化工进展 ›› 2019, Vol. 38 ›› Issue (07): 3207-3226.DOI: 10.16085/j.issn.1000-6613.2018-1858
收稿日期:
2018-09-14
出版日期:
2019-07-05
发布日期:
2019-07-05
作者简介:
张晓(1991—),女,硕士,助理工程师,研究方向为金属-有机框架材料、金属氧化物材料及其催化性能。E-mail:<email>zhangxiao@grinm.com</email>。
Xiao ZHANG(),Yaohua XU,Hao LIU,Feng WEI,Peng YUAN
Received:
2018-09-14
Online:
2019-07-05
Published:
2019-07-05
摘要:
金属氧化物型半导体气体传感器是目前常用的乙醇检测手段,深入研究和改进金属氧化物型半导体材料是提升传感器性能的重要方式。本文首先论述了气敏检测的机理和影响因素,并综述了近年来发展的主要金属氧化物型半导体气敏材料,重点介绍了不同微观结构的Co3O4、ZnO、SnO2及掺杂金属氧化物材料、氧化物异质结等的研究和发展情况,对它们的合成方法、结构特点以及结构与乙醇气敏性能之间的关系进行了探讨。分析表明,减小材料颗粒尺寸、构建大比表面积多孔结构、掺杂和复合改性,是提升金属氧化物材料气敏性能的有效措施。此外,基于传感器微小化的趋势,以微机电系统(MEMS)工艺为基础的微型传感器成为气体传感器的发展趋势。然而,目前针对金属氧化物气敏材料的制备依然缺乏一定的理论指导,气体检测缺乏相应的机理研究,亟需物理、化学、材料等多学科的相互结合,促进乙醇等半导体气体传感器的进一步发展。
中图分类号:
张晓, 徐瑶华, 刘皓, 魏峰, 苑鹏. 基于金属氧化物的乙醇检测气敏材料的研究进展[J]. 化工进展, 2019, 38(07): 3207-3226.
Xiao ZHANG, Yaohua XU, Hao LIU, Feng WEI, Peng YUAN. Recent advances of ethanol detection materials based on metal oxides[J]. Chemical Industry and Engineering Progress, 2019, 38(07): 3207-3226.
材料 | 形貌 | 材料 | 温度/℃ | 检测浓度 /μg?g-1 | 响应度 | 响应/恢复(时间)/s | 选择性(响应度) | 参考文献 | |||
---|---|---|---|---|---|---|---|---|---|---|---|
甲醇 | 甲醛 | 丙酮 | 氢气 | ||||||||
零维材料 | 立方颗粒 | Co3O4 | 200 | 100 | 5.0 | 无 | 3.0 | [ | |||
团聚颗粒 | Co3O4 | 300 | 100 | 5.5 | 150/55 | 5.1 | [ | ||||
纳米颗粒 | ZnO | 350 | 400 | 20.3 | 12/14 | 无 | [ | ||||
立方颗粒 | In2O3 | 200 | 100 | 17.0 | 无 | 5.0 | [ | ||||
一维材料 | 纳米纤维 | SnO2 | 330 | 10 | 4.5 | 13/13.9 | 无 | [ | |||
纳米线 | SnO2 | 380 | 100 | 17.0 | 22/18 | 无 | [ | ||||
纳米棒 | ZnO | 400 | 100 | 149.2 | 9/15 | 无 | [ | ||||
纳米线 | Co3O4 | 350 | 300 | 5.1 | 无 | 无 | [ | ||||
纳米棒 | Co3O4 | 160 | 500 | 71.0 | 90/60 | 38.8 | 20.1 | [ | |||
纳米棒 | Co3O4 | 300 | 100 | 25.7 | 29/13 | 20.1 | [ | ||||
纳米管 | Co3O4 | 300 | 100 | 24.7 | 49/13 | 26.3 | [ | ||||
纳米纤维 | TiO2 | 300 | 100 | 14.0 | 3/5 | 3.5 | [ | ||||
二维材料 | 纳米片 | ZnO | 350 | 400 | 23.3 | 12/5 | 无 | [ | |||
纳米片 | Co3O4 | 100 | 300 | 419.0 | 44/328 | 94.0 | 36.4 | 234.0 | [ | ||
纳米片 | Co3O4 | 300 | 100 | 57.5 | 66/10 | 56.0 | [ | ||||
层状结构 | CuO | 250 | 5 | 3.1 | 11.9/8.4 | 3.0 | 1.6 | 2.5 | [ | ||
三维材料 | 分级结构 | SnO2 | 350 | 100 | 10.5 | 5 | 无 | [ | |||
