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Identification of a Noxo1 inhibitor by addition of a polyethylene glycol chain
Mokhtarpour, Nazanin ; Sterling, Alyssa ; Garcia, Joshua J. , et al. Bioorgan. Med. Chem.,2023,85,117274. DOI: 10.1016/j.bmc.2023.117274 PubMed ID: 37031566
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Abstract: Reactive oxygen species (ROS) are a heterogeneous group of highly reactive ions and mols. derived from mol. oxygen (O2) which can cause DNA damage and lead to skin cancer. NADPH oxidase 1 (Nox1) is a major producer of ROS in the skin upon exposure to UV light. Functionally, Nox1 forms a holoenzyme complex that generates two superoxide mols. and reduces NADPH. The signaling activation occurs when the organizer subunit Noxo1 translocates to the plasma membrane bringing a cytochrome P 450, through interaction with Cyba. We propose to design inhibitors that prevent Cyba-Noxo1 binding as a topical application to reduce UV-generated ROS in human skin cells. Design started from an apocynin backbone structure to generate a small mol. to serve as an anchor point. The initial compound was then modified by addition of a polyethylene glycol linked biotin. Both inhibitors were found to be non-toxic in human keratinocyte cells. Further in vitro experiments using isothermal calorimetric binding quantification showed the modified biotinylated compound bound Noxo1 peptide with a KD of 2 nM. Both using isothermal calorimetric binding and MALDI (TOF) MS showed that binding of a Cyba peptide to Noxo1 was blocked. In vivo experiments were performed using donated skin explants with topical application of the two inhibitors. Experiments show that UV light exposure of with the lead compound was able to reduce the amount of cyclobutene pyrimidine dimers in DNA, a mol. known to lead to carcinogenesis. Further synthesis showed that the polyethylene glycol but not the biotin was essential for inhibition.
Keywords: Reactive oxygen species ; Apocynin ; UV ; Noxo1 ; Cyba ; Cyclobutane pyrimidine dimer ; CPD ; UV protection
Purchased from AmBeed: 615-43-0 ; 58-85-5 ; 351422-73-6 ; 158407-04-6 ; 103-67-3 ; 103-67-3
CAS No. : | 158407-04-6 | MDL No. : | MFCD04115538 |
Formula : | C11H20BrNO2 | Boiling Point : | - |
Linear Structure Formula : | - | InChI Key : | YGJXBTRLYHCWGD-UHFFFAOYSA-N |
M.W : | 278.19 | Pubchem ID : | 15512811 |
Synonyms : |
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Chemical Name : | tert-Butyl 4-(bromomethyl)piperidine-1-carboxylate |
Signal Word: | Warning | Class: | N/A |
Precautionary Statements: | P261-P305+P351+P338 | UN#: | N/A |
Hazard Statements: | H302-H315-H319-H335 | Packing Group: | N/A |
GHS Pictogram: |
* All experimental methods are cited from the reference, please refer to the original source for details. We do not guarantee the accuracy of the content in the reference.
Yield | Reaction Conditions | Operation in experiment |
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With sodium hydride; In N,N-dimethyl-formamide; at 60℃; for 24h; | To a pressure vial equipped with a stir bar was added rt-butyl 4- (bromomethyl)piperidine-1-carboxylate (4.95 g, 17.8 mmol), <strong>[4983-28-2]2-chloropyrimidin-5-ol</strong>(Intermediate No.86 Step 2, 2.3 g, 17.8 mmol) and DMF (59 mL). Sodium hydride (60 wtpercent, 0.47 g, 19.6 mmol) was added and the vial was sealed and heated to 60 °C for 24 hours. The crude reaction mixture was diluted with ethyl acetate and filtered through a column pre-packed with Celite. The filtrate was concentrated in vacuo and the residue purified by flash chromatography (MPLC, 0-50percent EtOAc-hexanes) to give tert-butyl 4-[(2-chloropyrimidin-5- y l)oxy]methyl } piperidine- 1 -carboxylate.LRMS (ESI) calc'd for CI 1H15C1N303 [M+H]+: 272, Found: 272 (carbamic acid). |
