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In some cases, the surface coatings had little or no impact Pulmonary bioassay bridging study Inhalation studies Carbonyl iron particles α-quartz particles Intratracheal instillation stu

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18 Models for Testing the

Pulmonary Toxicity of Particles: Lung Bioassay Screening Studies

in Male Rats with a New

David B Warheit, Kenneth L Reed, and Christie M Sayes DuPont Haskell Laboratory for Health and Environmental Sciences

CONTENTS

18.1 Introduction 317

18.2 Methods 319

18.2.1 General Experimental Design 319

18.2.2 Animals 320

18.2.3 Particle Types 320

18.2.4 Lung Cell Proliferation Studies 320

18.2.5 Bronchoalveolar Lavage Methods 321

18.2.6 Lung Histopathology Studies 321

18.2.7 Statistical Analyses 321

18.3 Results 321

18.3.1 Lung Weights 321

18.3.2 Lung Cell Proliferation Results 321

18.3.3 Bronchoalveolar Lavage Fluid Results 323

18.3.3.1 Pulmonary Inflammation 323

18.3.3.2 Bronchoalveolar Lavage (BAL) Fluid Parameters 323

18.3.3.3 Pulmonary Histopathological Evaluations 325

18.4 Discussion 325

Acknowledgments 329

References 329

18.1 INTRODUCTION

Formulation changes in the form of altered surface treatments are known to frequently occur for a variety of commercialized particle-types The R-100 formulation of rutile-type titanium dioxide is a well-known low-toxicity particulate This study was designed as a pulmonary screening tool to

317

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encapsulated with pyrogenically deposited amorphous silica) may impart significant toxicity in the

study was to evaluate in the lungs of rats—using a well-developed, short-term pulmonary

samples and to compare the pulmonary toxicity of these samples with two other low toxicity particulate-types (reference negative controls), along with a cytotoxic particulate (reference positive control) sample Another aim was to bridge the results obtained herein with data previously generated from inhalation studies with crystalline silica-quartz particles and with carbonyl iron particulates as the inhalation/instillation bridge materials

Bridging studies can be useful in providing an inexpensive safety screen when assessing the hazards of new developmental compounds or when making small modifications to an existing commercial particle-type, such as surface treatments The strength of the bridging strategy is dependent upon having good inhalation toxicity data on one of the bridging compounds The particle-type for which inhalation data exists can then be used as a reference control material for

an intratracheal instillation bridging study (see Figure 18.1) The basic idea for the bridging concept

is that the effects of the instilled material serve as a control (known reference) material and then are

“bridged” on the one hand to the inhalation toxicity data for that material, as well as to the new materials being tested The results of bridging studies in rats are then useful as pulmonary toxicity screening (i.e., hazard) data, because consistency in the response of the inhaled and instilled control material serves to validate the responses with the newly tested particulate matter

Numerous studies have investigated the pulmonary toxicological impacts of surfaces treat-ments on titanium dioxide particles In some cases, the surface coatings had little or no impact

Pulmonary bioassay bridging study

Inhalation studies

Carbonyl iron particles

α-quartz particles

Intratracheal instillation studies

PBS sham α-quartzparticles

Carbonyl iron particles

R-100 &

Pigment A TiO2 particles

FIGURE 18.1 Schematic demonstrating the strategy for conducting pulmonary bioassay bridging studies Bridging studies can have utility in providing an inexpensive preliminary safety screen when evaluating the hazards of new developmental compounds The basic idea for the bridging concept is that the effects of the instilled material serve as a control (known) material and are then “bridged” to the inhalation toxicity data for that material and to the new materials being tested

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current study describes a model or pulmonary bioassay method for assessing the pulmonary hazard potential of intratracheally instilled particle-types The chapter also discusses the relevance of this screening methodology as a possible surrogate for inhalation studies with low-solubility particle-types

