Ag/N共改性TiO_2中空纳米棒阵列的制备及光催化性能
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摘要
当前环境问题和能源危机成为制约人类发展的两大瓶颈,半导体光催化技术有望成为解决环境和能源问题的有效方法。TiO_2由于其廉价、稳定、无毒、活性较好,在光催化研究中被人们经常采用。但是TiO_2能隙较宽,光生电子空穴分离能力差而限制了其实际应用。
近年来,人们尝试各种方法来提高光催化剂的效率:TiO_2纳米结构的形貌,尺寸的控制;利用理想匹配电子能级结构耦合不同半导体;贵金属纳米簇负载于TiO_2颗粒表面;金属,非金属元素掺杂TiO_2等。
本文从两个方面来实现对TiO_2的改性:
1. TiO_2纳米结构的形貌控制以ZnO纳米棒阵列为模板,利用液相沉积法制备TiO_2纳米棒/管阵列结构。通过改变前驱液中n(Ti)/n(B)摩尔比,反应温度等来控制TiO_2纳米结构的形貌。
2.金属、非金属元素共改性TiO_2纳米结构光催化剂以氟钛酸铵为原料,液相沉积法制备TiO_2中空纳米棒阵列(THNA)能够容易实现N掺杂,此基础上进行Ag负载,研究不同Ag浓度对光催化的影响。我们利用拉曼,扫描电子显微镜,透射电子显微镜,紫外可见吸收谱,光电子能谱等手段对样品进行表征。结果表明:Ag元素不仅能够促进锐钛矿相TiO_2向金红石转变,而且能够影响催化剂中N掺杂的含量。
以亚甲基蓝(MB)水溶液为模拟污染物,评价了催化剂在可见和紫外光照下的光催化性能。实验结果表明:当Ag/Ti摩尔比为0.02时,Ag、N共掺杂的TiO_2中空纳米棒阵列(Ag/N-THNA)的紫外光催化效果最佳,其MB降解率约为N单掺杂的TiO_2中空纳米棒阵列(N-THNA)的1.8倍;Ag/Ti摩尔比为0.026时,Ag/N-THNA的可见光催化效率达到最高,约为N-THNA的5.5倍。Ag、N共改性TiO_2中空纳米棒阵列的光催化性能的显著提高,归因于Ag负载,N掺杂以及多相结构(锐钛矿/金红石)等因素的协同效应。
Nowadays, environmental issues and energy crisis have seriously hindered the human development, and the semiconductor photocatalysis is a promising method for solving the environmental and energy problems. Due to relatively high reactivity, low cost, chemical stability and non-toxicity, TiO_2 is often applied in the field of photocatalysis. However, the practical applications of TiO_2 catalyst has been suppressed, due to its wide band gap, low quantum yield.
Recently, several attempts have been made to improve the photocatalytic activity,such as the control of TiO_2 nano-structure’s morphology or size, metal / non-metal doping, noble metal deposition on the surface of TiO_2, coupled semiconductor, etc.
This paper focues on two aspects as following:
1.The control of TiO_2 hollow nanorod arrays’morphology TiO_2 hollow nanorod arrays were synthesized by liquid phase deposition (LPD) method using ZnO nanorod arrays as template. The factors ( n(Ti) / n(B) molar ratio, reaction temperature) effecting on the morphology of TiO_2 hollow nanorod arrays were discussed.
2. TiO_2 nano-structure catalysts co-modified by both metal and non-metal elements
Using ammonium hexafluorotitanate ((NH4)2TiF6) as law material, N doped TiO_2 hollow nanorod arrays were easily achieved by liquid phase deposition (LPD) method. The effect of Ag loading with different content on the photocatalytic activity was also discussed. The catalysts were characterized by Raman spectrum, FESEM, HRTEM, UV-vis absorption spectrum and XPS. The results suggest that AgNO3 additive in the precursor solutions not only can promote the anatase to rutile phase transition, but also influence the amount of N doping in the samples.
The photocatalytic activity of all the samples was evaluated by photodegradation of methylene blue (MB) in aqueous solution. The results show that the photocatalytic degradation rate of Ag/N-THNA is 1.8 and 5.5 times higher than N-TANA under UV and Visble light irradiation, corresponding to the optimum Ag/Ti mole ratio of 0.02 and 0.026, respectively, which were attributed to the synergetic effect of Ag loading, N doping, and the multiphase structure (anatase/rutile).