介孔材料 | SnO2 | 225 | 100 | 17.3 | 8/780 | 2.5 | 2.5 | 3.0 | [ | ||
分级多孔 | SnO2 | 240 | 500 | 72.0 | 10/15 | 12.0 | 9.0 | 7.0 | [ | ||
(20μg?g-1) | |||||||||||
空心笼状 | ZnO | 300 | 1 | 8.0 | 无 | 14.8 | [ | ||||
介孔材料 | ZnO | 室温 | 300 | 1.4 | 42/40 | 无 | [ | ||||
分级多孔 | ZnO | 250 | 50 | 36.6 | 14/8 | 3.0 | [ | ||||
分级多孔 | ZnO | 220 | 100 | 8.5 | 10/80 | 5.0 | [ | ||||
分级结构 | ZnO | 370 | 100 | 340.0 | 12/约50 | 362.0 | [ | ||||
分级结构 | ZnO | 260 | 50 | 110.0 | 4/12 | 12.0 | 40.0 | 2.0 | [ | ||
纳米花 | ZnO | 350 | 400 | 30.4 | 10/4 | 无 | [ | ||||
三维微孔 | Co3O4@C | 170 | 100 | 14.7 | 无 | 11.0 | 7.8 | [ | |||
三维介孔 | Co3O4@CF | 320 | 100 | 4.2 | 44/31 | 无 | [ | ||||
介孔纳米片 | Co3O4/NCF | 100 | 100 | 10.4 | 45/140 | 1.7 | 1.6 | 1.3 | [ | ||
薄膜 | 薄膜 | SnO2 | 300 | 300 | 1.84 | 8/340 | 70.0 | [ | |||
薄膜 | ZnO | 室温 | 30 | 6.0 | 28/49 | 5.1 (10μg?g-1) | [ | ||||
薄膜 | ZnO | 400 | 50 | 55.0 | 362/147 | 无 | [ | ||||
阵列 | Co3O4 | 130 | 100 | 89.6 | 无 | 25.8 | 55.2 | [ | |||
薄膜 | CuO | 室温 | 200 | 1.24 | 15/15 | 无 | [ |
表1 不同形貌MO x 乙醇性能对比
材料 | 形貌 | 材料 | 温度/℃ | 检测浓度 /μg?g-1 | 响应度 | 响应/恢复(时间)/s | 选择性(响应度) | 参考文献 | |||
---|---|---|---|---|---|---|---|---|---|---|---|
甲醇 | 甲醛 | 丙酮 | 氢气 | ||||||||
零维材料 | 立方颗粒 | Co3O4 | 200 | 100 | 5.0 | 无 | 3.0 | [ | |||
团聚颗粒 | Co3O4 | 300 | 100 | 5.5 | 150/55 | 5.1 | [ | ||||
纳米颗粒 | ZnO | 350 | 400 | 20.3 | 12/14 | 无 | [ | ||||
立方颗粒 | In2O3 | 200 | 100 | 17.0 | 无 | 5.0 | [ | ||||
一维材料 | 纳米纤维 | SnO2 | 330 | 10 | 4.5 | 13/13.9 | 无 | [ | |||
纳米线 | SnO2 | 380 | 100 | 17.0 | 22/18 | 无 | [ | ||||
纳米棒 | ZnO | 400 | 100 | 149.2 | 9/15 | 无 | [ | ||||
纳米线 | Co3O4 | 350 | 300 | 5.1 | 无 | 无 | [ | ||||
纳米棒 | Co3O4 | 160 | 500 | 71.0 | 90/60 | 38.8 | 20.1 | [ | |||
纳米棒 | Co3O4 | 300 | 100 | 25.7 | 29/13 | 20.1 | [ | ||||
纳米管 | Co3O4 | 300 | 100 | 24.7 | 49/13 | 26.3 | [ | ||||
纳米纤维 | TiO2 | 300 | 100 | 14.0 | 3/5 | 3.5 | [ | ||||
二维材料 | 纳米片 | ZnO | 350 | 400 | 23.3 | 12/5 | 无 | [ | |||
纳米片 | Co3O4 | 100 | 300 | 419.0 | 44/328 | 94.0 | 36.4 | 234.0 | [ | ||
纳米片 | Co3O4 | 300 | 100 | 57.5 | 66/10 | 56.0 | [ | ||||
层状结构 | CuO | 250 | 5 | 3.1 | 11.9/8.4 | 3.0 | 1.6 | 2.5 | [ | ||
三维材料 | 分级结构 | SnO2 | 350 | 100 | 10.5 | 5 | 无 | [ | |||