18.2 METHODS

18.2.1 GENERALEXPERIMENTALDESIGN

The fundamental features of this pulmonary bioassay are dose-response evaluation, time-course assessments, and reference particle-types (positive and negative) The time-course studies are used

to assess the sustainability of the observed affect The major endpoints of this study were the (1) time-course and dose/response intensity of pulmonary inflammation and cytotoxicity (bronchoal-veolar lavage (BAL) parameters), (2) airway and lung parenchymal cell proliferation, and (3) histopathological evaluation of lung tissue (see Figure 18.2)

The lungs of rats were exposed via intratracheal instillation with single doses of 1 or 5 mg/kg

of entry technique is not a substitute for the more physiologically relevant inhalation method of exposure However, the intratracheal instillation method of exposure can be a qualitatively reliable screen for assessing the pulmonary toxicity of particles [1,2] All particles were prepared in a volume of phosphate-buffered saline (PBS) solution and subjected to probe sonication for at least 15 minutes Groups of PBS-instilled rats served as controls The lungs of PBS and particle-exposed rats were evaluated by BAL fluid analyses at 24 h, 1 week, 1 month, and 3 months postexposure (pe) For lung cell proliferation and histopathology studies, additional groups of animals were instilled with the particle-types listed above as well as a PBS solution

For the lung tissue studies, additional groups of animals (4 rats/group) were instilled with the particle-types listed above plus the vehicle control, i.e., PBS These studies were dedicated

to lung tissue analyses, but only the high-dose groups (5 mg/kg) and PBS controls were utilized

in the morphology studies These studies consisted of cell proliferation assessments and histo-pathological evaluations of the lower respiratory tract Similar to the BAL fluid studies, the intratracheal instillation exposure period was followed by 24-h, 1-week, 1-month, and 3-month recovery periods

Exposure groups

• PBS (vehicle control)Particle-types (1 and 5 mg/kg)

o R-100 fine-TiO2

o Pigment A-fine-TiO2coated with amorphous SiO2

o α-Quartz particles (positive control)

o Carbonyl iron (negative control) Instillation

exposure

Postexposure (pe) evaluation via BAL and lung tissue

24 h 1 week 1 month 3 months

FIGURE 18.2 Experimental design for bridging case study

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18.2.2 ANIMALS

Carolina) were used in this study The rats were approximately 8 weeks old at study start (mean weights in the range of 240–255 g) All procedures using animals were reviewed and approved by the Institutional Animal Care and Use Committee and the animal program is fully accredited by the Association for Assessment and Accreditation of Laboratory Animal Care (AAALAC)

18.2.3 PARTICLETYPES

The R-100 fine-titanium dioxide particles (w99 wt.% titanium dioxide, w1 wt.% alumina)

obtained from the DuPont Company A patented chloride process produced Pigment A

dioxide, w1 wt.% alumina, w3 wt.% amorphous silica (particle encapsulating)) possessing an

in the rutile crystal phase and hydrophilic in nature

Crystalline silica particles (a-quartz, Min-U-Sil 5) ranging in size from 0.3 to 3 mm were obtained from the US Silica Company Carbonyl iron (CI) particles ranging in size from 0.8 to 3.0 mm were obtained from GAF Corporation

18.2.4 LUNGCELLPROLIFERATIONSTUDIES

Groups of particulate-exposed rats and corresponding controls were pulsed 24 h after instillation,

as well as 1 week, 1 month, and 3 months postexposure, with an intraperitoneal injection of

dose of 100 mg/kg body weight The animals were euthanized 6 h later by pentobarbital injection Following cessation of spontaneous respiration, the lungs were infused with a neutral buffered

and the heart and lungs were carefully removed en bloc and immersion-fixed in formalin In addition, a 1 cm piece of duodenum (which served as a positive control) was removed and stored in formaldehyde Subsequently, parasagittal sections from the right cranial and caudal lobes and regions of the left lung lobes as well as the duodenal sections were dehydrated in 70% ethanol and sectioned for histology The sections were embedded in paraffin, cut, and mounted on glass slides The slides were stained with an anti-BrdU antibody, with an AEC (3-amino-9-ethyl carbazole) marker, and counter-stained with aqueous hematoxylin A minimum of 1000 cells/animal were counted in terminal bronchiolar and alveolar regions For each treatment group, immunostained nuclei in airways (i.e., terminal bronchiolar epithelial cells)

