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化学进展 2019, Vol. 31 Issue (8): 1086-1102 DOI: 10.7536/PC190117 前一篇   后一篇

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二硫化钼基复合材料的合成及光催化降解与产氢特性

吴正颖1, 刘谢1, 刘劲松2,**(), 刘守清1, 查振龙1, 陈志刚1,**()   

  1. 1. 苏州科技大学 化学生物与材料工程学院 江苏省环境功能材料重点实验室 苏州 215009
    2. 南京航空航天大学 材料科学与技术学院 南京 211106
  • 收稿日期:2019-01-12 出版日期:2019-08-15 发布日期:2019-05-30
  • 通讯作者: 刘劲松, 陈志刚
  • 基金资助:
    国家自然科学基金项目(51478285); 江苏省自然科学基金项目(BK20151198); 苏州市科技发展计划项目(SYG201818); 中央高校基本科研业务费专项资金(NS2017038)
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Molybdenum Disulfide Based Composites and Their Photocatalytic Degradation and Hydrogen Evolution Properties

Zhengying Wu1, Xie Liu1, Jinsong Liu2,**(), Shouqing Liu1, Zhenlong Zha1, Zhigang Chen1,**()   

  1. 1. Jiangsu Key Laboratory for Environment Functional Materials, School of Chemistry, Biology and Material Engineering, Suzhou University of Science and Technology, Suzhou 215009, China
    2. College of Material Science and Technology, Nanjing University of Aeronautics and Astronautics, Nanjing 211106, China
  • Received:2019-01-12 Online:2019-08-15 Published:2019-05-30
  • Contact: Jinsong Liu, Zhigang Chen
  • About author:
    ** E-mail: (Jinsong Liu)
    (Zhigang Chen)
  • Supported by:
    National Natural Science Foundation of China(51478285); Natural Science Foundation of Jiangsu Province(BK20151198); Science and Technology Development Project of Suzhou(SYG201818); Fundamental Research Funds for the Central Universities(NS2017038)

随着环境污染和能源短缺的加剧,无污染环境修复技术及清洁能源替代工程已成为一项重要而紧迫的任务。作为层状结构的过渡金属硫化物,二硫化钼带隙较窄,边缘具有高的反应活性,容易与其他物质形成复合结构,是近年来光催化环境修复及清洁能源领域的研究热点。本文详细介绍了半导体二硫化钼及其复合物的合成方法和光催化降解与产氢行为,重点阐述了二硫化钼及其复合物的具体复合方式、光催化降解污染物活性、光催化产氢活性以及具体的降解与产氢机理等方面的内容,并举例说明。二硫化钼及其复合物在光催化降解污染物和光催化产氢方面具有绿色、廉价、高效等优点,在环境修复及清洁能源领域具有巨大的潜力和应用发展前景。

关键词： 二硫化钼基复合物, 光催化降解, 光催化产氢, 催化机理

With the gradual aggravation of environmental pollution and energy shortage, both developing technology on non-pollution environmental restoration and exploring project on alternative clean energy have recently become a very important and quite urgent task. As one of the transition metal sulfides with layered structures similar to graphene, molybdenum disulfide(MoS2) has become a research hotspot in the field of photocatalytic environmental remediation and clean energy(hydrogen generation) due to its narrow band gap, high reaction activity of the edges, and ease of forming a composite structure with other substances. This paper mainly introduces the synthesis methods, photocatalytic degradation and hydrogen generation behaviors of the MoS2 and its composites. Detailed methodologies for the synthesis of semiconductor MoS2 and its composites, photocatalytic degradation activity of pollutants, photocatalytic hydrogen generation activity and the corresponding mechanisms are emphasized and illustrated by a great many of the typical examples. MoS2 and its composites have displayed many advantages including environment friendliness, low cost and high efficiency in photocatalytic degradation of pollutants and photocatalytic hydrogen production. As the bright future materials, MoS2 and its composites have a broad application prospect in the field of environmental restoration and clean energy with the further development of its general mechanism.

