中空多壳层结构材料的制备及气体传感应用研究进展

doi:10.7503/cjcu20190688

摘要/Abstract

摘要：

先进气体传感器技术在现代社会安全生产生活中扮演着极为重要的角色, 而高效敏感材料的设计与开发是其中的关键. 中空多壳层结构材料因其独特的层层嵌套的多壳层与多腔体结构而表现出特别的物理化学性质, 在气体传感领域显现出巨大的应用潜力. 传统的硬模板法、软模板法以及基于奥斯特瓦尔德熟化和柯肯德尔效应的无模板法在中空多壳层纳米结构材料的普适制备及壳层结构的精确调控等方面存在诸多限制. 次序模板法的出现突破了上述限制, 促进了该领域的迅速发展. 本文简要回顾了中空多壳层结构材料制备方法的发展历程, 介绍了其在甲醛、乙醇、丙酮、甲苯及二氧化氮等有害气体检测中的具体应用, 分析了其在气体传感领域的独特优势, 最后对该领域面临的挑战和发展前景进行了总结与展望.

关键词: 中空多壳层结构, 金属氧化物半导体, 次序模板法, 气体传感

Abstract:

Advanced gas sensing technology plays a very important role in the safe production and life of modern society, where the keypoint is the design and development of efficient sensing materials. Hollow multi-shell structured materials possess special physical and chemical properties due to their unique structures with both multiple shells and multi spaces and thus great potential in application for gas sensing. The conventional hard template and soft template methods as well as template-free method based on Osterwald ripening or Kirkendall effect have some limitations in the general preparation of hollow multi-shell structured materials and the precise control of the shell structure. The emergence of the sequential template approach greatly broke through the above-mentioned limitations and promoted the rapid development of the field. This paper briefly reviews the development of the preparative method of hollow multi-shell structured materials, introduces their applications in detecting formaldehyde, ethanol, acetone, toluene, nitrogen dioxide and other harmful gases, and analyzes their unique advantages in gas sensing, and finally summarizes and prospects the challenges and prospects.

Key words: Hollow multi-shell structure, Metal oxide semiconductor, Sequential templating approach, Gas sensing

中图分类号:

O614

TrendMD:

孙辉, 赖小勇. 中空多壳层结构材料的制备及气体传感应用研究进展. 高等学校化学学报, 2020, 41(5): 855.

SUN Hui, LAI Xiaoyong. Progress in Preparation and Gas-sensing Application of Hollow Multi-shell Structured Materials ^†. Chem. J. Chinese Universities, 2020, 41(5): 855.

图/表 18

Fig.1 Band bending in a wide bandgap semiconductor after chemisorption of charged species on surface sites[18] EC, EV and EF: conduction band, valence band, and the Fermi level; Λair: thickness of the space-charge layer; eVsurface: potential barrier. Copyright 2006, Wiley VCH.

Table 1 Preparation and property of typical hollow multi-shell structural materials

Year	Composition	Morphology	Shell number	Size/nm	Specific area/ (m²·g^-1)	Preparation characteristics		Ref.
2007	Cu₂O	Sphere	1—4	150—180	—	Vesicle templating		[81]
2007	SnO₂	Sphere	3	1000—2000	36.17	Chemical self-assembly		[82]
2009	MFe₂O₄	Sphere	1—3	1200	109.8	Sequential templating		[70]
	(M=Zn, Co, Ni, Cd)
2010	TiO₂	Sphere	1—4	1300	—	Sequential templating		[69]
2011	ZnO	Sphere	1—4	3500	85	Sequential templating		[83]
2012	WO₃	Sphere	1—3	ca.250	62	Sequential templating		[84]
2013	α-Fe₂O₃	Sphere	1—3	300—3000	17.3	Sequential templating		[85]
2014	Au/CeO₂	Sphere	1—4	300	90	Sequential templating		[86]
2014	Mn₂O₃	Sphere	1—4	500—800	36.55		pH value tuning and	[87]
							sequential templating
2014	Co₃O₄	Sphere	4—6	2600	6.4		Spray drying and	[88]
							sequential templating
2015	Cr₂O₃	Sphere	1—4	1000—3000	65.34		Sequential templating	[89]
2016	V₂O₅	Sphere	1—3	ca. 700	28.32		Sequential templating	[39]
2016	MoO₂/carbon	Sphere	1—4	580—1100	60.9		Solvothermal and	[90]
							sequential templating
2017	MOFs(MIL-101)	Truncated octahedral	1—3	350	1486		Layer-by-layer self-	[79]
							assembly and etching
2017	NiCo₂O₄	Sphere	1—3	200—300	27.91		Sequential templating	[91]
2018	ZnO	Mesoporous sphere	1—3	ca. 1500	20		Hydrothermal and	[92]
							sequential templating
2018	ZnO/ZnFe₂O₄	Sphere	1—3	850—1000	62.4		Sequential templating	[93]
2018	ZnS-CdS	Rhombic dodecahedrons	1—5	ca. 2200	—		MOFs as template and	[94]
							sequential templating
2019	Co₃O₄	Dodecahedron	1—4	ca.2200	—		MOFs as template and	[51]
							sequential templating
2019	CoS	Cube	2—5	800	—		MOFs as template and	[95]
							sequential templating
2019	Co/Mn oxide	Dodecahedra	1—3	2300	84.60		MOFs as template and	[96]
							sequential templating

