Ag3PO4微纳米材料的制备及光催化性能研究

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磷酸银光催化剂的制备及应用研究进展

磷酸银光催化剂的制备及应用研究进展

磷酸银光催化剂的制备及应用研究进展汤春妮【摘要】Silver phosphate (Ag3PO4) photocatalyst receives great attention because of its high photocatalytic activity.In this paper,we summarized the achieved results and development of silver phosphate photocatalyst at home and abroad from the perspective of materials preparation and application of photocatalysis fields.This paper provided a significant guidance for the development and application of silver orthophosphate photocatalyst.%可见光催化剂磷酸银因具有极高的光催化活性而受到密切关注.本文从材料制备及其光催化领域应用的角度,梳理总结了国内外在此相研究中取得的一些成果及进展,以其对磷酸银光催化剂的开发和应用研究提供参考.【期刊名称】《化学工程师》【年(卷),期】2018(000)003【总页数】5页(P41-45)【关键词】磷酸银;光催化剂;制备;应用【作者】汤春妮【作者单位】陕西国防工业职业技术学院化学工程学院,陕西西安 710300【正文语种】中文【中图分类】TQ032;O482.3光催化技术是一种在常温常压下借助光催化剂直接利用太阳能驱动的催化反应技术,具有反应条件温和、节能环保、反应活性高等优点,因此,受到材料、化学、环境等领域研究者的广泛关注。

