球磨法制备Tm~(3+)和Tm_2O_3掺杂TiO_2及光催化活性研究
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摘要
为了提高TiO_2的光催化活性,优化球磨工艺,采用球磨法制备稀土金属Tm掺杂TiO_2光催化剂,在300W中压汞灯光照下,对模拟染料亚甲基蓝(MB)溶液进行降解,考察稀土金属Tm以离子态或氧化物掺杂TiO_2的光催化活性,探究球磨中掺杂比、球料比对TiO_2光催化活性的影响,并用XRD、UV-vis DRS、SEM-EDS等对催化剂进行表征。结果表明,Tm~~(3+)的存在可以诱导TiO_2产生晶格畸变,Tm~2O_3/TiO_2和Tm~~(3+)/TiO_2对可见光产生响应,禁带宽度分别降低至2. 97 eV和3. 05 eV。当催化剂投入量为0. 2 g·L~(-1),亚甲基蓝(MB)溶液浓度为25 mg·L~(-1),Tm~~(3+)/TiO_2和Tm~2O_3/TiO_2的最佳掺杂比分别为2. 5%和3%、球料比为4:1、球磨转速为500rpm时,Tm~~(3+)/TiO_2、Tm~2O_3/TiO_2和纯TiO_2的一级反应速率常数分别可达0. 0689 min~(-1)、0. 0562 min~(-1)和0. 0263min~(-1)。
In order to improve the photocatalytic activity of TiO_2 and optimize the ball milling process,Tm~~(3+)/TiO_2 and Tm~2O_3/TiO_2 photocatalysts were prepared by ball milling method.The photocatalytic activities of Tm~~(3+)/TiO_2 and Tm~2O_3/TiO_2 were evaluated by the degradation of methylene blue in aqueous equipped with a 300 W medium pressure mercury lamp.The effects of doping ratio and ball-to-powder weight ratio on the photocatalytic activity of TiO_2 were investigated. XRD,UV-vis DRS and SEM-EDS were used to characterize the as-prepared TiO_2 photocatalysts.Results show that the existence of Tm~~(3+)can induce lattice distortion of TiO_2. The band gap energies of Tm~2O_3/TiO_2 and Tm~~(3+)/TiO_2 decrease to 2. 97 eV and 3. 05 eV,respectively and it leads to visible light absorption response.The first order reaction rate constants of Tm~~(3+)/TiO_2,Tm~2O_3/TiO_2 and pure TiO_2 are 0. 0713 min~(-1),0. 0588 min~(-1)and 0. 0263 min~(-1),respectively with catalysts loading of 0. 2 g·L~(-1),initial concentration of 25 mg·L~(-1)for MB,mole ratios of Tm~~(3+)/TiO_2 and Tm~2O_3/TiO_2 for 2. 5%and 3%,ball-to-powder weight ratio of 4: 1 and ball milling rate of 500 rpm.
In order to improve the photocatalytic activity of TiO_2 and optimize the ball milling process,Tm~~(3+)/TiO_2 and Tm~2O_3/TiO_2 photocatalysts were prepared by ball milling method.The photocatalytic activities of Tm~~(3+)/TiO_2 and Tm~2O_3/TiO_2 were evaluated by the degradation of methylene blue in aqueous equipped with a 300 W medium pressure mercury lamp.The effects of doping ratio and ball-to-powder weight ratio on the photocatalytic activity of TiO_2 were investigated. XRD,UV-vis DRS and SEM-EDS were used to characterize the as-prepared TiO_2 photocatalysts.Results show that the existence of Tm~~(3+)can induce lattice distortion of TiO_2. The band gap energies of Tm~2O_3/TiO_2 and Tm~~(3+)/TiO_2 decrease to 2. 97 eV and 3. 05 eV,respectively and it leads to visible light absorption response.The first order reaction rate constants of Tm~~(3+)/TiO_2,Tm~2O_3/TiO_2 and pure TiO_2 are 0. 0713 min~(-1),0. 0588 min~(-1)and 0. 0263 min~(-1),respectively with catalysts loading of 0. 2 g·L~(-1),initial concentration of 25 mg·L~(-1)for MB,mole ratios of Tm~~(3+)/TiO_2 and Tm~2O_3/TiO_2 for 2. 5%and 3%,ball-to-powder weight ratio of 4: 1 and ball milling rate of 500 rpm.
引文
[1]Miaralipour S,Friedmann D,Scott J,et al.TiO2/porous adsorbents:Recent advances and novel applications[J].Journal of Hazardous Materials,2018,341:404-423.
