建筑環境中有機磷酸酯污染特征和控制技術研究進展

韓旭; 厲文輝; 劉杰民; 吳傳東; 莊媛; 裴素云

doi:10.13374/j.issn2095-9389.2021.05.11.001

建筑環境中有機磷酸酯污染特征和控制技術研究進展

doi: 10.13374/j.issn2095-9389.2021.05.11.001

北京科技大學化學與生物工程學院，北京 100083

基金項目: 國家自然科學基金資助項目（21878013，21906006，22178022）；中央高校基本科研業務費資助項目（FRF-IDRY-20-016，FRF-IDRY-19-026，FRF-BR-20-03B，FRF-MP-19-012，FRF-TP-20-018A2）

詳細信息

通訊作者:
厲文輝, E-mail: liwh@ustb.edu.cn

劉杰民, E-mail: liujm@ustb.edu.cn

中圖分類號: X506
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- HTML全文瀏覽量: 287
- PDF下載量: 47
- 被引次數: 0
出版歷程
- 收稿日期: 2021-05-11
- 網絡出版日期: 2021-07-06
- 刊出日期: 2022-02-15

Controlling techniques and characteristics of organophosphate esters in building environment: A review

School of Chemistry and Biological Engineering, University of Science and Technology Beijing, Beijing 100083, China

More Information

Corresponding author: LI Wen-hui, E-mail: liwh@ustb.edu.cn; LIU Jie-min, E-mail: liujm@ustb.edu.cn

摘要

摘要: 有機磷酸酯（Organophosphate esters, OPEs）作為一類阻燃劑和增塑劑，在建筑材料和室內裝修材料中廣泛使用。由于該類物質主要以物理添加而非化學鍵合的方式加入到材料中，因此易在使用過程中進入環境。研究表明OPEs普遍存在于室內環境中，并且濃度較高，人體長期暴露在高濃度OPEs的室內環境中，可能存在一定的健康風險。本文在綜述了常見OPEs的性質、應用和生物毒性的基礎上，總結了其在建筑環境中的污染特征、環境行為和暴露水平，介紹了建筑環境中OPEs的源匯特性、控制技術與人體暴露風險，并對未來研究方向進行了展望。
- 有機磷酸酯 /
- 建筑環境 /
- 污染特征 /
- 源匯特性 /
- 控制技術
Abstract: Organophosphate esters (OPEs) are widely used as flame retardants, plasticizers, stabilizers, and antifoaming agents in various building materials, such as plastics, foam, coatings, textiles and furniture, and interior decoration materials. In general, most OPEs are combined physically rather than chemically during production. This makes these chemical compounds to be easily released in an indoor environment. Also, previous studies have shown that OPEs were commonly found in an indoor environment at elevated concentrations. Long-term exposure to high concentrations of OPEs in an indoor environment might result in certain health risks. However, there is limited information on the distribution characteristics and risk assessment of OPEs in the building environment. In this study, we discussed the properties, applications, and biological toxicity of common OPEs. In addition, we reviewed the environmental behavior, pollution characteristics, and exposure level of OPEs in the building environment. Building materials and household products are important sources of OPEs in an indoor environment. The levels of OPEs in these productions were significantly associated with the concentration of OPEs in indoor air and dust. In general, indoor air and dust are regarded as the two major sinks of OPEs in the building environment. However, more volatile OPEs, such as TCIPP, TCEP, and TnBP were found predominantly in indoor air, while less volatile OPEs, such as TDCIPP and TPhP were often detected in dust due to their low vapor pressure and high affinity for particles. In general, humans can be exposed to OPEs in a building environment through three main routes of exposure: inhalation, dermal absorption, and ingestion. This study revealed that dust ingestion is the dominant route of human exposure to OPEs, while dermal absorption and inhalation were minor contributors to the total daily exposures. In addition, the relative mass transfer model and release characteristics of OPEs in the building environment were also introduced in this study. Based on the characteristics of OPEs in the building environment, the controlling techniques, which include microporous control technology, barrier control technology, compound purification technology, and an alternative strategy of OPEs, were introduced. However, prospects for future research were considered.
- organophosphorus esters /
- building environment /
- pollution characteristics /
- source and sink characteristics /
- control technology

