在紫外光下以玉米秸秆为牺牲剂提升光催化分解水制氢
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摘要
将玉米秸秆加入Pt/TiO_2的悬浊液中,在紫外光照射下实现了光催化分解水制氢速率的提升。通过SEM、XRD、FT-IR和TGA对玉米秸秆在光催化反应后的结构特征的变化进行了表征和分析讨论。通过单因素实验和正交实验研究了辐照时间、玉米秸秆颗粒浓度、秸秆颗粒粒径和催化剂浓度对氢气产率及产氢量的影响。实验结果表明:催化剂浓度和秸秆颗粒浓度对产氢的影响较大。产氢量随着催化剂浓度的增加先增后减,在催化剂浓度为4×10~(-3)～6×10~(-3)g/ml时产氢量最高。当秸秆颗粒浓度大于0.5×10~(-3)g/ml时,产氢量随着秸秆颗粒浓度的增加出现明显的下降,而且在不同的秸秆颗粒浓度下氢气产率随着反应时间的增加呈现出不同的变化规律,而过小的秸秆颗粒粒径会产生负面的影响。
In this study, addition of corn stover to the water suspension of Pt/TiO_2 significantly improved H_2 evolution from water splitting under UV light. The structural characteristics of corn stover after photocatalytic reaction were characterized by SEM, XRD, FT-IR and TGA. The effects of irradiation time, corn stover particle concentration, stover particle size and catalyst concentration on hydrogen production were studied by single factor experiment and orthogonal experiment. The results show that the catalyst concentration and corn stover particle concentration have a greater impact on hydrogen production. Under the experimental conditions in this paper, the hydrogen production rate and hydrogen yield increase first and then decrease with the increase of catalyst concentration, and the catalyst concentration is 4×10~(-3) g/ml to 6×10~(-3) g/ml. The highest hydrogen yield is obtained.When the concentration of stover granules is more than 0.5×10~(-3) g/ml, the hydrogen production rate decreases with the increase of stover granule concentration. And the hydrogen yield shows different patterns of change with the irradiation time in different stover granule concentration. However, too small corn stover particle size will have a negative impact of hydrogen production.
In this study, addition of corn stover to the water suspension of Pt/TiO_2 significantly improved H_2 evolution from water splitting under UV light. The structural characteristics of corn stover after photocatalytic reaction were characterized by SEM, XRD, FT-IR and TGA. The effects of irradiation time, corn stover particle concentration, stover particle size and catalyst concentration on hydrogen production were studied by single factor experiment and orthogonal experiment. The results show that the catalyst concentration and corn stover particle concentration have a greater impact on hydrogen production. Under the experimental conditions in this paper, the hydrogen production rate and hydrogen yield increase first and then decrease with the increase of catalyst concentration, and the catalyst concentration is 4×10~(-3) g/ml to 6×10~(-3) g/ml. The highest hydrogen yield is obtained.When the concentration of stover granules is more than 0.5×10~(-3) g/ml, the hydrogen production rate decreases with the increase of stover granule concentration. And the hydrogen yield shows different patterns of change with the irradiation time in different stover granule concentration. However, too small corn stover particle size will have a negative impact of hydrogen production.
引文
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[32]Ping W,Liu J,Li Z.Effect of Pt loading and calcination temperature on the photocatalytic hydrogen production activity of TiO2microspheres[J].Ceramics International,2013,39(5):5387-5391.
[33]Antony R P,Mathews T,Ramesh C,et al.Efficient photocatalytic hydrogen generation by Pt modified TiO2nanotubes fabricated by rapid breakdown anodization[J].International Journal of Hydrogen Energy,2012,37(10):8268-8276.
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[2]黄浩,胡国新.Ca(OH)2对生物质水蒸气气化制氢的影响[J].上海交通大学学报,2007,41(12):1930-1933.Huang H,Hu G X.The influence of Ca(OH)2on hydrogen production from biomass by steam gasification[J].Journal of Shanghai Jiaotong University,2007,41(12):1930-1933.
[3]刘刚,孙丽娜,李久海,等.秸秆燃烧排放的正构烷烃及其碳同位素组成特征[J].中国环境科学,2012,32(12):2184-2191.Liu G,Sun L N,Li J H,et al.Chemical and stable carbon isotopic composition of n-alkanes in maize straw and its smoke[J].China Environmental Science,2012,32(12):2184-2191.
[4]李日强,席玉英,曹志亮,等.纤维素类废弃物的综合利用[J].中国环境科学,2002,(1):25-28.Li R Q,Xi Y Y,Cao Z L,et al.Complex use of wastes containing cellulose[J].China Environmental Science,2002,(1):25-28.