[2]Li J,Liu C H,Li X,et al.Unraveling the origin of visible light capture by core-shell Ti O2nanotubes[J]. Chemistry Materials,2016,28(12):4467-4475.
[3]Schneider J,Matsuoka M,Takeuchi M,et al.Understanding Ti O2photocatalysis:mechanisms and materials[J]. Chemical Reviews,2014,114:9919-9986.
[4]Phongamwong T,Chareonpanich M,Limtrakul J. Role of chlorophyll in spirulina on photocatalytic activity of CO2reduction under visible light over modified N-doped Ti O2photocatalysts[J]. Applied Catalysis B:Environmental,2015,168:114-124.
[5]Setvin M,Shi X,Hulva J,et al.Methanol on anatase Ti O2(101):Mechanistic insights into photocatalysis[J]. ACS Catalysis,2017,7(10):7081-7091
[6]Zhang J,Wu W C,Yan S,et al.Enhanced photocatalytic activity for the degradation of rhodamine B by Ti O2modified with Gd2O3calcined at high temperature[J]. Applied Surface Science,2015,344:249-256.
[7]Hu X,Hu X J,Tang C F,et al. Mechanisms underlying degradation pathways of microcystin-LR with doped Ti O2photocatalysis[J]. Chemical Engineering Journal,2017,330:355-371.
[8]Todorova N,Giannakopoulou T,Pomoni K,et al.Photocatalytic NOxoxidation over modified Zn O/Ti O2thin films[J].Catalysis Today,2015,252:41-46.
[9]Zhang L W,Fu H B,Zhu Y F.Efficient Ti O2photocatalysts from surface hybridization of Ti O2particles with graphitelike carbon[J]. Advanced Functional Materials,2008,18:2180-2189.
[10]Reli M,Ambro6ováN,Sihor M,et al.Novel cerium doped titania catalysts for photocatalytic decomposition of ammonia[J].Applied Catalysis B:Environmental,2015,178:108-116.
[11]Fang J,Wang F,Qian K,et al.Bifunctional N-doped mesoporous Ti O2photocatalysts[J]. Journal of Physical Chemistry C,2008,112:18150-18156.
[12]万建新,任学昌,刘宏伟,等.Zn O/g-C3N4复合型光催化剂的制备及其光催化性能[J].环境化学,2018,37(4):792-797.
[13]Ruokolainen M,Ollikainen E,Sikanen T,et al.Oxidation of tyrosine-phosphopeptides by titanium dioxide photocatalysis[J]. Journal of the American Chemical Society,2016,138(24):7452-7455.
[14]Wang H X,Wang C H,Cui X M,et al.Design and facile one-step synthesis of Fe WO4/Fe2O3di-modified WO3with super high photocatalytic activity toward degradation of quasi-phenothiazine dyes[J]. Applied Catalysis B:Environmental,2018,221:169-178.
[15]任学昌,马学琴,任晓亮,等.TiO2/PANI/Fe3O4的低温水热法制备及其光催化活性与磁回收性能[J].环境化学,2013,32(11):2149-2155.
[16]Zhan C C,Chen F,Yang J T,et al.Visible light responsive sulfated rare earth doped Ti O2@fumed Si O2composites with mesoporosity:Enhanced photocatalytic activity for methyl orange degradation[J]. Journal of Hazardous Materials,2014,267:88-97.
[17]Chen B,Meng Y H,Sha J W,et al.Preparation of MoS2/Ti O2based nanocomposites for photocatalysis and rechargeable batteries:progress,challenge and perspective[J].Nanoscale,2018,10:34-68.
[18]Zhou J W,Zhang M,Zhu Y F. Photocatalytic Enhancement of Hybrid C3N4/Ti O2prepared via ball milling method[J]. Physical Chemistry Chemical Physics,2015,17(5):3647-3652.
[19]Hu X L,Liu X,Tian J,et al.Towards full-spectrum(UV,visible,and near-infrared)photocatalysis:Achieving an all-solid-state Z-scheme between Ag2O and Ti O2using reduced graphene oxide as the electron mediator[J].Catalysis Science&Technology,2017,7:4193-4205.
[20]Shang M,Wang W Z,Sun S M,et al.Bi2WO6nanocrystals with high photocatalytic activities under visible light[J].Journal of Physical Chemistry C,2008,112:10407-10411.
