#METABOLOMICS WORKBENCH RCulpHill_20210318_135702_mwtab.txt DATATRACK_ID:2535 STUDY_ID:ST001731 ANALYSIS_ID:AN002818 PROJECT_ID:000000 VERSION 1 CREATED_ON March 24, 2021, 2:58 pm #PROJECT PR:PROJECT_TITLE Mitochondrial ATP fuels ABC transporter-mediated drug efflux in cancer PR:PROJECT_TITLE chemoresistance PR:PROJECT_SUMMARY Chemotherapy remains the standard of care for most cancers worldwide, however PR:PROJECT_SUMMARY development of chemoresistance due to the presence of the drug-effluxing ABC PR:PROJECT_SUMMARY transporters remains a significant problem. The development of safe and PR:PROJECT_SUMMARY effective means to overcome chemoresistance is critical for achieving durable PR:PROJECT_SUMMARY remissions in many cancer patients. We have investigated the energetic demands PR:PROJECT_SUMMARY of ABC transporters in the context of the metabolic adaptations of PR:PROJECT_SUMMARY chemoresistant cancer cells. Here we show that ABC transporters use PR:PROJECT_SUMMARY mitochondrial-derived ATP as a source of energy to efflux drugs out of cancer PR:PROJECT_SUMMARY cells. We further demonstrate that the loss of MCJ (DnaJC15), an endogenous PR:PROJECT_SUMMARY negative regulator of mitochondrial respiration, in chemoresistant cancer cells PR:PROJECT_SUMMARY boosts their ability to produce ATP from mitochondria and fuel ABC transporters. PR:PROJECT_SUMMARY We have developed novel MCJ mimetics that can attenuate mitochondrial PR:PROJECT_SUMMARY respiration and safely overcome chemoresistance in vitro and in vivo. PR:PROJECT_SUMMARY Administration of MCJ mimetics in combination with standard chemotherapeutic PR:PROJECT_SUMMARY drugs could therefore become an new strategy for treatment of multiple cancers. PR:INSTITUTE University of Colorado Denver PR:DEPARTMENT Biochemistry and Molecular Genetics PR:LABORATORY Angelo D'Alessandro PR:LAST_NAME Culp-Hill PR:FIRST_NAME Rachel PR:ADDRESS 12801 E 17th Ave L18-9403D, Aurora, Colorado, 80045, USA PR:EMAIL rachel.hill@cuanschutz.edu PR:PHONE 303-724-5798 #STUDY ST:STUDY_TITLE Mitochondrial ATP fuels ABC transporter-mediated drug efflux in cancer ST:STUDY_TITLE chemoresistance (part-II) ST:STUDY_SUMMARY Chemotherapy remains the standard of care for most cancers worldwide, however ST:STUDY_SUMMARY development of chemoresistance due to the presence of the drug-effluxing ABC ST:STUDY_SUMMARY transporters remains a significant problem. The development of safe and ST:STUDY_SUMMARY effective means to overcome chemoresistance is critical for achieving durable ST:STUDY_SUMMARY remissions in many cancer patients. We have investigated the energetic demands ST:STUDY_SUMMARY of ABC transporters in the context of the metabolic adaptations of ST:STUDY_SUMMARY chemoresistant cancer cells. Here we show that ABC transporters use ST:STUDY_SUMMARY mitochondrial-derived ATP as a source of energy to efflux drugs out of cancer ST:STUDY_SUMMARY cells. We further demonstrate that the loss of MCJ (DnaJC15), an endogenous ST:STUDY_SUMMARY negative regulator of mitochondrial respiration, in chemoresistant cancer cells ST:STUDY_SUMMARY boosts their ability to produce