Key words: molybdenum disulfide based composites, photocatalytic degradation, photocatalytic hydrogen evdution, catalytic mechanism
()
图1 (a)半导体光催化过程机理[14],(b)二硫化钼的三种晶体结构[15],(c)二硫化钼本体和单层的能带结构[15]
Fig. 1 (a) Schematic illustration of basic mechanism of a semiconductor photocatalytic process[14],(b) three crystal structures of molybdenum disulfide[15],(c) band structures for bulk and monolayer MoS2[15]
图2 不同半导体的导带和价带位置
Fig. 2 Conductor band and valence band positions of different semiconductors
图3 (a)花状MoS2微球的SEM图[21],(b)花状MoS2纳米微球的SEM图[22],(c)MoS2纳米片的TEM图[23],(d)无定形球状MoS2的TEM图[24]
Fig. 3 (a) SEM image of flower-like MoS2 microsphere[21],(b) SEM image of flower-like MoS2 spheres[22],(c) TEM image of MoS2 nanosheets[23], and(d) TEM image of amorphous spherical MoS2[24]
图4 (a)少层MoS2包覆TiO2纳米带的TiO2@MoS2异质结构SEM图[27],(b)MoS2@TiO2异质结构SEM图[35],(c)TiO2@MoS2异质结构SEM图[35], (d)MoS2@SnO2复合物的SEM图[42], (e)MoS2/MoOx异质结构的SEM图[44], (f)MoS2/BiVO4复合物异质结构的SEM图[48]和(g)少层MoS2/BiOBr空心微球的TEM图[49]
Fig. 4 (a) SEM image of MoS2 thin layer coated with TiO2 nanobelt TiO2@MoS2 heterostructure[27],(b) SEM image of MoS2@TiO2 heterostructure[35],(c) SEM image of TiO2@MoS2 heterostructure[35],(d) SEM image of MoS2@SnO2 complex[42],(e) SEM image of heterogeneous structured MoS2/MoO4[44],(f) SEM image of heterogeneous structured MoS2/BiVO4 composite[48],(g) TEM image of low layer MoS2/BiOBr hollow microsphere[49]
图5 (a)CdS/MoS2异质结构的SEM图[51],(b)MoS2/还原氧化石墨烯rGO复合物的TEM图[36],(c)Z-scheme结构的Ag3PO4/MoS2复合物示意图[76],(d)Ag3PO4/MoS2复合物TEM图[78]
Fig. 5 (a) SEM image of heterogeneous structured CdS/MoS2[51],(b) TEM image of MoS2/reduced graphene(rGO) composite[36],(c) schematic diagram of Ag3PO4/MoS2 composite in the Z-scheme structure[76],(d) TEM image of Ag3PO4/MoS2 composite[78]
图6 (a)叶片状MoS2对MO的降解,(b)叶片状MoS2的光催化稳定性[23]
Fig. 6 (a) Degradation of MO by leaf-shaped MoS2 and (b) photocatalytic stability of the leaf-shaped MoS2[23]
图7 不同复合材料对MB的降解效率:(a)MoS2/ZnO异质结[38](b)MoS2/SnO2纳米花[42],(c)MoS2/BiVO4纳米花[48],(d)MoS2/CdS异质结[51]
Fig. 7 Degradation efficiency to MB by different composites:(a) MoS2/ZnO heterojunction[38],(b) MoS2/SnO2[42],(c) MoS2/BiVO4[48], and(d) MoS2/CdS heterojunction[51]
图8 不同样品对RhB的降解效率:(a)MoS2/MoOx异质结纳米片对RhB的降解[21],(b)MoS2/BiOBr空心微球对RhB的降解[49],(c)TiO2/MoS2核-壳异质结对RhB的降解[26],(d)CdS/MoS2异质结对RhB的降解[51]