近年来,人们尝试各种方法来提高光催化剂的效率:TiO_2纳米结构的形貌,尺寸的控制;利用理想匹配电子能级结构耦合不同半导体;贵金属纳米簇负载于TiO_2颗粒表面;金属,非金属元素掺杂TiO_2等。
本文从两个方面来实现对TiO_2的改性:
1. TiO_2纳米结构的形貌控制以ZnO纳米棒阵列为模板,利用液相沉积法制备TiO_2纳米棒/管阵列结构。通过改变前驱液中n(Ti)/n(B)摩尔比,反应温度等来控制TiO_2纳米结构的形貌。
2.金属、非金属元素共改性TiO_2纳米结构光催化剂以氟钛酸铵为原料,液相沉积法制备TiO_2中空纳米棒阵列(THNA)能够容易实现N掺杂,此基础上进行Ag负载,研究不同Ag浓度对光催化的影响。我们利用拉曼,扫描电子显微镜,透射电子显微镜,紫外可见吸收谱,光电子能谱等手段对样品进行表征。结果表明:Ag元素不仅能够促进锐钛矿相TiO_2向金红石转变,而且能够影响催化剂中N掺杂的含量。
以亚甲基蓝(MB)水溶液为模拟污染物,评价了催化剂在可见和紫外光照下的光催化性能。实验结果表明:当Ag/Ti摩尔比为0.02时,Ag、N共掺杂的TiO_2中空纳米棒阵列(Ag/N-THNA)的紫外光催化效果最佳,其MB降解率约为N单掺杂的TiO_2中空纳米棒阵列(N-THNA)的1.8倍;Ag/Ti摩尔比为0.026时,Ag/N-THNA的可见光催化效率达到最高,约为N-THNA的5.5倍。Ag、N共改性TiO_2中空纳米棒阵列的光催化性能的显著提高,归因于Ag负载,N掺杂以及多相结构(锐钛矿/金红石)等因素的协同效应。
Nowadays, environmental issues and energy crisis have seriously hindered the human development, and the semiconductor photocatalysis is a promising method for solving the environmental and energy problems. Due to relatively high reactivity, low cost, chemical stability and non-toxicity, TiO_2 is often applied in the field of photocatalysis. However, the practical applications of TiO_2 catalyst has been suppressed, due to its wide band gap, low quantum yield.
Recently, several attempts have been made to improve the photocatalytic activity,such as the control of TiO_2 nano-structure’s morphology or size, metal / non-metal doping, noble metal deposition on the surface of TiO_2, coupled semiconductor, etc.
This paper focues on two aspects as following:
1.The control of TiO_2 hollow nanorod arrays’morphology TiO_2 hollow nanorod arrays were synthesized by liquid phase deposition (LPD) method using ZnO nanorod arrays as template. The factors ( n(Ti) / n(B) molar ratio, reaction temperature) effecting on the morphology of TiO_2 hollow nanorod arrays were discussed.
2. TiO_2 nano-structure catalysts co-modified by both metal and non-metal elements
Using ammonium hexafluorotitanate ((NH4)2TiF6) as law material, N doped TiO_2 hollow nanorod arrays were easily achieved by liquid phase deposition (LPD) method. The effect of Ag loading with different content on the photocatalytic activity was also discussed. The catalysts were characterized by Raman spectrum, FESEM, HRTEM, UV-vis absorption spectrum and XPS. The results suggest that AgNO3 additive in the precursor solutions not only can promote the anatase to rutile phase transition, but also influence the amount of N doping in the samples.
The photocatalytic activity of all the samples was evaluated by photodegradation of methylene blue (MB) in aqueous solution. The results show that the photocatalytic degradation rate of Ag/N-THNA is 1.8 and 5.5 times higher than N-TANA under UV and Visble light irradiation, corresponding to the optimum Ag/Ti mole ratio of 0.02 and 0.026, respectively, which were attributed to the synergetic effect of Ag loading, N doping, and the multiphase structure (anatase/rutile).
引文
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