ATP from mitochondria and fuel ABC transporters. ST:STUDY_SUMMARY We have developed novel MCJ mimetics that can attenuate mitochondrial ST:STUDY_SUMMARY respiration and safely overcome chemoresistance in vitro and in vivo. ST:STUDY_SUMMARY Administration of MCJ mimetics in combination with standard chemotherapeutic ST:STUDY_SUMMARY drugs could therefore become an new strategy for treatment of multiple cancers. ST:INSTITUTE University of Colorado Denver ST:DEPARTMENT Biochemistry and Molecular Genetics ST:LABORATORY Angelo D'Alessandro ST:LAST_NAME Culp-Hill ST:FIRST_NAME Rachel ST:ADDRESS 12801 E 17th Ave L18-9403D, Aurora, Colorado, 80045, USA ST:EMAIL rachel.hill@cuanschutz.edu ST:PHONE 303-724-5798 #SUBJECT SU:SUBJECT_TYPE Cultured cells SU:SUBJECT_SPECIES Homo sapiens SU:TAXONOMY_ID 9606 #SUBJECT_SAMPLE_FACTORS: SUBJECT(optional)[tab]SAMPLE[tab]FACTORS(NAME:VALUE pairs separated by |)[tab]Raw file names and additional sample data SUBJECT_SAMPLE_FACTORS - control1 Factor:Control RAW_FILE_NAME=control1 SUBJECT_SAMPLE_FACTORS - control2 Factor:Control RAW_FILE_NAME=control2 SUBJECT_SAMPLE_FACTORS - control3 Factor:Control RAW_FILE_NAME=control3 SUBJECT_SAMPLE_FACTORS - control4 Factor:Control RAW_FILE_NAME=control4 SUBJECT_SAMPLE_FACTORS - siMCJ1 Factor:siMCJkd RAW_FILE_NAME=siMCJ1 SUBJECT_SAMPLE_FACTORS - siMCJ2 Factor:siMCJkd RAW_FILE_NAME=siMCJ2 SUBJECT_SAMPLE_FACTORS - siMCJ3 Factor:siMCJkd RAW_FILE_NAME=siMCJ3 SUBJECT_SAMPLE_FACTORS - siMCJ4 Factor:siMCJkd RAW_FILE_NAME=siMCJ4 #COLLECTION CO:COLLECTION_SUMMARY MCF7 cells were purchased from American Type Culture Collection (ATCC). All CO:COLLECTION_SUMMARY cancer cell lines were maintained in RPMI 1640 (Sigma R8758) containing glucose CO:COLLECTION_SUMMARY (2 mg/ml) and glutamine (0.6 mg/ml) but no pyruvate and was supplemented with 5% CO:COLLECTION_SUMMARY Fetal calf serum. CO:SAMPLE_TYPE Cultured cells #TREATMENT TR:TREATMENT_SUMMARY MCF7 cell transfections were performed using siPORT NeoFX Transfection Agent TR:TREATMENT_SUMMARY (ThermoFisher Scientific) following the recommended protocol for an TR:TREATMENT_SUMMARY oligonucleotide siRNA based on the previously described MCJ targeting sequence. #SAMPLEPREP SP:SAMPLEPREP_SUMMARY All cancer cell lines were maintained in RPMI 1640 (Sigma R8758) containing SP:SAMPLEPREP_SUMMARY glucose (2 mg/ml) and glutamine (0.6 mg/ml) but no pyruvate and was supplemented SP:SAMPLEPREP_SUMMARY with 5% Fetal calf serum. Metabolic profile comparisons of cells were performed SP:SAMPLEPREP_SUMMARY on equal cell numbers. Cells were cultured under normal conditions, detached SP:SAMPLEPREP_SUMMARY using trypsin-EDTA (0.05 %), counted, normalized to 0.5 x 10e6 in each sample, SP:SAMPLEPREP_SUMMARY and cell pellets were snap frozen in liquid nitrogen prior to analysis. Briefly, SP:SAMPLEPREP_SUMMARY 2 x 10e6 cells and 20μL cell media were extracted in 1mL and 980μL cold lysis SP:SAMPLEPREP_SUMMARY and extraction buffer (methanol : acetonitrile : water, 5:3:2), respectively, SP:SAMPLEPREP_SUMMARY and pellets were discarded. #CHROMATOGRAPHY CH:CHROMATOGRAPHY_SUMMARY Negative Mode 10 μL of