{110}晶面外露的Cu_2O颗粒的合成及其对高氯酸铵热分解催化活性
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摘要
通过液相合成法,利用油酸作为形貌导向剂,通过控制油酸的用量,制备出不同形貌的Cu_2O催化剂。其中,外露面为{110}的十二面体Cu_2O单晶,对高氯酸铵(AP)的低温分解的催化效果最佳,使AP的低温分解温度降低约61℃,使其分解峰值温度降到269℃。此外,当十二面体Cu_2O单晶的添加量由2%增加到5%时,AP的低温阶段分解的质量分数由25.1%增加至98.1%。
Cu_2O particles were successfully fabricated by a facile hydrothermal method, and its shape of the particles depends on the amount of morphology inducing agent, i.e. oleic acid. Cu_2 O with various morphology effectively promotes the pyrolysis of ammonium perchlorate(AP), and the dodecahedral Cu_2 O with exposed {110} plane presents the best catalytic effect on the low temperature decomposition of AP. The dodecahedral Cu_2 O substantially decreases the temperature of first-stage decomposition of AP to 269 ℃. Furthermore, the decomposed mass fraction of AP in low temperature stage increased markedly from 25.1% to 98.1% as the additive amount of dodecahedral Cu_2 O increased from 2% to 5%.
Cu_2O particles were successfully fabricated by a facile hydrothermal method, and its shape of the particles depends on the amount of morphology inducing agent, i.e. oleic acid. Cu_2 O with various morphology effectively promotes the pyrolysis of ammonium perchlorate(AP), and the dodecahedral Cu_2 O with exposed {110} plane presents the best catalytic effect on the low temperature decomposition of AP. The dodecahedral Cu_2 O substantially decreases the temperature of first-stage decomposition of AP to 269 ℃. Furthermore, the decomposed mass fraction of AP in low temperature stage increased markedly from 25.1% to 98.1% as the additive amount of dodecahedral Cu_2 O increased from 2% to 5%.
引文
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[2]KUO C H,YANG Y C,GWO S,et al.Facet–dependent and Au nanocrystals–enhanced electrical and photocatalytic properties of Au–Cu2O core–shell heterostructures[J].J Am Chem Soc,2011,133(4):12040–12041.
[3]TAN C S,HSU S C,KE W H,et al.Facet–dependent electrical conductivity properties of Cu2O crystals[J].Nano Lett,2015,15(3):2155–2160.
[4]HUANG M H,REJ S,HSU S C.Facet–dependent properties of polyhedral nanocrystals[J].Chem Commun,2014,50(14):1634–1645.
[5]OUYANG J J,PEI J,KUANG Q,et al.Supersaturation–controlled shape evolution of Fe2O3 nanocrystals and their facet–dependent catalytic and sensing properties[J].ACS Appl Mater Interfaces,2014,6:12505–12514.
[6]XU H,OUYANG S X,LI P,et al.High–active anatase Ti O2 nanosheets exposed with 95%{100}facets towards efficient H2 evolution and CO2photoreduction[J].ACS Appl Mater Interfaces,2013,5(4):1348–1354.
[7]PAN J,LIU G,LU Q,et al.On the true photoreactivity order of{001},{010},and{101}facets of anatase Ti O2 crystals[J].Angew Chem Int Ed,2011,50:2133–2137.
[8]ZHANG Y L,ZHANG Q,XIA T,et al.The influence of reaction temperature on the formation and photocatalytic hydrogen generation of(001)faceted Ti O2 nanosheets[J].Chem Nano Mater,2015,1(4):270–275.
[9]SUI Y M,FU W Y,YANG H B,et al.Low temperature synthesis of Cu2O crystals:shape evolution and growth mechanism[J].Cryst Growth Des,2010,10(1):99–108.
[10]CAO Y B,FAN J M,BAI L Y,et al.Morphology evolution of Cu2O from octahedra to hollow structures[J].Cryst Growth Des,2010,10(1):232–236.
[11]SUSMAN M D,FELDMAN Y,VASKEVICH A,et al.Chemical deposition of Cu2O nanocrystals with precise morphology control[J].ACS Nano,2014,8(1):162–174.
[12]罗元香,陆路德,汪信.纳米级过渡金属氧化物对高氯酸铵催化性能的研究[J].含能材料,2002,10(4):148–152.LUO Yuanxiang,LU Lude,WANG Xin.Chin J Energ Mater(in Chinese),2002,10(4):148–152.
[13]罗小林,杨德锁,原春兰,等.不同结构Cu2O多晶的合成及其对高氯酸铵热分解的催化作用[J].物理化学学报,2014,30(3):520–526.LUO Xiaolin,YANG Desuo,YUAN Chunlan,et al.Acta Phys Chim Sin(in Chinese),2014,30(3):520–526.
[14]HENG B J,XIAO T,HUA X Y,et al.Catalytic activity of Cu2O micro–particles with different morphologies in the thermal decomposition of ammonium perchlorate[J].Thermochim Acta,2011,524(2):135–139.
[15]REN Y,MA Z,BRUCE P G.Ordered mesoporous metal oxides:synthesis and applications[J].Chem Soc Rev,2012,41(14):4909–4927.
[16]PATZKE G R,ZHOU Y,KONTIC R,et al.Oxide nanomaterials:synthetic developments,mechanistic studies,and technological innovations[J].Angew Chem Int Ed,2011,50(4):826–859.
[17]CHANDA C,REJ S,HUANG M H.Facet–dependent catalytic activity of Cu2O nanocrystals in the one–pot synthesis of1,2,3,–triazoles by multicomponent click reactions[J].Chem Eur J,2013,19:16036–16043.
[18]朱俊武,陈海洋,谢波,等.纳米Cu2O的制备及其对高氯酸铵热分解的催化性能[J].催化学报,2004,25(8):637–642.ZHU Junwu,CHEN Haiyang,XIE Bo,et al.Chin J Catal(in Chinese),2004,25(8):637–642.
[19]BOLDYREV V V.Thermal decomposition of ammonium per chlorate[J].Thermochim Acta,2006,443(1):1–36.
[20]罗小林,韩银凤,杨德锁,等.溶剂热合成Cu2O微球及其对高氯酸铵热分解的催化作用[J].物理化学学报,2012,28(2):297–302.LUO Xiaolin,HAN Yinfeng,YANG Desuo,et al.Acta Phys Chim Sin(in Chinese),2012,28(2):297–302.
[21]ZHANG Y,DENG B,ZHANG T,et al.Shape effects of Cu2O polyhedral microcrystals on photocatalytic activity[J].J Phys Chem C,2010,114(11):5073–5079.
[22]LI L P,SUN X F,QIU X Q,et al.Nature of catalytic activities of Co O nanocrystals in thermal decomposition of ammonium perchlorate[J].Inorg Chem,2008,47:8839–8846.
[23]HO J Y,HUANG M H.Synthesis of submicrometer–sized Cu2O crystals with morphological evolution from cubic to hexapod structures and their comparative photocatalytic activity[J].J Phys Chem C,2009,113(32):14159–14164.
[24]EL–AWAD A M,SAID A A,ABD EL–SALAAM M M.Thermal decomposition of KCl O4 catalyzed by Mn O2–Cu O mixed oxides systems[J].Thermochim Acta,1988,126,17–24.
[25]MAKHLOUF S A.Magnetic properties of Co3O4 nanoparticles[J].J Magn Magn Mater,2002,246:184–190.