光催化技术的核心是光催化材料的开发和应用。

理想的光催化材料应该具有光响应范围宽、载流子分离效率高、光催化活性高、稳定性好、回收利用便捷等特点。

Ag_Ag3PO4_g-C3N4复合光催化剂的合成与再生及其可见光下的光催化性能

Ag_Ag3PO4_g-C3N4复合光催化剂的合成与再生及其可见光下的光催化性能

[Article]物理化学学报(Wuli Huaxue Xuebao )Acta Phys.-Chim.Sin .2014,30(4),729-737April Received:December 9,2013;Revised:February 24,2014;Published on Web:February 24,2014.∗Corresponding author.Email:wyfwyf53540708@;Tel:+86-139********.The project was supported by the National Natural Science Foundation of China (21206105,21176168).国家自然科学基金(21206105,21176168)资助项目©Editorial office of Acta Physico -Chimica Sinicadoi:10.3866/PKU.WHXB 201402243Ag/Ag 3PO 4/g-C 3N 4复合光催化剂的合成与再生及其可见光下的光催化性能刘建新王韵芳*王雅文樊彩梅(太原理工大学洁净化工研究所,太原030024)摘要:研究了用离子交换沉淀法制备的Ag/Ag 3PO 4/g-C 3N 4的可见光光催化性能及再生方法.通过X 射线衍射(XRD)、场发射扫描电子显微镜(FESEM)、紫外-可见(UV-Vis)吸收光谱及X 射线光电子能谱(XPS)对其进行了结构特性分析.XRD 结果显示再生后催化剂的结构未发生改变.FESEM 及UV-Vis 分析结果说明催化剂由Ag 3PO 4与g-C 3N 4复合而成.XPS 分析结果表明催化剂表面出现少量的银单质.利用可见光(λ>420nm)照射下的苯酚降解实验评价了样品的光催化活性,并通过活性物种及能带结构的分析对催化剂的光催化机理进行了推测.研究表明,Ag/Ag 3PO 4/g-C 3N 4的光催化活性明显高于纯Ag 3PO 4及纯g-C 3N 4,主要原因归结为单质银、Ag 3PO 4及g-C 3N 4的协同效应.经过氧化氢和磷酸氢铵钠(NaNH 4HPO 4)的再生可完全恢复催化剂的活性,这表明该绿色环保的再生方法可实现Ag/Ag 3PO 4/g-C 3N 4催化剂在环境中的实际应用.关键词:磷酸银;g-C 3N 4;金属银;催化剂再生;苯酚;光催化中图分类号:O644;O649Synthesis,Regeneration and Photocatalytic Activity under Visible-LightIrradiation of Ag/Ag 3PO 4/g-C 3N 4Hybrid PhotocatalystsLIU Jian-XinWANG Yun-Fang *WANG Ya-WenFAN Cai-Mei(Institute of Clean Technique for Chemical Engineering,Taiyuan University of Technology,Taiyuan 030024,P .R.China )Abstract:Ag/Ag 3PO 4/g-C 3N 4(g denotes graphitic)was synthesized via an anion-exchange precipitation method,and its photocatalytic activity under visible light and regeneration with H 2O 2and NaNH 4HPO 4were investigated.The structural characteristics were analyzed using X-ray diffraction (XRD),field-emission scanning electron microscopy (FESEM),ultraviolet-visible (UV-Vis)absorption spectroscopy,and X-ray photoelectron spectroscopy (XPS).The XRD results showed that the structure of the regenerated catalyst was unchanged.The FESEM and UV-Vis absorption spectroscopy results showed that the Ag/Ag 3PO 4/g-C 3N 4catalyst was composed of Ag 3PO 4and g-C 3N 4.XPS showed that a small amount of Ag particles were present on the catalyst surface.The photocatalytic activity was evaluated using phenol degradation under visible light (λ>420nm)and the photocatalytic mechanism was discussed based on the active species during the photocatalytic process and the band structure.Experimental studies showed that the photocatalytic activity of the as-prepared Ag/Ag 3PO 4/g-C 3N 4was higher than those of pure Ag 3PO 4and g-C 3N 4.The high photocatalytic performance of the Ag/Ag 3PO 4/g-C 3N 4composite can be attributed to the synergistic effect of Ag 3PO 4,g-C 3N 4,and a small amount of Ag 0.Regeneration using H 2O 2and NaNH 4HPO 4∙4H 2O fully restored the photoactivity of the catalyst,showing that this green regeneration method could make Ag/Ag 3PO 4/g-C 3N 4an environmentally friendly catalyst for practical applications.729Acta Phys.-Chim.Sin.2014V ol.301IntroductionThe quest for solar-energy utilization has led to the search for functional semiconductor photocatalysts that can directly split water and photodegrade organic pollutants.Accordingly, exploring novel functional materials,such as development of new monomer photocatalysts,graphene-based composite pho-tocatalysts,metal core/semiconductor shell nanocomposites, have become research focus.1-12Ye et al.13reported Ag3PO4as a new type of photocatalyst that exhibits extremely high photo-oxidative capabilities for O2evolution from water and for de-composing organic dyes under visible-light irradiation.The quantum efficiency of Ag3PO4is significantly higher than that of currently known visible light photocatalysts,such as g-C3N4, N-doped TiO2,and BiVO4.14-16Ag3PO4photocorrodes and decomposes to weakly active Ag during photocatalysis,and trace amount of silver as an electron scavenger can improve quantum efficiency and photocatalytic activity.Unfortunately,the photolysis of a large amount of Ag3PO4results in catalyst deactivation,and excess elemental silver affects catalyst contact with sunlight,thereby seriously hampering the practical application of Ag3PO4in photocataly-sis.To solve this problem,many composite photocatalysts, such as AgX(Br,I)/Ag3PO4,17,18TiO2/Ag3PO4,19Ag/Ag3PO4/g-C3N4,20and Ag3PO4/SnO2,21have been developed,and very good results have been achieved.Interestingly,Wang et al.22pro-posed a solution to the problem of recycling Ag from the photo-corrosion and decomposition of Ag3PO4using H2O2as a clean oxidant.However,their method cannot fully restore the catalyt-ic activity of Ag3PO4,and Ag3PO4is lost during the degradation process because Ag3PO4is slightly soluble in aqueous solution, which affects the utilization of the precious metal silver.This study aimed to completely restore activity of photocat-alysts and to avoid the loss of Ag3PO4during catalyst prepara-tion and regeneration.To this end,insoluble g-C3N4was used with Ag3PO4for the chemisorption between g-C3N4and Ag3PO4 to prevent the dissolution of silver phosphate.H2O2and alka-line NaNH4HPO4were used to regenerate the used Ag/Ag3PO4/ g-C3N4hybrid composite photocatalysts that were recycled af-ter the photocatalytic degradation reactions.2Materials and methods2.1Preparation of fresh pure Ag3PO4,pure g-C3N4,and Ag/Ag3PO4/g-C3N4All the reagents were purchased from Sinopharm and used without further purification.Pure Ag3PO4was prepared by the ion-exchange method.About0.39g of AgNO3was dispersed in distilled water(30mL),and an aqueous solution of NaNH4HPO4∙4H2O(15.6mL0.05mol∙L-1)was added.After vigorous stirring for1h,the yellow precipitate was collected by centrifugation,rinsed with distilled water three times,and dried at150°C for4h to obtain Ag3PO4.Pure g-C3N4was pre-pared by heating urea to400°C for0.5h to obtain melamine, and then heating was continued at575°C for2h.To prepare Ag/Ag3PO4/g-C3N4hybrid photocatalysts,the as-prepared g-C3N4power(0.1g)was dispersed in30mL of distilled water under ultrasonication for30min.About0.39g of AgNO3was added to ensure the molar ratio of Ag3PO4to g-C3N4is1:3, which is the optimum ratio,and the mixture was stirred at room temperature.NaNH4HPO4∙4H2O(15.6mL0.05mol∙L-1) was then added dropwise with continuous stirring for1h.The obtained solid product was centrifuged,washed,and dried at 150°C for4h.2.2Catalyst regenerationAfter phenol photodegradation in an aqueous solution under visible-light irradiation,the photocatalyst Ag/Ag3PO4/g-C3N4 was centrifuged,washed three times with distilled water,and dried at150°C for4h.In a typical regeneration reaction,the used photocatalyst was dispersed in NaNH4HPO4aqueous solu-tion(20mL)after each use.Then,H2O2(15%)was added drop-wise to the above suspension until the end of reaction(no bub-ble release).The products were subsequently collected by cen-trifugation,washed three times with distilled water,and dried at150°C for4h.2.3Characterisation of photocatalystsThe crystalline phases of the samples were examined by an X-ray diffraction(XRD)instrument(Rigaku,D/max-2500)us-ing Cu Kαradiation(λ=0.15406nm)within the2θrange from 10°to80°.The accelerating voltage and applied current were 40kV and30mA,respectively,and the scan rate was8(°)∙min-1.Morphological analysis and product compositions were investigated by field-emission scanning electron microscopy (FESEM,Japan JSM-7001F).The light absorption properties of the samples were recorded on an ultraviolet-visible(UV-Vis)spectrophotometer.Elemental compositions were detected by X-ray photoelectron spectroscopy(XPS,Thermo,ESCAL-AB250Xi).The shift in binding energy caused by relative sur-face charges was referenced to the C1s peak of the surface ad-ventitious carbon.2.4Photocatalytic activityThe photocatalytic activities of Ag/Ag3PO4/g-C3N4and re-Ag/Ag3PO4/g-C3N4(regenerated composite photocatalyst)were evaluated by the photocatalytic degradation of phenol in an aqueous solution under visible-light irradiation.For photocata-lytic phenol degradation,0.07g of the as-prepared photocata-lysts was mixed with100mL of15mg∙L-1phenol solution. During photocatalysis,the samples were periodically with-drawn(sampling time of30min),centrifuged to separate the photocatalyst powder from the solution,and subjected to absor-Key Words:Silver phosphate;g-C3N4;Metallic silver;Catalyst regeneration;Phenol;Photocatalysis730LIU Jian-Xin et al.:Synthesis,Regeneration and Photocatalytic Activity under Visible-Light of Ag/Ag3PO4/g-C3N4 No.4bance measurements.The photocatalytic activity of the com-posites was compared with those of the pure g-C3N4and pureAg3PO4powders under the same experimental conditions.Theregenerated photocatalysts were used to repeat the same degra-dation experiment for three cycles to determine their photosta-bility.3Results and discussion3.1Catalyst characterisationX-ray photoelectron spectroscopy was carried out to deter-mine the chemical composition of Ag3PO4,Ag/Ag3PO4/g-C3N4,and re-Ag/Ag3PO4/g-C3N4,as well as the valence states of vari-ous species present therein.The binding energies obtained inthe XPS analysis were corrected for specimen charging by ref-erencing C1s to284.60eV.Photoelectron peaks of Ag,O,P,N,and C were clearly observed in the Ag/Ag3PO4/g-C3N4andre-Ag/Ag3PO4/g-C3N4hybrids,as shown in Fig.1(A),whichconfirmed the presence of Ag,O,P,N,and C in the compos-ites.The comparison of O1s spectra in Fig.1(B)revealed thatthe O1s peak was fitted using XPS PEAK software to separatelattice oxygen and adsorbed oxygen located at530.62and532.80eV,respectively.The presence of adsorbed oxygen canimprove photocatalytic efficiency.25For Ag3PO4,the binding en-ergies of Ag3d5/2and Ag3d3/2peaks were located at367.7and373.7eV,respectively,consistent with the presence of Ag+onthe pared with Ag3PO4,the binding ener-gies of Ag3d5/2and Ag3d3/2in the other samples shifted to368.2and374.2eV,26,27respectively,as shown in Fig.1(C).Thisresult indicated that Ag0particles existed on the photocatalystsurface.Given the electron-rich structure of C3N4units,theycan transfer their electron density to Ag3PO4by overlappingwith the p z orbitals of heterocyclic nitrogens during the prepara-tion of the catalyst,which have the exact symmetry of the high-est unoccupied p-type orbital in the Huckel