TABLE 18.1

and a-Quartz Particulates

Particle Crystallinity Surface Area (m 2 /g) Average ParticleDiameter (nm)

Pigment A coated with amorph SiO 2 Rutile 8 w290

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or lung parenchyma (i.e., epithelial, interstitial cells, or macrophages) were counted by light

18.2.5 BRONCHOALVEOLARLAVAGEMETHODS

The lungs of sham and particulate-exposed rats were lavaged with a warmed PBS solution as described previously Methodologies for cell counts, differentials, and pulmonary biomarkers in lavaged fluids were conducted as previously described [3,4] Briefly, the first 12 mL of lavaged fluids recovered from the lungs of PBS or particulate-exposed rats was centrifuged at 700 g, and

2 mL of the supernatant was removed for biochemical studies All biochemical assays were

alka-line phosphatase (ALP), and lavage fluid protein were measured using Roche Diagnostics

injury ALP activity is a measure of Type II alveolar epithelial cell secretory activity, and increased ALP activity in BAL fluids is considered to be an indicator of Type II lung epithelial cell toxicity Increases in BAL fluid micro protein (MTP) concentrations generally are consistent with enhanced permeability of vascular proteins into the alveolar regions, indicating a breakdown in the integrity

of the alveolar-capillary barrier

18.2.6 LUNGHISTOPATHOLOGYSTUDIES

The lungs of rats exposed to particulates or PBS controls were prepared for light microscopy by

month, and 3 months postexposure Sagittal sections of the left and right lungs were made using a razor blade Tissue blocks were dissected from left, right upper, and right lower regions of the lung and were subsequently prepared for light microscopy (paraffin embedded, sectioned, and hematox-ylin–eosin stained) [3,4]

18.2.7 STATISTICALANALYSES

For analyses, each of the experimental values were compared to their corresponding sham control values for each time point A one-way analysis of variance (ANOVA) and Bartlett’s test were calculated for each sampling time When the F test from ANOVA was determined to be significant, the Dunnett’s test was utilized to compare means from the control group and each of the groups exposed to particulates Significance was judged at the 0.05 probability level

18.3 RESULTS

18.3.1 LUNGWEIGHTS

Lung weights of rats were enhanced with increasing age on the study (i.e., increased postexposure time periods following intratracheal instillation exposures) Lung weights in high-dose quartz-exposed rats were slightly increased relative to controls at 1 week, and at 1 month and 3 months postexposure (data not shown)

18.3.2 LUNGCELLPROLIFERATIONRESULTS

Tracheobronchial cell proliferation rates (percentage of immunostained cells with BrdU) were measured only in high-dose (5 mg/kg) particulate-exposed rats and corresponding controls at

24 h, 1 week, 1 month, and 3 months postexposure (pe) Although increases in cell labeling

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indices were measured in R-100 fine-TiO2as well as a-quartz-exposed animals at 24 h postexpo-sure, these effects were not sustained (data not shown)

Lung parenchymal cell proliferation rates (percentage of immunostained cells with BrdU) were measured only in high-dose (5 mg/kg) particulate-exposed rats and corresponding controls at 24 h,

1 week, 1 month, and 3 months postexposure (pe) Small but significant transient increases in lung

particle-exposed rats at 24 h, but these effects were not sustained at any other postexposure time points Significantly larger increases in cell proliferation indices were measured in the lungs of a-quartz exposed rats measured from 24 h postexposure through 3 months postexposure (data not shown)

To summarize, exposures to 5 mg/kg quartz particles produced increased tracheobronchial cell proliferation compared to PBS controls, but increases were statistically significant only at 24 h postexposure In contrast to tracheobronchial cell labeling indices, exposures to 5 mg/kg quartz particles produced substantially greater lung parenchymal cell proliferation rates at all time points postexposure, suggesting a greater likelihood to result in lung cell genotoxicity or other adverse pulmonary effects over time with continued exposures

Total cells in BAL fluids of rats exposed to pigment A TiO2particles and other particulates