[5]王艳,郝炜伟,程轲,等.秸秆露天焚烧典型大气污染物排放因子[J].中国环境科学,2018,38(6):2055-2061.Wang Y,He W W,Cheng K,et al.Emission factors of typical air pollutants from open burning of crop straws[J].China Environmental Science,2018,38(6):2055-2061.
[6]吕鹏梅,熊祖鸿,王铁军,等.生物质流化床气化制取富氢燃气的研究[J].太阳能学报,2003,24(6):758-764.Lyu P M,Xiong Z H,Wang T J,et al.Biomass gasification in a fluidized bed to produce hydrogen rich gas[J].Acta Energiae Solaris Sinica,2003,24(6):758-764.
[7]刘江华,方新湘,周华.我国氢能源开发与生物制氢研究现状[J].新疆农业科学,2004,41(s1):85-87.Liu J H,Fang X X,Zhou H.The state of hydrogen energy R&Dand biohydrogen study in China[J].Xinjiang Agricultural Sciences,2004,41(s1):85-87.
[8]Fujishima A,Honda K.Photolysis-decomposition of water at surface of an irradiated semiconductor[J].Nature,1972,238(1):238-245.
[9]郭烈锦,赵亮.可再生能源制氢与氢能动力系统研究[J].中国科学基金,2002,16(4):210-212.Guo L J,Zhao L.Hydrogen production using solar energy and the study on hydrogen power system[J].Bull.Natl.Nat.Sci.Found.China.,2002,16(4):210-212.
[10]尹忠环,李越湘,彭绍琴,等.污染物乙醇胺Pt/TiO2光催化制氢[J].分子催化,2007,21(2):155-161.Yi Z H,Li Y X,Peng S Q,et al.Photocatalytic hydrogen generation in the presence of ethanolamines over Pt/TiO2[J].Journal of Molecular Catalysis(China),2007,21(2):155-161.
[11]Liu H,Zhou D,Li X,et al.Photoelectrocatalytic degradation of Rhodamine B using mesh Ti/TiO2electrode[J].Chinese Journal of Enviromental Science,2002,23(23):47-51.
[12]Wang D,Zou Y,Wen S,et al.A passivated codoping approach to tailor the band edges of TiO2for efficient photocatalytic degradation of organic pollutants[J].Applied Physics Letters,2009,95(1):829.
[13]Kadam S,Mate V R,Panmand R,et al.A green process for efficient lignin(biomass)degradation and hydrogen production via water splitting using nanostructured C,N,S-doped ZnO under solar light[J].RSC Advances,2014,4(105):60626-60635.
[14]Speltini A,Sturini M,Dondi D,et al.Sunlight-promoted photocatalytic hydrogen gas evolution from water-suspended cellulose:a systematic study[J].Photochemical&Photobiological Sciences Official Journal of the European Photochemistry Association&the European Society for Photobiology,2014,13(10):1410.
[15]董庆华.半导体光催化[J].影像科学与光化学,1993,(2):78-83.Dong Q H.Semiconductor photocatalysis[J].Photographic Science and Photochemistry,1993,(2):78-83.
[16]CurcóD,Giménez J,Addardak A,et al.Effects of radiation absorption and catalyst concentration on the photocatalytic degradation of pollutants[J].Catalysis Today,2002,76(2):177-188.
[17]Heyduk A F,Nocera D G.Hydrogen produced from hydrohalic acid solutions by a two-electron mixed-valence photocatalyst[J].Science,2001,293(5535):1639-1641.
[18]Kato H,Asakura K,Kudo A.Highly efficient water splitting into H2and O2over lanthanum-doped NaTaO3photocatalysts with high crystallinity and surface nanostructure[J].Journal of the American Chemical Society,2003,125(10):3082-3089.
[19]Sakata T,Kawai T.Conversion of carbohydrate into hydrogen fuel by a photocatalytic process[J].Nature,1980,286:474-476.
[20]Sakata T,Kawai T.Heterogeneous photocatalytic production of hydrogen and methane from ethanol and water[J].Chemical Physics Letters,1981,80(2):341-344.
[21]Sakata T,Kawai T,Hashimoto K.Heterogeneous photocatalytic reactions of organic acids and water.New reaction paths besides the photo-Kolbe reaction[J].Journal of Physical Chemistry,1984,88(11):2344-2350.
[22]Kawai T,Sakata T.Hydrogen evolution from water using solid carbon and light energy[J].Nature,1979,282(5736):283-284.
