bioRxiv preprint doi: https://doi.org/10.1101/2020.04.25.061903; this version posted April 27, 2020. The copyright holder for this preprint (which was not certified by peer review) is the author/funder. All rights reserved. No reuse allowed without permission.

1 DNA Methylation-based Signatures Classify Sporadic Pituitary Tumors According to

2 Clinicopathological Features.

3 Maritza S. Mosella 1,2,3, Thais S. Sabedot 1,2, Tiago C. Silva 3,#, Tathiane M. Malta 1,2,&,

4 Felipe D. Segato 3,*, Karam P. Asmaro 1,2, Michael Wells 1,2, Abir Mukherjee 4, Laila M.

5 Poisson 5, James Snyder 2, Ana C. deCarvalho 1, Tobias Walbert T 2, Todd Aho 6, Steven

6 Kalkanis 1, Paula C. Elias 7; Sonir R. Antonini 8, Jack Rock 1, Houtan Noushmehr 1,2,3,↟ ,

7 Margaret Castro 7↟ ; Ana Valeria Castro1,2,↟ ,^

8 1Department of Neurosurgery, Hermelin Brain Tumor Center, Henry Ford Health System,

9 Detroit, MI, USA. 2Department of Neurosurgery, Omics Laboratory, Henry Ford Health

10 System, Detroit, MI, USA. 3Department of Genetics, Ribeirao Preto Medical School,

11 University of São Paulo, Ribeirao Preto, Brazil. 4Department of Pathology, Henry Ford

12 Health System, Detroit, MI, USA. 5Department of Biostatistics, Henry Ford Health System,

13 Detroit, MI, USA; 6Department of Radiology, Henry Ford Health System, Detroit, MI, USA.

14 7Internal Medicine Department, Ribeirao Preto Medical School, University of São Paulo,

15 Ribeirao Preto, Brazil. 8Department of Pediatrics, Ribeirao Preto Medical School, University

16 of São Paulo, Ribeirao Preto, Brazil.

17 ^Corresponding author:

18 Ana Valeria Castro

19 Scientist/Professor

20 Department of Neurosurgery

21 Hermelin Brain Tumor Center

22 Henry Ford Health System

23 2799 West Grand Blvd, E&R 3096

24 Detroit, MI, 48202

25 [email protected]

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26 Running title

27 DNA-methylation markers classify pituitary tumors

28 Funding

29 This work was supported by the Henry Ford Health System, Department of Neurosurgery,

30 and the Hermelin Brain Tumor Center. Additionally, MSM and MC are supported by The

31 São Paulo Research Foundation (FAPES), Brazil ( #16/11039-3; #17/10357-4,#14/03989-6);

32 AC and KPA by Henry Ford Hospital (A30935, A30957; GME 202199); LMP, HN, AD,

33 MW, and AM are supported by the National Institutes of Health (R01CA222146), HN, TSS,

34 TMM, LMP, and AD are supported by the Department of Defense (CA170278).

35 Conflict of interest

36 The authors declare to have no competing interests.

37 Authorship

38 Overall concept and coordination of the study: AVC, MC, HN, SA, PE; retrieval of publicly

39 available molecular and clinical data: MSM; Bioinformatic and statistical analyses: MSM,

40 TSS, TCS, TMM, FSD, HN and input from LMP; HFHF cohort: pathology review MF, AM;

41 clinicopathological and radiological data were generation and collection: AVC, MSM, KPA,

42 AM, MF, TA; molecular data generation: AC, TMM; manuscript was written by MSM,

43 AVC, HN, intellectual contribution: JS, SK, TW. All authors contributed to the revision of

44 the manuscript. # Present address: University of Miami, FL, USA & Present address:

45 University of São Paulo, Ribeirao Preto, Brazil * Present address: Cedars-Sinai Medical

46 Center, Los Angeles, CA, USA. ↟ Contributed equally

47 Word count

48 Abstract: 230

49 Article text: 3,182

50 Reference list: 1,187

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51 Figures and Tables captions: 782

52 Manuscript text: 5,095 (Title: 414; abstract: 230; article text: 3,182; Acknowledgements: 82;

53 reference list: 1,187)

54

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55 ABSTRACT

56 Background: Distinct genome-wide methylation patterns have consistently clustered pituitary

57 neuroendocrine tumors (PT) into molecular groups associated with specific clinicopathological

58 features. Here we aim to identify, characterize and validate the methylation signatures that

59 objectively classify PT into those molecular groups.

60 Methods: Combining in-house and publicly available data, we conducted an analysis of the

61 methylome profile of a comprehensive cohort of 177 tumor and 20 non-tumor specimens from

62 the pituitary gland. We also retrieved methylome data from an independent pituitary tumor

63 (PT) cohort (N=86) to validate our findings.

64 Results: We identified three methylation clusters associated with functional status and

65 adenohypophyseal cell lineages using an unsupervised approach. We also identified signatures

66 based on differentially methylated CpG probes (DMP), some of which overlapped with

67 pituitary-specific factors (SF1 and Tpit), that significantly distinguished

68 pairs of clusters related to functional status and adenohypophyseal cell lineage. These findings

69 were reproduced in an independent cohort, validating these methylation signatures. The DMPs

70 were mainly annotated in enhancer regions associated with pathways and genes involved in

71 cell identity and tumorigenesis.

72 Conclusions: We identified and validated methylation signatures that distinguished PT by

73 distinct functional status and adenohypophyseal cell lineages. These signatures, annotated in

74 enhancer regions, indicate the importance of these elements in pituitary tumorigenesis. They

75 also provide an unbiased approach to classify pituitary tumors according to the most recent

76 classification recommended by the WHO 2017 using methylation profiling.

77 Key-words: DNA methylation; classification; regulatory elements; enhancers; pituitary

78 tumors.

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79 Key-points

80 ● Distinct methylation landscapes define PT groups with specific functional

81 status/subtypes and adenohypophyseal lineages subtypes.