[21]Huang L W,Fu W Y,Fu X L,et al.Facile and large-scale preparation of N doped Ti O2photocatalyst with high visible light photocatalytic activity[J]. Materials Letters,2017,209:585-588.
[22]Mazierska P,Malankowska A,Kobylanski M,et al.Photocatalytically active Ti O2/Ag2O nanotube arrays interlaced with silver nanoparticles obtained from the one-step anodic oxidation of Ti-Ag alloys[J]. ACS Catalysis,2017,7(4):2753-2764.
[23]Minato T,Kajita S,Pang C L,et al.Tunneling desorption of single hydrogen on the surface of titanium dioxide[J].ACS Nano,2015,9(7):6837-6842.
[24]Liu M,Qiu X Q,Miyauchi M,et al.Cu(II)oxide amorphous nanoclusters grafted Ti3+self-doped Ti O2:An efficient visible light photocatalyst[J]. Chemistry of Materials,2011,23:5282? 5286.
[25]Dong H R,Zeng G M,Tang L,et al.An overview on limitations of Ti O2-based particles for photocatalytic degradation of organic pollutants and the corresponding countermeasures[J].Water Research,2015,79:128-146.
[26]Parnicka P,Mazierska P,Grzyb T,et al.Preparation and photocatalytic activity of Nd-modified Ti O2photocatalysts:Insight into the excitation mechanism under visible light[J].Journal of Catalysis,2016,370:211-222.
[27]Kar A,Smith Y R,Subramanian V.Improved photocatalytic degradation of textile dye using titanium dioxide nanotubes formed over titanium wires[J]. Environmental Science&Technology,2009,43:3260-3265.
[28]Zhang H,Zong R,Zhao J,et al.Dramatic visible photocatalytic degradation performances due to synergetic effect of Ti O2with PANI[J]. Environmental Science&Technology,2008,42:3803-3807.
[29]Trapalis A,Todorova N,Giannakopoulou T,et al. Ti O2/Graphene composite photocatalysts for NOxremoval:A comparison of surfactant-stabilized graphene and reduced graphene oxide[J]. Applied Catalysis B:Environmental,2016,180:637-647.
[30]Primc D,Zeng G B,Leute R,et al.Chemical substitutionalignment of the surface potentials for efficient charge transport in nanocrystalline Ti O2photocatalysts[J].Chemistry of Materials,2016,28(12):4223-4230.
[31]Kong L N,Wang C H,Zheng H,et al. Defect-induced yellow color in Nb-doped Ti O2and its impact on visiblelight photocatalysis[J].Journal of Physical Chemistry C,2015,119:16623-16632.
[32]Wu D,Li C,Kong Q S,et al. Photocatalytic activity of Lu3+/Ti O2prepared by ball milling method[J]. Journal of Rare Earths,2018,36:819-825.
[33]Liu M P,Su T T,Sun L,et al.Facile preparation of yolkshell structured Si/Si C@C@Ti O2nanocomposites as highly efficient photocatalysts for degrading organic dye in wastewater[J].RSC Advances,2016,6:4063-4069.
[34]Yang X,Zhao H,Feng J F,et al.Visible-light-driven selective oxidation of alcohols using a dye-sensitized Ti O2-polyoxometalate catalyst[J]. Journal of Catalysis,2017,351:59-66.
[35]Shi H F,Yu Y C,Zhang Y,et al.Polyoxometalate/Ti O2/Ag composite nanofibers with enhanced photocatalytic performance under visible light[J]. Applied Catalysis B:Environmental,2018,221:280-289.
[36]吴迪,李晨,季日鑫,等.球磨法制备La2O3和La3+掺杂Ti O2剂光催化活性研究[J].化学研究与应用,2018,30(5):689-695.
[37]Chen X B,Mao S S.Titanium dioxide nanomaterials:synthesis,properties,modifications,and applications[J].Chemical Reviews,2007,107:2891-2959.
[38]Jaiswal R,Bharambe J,Patel N,et al.Copper and Nitrogen co-doped Ti O2photocatalyst with enhanced optical absorption and catalytic activity[J]. Applied Catalysis B:Environmental,2015,168:333-341.
[39]张毛进,常薇,王晗,等.改性介孔Ti O2对亚甲基蓝的光催化降解[J].化学研究与应用,2017,29(11):1747-1750.
[40]Yao X L,Chen L,Liu M Y,et al.Rational design of Si/Ti O2heterojunction photocatalysts:transfer matrix method[J]. Applied Catalysis B:Environmental,2018,221:70-76.