water and methanol soluble fractions were run through a CH:CHROMATOGRAPHY_SUMMARY Kinetex C18 1.7 μm, 100 x 2.1 mm (Phenomenex) reversed phase column (Negative CH:CHROMATOGRAPHY_SUMMARY ion mode – phase A: 1 mM NH4Ac 95:5 water : acetonitrile; phase B: 1 mM NH4Ac CH:CHROMATOGRAPHY_SUMMARY 95:5 acetonitrile : water) via an ultra-high performance chromatographic system CH:CHROMATOGRAPHY_SUMMARY (UHPLC - Vanquish, Thermo Fisher). UHPLC was coupled in line with a CH:CHROMATOGRAPHY_SUMMARY high-resolution quadrupole Orbitrap instrument run in negative polarity mode CH:CHROMATOGRAPHY_SUMMARY (QExactive, Thermo Fisher) at 70,000 resolution (at 200 m/z). Gradients and CH:CHROMATOGRAPHY_SUMMARY other technical parameters and the variants employed herein have been CH:CHROMATOGRAPHY_SUMMARY extensively described. CH:CHROMATOGRAPHY_TYPE Reversed phase CH:INSTRUMENT_NAME Thermo Vanquish CH:COLUMN_NAME Phenomenex Kinetex C18 (150 x 2.1mm, 2.6 um) #ANALYSIS AN:ANALYSIS_TYPE MS #MS MS:INSTRUMENT_NAME Thermo Q Exactive Orbitrap MS:INSTRUMENT_TYPE Orbitrap MS:MS_TYPE ESI MS:ION_MODE NEGATIVE MS:MS_COMMENTS UHPLC was coupled in line with a high-resolution quadrupole Orbitrap instrument MS:MS_COMMENTS run in negative polarity mode (QExactive, Thermo Fisher) at 70,000 resolution MS:MS_COMMENTS (at 200 m/z). Gradients and other technical parameters and the variants employed MS:MS_COMMENTS herein have been extensively described. #MS_METABOLITE_DATA MS_METABOLITE_DATA:UNITS Relative Abundance MS_METABOLITE_DATA_START Samples control1 control2 control3 control4 siMCJ1 siMCJ2 siMCJ3 siMCJ4 Factors Factor:Control Factor:Control Factor:Control Factor:Control Factor:siMCJkd Factor:siMCJkd Factor:siMCJkd Factor:siMCJkd ATP 1254300 1530584 995836 958442 1172597 860470 890423 779232 ADP 6062622 7955310 5602974 5072800 7228896 6342440 6842992 6700468 AMP 32556540 31746980 29555320 22912970 32130200 27251380 24645710 28246100 GTP 124908 136036 71206 57904 71946 55728 45124 44497 GDP 566391 731503 441869 417703 605072 518753 584348 565662 GMP 5863058 5720972 5323990 4369844 5765728 4915186 5296294 5309808 Guanosine 184637 200140 224381 230934 198290 202758 210254 234991 Cytidine 4258840 4081814 3979304 3723048 3679043 3794888 4158999 4078820 dTMP 411511 429250 485030 352213 483114 463847 380226 458784 Thymine 372827 355949 339870 304087 408072 362376 392651 421047 UDP 2405901 2709062 2410566 2182940 3024296 2483881 3412353 3136296 UMP 18035190 18319170 15641880 13280450 19345150 14814690 16090320 17774450 Inosine 2169625 1967127 2384894 2400882 2238472 2021310 2558873 2838437 Hypoxanthine 6860700 7321158 6882526 6655866 7745394 6562548 8191108 8814087 Xanthine 117782 113028 117431 98068 123021 89240 131549 136834 (S)(+)-Allantoin 98624 155866 111863 117258 146701 101435 159993 145454 3',5'-Cyclic AMP 380352 330791 273790 330435 216173 228182 241637 326333 5'-Phosphoribosyl-N-formylglycinamide 1006487 1064766 813768 799089 859778 661648 863961 884149 5-6-Dihydrothymine 5289740 5171485 5010136 4178330 5552880 4710194 5459394 5261210 Pyridoxal 77857 95526 91445 95018 177061 131465 167540 139187 UDP-glucose 