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Pd/TiO2光催化苯甲酸水溶液产氢性能研究

李福颖 牛玉 王仁章

李福颖, 牛玉, 王仁章. Pd/TiO2光催化苯甲酸水溶液产氢性能研究[J]. 环境科学研究, 2016, 29(7): 1089-1095.
引用本文: 李福颖, 牛玉, 王仁章. Pd/TiO2光催化苯甲酸水溶液产氢性能研究[J]. 环境科学研究, 2016, 29(7): 1089-1095.
LI Fuying, NIU Yu, WANG Renzhang. Photocatalytic Hydrogen Evolution from Water over Pd/TiO2 with Benzoic Acid Compounds as Sacrificial Agents[J]. Research of Environmental Sciences, 2016, 29(7): 1089-1095.
Citation: LI Fuying, NIU Yu, WANG Renzhang. Photocatalytic Hydrogen Evolution from Water over Pd/TiO2 with Benzoic Acid Compounds as Sacrificial Agents[J]. Research of Environmental Sciences, 2016, 29(7): 1089-1095.

Pd/TiO2光催化苯甲酸水溶液产氢性能研究

基金项目: 福建省2011洁净煤气化技术协同创新中心项目(XK1401);福建省科技厅自然科学基金项目(2015J01601); 福建省教育厅青年基金项目(JA15475)

Photocatalytic Hydrogen Evolution from Water over Pd/TiO2 with Benzoic Acid Compounds as Sacrificial Agents

  • 摘要: 为了探讨在光催化分解水(下称光解水)制氢反应中含苯有机废水作为牺牲剂的可行性,以光沉积法制备了Pd/TiO2〔w(Pd)为0.5%〕模型催化剂,并且通过XRD(X射线衍射)、BET(N2物理吸附)、TEM(透射电镜)、XPS(X射线光电子能谱)和UV-vis DRS(紫外-可见漫反射吸收光谱)等表征手段考察了催化剂的微观结构及性质, 使用泊菲莱Labsolar-Ⅲ AG系统评价了苯甲酸、邻苯二甲酸、间苯三甲酸作为牺牲剂的光催化性能. 结果表明:引入的Pd以Pb0和Pb2+高度分散在TiO2基底表面,未改变TiO2的晶体结构;与TiO2相比,Pd/TiO2具有更大的比表面积、更小的孔径和更强的光吸收性能. 苯甲酸、邻苯二甲酸、间苯三甲酸光解水产氢速率分别为4.264、6.429和5.400 mmol/(g·h),分别为空白处理〔无牺牲剂,0.733 mmol/(g·h)〕的5.8、8.8、7.4倍. 依据乙酸和三氟乙酸的光解水产氢速率数据及结构特征,初步探讨了苯甲酸参与价带空穴氧化反应的机理,发现光解水产氢速率的大小与苯甲酸牺牲剂的还原性强弱、羧基个数以及空间位阻有关,表现为牺牲剂发生photo-Kolbe脱羧反应越容易、羰基数目越多、空间位阻越小,其光解水产氢速率越高. 未来应进一步探寻高效、稳定的模型牺牲剂,以应用于氢能源生产研究.

     