82 ● Methylation abnormalities in each cluster mainly occur in CpG annotated in distal

83 regions overlapping predicted enhancers regions associated with pathways and genes

84 involved in cell identity and tumorigenesis.

85 ● DNA methylation signatures provide an unbiased approach to classify PT.

86 Importance of the study

87 This study harnessed the largest methylome data to date from a comprehensive cohort

88 of pituitary specimens obtained from four different institutions. We identified and validated

89 methylation signatures that distinguished pituitary tumors into molecular groups that reflect the

90 functionality and adenohypophyseal cell lineages of these tumors. These signatures, mainly

91 located in enhancers, are associated with pathways and genes involved in cell identity and

92 tumorigenesis. Our results show that methylome profiling provides an objective approach to

93 classify PT according to the most recent classification of PT recommended by the 2017 WHO.

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94 1 Introduction

95 Pituitary tumors (PT), a type of neuroendocrine tumors, comprise the second most

96 common neoplasm of the central nervous system (CNS) (~17%) 1–3 with an annual average

97 age-adjusted incidence of 4.08 per 100,000 population 3. Stratified by endocrine status, PT are

98 classified as functioning (FPT) (46-64%) or nonfunctioning (NFPT) (36%–54%) subtypes, the

99 latter also referred to as silent adenomas 1,4. In relation to the histopathological classification

100 the most recent recommendation by the World Health Organization (WHO) in 2017 is based

101 on immunostaining for adenohypophyseal hormones and cell-lineage 5. Despite its importance

102 and extensive use for tumor classification, the immunopathology method is limited by its

103 subjectivity and inaccuracy in pituitary and several other tumors 6,7. To circumvent these

104 limitations and/or to complement pathology results, inclusion of genomic-based signatures

105 such as recurrent somatic mutations and number alterations has advanced and

106 refined the classification of many tumors, including CNS neoplasms 8,9. However, in contrast

107 to other CNS tumors, genomic alterations are rare in PT or are restricted to some subtypes (i.e.

108 GNAS mutation in somatotroph adenomas) 10–12. Contrariwise, distinct genome-wide DNA

109 methylation patterns are consistently associated with their clinicopathological features such as

110 function and histological variants. In contrast to other CNS tumors, the importance of

111 methylation markers in the taxonomy of PT has not been explored to date 7,10,13–17. A recent

112 study reported that the combination of genome-wide molecular profiling of multiple platforms,

113 including DNA methylation, provided an objective approach to the classification of PT 10.

114 However, the identification of specific methylation signatures to classify PT into these

115 methylome-based groups has not been exploited.

116 To address this knowledge gap, we aimed to identify, characterize and validate

117 methylation-based markers that define PT according to clinicopathological features. For this

118 purpose, we compiled and performed a comprehensive analysis of the genome-wide DNA

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119 methylation data on 177 adult sporadic tumors and 20 non-tumorous tissue from the pituitary

120 gland obtained from a multicenter source and validated our findings in an independent cohort.

121 We identified methylation signatures that classified PT according to methylation groups that

122 reflected the functionality and the adenohypophyseal lineages of these tumors.

123 2 Subjects and methods

124 2.1 Patients and tissue specimens

125 DNA methylation data were retrieved from 3 publicly available cohort datasets (data

126 retrieval freeze on August 2018) 7,13,14 and from our cohort at the Hermelin Brain Tumor Center

127 (HBTC) of the Henry Ford Health System (Detroit, MI, USA) (n=23; HBTC cohort,

128 unpublished). The final cohort consists of 20 non-neoplastic pituitary glands (non-tumor/NT)

129 and 177 PT from patients over 18 years (Pan-pit), composed of 87 FPT and 90 NFPT. Clinical

130 information about this study cohort is summarized in Table 1 and detailed in Supplementary

131 Table S1. The PT clinicopathological classification criteria of features such as invasion from

132 our internal cohort were matched with the criteria provided by the authors of the external

133 cohorts 7,13,14. Specific transcription factor-based adenohypophyseal lineages were assigned to

134 each PT subtype in accordance with the 2017 WHO classification 5. All the studies were

135 approved by their respective Institutional Review Boards and ethics committees and written

136 consent obtained from each patient at the attending institutions 7,10,13,14.

137 2.2 Data retrieval and preprocessing

138 DNA from pituitary tissue was obtained from fresh-frozen (FF) 13,14 or formalin-fixed-

139 paraffin-embedded specimens (FFPE) 7. The method of DNA extraction, processing, and

140 assays for each cohort included in this study is reported in the respective manuscripts 7,13,14 and

141 for the HBTC cohort is available in the Supplementary Methods. The IDAT files for the DNA

142 methylation bead arrays (450K or 850K/EPIC) from the Ling, Kober, and Capper cohorts 7,13,14,

143 were retrieved through the GEOquery package 18 and preprocessed simultaneously using minfi

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144 package19. The EPIC array data from Capper and HBTC were processed separately using the

145 same approach. Detailed information about preprocessing of IDAT files is depicted in

146 Supplementary methods. Principal component analysis (PCA) revealed that there were no

147 batch effects related to the cohort, tissue sources (FFPE or FF) and array platform (450K/EPIC)

148 (Supplementary Figure S1A-C). The HBTC DNA methylation data was submitted to

149 Expression Omnibus (GSEXXXX).

150 To test the reproducibility of our findings, we retrieved the methylome data from 86

151 patients with PT obtained from an independent study published after our data freeze (EMBL-

152 EBI accession number E-MTAB-7762) 10.

153 2.3 Unsupervised and supervised analysis of the PT methylome

154 To reduce noise, the most variable probes were sorted according to standard deviation

155 across the 177 PT specimens. Next, a consensus clustering analysis20 was applied to the top

156 1% most variant probes (n=4,526). Agglomerative hierarchical clustering with 1000

157 resampling steps, upon euclidean distance was used, as described previously 8,20. Optimal

158 clusters were selected based on statistical parameters: Calinski-Harabasz curve and consensus

159 cluster delta area and overlapped with clinicopathological annotations.