3653380 3493188 2978648 2779505 3249187 2494146 2863122 2477913 Diphosphate 11289200 11573440 11066300 10486700 10877330 9102285 10798810 11402520 D-Glucose 313115 361059 362209 405710 634458 595383 636154 663155 D-Fructose 1-6-bisphosphate 804793 840657 737929 678194 770357 736081 844272 723142 2/3-Phospho-D-glycerate 371953 437780 577738 675923 502133 485860 565517 445766 Pyruvate 857692 586692 712240 597797 705659 511209 678480 707869 Lactate 99169860 103555700 100624600 86221250 107050900 85463360 106173000 109132600 Mannitol 358611 356649 1694934 1320946 481049 362446 814153 572011 D-Arabitol 84435 88475 82179 74284 111884 93793 123191 141977 Citrate 16947670 15848090 14117900 13776620 13266000 11757570 13457180 13584280 2-Oxoglutarate 75375 77974 93350 89229 78770 64490 75362 81925 Succinate 13116930 15193850 11575270 11157310 13738470 11741650 14665800 15966020 Fumarate 2576042 2734026 2415042 2376355 2985058 2251292 3186203 3329032 Malate 20146110 19592960 17385440 16860250 22124660 17198740 24288390 26901990 2-Hydroxyglutarate/Citramalate 210640 197732 168370 191753 187260 163526 206275 230365 6-Phospho-D-gluconate 295199 191750 246602 235570 306045 229841 272630 314959 alpha-D-Ribose 1-phosphate 1277626 1163309 1256278 1355930 1008270 1137660 1211630 1351017 5-Oxoproline 25693300 24988140 22985370 22522250 27009610 21710950 25953930 25440620 S-Glutathionyl-L-cysteine 54479 129703 117643 92305 205193 199424 296115 262389 Ascorbate 497502 594698 502170 502201 735509 556435 756336 732785 Dehydroascorbate 256522 281027 230112 252942 251598 210344 223946 222209 gamma-L-Glutamyl-D-alanine 960131 778232 868993 878824 875188 783620 1003342 878359 Dimethylglycine 1154989 1137117 982330 1015306 1187938 1042712 1212398 1362486 Argininosuccinate 982536 1165253 915336 873787 1128066 941351 1141313 1113643 UDP-N-acetyl-D-glucosamine 24491450 23210390 21126130 18737620 24766050 18033610 22331370 18059450 CMP-N-acetylneuraminate 86112 90328 77382 71631 112023 66512 99514 79291 N-Acetylornithine 125452 133242 100055 111005 98479 115803 122869 133571 trans-4-Hydroxy-L-proline 4872758 4482142 4430822 4105438 5598324 4854798 5688126 5104546 Pantothenol 1362851 1488301 996820 875921 1211968 982701 1397303 1160601 5-6-Dihydrouracil 1110577 1039200 976594 763332 1046147 1062221 1052752 1023356 L-Methionine S-oxide 55844 41614 30716 42270 66012 44709 51428 26496 5-Hydroxyindoleacetate 253555 230227 198427 203415 257974 200634 269094 273664 Indole 29775 27821 28361 26927 36856 30704 35785 34315 quinolinic acid 397788 459096 374195 329539 454323 354074 458894 485588 g-Oxalo-crotonate 65875 71575 90277 82450 99906 84382 113278 109916 Glycerol 3-phosphate 613026 867648 540304 574563 829118 549075 783487 815413 Ethanolamine phosphate 4859090 4268548 4652242 4026841 6680066 5494050 6257162 6691882 N-Methylethanolamine phosphate 598252 510990 614603 506422 700694 496993 647677 667469 sn-glycero-3-Phosphoethanolamine 16993300 16567120 14804800 13322880 17145990 15428490 12634840 15733880 CDP-choline 82260 107749 97313 121942 159146 106890 180757 203211 Pentanoate (valerate) 35819 39556 40807 