• <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 ?

    CdBiO2Br nanosheets in situ strong coupling to carbonized polymer dots and improved photocatalytic activity for organic pollutants degradation

    2023-01-30 06:49:12ZhiyunPngBinWngXingwngYnChongtiWngShengYinHumingLiJiexingXi
    Chinese Chemical Letters 2022年12期

    Zhiyun Png ,Bin Wng ,Xingwng Yn,Chongti Wng ,Sheng Yin,Huming Li ,Jiexing Xi ,*

    a School of Chemistry and Chemical Engineering,Institute for Energy Research,Jiangsu University,Zhenjiang 212013,China

    b School of Chemistry and Chemical Engineering,the Key Laboratory of Electrochemical Energy Storage and Energy Conversion of Hainan Province,Hainan Normal University,Haikou 571158,China

    Keywords:Carbonized polymer dots CdBiO2Br Direct Z-scheme heterojunction Pollutant degradation Photocatalytic activity

    ABSTRACT Carbonized polymer dots(CPDs)modified layer-structured CdBiO2 Br(CPDs/CdBiO2Br)Z-scheme heterojunction hybrid material has been synthesized via simple solvothermal method.The hybrid material with Z-scheme heterojunction can effectively maintain the original highly oxidizing holes of CdBiO2Br and the highly reducing electrons of CPDs.In addition,the construction of heterostructure is beneficial to the migration and separation of photogenerated carriers.Under visible light irradiation,6 wt%CPDs/CdBiO2Br showed the best catalytic activity for degradation of organic pollutants.Free radical capture experiments and ESR analysis confirmed that the main active species are?O2?and h+.The decomposition process of organic pollutants was analyzed by LC-MS.Finally,the probable visible light mechanism performance of CPDs/CdBiO2Br as direct Z-scheme heterojunction photocatalytic materials was proposed.

    Photocatalytic technology has gradually stood out among many catalytic methods[1,2],which can utilize inexhaustible and inexhaustible solar energy and is nontoxic to the environment[3,4].However,the low efficiency of photogenerated carrier migration and separation can lead to the low activity of catalysts,which has become an urgent problem in photocatalytic technology[5,6].Therefore,how to improve the carrier migration and separation efficiency is the current research focus in the field of semiconductor photocatalysis[7,8].

    Layered-structured materials such as bismuth oxybromide(BiOBr)have attracted much attention in the most recent years for brand-new layered material structure in the field of environmental remediation and photocatalytic energy conversion[9,10].BiOBr is characterized by nontoxicity,high stability,good photocatalytic activity and suitable band gap[11,12].While suitable band gap determines its remarkable position in the photocatalysis field,while the covalent metal oxygen layers[Bi2O2]2+are separated by the halide layers along the(001)direction,forming an alternate structure with the double-layer halogen atoms[13,14].However,the higher negative recombination rate of photogenerated electron-hole pair and the lower light absorption capacity still restrict the further development of BiOBr[15,16].A part of Bi in the[Bi2O2]2+layer is replaced by other metal elements to form a covalent bimetallic oxide ion([ABiO2]+,A=Ba,Sr,Ca,Pb,Cd,etc.)layer[17].At this time,halide ion([X]?)layers are modified from double to single,[ABiO2]+and[X]?are arranged alternately,the interlayer gap was greatly reduced,and carrier migration was easier due to the improvement of the passage,which could promote the generation of more reactive oxygen species[18].On this basis,a hybrid cationic mix-layered catalyst,CdBiO2Br,was developed to better promote the migration of photogenerated electron holes.However,after the electrons migrated to the surface of CdBiO2Br,its separation process was not further improved[19,20].

    Carbonized polymer dots(CPDs)have attracted much attention as a new type of carbon nanomaterial[21,22].It has excellent characteristics of particle size less than 10 nm,spherical or quasi spherical morphology,and the surface has abundant polar groups(hydroxyl or carboxyl)[23,24].Notably,CPDs have a unique conjugatedπstructure that can make it outstanding in electron transfer/storage properties and have also been successfully introduced into semiconductors,thus playing an improved role on photocatalytic performance.Combined with the above superiority of CPDs and CdBiO2Br ultrathin material,a novel Z-scheme composite semiconductor photocatalytic system CPDs/CdBiO2Br was successfully constructed,which is greatly desired to gain simple and efficient photocatalytic materials to degrade organic pollutants[25,26].

    Fig.1.(a)XRD pattern and(b)FT-IR of the as-prepared CPDs/CdBiO2 Br samples with different contents of CPDs;(c)TEM and(d)HRTEM images of the 6 wt%CPDs/CdBiO2 Br hybrid materials.

    In this paper,CPDs/CdBiO2Br hybrid materials were prepared by self-sacrificing ionic liquid glue at the first time.More CPDs could be anchored on the surface of CdBiO2Br materialsin situby the existence of Coulombic forces and hydrogen bonding interactions between ionic liquids and CPDs.The existence of intense physical and electronic coupling effects can make the migration and separation of photogenerated carriers at the heterojunction interface greatly improved.Construction of Z-scheme heterojunction,which can form a completely new carrier transport path,significantly inhibits the recombination of photogenerated electron holes and improves the separation efficiency of photogenerated carriers.This work points out a feasible direction for the design and preparation of simpler as well as more efficient photocatalytic materials for visible light degradation of pollutants.

    The phase structures of the as-prepared CPDs/CdBiO2Br composite materials with different quantity of CPDs were analyzed by the characterization of XRD(Fig.1a).All the diffraction peaks were of great consistence with the structure corresponding to the JCPDS No.74–0239.Diffraction peaks located at 2θvalues of 23.6°,31.1°,32.1°,46.0°,52.4°,54.6°,56.5°,68.1°and 76.5°could be assigned to the(101),(103),(200),(211),(116),(213),(220),(310)and(317)crystallographic planes of the CdBiO2Br,respectively.This result indicated the introduction of CPDs with present weight ratios does not have influence on the structure of CdBiO2Br material.Moreover,the signal about the CPDs could not be detected by XRD because the content of CPDs was low in the sample,which might be the good dispersion of CPDs in the CPDs/CdBiO2Br composite materials.Many previous literatures have reported these similar phenomena as well[27,28].