160 Two-tailed Wilcoxon rank sum tests were conducted for each CpG in order to identify

161 pairwise differentially methylated probes (DMP) between the methylation clusters and

162 invasion status. DMP were defined based on differences in mean methylation (diffmean) and

163 adjusted p-value significance. For those comparisons with the highest number of significant

164 probes (e.g. for NFPT-e vs. FPT-e), we applied a more stringent adjusted p-value cutoff, in

165 order to retrieve DMP sets with similar number of probes. An absolute diffmean of 0.3 was

166 used as a threshold for all methylation clusters comparisons. Between ACTH-e vs. NFPT-e

167 clusters comparison adjusted p-values <1e-17 were obtained for both hypo- and

168 hypermethylated probes; for ACTH-e vs. FPT-e and NFPT-e vs. FPT-e comparisons, the

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169 following adjusted p-values for the respective hypo and hypermethylated probes were obtained:

170 p< 1e-16 and p<1e-19 and p<1e-21 p<1e-38, respectively. No significant adjusted p-values

171 were obtained from the invasion status comparative analysis, therefore, the results are related

172 to non-adjusted p-value <0.001 along with delta diffmean of 0.15, similar to the approach

173 reported by other authors 13,14.

174 CpG probes were mapped to their CpG genomic location as CpG islands (CGI), shores,

175 shelves, and open sea regions as previously defined 21–24. DMPs were integrated with predicted

176 enhancers listed in the GeneHancer database 25 through the Genomic Ranges package

177 (https://bioconductor.org/packages/release/bioc/html/GenomicRanges.html). Enrichment or

178 depletion frequencies of DMP sets by genomic location and enhancer overlap were calculated

179 as Odds Ratio using the 485,000 probes from HM450K platform as the reference.

180 Determination of the number of overlapping and distinct DMPs (hyper or

181 hypomethylated) between pairwise comparisons were calculated using the UpsetR package 26.

182 2.4 DNA motif analysis

183 To predict transcription factor binding sites, we surveyed the DNA motifs within

184 enhancer regions which overlapped our DMPs (namely enhancer-related DMP or eDMP).

185 Sequence motifs were identified within ±200 bp from the core of the hyper- or hypomethylated

186 enhancer regions using the bioinformatic tools HOMER 27 . To increase the sensitivity of motif

187 detection, up to two mismatches were allowed in each oligonucleotide sequence. The

188 distributions of motif content in ‘target’ (i.e., the enhancer regions) and random ‘background’

189 sequences were assessed for fold change values.

190 2.5 Integrative analysis between methylation and enhancer prediction databank

191 We identified CpG probes that overlapped with their predicted regulatory regions listed

192 in the GeneHancer database 25. Based on the GeneHancer’s annotation confidence score for

193 functional enhancers 25, the highest scored enhancers for each DMP set were selected. The

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194 selected enhancers were connected to their putative target genes as defined by four

195 experimental metrics 25. The genes with the highest enhancer-gene pairing association score

196 were selected (GeneHancer interaction score)25 and their expressions per methylation cluster

197 are depicted as boxplots .

198 2.6 Methylation status of pituitary-specific transcription factors-related probes

199 We assessed the DNA methylation profile of CpG probes related to pituitary-specific

200 transcription factor (TF) coding genes, known to determine the development of various

201 adenohypophyseal cell types in the pituitary gland: Pit-1 (POU1F1), Tpit (TBX19), ER-alpha

202 (ESR1), GATA2 and SF1 (NR5A1) 1,22. Next, we overlapped the pituitary-specific TF-related

203 probes with the three DMP sets obtained from the pairwise comparison between the clusters.

204 For each significant TF-related probe, we established methylation degree cutoffs that

205 distinguished between clusters. The accuracy of these cutoffs in defining PT subtypes was

206 investigated in the validation cohort 10.

207 3 Results

208 3.1 Genome-wide DNA methylation patterns define three groups of pituitary tumors

209 related to specific functional subtypes and adenohypophyseal cell-lineages.

210 Consensus clustering of the most variable DNA methylation probes in the pan-pit

211 dataset, revealed three main clusters. The clusters were named according to their enrichment

212 for specific functional subtypes (Figure 1A-B and Supplementary Figure S1C). The

213 adrenocorticotropic hormone-enriched cluster (ACTH-e; n=29) is composed mainly of

214 corticotroph adenomas (n=21) and 8 NFPT, including 1 silent corticotroph adenoma, 1

215 gonadotroph, 1 null cell adenoma and 5 of unknown histological NFPT subtypes. The NFPT-

216 e cluster (n=82) consists mainly of NFPT (n=69), including 60 gonadotrophs, 7 null cell

217 tumors, and 2 mixed non-functioning adenomas (LH/FSH/TSH), 1 FPT (lactotroph adenoma)

218 and 12 tumors with unknown histological subtypes. The FPT-e cluster (n=66) is composed

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219 mainly of FPT (n=65), i.e., 41 somatotrophs, 11 thyrotrophs, 8 lactotrophs, 5

220 plurihormonal/mixed adenomas (2 GH/PRL, 1 GH/TSH, 2 GH/PRL/TSH) and 1 NFPT

221 (gonadotroph). The top most variant probes (according to standard deviation) across tumor

222 specimens (n=4,526) are hypomethylated in the FPT-e cluster, hypermethylated in the NFPT-

223 e cluster, and present an intermediate methylation pattern in the ACTH-e cluster (Figure 1B

224 and 1C). ACTH-e, NFPT-e and FPT-e clusters are composed mainly by Tpit- (22/24; 92%);

225 SF1- (60/70; 86%) and Pit-1 (65/66; 98%) cell lineages-derived subtypes, respectively.

226 3.2 Differential methylation between the three methylation-based PT clusters is observed

227 in distal regions overlapping enhancer elements.