0.00E+00 5.00E+06 1.00E+07 1.50E+07 2.00E+07 2.50E+07 Control

1 mg/kg

5 mg/kg

1 mg/kg

5 mg/kg

1 mg/kg

5 mg/kg

1 mg/kg

5 mg/kg

Mean number total cells in BAL fluids

3 month

1 month

1 week

24 h

FIGURE 18.3 Total number of cells in BAL fluids recovered from particulate-exposed rats and controls as evidenced by % neutrophils (PMN) in BAL fluids at 24 h, 1 week, 1 month, and 3 months postexposure (pe) Values given are meansGS.D The numbers of BAL cells recovered from the lungs of high-dose quartz groups were substantially higher than any other groups for all postexposure time periods

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18.3.3 BRONCHOALVEOLARLAVAGEFLUIDRESULTS

18.3.3.1 Pulmonary Inflammation

The numbers of cells recovered by BAL from the lungs of high-dose a-quartz-exposed (5 mg/kg) groups were substantially higher than any of the other groups for all postexposure time periods (Figure 18.3) Intratracheal instillation exposures of virtually all particle-types produced a short-term pulmonary inflammatory response, as evidenced by an increase in the percentages/numbers of BAL-recovered neutrophils, measured at 24 h postexposure However, only the exposures to a-quartz particles (1 and 5 mg/kg) produced sustained pulmonary inflammatory responses, as measured through 3 months postexposure (Figure 18.4)

18.3.3.2 Bronchoalveolar Lavage (BAL) Fluid Parameters

Transient and reversible increases in (BAL) fluid LDH values, as an indicator of general

week postexposure, but were not sustained through the other postexposure time periods In contrast, exposures to high-dose (5 mg/kg) a-quartz particles produced a persistent enhancement in BAL

Percent neutrophils in BAL fluids of rats exposed to pigment A TiO2particles and other particulates

Control

1 mg/kg

5 mg/kg

1 mg/kg

5 mg/kg

1 mg/kg

5 mg/kg

1 mg/kg

5 mg/kg

Carbonyl iron

Mean % PMNs

3 month

1 month

1 week

24 h

* **

*

*

*

*

*

FIGURE 18.4 Pulmonary inflammation in particulate-exposed rats and controls as evidenced by % neutro-phils (PMN) in BAL fluids at 24 h, 1 week, 1 month, and 3 months postexposure (pe) Values given are meansGS.D Intratracheal instillation exposures of several particle-types produced a short-term, pulmonary inflammatory response, as evidenced by an increase in the percentages/numbers of BAL-recovered neutro-phils, measured at 24 h postexposure However, only the exposures to quartz particles (1 and 5 mg/kg) produced sustained pulmonary inflammatory responses, as measured through 3 months postexposure

*p!0.05

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Control 0.00 50.00 100.00 150.00 200.00 250.00

u/L

LDH

MTP

Alkaline phosphatase

300.00 350.00 400.00 450.00

1 mg/kg

5 mg/kg

1 mg/kg

5 mg/kg

1 mg/kg

5 mg/kg

1 mg/kg

5 mg/kg

Carbonyl iron

3 month

1 month

1 week

24 h

*

Control 0.00 10.00 20.00 30.00 40.00 50.00

mg/dL

60.00

1 mg/kg

5 mg/kg

1 mg/kg

5 mg/kg

1 mg/kg

5 mg/kg

1 mg/kg

5 mg/kg

Carbonyl iron

3 month

1 month

1 week

24 h

*

*

*

*

*

Control 0.00 20.00 40.00 60.00 80.00 100.00

u/L 120.00 140.00 160.00 180.00 200

1 mg/kg

5 mg/kg

1 mg/kg

5 mg/kg

1 mg/kg

5 mg/kg

1 mg/kg

5 mg/kg

Carbonyl iron

3 month

1 month

1 week

24 h

A

B

C

FIGURE 18.5 (See facing page.)