    The possible interactions between CPDs and CdBiO2Br can get further confirmedviaFT-IR analysis.The absorption bands at 554 cm?lmay be due to Bi?O stretching mode,which imply the existence of CdBiO2Br(Fig.1b).The stretching vibrations of C=C at 1548 cm?1and O?H at 1342 cm?lcan be observed for the CPDs/CdBiO2Br hybrid materials.Meanwhile,appearing peaks at 1047 cm?1could be due to C?O,revealing the CPDs/CdBiO2Br hybrid materials possess the existence of CPDs[29].Through the FTIR spectra of the CPDs/CdBiO2Br hybrid,the characteristic peak at 555 cm?1ascribed to Bi?O stretching mode tended to shift slightly higher,indicating the occurrence of interfacial interactions between CPDs and CdBiO2Br.

    To understand the flow direction of electrons and the chemical composition of these samples and the interaction between CPDs and CdBiO2Br,XPS was performed[15,30].Fig.S1a(Supporting information)showed the CdBiO2Br and CPDs/CdBiO2Br samples contained five elements of cadmium,bismuth,oxygen,bromine and carbon in the XPS survey scan spectra.The XPS high-resolution spectra Cd 3d for the CdBiO2Br and CPDs/CdBiO2Br samples are shown in Fig.S1b(Supporting information).The values of 411.9 eV and 405.1 eV in binding energies exist in the form of Cd2+respectively.For the sample of CdBiO2Br,the crystal structures of Bi 4f7/2and Bi 4f5/2of[Bi2O2]2+are corresponding to 159.0 eV and 164.6 eV,respectively.They are at the center of the spin orbit component of the Bi 4f peak as well(Fig.S1c in Supporting information).This suggests the existence of Bi3+in the pure CdBiO2Br and CPDs/CdBiO2Br.Compared to CdBiO2Br sample,the peak of Bi 4f in the CPDs/CdBiO2Br sample moves slightly to the higher binding energy,which indicates that the surface chemical environment of the element Bi in CPDs/CdBiO2Br hybrid has made some changes.The 531.3 eV and 529.9 eV value of oxygen in[Bi2O2]2+at O 1s peaks(Fig.S1d in Supporting information)result from the oxygen in the CdBiO2Br crystal.The slight shift of the O 1s peak in the CPDs/CdBiO2Br also indicates the change of chemical environment by the addition of CPDs.Similarly,it is known that the change of chemical environment also occurs on Br?,as can be intuitively seen from the shift of Br 3d peaks(Fig.S1e in Supporting information)from 69.2 eV and 68.1 eV to 69.9 eV and 68.6 eV,which may be related to the presence of interaction between the CdBiO2Br and CPDs.Fig.S1f(Supporting information)displays the high-resolution XPS spectrum of C 1s,indicating that the main peak of 284.7 eV results from C?C bonds on sp2orbitals.The binding energies of 289.0 eV and 286.5 eV may be the center of the XPS peaks of C 1s,which are also resulted from C=O and C?O?C.XPS analysis results showed that the CPDs/CdBiO2Br hybrid has the existence of both CdBiO2Br and CPDs.The CPDs were modified and intimately integrated on CdBiO2Br successfully as a result.

    Fig.2.(a)UV–vis diffuse reflectance spectra of the as-prepared CPDs/CdBiO2 Br hybrid materials;(b)(αE photon)1/2 vs.E photon curves;(c)photocatalytic degradation of RhB under visible light irradiation;(d)kinetic fit for the degradation of RhB;(e)cycling runs for the photodegradation of RhB;(f)photocatalytic degradation of TC in the presence of pure CdBiO2 Br,CPDs/CdBiO2Br hybrid materials under visible light irradiation.

    To further investigate the microstructure of CdBiO2Br and CPDs/CdBiO2Br hybrid,TEM analysis was carried out.It could be seen that pure CdBiO2Br reveals porous ultrathin nanosheet structure(Fig.S2a in Supporting information),while the difference of crystal morphology is not great after the introduction of CPDs(Fig.S2b in Supporting information).From Fig.1c,numerous dark dots are dispersed on nanosheets,which signifies CPDs have been introduced to CdBiO2Br uniformly.In the HRTEM image(Fig.1d),the lattice fringe spacing of 0.27 nm and 0.21 nm belongs to the(110)crystallographic planes of CdBiO2Br crystallites and the(100)crystal plane of CPDs,respectively[31].The crystallites of CPDs and CdBiO2Br have constituted an excellent combination,and the close mutual contact between the two crystal planes proved that the preparation of CPDs/CdBiO2Br hybrid material was successful.

    The N2adsorption-desorption isotherms determination performed on the obtained hybrid samples can make the specific surface area determined(Fig.S3 in Supporting information).The values of specific surface were 93.90 m2/g for pure CdBiO2Br and 122.47 m2/g for 6 wt%CPDs/CdBiO2Br,respectively.Obviously,with the introduction of CPDs into CdBiO2Br,the value of specific surface area is raised obviously[32].A higher BET specific surface area can get more and more active reactants and species absorbed at their surface,resulting in higher activity of photocatalysis after the improvement.