228 The supervised comparisons between the clusters retrieved three DMP sets totaling

229 3,316 differentially methylated probes (Figure 2A discovery heatmap) that distinguished

230 among the groups which were validated in an external cohort 10 (Figure 2A, validation

231 heatmap). We observed that 1,973 (59%) out of 3,316 DMPs were located in enhancer regions

232 (Figure 2A, left row label track). DMPs were enriched in open sea regions (n=2,257, 68%),

233 while depleted in CGI, for the three pairwise methylation cluster comparisons (Figure 2B).

234 Detailed information about the distribution of the number of DMPs according to methylation

235 direction and CpG annotation is depicted in Table S2 (Supplemental material). The survey of

236 common or exclusive DMPs among the methylation cluster comparisons are depicted in Figure

237 2C and D, based on the methylation direction (hypo or hypermethylated).

238 When we surveyed for DNA motifs in differentially methylated enhancer candidates

239 that overlapped our DMPs, we identified 31 TF predicted to bind to DNA motifs in the 295

240 hypomethylated eDMP from the comparison between ACTH-e vs. NFPT-e (adjusted p-

241 value<0.05). The top binding site was predicted to bind to Fra1/Fra2 subunits of the Activator

242 (AP-1) (Figure 3A). Hypermethylated eDMP (n=88) predicted to bind to NR5A2

243 presented a trend to be significant (adjusted p-value= 0.06). Hypermethylated DMP from

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244 ACTH-e vs. FPT-e comprised cluster-related hypermethylated eDMP (n=360) presented Basic

245 -Leucine Zipper domain (bZIP) motifs predicted to bind to 17 TFs, which are also known to

246 interact with AP-1 subunits (Figure 3A). NFPT-e vs. FPT-e comparison retrieved

247 hypermethylated eDMP-related DNA motifs (n=398) predicted to bind to 12 TF. The top most

248 enriched TF was Jun, another subunit of AP-1 and related to the bZIP DNA binding

249 (Figure 3A). No adjusted significant DNA motifs were retrieved from the hypomethylated

250 eDMP regions from ACTH-e vs. FPT-e or from NFPT-e vs. FPT-e comparisons (n=15 or 48

251 hypo-DMP, respectively). The eDMPs related to the top three high-scored enhancers are

252 depicted in Figure 3B. Their respective associated target gene (TEAD3, PTCH1 and BAHCC1)

253 expression levels are depicted in Figure 3C.

254 We observed a tendency of a negative association between the methylation degree of

255 the eDMP and the expression of some of their putative target genes (p>0.05). For instance, in

256 association with the correspondent hypomethylation in the eDMP, the expression of TEAD3

257 was higher in ACTH-e than in the NFPT-e cluster (Figure 3C). Hypomethylated eDMP in the

258 FPT-e cluster (compared to ACTH-e) was related to upregulation of PTCH1 (Figure 3B-C) and

259 ERCC6L2 target genes (not shown) in the FPT-e cluster. In the comparison between NFPT-e

260 and FPT-e, we identified a cluster of 3 CpG probes overlapping a large enhancer

261 (GH171061384) that presented a heterogeneous methylation pattern. Two out of three probes

262 in this eDMP were hypomethylated in NFPT-e in relation to FPT-e. Their putative highest

263 scored target genes, BAHCC1 and a lncRNA (AC110285.7), were upregulated in NFPT-e. A

264 Genome Browser overview is used to highlight chromatin interactions between the top

265 enhancer and putative genes pairs (Figure 3D).

266 3.3 Pituitary-related transcription factors Tpit (TBX19) and SF1 (NR5A1)-related probes

267 differentiate specific methylation clusters.

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268 We investigated whether pituitary-specific TF probes were differentially methylated

269 among the clusters. We found 125 probes-related to these TF (data not shown). Among the

270 pituitary-specific TF investigated in our analysis, SF1 (NR5A1) and Tpit (TBX19) were

271 significantly differentially methylated between two or three clusters (Figure 4A). SF1-related

272 DMPs were all located within enhancer intronic regions (n=2), while Tpit-related DMPs mainly

273 overlapped promoter (n=3) and intronic regions (n=2). SF1 DMPs were significantly

274 hypermethylated in ACTH-e and FPT-e when compared to the NFPT-e (Figure 4A). Tpit-

275 DMPs were entirely hypomethylated in ACTH-e in comparison with NFPT-e

276 (promoter/intronic) and significantly distinguished from FPT-e-DMPs by hypomethylation in

277 the promoter region (Figure 4B). The intronic Tpit region also distinguished the

278 hypermethylated NFPT-e from the hypomethylated FPT-e cluster (Figure 4A). Taken together,

279 T-pit methylation significantly distinguished all three methylation clusters; SF1 intronic

280 methylation distinguished ACTH-e and NFPT-e and, less significantly, NFPT-e from FPT-e

281 cluster. We established SF-1-related cutoffs for the two probes that significantly distinguished

282 ACTH-e and NFPT-e. Specimens that presented SF1-related probes with methylation values

283 below 0.5 (cg14143574) and 0.3 (cg02853418) were assigned to belong to NFPT-e, while beta-

284 values above those cutoffs were considered to belong to ACTH-e cluster (Figure 4B). The

285 application of these cutoffs to the Neou cohort correctly assigned 95% to either ACTH/T-pit

286 or NFPT/ SF1 specimens (χ2-squared p-value = 1.68e-08). Likewise, three out of five T-pit-

287 related DMP accurately distinguished ACTH-e from non-ACTH-e specimens (NFPT-e and

288 FPT-e). Specimens with CpG methylation below the thresholds for at least two out of those 3

289 probes, i.e. 0.5 (cg26160839), 0.7 (cg01732037) and 0.5 (cg15140722), assigned samples to

290 the ACTH-e group (Figure 4B). Applying this criteria to the validation cohort 10, 75% of the

291 ACTH tumors were classified accordingly while 100% of the other functioning and

292 nonfunctioning PT were assigned as the nonACTH category (χ2-squared p-value = 7.56 e-14).