model.23,24Conse-quently,Ag0particles are generated in the preparation of Ag/Ag3PO4/g-C3N4hybrid photocatalyst.However,the content ofAg0particles is too low to be detected by XRD(Fig.2)in thebulk phase of Ag/Ag3PO4/g-C3N4hybrid photocatalyst becauseC3N4is merely excited during the reaction of AgNO3and NaNH4HPO4∙4H2O.The positions of binding energies of the Ag3d5/2and Ag3d3/2peaks of re-Ag/Ag3PO4/g-C3N4were the same as those of Ag/Ag3PO4/g-C3N4,and the XRD of re-Ag/ Ag3PO4/g-C3N4had no diffraction peaks of Ag0,indicating that the electron transfer process from g-C3N4to Ag3PO4occurred during catalyst regeneration,which was the same as the elec-tron transfer process that occurred during catalyst preparation. The intensity of Ag in the re-Ag/Ag3PO4/g-C3N4much lower than that in the original Ag/Ag3PO4/g-C3N4should attribute to the oxidation of hydrogen peroxide.During the catalyst regen-eration process,hydrogen peroxide as an oxidant to convert Ag0to Ag+.Therefore,the content of Ag0on the surface of the cata-lyst is decreased,and the intensity of Ag in the re-Ag/Ag3PO4/g-C3N4is much lower than that in the original Ag/Ag3PO4/g-C3N4.However,there are a small portion of the metallic silver which was wrapped by colloid group produced during catalyst regen-eration still on the surface of catalyst,avoiding the oxidation in-duced by hydrogen peroxide.After drying the catalyst,the met-al silver wrapped in the colloid group was exposed on the sur-face of the catalyst.As a result,a small amount of Ag0still ex-ists on the surface of the catalyst after regeneration.The XRD patterns of Ag/Ag3PO4/g-C3N4hybrid photocata-lysts exhibited coexistence of g-C3N4and Ag3PO4(JCPDS No. 02-0931)phases.27,28The diffraction peak at38.07°(JCPDS No. 04-0783)assigned to Ag0was found in the XRD patterns of the first used Ag/Ag3PO4/g-C3N4after one recycling run,29indicat-ing that severe photocorrosion of Ag3PO4occurred during pho-todegradation reaction.However the diffraction peaks of Ag disappeared in the XRD patterns of the re-Ag/Ag3PO4/g-C3N4, Fig.1XPS spectra of the photocatalysts(A)survey XPS spectra;(B)O1s spectra;(C)Ag3d spectra.(a)Ag3PO4;(b)Ag/Ag3PO4/g-C3N4;(c)re-Ag/Ag3PO4/g-C3N4731Acta Phys.-Chim.Sin .2014V ol.30and the diffraction peaks of re-Ag/Ag 3PO 4/g-C 3N 4had no signif-icant difference from that of the fresh one except that the main diffraction peaks of re-Ag/Ag 3PO 4/g-C 3N 4at 33.26°are little higher than peaks of Ag/Ag 3PO 4/g-C 3N 4,which means that the crystallization of composite photocatalyst has been improved after photocatalyst regeneration.Thus,Ag 0derived from light corrosion process transformed to Ag 3PO 4during photocatalyst regeneration.Therefore,the method of photocatalyst regenera-tion using NaNH 4HPO 4and H 2O 2(15%)effectively regenerated the composite photocatalyst.Fig.3shows the SEM images of Ag 3PO 4,re-Ag 3PO 4,Ag/Ag 3PO 4/g-C 3N 4,re-Ag/Ag 3PO 4/g-C 3N 4,and g-C 3N 4.Fig.3(A,B)reveals that both Ag 3PO 4and re-Ag 3PO 4particles had irregular spherical morphologies and non-uniform diameters.The mean size of Ag 3PO 4was estimated to be 100-500nm.However,the re-Ag 3PO 4particles obtained by photocatalyst regeneration were more regular in shape and homogeneous in distribution (Fig.3(B)).This finding was due to the rearrangement of Ag 3PO 4particles rebuilt from Ag during regeneration,with colloid coagulation and violent gas release.This variation in shape and distribution can be attributed to diffusion-limited aggregation and/or reaction-limited aggre-gation.30Fig.3(E)shows that g-C 3N 4had an irregular layered structure.The SEM images of Ag/Ag 3PO 4/g-C 3N 4and re-Ag/Ag 3PO 4/g-C 3N 4demonstrated a close connection between g-C 3N 4and Ag 3PO 4semiconductors (Fig.3(C,D)).No obvious sign of the presence of silver was observed because Ag was microscale.Importantly,all of them had the dimensionality,unique absorption edges,and morphologies of the original g-C 3N 4and Ag 3PO 4semiconductors.31Considering the different morphologies between Ag 3PO 4and re-Ag 3PO 4,the regeneration process markedly affected the morphology of re-Ag/Ag 3PO 4/g-C 3N pared with fresh Ag/Ag 3PO 4/g-C 3N 4,the layered structures of re-Ag/Ag 3PO 4/g-C 3N 4were more structured,and the distributions of Ag 3PO 4particles in the g-C 3N 4were more homogeneous.The UV-Vis diffuse reflectance measurements of pure g-C 3N 4,pure Ag 3PO 4,Ag/Ag 3PO 4/g-C 3N 4,and re-Ag/Ag 3PO 4/g-C 3N 4are shown in Fig.4(A).The absorption bands of Ag/Ag 3PO 4/g-C 3N 4and re-Ag/Ag 3PO 4/g-C 3N 4were almost identical in UV-Vis diffuse reflectance.This result further illustrated that this method of regenerating phosphorylation silver catalyst can restore the catalytic performance of the composite photocata-lyst.g-C 3N 4and Ag 3PO 4are direct-transition semiconductors.32,33Thus,the plot of (αh ν)1/2versus h νyielded the band gaps of pure g-C 3N 4,pure Ag 3PO 4,Ag/Ag 3PO 4/g-C 3N 4,and re-Ag/Ag 3PO 4/Fig.2XRD patterns of the photocatalysts(a)Ag/Ag 3PO 4/g-C 3N 4;(b)used-Ag/Ag 3PO 4/g-C 3N 4;(c)re-Ag/Ag 3PO 4/g-C 3N 4.A:Ag 3PO 4,C:g-C 3N4Fig.3SEM images of the photocatalysts(A)Ag 3PO 4;(B)re-Ag 3PO 4;(C)Ag/Ag 3PO 4/g-C 3N 4;(D)re-Ag/Ag 3PO 4/g-C 3N 4;(E)g-C 3N 4732LIU Jian-Xin et al .:Synthesis,Regeneration and Photocatalytic Activity under Visible-Light of Ag/Ag 3PO 4/g-C 3N 4No.4g-C 3N 4,as shown in Fig.4(B).Here,αand νare the adsorption coefficient and light frequency,respectively.The conduction band (CB)and valence band (VB)potentials of Ag 3PO 4and g-C 3N 4were determined to explain the mecha-nism of action of the synthesized photocatalysts.For a semi-conductor,CB and VB were calculated according to the follow-ing empirical equation:E CB =χ−E e −0.5E g E VB =E CB +E gwhere E CB and E VB are the CB and VB edge potentials,respec-tively;χis the electronegativity of the semiconductor,which is the geometric mean of the electronegativity of the constituent atoms;E e is the energy of free electrons on the hydrogen scale (about 4.5eV);and E g is the band-gap energy of the semicon-ductor.The calculated values of the CB and VB potentials of Ag 3PO 4and g-C 3N 4are listed in Table 1.3.2Photocatalytic performanceThe photocatalytic activities of as-prepared samples were evaluated by phenol degradation under visible light (>420nm).A phenol-photolysis test was also conducted for the same dura-tion under visible-light irradiation in the absence of catalyst.The blank test confirmed that phenol cannot be degraded with-in 120min under visible-light irradiation,indicating that phe-nol was a stable molecule and photolysis can be ignored.The photocatalytic efficiency of Ag/Ag 3PO 4/g-C 3N 4hybrid photocat-alysts was higher than those of pure g-C 3N 4and Ag 3PO 4as shown in Fig.5,which was calculated according to the absor-bance of solution at 270nm assigned to phenol.The cause of the photoactivity of Ag 3PO 4with 60min visible-light irradia-tion seemingly even better than that at 120min illumination is that some by-products had been generated during the photode-gration by pure Ag 3PO 4and the absorption of phenol at 270nm treated as the basis for calculating degradation rate is no longer applicable for system including a variety of materials.So,for the photodegration by pure Ag 3PO 4,the reduction of absorption of phenol at 270nm does not mean degradation of phenol.A more detailed demonstration was shown in Fig.6(A,B).During the photodegradation by pure Ag 3PO 4,the absorption peak at 244nm (the absorbance of 5mg of benzoquinone was deter-mined in all temporal absorption spectral patterns)that was rep-resentative of benzoquinone was observed in the absorption spectra.29And the irregular fluctuations of absorption of benzo-quinone and phenol during the whole photodegradation caused the absorption of phenol with 60min visible-light irradiation even lower than that at 120min illumination.Furthermore,the color of solution of phenol became pale yellow from colorless during the photodegration by pure Ag 3PO 4(the possible inter-mediates of degradation process of phenol are colorless except benzoquinone that is pale yellow solution),which is the further evidence of the existence of benzoquinone.Therefor phenol was not degraded and merely mutually transformed with benzo-quinone which was more toxic than phenol in aqueous solu-tion.However,during the same photodegradation of Ag/Ag 3PO 4/g-C 3N 4hybrid photocatalysts,the absorption peak of phenol was weakened,and no absorption peak of additional substances was observed in the absorption spectra of phenol.The same trend was found in the temporal absorption spectral patterns of phenol during photodegradation using re-Ag/Ag 3PO 4/g-C 3N 4and re-Ag 3PO 4,as shown in Fig.6(C,D),respec-Fig.4UV -Vis spectra and band gaps of as-synthesized samples(A)UV-Vis spectra;(B)band gaps.(a)Ag 3PO 4;(b)Ag/Ag 3PO 4/g-C 3N 4;(c)re-Ag/Ag 3PO 4/g-C 3N 4;(d)g-C 3N 4Table 1Calculation results of the CB and VB potentials ofAg 3PO 4and g-C 3N 4Ag 3PO 4g-C 3N 4χ5.964.55E g /eV 1.92.5E CB /eV 0.51-1.20E VB /eV 2.411.30Fig.5Photocatalytic degradation of phenol as a function of irradiation time under visible-light irradiation(a)phenol photolysis;(b)g-C 3N 4;(c)Ag 3PO 4;(d)Ag/Ag 3PO 4/g-C 3N 4733Acta Phys.