Table 1 Preparation and property of typical hollow multi-shell structural materials

Year	Composition	Morphology	Shell number	Size/nm	Specific area/ (m²·g^-1)	Preparation characteristics		Ref.
2007	Cu₂O	Sphere	1—4	150—180	—	Vesicle templating		[81]
2007	SnO₂	Sphere	3	1000—2000	36.17	Chemical self-assembly		[82]
2009	MFe₂O₄	Sphere	1—3	1200	109.8	Sequential templating		[70]
	(M=Zn, Co, Ni, Cd)
2010	TiO₂	Sphere	1—4	1300	—	Sequential templating		[69]
2011	ZnO	Sphere	1—4	3500	85	Sequential templating		[83]
2012	WO₃	Sphere	1—3	ca.250	62	Sequential templating		[84]
2013	α-Fe₂O₃	Sphere	1—3	300—3000	17.3	Sequential templating		[85]
2014	Au/CeO₂	Sphere	1—4	300	90	Sequential templating		[86]
2014	Mn₂O₃	Sphere	1—4	500—800	36.55		pH value tuning and	[87]
							sequential templating
2014	Co₃O₄	Sphere	4—6	2600	6.4		Spray drying and	[88]
							sequential templating
2015	Cr₂O₃	Sphere	1—4	1000—3000	65.34		Sequential templating	[89]
2016	V₂O₅	Sphere	1—3	ca. 700	28.32		Sequential templating	[39]
2016	MoO₂/carbon	Sphere	1—4	580—1100	60.9		Solvothermal and	[90]
							sequential templating
2017	MOFs(MIL-101)	Truncated octahedral	1—3	350	1486		Layer-by-layer self-	[79]
							assembly and etching
2017	NiCo₂O₄	Sphere	1—3	200—300	27.91		Sequential templating	[91]
2018	ZnO	Mesoporous sphere	1—3	ca. 1500	20		Hydrothermal and	[92]
							sequential templating
2018	ZnO/ZnFe₂O₄	Sphere	1—3	850—1000	62.4		Sequential templating	[93]
2018	ZnS-CdS	Rhombic dodecahedrons	1—5	ca. 2200	—		MOFs as template and	[94]
							sequential templating
2019	Co₃O₄	Dodecahedron	1—4	ca.2200	—		MOFs as template and	[51]
							sequential templating
2019	CoS	Cube	2—5	800	—		MOFs as template and	[95]
							sequential templating
2019	Co/Mn oxide	Dodecahedra	1—3	2300	84.60		MOFs as template and	[96]
							sequential templating

Fig.7 Illustration of the formation of multi-shelled mesoporous silica hollow nanospheres(A), SEM(B—D) and corresponding TEM(E—G) images prepared with different FC4/F127 molar ratios of 24(B, E), 48(C, F) and 72(D, G)[71] Copyright 2010, Royal Society of Chemistry.

Table 2 Application of hollow multi-shell structural materials in gas-sensing

Year	Composition	Shell number	Gas	Con.^a/ppm	Response	T^b/℃	$T Res. c$ /s	$T Rec. d$ /s	DL^e/ppm	Ref.
2009	Cu₇S₄	2	NH₃	481	—	25	89	48	127	[120]
2011	ZnO	3	Toluene	20	3.09	300	0.3	3	1	[121]
2011	α-Fe₂O₃	3	Ethanol	10	9	—	—	—	—	[106]
2013	ZnO	3	HCHO	5	5.2	240	1—3	2—4	5	[118]
2014	SnO₂/α-Fe₂O₃	2	Ethanol	10	ca.3.1	250	1	14	10	[122]
2015	Cr₂O₃	4	Ethanol	5	10.1	370	—	—	—	[89]
2015	SnO₂	2	Toluene	20	33.4	250	2.3	5.8	2	[123]
2016	SnO₂	3	Acetone	200	153	200	10	12	50	[66]
2016	WO₃	3	NO₂	50	100	100	245	374	0.05	[124]
2017	ZnSnO₃	3	HCHO	100	37.2	220	1	59	10	[125]
2017	Cu₂O/CuO	3	Ethanol	50	ca.2.5	140	—	—	—	[68]
2018	SnO₂/TiO₂	3	Ethanol	200	9.4	300	1.7	13.6	10	[126]
2018	ZnO/ZnFe₂O₄	3	Acetone	20	5.9	140	5.2	12.8	5	[93]
2018	ZnCo₂O₄	3	Acetone	500	38.2	200	19	71	1	[127]
2018	Au@SnO₂	2	CO	20	20.9	220	0.7	3.8	0.5	[128]
2019	Cu₂O	4	HCHO	200	9.6	120	5	3	5	[129]
2019	ZnSn(OH)₆	3	HCHO	100	56.6	60	1	89	1	[130]
2019	ZnCo₂O₄	7	HCHO	100	7.4	180	9	12	10	[131]
2019	Ni/Co/Fe/Cu/Zn oxide	3	Ethanol	50	10.91	80	85	160	0.5	[67]
2019	MCo₂O₄	3	Acetone	50	318	190	3	100	0.6	[132]
	(M=Mn, Ni, and Zn)
2019	Y₂O₃	3	Methanol	18	—	100	<10	<60	0.071	[133]