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293 4 Discussion

294 We conducted a comprehensive and integrative analysis between the molecular and

295 clinicopathological features of the largest multicentric methylome cohort of pituitary gland

296 specimens to date. An unsupervised analysis of the methylome cohort defined three groups of

297 PT characterized by hypo-, hyper- or intermediately methylated profiles mainly segregated by

298 functionality (functioning and nonfunctioning) as well as adenohypophyseal cell lineages,

299 namely FPT-e, NFPT-e and ACTH-e, respectively, similar to the results reported in recent

300 studies 10,15. These methylation clusters contain subtypes that recall and provide an epigenetic

301 support for the pituitary cell lineages-based criteria to classify PT recommended by the 2017

302 WHO classification, particularly to the Pit-1-derived tumors 5.

303 Notably, in the NFPT-e cluster, the methylome similarities between gonadotrophs and

304 null cell adenomas reported by us and others 10,15,28 may indicate that hypermethylation

305 underlies the pathogenesis of the lack of production and/or secretion of adenohypophyseal

306 hormones. In addition, we and others showed that silent and functioning corticotroph adenomas

307 (i.e. overt Cushing’s disease and subclinical) shared a more similar methylation profile

308 compared to each other and with NFPT. These results are concordant with a report that silent

309 ACTH and gonadotroph tumors share cytopathological features and clinical behavior 29.

310 Taking into account that cell-specific methylation patterns are preserved during development

311 and tumorigenesis, it is also possible that null cell, a subset of gonadotrophs and of corticotroph

312 adenomas share a common precursor 30,31 10,32,33 (Figure 1B). In addition, a study showed that

313 a subset of functioning corticotroph adenoma displayed a more intermediate methylation

314 profile between FPT and NFPT 10,32,33. Specific gene mutations such as GATA3 and USP8

315 accounted for the differences among these corticotroph adenomas variants 10,28. Altogether,

316 these results show that corticotroph adenomas consist of a molecularly heterogeneous tumor

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317 10,15,28. Whether the association between methylation patterns and mutations in these variants

318 are drivers or passengers remains to be elucidated.

319 Pairwise comparisons between the methylation clusters yielded the identification of a

320 significant number of DMP (Figure 2A) that were mainly located in enhancer regions and

321 enriched for open sea CpGs (Figure 3B). Validating our findings, the overlap of either the DMP

322 or the top eDMP with the methylome, assigned the specimens of an independent cohort 10 into

323 similar methylation and clinicopathological groups as we observed in the pan-pit cohort. These

324 novel results indicate that these regulatory regions may play key roles in pituitary

325 tumorigenesis as well as in cell-specific development and differentiation as described in other

326 tumors 34. The biological significance of the differentially methylated enhancers across the

327 methylation clusters are endorsed by their association with target genes involved in pathways

328 related to developmental cytodifferentiation and in the tumorigenic process (e.g. TEAD3,

329 TAF11, lnRNA/AC110285.7, ERCC6L2, PTCH1) (Figures 3B,C)35–42.

330 Recently, the integration of multiple platforms including genomic and epigenomic

331 features has been proposed as an unbiased molecular approach to classify PT 10. Despite its

332 thoroughness, the complexity and the current cost of profiling multiple platforms to classify a

333 sample may limit its application in the clinics. Interestingly, their methylation profiles showed

334 similar clusters of PT as we described here. In addition the methylation-based groups were

335 similar to the ones obtained using the pangenomic approach 10. Altogether, these findings

336 provide evidence that methylome profiling per se may be a reliable and an unbiased approach

337 to classify PT 10. In our analysis, we were able to identify specific methylation thresholds

338 related to SF-1 and T-pit genes that significantly distinguished ACTH-e/Tpit from NFPT-e/SF1

339 methylation groups in our cohort that correctly assigned ACTH and NFPT specimens in the

340 independent cohort 10. These results, if validated by other methods (e.g. , pyrosequencing),

15 bioRxiv preprint doi: https://doi.org/10.1101/2020.04.25.061903; thisDNA version Methylation-based posted April 27, 2020. Clusters The copyright in Pituitary holder for Tumors this preprint (which was not certified by peer review) is the author/funder. All rights reserved. No reuse allowed without permission.

341 suggest that the methylation degree of these probes could be used as an objective approach to

342 classify PT specimens according to adenohypophyseal cell lineage.

343 The prognostic and predictive significance of methylation-based stratification in PT is

344 not clear, in contrast to the findings reported in other CNS tumors such as gliomas and

345 meningiomas 8,43. We and others showed that PT methylation clusters were not associated with

346 features used as surrogates of aggressive behavior in PT (e.g. invasion, resistance to treatment

347 etc) 5,10,28. However, the association of PT methylation clusters with a prognostic grading which

348 has been validated as predictors of tumor aggressive behavior remains to be investigated

349 8,43,44,45.

350 Besides refining tumor classification and stratification, methylome profiling can also

351 be applied to differentiate tumors originated from different tissues 7,46. Indeed, one study

352 showed that distinct methylome patterns segregated PT apart from other CNS tumors7.

353 Potentially, PT-specific signatures, as the ones herein described, could be helpful to distinguish

354 PT from other primary or secondary sellar tumors whose diagnosis by morphologic and

355 immunohistochemical approaches may be challenging and inconclusive 7,47,48.

356 In summary, we identified and validated methylation signatures that distinguished PT

357 by distinct functional status/subtype and adenohypophyseal cell lineages. These signatures,

358 annotated in enhancer regions, indicate the importance of these elements in the pathogenesis

359 of these tumors. They also provide an unbiased approach to classify pituitary tumors according

360 to the most recent classification recommended by the 2017 WHO using methylation profiling.