    The optical and electronic properties of photocatalytic materials are also very important in terms of performance indicators.The optical absorption properties of CPDs/CdBiO2Br hybrid with different CPDs content and pure CdBiO2Br were analyzed through DRS,the results of which are displayed in Fig.2a.The CdBiO2Br underwent an electronic transition from VB to CB under the irradiation of visible light and then displayed the onset of absorption at around 500 nm.Compared with pure CdBiO2Br,the CPDs/CdBiO2Br hybrid exhibited an obvious red shift,and the light harvesting ability in the visible region was enhanced while the content of CPDs increasing.The band gap of CdBiO2Br is calculated to be around 2.32 eV(Fig.2b)by the classical Tauc approach and the XPS valence band spectra for samples are corresponding to 2.13 eV(Fig.S4a in Supporting information).As shown in Fig.S4b(Supporting information),the flat band position of CdBiO2Br material was found to be?0.53 eV by Mott Schottky analysis,while positive slopes revealing CdBiO2Br to be an n-type semiconductor.Therefore,the VB of CdBiO2Br is 1.60 Vvs.NHE.According to the formulaECB=EVB?Eg,the CB of CdBiO2Br is?0.72 Vvs.NHE.Previous studies have revealed that the CB and VB of CPDs were?1.23 and?0.56 Vvs.NHE,respectively,which reveal the energy bands of CPDs and CdBiO2Br are crossed[33,34].

    Rhodamine B(RhB)is an additive of added pigments and the solution is purplish red,which is widely used in the staining of paper and leather.Despite being banned for food staining due to carcinogenesis,the abuse of RhB leads to its ubiquitous presence in surface water bodies and gradually raises environmental pollution problems,and a suitable degradation method is urgently needed to deal with RhB in water bodies.Therefore,the photocatalytic activities of the CPDs/CdBiO2Br and pure CdBiO2Br material were analyzed by degrading the coloured organic pollutant RhB.Fig.2c displays the activities of pure CdBiO2Br and CPDs/CdBiO2Br hybrid with different amount of CPDs contents under the irradiation of visible light.Without catalyst,RhB almost did not undergo degradation and could be neglected,while different contents of CPDs may effectively improve the photocatalytic performance of CdBiO2Br.Results showed that the 6 wt%CPDs/CdBiO2Br hybrid exhibited significantly higher activity than other CPDs containing hybrids and pure CdBiO2Br hybrids.Meanwhile,the kinetics of the photocatalytic degradation of RhB by CPDs/CdBiO2Br hybrids were investigated(Fig.2d).The change concentration of RhB in CPDs/CdBiO2Br hybrid with irradiation time was fitted to the pseudo first order kinetic curve,while introducing CPDs could further improve the photocatalytic degradation rate[35].Compared with pure CdBiO2Br,the kinetic constant of 6 wt%CPDs/CdBiO2Br was raised from 0.017 min?1to 0.041 min?1,which was 2.41 times of pure CdBiO2Br.

    Fig.3.Possible pathways of photocatalytic degradation of(a)RhB and(b)TC by 6 wt%CPDs/CdBiO2 Br.

    Any one simple and effective photocatalyst material,without good reusability and stability,its practical application would be greatly hindered.So,the recycling reaction for photodegradation of RhB on 6 wt%CPDs/CdBiO2Br hybrid was carried out by irradiation of visible light to obtain the evaluation on the stability and reusability of CPDs/CdBiO2Br hybrid.After 4 consecutive cycles,the activity of the photocatalyst decreased by about 6%,implying that the CPDs/CdBiO2Br hybrid could maintain good stability and durability despite passing multiple cycles(Fig.2e).Furthermore,XRD measurements and analysis of 6 wt%CPDs/CdBiO2Br before and after the photocatalytic reaction were performed.Fig.S5(Supporting information).shows that the crystal structure has few changed,which reveal the CPDs/CdBiO2Br hybrid material is stable during the photodegradation process.

    Tetracycline(TC)is a broad-spectrum antibiotic widely used for its remarkable bactericidal effect.However,the abuse of TC leads to the rising levels in water bodies and gradually evolves into an urgent environmental pollution problem.Therefore,the degradation and removal of TC are very important.Therefore,we performed visible light degradation of TC by photocatalytic materials while examining the photocatalytic activity of photocatalysts.The activity of the prepared CPDs/CdBiO2Br hybrid has been further appraised by catalytic degradation of antibiotic TC under visible light(Fig.2f)[36].It is shown that the 6 wt%CPDs/CdBiO2Br hybrid exhibited much higher than pure CdBiO2Br for TC photodegradation in photocatalytic activity.The degradation reached equilibrium after 60 min,at which point the photocatalytic degradation efficiency of CPDs/CdBiO2Br improved over 10%compared to pure CdBiO2Br.The introduction of CPDs was effective to make the improvement of photocatalytic efficiency possible indicated by the results.

    To further investigate the degradation courses of RhB and TC in photocatalysis,an in-depth analysis of possible intermediates was carried out using an LC-MS method.The characteristic MS signals of above intermediates are shown in Fig.S6(Supporting information).For the degradation of RhB,Fig.3a presents the possible course of RhB degradation by 6 wt%CPDs/CdBiO2Br.The most initial RhB(P1,m/z445)loses two ethyl groups first to produce intermediate material P2 with a molecular weight of 387.In the subsequent degradation course,the above intermediate material again generates the intermediate product P3 with a molecular weight of 301 by losing one carboxyl group,one methylene group,as well as one ethyl group.Immediately afterwards,P3 undergoes carboxylation and generates P4 by losing the phenyl ring and one methyl group(m/z268).P4 then undergoes oxidation,denitrification,and ring opening reactions to produce the dihydroxybenzoic or glutaric acid predominant carboxylic acids P5(m/z153)and P6(m/z132)and stepwise to smaller molecule carboxylic acids such as butyric,propionic,and acetic acids.Finally,by mineralization,CO2and water molecules are obtained[37].

