalytic AOPs can also achieve the reduction of Cr(VI).The MoO2catalytic system not only achieves the goal of oxidizing organic pollutants,but also realizes the reduction of heavy metals.Thus,it can be expected that this work provides some guidance for1O2radicals dominated Fenton process and push forward the development of inorganic cocatalytic Fenton system for the mineralization of organic-inorganic contaminants to build a reliable platform for environmental remediation.

    The authors declare that they have no conflicts of interest to this work.

    Fig.2.(a)EPR spectra for the detection of· OH(the EPR signals are marked as green square)in the presence of DMPO by using water as the solvent.(b)EPR spectra for the detection of· O2-(the EPR signals are marked as yellow circle)in the presence DMPO by using methanol as the solvent.(c)EPR spectra for the detection of1O2(the EPR signals are marked as purple rhombus) in the presence of 2,2,6,6-tetramethylpiperidine (TEMP) by using water as the solvent.(d) Degradation curve of L-RhB (20 mg/L) over cocatalytic Fenton system in the presence of different radical scavengers including BQ and Trp for the quenching of· OH,·O2-and1O2,respectively,under the optimal situation.(e)Increasing TAB and BQ for the quenching of· OH and·O2-,respectively,for the degradation of L-RhB(20 mg/L).(f)Fe2+/Fe3+ratio during the Fenton reaction(blue line:conventional Fenton process, red line: MoO2 cocatalytic Fenton process).

    ? ? Bargen, Mediation im Verwaltungsprozess, DVBI.2004,S.472.

    In our case, MoO2powder is ineluctably dissolved in acidic aqueous solution.Therefore, it is important to study the effect of dissolved molybdenum ions(Mox+)on Fenton reaction.We soak the MoO2powders in an acidic water solution (pH 3.6) to ensure adequate molybdenum ions dissolving out.It has monitored the total content of Mox+in the solution at different time by ICP test,which shows that the concentration of dissolved Mox+would gradually reach a maximum value of 0.61 mg/L at about 90 min,and it would not to continue to increase(Fig.S11 in Supporting information).This shows that molybdenum ions do not dissolve continuously, so the possibility of secondary pollution can be excluded.The MoO2was immersed in the solution for 0 min, 30 min and 120 min, and the supernatant is used for the Fenton reaction,as shown in Fig.3f.It is foundthat with the extension of immersing time,the Fentonactivity for the degradation of L-RhB increased first and then decreased owing to the that excessive dissolution of Mox+ions can also consume the ROS.Different from the stable MoO2cocatalytic Fenton system(Fig.1f),the Mox+cocatalytic Fenton reaction shows a poor stability for the degradation of L-RhB(Fig.3g).It can be found that after two cycles,the Fenton efficiency has been reduced to 50%.And after three cycles,the efficiency merely achieved 30%.Overall,we can conclude that Mox+ionsin solution could have animpactin Fenton process,but not so competitive with the Mox+ions on MoO2's surface.

    Fig.3.(a)Coumarin and(b)benzoic acid fluorescence spectrophotometry for the detection of· OH;(c)Mo 3d XPS spectrum of MoO2;(d)Fe 2p XPS spectrum of iron adsorbed on MoO2 surface; (e) Schematic illustration of the cocatalytic mechanism of MoO2 in Fenton reaction; (f) Molybdenum ions (Mox+) cocatalytic Fenton reaction for the degradation of L-RhB(20 mg/L)(MoO2 was immersed in the solution for different times(pH 3.6):0 min,30 min,120 min);(g)Cycle test of Mox+cocatalytic Fenton system for the remediation of L-RhB (20 mg/L) (adding 4 μL of H2O2 for each cycle); (h) MoO2 cocatalytic Fenton reaction for the reduction of Cr(VI) (15 mg/L, K2Cr2O7); (i) Various control experiments for the reduction of Cr(VI) (15 mg/L, K2Cr2O7).