  • [1] 王新胜,谢黎明,张锦.二维半导体合金的制备、结构和性质.化学学报,2015,3(9):886-894.WANG Xinsheng,XIE Liming,ZHANG Jin.Preparation,structure and properties of two-dimensional semiconductor alloys.Acta Chimica Sinaca,2015,3(9):886-894.
    [2] 叶飞,刘荣,贡湘君,等.ZrO2晶相对锰铈系SCR催化剂脱硝活性的影响.环境科学研究,2015,8(11):1720-1727.YE Fei,LIU Rong,GONG Xiangjun,et al.Effects of zirconia crystallite phases on MnOx-CeO2 SCR deNOx catalysts.Research of Environmental Sciences,2015,8(11):1720-1727.
    [3] 朱立峰,石将建,李冬梅,等.多孔TiO2层厚度对钙钛矿太阳能电池性能的影响.化学学报,2015,3(3):261-266.ZHU Lifeng,SHI Jiangjian,LI Dongmei,et al.Effect of mesoporous TiO2 layer thickness on the cell performance of perovskite solar cells.Acta Chimica Sinaca,2015,3(3):261-266.
    [4] 李涛海,吴季怀,陈秀琴.需要牺牲剂可见光下分解水的光催化材料.化工新型材料,2004,2(4):1-4.LI Taohai,WU Jihuai,CHEN Xiuqin.Photocatalyst materials for water splitting in the presence of sacrificial reagent under visible light.New Chemical Materials,2004,2(4):1-4.
    [5] LO Choching,HUNG Chunghsuang,YUAN Chungshin,et al.Photoreduction of carbon dioxide with H2 and H2O over TiO2 and ZrO2 in a circulated photocatalytic reactor.Solar Energy Materials & Solar Cells,2007,1(19):1765-1774.
    [6] SUN Wei,ZHANG Shuqing,LIU Zhixiang,et al.Studies on the enhanced photocatalytic hydrogen evolution over Pt/PEG-modified TiO2 photocatalysts.International Journal of Hydrogen Energy,2008,3(4):1112-1117.
    [7] WEI Yuelin,LI Jing,HUANG Yunfang,et al.Photocatalytic water splitting with in-doped H2 LaNb2O7 composite oxide semiconductors.Solar Energy Materials & Solar Cells,2009,3(8):1176-1181.
    [8] MAENAKA Y,SUENOBU T,FUKUZUMI S.Hydrogen evolution from aliphatic alcohols and 1,4-Selective hydrogenation of NAD+catalyzed by a [C,N] and a [C,C] cyclometalated organoiridium complex at room temperature in water.Journal of the American Chemical Society,2012,4(22):9417-9427.
    [9] BISWAL N,DAS D P,MARTHA S,et al.Efficient hydrogen production by composite photocatalyst CdS-ZnS/Zirconiume-titanium phosphate (ZTP) under visible light illumination.International Journal of Hydrogen Energy,2011,6(21):13452-13460.
    [10] FAN Wenjuan,ZHOU Zhengfa,XU Weibing,et al.Preparation of ZnIn2S4/fluoropolymer fiber composites and its photocatalytic H2 evolution from splitting of water using Xe lamp irradiation.International Journal of Hydrogen Energy,2010,5(13):6225-6230.
    [11] MCCORMICK T M,CALITREE B D,ORCHARD A,et al.Reductive side of water splitting in artificial photosynthesis:new homogeneous photosystems of great activity and mechanistic insight.Journal of the American Chemical Society,2010,2(44):15480-15483.
    [12] ARNEY D,WATKINS T,MAGGARD P A.Effects of particle surface areas and microstructures on photocatalytic H2 and O2 production over PbTiO3.Journal of the American Ceramic Society,2011,4(5):1483-1489.
    [13] BARRECA D,FORNASIERO P,GASPAROTTO A,et al.The potential of supported Cu2O and CuO nanosystems in photocatalytic H2 production.Chemitry & Sustainability Energy & Materials,2009,2(3):230-233.
    [14] ASENJO N G,LVAREZ P,GRANDA M,et al.High performance activated carbon for benzene/toluene adsorption from industrial wastewater.Journal of Hazardous Materials,2011,2(3):1525-1532.
    [15] SABBAGHI S,MOHAMMADI M,EBADI H.Photocatalytic degradation of benzene wastewater using PANI-TiO2 nanocomposite under UV and solar light radiation.Journal of Environmental Engineering,2016,2(3):05015003.
    [16] SINGH P,BORTHAKUR A,SRIVASTAVA N,et al.Photocatalytic degradation of benzene and toluene in aqueous medium.Pollution,2016,2(2):199-210.
    [17] 邵春雷,顾丁红,陆晶,等.新型二氧化铅电极处理硝基苯废水.环境科学研究,2006,9(4):65-69.SHAO Chunlei,GU Dinghong,LU Jing,et al.Research on the treatment of nitrobenzene wastewater by electrolysis on a novel lead dioxide anode.Research of Environmental Sciences,2006,9(4):65-69.