    Likewise,the characteristic MS signals of corresponding intermediates(Fig.S7 in Supporting information)as well as the potential pathway of TC degradation by 6 wt%CPDs/CdBiO2Br(Fig.3b)were given.TC has a molecular weight of 445(M1),and the product M2(m/z431)could be generated by losing oneN-methyl group.Upon the creation of a cavity,M2 underwent further dealkylation dehydration to produce intermediate M3(m/z396),which subsequently underwent sequential generation of M4,M5,and M6viacarboxyl group removal,N-methyl group removal,and ring opening and oxidation reactions.Due to the action of h+,subsequently,M6 undergoes an elimination reaction and then generates M7(m/z230)after removing the keto group and one methyl group.Continued through ring opening reaction to generate M8,M9,and further gave some small molecular species.In summary,under the action of active species,TC molecules undergo ring opening reactions and cleavage of functional groups(N-methyl,hydroxyl or amino)to finally degrade into carbon dioxide and water molecules to achieve efficient degradation under photocatalysis[38,39].

    Fig.4.(a)EIS;(b)transient photocurrent response and(c)PL spectra of the as-prepared CPDs/CdBiO2Br hybrid materials and pure CdBiO2Br;(d)trapping experiment of active species during the photocatalytic degradation of RhB over CPDs/CdBiO2 Br hybrid material under visible light irradiation.

    Electrochemical impedance spectroscopy(EIS)studies were put into effect on 6 wt%CPDs/CdBiO2Br and pure CdBiO2Br material samples for further investigation of the interfacial charge transfer resistance.The results exhibited that the arc radius on the EIS Nyquist curve of the 6 wt%CPDs/CdBiO2Br hybrid material sample was not as big as that of the pure CdBiO2Br.The smaller the radius of the Nyquist circle is,the smaller the charge transfer resistance could become(Fig.4a).The unique conjugatedπstructure of CPDs can be used as an effective transporter to accelerate the charge transfer at the interface and reduce the resistance[39].This can allow the electron hole pairs to separate effectively,reaching the enhancement of photocatalytic efficiency finally.

    Photocurrent curves of 6 wt% CPDs/CdBiO2Br and pure CdBiO2Br material electrodes are presented in Fig.4b.When the illumination is activated,the response of photocurrent increases sharply,and it can maintain stable and reproducible performance within intermittent on-off irradiation for several cycles.CPDs is an excellent electron acceptor material with a unique conjugated structure,which can be an important condition for photoexcited carrier separation center.By taking advantage of the excellent conversion performance of CPDs,the electronic transitions of CdBiO2Br materials can be excited,which significantly promotes the efficient separation of photogenerated carriers of the composites.Compared to pure CdBiO2Br,the CPDs/CdBiO2Br hybrid material exhibits a higher light absorption and photocurrent response the irradiation of visible light,while the photoexcited electron and hole separation rates are also relatively fast[40].

    The charge migration,transfer and recombination processes of photocatalysts are the key links and can be studied by determining the photoluminescence(PL)spectra during chemical reactions[41].The probability of recombination of photoexcited charge carriers decreases with decreasing intensity.The PL spectra of 6 wt%CPDs/CdBiO2Br and pure CdBiO2Br material are presented in Fig.4c,indicating an emission peak of about 464 nm.The intensity of the emission band of CPDs/CdBiO2Br decreased significantly compared to that of CdBiO2Br,implying that photoexcited electrons were effectively transferred from CdBiO2Br to CPDs when CPDs was anchored evenly onto the surface of CPDs/CdBiO2Br.Consequently,introducing CPDs can effectively reduce the electron hole recombination rate of CdBiO2Br,and thus effectively promote the charge separation of CdBiO2Br to achieve the purpose of improving the photocatalytic activity of CdBiO2Br.

    To further reveal the roles of the active species on the photocatalysis process over CPDs/CdBiO2Br materials,radical trapping experiments were performed with different scavengers(nitrogen(N2)for?O2?,ammonium oxalate(AO)for holes,andtert–butanol alcohol(TBA)for?OH).As shown in Fig.4d,when AO and N2were added,the degradation efficiency was greatly inhibited,indicating that holes and?O2?were the main active components in the process of photocatalysis[42].However,when TBA was added,the effect on photodegradation efficiency was hardly obvious,indicating no?OH production[43].

    The mechanism of CPDs/CdBiO2Br and the active species generated during photodegradation under visible light irradiation can be further validated by ESR analysis.This analysis employs 5,5-dimethyl-1-pyrrolineN-oxide(DMPO)adsorbed on the photocatalyst or dissolved in methanol/water as a spin trap,allowing the detection of the spin reactivity?OH and?O2?.The strong ESR spectra corresponding to DMPO-?O2?adduct for both CPDs/CdBiO2Br and pure CdBiO2Br can be clearly observed(Fig.5a)[44].In addition,the ESR spectra intensity of DMPO-?O2?adduct for CPDs/CdBiO2Br hybrid is significantly higher than pure CdBiO2Br,indicating that more electrons are involved in the reaction of reducing O2to generate?O2?.The electron localized conjugation structure of CPDs makes the transfer of photogenerated electrons easier,thus achieving efficient separation of electron hole pair.While the DMPO-?O2?was obvious,the DMPO–hydroxyl radical(?OH)species were not detected.This is due to the VB potential of both OH?/?OH(2.34 Vvs.NHE)and H2O/?OH(1.99 Vvs.NHE)are more positive than those of CdBiO2Br and CPDs,thus no?OH production in terms of thermodynamics(Fig.5b)[45].

    We proposed the hypothesis that the as prepared CPDs/CdBiO2Br were conventional dual transfer structures,as shown in Fig.5c.Then the electrons were excited from the CB of CPDs,transferred to the CB of CdBiO2Br.However,the CB of CdBiO2Br is only 0.16 eV difference from the VB of CPDs,which would greatly increase the recombination rate of electrons on the CB of CdBiO2Br and holes on the VB of CPDs,greatly hindering the migration and separation of carriers.So,the holes in the VB of CPDs should combine with the electrons in the CB of CdBiO2Br,which can effectively separate the electrons and holes and generate more active species,therefore,CPDs/CdBi O2Br is more likely to be a direct Z-scheme heterojunction structure(Fig.5d).