47239 68585 65924 80118 86424 Hexanoic acid (caproate) 101152 128391 164320 166387 275949 287758 308075 325484 Cholesterol sulfate 2946209 1880575 2905510 4511776 6379068 3975874 5950348 7280414 Glycochenodeoxycholic acid 8750 13280 12094 8935 9303 12091 9220 11288 Tauroursodeoxycholic/taurochenodeoxycholic/taurodeoxycholic acid 21766 37584 26999 25254 22329 29121 22541 19325 S-Acylglutathione 207225 264194 258222 191920 205525 204185 275029 269634 Oxalosuccinate 8345 12707 17996 22311 38096 31260 49171 53897 MS_METABOLITE_DATA_END #METABOLITES METABOLITES_START metabolite_name CmpdID parent medRt ATP C00002 505.9879 0.62 ADP C00008 426.0219 0.65 AMP C00020 346.0555 0.71 GTP C00044 521.9827 0.62 GDP C00035 442.0166 0.63 GMP C00144 362.0505 0.68 Guanosine C00387 282.0841 0.75 Cytidine C00475 242.0791 0.72 dTMP C00364 321.0498 0.71 Thymine C00178 125.0343 0.71 UDP C00015 402.9945 0.62 UMP C00105 323.0283 0.67 Inosine C00294 267.0731 0.75 Hypoxanthine C00262 135.0300 0.73 Xanthine C00385 151.0251 0.75 (S)(+)-Allantoin C02350 157.0355 0.74 3',5'-Cyclic AMP C00575 328.0451 0.76 5'-Phosphoribosyl-N-formylglycinamide C04376 313.0441 0.67 5-6-Dihydrothymine C00906 127.0499 0.73 Pyridoxal C00250 166.0499 0.77 UDP-glucose C00029 565.0473 0.63 Diphosphate C00013 176.9349 0.65 D-Glucose C00031 179.0552 0.72 D-Fructose 1-6-bisphosphate C00354 338.9883 0.62 2/3-Phospho-D-glycerate C00631 184.9846 0.63 Pyruvate C00022 87.0073 0.70 Lactate C01432 89.0229 0.69 Mannitol C00392 181.0703 0.75 D-Arabitol C01904 151.0604 0.73 Citrate C00158 191.0188 0.66 2-Oxoglutarate C00026 145.0131 0.63 Succinate C00042 117.0179 0.65 Fumarate C00122 115.0023 0.65 Malate C00149 133.0129 0.64 2-Hydroxyglutarate/Citramalate C02630 147.0288 0.65 6-Phospho-D-gluconate C00345 275.0176 0.62 alpha-D-Ribose 1-phosphate C00620 229.0114 0.67 5-Oxoproline C01879 128.0340 0.69 S-Glutathionyl-L-cysteine C05526 425.0806 0.67 Ascorbate C00072 175.0239 0.59 Dehydroascorbate C05422 173.0081 0.65 gamma-L-Glutamyl-D-alanine C03738 217.0823 0.71 Dimethylglycine C01026 102.0546 0.68 Argininosuccinate C03406 289.1150 0.67 UDP-N-acetyl-D-glucosamine C00043 606.0743 0.64 CMP-N-acetylneuraminate C00128 613.1400 0.63 N-Acetylornithine C00437 173.0922 0.74 trans-4-Hydroxy-L-proline C01157 130.0497 0.75 Pantothenol C00864 218.1028 0.75 5-6-Dihydrouracil C00429 113.0343 0.71 L-Methionine S-oxide C02989 164.0375 0.73 5-Hydroxyindoleacetate C05635 190.0527 0.75 Indole C00463 116.0492 1.80 quinolinic acid C03722 166.0162 0.71 g-Oxalo-crotonate C03453 157.0123 0.94 Glycerol 3-phosphate C00093 171.0053 0.67 Ethanolamine phosphate C00346 140.0106 0.72 N-Methylethanolamine phosphate C01210 154.0264 0.70 sn-glycero-3-Phosphoethanolamine C01233 214.0478 0.71 CDP-choline C00307 487.0990 0.67 Pentanoate (valerate) C00803 101.0594 1.80 Hexanoic acid (caproate) C01585 115.0751 1.86 Cholesterol sulfate C18043 465.3048 2.12 Glycochenodeoxycholic acid C05466 448.3067 1.86 Tauroursodeoxycholic/taurochenodeoxycholic/taurodeoxycholic acid BA109 498.2892 1.86 S-Acylglutathione C02589 333.0590 0.67 Oxalosuccinate C05379 189.0066 1.28 METABOLITES_END #END