-Chim.Sin.2014V ol.30tively.Conclusively,the Ag/Ag3PO4/g-C3N4hybrid photocatalysts effectively degraded phenol and possessed more excellent pho-tocatalytic properties than pure Ag3PO4and g-C3N4photocata-lysts.And the method of catalyst regeneration completely re-stored the activity of Ag/Ag3PO4/g-C3N4hybrid photocatalysts.3.3Recycling of Ag/Ag3PO4/g-C3N4and re-Ag/Ag3PO4/g-C3N4Fig.7shows cycling runs for the photocatalytic degradation of phenol in the presence of used Ag/Ag3PO4/g-C3N4without any regeneration process and re-Ag/Ag3PO4/g-C3N4regenerated after each photodegradation experiment in aqueous solution un-der visible-light irradiation.For Ag/Ag3PO4/g-C3N4hybrid pho-tocatalysts without regeneration,the rate of phenol degradation under visible-light irradiation significantly decreased in three successive experimental runs.However,under the same condi-tions,the ultimate degradation rate of phenol under visible-light irradiation for re-Ag/Ag3PO4/g-C3N4nearly had no difference from fresh Ag/Ag3PO4/g-C3N4hybrid photocatalysts.This re-sult indicated that the photocatalyst regeneration method using H2O2and NaNH4HPO4effectively restored photocatalytic activ-ity.More importantly,the method can be used continuously without restrictions.3.4Mechanism of Ag3PO4regeneration from AgAg3PO4is known to facilitate easy photolysis.When Ag3PO4 was used as a photocatalyst without a sacrificial reagent,13 Ag3PO4photocorroded and decomposed to weakly active Ag during photodegradation.A small amount of silver as an elec-tron-capture agent contributed to photocatalytic activity.35How-ever,as the reaction proceeded,the increase in silver content hindered contact between Ag3PO4and illumination.Conse-quently,photocatalytic activity gradually deteriorated,thereby limiting the practical application of Ag3PO4as a recyclable highly efficient photocatalyst.In the case of pure Ag3PO4and Ag/Ag3PO4/g-C3N4,the yellow catalysts were observed to dark-en when the photocatalytic reaction was completed.This phe-nomenon confirmed that Ag+in Ag/Ag3PO4/g-C3N4and Ag3PO4 decomposed to Ag0.The redox potential of the Ag+/Ag pair is0.80V,whereas in the presence of a mass of PO43-ions,the redox potential of Ag species markedly decreased to0.45V(Ag3PO4/Ag).36The H2O2/ OH-pair has a redox potential of0.867V in alkalinecondi-Fig.6Temporal absorption spectra of phenol dye during thephotodegradation process(A)Ag/Ag3PO4/g-C3N4;(B)Ag3PO4;(C)re-Ag/Ag3PO4/g-C3N4;(D)re-Ag3PO4Fig.7Cycling runs for the photocatalytic degradation of phenolunder visible-light irradiation(a)Ag/Ag3PO4/g-C3N4;(b)re-Ag/Ag3PO4/g-C3N4734LIU Jian-Xin et al .:Synthesis,Regeneration and Photocatalytic Activity under Visible-Light of Ag/Ag 3PO 4/g-C 3N 4No.4tions,which is higher than that of Ag 3PO 4/Ag.More important-ly,H 2O 2can oxidize Ag without contaminating the system with any impurity.17Thus,hydrogen peroxide as a clear oxidant can oxidized Ag 0to Ag +.The acid environment of their aqueous so-lution can dissolve Ag 3PO 4,and the decomposition rate of H 2O 2was fast.Thus,the weakly alkaline NaNH 4HPO 4was chosen asthe PO 43-source to prevent the loss of Ag 3PO 4.Once H 2O 2was added dropwise to the beaker with NaNH 4HPO 4aqueous solution and the precipitate of used pho-tocatalyst (used-Ag 3PO 4or used-Ag/Ag 3PO 4/g-C 3N 4)during re-generation,severe outgassing was observed and the boundaries between solution and precipitate disappeared.For Ag/Ag 3PO 4/g-C 3N 4,the used-Ag/Ag 3PO 4/g-C 3N 4transformed to g-C 3N 4/Ag 3PO 4/Ag 2O (colloid),and colloid coagulation occurred with g-C 3N 4/Ag 3PO 4/Ag 2O (colloid)and NaNH 4HPO 4.At the same time,electrons of g-C 3N 4transferred to Ag 3PO 4similar to the transfer that occurred during preparation,and the final product Ag/Ag 3PO 4/g-C 3N 4containing only a minimal content of silver was obtained.The reaction process of Ag 3PO 4also applied to pure Ag 3PO 4,which followed the reaction below:4Ag+4H 2O 2=2Ag 2O (colloid)+4H 2O+O 2(1)3Ag 2O+2PO 43-+6H +=2Ag 3PO 4+3H 2O (2)After the easy regeneration reaction using H 2O 2with NaNH 4HPO 4,the color of Ag/Ag 3PO 4/g-C 3N 4returned from black to pale yellow,the majority of Ag 0disappeared and be-came Ag 3PO 4,and the activity of the composite photocatalyst was restored.Although there is the appearance of chromatic ab-erration between Ag/Ag 3PO 4/g-C 3N 4and re-Ag/Ag 3PO 4/g-C 3N 4as shown in Fig.8for the changes of crystal form and morphol-ogy of the photocatalyst during the colloid coagulation,no ob-vious change was observed in photocatalytic activity.It can be concluded that the catalyst regeneration method used using H 2O 2and NaNH 4HPO 4is effective.3.5Detection of reactive oxygen speciesDuring photocatalytic oxidation,a series of reactive oxygen species,such as h +,∙OH,or O 2-●,are supposed to be involved.To examine the role of these reactive species,the effects ofsome radical scavengers and N 2purging on phenol photodegra-dation were investigated to propose a reaction pathway.The ex-periment on identifying reactive oxygen species was similar to the photodegradation experiment.Different quantities of scav-engers were introduced into the phenol solution prior to cata-lyst addition.In this study,tert-butanol (TB)was added to the reaction system as an ∙OH scavenger,and ammonium oxalate (AO)was introduced as a scavenger of h +.N 2purging was thenadopted to quench O 2-●.37-39Fig.9shows that in the presence of scavengers or when N 2purging was conducted,phenol photodegradation was inhibited in varying degrees compared with no scavenger under the same conditions,indicating that all reactive oxygen species act-ed together for phenol degradation.This finding suggested that phenol photodegradation by Ag/Ag 3PO 4/g-C 3N 4hybrid photo-catalysts was a collaborative process of all reactive oxygen spe-cies.This process differed from methyl orange (MO)photodeg-radation under the same conditions,wherein dissolved O 2had no effect on photodegradation under visible-light irradiation.35This experimental result proved that Ag/Ag 3PO 4/g-C 3N 4hy-brid photocatalysts produced a variety of active substancesthatFig.8Schematic diagram for the processes of the photodegradation,regeneration,and recycling of Ag/Ag 3PO 4/g-C 3N4Fig.9Effects of different scavengers on the degradation of phenol in the presence of Ag/Ag 3PO 4/g-C 3N 4photocatalystsunder visible-light irradiation(a)ammonium oxalate;(b)tert -butanol;(c)N 2purging;(d)no scavenger735Acta Phys.-Chim.Sin.2014V ol.30jointly played an important role in phenol photodegradation un-der visible-light irradiation.3.6Mechanism of improved photocatalysisThe photocatalytic activity of catalysts depends on many fac-tors affecting photocatalysts,such as efficient charge separa-tion,surface property,morphology,optical property,and size.Meanwhile,the properties and characteristics of target organicpollutants affect photodegradation efficiency.41-46In our case,the photodegradation capability of both pure Ag3PO4and pureg-C3N4was insufficient for complete phenol degradation,be-cause this process generated other byproducts or had very lowdegradation efficiency.However,the photocatalysis resultsshowed the excellent photoactivity of the Ag/Ag3PO4/g-C3N4composite samples on phenol degradation,indicating that thecombination of g-C3N4and Ag3PO4was feasible and practical.Based on the above results and current literature,20,22,31,35a mechanism was proposed to explain the enhanced photocatalyt-ic activity of Ag/Ag3PO4/g-C3N4photocatalysts for phenol un-der visible-light irradiation.The energy band edge position be-tween g-C3N4and Ag3PO4and the corresponding enhancement of redox ability were found to improve the photocatalytic abili-ty of Ag/Ag3PO4/g-C3N4photocatalysts for phenol.In general,a more positive VB top corresponded to stronger oxidation abili-ty,and a more negative CB bottom corresponded to stronger re-duction ability.17In the process of photocatalytic reaction by Ag/Ag3PO4/g-C3N4photocatalysts under visible-light irradiation, both Ag3PO4and g-C3N4were excited,and the photogenerated electrons and holes were in their CB and VB,respectively.The electrons in the CB of g-C3N4with a more negative potential displayed strong reduction power,whereas holes in the VB of Ag3PO4showed strong oxidation ability.In more detail,the CB edge potential of g-C3N4(E CB=-1.2eV vs NHE(normal hydro-gen electrode))was more negative than E0(O2/O2-●)(-0.286eV vs NHE)and E0(O2/H2O2)(+0.286eV vs NHE).This finding in-dicated that e-can directly reduce the adsorbed O2molecules into O2-●radicals and H2O2.Moreover,the VB edge potentials of Ag3PO4(E VB=+2.51eV vs NHE)were more positive than E0 (∙OH/H2O)(+2.27eV vs NHE),which demonstrated that the h+of Ag3PO4can provide sufficient potential to oxidise H2O to∙OH.The Ag/Ag3PO4/g-C3N4photocatalysts can simultaneous-ly produce a variety of active substances that cooperatively act on the organic substance,consistent with the finding of the ex-perimental detection of reactive species.Then,all active sub-stances simultaneously reacted with phenol,which differed from the interpretation of some previous studies that organic pollutants react with only one active substance at the same time.40The exclusive use of pure Ag3PO4or pure g-C3N4was unable to generate sufficient active substance because of the lack of redox ability.Additional,according to the Z-scheme principle,the photogenerated electrons moved from the CB bot-tom of Ag3PO4(0.51eV)to Ag0and then continued to shift to the VB top of g-C3N4(1.5eV),recombing with the holes there as shown in Fig.10.47Conclusively,the photocatalytic ability of Ag/Ag3PO4/g-C3N4that can complete phenol degradation was due to the synergistic effects among Ag3PO4nanoparticles and the g-C3N4sheet.Some special properties of g-C3N4and Ag3PO4also affected the activity of the composite photocatalyst.The electronic con-ductivity of g-C3N4with a graphite-like structure accelerated the combination of e-and oxygen,reduced the recombination of electrons and holes,and enhanced the quantum efficiency of Ag/Ag3PO4/g-C3N4photocatalysts.For pure Ag3PO4,the ability to dissolve in water led to loss of photocatalytic performance. Given the chemical adsorption between g-C3N4and Ag3PO4, the insoluble g-C3N4sheet can protect Ag3PO4from dissolution in aqueous solution.4ConclusionsFor application of semiconductor in the field of photocataly-sis,photocatalytic activity and recyclable use of photocatalyst were the most critical factors.In this paper,Ag/Ag3PO4/g-C3N4 hybrid photocatalysts containing traces of silver were easily synthesized,which exhibited great higher photocatalytic activi-ty than pure Ag3PO4or pure g-C3N4for phenol photodegrada-tion under visible-light irradiation(>420nm).And H2O2and NaNH4HPO4were adopted to regenerate Ag3PO4from weak photocatalytically active Ag as a recyclable highly efficient photocatalyst,which almost completely restored the catalytic activity.More importantly,the method of synthesis and regen-eration of Ag/Ag3PO4/g-C3N4hybrid photocatalysts was green, simple,and repeatable.References(1)Fujishima,A.;Honda,K.Nature1972,238(5358),37.doi:10.1038/238037a0(2)Hagfeldt,A.;Grätzel,M.Chem.Rev.1995,95(1),49.doi:10.1021/cr00033a003(3)Chen,W.;Dong,X.F.;Chen,Z.S.;Chen,S.Z.;Lin,W.M.Acta Phys.-Chim.Sin.2009,25(6),1107.[陈威,董新法,陈之善,陈胜洲,林维明.物理化学学报,2009,25(6),1107.] Fig.10Schematic diagram of possible reaction mechanism over Ag/Ag3PO4/g-C3N4hybrid photocatalyst undervisible-light irradiation736。