    [18] ZHANG Fuxiang,CHEN Jixin,ZHANG Xiu,et al.Simple and low-cost preparation method for highly dispersed Pd/TiO2 catalysts.Catalysis Today,2004,3:645-650.
    [19] YONEYAMA H,NISHIMURA N,TAMURA H.Photodeposition of palladium and platinum onto titanium dioxide single crystals.The Journal of Physical Chemistry,1981,5(3):268-272.
    [20] WANG Hou,YUAN Xingzhong,WU Yan,et al.Photodeposition of metal sulfides on titanium metal-organic frameworks for excellent visible-light-driven photocatalytic Cr(Ⅵ) reduction.RSC Advances,2015,1(5):32531-32535.
    [21] FU Xianliang,WANG Xuxu,DENNIS Y C L,et al.Photocatalytic reforming of C3-polyols for H2 production:Part Ⅰ.role of their OH groups.Applied Catalysis B:Environmental,2011,6(3/4):681-688.
    [22] GROEN J C,RAMIREZ J P.Critical appraisal of mesopore characterization by adsorption analysis.Applied Catalysis A:General,2004,8(1/2):121-125.
    [23] LEE Y W,KIM M,KIM Z H,et al.One-step synthesis of Au@Pd core-shell nanooctahedron.Journal of the American Chemical Society,2009,1(47):17036-17037.
    [24] YU Jiaguo,QI Lifang,JARONIEC M.Hydrogen production by photocatalytic water splitting over Pt/TiO2 nanosheets with exposed (001) facets.Journal of Physical Chemistry C,2010,4(30):13118-13125.
    [25] CUI Chunyue,WU Juan,XIN Yanjun,et al.Highly stable palladium-loaded TiO2 nanotube array electrode for the electrocatalytic hydrodehalogenation of polychlorinated biphenyls.Korean Journal of Chemical Engineering,2015,2(6):1069-1074.
    [26] KWAK B S,CHAE J,KIM J,et al.Enhanced hydrogen production from methanol/water photo-splitting in TiO2 including Pd component.Bulletin of the Korean Chemical Society,2009,0(5):1047-1053.
    [27] WU Zhongbiao,SHENG Zhongyi,WANG Haiqiang,et al.Relationship between Pd oxidation states on TiO2 and the photocatalytic oxidation behaviors of nitric oxide.Chemosphere,2009,7(2):264-268.
    [28] ZHANG Fuxiang,CHEN Jixin,ZHANG Xiu,et al.Synthesis of titania-supported platinum catalyst:the effect of pH on morphology control and valence state during photodeposition.Langmuir,2004,0(21):9329-9334.
    [29] HOFFMANN M R,MARTIN S T,CHOI W,et al.Environmental applications of semiconductor photocatalysis.Chemical Reviews,1995,5(1):69-96.
    [30] BANDARA J,UDAWATTA C,RAJAPAKSE C.Highly stable CuO incorporated TiO2 catalyst for photocatalytic hydrogen production from H2O.Photochemical & Photobiological Sciences,2005,4(11):857-861.
    [31] ALLEN M R,THIBERT A,SABIO E M,et al.Evolution of physical and photocatalytic properties in the layered titanates A2Ti4O9 (A=K,H) and in nanosheets derived by chemical exfoliation.Chemistry of Materials,2010,2(3):1220-1228.
    [32] NG B J,XU Shiping,ZHANG Xiwang,et al.Hybridized nanowires and cubes:a novel architecture of a heterojunctioned TiO2 /SrTiO3 thin film for efficient water splitting.Advanced Functional Materials,2010,0(24):4287-4294.
    [33] BERNHARD K,ALLEN J B.Photoelectrosynthesis of ethane from acetate ion at an n-type titanium dioxide electrode.the photo-kolbe reaction.Journal of the American Chemical Society,1977,9(23):7729-7731.
    [34] 龚艳,林鹿,孙勇,等.脱羧反应途径及其机制的研究进展.化学与生物工程,2008,5(4):1-6.GONG Yan,LIN Lu,SUN Yong,et al.Research progress of pathways and mechanisms of decarboxylation.Chemistry & Bioengineering,2008,5(4):1-6.
    [35] 邝代治,冯泳兰,许金生,等.链型脂肪族饱和二元酸的结构与反应性的讨论.长沙电力学院学报(自然科学版),2006,1(4):107-112.KUANG Daizhi,FENG Yonglan,XU Jinsheng,et al.Structure and reactivity of aliphatic saturated hydrocarbon dicarboxylic acids.Journal of Changsha University of Electric Power (Natural Science),2006,1(4):107-112.
    [36] 杨桂朋,张正斌.海水中酚类有机污染物在粘土表面上的交换作用-酚类有机污染物在粘土表面上的交换等温线及其分级交换的空间位阻效应.海洋学报,1992,4(5):135-141.
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出版历程
  • 收稿日期:  2015-12-14
  • 修回日期:  2016-04-22
  • 刊出日期:  2016-07-25

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