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表 1 常見有機磷酸酯（OPEs）的性質和應用

Table 1. Properties and applications of common organophosphate esters

Group	Compound	Abbr.	Formula	BP/℃	logK_ow	lologK_oa	Vp/Torr	Application
Cl-OPEs	Tris(2-chloroethyl) phosphate	TCEP	C₆H₁₂O₄P	351	1.63	7.42	3.91×10^?4	Flame retardant, plasticizer, glue, lacquer, paint, industrial processes
	Tris(2-chloropropyl) phosphate	TCIPP	C₉H₁₈Cl₃O₄P	342	2.89	8.20	5.64×10^?5	Flame retardant, plasticizer
	Tris(1,3-dichloro- 2-propyl)phosphate	TDCIPP	C₉H₁₅Cl₆O₄P	457	3.65	10.6	2.86×10^?7	Flame retardant, plasticizer, paint, glue
Alkyl-OPEs	Triethyl phosphate	TEP	C₆H₁₅O₄P	216	0.87	6.63	0.165	Plasticizer, polyvinylchloride, polyester resins, polyurethane foam
	Tripropyl phosphate	TPrP	C₉H₂₁O₄P	254	2.67	6.5	2.9×10^?2	Plasticizer
	Tri-n-butyl phosphate	TnBP	C₁₂H₂₇O₄P	289	4.00	9.21	1.1×10^?3	Plasticizer, hydraulic fluids, lacquer, paint, glue, anti-foam agent
	Tri-iso-butyl phosphate	TiBP	C₁₂H₂₇O₄P	264	3.60	7.48	1.28×10^?2	Plasticizer, lubricant, concrete
	Tris(2-butoxyethyl) phosphate	TBEP	C₁₈H₃₉O₇P	228	3.00	13.0	1.23×10^?6	Flame retardant, plasticizer, floor Flame retardant, plasticizer, floor finish, wax, lacquer, paint, glue
	Tris(2-ethylhexyl) phosphate	TEHP	C₂₄H₅₁O₄P	220	9.49	14.9	6.07×10^?7	Flame retardant, plasticizer, fungus resistance
Aryl-OPEs	Tricresyl phosphate	TCrP	C₂₁H₂₁O₄P	265	5.11	12.0	3.49×10^?8	Plasticizer, PVC, hydraulic fluid, cellulose, cutting oil, transmission fluid
	Triphenyl phosphate	TPhP	C₁₈H₁₅O₄P	370	4.70	8.45	4.72×10^?7	Flame retardant, plasticizer, hydraulic fluids, lacquer, paint, glue
	2-Ethylhexyl diphenyl phosphate	EHDPP	C₂₀H₂₇O₄P	421	6.30	8.92	3.34×10^?5	Plasticizer, hydraulic fluids
	Triphenylphosphine oxide	TPPO	C₁₂H₂₄N₃OP	389	2.87	—	1.24×10^?6	Flame retardant, catalyst, extractant
Note: BP—boiling point；logK_ow—octanol-water partition coefficient；logK_oa—octanol-air partition coefficient；V_p—vapor pressure.