    Fig.5.(a,b)ESR spectra of radical adducts trapped by DMPO in CPDs/CdBiO2Br hybrid materials aqueous dispersion under visible light irradiation.Energy band diagram of(c)traditional photocatalytic system and(d)direct Z-scheme photocatalytic system for the CPDs/CdBiO2 Br composite material.

    In summary,a direct Z-scheme heterojunction photocatalytic material has been designed.A novel CPDs/CdBiO2Br photocatalytic material has been successfully constructed by introducing CPDs into the surface of CdBiO2Brviaa simple solvothermal method,and the photocatalytic degradation activity of CdBiO2Br toward TC and RhB under the irradiation of visible light was improved by introducing CPDs for modification.Contrasting different mass fractions revealed that the 6 wt%CPDs/CdBiO2Br hybrid showed the best performance of photocatalysis.Moreover,the excellent stability and reusability of the CPDs/CdBiO2Br hybrid material play a vital role in the application of environmental protection.?O2?,and h+are the main active species in the process of photocatalysis.In summary,the efficiency of charge separation can be improved effectively by the introduction of CPDs and thus significantly improve the activity of photocatalysis at last.Various works in this thesis can also play important enlightening and guiding roles for the development and research of CPDs based photocatalytic hybrid material.

    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 the National Natural Science Foundation of China(No.22108106,21676128),China Postdoctoral Science Foundation(No.2020M680065),Hong Kong Scholar Program (No.XJ2021021),Key Laboratory of Electrochemical Energy Storage and Energy Conversion of Hainan Province(No.KFKT2021005).

    Supplementary materials

    Supplementary material associated with this article can be found,in the online version,at doi:10.1016/j.cclet.2022.01.054.