介孔材料 | SnO2 | 225 | 100 | 17.3 | 8/780 | 2.5 | 2.5 | 3.0 | [ | ||
分级多孔 | SnO2 | 240 | 500 | 72.0 | 10/15 | 12.0 | 9.0 | 7.0 | [ | ||
(20μg?g-1) | |||||||||||
空心笼状 | ZnO | 300 | 1 | 8.0 | 无 | 14.8 | [ | ||||
介孔材料 | ZnO | 室温 | 300 | 1.4 | 42/40 | 无 | [ | ||||
分级多孔 | ZnO | 250 | 50 | 36.6 | 14/8 | 3.0 | [ | ||||
分级多孔 | ZnO | 220 | 100 | 8.5 | 10/80 | 5.0 | [ | ||||
分级结构 | ZnO | 370 | 100 | 340.0 | 12/约50 | 362.0 | [ | ||||
分级结构 | ZnO | 260 | 50 | 110.0 | 4/12 | 12.0 | 40.0 | 2.0 | [ | ||
纳米花 | ZnO | 350 | 400 | 30.4 | 10/4 | 无 | [ | ||||
三维微孔 | Co3O4@C | 170 | 100 | 14.7 | 无 | 11.0 | 7.8 | [ | |||
三维介孔 | Co3O4@CF | 320 | 100 | 4.2 | 44/31 | 无 | [ | ||||
介孔纳米片 | Co3O4/NCF | 100 | 100 | 10.4 | 45/140 | 1.7 | 1.6 | 1.3 | [ | ||
薄膜 | 薄膜 | SnO2 | 300 | 300 | 1.84 | 8/340 | 70.0 | [ | |||
薄膜 | ZnO | 室温 | 30 | 6.0 | 28/49 | 5.1 (10μg?g-1) | [ | ||||
薄膜 | ZnO | 400 | 50 | 55.0 | 362/147 | 无 | [ | ||||
阵列 | Co3O4 | 130 | 100 | 89.6 | 无 | 25.8 | 55.2 | [ | |||
薄膜 | CuO | 室温 | 200 | 1.24 | 15/15 | 无 | [ |
掺杂物 | 形貌 | 材料 | 温度 /℃ | 检测浓度 /μg?g-1 | 响应度 | 响应/恢复(时间)/s | 选择性(响应度) | 参考 文献 | |||
---|---|---|---|---|---|---|---|---|---|---|---|
甲醇 | 甲醛 | 丙酮 | 氨气 | ||||||||
贵金属 | 中空纳米球 | Pt-SnO2 | 325 | 5 | 1399.9 | 1/525 | 600.0 | 700.0 | 200 | [ | |
纳米棒 | Pt-SnO2 | 320 | 200 | 8.3 | 3~5/5~15 | 无 | [ | ||||
纳米颗粒 | Pt-SnO2 | 275 | 100 | 1.9 | 1/5 | 无 | [ | ||||
空心材料 | Pd-SnO2 | 300 | 50 | 2.0 | 1.5/18 | 0.9 | 0.9 | 1.0 | [ | ||
纳米花 | Au-SnO2 | 340 | 150 | 29.3 | 5/10 | 13.3 | 20.3 | [ | |||
(100μg·g-1) | |||||||||||
薄膜 | Pt-In2O3 | 室温 | 0.095 | 12.2 | 1/2 | 无 | [ | ||||
纳米颗粒 | Pt-In2O3 | 250 | 100 | 32.6 | 2.2/0.7 | 4.0 | [ | ||||
纳米片 | Au-WO3 | 320 | 100 | 97.2 | 无 | 8.0 | 3.0 | 11.0 | [ | ||
非贵金属 | 纳米颗粒 | CuZn-SnO2 | 110 | 50 | 210.0 | 无 | 10.0 | [ | |||
纳米棒 | Ni-SnO2 | 450 | 50 | 2000.0 | 30/600 | 无 | [ | ||||
纳米微球 | Ni-SnO2 | 260 | 100 | 28.9 | 11/54 | 6.0 | 4.0 | [ | |||
纳米颗粒 | Ce-SnO2 | 室温 | 400 | 4.8 | 2~25/30~60 | 无 | [ | ||||
立方中空 | ZnSnO3 | 260 | 100 | 34.1 | 2/276 | 11.0 | 3 | [ | |||
纳米棒 | Cr-ZnO | 300 | 400 | 45.0 | 无 | 无 | [ | ||||
海绵状 | Co-ZnO | 220 | 100 | 120.0 | 10/5 | 18.0 | 24.0 | [ | |||
六边形 | Cr-Co3O4 | 300 | 100 | 28.9 | 1/7 | 4.0 | 3.0 | [ | |||