Ag3PO4埃洛石可见光催化降解抗生素性能研究

Ag3PO4埃洛石可见光催化降解抗生素性能研究

第43卷第4期非金属矿Vol.43 No.4 2020年7月 Non-Metallic Mines July, 2020Ag3PO4/埃洛石可见光催化降解抗生素性能研究朱鹏飞 段 明* 王萍平 冉 尧 张朝莉 贾鸿珊(西南石油大学化学化工学院,四川成都 610500)摘 要以埃洛石为载体,采用超声辅助-沉淀法制备了系列Ag3PO4/埃洛石复合光催化剂。

结果表明,Ag3PO4/埃洛石复合光催化剂中,部分Ag3PO4进入到埃洛石管腔层间,二者通过界面效应和量子化效应增强了催化剂的光吸收能力,并拓宽了催化剂的光谱响应范围。

光催化降解盐酸四环素试验表明,Ag3PO4含量(质量分数)为10%的Ag3PO4/埃洛石光催化活性更优,当催化剂投加量为1.0 g/L,溶液初始pH值为6,H2O2的投加量为15 mL/L,可见光下反应120 min时,20 mg/L盐酸四环素降解率达89.13%,表现出比纯Ag3PO4更好的光催化活性和稳定性,该催化剂对其他几种抗生素也表现出良好的降解效果。