361

362 Acknowledgements

363 The authors are grateful to the HFHS patients who consented to the usage of PT for research

364 purposes. We thank Nancy Takacs and Heather Mengel for their administrative support;

365 Kevin Nelson for the collection, handling and maintenance of the tumor bank at the Hermelin

16 bioRxiv preprint doi: https://doi.org/10.1101/2020.04.25.061903; thisDNA version Methylation-based posted April 27, 2020. Clusters The copyright in Pituitary holder for Tumors this preprint (which was not certified by peer review) is the author/funder. All rights reserved. No reuse allowed without permission.

366 Brain Tumor Center; Andrea Transou for tumor pathology processing; Laura A. Hasselbach

367 for DNA extraction; Daniel Weisenberger and team at USC Epigenome Center for assistance

368 with DNA methylation profiling (HFHS support);Susan MacPhee for proofreading the

369 manuscript.

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514 Figure captions

515 Figure 1 - Methylome landscape segregates pituitary tumors into three distinct groups in

516 a multicenter cohort.

517 (A) Consensus Cluster correlation heatmap depicting three identified methylation-based

518 groups among pituitary tumors.

519 (B) Heatmap of the most variant CpG methylated probes (n=4,526) among 177 pituitary tumors

520 according to their methylation-based cluster and for 20 non-tumor pituitary specimens.

521 Columns represent specimens; rows represent the CpG probes.

522 (C) Boxplots depicting the mean DNA methylation of the top most variant probes according

523 to non-tumor and tumor pituitary specimens methylation groups.

524 Figure 2 - Differentially methylated distal probes define three clusters.

525 A) Heatmap of the differentially methylated CpG probes (DMPs) from pairwise comparisons

526 among clusters. Heatmap on the left displays the methylation landscape of the pan-pit cohort

527 (discovery, n=177) and the heatmap on the right depicts the methylation patterns of the

528 corresponding CpG applied to the Neou cohort (validation, n=86).

529 (B) Odds Ratio for the frequencies of DMPs for each pairwise comparison, depicting genomic

530 location and enhancer overlap relative to the expected genome-wide distribution of 450K

531 probes. Relative to the first cluster of the pairwise comparison label, red- and blue-shaded

532 boxes represent hypermethylated and hypomethylated probes respectively.

533 (C) Barplots showing the number of hypermethylated DMP that are unique or common in the

534 intersection among the three differentially methylated probe sets.

535 (D) Barplots showing the number of hypomethylated DMP that are unique or common in the

536 intersection among the three differentially methylated probe sets.

537 Figure 3 - Differentially methylated candidate enhancers predicted AP-1 and NR5A2

538 transcription factors and respective putative enhancer-target genes.

24 bioRxiv preprint doi: https://doi.org/10.1101/2020.04.25.061903; thisDNA version Methylation-based posted April 27, 2020. Clusters The copyright in Pituitary holder for Tumors this preprint (which was not certified by peer review) is the author/funder. All rights reserved. No reuse allowed without permission.

539 (A) Representation of DNA motifs significantly enriched among differentially methylated

540 enhancer regions obtained from the pairwise comparison between ACTH-e, NFPT-e and FPT-

541 e.

542 (B) Methylation of probes in the top three highest-scored enhancers.

543 (C) Expression of the high scored enhancer-target genes expression, per methylation cluster.

544 (D) Genome browser view of top enhancers and the highest scored target genes, depicting the

545 GENCODE transcripts, the predicted chromatin interactions and the conservation among

546 vertebrates.

547 Figure 4 - Pituitary-specific transcription factors found differentially methylated among

548 the three methylation clusters.

549 (A) Heatmap indicating significant differentially methylated probes associated with SF-1

550 (NR5A1) and T-pit (TBX19) among the three methylation clusters: ACTH-e, NFPT-e and

551 FPT-e. Heatmap on the left displays the pan-pit cohort (discovery, n=177) and the heatmap on

552 the right depicts the methylation patterns of the corresponding CpG applied to the Neou cohort

553 (validation, n=86).

554 (B) Density plots on the distribution of beta value and tentative thresholds (vertical dashed

555 lines) for SF-1- and T-pit-related differentially methylated probes that distinguish the ACTH-

556 e from NFPTs and ACTH from non-ACTHs, respectively.

557 Table caption

558 Table 1 - Clinicopathological classification features of pituitary tumors from a multicenter

559 cohort. NFPT: Nonfunctioning pituitary tumor; Supplementary Figures

560 Figure S1 - Principal component analysis (PCA) colored by (A) cohort source; (B) by PT

561 functional status; (C) by methylation cluster; (D) Cumulative distribution function of consensus

562 clustering classification and (E) Consensus cluster delta area plot of consensus clustering

563 classification.

25 bioRxiv preprint doi: https://doi.org/10.1101/2020.04.25.061903; thisDNA version Methylation-based posted April 27, 2020. Clusters The copyright in Pituitary holder for Tumors this preprint (which was not certified by peer review) is the author/funder. All rights reserved. No reuse allowed without permission.

564 Figure S2 - DNA methylation-based stemness index (mDNAsi) of pan-pituitary cohort

565 specimens, according to methylation clusters and clinicopathological features.

566 (A) By methylation clusters.

567 (B) By functional status.

568 (C) By the high risk subtypes according to the 2017 WHO classification.

569 (D) By gender.

570 (E) By age.

571 *=p<0.05;**=p<0.01;***=p<0.001;****=p<0.0001

572 Figure S3 - Supervised analysis of the methylome according to invasion status.

573 (A) Heatmap of the 13 differentially methylated probes between invasive vs. noninvasive PT

574 (n=34 vs. n=46, respectively; p< 0.001 and ∆β=0.15).

575 (B) Venn diagram depicting common and distinct differentially methylated genes from our

576 study compared to several studies.

577 (C) Differentially methylated probes overlapping enhancer regions (eDMPs) and the respective

578 candidate enhancer-target genes correlation according to genomic context.

579 (D) Differentially methylated probes overlapping enhancer regions (eDMPs) and the respective

580 candidate enhancer-target genes correlation according to invasion status.