纳米球 | Co3O4/pCNH | 210 | 500 | 30.2 | 无 | 2.0 | 7.0 | [ |
表2 不同金属掺杂MO x 性能对比
掺杂物 | 形貌 | 材料 | 温度 /℃ | 检测浓度 /μg?g-1 | 响应度 | 响应/恢复(时间)/s | 选择性(响应度) | 参考 文献 | |||
---|---|---|---|---|---|---|---|---|---|---|---|
甲醇 | 甲醛 | 丙酮 | 氨气 | ||||||||
贵金属 | 中空纳米球 | Pt-SnO2 | 325 | 5 | 1399.9 | 1/525 | 600.0 | 700.0 | 200 | [ | |
纳米棒 | Pt-SnO2 | 320 | 200 | 8.3 | 3~5/5~15 | 无 | [ | ||||
纳米颗粒 | Pt-SnO2 | 275 | 100 | 1.9 | 1/5 | 无 | [ | ||||
空心材料 | Pd-SnO2 | 300 | 50 | 2.0 | 1.5/18 | 0.9 | 0.9 | 1.0 | [ | ||
纳米花 | Au-SnO2 | 340 | 150 | 29.3 | 5/10 | 13.3 | 20.3 | [ | |||
(100μg·g-1) | |||||||||||
薄膜 | Pt-In2O3 | 室温 | 0.095 | 12.2 | 1/2 | 无 | [ | ||||
纳米颗粒 | Pt-In2O3 | 250 | 100 | 32.6 | 2.2/0.7 | 4.0 | [ | ||||
纳米片 | Au-WO3 | 320 | 100 | 97.2 | 无 | 8.0 | 3.0 | 11.0 | [ | ||
非贵金属 | 纳米颗粒 | CuZn-SnO2 | 110 | 50 | 210.0 | 无 | 10.0 | [ | |||
纳米棒 | Ni-SnO2 | 450 | 50 | 2000.0 | 30/600 | 无 | [ | ||||
纳米微球 | Ni-SnO2 | 260 | 100 | 28.9 | 11/54 | 6.0 | 4.0 | [ | |||
纳米颗粒 | Ce-SnO2 | 室温 | 400 | 4.8 | 2~25/30~60 | 无 | [ | ||||
立方中空 | ZnSnO3 | 260 | 100 | 34.1 | 2/276 | 11.0 | 3 | [ | |||
纳米棒 | Cr-ZnO | 300 | 400 | 45.0 | 无 | 无 | [ | ||||
海绵状 | Co-ZnO | 220 | 100 | 120.0 | 10/5 | 18.0 | 24.0 | [ | |||
六边形 | Cr-Co3O4 | 300 | 100 | 28.9 | 1/7 | 4.0 | 3.0 | [ | |||
纳米球 | Co3O4/pCNH | 210 | 500 | 30.2 | 无 | 2.0 | 7.0 | [ |
异质结 | 材料 | 温度/℃ | 检测浓度/μg?g-1 | 响应度 | 响应/恢复时间/s | 选择性(响应度) | 参考 文献 | |||
---|---|---|---|---|---|---|---|---|---|---|
甲醇 | 甲醛 | 丙酮 | 氨气 | |||||||
MO x -MO x | ZnO/SnO2 | 225 | 30 | 34.8 | 1/120 | 53.7 | 8.9 | 52.1 | [ | |
(100μg?g-1, 此时乙醇响应度为78.2) | ||||||||||
NiO/SnO2 | 250 | 100 | 7.9 | 15/100 | 无 | [ | ||||
Fe2O3/SnO2 | 300 | 200 | 57.6 | 无 | 20.0 | 15.0 | 35.0 | [ | ||
CoO/SnO2 | 250 | 100 | 145.0 | 无 | 56.0 | 15.0 | 54.0 | [ | ||
SnO2/ZnO | 350 | 100 | 13.3 | 无 | 4.0 | 4.0 | 1.4 | [ | ||
SnO2/Fe2O3 | 260 | 100 | 41.7 | 3/4 | 9.0 | 5.0 | [ | |||
SnO2/Fe2O3 | 240 | 100 | 5.9 | 1/5 | 1.0 | 2.5 | 1.5 | [ | ||
ZnO/CuO | 300 | 10 | 2.2 | 22/26 | 1.2 | 0.7 | [ | |||
ZnO/Co3O4 | 200 | 1000 | 106.0 | 7/236 | 无 | [ | ||||
LaMnO3/ZnO | 300 | 50 | 6.0 | 8/17 | 无 | [ | ||||
CuO/ZnO | 320 | 200 | 97.0 | 5/25 | 57.0 | 20.0 | [ | |||