    Since it has been known that the cocatalytic reactions occur mainly on the surface of MoO2, studying the surface chemistry of the catalyst is crucial to reveal the cocatalytic Fenton mechanism.Mo 3d XPS spectra were employed to study the surface chemical environment of MoO2powder,as shown in Fig.3c.As to the MoO2powder, there are two types of molybdenum ions on the surface:Mo4+and Mo6+.Seen from Fig.3d,it is confirmed the existence of Fe3+ions on the catalysts surface, whose characteristic binding energy located at 710.5 eV [22].This founding suggests the occurring of Fe3+/Fe2+cycle reaction on the surface of MoO2.To further investigate the reaction mechanism of MoO2cocatalytic Fenton reaction, the effect of MoO2powder on the Fe3+/Fe2+conversion was studied in this case.The concentration of ferrous and ferric ions in the solution can be observed by using UV-vis analysis with potassium thiocyanate and 1,10-ophenanthroline acting as the probes for the detection of Fe3+and Fe2+,respectively(Fig.S9 in Supporting information).It can be observed that Fe2+was instantly oxidized to Fe3+by H2O2(Eq.1).Interestingly, the addition of MoO2powder can significantly increase the Fe2+ions but decrease the Fe3+ions in solution(Eq.5 and Fig.S9).It can be concluded that the exposed metallic active sites of Mo4+with reductive properties over MoO2powder are expected to accelerate the rate-limiting step of Fe3+/Fe2+conversion and promote the decomposition of H2O2to form·O2-and·OH radicals.Moreover,the H2O2decomposition efficiency can also be obviously increased by the adding of MoO2powder in the Fenton reaction (Fig.S10 in Supporting information).Based on above analysis, it can be proposed the possible mechanism, as shown in Fig.3e.The first step was involved with the exposed Mo4+for the reduction of Fe3+adsorbed on the MoO2surface, which could accelerate the ratelimiting step of Fe3+/Fe2+conversion (Eq.5).Simultaneously, the Fe2+ions in solution reacted with O2to produce·O2-radicals(Eq.6).Subsequently,the H2O2reacted with·O2-or Fe2+to produce·OH radicals(Eqs.7 and 8).Due to the short lifespan of·OH radicals,the generated·OH radicals would transform into1O2on the MoO2surface by the disproportionation reaction (Eq.9).As a result,the enhanced efficiency of Fe3+/Fe2+conversion would decrease the Fe3+amount and weaken the catalysts poisoning during the Fenton reaction.And the generated1O2would migrate into solution to degrade the organic pollutants.

    Since it has been proved that molybdenum ions on the surface of MoO2can promote the conversion from Fe3+to Fe2+, we cannot ignore the reduction performance of MoO2in the Fenton reaction.It is well known that inorganic contamination is a significant environmental hazard to drinking water treatment.To be specific,hexavalent chromium species Cr(VI),are highly toxic agents,acting as carcinogens,mutagens,and teratogens in biological systems[23].According to the U.S.EPA action level,the standard for chromium is 0.1 mg/L for Cr [24].Commonly, hexavalent chromium exists in was tewater as oxyanions,suchaschromate(CrO42-)and dichromate(Cr2O72-), which do not precipitate easily using conventional precipitation methods.Thus, adsorption technology, as one of the most promising techniques for removal of chromium from industrial waste waters,has been employed for many years[25,26].However,the adsorption method cannot only remove Cr(VI)but also recover them back into the industrial process[27].Thus,it is imperative to develop an effective method to restrain the Cr(VI) back to the industrial process.Chemical redox followed by precipitation is often employed for the remediation of Cr(VI) [28-30].In our previous work,it was found that Fenton system could reduce Cr(VI)to Cr(III)[1],via the cocatalytic effect of WS2.However,sulfides can release hydrogen sulfide and cause the potential risk of secondary pollution.In this work,MoO2was employed as cocatalyst in Fenton process for the reduction of Cr(VI), owing to the exposed metallic Mo4+sites.The Cr(VI) reduction rate can be enhanced about 40%(Fig.3h), in comparison with the conventional Fenton process.Single ferrousions couldreduce Cr(VI)(Fig.3i),ascribed to the redox reaction(Eq.10)[31].Apparently,the ferric ions were not beneficial to reduce Cr(VI).Similarly, Fe2++H2O2system exhibits higher reduction activity than Fe3++H2O2system, owing to the weak reducing capacity of Fe3+.And Fe3++H2O2system shows a higher reducing activity than that of blank Fe3+,because of the reduction ability of H2O2[32].However, both Fe2++H2O2and Fe3++H2O2systems show an inhibition trend after 5 min,attributing to the loss of ferrous ions in suspension.Unsurprisingly, when MoO2was added into the system, it was obviously found that the inhibition effect of Cr(VI) could be ended.The MoO2's surface is positively charged(pH~4)(Fig.S8),leading to the adsorption of Cr2O72-onthe surface of MoO2due to the electrostatic effect.Hence, it can be proposed that the exposed metallic Mo4+sites also can directly reduce Cr(VI)(Eq.11).It is not strange that the Fe2++MoO2system could reduce Cr(VI)more effectively than Fe2++H2O2+MoO2,owing to the reducing of Cr(VI) by the exposed metallic Mo4+.Although H2O2has certain reducibility(Fig.S12 in Supporting information),its property is very unstable.Especially in the presence of Fe2+,H2O2preferentially oxidizes Fe2+into Fe3+(Eq.1), thus weakening the activity of Fe2+in reducing Cr(VI).Therefore,under the presence of H2O2,Cr(VI)reduction is not necessarily promoted.