Fig. 8 Degradation efficiency to RhB by different composites:(a) MoS2/MoOx heterojunction nanosheets[21],(b) MoS2/BiOBr hollow microspheres[49],(c) TiO2/MoS2 core-shell heterojunctions[26], and (d) CdS/MoS2 heterojunctions[51]
图9 不同样品的产氢速率:(a)TiO2@MoS2异质结构[30],(b)MoS2纳米片包覆ZnO异质结构[39],(c)MoS2-CdS光催化剂[55],(d)MoS2纳米片/CdS纳米棒异质结构[90]
Fig. 9 Hydrogen production rates of different samples:(a) TiO2@MoS2 heterostructure[30],(b) MoS2 nanosheet-coated ZnO heterostructure[39],(c) MoS2-CdS photocatalyst[55], and(d) MoS2 nanosheet/CdS nanorod heterostructure[90]
图10 不同样品的产氢速率:(a)CuS2-TiO2[62],(b)MoS2/ZnIn2S4异质结构[66],(c)三元复合物Sm2O3@Co1-xS/MoS2催化剂[64],(d)Ag/MoS2纳米复合材料[92]
Fig. 10 Hydrogen production rates of different samples:(a) CuS2-TiO2[62],(b) MoS2/ZnIn2S4 heterostructure[66],(c) Sm2O3@Co1-xS/MoS2 photocatalyst[64], and(d) Ag/MoS2 nanocomposite[92]
图11 不同样品的产氢速率:(a)Au纳米粒子负载的MoS2/RGO复合物[75],(b)CQDs/MoS2复合物[71],(c)MoS2/空心HCNS球[82],(d)MoS2 QDs/UiO-66-NH2/G复合材料[85]
Fig. 11 Hydrogen production rates of different samples:(a) Au nanoparticle-supported MoS2/RGO composite[75],(b) CQDs/MoS2 composite [71],(c) MoS2/HCNS hollow sphere[82], and(d) MoS2 QDs/UiO-66-NH2/G composite[85]
图12 (a)MoS2沿(002)方向生长示意图[22],(b)Bi2O3/Bi2S3/MoS2异质结的降解机理图,(c)MoS2/MoOx异质结的降解机理图[44],(d)MoS2/Bi2MoO6复合物的降解机理图,(e)N-TiO2-x@MoS2核壳结构的降解机理图,(f)Ag3PO4/MoS2异质结的降解机理图,(g)MoS2/C3N4异质结构的降解机理图[80]
Fig. 12 (a) Schematic diagram of MoS2 grows along(002) direction[22],(b) degradation mechanism of Bi2O3/Bi2S3/MoS2 heterostructure,(c) degradation mechanism of MoS2/MoOx heterostructure[44],(d) degradation mechanism of MoS2/Bi2MoO6 composite,(e) degradation mechanism of N-TiO2-x@MoS2 nuclear shell structure,(f) degradation mechanism of Ag3PO4/MoS2 heterojunction,(g) degradation mechanism of MoS2/C3N4 heterojunction[80]
图13 不同样品的产氢机理:(a)MoS2在基片上垂直排列[32],(b)金属性MoS2与ZnO之间形成紧密界面[39],(c)形成空间电荷区[92],(d)表面等离子体共振效应机理[75],(e)TiO2导带电子转移到MoS2[30],(f)电子从MoS2导带转移到ZnO导带[41],(g)传统Ⅱ型异质结[31],(h)敏化作用[64],(i)Z-scheme结构[84]
Fig. 13 Hydrogen production mechanism of different samples:(a) vertical MoS2 on the substrate[32],(b) a compact interface between metallic MoS2 and ZnO[39],(c) space charge region[92],(d) surface plasmon resonance effect[75],(e) electrons transfer from TiO2to MoS2[30],(f) electrons transfer from MoS2to ZnO[41],(g) traditional type Ⅱ heterojunction[31],(h) sensitization effect[64],(i) Z-scheme structure[84]
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