Yield | Reaction Conditions | Operation in experiment |
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32 mg | A mixture of <strong>[628692-15-9](2-methoxypyrimidin-5-yl)boronic acid</strong> (48 mg, 0.315 mmol), 3-(l-(4-methoxybenzyl)- lH-pyrazol-4-yl)-4,5,7,8-tetrahydro-lH-oxepino[4,5-c]pyrazole (100 mg) and DMAP (75 mg, 0.617 mmol) were combined in MeCN (1 mL) and treated with copper (II) acetate (84 mg, 0.462 mmol). The reaction mixture was stirred for three days at 40 °C, open to air, then allowed to cool to room temperature. The material was mixed with a batch that had been similarly prepared using (2-methoxypyrimidin-5- yl)boronic acid (131 mg, 0.848 mmol), 3-(l-(4-methoxybenzyl)-lH-pyrazol-4-yl)-4,5,7,8-tetrahydro- lH-oxepino[4,5-c]pyrazole (250 mg, 0.771 mmol), DMAP (188 mg, 1.541 mmol) and copper (II) acetate (210 mg, 1.156 mmol) in MeCN (5 mL).The combined reaction mixtures were treated with ammonium hydroxide (10 mL), water (10 mL) and partitioned with EtOAc (15 mL). The organic layer was isolated, and the aqueous layer re-extracted with EtOAc (2 x 15 mL). The combined organic layer was washed with brine (15 mL), passed through a hydrophobic frit and concentrated under reduced pressure, then loaded in MeOH (4 mL) onto an SCX-SPE cartridge that had been pre-conditioned with MeOH. The SCX-SPE cartridge was eluted with MeOH (3 x 15 mL) and combined eluants concentrated under reduced pressure to give a crude mixture the title compounds (308 mg). LCMS (Method C): Rt = 0.97 min, MH+ 433. Crude material was taken forward to the next reaction step without further purification. Intermediate 13. 2-(2-Methoxypyrimidin-5-yl)-3-(lH-pyrazol-4-yl)-4.5,7,8-tetrahydro- 2H-oxepinor4.5-c1pyrazole and l-(2-methoxypyrimidin-5-yl)-3-(lW-pyrazol-4-yl)- 4.5.7.8-tetrahydro-lH-oxepinor4.5-c1pyrazole A crude mixture of 3-(l-(4-methoxybenzyl)-lH-pyrazol-4-yl)-2-(2-methoxypyrimidin-5-yl)-4,5,7,8- tetrahydro-2H-oxepino[4,5-c]pyrazole and 3-(l-(4-methoxybenzyl)-lH-pyrazol-4-yl)-l-(2- methoxypyrimidin-5-yl)-4,5,7,8-tetrahydro-lH-oxepino[4,5-c]pyrazole (308 mg) in DCM (2 mL) was treated with TFA (2 mL, 26.0 mmol) and then heated using a microwave at 70 °C for 6 h. The reaction mixture was neutralised to pH 7 using sodium bicarbonate, diluted with water (10 mL) and extracted with EtOAc (15 mL). The organic layer was isolated, and the aqueous layer re-extracted with EtOAc (2 x 15 mL). The combined organic layer was washed with brine (10 mL), passed through a hydrophobic frit and concentrated under reduced pressure to give a crude mixture of the title compounds (232 mg). LCMS (Method C): Rt = 0.67 min, MH+ 313. Crude material was taken forward to the next reaction step without further purification. Intermediate 14. tert-Butyl 4-((4-(2-(2-methoxypyrimidin-5-yl)-4.5.7.8-tetrahydro-2W- oxepinor4.5-c1pyrazol-3-yl)-lW-pyrazol-l-yl)methyl)piperidine-l-carboxylate and tert- butyl 4-((4-(l-(2-methoxypyrimidin-5-yl)-4,5,7,8-tetrahydro-lH-oxepinor4,5-c1pyrazol- 3-yl)-lH-pyrazol-l-yl)methyl)piperidine-l-carboxylate A crude mixture of the 2-(2-methoxypyrimidin-5-yl)-3-(lH-pyrazol-4-yl)-4,5,7,8-tetrahydro-2H- oxepino[4,5-c]pyrazole and l-(2-methoxypyrimidin-5-yl)-3-(lH-pyrazol-4-yl)-4,5,7,8-tetrahydro-lH- oxepino[4,5-c]pyrazole (232 mg) was dissolved in DMF (2 mL) and placed under an atmosphere of nitrogen. The mixture was treated with NaH (17 mg, 0.423 mmol, 60percent suspension in mineral oils) and stirred for 30 min then treated with tert-butyl 4-(bromomethyl)piperidine-l-carboxylate (86 mg, 0.310 mmol) and stirred for a further 24 h. The reaction mixture was acidified to pH 5 using a 2 M solution of HCI and diluted with water (25 mL) then partitioned with EtOAc (25 mL). The organic layer was isolated and the aqueous layer re-extracted with EtOAc (25 mL). The combined organic layer was washed with LiCI (5percent solution in water, 2 x 25 mL) and brine (25 mL), and passed through a hydrophobic frit then concentrated under reduced pressure to give a crude mixture of the title compounds (90 mg). LCMS (Method A): Rt = 1.08 min, MH+ 510. Crude material was taken forward to the next reaction step without further purification. Intermediate 15. 