Table 2 Application of hollow multi-shell structural materials in gas-sensing

Year	Composition	Shell number	Gas	Con.^a/ppm	Response	T^b/℃	$T Res. c$ /s	$T Rec. d$ /s	DL^e/ppm	Ref.
2009	Cu₇S₄	2	NH₃	481	—	25	89	48	127	[120]
2011	ZnO	3	Toluene	20	3.09	300	0.3	3	1	[121]
2011	α-Fe₂O₃	3	Ethanol	10	9	—	—	—	—	[106]
2013	ZnO	3	HCHO	5	5.2	240	1—3	2—4	5	[118]
2014	SnO₂/α-Fe₂O₃	2	Ethanol	10	ca.3.1	250	1	14	10	[122]
2015	Cr₂O₃	4	Ethanol	5	10.1	370	—	—	—	[89]
2015	SnO₂	2	Toluene	20	33.4	250	2.3	5.8	2	[123]
2016	SnO₂	3	Acetone	200	153	200	10	12	50	[66]
2016	WO₃	3	NO₂	50	100	100	245	374	0.05	[124]
2017	ZnSnO₃	3	HCHO	100	37.2	220	1	59	10	[125]
2017	Cu₂O/CuO	3	Ethanol	50	ca.2.5	140	—	—	—	[68]
2018	SnO₂/TiO₂	3	Ethanol	200	9.4	300	1.7	13.6	10	[126]
2018	ZnO/ZnFe₂O₄	3	Acetone	20	5.9	140	5.2	12.8	5	[93]
2018	ZnCo₂O₄	3	Acetone	500	38.2	200	19	71	1	[127]
2018	Au@SnO₂	2	CO	20	20.9	220	0.7	3.8	0.5	[128]
2019	Cu₂O	4	HCHO	200	9.6	120	5	3	5	[129]
2019	ZnSn(OH)₆	3	HCHO	100	56.6	60	1	89	1	[130]
2019	ZnCo₂O₄	7	HCHO	100	7.4	180	9	12	10	[131]
2019	Ni/Co/Fe/Cu/Zn oxide	3	Ethanol	50	10.91	80	85	160	0.5	[67]
2019	MCo₂O₄	3	Acetone	50	318	190	3	100	0.6	[132]
	(M=Mn, Ni, and Zn)
2019	Y₂O₃	3	Methanol	18	—	100	<10	<60	0.071	[133]

Fig.8 Six-axe spider web graph for evaluating the working temperature of the sensors(A), selectivity of the sensors at a concentration of 200 ppm at 120 ℃(B) and resistance transients(120 ℃) to 200 ppm HCHO(C)[129] Copyright 2019, Elsevier.

Fig.9 Responses of the hollow metal oxides based sensor toward 50 ppm of ethanol(A), responses at 25 and 80 ℃(B), response curve toward ethanol gas(C) and comparing the responses with different metal oxides(D)[67] Copyright 2019, American Chemical Society.

Fig.10 Effect of working temperatures(A), dynamic response-recovery transients(B), responses at different acetone concentrations(C), resistance transient towards 20 ppm acetone(D) and proposed sensing mechanism(E, F)[93] Copyright 2018, Elsevier.

Fig.12 Gas responses of triple-shell WO3 sensor to 100 ppb NO2, 5 ppm acetone, 5 ppm CO and 5 ppm NH3 at 200 ℃ in dry(A) and wet(B) atmosphere(RH: 80% at 25 ℃), gas responses(Rg/Ra) to 50 ppb NO2 of solid(C), double-shell(D) and triple-shell(E) WO3 spheres[124] Copyright 2016, Elsevier.

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