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Similarly, transient increases in BAL fluid microprotein (MTP) values were measured in the lung

different from control values at 1 week postexposure In contrast, exposures to 5 mg/kg a-quartz particles produced persistent increases in BAL fluid microprotein values at 24 h, 1 week, 1 month,

substantial increases in BAL fluid ALP values were measured at 1 week through 3 months post-exposure in rats exposed to 5 mg/kg a-quartz particles (Figure 18.5C)

To summarize the results from BAL fluid biomarker studies, intratracheal instillation exposures

to a-quartz particles resulted in sustained, dose-dependent, lung inflammatory responses, associ-ated with cytotoxic and lung permeability effects, measured from 24 h through 3 months

transient pulmonary inflammatory responses, and these effects were not sustained Exposures to

24 h postexposure; however, this was in large part related to the bolus dose associated with the intratracheal instillation exposure methodology

18.3.3.3 Pulmonary Histopathological Evaluations

Histopathological analyses of lung tissues revealed that pulmonary exposures to carbonyl iron, to

adverse effects when compared to PBS-exposed controls, as evidenced by the normal lung architecture observed in the exposed animals at postinstillation exposure time periods ranging

tissue section of a rat instilled with 5 mg/kg carbonyl iron particles at 1 month postexposure demonstrated appropriate alveolar macrophage phagocytic responses and normal lung

particle-exposed rats at each postexposure time period, and demonstrated normal pulmonary architecture

Histopathological analyses of lung tissues in rats exposed to a-quartz particulates in rats revealed that pulmonary exposures produced dose-dependent pulmonary inflammatory responses characterized by neutrophils and accumulations of foamy (lipid-containing) alveolar macrophage

In addition, lung tissue thickening as a prerequisite to the development of fibrosis was observed and progressive over postexposure time periods (Figure 18.6C and Figure 18.6D)

18.4 DISCUSSION

This chapter presents a case study and methodology designed to investigate the hazard potential of

FIGURE 18.5 BAL fluid analyses for particulate-exposed rats and corresponding controls at 24 h, 1 week,

1 month, and 3 months postexposure (pe) (A) LDH (lactate dehydrogenase), (B) MTP (microprotein values), and (C) alkaline phosphatase Values given are meansGS.D Transient and reversible increases in BAL fluid

postexpo-sure In contrast, exposures to 5 mg/kg a-quartz particles produced sustained increases in BAL fluid LDH values through the 3-month postexposure period *p!0.05

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compared with other negative control, reference particle-types such as R-100 fine-TiO2particles or carbonyl iron particles The combination of BAL and lung tissue studies concomitant with an experimental design consisting of dose-response, time-course evaluations, and the inclusion of reference particle-types provides a powerful tool for assessing the acute pulmonary toxicity of this new particle-type

The bioassay described herein provides evidence that toxicological information on a particle’s various surface treatments can be assessed in a routine systematic manner A beneficial feature of the bioassay is the ability to compare, via bridging strategies, the effects of inhaled versus instilled particulate materials In this regard, pulmonary bridging studies can generate important preliminary hazard data when assessing the safety of new developmental or commercial compounds or when making modifications to existing chemical products, such as surface coatings on particulates The strength of the bridging strategy is dependent upon having good inhalation toxicity data for comparisons to the instillation data The materials for which there is inhalation data can then be used as control particle-types for comparing with an intratracheal instillation bridging study (Figure 18.1) The basic idea for the bridging concept is that the effects of the instilled material serve as a control (known) material and then are “bridged” to the inhalation toxicity data for that material, as well as to the new materials being tested The results of bridging studies in rats are then useful as preliminary pulmonary toxicity screening (i.e., hazard) data, because consistency in the response of the inhaled and instilled control material serves to validate the responses with the newly

TB

AD

AD

TB

AD AD

A

C

B

D

FIGURE 18.6 Light micrographs of lung tissue from a rat exposed to (A) carbonyl iron particles (5 mg/kg) at

(A) and (B), these micrographs illustrate the terminal bronchial (TB) and corresponding alveolar ducts (AD) and demonstrate the lung architecture and normal macrophage phagocytosis of each particle (arrows) For (C) and (D), the arrows demonstrate accumulation of foamy alveolar macrophages in the alveolar regions of quartz-exposed rats

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