桥连氧化钨纳米线的可控合成及气敏性质

doi:10.3866/PKU.WHXB201911036

Abstract

Abstract:

The rapid development of industrialization has resulted in severe environmental problems. A comprehensive assessment of air quality is urgently required all around the world. Among various technologies used in gas molecule detection, including Raman spectroscopy, Fourier transform infrared (FTIR) spectroscopy, mass spectroscopy (MS), electrochemical sensors, and metal oxide semiconductor (MOS) gas sensors, MOS gas sensors possess the advantages of small dimension, low power consumption, high sensitivity, low production cost, and excellent silicon chip compatibility. MOS sensors hold great promise for future Internet of Things (IoT) sensors, which will have a profound impact on indoor and outdoor air quality monitoring. The development of nanotechnology has significantly enhanced the development of MOS gas sensors. Among various nanostructures like nanoparticles, nanosheets and nanowires, the emergence of quasi-one-dimensional (q1D) nanowires/nanorods/nanofibers, with unique q1D geometry (facilitating fast carrier transport) and large surface-to-volume ratio, potentially act as ideal sensing channels for MOS sensors with extremely small dimension, and good stability and sensitivity. These structures have thus been the focus of extensive research. Among the various MOS nanomaterials available, tungsten oxide (WO_3-x, 0 ≤ x < 1) nanowires feature the characteristic properties (multiple oxidation states, rich substoichiometric oxides with distinct properties, photo/electrochromism, (photo)catalytic properties, etc.), and unique q1D geometry (single-crystalline pathway for fast carrier transport, large surface-to-volume ratio, etc.). WO_3-x nanowires have broad applications in smart windows, energy conversation & storage, and gas sensing devices, and have thus become a focus of attention. In this paper, the fundamental properties of tungsten oxide, synthesis methods and growth mechanism of tungsten oxide nanowires are reviewed. Among various (vapor-liquid-solid (VLS), vapor-solid (VS) and thermal oxidation) growth methods, the thermal oxidation method enables an in situ integration of WO_3-x nanowires on predefined electrodes (so-called bridged nanowire devices) via the oxidation of lithographically patterned W film at relatively low growth temperature (~500 ℃) because of interfacial strain, defects and oxygen on the surface of the W film. The novel bridged nanowire-based sensor devices outperform traditional lateral nanowire devices in terms of larger exposure area, low power consumption via self-heating, and greater convenience in device processing. Recent progress in bridged WO_3-x nanowire devices and sensitive NO_x molecule detection under low power consumption have also been reviewed. Power consumption of as low as a few milliwatts was achieved, and the detection limit of NO₂ was reduced to 0.3 ppb (1 ppb = 1 × 10^-9, volume fraction). In situ formed bridged WO_3-x nanowire devices potentially satisfy the strict requirements of IoT sensors (small dimension, low power consumption, high integration, low cost, high sensitivity, and selectivity), and hold great promises for future IoT sensors.

Key words: Bridged tungsten oxide nanowires, Thermal oxidation, Low power consumption, High sensitivity, In situ integration, Gas sensing

Tiantian Dai, Zanhong Deng, Gang Meng, Bin Tong, Hongyu Liu, Xiaodong Fang. Controllable Synthesis and Gas Sensing Properties of Bridged Tungsten Oxide Nanowires[J]. Acta Phys. -Chim. Sin. 2021, 37(10), 1911036. doi: 10.3866/PKU.WHXB201911036

Figures/Tables 12

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W source	Growth mechanism	Solvent	T/℃	t/h	Product	Length	Diameter/nm	Ref.
H₂WO₄·nH₂O	Hydrothermal	(NH₄)₂SO₄	200	48	h-WO₃	10–100 μm	25	44
Na₂WO₄	Hydrothermal	Rb₂SO₄	180	2–72	h-WO₃	10–100 μm	25	45
Na₂WO₄·2H₂O	Hydrothermal	Na₂SO₄, K₂SO₄	180	24	h-WO₃	2.5 μm	80	41
H₂WO₄	Hydrothermal	K₂SO₄	180	12	WO₃	10–100 μm	10–20	46
Na₂WO₄·2H₂O	Hydrothermal	Na₂SO₄	180	12	h-WO₃	1.5–2.5 μm	20	47
Li₂WO₄	Hydrothermal	Li₂SO₄	180	24–48	h-WO₃	0.1–1 μm	25~50	48
W(CO)₆	Solvothermal	1-Octadecanol/1-Octadecene	200	0.33	W₂₀O₅₈	100 nm	5	49
WCl₆, W(C₂H₅O)₆	Solvothermal	Ethanol/propanol	200	24	W₁₈O₄₉	< 50 nm	10	42
WCl₆	Solvothermal	cyclohexanol	200	5–7	W₁₈O₄₉	–	< 5	51
H₂WO₄	Solvothermal	Ethanol/oleylamine	220	12	W₁₈O₄₉	50 nm	< 3	43
WCl₆	Solvothermal	1-propanol	200	9	W₁₈O₄₉	500–1000 nm	10	52
WCl₆	Solvothermal	Ethanol	180	24	W₁₈O₄₉	–	5	50

W source	Growth method	Catalyst	T/℃	t	Product	Ref.
W film	Vapor-liquid-solid	Ni	470	2–6 h	WO₂	2
W film	Vapor-liquid-solid	Au	500	3 h	WO₃	61
W plate	Vapor-liquid-solid	KOH	610	2 h	W₃O₈	62
W plate	Vapor-liquid-solid	KI	650	2 h	WO₃	63
WO_2.9 powder	Vapor-solid	–	900	1.5 h	WO₃	67
W rod	Vapor-solid	–	850	2 h	W₁₈O₄₉	68
WO₃ powder	Vapor-solid	–	900	3 h	W₁₈O₄₉	53
W film	Vapor-solid	–	800	10 min	WO₃	69
W film	Vapor-solid	–	850	1–3 h	W₁₈O₄₉	70
W film	Vapor-solid	–	650	4–10 h	WO₃	66
W powder	Vapor-solid	–	1000	1 h	WO₃	71
W wire	Vapor-solid	–	1445	10 min	WO_2.9	72
W spiral coil	Thermal oxidation	–	437	–	WO_2.9	73
W film	Thermal oxidation	–	650	1 h	W₁₈O₄₉	11
W film	Thermal oxidationThermal oxidation	–	550	1 h	WO₃	74
W film	Thermal oxidation	–	600	30 min	WO₃	64
W film	Thermal oxidation	–	680	1 h	WO_2.9	65

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Controllable Synthesis and Gas Sensing Properties of Bridged Tungsten Oxide Nanowires

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Materials	T/℃	Gas	C/ppm	Response	Ref.
WO₃ thin film	300	NO₂	10	70	93
WO₃ thin film	350	NO₂	10	9	94
WO₃ thin film	250	NO₂	10	8	95
WO₃ nanofibers	250	NO₂	5	12	96
WO₃ nanotubes	300	NO₂	10	8.8	97
WO₃ nanorods	200	NO₂	5	8	98
Bridged W₁₈O₄₉ nanowires	250	NO₂	10	144.3	77