Emission Rates of Multiple Air Pollutants Generated from Chinese

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Emission Rates of Multiple Air Pollutants Generated from Chinese Residential Cooking Chen Chen, Yuejing Zhao, and Bin Zhao Environ. Sci. Technol., Just Accepted Manuscript • DOI: 10.1021/acs.est.7b05600 • Publication Date (Web): 05 Jan 2018 Downloaded from http://pubs.acs.org on January 5, 2018

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Environmental Science & Technology

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Emission Rates of Multiple Air Pollutants Generated

2

from Chinese Residential Cooking

3

Chen Chen†,§, Yuejing Zhao†,§, Bin Zhao*,†,‡

4

†

5

China.

6

‡

7

Beijing, 100084, China.

Department of Building Science, School of Architecture, Tsinghua University, Beijing, 100084,

Beijing Key Laboratory of Indoor Air Quality Evaluation and Control, Tsinghua University,

8 9 10

KEYWORDS: Indoor air quality; particulate matter; volatile organic compounds; formaldehyde; range hood

ACS Paragon Plus Environment

1


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ABSTRACT

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Household air pollution generated from cooking is severe, especially for Chinese-style cooking.

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We measured the emission rates of multiple air pollutants including fine particles (PM2.5),

14

ultrafine particles (UFPs), and volatile organic compounds (VOCs, including formaldehyde,

15

benzene, and toluene) that were generated from typical Chinese cooking in a residential kitchen.

16

The experiment was designed through five-factor and five-level orthogonal testing. The five key

17

factors were cooking method, ingredient weight, type of meat, type of oil, and meat/vegetable

18

ratio. The measured emission rates (mean value ± standard deviation) of PM2.5, UFPs,

19

formaldehyde, total volatile organic compounds (TVOCs), benzene, and toluene were 2.056 ±

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3.034 mg/min, 9.102 ± 6.909 × 1012 #/min, 1.273 ± 0.736 mg/min, 1.349 ± 1.376 mg/min, 0.074

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± 0.039 mg/min, and 0.004 ± 0.004 mg/min. Cooking method was the most influencing factor for

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the emission rates of PM2.5, UFPs, formaldehyde, TVOCs, and benzene, but not for toluene.

23

Meanwhile, the emission rate of PM2.5 was also significantly influenced by ingredient weight,

24

type of meat, and meat/vegetable ratio. Exhausting the range hood decreased the emission rates

25

by approximately 58%, with a corresponding air change rate of 21.38 /h for the kitchen room.


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INTRODUCTION

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Cooking can generate high levels of multiple pernicious air pollutants including fine particles

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(PM2.5; particulate matter with aerodynamic diameter less than 2.5 µm)1, ultrafine particles

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(UFPs; particulate matter with diameter less than 0.1 µm)1 and other volatile organic compounds

30

(VOCs)2, and polycyclic aromatic hydrocarbons (PAHs)3. Epidemiologic evidence confirmed the

31

association between exposure to cooking fumes and lung cancer risk, especially in poor

32

ventilation situations4-8. Considering the fact that people spend 60-70% of their time in

33

residences9-12 and cooking is a significant source of indoor air pollutants13, assessing human

34

exposure to residential cooking fumes is important. Compared with Western cooking, household

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air pollution generated from Chinese cooking is much more severe, with more air pollutants

36

produced owing to the special cooking style14. The majority of Chinese women have cooked

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daily for years15, but over half of Chinese residential kitchens are poorly ventilated15-16, leading

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to long-term exposure to indoor high-concentration cooking-generated pollutants, and thus

39

resulting in adverse health effects in China.