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表 2 不同國家各種微環境室內灰塵中的OPEs

Table 2. OPEs in indoor dust of various microenvironments of different countries

Region		Sample site	TCEP/ (ng?g^?1)	TCIPP/ (ng?g^?1)	TDCIPP/ (ng?g^?1)	TEHP/ (ng?g^?1)	TnBP/ (ng?g^?1)	TBEP/ (ng?g^?1)	TPhP/ (ng?g^?1)	EHDPP/ (ng?g^?1)	ΣOPEs/ (ng?g^?1)	References
China	Dali	E-waste disposal plant (n=13)	76–1740	640–8790	68–566	19–2100	<MDL–1730	<MDL–1060	31–6660	28–4550	934–21500	[31]
	Guiyu town	E-waste disposal plant（n=14）	149–6920	854–10000	13–2550	24–789	228–14,100	<MDL–1860	371–332000	222–6900	4660–350000	[31]
	Beijing	House（n=21）	2231–30847	220–13804	<80–350	<7–1018	<7–1531	493–41917	122–1829		767–23000	[32]
	Beijing	Daycare center（n=16）	391–17805	71–30157	<80–13,113	<7–660	<7–3741	85–4561	41–3514			[32]
	Beijing	Office （n=23）	11–1180	36200–191000	533–2410	<7–83	268–3980	1830–13000	350–1890	463–1840	124000(Mean)	[33]
Egypt	Asyut	House（n=20）	<8–132	<15–123		<2–26	<10–557	<3–305	8–289	<2–102	38–962	[36]
		Offices（n=20）	<8–125	<15–700		<2–46	<10–490	<3–1244	11–337	<2–74	38–1514
		Public places (n=20)	<8–538	<15–465		<2–261	<10–1616	<3–1029	116–2357	<2–74	937–5235
Saudi Arabia	Jeddah	House（n=20）	125–1650	200–3700	<MDL–270	<MDL–165	150–8700	<MDL–2750	65–1200	55–520	1000–13800	[37]
Pakistan	Faisalabad	Urban house（n=15）	<MDL–175	<MDL–85	<MDL–50	<MDL–22	<MDL–255	<MDL–145	<MDL–330	<MDL–360	49.4–473	[38]
	Gujarat	Rural house（n=31）						<MDL–340	15–185			[35]
	Islamabad Faisalabad	Electronics stores(n=30)		6–620	<MDL–1025		<MDL–1475	<MDL–100	10–5000	2–830	6555(Mean)	[24]
		Clothing stores（n=15）		<MDL–95	<MDL–175		<MDL–30	<MDL–70	<MDL–220	<MDL–120	967(Mean)
		Offices（n=16）		<MDL–320	<MDL–4100		<MDL–185	<MDL–11,900	10–23450	5–285	575(Mean)
Philippines	Malate	Rural house（n=17）	<MDL–1200		4–970	<MDL–79			8.5–2100	8–770	1800(Mean)	[36]
Kuwait		Urban house（n=15）	275–1800	120–7065	<5–340	21–800	60–1555	31–140,450	44–6890	75–10990	633–44400	[38]
Germany	Ludwigsburg	Offices（n=10）	<80–170	180–940		<30–410	<80–290	2900–13000	470–4800	21–210	4300–32000	[37]
Germany	Ludwigsburg	House（n=16）	140–280	370–960		<30–250	<80–110	<60–2800	180–1300	30–66	800–6000	[37]
Sweden	Stockholm	House（n=10）	<MDL–33	0.7–11	<MDL–0.2	<MDL–1.7	2.2–27	0.6–30			69800(Mean)	[34]
Sweden	Stockholm	Daycare center（n=10）	2.5–150	0.8–12	<MDL–0.7	0.1–6.2	3.9–150	31–4100			78000(Mean)	[34]
US	New York	House（n=18）	<MDL–2130	458–750	77–1440	12–394	536–5520		<MDL–3500	<MDL–4560	1930–101000	[38]
Japan		House（n=14）	<MDL–28000	47.1–34,300	103–166000	<MDL–424	13.0–507	3240–91000	50.8–833	15.8–192	7720–238000	[39]
Korea		House（n=30）	192–15400	19.7–8290	<MDL–20500	17.9–2930	<MDL–1690	982–234000	66.8–25200	15.4–1490	3090–249000	[39]
Note: MDL presents the method detection limit.

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表 3 不同國家各種微環境室內空氣中的OPEs

Table 3. OPEs in indoor air of various microenvironments of different countries

Region	Sample site	TCEP/ (ng?m^?3)	TCIPP/ (ng?m^?3)	TDCIPP/ (ng?m^?3)	TEHP/ (ng?m^?3)	TnBP/ (ng?m^?3)	TBEP/ (ng?m^?3)	TEP/ (ng?m^?3)	TiBP/ (ng?m^?3)	TPhP/ (ng?m^?3)	ΣOPEs/ (ng?m^?3)	References
Sweden	House（n=66）	<MDL–230	<MDL–1200			2.5–370	<MDL–86	0.18–300	2–54	<MDL–25		[34]
Germany	House（n=56）	<MDL–9.2	1.2–496.9	<MDL–29.9	<MDL–9.6	<MDL–112.1	<MDL–17.5	<MDL–27.1	<MDL–663	<MDL–8.9	3.3–751	[46]
New York, US	House（n=54）	<MDL–18.7	<MDL–293	<MDL–45.2	<MDL–0.9	<MDL–29.3	<MDL–137	0.2-332		<MDL–43.7	2.9-635	[4]
Oslo, Norway	Offices（n=58）	<MDL–76	1.2-128	<MDL–31	<MDL–42	<MDL–119				<MDL–9	28-1018	[42]
Hangzhou, China	Offices（n=10）	1.03?13.38	0.8?81	0.04?14.3	0.3?2.6	0.01?90.3	0.02?5.5			0.3?10.2	5?147.8	[47]
Stockholm, Sweden	House（n=10）	<MDL – 28	2.4–64	<MDL–17	—	3.5–45	<MDL–4.5	3.2–16	3.0–66		12–240	[34]
	Offices（n=10）	<MDL–140	16–240	<MDL–73	—	<MDL–100	<MDL–73	0.7–91	4.4–13	<MDL–2.7	21–630
	Daycare center（n=10）	7.8–230	1.3–72	<MDL–30	—	3.7–320	<MDL–380	0.8–20	<MDL–63	<MDL–0.9	14–1110
	Library（n=1）	590	40	<0.7	<0.8		<0.8		7.8	<0.4	640	[45]
	Bowling alley (n=1)	460	93	<0.4	<0.4		3.3	<0.4	<0.2	6.6	570
	Radio Shop(n=4)	29	0.4–10	<0.4	<0.4		<0.5	<0.4	0.4–3.6	0.4–13	42–68
Zurich, Switzerland	Offices（n=4）	6.1–56	<MDL–260	—	<MDL–0.6	<MDL–8.1	<MDL–1.2			0.9–3.1		[48]
Zurich, Switzerland	Building material markets（n=4）	6.3–11.9	46–57	—	1.2–0.6	14–17	<MDL–2.5			0.6–1.1		[48]