2-(2-Methoxypyrimidin-5-yl)-3-(l-(piperidin-4-ylmethyl)-lH-pyrazol-4-yl)-4,5.7,8-tetrahydro-2H-oxepinor4,5-c1pyrazole and l-(2-methoxypyrimidin-5-yl)-3-(l-(piperidin-4-ylmethyl)-lH-pyrazol-4-yl)-4,5,7,8-tetrahydro-lH-oxepinor4,5- clpyrazole A mixture of tert-butyl 4-((4-(l-(2-methoxypyrimidin-5-yl)-4,5,7,8-tetrahydro-lH-oxepino[4,5- c]pyrazol-3-yl)-lH-pyrazol-l-yl)methyl)piperidine-l-carboxylate and tert-butyl 4-((4-(2-(2- methoxypyrimidin-5-yl)-4,5,7,8-tetrahydro-2H-oxepino[4,5-c]pyrazol-3-yl)-lH-pyrazol-l- yl)methyl)piperidine-l-carboxylate (90 mg) was dissolved in DCM (2 mL). The reaction mixture was placed under an atmosphere of nitrogen and treated with TFA (0.068 mL, 0.883 mmol) then stirred for 1 h. The reaction mixture was treated with saturated aqueous sodium carbonate solution (5 mL) and partitioned with EtOAc (15 mL). The organic layer was isolated and the aqueous layer re-extracted with EtOAc (2 x 15 mL). The combined organic layer wa... |
Yield | Reaction Conditions | Operation in experiment |
---|---|---|
A mixture of <strong>[628692-15-9](2-methoxypyrimidin-5-yl)boronic acid</strong> (48 mg, 0.315 mmol), 3-(l-(4-methoxybenzyl)- lH-pyrazol-4-yl)-4,5,7,8-tetrahydro-lH-oxepino[4,5-c]pyrazole (100 mg) and DMAP (75 mg, 0.617 mmol) were combined in MeCN (1 mL) and treated with copper (II) acetate (84 mg, 0.462 mmol). The reaction mixture was stirred for three days at 40 °C, open to air, then allowed to cool to room temperature. The material was mixed with a batch that had been similarly prepared using (2-methoxypyrimidin-5- yl)boronic acid (131 mg, 0.848 mmol), 3-(l-(4-methoxybenzyl)-lH-pyrazol-4-yl)-4,5,7,8-tetrahydro- lH-oxepino[4,5-c]pyrazole (250 mg, 0.771 mmol), DMAP (188 mg, 1.541 mmol) and copper (II) acetate (210 mg, 1.156 mmol) in MeCN (5 mL).The combined reaction mixtures were treated with ammonium hydroxide (10 mL), water (10 mL) and partitioned with EtOAc (15 mL). The organic layer was isolated, and the aqueous layer re-extracted with EtOAc (2 x 15 mL). The combined organic layer was washed with brine (15 mL), passed through a hydrophobic frit and concentrated under reduced pressure, then loaded in MeOH (4 mL) onto an SCX-SPE cartridge that had been pre-conditioned with MeOH. The SCX-SPE cartridge was eluted with MeOH (3 x 15 mL) and combined eluants concentrated under reduced pressure to give a crude mixture the title compounds (308 mg). LCMS (Method C): Rt = 0.97 min, MH+ 433. Crude material was taken forward to the next reaction step without further purification. Intermediate 13. 2-(2-Methoxypyrimidin-5-yl)-3-(lH-pyrazol-4-yl)-4.5,7,8-tetrahydro- 2H-oxepinor4.5-c1pyrazole and l-(2-methoxypyrimidin-5-yl)-3-(lW-pyrazol-4-yl)- 4.5.7.8-tetrahydro-lH-oxepinor4.5-c1pyrazole A crude mixture of 3-(l-(4-methoxybenzyl)-lH-pyrazol-4-yl)-2-(2-methoxypyrimidin-5-yl)-4,5,7,8- tetrahydro-2H-oxepino[4,5-c]pyrazole and 3-(l-(4-methoxybenzyl)-lH-pyrazol-4-yl)-l-(2- methoxypyrimidin-5-yl)-4,5,7,8-tetrahydro-lH-oxepino[4,5-c]pyrazole (308 mg) in DCM (2 mL) was treated with TFA (2 mL, 26.0 mmol) and then heated using a microwave at 70 °C for 6 h. The reaction mixture was neutralised to pH 7 using sodium bicarbonate, diluted with water (10 mL) and extracted with EtOAc (15 mL). The organic layer was isolated, and the aqueous layer re-extracted with EtOAc (2 x 15 mL). The combined organic layer was washed with brine (10 mL), passed through a hydrophobic frit and concentrated under reduced pressure to