[23]Yoshida H,Hirao K,Nishimoto J I,et al.Hydrogen production from methane and water on platinum loaded titanium oxide photocatalysts[J].The Journal of Physical Chemistry C,2008,112(14):5542-5551.
[24]Kawai T,Sakata T.Photodecomposition of water by using organic compounds[J].Chem.Jpn.,1981,39:589-602.
[25]刘芳,樊丰涛,吕玉翠,等.石墨烯/TiO2复合材料光催化降解有机污染物的研究进展[J].化工学报,2016,67(5):1635-1643.Liu F,Fan F T,Lyu Y C,et al.Research progress on photocatalytic degradation of organic pollutants by graphene/TiO2composite materials[J].CIESC Journal,2016,67(5):1635-1643.
[26]孙怡,于利亮,黄浩斌,等.高级氧化技术处理难降解有机废水的研发趋势及实用化进展[J].化工学报,2017,68(5):1743-1756.Sun Y,Yu L L,Huang H B,et al.Research trend and practical development of advanced oxidation process on degradation of recalcitrant organic wastewater[J].CIESC Journal,2017,68(5):1743-1756.
[27]Zhang G,Ni C,Huang X,et al.Simultaneous cellulose conversion and hydrogen production assisted by cellulose decomposition under UV-light photocatalysis[J].Chemical Communications,2016,52(8):1673-1676.
[28]Wakerley D W,Kuehnel M F,Orchard K L,et al.Solar-driven reforming of lignocellulose to H2with a CdS/CdOx photocatalyst[J].Nature Energy,2017,2(4):17021.
[29]Yang J C,Kim Y C,Shul Y G,et al.Characterization of photoreduced Pt/TiO2and decomposition of dichloroacetic acid over photoreduced Pt/TiO2catalysts[J].Applied Surface Science,1997,121(1):525-529.
[30]Hu F,Jung S,Ragauskas A.Pseudo-lignin formation and its impact on enzymatic hydrolysis[J].Bioresource Technology,2012,117(4):7-12.
[31]张浩,朱庆明.工业废水处理中纳米TiO2光催化技术的应用[J].工业水处理,2011,31(5):17-20.Zhang H,Zhu Q M.Applications of nano-TiO2photocatalytic technology to the treatment of industrial wastewater[J].Industrial Water Treatment,2011,31(5):17-20.
[32]Ping W,Liu J,Li Z.Effect of Pt loading and calcination temperature on the photocatalytic hydrogen production activity of TiO2microspheres[J].Ceramics International,2013,39(5):5387-5391.
[33]Antony R P,Mathews T,Ramesh C,et al.Efficient photocatalytic hydrogen generation by Pt modified TiO2nanotubes fabricated by rapid breakdown anodization[J].International Journal of Hydrogen Energy,2012,37(10):8268-8276.
[34]唐玉朝,李薇,胡春.TiO2形态结构与光催化活性关系的研究[J].化学进展,2003,15(5):379-384.Tang Y C,Li W,Hu C.Studies on morphological structure and photoactivity of TiO2heterogeneous photocatalysts[J].Progress in Chemistry,2003,15(5):379-384.
[35]Puga A V.Photocatalytic production of hydrogen from biomassderived feedstocks[J].Coordination Chemistry Reviews,2016,315:1-66.
[36]Malato S,Maldonado M I,Fernández-Ibá?ez P,et al.Decontamination and disinfection of water by solar photocatalysis:the pilot plants of the Plataforma Solar de Almeria[J].Materials Science in Semiconductor Processing,2016,42(1):15-23.
[37]吴树新,尹燕华,何菲,等.掺铜TiO2光催化剂光催化氧化还原性能的研究[J].感光科学与光化学,2005,23(5):333-335.Wu S X,Yin Y H,He F,et al.Photocatalytic redox performance of copper doped TiO2photocatalyst[J].Photographic Science and Photochemistry,2005,23(5):333-335.
[38]李梓木.可抽提物对玉米秸秆水热预处理效果的影响研究[D].哈尔滨:哈尔滨工业大学,2016.Li Z M.Study on influences of extractives on hydrothermal pretreatment of corn stover[D].Harbin:Harbin Institute of Technology,2016.
[39]Liao G,Chen S,Quan X,et al.Remarkable improvement of visible light photocatalysis with PANI modified core-shell mesoporous TiO2microspheres[J].Applied Catalysis BEnvironmental,2011,102(1/2):126-131.
[40]Fahma F,Iwamoto S,Hori N,et al.Isolation,preparation,and characterization of nanofibers from oil palm empty-fruit-bunch(OPEFB)[J].Cellulose,2010,17(5):977-985.
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