关键词Ag3PO4;埃洛石;可见光催化降解;抗生素中图分类号: X703; O643.36 文献标识码:A 文章编号:1000-8098(2020)04-0092-04Visible Light Photocatalytic Degradation of Antibiotics by Ag3PO4/HalloysiteZhu Pengfei Duan Ming*Wang Pingping Ran Yao Zhang Chaoli Jia Hongshan(School of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu, Sichuan 610500) Abstract A series of Ag3PO4/halloysite composite photocatalysts were prepared by ultrasonic assisted-precipitation method using halloysite as the carrier. The characteristic results show that part of Ag3PO4 enters into the halloysite lumen layer in the composite photocatalyst. Ag3PO4 and halloysite enhance the light absorption capacity and widen the spectral response range of the catalyst through the interface effect and quantization effect. The experiment of photocatalytic degradation of tetracycline hydrochloride exhibits that the photocatalytic activity of Ag3PO4/halloysite with 10% Ag3PO4 content shows the best photodegradation effect. When the dosage of catalyst is 1.0 g/L, the initial pH value of the solution is 6, and the dosage of H2O2 is 15 mL/L, the degradation rate of 20 mg/L tetracycline hydrochloride reached 89.13% under visible light irradiation for 120 min, showing better photocatalytic activity and stability than pure Ag3PO4, and the catalyst also performed good degradation effect on several other antibiotics.Key words Ag3PO4; halloysite; visible-light photocatalytic degradation; antibiotics近年来,人类对抗生素的用量日益增加,抗生素被人体和动物吸收经代谢后,通常以原药和代谢物的形式进入水环境,水中抗生素的残留会使病原微生物抗药性增强,甚至引起“三致”效应,对生态环境和人类健康产生危害[1-3]。

Ag3PO4的可见光光催化性能及机理分析 (1)

Ag3PO4的可见光光催化性能及机理分析 (1)

无机化学学报第28卷用密度泛函理论计算以分析Ag舯。

具有良好可见光光催化活性的原因.而对于A93PO。

在光催化降解水中有机物的研究还未见报道。

本工作采用一种制备方法简单、无需高温煅烧.具有节能等优点的沉淀置换法.合成一种活性较高的可见光光催化材料A93PO。

在模拟太阳光氙灯照射下考察了其对水中微污染有机物的光催化降解性能.同时采用XRD、UV.Vis及XPS对其进行了表征。

进而对其光催化机理进行了详细的分析.以期能为A93PO。

水中微污染有机物处理的实际应用提供基础数据。

1实验部分1.1催化剂的制备将稍过量的NaHCO,溶液缓慢滴人40mL0.1mo卜L-一的AgNO,溶液中得白色浑浊液l。

滴加完毕后。

于室温下继续搅拌2.5h;然后,将相应量的0.1tool・L。

1K2HP04溶液缓慢滴入浑浊液l中即得A妒O。

沉淀,于室温下继续搅拌5h,经离心分离并用蒸馏水和无水乙醇洗涤催化剂样品.最后再在80℃下干燥24h。

即可制备出A93PO。

光催化材料[91.过程反应方程式可表示为:2AgN03+NaHC03_A92C03J,+NaN03+HN03(1)3A92C03+2K2HP04一+2A93P04Jr+2K2C03+C02+H20(2)1.2催化剂的表征样品的晶体结构采用RigakuD/max.2500V型X射线衍射仪分析,X射线源为CuKa线,经融,剥离处理,A=0.15406nm,加速电压为40kV。

电流为100mA.扫描速度80.min一。

扫描范围2p为50。

650.步长为0.020。

样品的光电子能谱采用ESCAL-ab220i—XL型光电子能谱仪分析.激发源为AIKa射线.功率约为300W.分析时的基础真空为3x104Pa.所测元素的结合能均以CIs峰(284.6eV)作为内标校正:催化剂粉体的UV.Vis吸收光谱采用VarianCary50紫外一可见分光光度计测定.扫描范围为200~800砌.数据在室温下的空气氛围中进行采集。

《Ag@AgCl和Ag3PO4基异质结光催化剂的构建及其性能研究》

《Ag@AgCl和Ag3PO4基异质结光催化剂的构建及其性能研究》

《Ag@AgCl和Ag3PO4基异质结光催化剂的构建及其性能研究》篇一一、引言随着环境问题的日益严重和能源资源的日益紧张,光催化技术作为新兴的环保和能源利用手段,已成为研究热点。

异质结光催化剂由于具备高效率、稳定性和广谱响应等优点,在污水处理、空气净化以及太阳能转换等领域具有广阔的应用前景。

本文重点研究了Ag@AgCl和Ag3PO4基异质结光催化剂的构建过程及其性能,旨在通过科学实验与数据分析,探讨其在光催化领域的应用潜力。

二、材料与方法1. 材料准备(1)银(Ag)纳米粒子;(2)氯化银(AgCl)粉末;(3)磷酸银(Ag3PO4)粉末;(4)其他化学试剂及实验设备。

2. 构建方法(1)通过化学还原法合成Ag纳米粒子;(2)采用沉淀法将AgCl和Ag3PO4与Ag纳米粒子结合,形成异质结结构。

3. 性能测试(1)利用紫外-可见光谱分析光吸收性能;(2)通过光电化学测试评估光电流及光响应速度;(3)在模拟太阳光照射下进行光催化实验,观察催化剂对有机污染物的降解效果。

三、结果与讨论1. 异质结光催化剂的构建通过化学方法成功构建了Ag@AgCl和Ag3PO4基异质结光催化剂。

在合成过程中,Ag纳米粒子作为核心,外层分别包覆AgCl和Ag3PO4,形成核壳结构。

这种结构有助于提高光催化剂的稳定性和光吸收能力。

2. 光吸收性能分析紫外-可见光谱分析显示,Ag@AgCl和Ag3PO4基异质结光催化剂具有较好的光吸收性能,特别是在可见光区域。

这归因于Ag纳米粒子的等离子共振效应以及AgCl和Ag3PO4的宽带隙特性。

3. 光电化学性能评估光电化学测试结果表明,Ag@AgCl和Ag3PO4基异质结光催化剂具有较高的光电流密度和快速的光响应速度。

这表明该类催化剂在光电转换方面具有较高的效率。

4. 光催化性能研究在模拟太阳光照射下,Ag@AgCl和Ag3PO4基异质结光催化剂对有机污染物表现出良好的降解效果。

这得益于其优异的光吸收性能和光电化学性能,使得催化剂能够更有效地利用太阳能进行光催化反应。

AgBr@Ag3PO4的制备及其可见光催化降解盐酸莫西沙星的性能

AgBr@Ag3PO4的制备及其可见光催化降解盐酸莫西沙星的性能

AgBr@Ag3PO4的制备及其可见光催化降解盐酸莫西沙星的性能徐秀泉; 吴春笃【期刊名称】《《石油化工》》【年(卷),期】2013(042)004【摘要】以Ag3PO4为前体,采用超声辅助原位离子交换法制备了AgBr@Ag3PO4光催化剂,并利用XRD,SEM,UV-Vis等方法对其进行了表征。

以盐酸莫西沙星(MX)模拟自然水体中的抗菌药物残留,考察了该催化剂在可见光下的光催化性能,探讨了溶液pH、催化剂用量、MX初始浓度及催化剂循环使用次数对AgBr@Ag3PO4光催化性能及降解动力学的影响。

研究了AgBr@Ag3PO4在可见光下的光催化反应机理。

实验结果表明,AgBr和Ag3PO4形成了简单的物理复合物;AgBr@Ag3PO4对MX具有很强的可见光催化降解活性;在溶液pH=11、MX初始浓度20μmol/L、ρ(AgBr@Ag3PO4)=1.0 g/L的条件下,MX在可见光下照射15 min后,降解率达到97.5%;催化机理研究表明,空穴和.OH是该光催化反应中主要的氧化性物质。