    Declaration of competing interest

    Based on the above experimental results,all the Fenton systems for the degradation of L-RhB are fixed under the optimal reaction condition: pH~3.4, FeSO4·7H2O dosage of 30 mg/L, H2O2concentration of 0.4 mmol/L and MoO2powder dosage of 30 mg/L, as shown in Fig.1e.The MoO2+FeSO4+H2O2system can degrade 99% of L-RhB within 3 min, whereas the conventional Fenton system merely degraded 60% in 3 min.And it was found that the MoO2Fenton system can develop the TOC removal rate of L-RhB from 30.53% to 70.53% comparing to the conventional Fenton (Fig.S2 in Supporting information).In addition, although MoO2is a kind of semiconductor,it has no photocatalytic activity for degrading L-RhB under the simulated solar light irradiation(Fig.S3 in Supporting information).Meanwhile, in the absence of Fe2+ions or H2O2, the corresponding efficiencies for the remediation of L-RhB could be neglected(<10%).Various concentrations of L-RhB were also be degraded by the conventional Fenton and MoO2cocatalytic Fenton systems (Fig.S4 in Supporting information).When the concentration of L-RhB increases from 20 mg/L to 80 mg/L, it shows a downward trend.Furthermore, it has been explored the intermediates by high performance liquid chromatography(HPLC)during the Fenton process(Fig.1h).Three systems(blank LRhB, conventional Fenton, MoO2cocatalytic Fenton) were compared for HPLC detection.It can be clearly elucidated that the peak of residual L-RhB corresponding to the MoO2cocatalytic system is the weakest, and the peaks of intermediate products are also the least.In addition, the cyclic experiment of cocatalytic Fenton system is conducted as well, as shown in Fig.1f and g.The degradation rate can keep up to 99.9%after 5 cycles,and the mass and microstructure of MoO2are almost unchanged after cycle test (Fig.S5 in Supporting information), further confirming the stability of MoO2during the Fenton reaction.The low dosage of Fe2+(0.105 mmol/L) and H2O2(0.4 mmol/L) used in the MoO2cocatalytic Fenton reaction can effectively prevent the formation of iron sludges, thus avoiding catalyst poisoning.To further understand the decomposition mechanism of organic pollutant,the mass spectra of intermediates in LC chromatogram during the degradation process of L-RhB over MoO2cocatalytic Fenton system was analyzed, as shown in Fig.S6 (Supporting information).The whole degradation process has gone through deoxygenation,debenzene ring, deethylation and dehydroxylation steps.As a result,the L-RhB was finally decomposed into small fatty molecule of CH3COOH.

    日前,山東省農(nóng)藥管理評審專家委員會在省農(nóng)業(yè)農(nóng)村廳召開2018年度評審例會,經(jīng)集體審議,萊陽市豐禾植保農(nóng)資有限責任公司等65家經(jīng)營者符合限制使用農(nóng)藥經(jīng)營許可條件。對審議通過的經(jīng)營者,經(jīng)公示無異議后,予以核發(fā)農(nóng)藥經(jīng)營許可證。

    白粉虱又稱小白蛾子,其成蟲和若蟲群聚在西葫蘆葉片背面吸食汁液,使葉片褪綠、變黃、葉片萎蔫,甚至全株枯死,降低產(chǎn)量和品質(zhì)。白粉虱還能傳播病毒病和分泌大量的蜜露污染葉片和果實。

    To study the mechanism of MoO2cocatalytic Fenton process,it is of great significance to identify the ROS during the reaction.It has been reported that·OH, as well as·O2-and1O2co-work in Fenton process [18].Moreover, some researchers have reported that the1O2can be generated by the disproportionation of·OH radicals [19].In this case, 5,5-dimethyl-1-pyrrolidine-N-oxide(DMPO) and 2,2,6,6-tetramethylpiperidine (TEMP) are employed to capture the·OH/·O2-and1O2, respectively, for the EPR characterization (Figs.2a-c).It can be clearly seen that the MoO2cocatalytic Fenton system exhibits an obvious decrease of·OH/·O2-radicals, whereas a slight increase of·O2-radicals,compared with that of conventional Fenton reaction.This result is totally opposed to previous research [20], which means that the MoO2cocatalytic Fenton system undergoes different reaction paths.The decrease generation of·OH and·O2-radicals may contribute to the increased1O2generated in MoO2cocatalytic system.To further investigate the mechanism of MoO2cocatalytic Fenton process,some quenching tests have been conducted under various conditions.Tert-butyl alcohol(TBA),p-benzoquinone(BQ)and tryptophan (Trp) were used as the quenching agents of·OH,·O2-and1O2,respectively[21].In Fig.2d,it is found that the adding of TBA and BQ cannot effectively inhibit the reaction; however,when Trp was added, the Fenton efficiency was obviously constrained.To be more specific,~3-fold amounts of the TBA and BQ are added in the reaction, and it merely showed a slight inhibitory effect(Fig.2e).Based on these results,we can conclude that1O2radicals play a vital role in cocatalytic Fenton reaction.Additionally, the concentration of Fe2+ion in Fenton is an important quantitative standard.Seen from Fig.2f, the Fe2+/Fe3+ratio increased to 4.38 in MoO2cocatalytic system compared with conventional Fenton reaction,indicating the enhancing conversion efficiency from Fe3+to Fe2+by the cocatalytic effect of MoO2.In addition, it has been added the data of Fenton degradation performance of L-RhB by adding Fe3+instead of Fe2+.Seen from Fig.S7 (Supporting information), the results showed that the activity of Fe3++H2O2was very poor for the degradation of L-RhB,but once MoO2was added, the Fenton activity of Fe3+decomposition of H2O2was greatly increased,which indicated that MoO2could rapidly reduce Fe3+to Fe2+, thus showing excellent Fenton activity.