    欧美bdsm另类| 午夜福利在线观看免费完整高清在 | 国产黄a三级三级三级人| 大又大粗又爽又黄少妇毛片口| 一个人观看的视频www高清免费观看| 精品人妻偷拍中文字幕| 国产又黄又爽又无遮挡在线| 欧美成人一区二区免费高清观看| 午夜福利18| 午夜日韩欧美国产| 麻豆精品久久久久久蜜桃| 他把我摸到了高潮在线观看| 在线a可以看的网站| 国产欧美日韩一区二区精品| av.在线天堂| 亚洲aⅴ乱码一区二区在线播放| 天堂av国产一区二区熟女人妻| 免费不卡的大黄色大毛片视频在线观看 | 国产一区二区三区视频了| 亚洲最大成人手机在线| 人妻制服诱惑在线中文字幕| 一区二区三区四区激情视频 | 国模一区二区三区四区视频| 亚洲精品日韩av片在线观看| 99热网站在线观看| 亚洲va日本ⅴa欧美va伊人久久| 国产日本99.免费观看| 亚洲精品影视一区二区三区av| 黄片wwwwww| 在线观看66精品国产| 久久久久久久久久久丰满 | 啪啪无遮挡十八禁网站| a级一级毛片免费在线观看| 日本一二三区视频观看| 男女边吃奶边做爰视频| 91午夜精品亚洲一区二区三区 | 日本精品一区二区三区蜜桃| 日韩一本色道免费dvd| 亚洲精华国产精华液的使用体验 | 欧美+亚洲+日韩+国产| 国产精品1区2区在线观看.| 国内精品久久久久精免费| 女的被弄到高潮叫床怎么办 | 成人永久免费在线观看视频| 欧美成人免费av一区二区三区| 欧美成人一区二区免费高清观看| 久久精品综合一区二区三区| 久久精品久久久久久噜噜老黄 | 国产毛片a区久久久久| 又黄又爽又刺激的免费视频.| 一本一本综合久久| 亚洲国产欧洲综合997久久,| 国产精品无大码| 国内少妇人妻偷人精品xxx网站| 内射极品少妇av片p| 免费人成在线观看视频色| 老司机午夜福利在线观看视频| 精品一区二区三区视频在线| 听说在线观看完整版免费高清| 欧美又色又爽又黄视频| 免费在线观看影片大全网站| 欧美日韩国产亚洲二区| 欧美潮喷喷水| 欧洲精品卡2卡3卡4卡5卡区| 熟女人妻精品中文字幕| 成人无遮挡网站| 噜噜噜噜噜久久久久久91| 美女大奶头视频| 老熟妇仑乱视频hdxx| 老熟妇乱子伦视频在线观看| 中文字幕免费在线视频6| 免费高清视频大片| av在线亚洲专区| 精品无人区乱码1区二区| 97人妻精品一区二区三区麻豆| 18+在线观看网站| 亚洲国产色片| 91久久精品国产一区二区成人| 国产精品日韩av在线免费观看| 神马国产精品三级电影在线观看| 人妻丰满熟妇av一区二区三区| 精品人妻熟女av久视频| 成年女人永久免费观看视频| 国产毛片a区久久久久| 欧美极品一区二区三区四区| 色精品久久人妻99蜜桃| 99久久精品热视频| 黄色日韩在线| 国产aⅴ精品一区二区三区波| 男人的好看免费观看在线视频| 精品乱码久久久久久99久播| 五月玫瑰六月丁香| 国产黄a三级三级三级人| 床上黄色一级片| 久久久久久久午夜电影| 亚洲国产欧美人成| 亚洲18禁久久av| 天堂√8在线中文| 亚洲精品粉嫩美女一区| 国产精品日韩av在线免费观看| 国产欧美日韩精品亚洲av| 国产精品国产三级国产av玫瑰| 精品一区二区免费观看| 亚洲欧美日韩无卡精品| 少妇人妻一区二区三区视频| 久久久成人免费电影| 久久精品夜夜夜夜夜久久蜜豆| 美女免费视频网站| 老熟妇仑乱视频hdxx| 国产精品一区二区性色av| 日本成人三级电影网站| 在线a可以看的网站| 波野结衣二区三区在线| 国语自产精品视频在线第100页| 欧美日韩瑟瑟在线播放| 在线观看舔阴道视频| 免费一级毛片在线播放高清视频| 大又大粗又爽又黄少妇毛片口| 啦啦啦观看免费观看视频高清| 日韩大尺度精品在线看网址| 天堂网av新在线| 国产综合懂色| 男女那种视频在线观看| 亚洲国产精品久久男人天堂| 国产精品久久电影中文字幕| 精品日产1卡2卡| 国产日本99.免费观看| 国产欧美日韩一区二区精品| 午夜精品在线福利| 久久午夜福利片| 99久久精品国产国产毛片| 一本久久中文字幕| 国内精品宾馆在线| 少妇猛男粗大的猛烈进出视频 | 最好的美女福利视频网| 日本免费一区二区三区高清不卡| 成人特级黄色片久久久久久久| 国产白丝娇喘喷水9色精品| 日韩在线高清观看一区二区三区 | 免费无遮挡裸体视频| 国产精品不卡视频一区二区| 又黄又爽又刺激的免费视频.| 精品人妻一区二区三区麻豆 | 亚洲内射少妇av| 波多野结衣高清作品| 亚洲五月天丁香| 丝袜美腿在线中文| 最近最新免费中文字幕在线| 国产精品久久久久久av不卡| 男插女下体视频免费在线播放| 午夜福利在线观看吧| 色播亚洲综合网| 夜夜爽天天搞| 亚洲精品久久国产高清桃花| 欧美成人性av电影在线观看| 午夜福利在线观看吧| 亚洲,欧美,日韩| 日韩欧美在线乱码| 国产亚洲精品av在线| 午夜日韩欧美国产| 国产午夜精品论理片| 伊人久久精品亚洲午夜| 日韩欧美在线乱码| 国产精品一区二区三区四区免费观看 | netflix在线观看网站| 99精品在免费线老司机午夜| 免费观看精品视频网站| 波多野结衣巨乳人妻| 亚洲最大成人中文| 日韩精品中文字幕看吧| 国产毛片a区久久久久| 国产精品一区二区三区四区免费观看 | 高清毛片免费观看视频网站| 久久国内精品自在自线图片| 男人和女人高潮做爰伦理| 麻豆成人午夜福利视频| 一级黄片播放器| 久久精品国产亚洲网站| 亚洲人成伊人成综合网2020| 午夜爱爱视频在线播放| 成年女人毛片免费观看观看9| 欧美国产日韩亚洲一区| 国产av麻豆久久久久久久| 亚洲中文日韩欧美视频| 国产老妇女一区| 精品久久久久久,| 久久久久久久久久黄片| 国产一区二区激情短视频| 亚洲av第一区精品v没综合| 国产亚洲精品久久久com| aaaaa片日本免费| 精品人妻一区二区三区麻豆 | 国产精品一区www在线观看 | 日本五十路高清| 日日撸夜夜添| 99九九线精品视频在线观看视频| 性色avwww在线观看| 久久精品国产亚洲网站| 老司机福利观看| 久久久久久久亚洲中文字幕| 