【总页数】6页(P445-450)【作者】徐秀泉; 吴春笃【作者单位】江苏大学药学院江苏镇江212013; 江苏大学环境学院江苏镇江212013; 扬州环境资源职业技术学院江苏扬州225002【正文语种】中文【中图分类】TQ426.8【相关文献】1.AgBr@Ag3PO4/GO光催化剂的制备及其可见光催化降解染料性能 [J], 陈浩;万涛;赖鑫林;蒋燕;卢智;黄正根;王春杰;徐舒蕊2.AgBr@Ag3P04的制备及其可见光催化降解盐酸莫西沙星的性能 [J], 徐秀泉; 吴春笃3.ZnFe2O4/Ag3PO4的制备及其可见光催化降解性能的研究 [J], 郑宇翔;关梦圆;任永恒;白娟;张凯欣;景泓菲;高竹青4.Ag@AgBrH_2WO_4异质结光催化剂的制备及其可见光催化降解盐酸莫西沙星性能 [J], 徐秀泉;吴春笃5.Ag_(3)PO_(4)/Cu-BiVO_(4) p-n异质结的制备及其增强可见光催化降解四环素性能 [J], 郭冀峰;李靖;孙泽鑫;李泽恩;卢昶雨因版权原因,仅展示原文概要,查看原文内容请购买。

Ag3PO4的制备及可见光催化性能研究

Ag3PO4的制备及可见光催化性能研究

Ag3PO4的制备及可见光催化性能研究
作者:刘长安, 黄应兴, 解泉华, 苏文悦, 王绪绪, 付贤智
作者单位:福州大学光催化研究所 福州 350002
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6.姚伟峰.Cunping Huang.徐群杰.周笑绿Pd/Cr2O3复合光催化助催化剂的制备及性能研究[会议论文]-2010
7.田宝柱.曾翠云.张金龙不同形貌卤化银的制备及其光催化性能研究[会议论文]-2010
8.刘海津.刘国光新方法制备锆、氮共掺杂TiO2纳米管阵列[会议论文]-2010
9.段丽萍.DUAN Li-ping磷酸体系的平衡计算及磷酸银生成条件的探索[期刊论文]-阴山学刊(自然科学版)2007,21(2)
10.黄雅丽.李旦振.付贤智.王绪绪.HUANG Ya-li.LI Dan-zhen.FU Xian-zhi.WANG Xu-xu Gd/TiO2气相光催化降解乙烯的动力学研究[期刊论文]-稀土2007,28(6)
引用本文格式:刘长安.黄应兴.解泉华.苏文悦.王绪绪.付贤智Ag3PO4的制备及可见光催化性能研究[会议论文] 2010。

Ag3PO4光催化剂的制备、表征及可见光催化性能研究的开题报告

Ag3PO4光催化剂的制备、表征及可见光催化性能研究的开题报告

Ag3PO4光催化剂的制备、表征及可见光催化性能研究的开题报告一、选题背景和意义随着环境污染日益加剧和能源危机的不断加剧,利用可再生能源和绿色技术来处理废水和废气成为了迫切的需求。

光催化技术具有广泛的适用性,并且具有高效、低成本的优势,因此受到了广泛的关注。

光催化反应需要催化剂作为催化剂,因此制备和研究高效的光催化剂对于光催化技术的发展具有重要意义。

二、研究内容和目标本研究将以Ag3PO4为研究对象,制备Ag3PO4光催化剂并进行表征,探究其可见光催化性能。

主要研究内容包括以下方面:1)利用共沉淀法制备Ag3PO4光催化剂;2)采用X射线衍射谱(XRD)、透射电子显微镜(TEM)、紫外-可见漫反射光谱(UV-Vis DRS)等手段对Ag3PO4进行表征;3)探究Ag3PO4的可见光吸收能力、光生电子-空穴对复合速率等性能指标;4)利用Ag3PO4光催化剂处理废水中的污染物,探究其可见光催化降解效果和稳定性。

三、研究计划1)文献调研:了解Ag3PO4的制备方法、表征方法和催化性能等相关信息;2)实验制备Ag3PO4光催化剂:采用共沉淀法制备Ag3PO4,探究不同制备条件对催化剂性能的影响;3)表征催化剂:采用XRD、TEM、UV-Vis DRS等手段对Ag3PO4进行表征;4)评价催化剂催化性能:考察Ag3PO4光催化剂的可见光吸收能力、光生电子-空穴对复合速率等指标;5)利用Ag3PO4光催化剂处理污水:采用甲基橙和罗丹明B等污染物进行降解实验,探究其催化降解效果和稳定性。

四、预期成果和意义1)成功制备Ag3PO4光催化剂,并对其进行表征;2)探究Ag3PO4光催化剂的可见光催化性能;3)对比Ag3PO4催化剂和其他光催化剂的催化性能,分析其优缺点;4)为污水处理提供一种高效、低成本、环保的方法,为光催化技术的发展提供新思路和新途径。

五、可行性分析Ag3PO4光催化剂是一种有效、低成本的光催化剂,已在多种废水处理中被应用。

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毕业论文材料科学与工程学院二零一五年六月天津工业大学毕业论文Ag3PO4微纳米材料的制备及光催化性能研究姓名刘兴政学院材料科学与工程专业复合材料指导教师王立敏职称教授2015年6月天津工业大学毕业设计(论文)任务书题目Ag3PO4微纳米材料的制备及光催化性能研究学生姓名刘兴政学院名称材料科学与工程学院专业班级复合1104 课题类型应用研究课题意义光催化具有光分解水制氢、光降解有机污染物和光还原CO2等功能,光催化在解决能源问题、环境问题和温室气体处理方面有重要的应用前景。

Ag3PO4作为一种高效的光催化剂,由于其制备简单,环境友好光催化降解光电化学领域最有应用前景的材料之一。

这一工作为Ag3PO4在光电化学领域的循环利用提供了重要的理论和实践参考价值。

任务与进度要求研究磷酸银的合成方法,合成几种磷酸银并对其进行催化性质研究。

4.1-4.15 查阅有关磷酸银催化剂的文献,写出开题报告。

4.16-4.30 研究磷酸银催化剂的合成方法。

5.1-5.14 探讨各种磷酸银催化剂对有机废水的降解效果。

5.15-5.30 总结实验过程,写论文。

5.31-6.10 准备答辩、毕业答辩、提交论文。

主要参考文献[1] Bi YP, Hu HY, et al. Two-dimensional dendritic Ag3PO4 nanostructuresand their photocatalytic properties. [J]. Phys. Chem. Chem. Phys., 2012, 14, 14486–14488.[2] Dong LH, Wang P, et al. A simple way for Ag3PO4 tetrahedron andtetrapod microcrystals with high visible-light-responsive activity [J].Materials Letters, 2014, 134, 158–161.[3] Yang ZM, Tian Y, et al. Novel 3D flower-like Ag3PO4 microspheres withhighly enhanced visible light photocatalytic activity [J]. MaterialsLetters, 2014, 116, 209–211.[4] 李军奇,郭占云,王德方,王玉.立方体形Ag3PO4可见光光催化剂的制备及其性能研究[J]. 陕西科技大学学报,2013,31:24-37.起止日期3月20日-6月10日备注院长教研室主任指导教师毕业设计(论文)开题报告表2015 年4月3日姓名刘兴政学院材料科学与工程学院专业复合材料班级1104题目Ag3PO4微纳米材料的制备及光催化性能研究指导教师王立敏与本课题有关的国内外研究情况、课题研究的主要内容、目的和意义:光催化具有光分解水制氢、光降解有机污染物等功能,在解决能源问题、环境问题和温室气体处理方面有重要的应用前景。