581 Figure S4 - DNA methylation-based stemness index and RNA-based stemness index of

582 Pan-pit cohort and integrative subset cohort based on the invasion status.

583 (A) DNA methylation-based stemness index (mDNAsi) of the pan-pituitary specimens cohort

584 colored by invasion status (n=197).

585 (B) DNA methylation-based stemness index (mDNAsi) of a subset of the pan-pituitary cohort

586 colored by invasion status (n=23)

587 (C) RNA expression-based stemness index (mRNAsi) of a PT cohort subset, colored by

588 invasion status (n=23).

26 bioRxiv preprint doi: https://doi.org/10.1101/2020.04.25.061903; thisDNA version Methylation-based posted April 27, 2020. Clusters The copyright in Pituitary holder for Tumors this preprint (which was not certified by peer review) is the author/funder. All rights reserved. No reuse allowed without permission.

589 Supplementary tables

590 Table S1 - Compiled clinical information for each patient pituitary specimen.

591 Table S2 - Differentially methylated probes from supervised comparisons. 1-3) differentially

592 methylated probes (DMP) among the three methylation clusters comparisons; 4) DMPs

593 between tumorous and non-tumorous pituitary specimens. 5) DMPs between invasive and

594 noninvasive PT.

595

27 bioRxiv preprint doi: https://doi.org/10.1101/2020.04.25.061903; this version posted April 27, 2020. The copyright holder for this preprint (which was not certified by peer review) is the author/funder. All rights reserved. No reuse allowed without permission.

A B PITUITARY ADENOMAS (n=177) NT (n=20) PITUITARY ADENOMAS (n=177) Methylation cluster samples (n=197) Cell lineage TF samples (n=197) Functional status Cohort Hormone staining WHO 2017_High risk Gender Age

Correlation Methylation 1 1 0.8 0.8 0.6 0.6 0.4 0.4 0.2 0.2 0 0

PROBE LEGEND CpG Location CpG.island Shore Shelf Open.sea Top 1% most variant probes (n= 4,526) 1% Top (n= probes variant most

C Top 1% most variant probes (n= 4,526)

0.8 lation

y 0.6 Methylation cluster

th Non-tumor ACTH−e NFPT−e SAMPLE LEGEND A me FPT−e Methylation cluster Functional status Hormone staining WHO 2017.High risk 0.4 ACTH−e Functioning ACTH Yes NFPT−e Nonfunctioning GH No FPT−e GH/PRL Undetermined GH/TSH Cell lineage TF Cohort GH/PRL/TSH Gender Female mean DN Pit−1 Nontumor-Kober GH densely T−pit Nontumor-Capper GH sparsely Male 0.2 Pit−1, ER-α Nontumor-HFHS LH and/or FSH Age Pit−1, GATA2 Tumor-Ling LH/FSH/TSH 18−20 SF−1, GATA2, ER-α Tumor-Kober TSH 20−40 SF−1, GATA2, ER-α, Pit-1 Tumor-Capper Non-tumor ACTH-e NFPT-e FPT-e PRL 40−60 All Tumor-HFHS PRL densely 60−80 None Null cell >80 Methylation cluster Unknown Unknown bioRxiv preprint doi: https://doi.org/10.1101/2020.04.25.061903; this version posted April 27, 2020. The copyright holder for this preprint (which was not certified by peer review) is the author/funder. All rights reserved. No reuse allowed without permission.

A DISCOVERYDISCOVERYDISCOVERY VALIDATION NT (n=20) TUMOR (n=177) TUMOR (n=86) MethMethylationyMethylationlation clust cluster clusterer Functional group CellCell Celllineag lineage lineagee TF TF TF TF cell lineage WHOWHOWHO 2017 2017 2017 WHO 2017

SAMPLE LEGEND

Methylation cluster Functional group

(n=1,067) ACTH−e ACTH NFPT-e NFPT

ACTH vs NFPT FPT-e FPT

NFPT-e vs ACTH-e silent ACTH subclinical ACTH

Cell lineage TF TF cell lineage Pit−1 Pit−1 T−pit T−pit Pit−1, ERalpha SF−1 Methylation Pit−1, GATA2 None 1 SF−1, GATA2, ERalpha 0.8 0.6 SF−1, GATA2, ERalpha, Pit−1

(n=1,039) 0.4 All 0.2 None

FPT vs ACTH 0 Unknown

FPT-e vs ACTH-e PROBE LEGEND

WHO 2017 CpG Location Corticotroph CpG island Silent corticotroph Shore Somatotroph Shelf Mammosomatotroph Open sea Plurihormonal Densely somatotroph Enhancer Sparsely somatotroph No Gonadotroph Yes Thyrotroph (n=1,210) Lactotroph Null cell FPT NFPT vs Undetermined FPT-e vs NFPT-e n er o i c at an c h o L En G Cp

B ACTH-e vs. FPT-e C D ACTH-e vs. NFPT-e ACTH-e vs. FPT-e NFPT-e vs. FPT-e Enhancer 800 733 793 750 630 Not enhancer 600

500 ion Size Open.sea ion Size 400 e 345 r sect sect u t er er

a Shelf 220 250 e Int 200 Int F 131 Shore 17 9 37 0 0 1

CpG.island

0 1 2 3 0 1 2 3 0 1 2 3 900 600 300 0 800 600 400 200 0 Odds−ratio Set Size Set Size

LEGEND Significance Probe direction DMP sets Depleted ACTH-e (n=29) vs. NFPT-e (n=82) Hypermethylated probes Enriched ACTH-e (n=29) vs. FPT-e (n=66) Hypomethylated probes Non-significant NFPT-e (n=82) vs. FPT-e (n=66) bioRxiv preprint doi: https://doi.org/10.1101/2020.04.25.061903; this version posted April 27, 2020. The copyright holder for this preprint (which was not certified by peer review) is the author/funder. All rights reserved. No reuse allowed without permission.