    Acknowledgments

    This work was supported by the State Key Research Development Program of China (No.2016YFA0204200), National Natural Science Foundation of China (Nos.21822603, 21811540394,5171101651, 21677048, 21773062, 21577036), Shanghai Pujiang Program(No.17PJD011),and the Fundamental Research Funds for the Central Universities(No.22A201514021).Project supported by Shanghai Municipal Science and Technology Major Project (No.2018SHZDZX03) and the Program of Introducing Talents of Discipline to Universities (No.B16017).The authors thank to Research Center of Analysis and Test of East China University of Science and Technology for the help on the characterization.

    Appendix A.Supplementary data

    Supplementary material related to this article can be found,inthe online version,at doi:https://doi.org/10.1016/j.cclet.2019.09.052.

    猜你喜歡
    萊陽市蜜露白粉
    踢毽子
    蔬菜白粉虱 秋防正當時
    蝴蝶花
    清風(2020年12期)2020-09-10 08:34:54
    這是我應(yīng)該知道的
    這是我應(yīng)該知道的
    做個內(nèi)心強大的人
    保護地蔬菜白粉虱的發(fā)生與防治
    1981—2010年冬季萊陽市低溫日的氣候特征分析
    文化語言學視角下的萊陽村莊地名探究
    白僵菌防治溫室大棚白粉虱藥效試驗
    国产亚洲91精品色在线| 国产亚洲av片在线观看秒播厂| 亚洲精品一二三| 制服丝袜香蕉在线| 菩萨蛮人人尽说江南好唐韦庄| 少妇裸体淫交视频免费看高清| 在线 av 中文字幕| 91成人精品电影| 女人久久www免费人成看片| 亚洲国产精品一区二区三区在线| 亚洲精品色激情综合| av国产久精品久网站免费入址| 久久久久久久大尺度免费视频| 97超碰精品成人国产| 成人毛片a级毛片在线播放| 色吧在线观看| 日本欧美国产在线视频| 国产色婷婷99| 美女大奶头黄色视频| xxx大片免费视频| 国产成人免费无遮挡视频| 日本黄色片子视频| 久久久久久久久久成人| 国产精品福利在线免费观看| 久久青草综合色| 欧美丝袜亚洲另类| 国产成人freesex在线| 国产黄频视频在线观看| 啦啦啦中文免费视频观看日本| 日本黄色片子视频| 精品人妻熟女毛片av久久网站| 亚洲精品久久久久久婷婷小说| 午夜久久久在线观看| 国产精品嫩草影院av在线观看| 狠狠精品人妻久久久久久综合| 欧美人与善性xxx| 蜜臀久久99精品久久宅男| 欧美少妇被猛烈插入视频| 日韩亚洲欧美综合| 日韩精品免费视频一区二区三区 | videos熟女内射| 久久久久久久久久久免费av| av免费在线看不卡| 在线 av 中文字幕| 国产精品国产av在线观看| 天天躁夜夜躁狠狠久久av| 午夜激情久久久久久久| 少妇 在线观看| 午夜视频国产福利| 国产精品成人在线| 日日摸夜夜添夜夜爱| 如何舔出高潮| 国产男女超爽视频在线观看| 大码成人一级视频| 狂野欧美白嫩少妇大欣赏| 