Ag3PO4作为一种高效的可见光催化剂,由于其制备简单,环境友好,是光电化学领域最有应用前景的材料之一。

课题研究的主要内容:Ag3PO4微纳米材料的制备及可见光光催化性能目的和意义:通过调控Ag3PO4微纳米材料的形貌及在可见光下进行光催化降解有机染料,更好的用于处理废水中典型的污染物二、进度及预期结果:起止日期主要内容预期结果4月5月6月—探索大量阅读文献,摸索实验方案,翻译英文文献—创新进行主体实验,并开始论文的框架书写,到月底争取完成实验和论文初稿—修改进行最后的论文查重,格式内容修改,准备答辩掌握Ag3PO4微纳米材料的制备方法,完成初步实验,确定实验方案完成实验及测试,分析结果,完成论文大纲修改论文,完成答辩答辩完成课题的现有条件实验室现有的实验设备及药品,材料学院分析测试中心的精密实验仪器审查意见指导教师:年月日学院意见主管领导:年月日题目Ag3PO4微纳米材料的制备及光催化性能研究学生姓名刘兴政学生班级复合1104指导教师姓名王立敏评审项目指标满分评分选题能体现本专业培养目标,使学生得到较全面训练。

题目大小、难度适中,学生工作量饱满,经努力能完成。

10 题目与生产、科研等实际问题结合紧密。

10课题调研、文献检索能独立查阅文献以及从事其他形式的调研,能较好地理解课题任务并提出实施方案;有分析整理各类信息,从中获取新知识的能力。

15论文撰写结构严谨,理论、观点、概念表达准确、清晰。

10 文字通顺,用语正确,基本无错别字和病句,图表清楚,书写格式符合规范。

10外文应用能正确引用外文文献,翻译准确,文字流畅。

5论文水平论文论点正确,论点与论据协调一致,论据充分支持论点,论证过程有说服力。

15 有必要的数据、资料支持,数据、资料翔实可靠,得出的结论有可验性。

15 论文有独到见解或有一定实用价值。

10合计100意见及建议:评阅人签名:年月日学生姓名刘兴政学院名称材料科学与工程专业班级复合1104题目Ag3PO4微纳米材料的制备及光催化性能研究1.毕业论文指导教师评语及成绩:指导教师签字:年月日2.毕业论文答辩委员会评语及成绩:答辩主席(或组长)签字:年月日3.毕业论文总成绩:a.指导教师给定成绩b.评阅教师给定成绩c.毕业答辩成绩总成绩(a×0.3+b×0.3+c×0.4)成绩:成绩:摘要本文采用直接法、Ag+络合法、改变溶剂极性法、Ag+络合并加入表面活性剂法、超声法制备出了不同形貌的磷酸银可见光光催化剂,运用X射线衍射(XRD)、场发射扫描电镜(SEM)等手段对所制备的产品进行了表征。

直接法得到的大部分微粒呈球状,并聚集在一起形成类似四足状磷酸银;氨水络合Ag+法得到四面体形貌磷酸银;改变溶剂极性法得到的磷酸银大部分呈六面体结构;氨水络合Ag+、表面活性剂调控法得到层状六面体形貌磷酸银;超声法得到形貌均一且分散性好的多面体状磷酸银。

以光催化降解罗丹明B溶液为目标测试了不同方法得到的磷酸银的光催化性能。

UV-Vis图证实Ag3PO4在波长约550 nm处有明显吸收,可利用太阳光中的可见光。

经光催化反应90 min后,不同方法得到的磷酸银对罗丹明B 溶液有不同的光催化降解率。

结果表明,光催化降解率的不同跟产品的形貌有很大关系,形貌规整、比表面积大的产品有更多的活性位点和更大的接触面积,因而有更好的光催化性能。

关键词:磷酸银;可见光光催化剂;罗丹明B;光催化降解率ABSTRACTIn this paper, direct method, Ag+complexation method, changing the solvent polarity method, Ag+ complexation method and adding surfactant method as well as ultrasonic method have been used to synthesize silver phosphate visible light photocatalyst with different morphologies. The as-prepared products have been characterized by X-ray diffraction (XRD), field emission scanning electron microscope (SEM) and so on. The spherical particles were obtained by direct method, and the particles gathered together to form similar four-feet shape silver phosphate. Tetrahedron morphology silver phosphate was produced by ammonia complexing Ag+method. Hexahedral structure was obtained by changing the solvent polarity method. Layered hexahedron morphology silver phosphate was generated through ammonia complexing Ag+ and the surfactant controlling method. Polyhedron shape silver phosphate with uniform morphology and good dispersion has been obtained by ultrasonic method.The photocatalytic property tests of the obtained products have been performed via the photocatalytic degradation of rhodamine B solution. The UV-Vis figure confirmed that Ag3PO4 have obvious absorption at the wavelength of ~550 nm, and can use the visible light from the sun. Silver phosphate prepared by different methods have different photocatalytic degradation rate to rhodamine B solution after the 90 min of photocatalytic reaction. The results show that the photocatalytic degradation performance of silver phosphate has much to do with the morphology of products. The products with uniform morphology and large specific surface area have more active sites and larger contact area, and thus have better photocatalytic degradation performance.Key words: Silver phosphate; Visible light photocatalyst; Rhodamine B;Photocatalytic degradation rate目录第一章绪论 (1)1.1前言 (1)1.2纳米材料 (3)1.2.1纳米材料的简介 (3)1.2.2纳米材料的制备方法 (3)1.2.3纳米材料的性质 (5)1.3磷酸银 (6)1.3.1磷酸银的简介 (6)1.3.2纳米磷酸银的研究现状 (7)1.4光催化 (8)第二章实验部分 (11)2.1实验试剂与仪器 (11)2.1.1实验试剂 (11)2.1.2实验仪器 (11)2.1.3实验测试设备 (11)2.2磷酸银的制备 (11)2.2.1直接沉淀法制备磷酸银 (11)2.2.2氨水络合Ag+法制备磷酸银 (12)2.2.3改变溶剂极性法制备磷酸银 (12)2.2.4氨水络合Ag+、表面活性剂调控法制备磷酸银 (12)2.2.5超声法制备磷酸银 (13)第三章磷酸银的表征与分析 (15)3.1直接沉淀法制备磷酸银的表征 (15)3.2氨水络合Ag+法制备磷酸银的表征 (15)3.3改变溶剂极性法制备磷酸银的表征 (16)3.4氨水络合Ag+、表面活性剂调控法制备磷酸银的表征 (17)3.5超声法制备磷酸银的表征 (19)3.6本章小结 (19)第四章磷酸银的光催化性能研究 (21)4.1罗丹明B介绍 (21)4.2磷酸银光催化剂的光催化降解罗丹明B实验 (21)4.2.1直接沉淀法制备的磷酸银光催化罗丹明B实验 (21)4.2.2氨水络合Ag+法制备的磷酸银光催化罗丹明B实验 (21)4.2.3改变溶剂极性法制备的磷酸银光催化罗丹明B实验 (22)4.2.4氨水络合Ag+、表面活性剂调控法制备的磷酸银光催化罗丹明B实验 (23)4.2.5超声法制备的磷酸银光催化罗丹明B实验 (24)4.3本章小结 (24)第五章结论 (27)附录一 (31)附录二 (37)致谢 (47)第一章绪论1.1前言当今世界,全球工业的快速发展带给人类社会的翻天覆地的变化,但是这把双刃剑也给人类带来了很多难题。

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