精品久久久噜噜| 波多野结衣巨乳人妻| 欧美精品啪啪一区二区三区| 1000部很黄的大片| 97人妻精品一区二区三区麻豆| 国产伦精品一区二区三区视频9| 免费高清视频大片| 岛国在线免费视频观看| 麻豆国产av国片精品| 亚洲成a人片在线一区二区| 亚洲天堂国产精品一区在线| 欧美最黄视频在线播放免费| 日日摸夜夜添夜夜添av毛片 | 美女xxoo啪啪120秒动态图| 一区二区三区免费毛片| 欧美极品一区二区三区四区| 内地一区二区视频在线| 真实男女啪啪啪动态图| 韩国av一区二区三区四区| 免费看光身美女| 熟女电影av网| 91久久精品电影网| 国产精品无大码| 国产主播在线观看一区二区| 亚洲国产欧洲综合997久久,| 欧美性猛交黑人性爽| 一区二区三区四区激情视频 | 少妇熟女aⅴ在线视频| 亚洲国产高清在线一区二区三| 亚洲精品在线观看二区| 午夜a级毛片| 亚洲熟妇熟女久久| 日本欧美国产在线视频| 久久精品人妻少妇| 免费电影在线观看免费观看| 毛片一级片免费看久久久久 | 九九在线视频观看精品| 在线观看一区二区三区| 日韩欧美精品免费久久| 欧洲精品卡2卡3卡4卡5卡区| 国产老妇女一区| 国产主播在线观看一区二区| 俺也久久电影网| 午夜福利成人在线免费观看| 十八禁国产超污无遮挡网站| 熟妇人妻久久中文字幕3abv| 在线观看一区二区三区| 国产精品三级大全| 久久久久九九精品影院| 老女人水多毛片| 精品福利观看| 亚洲精品在线观看二区| 亚州av有码| 一个人观看的视频www高清免费观看| 一进一出抽搐动态| 又爽又黄a免费视频| 国产成人一区二区在线| 身体一侧抽搐| 搡女人真爽免费视频火全软件 | 亚洲专区国产一区二区| 国产乱人视频| 色综合亚洲欧美另类图片| 亚洲狠狠婷婷综合久久图片| 精品人妻熟女av久视频| 国产在视频线在精品| 99久久九九国产精品国产免费| 成人特级黄色片久久久久久久| 国产精品福利在线免费观看| 丰满的人妻完整版| 国产精品爽爽va在线观看网站| 男女视频在线观看网站免费| av女优亚洲男人天堂| 国产精品伦人一区二区| 窝窝影院91人妻| 日韩精品青青久久久久久| 欧美性猛交╳xxx乱大交人| 亚洲一区高清亚洲精品| 尾随美女入室| 欧美日本亚洲视频在线播放| 69av精品久久久久久| 亚洲图色成人| 永久网站在线| 欧美性猛交黑人性爽| 国产成人av教育| 国产在线精品亚洲第一网站| 欧美日韩瑟瑟在线播放| 午夜a级毛片| 欧美成人性av电影在线观看| 亚洲av电影不卡..在线观看| 免费av观看视频| 久久热精品热| 丰满乱子伦码专区| 性欧美人与动物交配| 老司机深夜福利视频在线观看| 国产av在哪里看| 国产国拍精品亚洲av在线观看| 别揉我奶头~嗯~啊~动态视频| 午夜日韩欧美国产| 欧美又色又爽又黄视频| 国产av不卡久久| 男人的好看免费观看在线视频| 很黄的视频免费| 中国美白少妇内射xxxbb| 国产男靠女视频免费网站| 国产精品女同一区二区软件 | 看免费成人av毛片| 亚洲乱码一区二区免费版| 亚洲熟妇熟女久久| 亚洲av免费高清在线观看| 国产精品一区二区免费欧美| 夜夜看夜夜爽夜夜摸| 一a级毛片在线观看| 久久久精品欧美日韩精品| 日韩欧美精品免费久久| av在线老鸭窝| 日本黄大片高清| 男女下面进入的视频免费午夜| 搡老妇女老女人老熟妇| 干丝袜人妻中文字幕| 午夜视频国产福利| 悠悠久久av| 91久久精品国产一区二区三区| 亚洲人成伊人成综合网2020| 在线国产一区二区在线| 老熟妇仑乱视频hdxx| 亚洲国产欧洲综合997久久,| 男人和女人高潮做爰伦理| 人人妻人人看人人澡| 91av网一区二区| 给我免费播放毛片高清在线观看| 波多野结衣巨乳人妻| 午夜福利18| 岛国在线免费视频观看| 久久精品国产鲁丝片午夜精品 | 免费电影在线观看免费观看| 国内精品久久久久久久电影| 亚洲最大成人中文| 黄色女人牲交| 久久久久九九精品影院| 九色国产91popny在线| 亚洲色图av天堂| 精品久久久久久久久亚洲 | 伊人久久精品亚洲午夜| 国产高潮美女av| 久久久久久久久大av| 国产真实乱freesex| 淫妇啪啪啪对白视频| 中文亚洲av片在线观看爽| 国产精品,欧美在线| 中国美女看黄片| 色尼玛亚洲综合影院| 少妇高潮的动态图| 亚洲成人中文字幕在线播放| 免费看美女性在线毛片视频| 美女 人体艺术 gogo| 国产淫片久久久久久久久| 蜜桃亚洲精品一区二区三区| 亚洲成av人片在线播放无| 男女啪啪激烈高潮av片| 欧美精品国产亚洲| 99在线视频只有这里精品首页| 99精品在免费线老司机午夜| 我的老师免费观看完整版| 丰满人妻一区二区三区视频av| 免费人成视频x8x8入口观看| 成人亚洲精品av一区二区| 一个人看视频在线观看www免费| 国产精品福利在线免费观看| 国产一区二区亚洲精品在线观看| 国产人妻一区二区三区在| 99热精品在线国产| 亚洲第一区二区三区不卡| 日本精品一区二区三区蜜桃| 禁无遮挡网站| 99热精品在线国产| 国产女主播在线喷水免费视频网站 | 欧美bdsm另类| 岛国在线免费视频观看| 久久久国产成人精品二区| 亚洲成av人片在线播放无| 午夜福利在线在线| 欧美性猛交黑人性爽| bbb黄色大片| 少妇的逼水好多| 精品人妻偷拍中文字幕| 床上黄色一级片| 久久久久性生活片| 网址你懂的国产日韩在线| 国产91精品成人一区二区三区| 国产精品女同一区二区软件 | 全区人妻精品视频| 久久久成人免费电影| 久久久久国内视频| 国产av一区在线观看免费| 国产精品98久久久久久宅男小说| 久久人人精品亚洲av| 少妇裸体淫交视频免费看高清| 美女高潮的动态| 亚洲性久久影院| 午夜免费成人在线视频| 免费看美女性在线毛片视频| 色视频www国产| 久久久久免费精品人妻一区二区| 人人妻人人澡欧美一区二区| 欧美一区二区亚洲| 又爽又黄无遮挡网站| 国产成人一区二区在线| 国产一区二区三区av在线 | 欧美最黄视频在线播放免费| 欧美又色又爽又黄视频| 