午夜免费观看性视频| 欧美精品人与动牲交sv欧美| 日韩强制内射视频| 国产亚洲一区二区精品| 五月开心婷婷网| 少妇被粗大猛烈的视频| 成人无遮挡网站| 国产日韩欧美亚洲二区| 我的老师免费观看完整版| 自拍欧美九色日韩亚洲蝌蚪91 | 亚洲av中文av极速乱| 国产亚洲最大av| 国产中年淑女户外野战色| 国产在线男女| 日本色播在线视频| 少妇裸体淫交视频免费看高清| 免费看日本二区| 伊人久久精品亚洲午夜| 99久久精品热视频| 久久国内精品自在自线图片| 久久久精品免费免费高清| 两个人的视频大全免费| 激情五月婷婷亚洲| 建设人人有责人人尽责人人享有的| 中文资源天堂在线| 国产真实伦视频高清在线观看| 一级毛片久久久久久久久女| 九九爱精品视频在线观看| 国产成人精品福利久久| www.色视频.com| 成人无遮挡网站| 丝袜喷水一区| 亚洲av国产av综合av卡| 一区二区三区四区激情视频| av在线老鸭窝| 亚洲精品久久久久久婷婷小说| 美女xxoo啪啪120秒动态图| 久久99热6这里只有精品| 国产精品99久久久久久久久| 99热网站在线观看| 人妻少妇偷人精品九色| 精品少妇黑人巨大在线播放| 国产精品国产三级国产av玫瑰| 国内精品宾馆在线| 欧美高清成人免费视频www| 精品人妻偷拍中文字幕| 欧美日韩视频高清一区二区三区二| 嘟嘟电影网在线观看| 国产在线免费精品| 又粗又硬又长又爽又黄的视频| 人妻少妇偷人精品九色| www.av在线官网国产| 人人妻人人澡人人看| 精品国产国语对白av| 免费黄网站久久成人精品| 人人妻人人看人人澡| 亚洲,欧美,日韩| 久久久久久久久久人人人人人人| 久久99一区二区三区| 久久精品国产自在天天线| 啦啦啦在线观看免费高清www| 91久久精品国产一区二区三区| 亚洲欧美日韩卡通动漫| av.在线天堂| 特大巨黑吊av在线直播| 国产高清三级在线| a级片在线免费高清观看视频| 99re6热这里在线精品视频| 国内少妇人妻偷人精品xxx网站| 十分钟在线观看高清视频www | 精品一区二区三区视频在线| 一级av片app| 亚洲精品日韩在线中文字幕| 中文在线观看免费www的网站| 精品人妻熟女毛片av久久网站| 一级av片app| 久久精品国产亚洲av涩爱| 免费高清在线观看视频在线观看| 日韩成人av中文字幕在线观看| 99热6这里只有精品| 91精品一卡2卡3卡4卡| 高清黄色对白视频在线免费看 | 男女无遮挡免费网站观看| 制服丝袜香蕉在线| 国产精品三级大全| 久热久热在线精品观看| 国产熟女欧美一区二区| 色吧在线观看| 少妇熟女欧美另类| 午夜福利,免费看| 国产真实伦视频高清在线观看| 成人18禁高潮啪啪吃奶动态图 | 久久久久久久久久久丰满| 熟女电影av网| 激情五月婷婷亚洲| 欧美成人精品欧美一级黄| 国产白丝娇喘喷水9色精品| 国产成人91sexporn| 亚洲高清免费不卡视频| 国产日韩欧美在线精品| 国产亚洲5aaaaa淫片| 成人特级av手机在线观看| 啦啦啦视频在线资源免费观看| 国产精品久久久久久久久免| 亚洲国产最新在线播放| 国产一区有黄有色的免费视频| 亚洲电影在线观看av| 国产男女内射视频| 丝袜在线中文字幕| 午夜福利在线观看免费完整高清在| 一级片'在线观看视频| 少妇 在线观看| 麻豆成人av视频| 如日韩欧美国产精品一区二区三区 | 国产有黄有色有爽视频| 日韩中文字幕视频在线看片| 欧美丝袜亚洲另类| 国产有黄有色有爽视频| 久久综合国产亚洲精品| 国产色爽女视频免费观看| 伊人亚洲综合成人网| 777米奇影视久久| 国产中年淑女户外野战色| 人人妻人人爽人人添夜夜欢视频 | 国产视频内射| 国产av精品麻豆| 2018国产大陆天天弄谢| 香蕉精品网在线| 九九在线视频观看精品| 久久影院123| 亚洲国产欧美日韩在线播放 | 97精品久久久久久久久久精品| 国产精品99久久久久久久久| 国产一区亚洲一区在线观看| 欧美丝袜亚洲另类| 高清黄色对白视频在线免费看 | av福利片在线观看| 噜噜噜噜噜久久久久久91| 成年av动漫网址| 国产精品久久久久久久电影| 亚洲情色 