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Referring to the existing literature, we found the average or peak concentrations are frequently

41

constructed as a direct parameter of Chinese cooking emissions in most of the previous studies3,

42

14, 17-20

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conditions. A few previous studies on Chinese cooking (most are for commercial restaurants)

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present the emission rate to the atmosphere21-24, which is different from the emission rate to the

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indoor environment discussed in this study. The former is influenced by the exhaust air rate and

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the cooking procedures simultaneously and cannot be used to estimate the concentration levels of

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indoor pollutants. The previous emission rates of pollutants generated from Chinese cooking for

48

the indoor environment are based on oil heating or a limited number of specific dishes; hence,

; however, they are always influenced by various durations, room volumes, and ventilation


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the results only focus on particle emissions but fail to consider gaseous pollutants25-30. Thus,

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detailed information regarding the emission rate of multiple pollutants generated from Chinese

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cooking, which is the base for ventilation or other controlling measures design, is still lacking.

52

Therefore, it is of significance to study the emission rate of air pollutants generated via Chinese

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cooking, which has high potential use for population exposure assessment to air pollution and

54

ventilation design in residential kitchens.

55

We determined the emission rates of PM2.5, UFP, and VOCs based on orthogonal test methods

56

considering five key factors, i.e., cooking method, ingredient weight, type of meat,

57

meat/vegetable ratio, and type of oil. The removal efficiency of the range hood is also discussed.

58 59

MATERIALS AND METHODS

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Survey of factors influencing Chinese cooking

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It has been summarized that emissions of air pollutants during cooking depend strongly on the

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ingredients, type of oil, type of stove, cooking duration and oil temperature3, 20, 26. Oil weight,

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cooking duration and oil temperature are always influenced by the cooking methods. In China,

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most household fuel used for cooking is gas31. Therefore, five key factors, i.e., cooking method,

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the weight of ingredients (meat and vegetables), type of meat, ratio of meat to vegetables, and

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type of oil, were taken into consideration in this study.

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We conducted an online survey of 309 families to determine common cooking behaviors in

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China. Detailed results of such are listed in the Supporting Information (Tables S1-S5). The

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majority of Chinese families use natural gas for cooking (Table S1). The five most popular


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cooking methods, ingredient weights, types of meat, and types of oil were incorporated based on

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the survey (Tables S2-S5). The meat/vegetable ratios ranged from 0.00 (only vegetables) to 1.00

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(only meat) in intervals of 0.25. The survey showed that Chinese people prefer to stir-fry, boil,

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steam, stew, pan-fry, and deep-fry at home, 84.5% of which stir-fry most frequently. However,

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different from the other cooking methods, less than 10% of people wait in the kitchen while

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stewing, thus the other five most prevalent cooking methods, i.e., stir-frying, boiling, steaming,

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pan-frying, and deep-frying, were chosen for this study. 98% Chinese families cook for no more

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than five persons, thus ingredient weights used in this study were for 1-5 persons. According to

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the professional cook who performed the cooking in the experiments, the suggestive value of

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total ingredient weight per person is 120 g. The survey showed that 78.5% Chinese people prefer

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pork for cooking while another 20.8% people prefer beef, mutton, fish or chicken. Besides,

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91.9% Chinese people use peanut oil, blend oil, canola oil, sunflower oil or soybean oil during

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cooking.

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Orthogonal test

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We designed an orthogonal test to cover the typical Chinese cooking styles considering the five

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key factors above and a dummy blank factor simultaneously. The blank factor was set for error

86

estimation. The L25 (56) orthogonal table was designed with six factors (cooking method,

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ingredient weight, type of meat, type of oil, meat/vegetable ratio, and blank), as shown in the

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Supporting Information (Table S6), using SPSS 20.0 (IBM Corp., Armonk, NY, USA), each

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with five levels. The 25 rows correspond to 25 experiments. The cooking methods included stir-

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frying, boiling, steaming, pan-frying, and deep-frying. The ingredient weights were for one

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person to five persons. Pork, beef, mutton, fish and chicken were selected as the types of meat


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used in this study. The types of oil were peanut oil, blend oil, canola oil, sunflower oil and

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soybean oil. Meat/vegetable ratios were 0.00, 0.25, 0.50, 0.75 and 1.00.

