CDots-(001)TiO_2纳米片的制备及其光解水制氢性能
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摘要
以钛酸四丁酯、氢氟酸和石墨棒为原料,采用简单的水热法将具有高催化活性的碳点负载在TiO_2纳米片的(001)晶面上,制得CDots-(001)TiO_2纳米片。通过TiO_2纳米片高催化活性的(001)晶面与碳点的协同作用,提高TiO 2纳米片的光吸收、载流子的传输和分离效率,从而有效提高材料的光催化产氢性能。紫外-可见漫反射吸收谱(UV-visDRS)、光致发光光谱(PL)、瞬态光响应分析结果表明,暴露(001)晶面的TiO_2纳米片负载碳点后,可见光吸收增强,光生载流子的分离和传输速率加快,在间歇模拟太阳光照射下,CDots-(001)TiO 2纳米片的光电流密度约为TiO 2的4倍,当碳点的负载量为2%时,CDots-(001)TiO 2纳米片的光催化产氢速率达5859μmol/(h·g),量子效率达9.6%。
Carbon dots with high catalytic activity were loaded on(001) crystal plane of TiO_2 nanosheets by simple hydrothermal method to prepare CDots-(001) TiO_2 nanosheets using tetrabutyl titanate, hydrofluoric acid and graphite rod as raw materials. The synergistic effect of(001) crystal plane having high catalytic activity and carbon dots improved the light absorption, transport and separation efficiency of carriers of TiO_2 nanosheets, which efficiently enhanced the hydrogen production performance of TiO_2 nanosheets. The UV-vis DRS, PL, and transient photoresponse analysis results showed that the visible light absorption of TiO_2 nanosheets with exposed(001) crystal plane enhanced after loading with carbon dots, and the separation and transmission rate of photogenerated carriers were accelerated. The photocurrent density of CDots-(001)TiO_2 nanosheets was roughly four times as high as that of TiO_2 under intermittent visible light irradiation. The photocatalytic hydrogen production rate of CDots-(001)TiO_2 nanosheets was up to 5859 μmol/(h·g),when the loading of carbon dots was 2% and the quantum efficiency was up to 9.6%.
Carbon dots with high catalytic activity were loaded on(001) crystal plane of TiO_2 nanosheets by simple hydrothermal method to prepare CDots-(001) TiO_2 nanosheets using tetrabutyl titanate, hydrofluoric acid and graphite rod as raw materials. The synergistic effect of(001) crystal plane having high catalytic activity and carbon dots improved the light absorption, transport and separation efficiency of carriers of TiO_2 nanosheets, which efficiently enhanced the hydrogen production performance of TiO_2 nanosheets. The UV-vis DRS, PL, and transient photoresponse analysis results showed that the visible light absorption of TiO_2 nanosheets with exposed(001) crystal plane enhanced after loading with carbon dots, and the separation and transmission rate of photogenerated carriers were accelerated. The photocurrent density of CDots-(001)TiO_2 nanosheets was roughly four times as high as that of TiO_2 under intermittent visible light irradiation. The photocatalytic hydrogen production rate of CDots-(001)TiO_2 nanosheets was up to 5859 μmol/(h·g),when the loading of carbon dots was 2% and the quantum efficiency was up to 9.6%.
引文
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[4]Zhang A,Wang W,Chen J,et al.Epitaxial facet junctions on TiO2single crystals for efficient photocatalytic water splitting[J].Energy&Environmental Science,2018,11:1444-1448.
[5]Yu J,Low J,Xiao W,et al.Enhanced photocatalytic CO2 reduction activity of anatase TiO2 by coexposed{001}and{101}facets[J].Journal of American Chemical Society,2014,136(25):8839-8842.
[6]Zhang H,Zhou P,Chen Z,et al.Hydrogen-bond bridged water oxidation on{001}surfaces of anatase TiO2[J].Journal of Physical Chemistry C,2017,121(4):2251-2257.
[7]Liu X,Dong G,Li S,et al.Direct observation of charge separation on anatase TiO2 crystals with selectively etched{001}facets[J].Journal of American Chemical Society,2016,138(9):2917-2920.
[8]Zhang J,Ma X,Zhang L,et al.Constructing a novel n-p-n dual heterojunction between anatase TiO2 nanosheets with coexposed{101},{001}facets and porous Zn S for enhancing photocatalytic activity of TiO2[J].Journal of Physical Chemistry C,2017,121(11):6133-6140.
[9]Song X,Hu Y,Zheng M M,et al.Solvent-free in situ synthesis of g-C3N4/{001}TiO2 composite with enhanced UV-and visible-light photocatalytic activity for NO oxidation[J].Applied Catalysis B:Environmental,2016,182(5):587-597.
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[11]Shi Xin(石鑫),XU Jianping(徐建萍),Li Linlin(李霖霖),et al.Photoelectrochemical properties of TiO2 nanorod arrays loaded with carbon quantum dots[J].Chinese Journal of Luminescience(发光学报),2015,36(8):898-905.
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[13]Liu J,Liu Y,Liu N,et al.Metal-free efficient photocatalyst for stable visible water splitting via a two-electron pathway[J].Science,2015,347(6225):970-974.
[14]Han X,Kuang Q,Jin M,et al.Synthesis of titania nanosheets with a high percentage of exposed(001)facets and related photocatalytic properties[J].Journal of American Chemical Society,2009,131(9):3152-3153.
[15]Ming H,Ma Z,Liu Y,et al.Large scale electrochemical synthesis of high quality carbon nanodots and their photocatalytic property[J].Dalton Transactions,2012,41(31):9526-9531.
[16]Che W,Cheng W,Yao T,et al.Fast photoelectron transfer in(Cring)-C3N4 plane heterostructural nanosheets for overall water splitting[J].Journal of American Chemical Society,2017,139(8):3021-3026.
[17]Wu X,Yin Shu,Dong Q,et al.Photocatalytic properties of Nd and Ccodoped TiO2 with the whole range of visible light absorption[J].Journal of Physical Chemistry C,2013,117:8345-8352.
[18]Di J,Xia J,Ji M,et al.Nitrogen-doped carbon quantum dots/BiOBr ultrathin nanosheets:In situ strong coupling and improved molecular oxygen activation ability under visible light irradiation[J].ACSSustainable Chemistry&Engineering,2016,4(1):136-146.
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[23]Dong F,Guo S,Wang H Q,et al.Enhancement of the visible light photocatalytic activity of C-doped TiO2 nanomaterials prepared by a green synthetic approach[J].Journal of Physical Chemistry C,2011,115(27):13285-13292.
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[25]Li J,Cai L,Shang J,et al.Giant enhancement of internal electric field boosting bulk charge separation for photocatalysis[J].Advanced Materials,2016,28(21):4059-4064.