制服丝袜| 亚洲精品国产av蜜桃| 国产有黄有色有爽视频| 亚洲精品久久午夜乱码| 欧美97在线视频| 国产精品国产三级专区第一集| 中文字幕av电影在线播放| 精品亚洲成国产av| 中文欧美无线码| videossex国产| 成年女人在线观看亚洲视频| 人人妻人人澡人人看| 五月天丁香电影| 两个人免费观看高清视频 | 国产精品麻豆人妻色哟哟久久| 日韩一本色道免费dvd| 丰满迷人的少妇在线观看| 国产深夜福利视频在线观看| 国产亚洲5aaaaa淫片| 精品卡一卡二卡四卡免费| 在线免费观看不下载黄p国产| 国产无遮挡羞羞视频在线观看| 国产淫语在线视频| 亚洲av二区三区四区| 国产精品国产三级专区第一集| 国产真实伦视频高清在线观看| 亚洲高清免费不卡视频| 亚洲国产精品999| 国产一区二区在线观看av| 国产黄色视频一区二区在线观看| av天堂中文字幕网| 亚洲精品国产成人久久av| 欧美成人精品欧美一级黄| 午夜福利在线观看免费完整高清在| 国产精品一区二区在线不卡| 国产成人精品一,二区| 街头女战士在线观看网站| videossex国产| 在线播放无遮挡| 99热网站在线观看| 热re99久久精品国产66热6| 最近中文字幕2019免费版| 亚洲精品国产成人久久av| 精品99又大又爽又粗少妇毛片| 高清黄色对白视频在线免费看 | 肉色欧美久久久久久久蜜桃| 一区二区三区四区激情视频| 18+在线观看网站| 国产一区二区在线观看av| 亚洲精品第二区| 亚洲av二区三区四区| 国产视频首页在线观看| 成人美女网站在线观看视频| 久久久久精品久久久久真实原创| 丰满饥渴人妻一区二区三| 欧美最新免费一区二区三区| 日韩成人av中文字幕在线观看| 久久国产精品男人的天堂亚洲 | 这个男人来自地球电影免费观看 | 精品亚洲成国产av| 国产极品粉嫩免费观看在线 | 亚洲精品国产av蜜桃| 22中文网久久字幕| 午夜福利影视在线免费观看| 国产精品一区二区三区四区免费观看| 在线观看国产h片| 乱码一卡2卡4卡精品| 在线观看免费日韩欧美大片 | 夜夜爽夜夜爽视频| 99久久精品热视频| 欧美 日韩 精品 国产| 伊人亚洲综合成人网| 美女内射精品一级片tv| 久久久久国产网址| 国产精品女同一区二区软件| 亚洲人成网站在线观看播放| 亚洲自偷自拍三级| 精品人妻一区二区三区麻豆| 精品久久久久久久久亚洲| a 毛片基地| 成人免费观看视频高清| 一级毛片久久久久久久久女| 两个人免费观看高清视频 | 国产精品人妻久久久久久| 视频区图区小说| 一级黄片播放器| 日本免费在线观看一区| 午夜福利视频精品| 久久精品国产亚洲av涩爱| 国产亚洲午夜精品一区二区久久| 少妇精品久久久久久久| 亚洲美女视频黄频| 晚上一个人看的免费电影| 天天躁夜夜躁狠狠久久av| av国产久精品久网站免费入址| 国产精品不卡视频一区二区| 国产亚洲午夜精品一区二区久久| 久久久久久久亚洲中文字幕| 久久精品久久久久久噜噜老黄| 曰老女人黄片| 制服丝袜香蕉在线| 亚洲成人手机| 久久久久国产网址| 亚洲精品久久午夜乱码| 午夜免费观看性视频| 搡女人真爽免费视频火全软件| 欧美 亚洲 国产 日韩一| 亚洲无线观看免费| 国产视频首页在线观看| 欧美激情国产日韩精品一区| 国产视频首页在线观看| 久久久精品免费免费高清| 美女国产视频在线观看| 亚洲精品国产av蜜桃| 自拍偷自拍亚洲精品老妇| 男人爽女人下面视频在线观看| 亚洲成色77777| 在线观看美女被高潮喷水网站| 99久久精品一区二区三区| 国产精品国产三级国产av玫瑰| 亚洲国产成人一精品久久久| 深夜a级毛片| 久久精品夜色国产| 成人毛片60女人毛片免费| 男男h啪啪无遮挡| 中国美白少妇内射xxxbb| 久久久国产一区二区| 丁香六月天网| 一级毛片 在线播放| 国产91av在线免费观看| 最黄视频免费看| a级毛色黄片| 91午夜精品亚洲一区二区三区| 男人和女人高潮做爰伦理| 国产熟女欧美一区二区| 一本大道久久a久久精品| av天堂中文字幕网| 久久6这里有精品| 人人妻人人爽人人添夜夜欢视频 | 国产精品麻豆人妻色哟哟久久| 