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Determination of pollutant emission rates

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1) Emission rate of particulate matter

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Assuming that air is well mixed in the kitchen and the ambient concentration is steady, the mass

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balance equation for PM2.5 and UFPs can be expressed as:

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dCin, p ( t ) dt

= aPCout − λCin, p ( t ) +

Sp V

(1)

99

where , is the real-time indoor concentration of particulate matter at the measuring

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moment , is the air change rate, is the penetration factor of outdoor particles entering the

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indoor environment through the building envelope, is the outdoor concentration of

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particulate matter, is the total removal rate due to coagulation, deposition and air change rate in

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the kitchen, is the emission rate of particulate matter, and is the volume of the kitchen.

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To solve equation (1), we determined the particle concentration at the start time , , , as

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the steady-state indoor particle concentration before measurement: Cin , p ( t0 ) =

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reasonable because we waited for a specific long amount of time (at least 22 minutes) before

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each measurement. Then, the solution of indoor PM2.5 or UFP concentration for equation (1) is:

108

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Cin , p ( t ) = −

Sp

λV

e − λ∆t + Cin , p ( t0 ) +

Sp

λV

aPCout

λ

, which is

(2)

where ∆ is the duration of cooking, which is equal to − .


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The range hood was off and the windows and door were closed during measurements, leading to

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a small value of air change rate , which is helpful for improving the fitting accuracy for . The

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air change rate was measured via the CO2-decay method. The total removal rate λ was

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determined by measuring particle concentration decay after the cooking finished32.

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With the results of air change rate , the total removal rate λ, concentration , , and room

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volume , the nonlinear fitting of the indoor particle concentration increasing curves based on

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equation (2) was conducted to obtain the emission rate with Origin 9.0.0 (OriginLab Corp.,

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Northampton, MA, USA).

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2) Emission rate of gaseous pollutants

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For gaseous pollutants, the real-time concentration derived from the mass balance equation is: S  S  Cin , g ( t ) = Cin , g ( t0 ) − g  e − a∆t + g aV  aV 

120

(3)

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where , is the real-time indoor concentration of gaseous pollutants at the measuring

122

moment .

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The measured durations for formaldehyde and VOCs limit the measured frequencies, especially

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for a few minutes of stir-frying, pan-frying, and deep-frying. Therefore, formaldehyde and VOC

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concentrations were measured twice for each experiment. The first time was to measure the

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indoor gaseous pollutant concentration , at the start time ; the second time was to

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measure the average indoor gaseous concentration , during cooking (from to ), which can

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be expressed as:


7


1 − e − a ∆t a ∆ t + e − a ∆t − 1 = Cin , g ( t0 ) + Sg a∆t a 2V ∆t

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Cin , g

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Thus, the emission rate can be calculated as:

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Sg =

  a 2V ∆t e − a∆t − 1 C Cin , g ( t0 )  + in , g  − a∆t a ∆t + e −1  a ∆t 

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(4)

(5)

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3) Removal performance of the range hood

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The range hood ran during the cooking period for most cases in real-life scenarios. To check the

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removal effect of the range hood for the cooking-generated pollutants, we also measured the

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emission rates of air pollutants when the range hood was on.

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The removal efficiency of the range hood is defined as:

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 

η = 1 −

S hood S

  × 100% 

(6)

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where is the emission rate of air pollutants generated from Chinese cooking measured with the

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range hood off, and is the emission rate measured with the range hood on, the detailed

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determination of which is shown in Supporting Information “DETERMINATION OF

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EMISSION RATES WITH THE RANGE HOOD ON”. The windows and the door were closed

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when the range hood was turned on to ensure the indoor air well mixed.

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Instrumentation and measurement

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A residential kitchen ( = 10.88 m! ) located in Beijing was chosen for measurements from

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April 27, 2017, to September 23, 2017. The layout of the kitchen is shown in Figure 1 and Figure


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S1-(a). Two fans were used to mix the indoor air. The measurement at different locations in the

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kitchen showed that the average relative differences in the PM concentration is 14%, which

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indicates the indoor air was mixed well (details shown in Figure S1-(b)).