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表 4 不同種類建筑材料與家居產品中OPEs的含量

Table 4. Concentrations of OPEs in different types of building materials and household products

Region	Sample types	TnBP/ (ng?g^?1)	TBEP/ (ng?g^?1)	TEHP/ (ng?g^?1)	TCIPP/ (ng?g^?1)	TDCIPP/ (ng?g^?1)	TCEP/ (ng?g^?1)	TPhP/ (ng?g^?1)	EHDPP/ (ng?g^?1)	TPPO/ (ng?g^?1)	TCrP/ (ng?g^?1)	ΣOPEs/ (ng?g^?1)	References
Dalian, China	PVC wallpaper(n=3)	2?13.8	10.2?16.9	9984?12830	1124?1831	102.6?175.8	1703?2806	86.86?171.7	105.4?118.8	33.651?39	114.9?126.8	44460-48470	[51]
	Gypsum(n=2)	8.8?29.8	2.6?2.8	0.5?0.5	3.1?36.6	0.001?0.3	0.3?7.8	0.1?0.4	0.02?0.9	0.4?0.9	0.01?0.5	3.11?80.5
	Puttypowdr(n=2)	0.1?3.1	0.3?0.7	0.2?0.9	0.6?5.8	1.9?2.1	0.02?1.4	0.2?0.5	0.08?0.9	0.1?0.6	0.05?0.6	2.20?16.3
	Latex paint(n=6)	105.1?117.4	12?18.9	9.3?17.2	7.8?31.9	81.4?156.7	7.8?13.3	10.4?11.7	27.3?28.1	11.5?21.4	12.4?17.9	64.5?428
	Solid wood(n=4)	12.5?33.5	35.3?50.8	55.5?60	59.4?95.4	6.7?7	72?127	464?814	865?1720	5.6?9.1	4.8?4.9	1620?2790
	Porcelain glue(n=6)	34.8?77.3	10?20.8	9.6?16.4	652?759	880?1810	97.4?98.4	3.2?3.2	10.6?12.5	69.7?138	3.8?4.5	1770?2290
	Sealant(n=7)	746?1910	9.1?13.7	13.2?17.8	181?247	672?1580	67.1?106	24.4?31.9	5.7?9.2	4.6?7	1.4?3.7	1720?2360
Shenzhen, China	Textiles(n=8)					22.9?28.6	21.5?25.1				22?27.1		[52]
America	Polyurethane foams(n=102)					44,870,000 (Mean)	41,770,000 (Mean)						[53]
America	Polyurethane foams(n=115)				0.8–46	0.53–88.1		0.0013–15					[54]
Japan	TV rear cover(n=12)	1.5–16	<80	0.9–80	4–26	<2	4–9.0	870–14,000,000			47–4,500,000		[48]
	Curtain(n=2)	1300–1600	<80	<0.9	<3.0	<2	4–6.0	820,000–840,000			4900–190,000
	Heatshield(n=2)	4.8–8.8	140–890	0.9–6.4	28–37	2–6	9–10	5300–8700			190–570

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