亚洲伊人久久精品综合| 欧美成人午夜免费资源| 搡女人真爽免费视频火全软件| 国产精品蜜桃在线观看| 哪个播放器可以免费观看大片| 国产精品国产三级国产专区5o| 日韩av不卡免费在线播放| 在现免费观看毛片| 天天操日日干夜夜撸| 亚洲欧美清纯卡通| 精品熟女少妇av免费看| 国内精品宾馆在线| 亚洲国产精品一区二区三区在线| 老司机亚洲免费影院| 99精国产麻豆久久婷婷| 插阴视频在线观看视频| 一级毛片黄色毛片免费观看视频| 精品久久久精品久久久| 免费观看在线日韩| 男人和女人高潮做爰伦理| 肉色欧美久久久久久久蜜桃| 热99国产精品久久久久久7| 在线天堂最新版资源| 亚洲婷婷狠狠爱综合网| 99视频精品全部免费 在线| 午夜福利视频精品| 久久久国产精品麻豆| 亚洲欧美日韩卡通动漫| 亚洲经典国产精华液单| 精品久久久精品久久久| 亚洲欧美一区二区三区黑人 | 国产极品天堂在线| 日本黄色片子视频| 久久国产乱子免费精品| 在线亚洲精品国产二区图片欧美 | 亚洲成人手机| 九九在线视频观看精品| 日本欧美国产在线视频| 永久免费av网站大全| 色婷婷久久久亚洲欧美| 亚洲精品aⅴ在线观看| 老司机影院成人| 成年美女黄网站色视频大全免费 | 久久狼人影院| 国产亚洲午夜精品一区二区久久| 日韩在线高清观看一区二区三区| 色视频在线一区二区三区| 一个人看视频在线观看www免费| 亚洲情色 制服丝袜| 麻豆成人av视频| 视频中文字幕在线观看| 岛国毛片在线播放| 好男人视频免费观看在线| 大陆偷拍与自拍| 精品少妇内射三级| 日本免费在线观看一区| 国产淫片久久久久久久久| 天天操日日干夜夜撸| 水蜜桃什么品种好| 国产黄频视频在线观看| 特大巨黑吊av在线直播| 精品一区二区免费观看| 国产免费又黄又爽又色| 免费av中文字幕在线| 人妻 亚洲 视频| 国产高清国产精品国产三级| 在线精品无人区一区二区三| 国产成人免费无遮挡视频| 成人亚洲精品一区在线观看| 亚洲精品国产av成人精品| 亚洲第一区二区三区不卡| 亚洲av免费高清在线观看| 国产精品一区二区性色av| 曰老女人黄片| 亚洲精品,欧美精品| 欧美丝袜亚洲另类| 视频区图区小说| 高清在线视频一区二区三区| 欧美精品国产亚洲| 欧美高清成人免费视频www| 国产亚洲最大av| 欧美高清成人免费视频www| 9色porny在线观看| 在线精品无人区一区二区三| 免费观看无遮挡的男女| 精品国产一区二区三区久久久樱花| 一本大道久久a久久精品| 永久免费av网站大全| 亚洲精品第二区| 中文欧美无线码| 久久久久久久大尺度免费视频| 欧美bdsm另类| 精品亚洲乱码少妇综合久久| 午夜激情久久久久久久| 亚洲精华国产精华液的使用体验| 日韩成人av中文字幕在线观看| 一级毛片 在线播放| 97在线人人人人妻| 各种免费的搞黄视频| 日韩精品免费视频一区二区三区 | 男人舔奶头视频| 国产亚洲一区二区精品| 99热国产这里只有精品6| av在线app专区| 国产欧美另类精品又又久久亚洲欧美| 国产av一区二区精品久久| 美女xxoo啪啪120秒动态图| www.av在线官网国产| 王馨瑶露胸无遮挡在线观看| 永久免费av网站大全| 亚洲欧美日韩另类电影网站| 少妇人妻一区二区三区视频| 亚洲不卡免费看| 18禁裸乳无遮挡动漫免费视频| 大又大粗又爽又黄少妇毛片口| 丰满乱子伦码专区| 国产成人freesex在线| 一区二区三区免费毛片| 纵有疾风起免费观看全集完整版| 日本黄色片子视频| 国产一区二区在线观看av| 精品久久久噜噜| 免费av中文字幕在线| 国产精品99久久久久久久久| 好男人视频免费观看在线| 三级国产精品欧美在线观看| 麻豆精品久久久久久蜜桃| 一区在线观看完整版| 国产在线一区二区三区精| av又黄又爽大尺度在线免费看| 人妻 亚洲 视频| 亚洲精品久久午夜乱码| 你懂的网址亚洲精品在线观看| 女性被躁到高潮视频| 91午夜精品亚洲一区二区三区| 亚洲av综合色区一区| 国产精品秋霞免费鲁丝片| 黄色欧美视频在线观看| 亚洲av电影在线观看一区二区三区| 亚洲久久久国产精品| videossex国产| 交换朋友夫妻互换小说| 嘟嘟电影网在线观看| www.