149 150

Figure 1. Layout of the residential kitchen (three-dimensional view).

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One laser photometer equipped with a 2.5 µm impactor (AM510; TSI Inc., Shoreview, MN,

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USA) was used to monitor the real-time mass concentrations of PM2.5. A pump (LP-20; A.P.

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Buck Inc., Orlando, FL, USA) and a cutting head (PEM, Model 200, PEM-10-2.5; MSP Corp.,

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Shoreview, MN, USA) were used to collect indoor PM2.5 at a flow rate of 10 L/min during

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cooking. We calibrated the flow rate using a soap-film calibrator (M-30; A.P. Buck Inc.,

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Orlando, FL, USA) before sampling to ensure it matched the cutting head. The Teflon filters

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were weighed on a microbalance accurate to 0.001 mg before and after sampling. The

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monitoring results of the AM510 were calibrated against the gravimetric measurements. The


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lowest cutoff of an identical condensation particle counter (CPC3007; TSI Inc., Shoreview, MN,

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USA) is 10 nm (in electrical mobility diameter), and a great majority of the particles produced

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are less than 100 nm33, so the CPC3007 was used as a UFP monitor in this study with a dilution

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system (total volume flowrate is 0.7 L/min with a dilution factor of 100; Huifen Corp., Shanghai,

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China).

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Formaldehyde in the air was absorbed into a solution in a glass tube containing 5.0 mL of 50

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µg/mL 3-methyl-2-benzothiazolinone hydrazine (MBTH) using a pump (QC-2; Beijing

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Municipal Institute Labour Protection, Beijing, China) at a flow rate of 300 mL/min. To

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determine the formaldehyde concentrations, we added 0.4 mL of 10 g/L ferric ammonium sulfate

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solution to the sampling tube, shook the tube, and then waited for 15 min. Formaldehyde was

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converted into a blue cationic dye by the MBTH, and its light absorbance was measured via a

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spectrophotometer (UNIC 7200; UNIC apparatus Co. Ltd, Shanghai, China) at 630 nm.

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VOCs in the air was absorbed into a Tenax-TA tube (Markes, UK) using the same pump at a

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flow rate of 300 mL/min. The Tenax-TA tubes were analyzed by a thermo-desorber (Markes,

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UK) and gas chromatograph-mass spectrometer (7890B-5977B; Agilent, Santa Clara, CA, USA).

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Analytes were chromatographically resolved on a capillary column (60.0 m × 200 µm × 1.1 µm

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film thickness, HP-VOC; Agilent). The column temperature program was as follows: 40 ºC for 3

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min, ramped to 160 ºC at 15 ºC/min and maintained for 2 min, and then ramped to 240 ºC at 10

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ºC/min (total time 21 min). The mass spectrometer was operated in total ion scan mode so that

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the entire mass range (35 ≤ m/z ≤ 550) was scanned at a frequency of 1.5 Hz. The thermal

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desorption system was a two-stage desorption unit. The sequence of operations to thermally

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desorb the sample from the sorbent tube and transfer it to the gas chromatograph was: (1)

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primary (tube) desorption (300 ºC, 10 min) and then (2) secondary (trap) desorption (300 ºC, 3


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min). The VOCs toluene, benzene, ethylbenzene, p-xylene, o-xylene, acetic acid butyl ester,

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styrene, and undecane were quantified using standard compounds whereas the results of other

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VOCs were expressed as toluene-equivalent concentration.

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The measuring procedures are shown in the Supporting Information (Figure S2). The pan for

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stir-frying, pan-frying, and deep-frying was heated for 7 minutes before each experiment to

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eliminate the influence of particles generated from heating the organic film on the surface34. The

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residential Chinese cooking procedures were conducted by a professional cook including

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weighing and preparing the ingredients, cooking, and washing the pans (more than 15 times to

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repeat scrubbing), which enforced consistency among the repeated experiments. We repeated the

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measurements for the cooking methods that generated much more pollutants relatively.

