Low-Molecular-Weight Carbon Nitrides for Solar Hydrogen Evolution

被引:342
作者
Lau, Vincent Wing-hei [1 ,3 ]
Mesch, Maria B. [2 ]
Duppel, Viola [1 ,3 ]
Blum, Volker [4 ,5 ]
Senker, Juergen [2 ]
Lotsch, Bettina V. [1 ,3 ,6 ,7 ]
机构
[1] Max Planck Inst Solid State Res, D-70569 Stuttgart, Germany
[2] Univ Bayreuth, Dept Inorgan Chem 3, D-95447 Bayreuth, Germany
[3] Univ Munich, Dept Chem, D-81377 Munich, Germany
[4] Duke Univ, Dept Mech Engn & Mat Sci, Durham, NC 27708 USA
[5] Duke Univ, Ctr Mat Genom, Durham, NC 27708 USA
[6] NIM, D-80799 Munich, Germany
[7] Ctr Nanosci, D-80799 Munich, Germany
关键词
SOLID-STATE NMR; PHOTOCATALYTIC ACTIVITY; ELECTRON-DIFFRACTION; THERMAL CONDENSATION; LIGHT; WATER; MELEM; NANOPARTICLES; SEMICONDUCTORS; PLATINUM;
D O I
10.1021/ja511802c
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
This work focuses on the control of the polymerization process for melon (graphitic carbon nitride), with the aim of improving its photocatalytic activity intrinsically. We demonstrate here that reduction of the synthesis temperature leads to a mixture of the monomer melem and its higher condensates. We show that this mixture can be separated and provide evidence that the higher condensates are isolated oligomers of melem. On evaluating their photocatalytic activity for hydrogen evolution, the oligomers were found to be the most active species, having up to twice the activity of the monomer/oligomer mixture of the as-synthesized material, which in turn has 3 times the activity of the polymer melon, the literature benchmark. These results highlight the role of defects, i.e., chain terminations, in increasing the catalytic activity of carbon nitrides and at the same time point to the ample potential of intrinsically improving the photocatalytic activity of carbon nitride, especially through the selective synthesis of the active phase.
引用
收藏
页码:1064 / 1072
页数:9
相关论文
共 80 条
  • [21] Ishii A, 2007, PHOTOCH PHOTOBIO SCI, V6, P804, DOI 10.1039/b703751c
  • [22] Promotion of atomic hydrogen recombination as an alternative to electron trapping for the role of metals in the photocatalytic production of H2
    Joo, Ji Bong
    Dillon, Robert
    Lee, Ilkeun
    Yin, Yadong
    Bardeen, Christopher J.
    Zaera, Francisco
    [J]. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2014, 111 (22) : 7942 - 7947
  • [23] Melem (2,5,8-triamino-tri-s-triazine), an important intermediate during condensation of melamine rings to graphitic carbon nitride:: Synthesis, structure determination by X-ray powder diffractometry, solid-state NMR, and theoretical studies
    Jürgens, B
    Irran, E
    Senker, J
    Kroll, P
    Müller, H
    Schnick, W
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2003, 125 (34) : 10288 - 10300
  • [24] Organic-inorganic composite of g-C3N4-SrTiO3:Rh photocatalyst for improved H2 evolution under visible light irradiation
    Kang, Hyun Woo
    Lim, Sung Nam
    Song, Dongsu
    Park, Seung Bin
    [J]. INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2012, 37 (16) : 11602 - 11610
  • [25] Highly efficient water splitting into H2 and O2 over lanthanum-doped NaTaO3 photocatalysts with high crystallinity and surface nanostructure
    Kato, H
    Asakura, K
    Kudo, A
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2003, 125 (10) : 3082 - 3089
  • [26] Attempted chemical synthesis of graphite-like carbon nitride
    Komatsu, T
    [J]. JOURNAL OF MATERIALS CHEMISTRY, 2001, 11 (03) : 799 - 801
  • [27] Komatsu T, 2001, MACROMOL CHEM PHYSIC, V202, P19, DOI 10.1002/1521-3935(20010101)202:1<19::AID-MACP19>3.0.CO
  • [28] 2-G
  • [29] Bandgap modulation of TiO2 and its effect on the activity in photocatalytic oxidation of 2-isopropyl-6-methyl-4-pyrimidinol
    Lee, HS
    Woo, CS
    Youn, BK
    Kim, SY
    Oh, ST
    Sung, YE
    Lee, HI
    [J]. TOPICS IN CATALYSIS, 2005, 35 (3-4) : 255 - 260
  • [30] Condensed Graphitic Carbon Nitride Nanorods by Nanoconfinement: Promotion of Crystallinity on Photocatalytic Conversion
    Li, Xin-Hao
    Zhang, Jinshui
    Chen, Xiufang
    Fischer, Anna
    Thomas, Arne
    Antonietti, Markus
    Wang, Xinchen
    [J]. CHEMISTRY OF MATERIALS, 2011, 23 (19) : 4344 - 4348