[2]Li J,Liu C H,Li X,et al.Unraveling the origin of visible light capture by core-shell Ti O2nanotubes[J]. Chemistry Materials,2016,28(12):4467-4475.
[3]Schneider J,Matsuoka M,Takeuchi M,et al.Understanding Ti O2photocatalysis:mechanisms and materials[J]. Chemical Reviews,2014,114:9919-9986.
[4]Phongamwong T,Chareonpanich M,Limtrakul J. Role of chlorophyll in spirulina on photocatalytic activity of CO2reduction under visible light over modified N-doped Ti O2photocatalysts[J]. Applied Catalysis B:Environmental,2015,168:114-124.
[5]Setvin M,Shi X,Hulva J,et al.Methanol on anatase Ti O2(101):Mechanistic insights into photocatalysis[J]. ACS Catalysis,2017,7(10):7081-7091
[6]Zhang J,Wu W C,Yan S,et al.Enhanced photocatalytic activity for the degradation of rhodamine B by Ti O2modified with Gd2O3calcined at high temperature[J]. Applied Surface Science,2015,344:249-256.
[7]Hu X,Hu X J,Tang C F,et al. Mechanisms underlying degradation pathways of microcystin-LR with doped Ti O2photocatalysis[J]. Chemical Engineering Journal,2017,330:355-371.
[8]Todorova N,Giannakopoulou T,Pomoni K,et al.Photocatalytic NOxoxidation over modified Zn O/Ti O2thin films[J].Catalysis Today,2015,252:41-46.
[9]Zhang L W,Fu H B,Zhu Y F.Efficient Ti O2photocatalysts from surface hybridization of Ti O2particles with graphitelike carbon[J]. Advanced Functional Materials,2008,18:2180-2189.
[10]Reli M,Ambro6ováN,Sihor M,et al.Novel cerium doped titania catalysts for photocatalytic decomposition of ammonia[J].Applied Catalysis B:Environmental,2015,178:108-116.
[11]Fang J,Wang F,Qian K,et al.Bifunctional N-doped mesoporous Ti O2photocatalysts[J]. Journal of Physical Chemistry C,2008,112:18150-18156.
[12]万建新,任学昌,刘宏伟,等.Zn O/g-C3N4复合型光催化剂的制备及其光催化性能[J].环境化学,2018,37(4):792-797.
[13]Ruokolainen M,Ollikainen E,Sikanen T,et al.Oxidation of tyrosine-phosphopeptides by titanium dioxide photocatalysis[J]. Journal of the American Chemical Society,2016,138(24):7452-7455.
[14]Wang H X,Wang C H,Cui X M,et al.Design and facile one-step synthesis of Fe WO4/Fe2O3di-modified WO3with super high photocatalytic activity toward degradation of quasi-phenothiazine dyes[J]. Applied Catalysis B:Environmental,2018,221:169-178.
[15]任学昌,马学琴,任晓亮,等.TiO2/PANI/Fe3O4的低温水热法制备及其光催化活性与磁回收性能[J].环境化学,2013,32(11):2149-2155.
[16]Zhan C C,Chen F,Yang J T,et al.Visible light responsive sulfated rare earth doped Ti O2@fumed Si O2composites with mesoporosity:Enhanced photocatalytic activity for methyl orange degradation[J]. Journal of Hazardous Materials,2014,267:88-97.
[17]Chen B,Meng Y H,Sha J W,et al.Preparation of MoS2/Ti O2based nanocomposites for photocatalysis and rechargeable batteries:progress,challenge and perspective[J].Nanoscale,2018,10:34-68.
[18]Zhou J W,Zhang M,Zhu Y F. Photocatalytic Enhancement of Hybrid C3N4/Ti O2prepared via ball milling method[J]. Physical Chemistry Chemical Physics,2015,17(5):3647-3652.
[19]Hu X L,Liu X,Tian J,et al.Towards full-spectrum(UV,visible,and near-infrared)photocatalysis:Achieving an all-solid-state Z-scheme between Ag2O and Ti O2using reduced graphene oxide as the electron mediator[J].Catalysis Science&Technology,2017,7:4193-4205.
[20]Shang M,Wang W Z,Sun S M,et al.Bi2WO6nanocrystals with high photocatalytic activities under visible light[J].Journal of Physical Chemistry C,2008,112:10407-10411.