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We measured the air volume rate of the range hood by measuring the airflow speed in the pipe

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connecting the range hood with a hot-ball anemometer (FB-1; Tianjianhuayi Corp., Beijing,

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China).

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RESULTS AND DISCUSSION

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Emission rate of PM2.5

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The emission rates of PM2.5 generated from stir-frying, pan-frying, and deep-frying were

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calibrated by factors of 0.805, 0.832 and 0.911, respectively, against the gravimetric

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measurements. The emission rate of PM2.5 generated from Chinese cooking was 2.056 ± 3.034

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mg/min (mean value ± standard deviation, similarly hereinafter). The emission rate of PM2.5

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generated from stir-frying, pan-frying, and deep-frying was 3.352 ± 3.358 mg/min. The emission


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rate of PM2.5 generated from the actual cooking was much larger than the operation of the gas

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stove and the heating of the used pan, which was only 0.398 mg/min.

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As shown in Figure 2, cooking method, ingredient weight, type of meat, and meat/vegetable ratio

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were statistically significant factors effecting emission rates of PM2.5, compared to type of oil.

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The emission rates of PM2.5 generated from stir-frying and pan-frying were significantly higher

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than those of the other three cooking methods were. When the ingredient weight was small (for 1

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person), the emission rate of PM2.5 was significantly higher than that of the other four weights

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(for 2-5 persons). The different types of meat can be divided into three significantly different

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subsets (fish, chicken, and beef; beef and pork; pork and mutton). Chinese cooking for which the

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meat/vegetable ratio is 0.25 generated significantly more PM2.5 than the other four ratios did.

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Detailed PM2.5 results are shown in the Supporting Information (Table S7). In general, the

214

emission rates of PM2.5 generated from Chinese cooking are in the same magnitude of the

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emission rates generated from Western cooking (details shown in Figure S5).


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Figure 2. Emission rates of PM2.5 generated from Chinese cooking (factors sorted from the

218

largest F value to the smallest one).

219

Emission rate of UFPs

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The emission rate of UFPs generated from Chinese cooking was 9.102 ± 6.909 × 1012 #/min,

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which was much larger than the operation of the gas stove and the heating of the used pan (5.048

222

× 1011 #/min). As shown in Figure 3, cooking method was a statistically significant factor

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affecting emission rates of UFPs compared to the other factors. Stir-frying and pan-frying

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generated significantly more UFPs than deep-frying did, whereas deep-frying generated

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significantly more UFPs than boiling and steaming did. Detailed measured emission rates of

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UFPs are shown in the Supporting Information (Table S8). The emission rates of UFPs generated


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from Chinese cooking are higher than the emission rates generated from Western cooking due to

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its special cooking method (details shown in Figure S5).

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Figure 3. Emission rates of UFPs generated from Chinese cooking (factors sorted from the

231


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Emission rate of VOCs

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The emission rate of formaldehyde generated from Chinese cooking was 1.273 ± 0.736 mg/min.

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As shown in Figure 4, cooking method was a statistically significant factor affecting emission

235

rates of formaldehyde compared to the other factors. Pan-frying and stir-frying generated

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significantly more formaldehyde than deep-frying did, whereas deep-frying generated

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significantly more formaldehyde than boiling and steaming did. Detailed measured emission

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rates of formaldehyde are shown in the Supporting Information (Table S9).


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Figure 4. Emission rates of formaldehyde generated from Chinese cooking (factors sorted from

241

the largest F value to the smallest one).

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Benzene was generated from cooking for all the typical Chinese recipes, and toluene was

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generated from cooking for 68% of the recipes. The emission rate of benzene was 0.074 ± 0.039

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mg/min and that of toluene was 0.004 ± 0.004 mg/min. Detailed results are shown in the

245

Supporting Information (Tables S10-11 and Figures S3-4).

