g-C_3N_4纳米片光催化还原二氧化碳的性能研究
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摘要
光催化还原CO_2制备CH_4和CH_3OH等高附加值化学品,具有对环境友好、反应条件温和与耗能低等优点。自1979年Inoue等报道TiO_2,ZnO,Ga P和Si C半导体在光照下能将CO_2转化为CH_4,CH_3OH,HCOOH和HCHO以来[1],光催化还原CO2研究受到了极大关注[2]。g-C3N4具有类石墨层状结构,原料廉价,易制备,且具有非常好的热稳定性和化学稳定性。由于其优异的稳定性和独特的电子能带结构(禁带宽度为2.7 e V),作为可见光半导体光催化剂材料在太阳能转换和环境污染物降解等领域得到了广泛应用[3,4]。本工作以尿素为原料,在马弗炉中550 oC下烧结4 h后制备了g-C_3N_4的多孔纳米片,并进行了相应的XRD,BET,SEM,TEM,FT-IR,PL和UV-vis等性质表征。实验发现我们所制备的g-C_3N_4多孔纳米片对光催化还原CO_2具有较高的催化活性,主要还原产物为CH_4。通过对g-C_3N_4多孔纳米片进行表面改性处理后,可进一步提高其对CO_2的光催化还原性能,借助光电化学等技术详细研究了g-C_3N4表面改性对光催化性能提高的影响机制。
Photocatalytic reduction of CO_2 into CH_4, CH_3OH and other value-added chemicals has the merits of environment-friendly, mild reaction conditions, low-energy consumption, etc. Since Inoue reported the reduction of CO_2 in the presence of photosensitive semiconductors as the catalysts in 1979, photocatalytic reduction of CO_2 has drawn great attention. Similar to the graphite, g-C_3N_4 has a layered structure and shows great potential as visible light photocatalyst material in solar energy conversion and degradation of environmental pollutants by virtue of its high stability, unique electronic band structure, low cost and easy synthesis. Here we report the preparation of g-C_3N_4 porous nanosheets by annealing urea precursor, which have shown high photocatalytic activity for CO_2 reduction, the main product is CH_4. The g-C_3N_4 porous nanosheets exhibit enhanced photocatalytic activity in CO_2 reduction after surface treatment. The possible influence mechanism of surface modification on CO_2 reduction is also investigated by using different approaches like photoelectrochemistry.
引文
[1]Inoue,T.;Fujishima,A.;Konishi,S.;Honda,K.Nature 1979,277:637.
    [2]Ehsan,M.F.;He,T.Appl.Catal.B 2015,166-167:345.
    [3]Wang,X.C.;Maeda,K.;Thomas,A.;Takanabe,K.;Xin,G.;Carlsson J.M.;Domen,K.;Antonietti,M.Nat.Mater.2009,8:76.
    [4]Huang,Y.;Wang Y.J.;Bi,Y.Q.;Jin,J.R.;Ehsan,M.F.;Fu,M.;T.He,RSC Adv.2015,5:33254.

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