色视频.com| 欧美97在线视频| 美女xxoo啪啪120秒动态图| 成人亚洲精品一区在线观看| 简卡轻食公司| 3wmmmm亚洲av在线观看| 国产色爽女视频免费观看| 91久久精品国产一区二区三区| 国产欧美亚洲国产| 国产精品嫩草影院av在线观看| 男人舔奶头视频| 狠狠精品人妻久久久久久综合| av免费在线看不卡| 久久人人爽人人片av| av免费观看日本| 又黄又爽又刺激的免费视频.| 欧美国产精品一级二级三级 | 婷婷色综合www| 久久免费观看电影| 欧美成人精品欧美一级黄| 爱豆传媒免费全集在线观看| 熟女av电影| 国产免费视频播放在线视频| 纵有疾风起免费观看全集完整版| 亚洲精品456在线播放app| 丰满人妻一区二区三区视频av| 国产av一区二区精品久久| 日日摸夜夜添夜夜爱| 亚洲欧美精品自产自拍| 久久精品久久久久久久性| 亚洲av.av天堂| av视频免费观看在线观看| 日日摸夜夜添夜夜爱| 久久99一区二区三区| 在线观看www视频免费| 国产欧美日韩综合在线一区二区 | 国产欧美日韩综合在线一区二区 | 亚洲av.av天堂| 少妇被粗大的猛进出69影院 | 搡女人真爽免费视频火全软件| 男女无遮挡免费网站观看| 日本爱情动作片www.在线观看| 插逼视频在线观看| 亚洲人与动物交配视频| 久久精品久久久久久噜噜老黄| 青春草视频在线免费观看| 校园人妻丝袜中文字幕| 亚洲av日韩在线播放| 免费看日本二区| xxx大片免费视频| 国产探花极品一区二区| 婷婷色综合www| 国产黄频视频在线观看| 国产色爽女视频免费观看| 18禁在线播放成人免费| 免费观看av网站的网址| 热re99久久精品国产66热6| 最近最新中文字幕免费大全7| 久久久欧美国产精品| 美女福利国产在线| 天天躁夜夜躁狠狠久久av| 蜜桃久久精品国产亚洲av| 午夜久久久在线观看| 国产在线免费精品| 欧美精品亚洲一区二区| 亚洲欧美成人综合另类久久久| 成人午夜精彩视频在线观看| 一二三四中文在线观看免费高清| 91久久精品电影网| 自线自在国产av| 国国产精品蜜臀av免费| h日本视频在线播放| 97精品久久久久久久久久精品| 日本wwww免费看| 国产精品人妻久久久久久| 亚洲国产最新在线播放| 国产黄频视频在线观看| 国产一区有黄有色的免费视频| 观看美女的网站| 永久网站在线| 嘟嘟电影网在线观看| 2018国产大陆天天弄谢| 看十八女毛片水多多多| 欧美日韩av久久| 日本午夜av视频| 欧美一级a爱片免费观看看| a级毛片免费高清观看在线播放| 欧美日本中文国产一区发布| 国产片特级美女逼逼视频| 又大又黄又爽视频免费| 青春草视频在线免费观看| 国产免费视频播放在线视频| 亚洲一区二区三区欧美精品| 又爽又黄a免费视频| 成人18禁高潮啪啪吃奶动态图 | 免费高清在线观看视频在线观看| 一个人免费看片子| 成人漫画全彩无遮挡| 久久人妻熟女aⅴ| 女的被弄到高潮叫床怎么办| 国产国拍精品亚洲av在线观看| 亚洲国产日韩一区二区| 国产黄色视频一区二区在线观看| 亚洲国产精品专区欧美| 国产精品99久久久久久久久| av女优亚洲男人天堂| 国内揄拍国产精品人妻在线| 国产成人午夜福利电影在线观看| av国产久精品久网站免费入址| 国产极品天堂在线| 国产成人精品一,二区| 欧美日韩视频高清一区二区三区二| 成年美女黄网站色视频大全免费 | 国产一区二区三区综合在线观看 | 99久久精品国产国产毛片| 少妇人妻一区二区三区视频| 秋霞伦理黄片| 成人无遮挡网站| 街头女战士在线观看网站| 美女中出高潮动态图| av卡一久久| 欧美亚洲 丝袜 人妻 在线| 亚洲av成人精品一区久久| 免费观看性生交大片5| 亚洲精品乱码久久久久久按摩| 久久久a久久爽久久v久久| 亚洲欧美日韩卡通动漫| freevideosex欧美| 免费黄频网站在线观看国产| 久久精品久久精品一区二区三区| 男女边摸边吃奶| 国产一区有黄有色的免费视频| 国产成人免费无遮挡视频| 免费高清在线观看视频在线观看| 日本欧美视频一区| 六月丁香七月| 国产精品福利在线免费观看|