[21]Huang L W,Fu W Y,Fu X L,et al.Facile and large-scale preparation of N doped Ti O2photocatalyst with high visible light photocatalytic activity[J]. Materials Letters,2017,209:585-588.
[22]Mazierska P,Malankowska A,Kobylanski M,et al.Photocatalytically active Ti O2/Ag2O nanotube arrays interlaced with silver nanoparticles obtained from the one-step anodic oxidation of Ti-Ag alloys[J]. ACS Catalysis,2017,7(4):2753-2764.
[23]Minato T,Kajita S,Pang C L,et al.Tunneling desorption of single hydrogen on the surface of titanium dioxide[J].ACS Nano,2015,9(7):6837-6842.
[24]Liu M,Qiu X Q,Miyauchi M,et al.Cu(II)oxide amorphous nanoclusters grafted Ti3+self-doped Ti O2:An efficient visible light photocatalyst[J]. Chemistry of Materials,2011,23:5282? 5286.
[25]Dong H R,Zeng G M,Tang L,et al.An overview on limitations of Ti O2-based particles for photocatalytic degradation of organic pollutants and the corresponding countermeasures[J].Water Research,2015,79:128-146.
[26]Parnicka P,Mazierska P,Grzyb T,et al.Preparation and photocatalytic activity of Nd-modified Ti O2photocatalysts:Insight into the excitation mechanism under visible light[J].Journal of Catalysis,2016,370:211-222.
[27]Kar A,Smith Y R,Subramanian V.Improved photocatalytic degradation of textile dye using titanium dioxide nanotubes formed over titanium wires[J]. Environmental Science&Technology,2009,43:3260-3265.
[28]Zhang H,Zong R,Zhao J,et al.Dramatic visible photocatalytic degradation performances due to synergetic effect of Ti O2with PANI[J]. Environmental Science&Technology,2008,42:3803-3807.
[29]Trapalis A,Todorova N,Giannakopoulou T,et al. Ti O2/Graphene composite photocatalysts for NOxremoval:A comparison of surfactant-stabilized graphene and reduced graphene oxide[J]. Applied Catalysis B:Environmental,2016,180:637-647.
[30]Primc D,Zeng G B,Leute R,et al.Chemical substitutionalignment of the surface potentials for efficient charge transport in nanocrystalline Ti O2photocatalysts[J].Chemistry of Materials,2016,28(12):4223-4230.
[31]Kong L N,Wang C H,Zheng H,et al. Defect-induced yellow color in Nb-doped Ti O2and its impact on visiblelight photocatalysis[J].Journal of Physical Chemistry C,2015,119:16623-16632.
[32]Wu D,Li C,Kong Q S,et al. Photocatalytic activity of Lu3+/Ti O2prepared by ball milling method[J]. Journal of Rare Earths,2018,36:819-825.
[33]Liu M P,Su T T,Sun L,et al.Facile preparation of yolkshell structured Si/Si C@C@Ti O2nanocomposites as highly efficient photocatalysts for degrading organic dye in wastewater[J].RSC Advances,2016,6:4063-4069.
[34]Yang X,Zhao H,Feng J F,et al.Visible-light-driven selective oxidation of alcohols using a dye-sensitized Ti O2-polyoxometalate catalyst[J]. Journal of Catalysis,2017,351:59-66.
[35]Shi H F,Yu Y C,Zhang Y,et al.Polyoxometalate/Ti O2/Ag composite nanofibers with enhanced photocatalytic performance under visible light[J]. Applied Catalysis B:Environmental,2018,221:280-289.
[36]吴迪,李晨,季日鑫,等.球磨法制备La2O3和La3+掺杂Ti O2剂光催化活性研究[J].化学研究与应用,2018,30(5):689-695.
[37]Chen X B,Mao S S.Titanium dioxide nanomaterials:synthesis,properties,modifications,and applications[J].Chemical Reviews,2007,107:2891-2959.
[38]Jaiswal R,Bharambe J,Patel N,et al.Copper and Nitrogen co-doped Ti O2photocatalyst with enhanced optical absorption and catalytic activity[J]. Applied Catalysis B:Environmental,2015,168:333-341.
[39]张毛进,常薇,王晗,等.改性介孔Ti O2对亚甲基蓝的光催化降解[J].化学研究与应用,2017,29(11):1747-1750.
[40]Yao X L,Chen L,Liu M Y,et al.Rational design of Si/Ti O2heterojunction photocatalysts:transfer matrix method[J]. Applied Catalysis B:Environmental,2018,221:70-76.