CdO/ZnO | 250 | 100 | 65.5 | 2/136 | 10.0 | 9.0 | 15.0 | [ | ||
CdO/Mn-ZnO | 340 | 20 | 11.4 | 11.4/12.4 | 2.0 | 1.2 | [ | |||
α-Fe2O3/ZnO/Au | 280 | 100 | 170.0 | 4/5 | 无 | [ | ||||
MoO3/WO3 | 320 | 100 | 28.5 | 13/10 | 18.2 | [ | ||||
Cr2O3/WO3 | 300 | 200 | 5.6 | 约46/57 | 4.1 | [ | ||||
MoO3/In2O3 | 185 | 100 | 7.0 | 11/94 | 2.5 | [ | ||||
有机材料&石墨烯/MO x | PANI/TiO2 | 室温 | 200 | 约47.0 | 115/340 | 无 | [ | |||
Zn2SnO4/rGO | 275 | 100 | 38.0 | 11/18 | 15.0 | 3.5 | 16 | [ | ||
rGO-SnO2 | 300 | 100 | 70.4 | 11/ | 42.0 | 13 | [ | |||
Fe3O4/rGO | 400 | 100 | 9.0 | 3/138 | 1.100 | [ | ||||
TiO2[/多孔硅 | 150 | 100 | 1.4 | 无 | 1.03 | [ |
表3 不同异质结MO x 性能对比
异质结 | 材料 | 温度/℃ | 检测浓度/μg?g-1 | 响应度 | 响应/恢复时间/s | 选择性(响应度) | 参考 文献 | |||
---|---|---|---|---|---|---|---|---|---|---|
甲醇 | 甲醛 | 丙酮 | 氨气 | |||||||
MO x -MO x | ZnO/SnO2 | 225 | 30 | 34.8 | 1/120 | 53.7 | 8.9 | 52.1 | [ | |
(100μg?g-1, 此时乙醇响应度为78.2) | ||||||||||
NiO/SnO2 | 250 | 100 | 7.9 | 15/100 | 无 | [ | ||||
Fe2O3/SnO2 | 300 | 200 | 57.6 | 无 | 20.0 | 15.0 | 35.0 | [ | ||
CoO/SnO2 | 250 | 100 | 145.0 | 无 | 56.0 | 15.0 | 54.0 | [ | ||
SnO2/ZnO | 350 | 100 | 13.3 | 无 | 4.0 | 4.0 | 1.4 | [ | ||
SnO2/Fe2O3 | 260 | 100 | 41.7 | 3/4 | 9.0 | 5.0 | [ | |||
SnO2/Fe2O3 | 240 | 100 | 5.9 | 1/5 | 1.0 | 2.5 | 1.5 | [ | ||
ZnO/CuO | 300 | 10 | 2.2 | 22/26 | 1.2 | 0.7 | [ | |||
ZnO/Co3O4 | 200 | 1000 | 106.0 | 7/236 | 无 | [ | ||||
LaMnO3/ZnO | 300 | 50 | 6.0 | 8/17 | 无 | [ | ||||
CuO/ZnO | 320 | 200 | 97.0 | 5/25 | 57.0 | 20.0 | [ | |||
CdO/ZnO | 250 | 100 | 65.5 | 2/136 | 10.0 | 9.0 | 15.0 | [ | ||
CdO/Mn-ZnO | 340 | 20 | 11.4 | 11.4/12.4 | 2.0 | 1.2 | [ | |||
α-Fe2O3/ZnO/Au | 280 | 100 | 170.0 | 4/5 | 无 | [ | ||||
MoO3/WO3 | 320 | 100 | 28.5 | 13/10 | 18.2 | [ | ||||
Cr2O3/WO3 | 300 | 200 | 5.6 | 约46/57 | 4.1 | [ | ||||
MoO3/In2O3 | 185 | 100 | 7.0 | 11/94 | 2.5 | [ | ||||
有机材料&石墨烯/MO x | PANI/TiO2 | 室温 | 200 | 约47.0 | 115/340 | 无 | [ | |||
Zn2SnO4/rGO | 275 | 100 | 38.0 | 11/18 | 15.0 | 3.5 | 16 | [ | ||
rGO-SnO2 | 300 | 100 | 70.4 | 11/ | 42.0 | 13 | [ | |||
Fe3O4/rGO | 400 | 100 | 9.0 | 3/138 | 1.100 | [ | ||||
TiO2[/多孔硅 | 150 | 100 | 1.4 | 无 | 1.03 | [ |
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