国产精品自产拍在线观看55亚洲| 精品无人区乱码1区二区| 人人妻人人看人人澡| 99国产极品粉嫩在线观看| 免费大片18禁| 人妻久久中文字幕网| 看十八女毛片水多多多| 国产精品av视频在线免费观看| 久久天躁狠狠躁夜夜2o2o| 欧美高清性xxxxhd video| 小说图片视频综合网站| 五月玫瑰六月丁香| 国产精品美女特级片免费视频播放器| 免费一级毛片在线播放高清视频| 97碰自拍视频| 俄罗斯特黄特色一大片| 午夜福利成人在线免费观看| 欧美日韩综合久久久久久 | 免费看美女性在线毛片视频| 国产精品伦人一区二区| 在线观看66精品国产| 欧美精品国产亚洲| bbb黄色大片| 国产探花极品一区二区| 国产伦精品一区二区三区视频9| 日本欧美国产在线视频| 色综合婷婷激情| 精品人妻视频免费看| 男女视频在线观看网站免费| 网址你懂的国产日韩在线| 一级a爱片免费观看的视频| 嫩草影院新地址| 别揉我奶头 嗯啊视频| 精品一区二区三区视频在线观看免费| 国产亚洲91精品色在线| 韩国av在线不卡| 欧美日韩瑟瑟在线播放| 日日撸夜夜添| 99精品久久久久人妻精品| 午夜日韩欧美国产| 亚洲成人中文字幕在线播放| 99riav亚洲国产免费| 成人一区二区视频在线观看| 欧美+亚洲+日韩+国产| 一夜夜www| 乱码一卡2卡4卡精品| 日本免费一区二区三区高清不卡| 偷拍熟女少妇极品色| 亚洲不卡免费看| 日韩欧美 国产精品| 女生性感内裤真人,穿戴方法视频| 最新在线观看一区二区三区| 网址你懂的国产日韩在线| 国产精品一区二区三区四区久久| 国产精品美女特级片免费视频播放器| 老司机深夜福利视频在线观看| 免费电影在线观看免费观看| 老司机午夜福利在线观看视频| 国产精品久久久久久亚洲av鲁大| a级毛片a级免费在线| 国产成人aa在线观看| 中文亚洲av片在线观看爽| 亚洲av熟女| 日韩欧美在线乱码| 国产精品国产三级国产av玫瑰| 麻豆av噜噜一区二区三区| 久久香蕉精品热| 偷拍熟女少妇极品色| 精品一区二区三区av网在线观看| 精品久久久久久,| 99在线视频只有这里精品首页| 日韩精品中文字幕看吧| 国产精品日韩av在线免费观看| 亚洲不卡免费看| 日本免费一区二区三区高清不卡| 一个人观看的视频www高清免费观看| 成人一区二区视频在线观看| 一a级毛片在线观看| 麻豆成人午夜福利视频| 欧美日韩瑟瑟在线播放| 国产亚洲91精品色在线| 成熟少妇高潮喷水视频| 亚洲国产高清在线一区二区三| 超碰av人人做人人爽久久| 成人综合一区亚洲| av国产免费在线观看| 成人性生交大片免费视频hd| 国产极品精品免费视频能看的| 69人妻影院| 大又大粗又爽又黄少妇毛片口| 国产一区二区在线观看日韩| 日韩 亚洲 欧美在线| 一个人看的www免费观看视频| 麻豆国产97在线/欧美| 亚洲国产精品久久男人天堂| 亚洲 国产 在线| 禁无遮挡网站| 搞女人的毛片| a级毛片免费高清观看在线播放| 高清在线国产一区| 午夜影院日韩av| 国产亚洲av嫩草精品影院| 国产精品99久久久久久久久| 国产亚洲91精品色在线| 99热这里只有精品一区| 国产一区二区三区av在线 | 日日摸夜夜添夜夜添av毛片 | 国产单亲对白刺激| 亚洲一区二区三区色噜噜| 久久6这里有精品| 小蜜桃在线观看免费完整版高清| 国产主播在线观看一区二区| 国内精品久久久久久久电影| 九九在线视频观看精品| 国内毛片毛片毛片毛片毛片| 国产大屁股一区二区在线视频| 自拍偷自拍亚洲精品老妇| 真人一进一出gif抽搐免费| 日韩精品中文字幕看吧| 18禁在线播放成人免费| 国内精品久久久久精免费| eeuss影院久久| 午夜激情福利司机影院| 九九在线视频观看精品| 免费观看人在逋| 赤兔流量卡办理| 国产精品,欧美在线| 99久久成人亚洲精品观看| 国产 一区精品| 一进一出抽搐动态| 精品不卡国产一区二区三区| 欧美日韩乱码在线| 国产精品电影一区二区三区| 九九久久精品国产亚洲av麻豆| 日韩 亚洲 欧美在线| 欧美区成人在线视频| 最近中文字幕高清免费大全6 | 中文字幕免费在线视频6| 麻豆久久精品国产亚洲av| 欧美成人a在线观看| 一个人看视频在线观看www免费| 18禁在线播放成人免费| 人人妻人人看人人澡| 亚洲精品国产成人久久av| 国产伦在线观看视频一区| 亚洲av熟女| 国产精品亚洲一级av第二区| 在现免费观看毛片| 一进一出抽搐gif免费好疼| 中文字幕精品亚洲无线码一区| 亚洲自拍偷在线| 精品久久久久久成人av| 日日撸夜夜添| 级片在线观看| 国产主播在线观看一区二区| 国产av一区在线观看免费| 免费av毛片视频| 男女那种视频在线观看| 天堂√8在线中文| 中文字幕高清在线视频| 免费观看人在逋| 国产精品亚洲美女久久久| 男女边吃奶边做爰视频| 亚洲欧美日韩高清在线视频| 99在线人妻在线中文字幕| 国产激情偷乱视频一区二区| 淫秽高清视频在线观看| 又黄又爽又刺激的免费视频.| 热99在线观看视频| 如何舔出高潮| 97人妻精品一区二区三区麻豆| 18禁黄网站禁片午夜丰满| 国产免费一级a男人的天堂| 男插女下体视频免费在线播放| 在线观看免费视频日本深夜| 91久久精品国产一区二区成人| 伦精品一区二区三区| 成人特级av手机在线观看| 成人美女网站在线观看视频| 香蕉av资源在线| 亚洲国产精品久久男人天堂| 日韩中字成人| 色视频www国产| 国产av在哪里看| 久99久视频精品免费| 三级国产精品欧美在线观看| 男人的好看免费观看在线视频| 日本成人三级电影网站| 最近最新免费中文字幕在线| 在线观看66精品国产| 亚洲精品久久国产高清桃花| av福利片在线观看| 午夜福利在线观看吧| 国产视频一区二区在线看| videossex国产| 国产精品98久久久久久宅男小说| 欧美成人a在线观看| 一个人看的www免费观看视频| 亚洲黑人精品在线| 亚洲专区国产一区二区| 亚洲五月天丁香| 九九在线视频观看精品| 最近最新免费中文字幕在线| 亚洲经典国产精华液单| 亚洲精品影视一区二区三区av|