A Hypo enhancers in ACTH-e (n=295) from ACTH-e vs. NFPT-e Hyper enhancers in ACTH-e (n=88) from ACTH-e vs. NFPT-e Hyper enhancers in ACTH-e (n=360) from ACTH-e vs. FPT-e p.value =1e-3; 3.9 Fold p.value =1e-11; 3.2 Fold

bZIP motif AP-1(Fra1/Fra2) NR motif Nr5a2

2 2

1 1 mation content mation content or or 0 Inf Inf 0 1 2 3 4 5 6 7 8 9 10 11 12 1 2 3 4 5 6 7 8 9 10 Position Position B C

NT (n=20) PITUITARY ADENOMAS (n=177)

Methylation cluster Top enhancer target-genes expression Methylation Cell lineage TF 1 GH06I035483 GH09I095503 GH17I081384 0.8 Functional status PTCH1 BAHCC1 0.6 TEAD3 Hormone staining 0.4 0.2 WHO 2017_High risk 0 Gender SAMPLE LEGEND Methylation cluster WHO 2017_High risk 0.6 Age ACTH−e Yes NFPT−e No FPT−e Undetermined Functional status cg02333187_GH06I035483 Functioning Gender Nonfunctioning Female Male Cell lineage TF Pit−1 Age 0.4 T−pit 18−20

=5) Pit−1, ER-α 20−40 cg13754720_GH09I095503 Pit−1, GATA2

(n 40−60 2(TPM + 1)

n SF−1, GATA2, ER-α

60−80 g o o i SF−1, GATA2, ER-α, Pit-1 >80 l

at All l

y None h Unknown et PTCH1 0.2 cg06636541_GH17I081384 Hormone staining m ACTH er GH c GH/PRL an GH/TSH h cg11031567_GH17I081384 GH/PRL/TSH En GH densely GH sparsely LH and/or FSH 0.0 LH/FSH/TSH TSH ACTH−e NFPT−e ACTH−e FPT−e NFPT−e FPT−e cg26218110_GH17I081384 PRL PRL densely Null cell Unknown

D chr6 (p21.31) 6p22.3 6q126q13 q14.1 q15 16.1 6q21 22.31 26 6q27

10 kb hg38 35,485,000 35,490,000 35,495,000 35,500,000 35,505,000 GENCODE Transcript Set TEAD3 TEAD3

483 Predicted chromatin interactions D3 GH06I035483 TEAD3 TEA 4.88 _ 100 vertebrates Basewise Conservation by PhyloP GH06I035 0 - -4.5 _ 21.1 21.3 9p23 (q22.32) chr9

chr9 (q22.32) 9p23 21.3 21.1 11 9q12 13 31.1 32 33.1

200 kb hg38

D3 95,600,000 95,700,000 95,800,000 95,900,000 96,000,000

PTCH1 PTCH1 GENCODE Transcript Set ERCC6L2 PTCH1 PTCH1 PTCH1 PTCH1 TEA PTCH1 9IPTCH1095503 PTCH1 PTCH1 ERCC6L2 PTCH1 ERCC6L2 PTCH1

503 ERCC6L2 ERCC6L2 H1 Predicted chromatin interactions C GH09I095503 ERCC6L2 PT PTCH1 GH09I095

100 vertebrates Basewise Conservation by PhyloP 4.88 _

0 - -4.5 _

21.1 21.3 9p23 (q22.32) chr9 chr17 (q25.3) 13.3 13.2 p13.1 17p12 17p11.2 17q11.2 17q12 21.31 17q22 23.2 q24.3 q25.1 17q25.3

10 kb hg38 81,385,000 81,390,000 81,395,000 81,400,000 81,405,000 81,410,000 GENCODE Transcript Set

BAHCC1 AC110285.6 BAHCC1 384

C1 Predicted chromatin interactions

BAHCC1 GH17I081384 AHC B

GH17I081 100 vertebrates Basewise Conservation by PhyloP 4.88 _

0 - -4.5 _ bioRxiv preprint doi: https://doi.org/10.1101/2020.04.25.061903; this version posted April 27, 2020. The copyright holder for this preprint (which was not certified by peer review) is the author/funder. All rights reserved. No reuse allowed without permission.

A DISCOVERY VALIDATION

NT (n=20) PITUITARY ADENOMAS (n=177) PITUITARY ADENOMAS (n=86) Methylation cluster Functional group Cell lineage TF TF cell lineage WHO 2017 WHO 2017

cg14143574 SF-1 cg02853418

Methylation cg15140722 1 0.8 0.6 cg01732037 0.4 0.2 0 T-pit cg26160839

cg06941869

cg17095936

SAMPLE LEGEND Methylation cluster Cell lineage TF WHO 2017 ACTH−e Pit−1 Corticotroph NFPT-e T−pit Silent corticotroph FPT-e Pit−1, ERalpha Somatotroph Pit−1, GATA2 Mammosomatotroph SF−1, GATA2, ERalpha Plurihormonal Functional group SF−1, GATA2, ERalpha, Pit−1 Densely somatotroph ACTH All Sparsely somatotroph NFPT None Gonadotroph FPT Unknown Thyrotroph silent ACTH Lactotroph subclinical ACTH TF cell lineage Null cell Pit−1 Undetermined T−pit SF−1 None

B SF-1 (NR5A1) cg14143574 cg02853418 1.00 Methylation cluster 0.75 ACTH−e 0.50 NFPT−e FPT−e 0.25

0.00 0.00 0.25 0.50 0.75 1.00 0.00 0.25 0.50 0.75 1.00

NFPT-e ACTH-e NFPT-e ACTH-e

y / Count T-pit (TBX19) cg26160839 cg01732037 cg15140722 1.00 Densit

0.75

0.50

0.25

0.00 0.00 0.25 0.50 0.75 1.00 0.00 0.25 0.50 0.75 1.00 0.00 0.25 0.50 0.75 1.00

ACTH-e Non-ACTHs ACTH-e Non-ACTHs ACTH-e Non-ACTHs

cg26160839 DNA methcg26160839ylation level cg26160839