246

The emission rate of TVOCs generated from Chinese cooking was 1.349 ± 1.376 mg/min. As

247

shown in Figure 5, cooking method and ingredient weight were statistically significant factors

248

affecting emission rates of TVOCs compared to the other three factors. Pan-frying and stir-frying

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generated significantly more TVOCs than the other three methods did. The emission rate of


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250

TVOCs during cooking for a person was significantly higher than that during cooking for 2-5

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persons. Detailed results are shown in the Supporting Information (Table S11).

252 253

Figure 5. Emission rate of TVOCs generated from Chinese cooking (factors sorted from the

254


255

Removal performance of the range hood

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We measured the emission rates of PM2.5, UFPs, and formaldehyde for the 6th and 23rd Chinese

257

recipes listed in Table S6 when the range hood was on. The reason why these two recipes were

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selected is that they are very common Chinese residential dishes and the pollutant emission rates

259

for them are high.


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The measured exhaust air volume rate of the range hood was 3.88 m3/min for the repeated

261

measurements of the emission rate, the corresponding air change rate of which was 21.38 /h for

262

the kitchen room. The exhaust air rate is rated at 15 m3/min, which are in the range of the typical

263

exhaust air rate in our survey (details shown in Figure S7).

264

The removal efficiency of the range hood was 58 ± 6% for PM2.5, 49 ± 4% for UFPs, and 68 ±

265

8% for formaldehyde.

Removal efficiency of range hood

100% 90% 78%

80% 70% 60%

65% 63%

60% 63% 53%

52%

47%

50%

46%

40% 30% 20% 10% 0% PM2.5 PM

UFP UFPs

2.5

1st measurement

2nd measurement

Formaldehyde Formaldehyde 3rd measurement

266 267

Figure 6. Removal efficiency of the range hood.

268 269

ASSOCIATED CONTENT

270

Supporting Information. The following files are available free of charge:

271

Survey results of cooking behaviors (Page S2, Tables S1-5).

272

Orthogonal test design (Page S3, Table S6).

273

Determination of emission rates with the range hood on (Page S4).


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274

Uniformity of spatial pm concentrations (Page S5, Figure S1-(a), Figure S1-(b)).

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The measuring procedures (Page S6, Figure S2).

276 277

Air pollutant emission rates generated from typical Chinese cooking (Page S7-S20, Figure S3-4, Tables S7-12).

278

Comparison of emission rates with previous studies (Page S21, Figure S5).

279

Survey results of range hoods (Page S22, Figure S6).

280

The duration time of typical Chinese cooking (Page S23, Table S13).

281

The air change rate during measurement (Page S24, Table S14).

282 283

Comparisons of flow rate and the efficiency of range hood with previous studies (Page S25, Figure S7).

284

Comparison between two AM510 monitors (Page S26, Figure S8).

285 286

AUTHOR INFORMATION

287

Corresponding Author

288

*Address correspondence to Dr. Bin Zhao, Department of Building Science, School of

289

Architecture, Tsinghua University, Beijing 100084, PR China. Tel: 86-10-62779995. Fax: 86-10-

290

62773461. Email: [email protected]

291

Author Contributions

292

§

293

Notes

294

The authors declare no competing financial interest.

Co-first authors that contributed equally to this work.

295 296

ACKNOWLEDGMENTS


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297

This work was financial supported by the National Key Project of the Ministry of Science and

298

Technology, China on “Green Buildings and Building Industrialization” through Grant No.

299

2016YFC0700500 and funding from Innovative Research Groups of the National Natural

300

Science Foundation of China (No. 51521005). The authors would like to thank Prof. Xudong

301

Yang, Ms. Caiyun Lu, Mr. Junzhou He, Mr. Mengqiang Lv, and Mr. Shen Yang for kindly

302

helping with the measurements.

303 304

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Table of Contents (TOC)


1

Emission Rates of Multiple Air Pollutants Generated from Chinese

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