give a crude mixture of the title compounds (232 mg). LCMS (Method C): Rt = 0.67 min, MH+ 313. Crude material was taken forward to the next reaction step without further purification. Intermediate 14. tert-Butyl 4-((4-(2-(2-methoxypyrimidin-5-yl)-4.5.7.8-tetrahydro-2W- oxepinor4.5-c1pyrazol-3-yl)-lW-pyrazol-l-yl)methyl)piperidine-l-carboxylate and tert- butyl 4-((4-(l-(2-methoxypyrimidin-5-yl)-4,5,7,8-tetrahydro-lH-oxepinor4,5-c1pyrazol- 3-yl)-lH-pyrazol-l-yl)methyl)piperidine-l-carboxylate A crude mixture of the 2-(2-methoxypyrimidin-5-yl)-3-(lH-pyrazol-4-yl)-4,5,7,8-tetrahydro-2H- oxepino[4,5-c]pyrazole and l-(2-methoxypyrimidin-5-yl)-3-(lH-pyrazol-4-yl)-4,5,7,8-tetrahydro-lH- oxepino[4,5-c]pyrazole (232 mg) was dissolved in DMF (2 mL) and placed under an atmosphere of nitrogen. The mixture was treated with NaH (17 mg, 0.423 mmol, 60percent suspension in mineral oils) and stirred for 30 min then treated with tert-butyl 4-(bromomethyl)piperidine-l-carboxylate (86 mg, 0.310 mmol) and stirred for a further 24 h. The reaction mixture was acidified to pH 5 using a 2 M solution of HCI and diluted with water (25 mL) then partitioned with EtOAc (25 mL). The organic layer was isolated and the aqueous layer re-extracted with EtOAc (25 mL). The combined organic layer was washed with LiCI (5percent solution in water, 2 x 25 mL) and brine (25 mL), and passed through a hydrophobic frit then concentrated under reduced pressure to give a crude mixture of the title compounds (90 mg). LCMS (Method A): Rt = 1.08 min, MH+ 510. Crude material was taken forward to the next reaction step without further purification. |
Yield | Reaction Conditions | Operation in experiment |
---|---|---|
A mixture of <strong>[628692-15-9](2-methoxypyrimidin-5-yl)boronic acid</strong> (48 mg, 0.315 mmol), 3-(l-(4-methoxybenzyl)- lH-pyrazol-4-yl)-4,5,7,8-tetrahydro-lH-oxepino[4,5-c]pyrazole (100 mg) and DMAP (75 mg, 0.617 mmol) were combined in MeCN (1 mL) and treated with copper (II) acetate (84 mg, 0.462 mmol). The reaction mixture was stirred for three days at 40 °C, open to air, then allowed to cool to room temperature. The material was mixed with a batch that had been similarly prepared using (2-methoxypyrimidin-5- yl)boronic acid (131 mg, 0.848 mmol), 3-(l-(4-methoxybenzyl)-lH-pyrazol-4-yl)-4,5,7,8-tetrahydro- lH-oxepino[4,5-c]pyrazole (250 mg, 0.771 mmol), DMAP (188 mg, 1.541 mmol) and copper (II) acetate (210 mg, 1.156 mmol) in MeCN (5 mL).The combined reaction mixtures were treated with ammonium hydroxide (10 mL), water (10 mL) and partitioned with EtOAc (15 mL). The organic layer was isolated, and the aqueous layer re-extracted with EtOAc (2 x 15 mL). The combined organic layer was washed with brine (15 mL), passed through a hydrophobic frit and concentrated under reduced pressure, then loaded in MeOH (4 mL) onto an SCX-SPE cartridge that had been pre-conditioned with MeOH. The SCX-SPE cartridge was eluted with MeOH (3 x 15 mL) and combined eluants concentrated under reduced pressure to give a crude mixture the title compounds (308 mg). LCMS (Method C): Rt = 0.97 min, MH+ 433. Crude material was taken forward to the next reaction step without further purification. Intermediate 13. 2-(2-Methoxypyrimidin-5-yl)-3-(lH-pyrazol-4-yl)-4.5,7,8-tetrahydro- 2H-oxepinor4.5-c1pyrazole and l-(2-methoxypyrimidin-5-yl)-3-(lW-pyrazol-4-yl)- 4.5.7.8-tetrahydro-lH-oxepinor4.5-c1pyrazole A crude mixture of 3-(l-(4-methoxybenzyl)-lH-pyrazol-4-yl)-2-(2-methoxypyrimidin-5-yl)-4,5,7,8- tetrahydro-2H-oxepino[4,5-c]pyrazole and 3-(l-(4-methoxybenzyl)-lH-pyrazol-4-yl)-l-(2- methoxypyrimidin-5-yl)-4,5,7,8-tetrahydro-lH-oxepino[4,5-c]pyrazole (308 mg) in DCM (2 mL) was treated with TFA (2 mL, 26.0 mmol) and then heated using a microwave at 70 °C for 6 h. The reaction mixture was neutralised to pH 7 using sodium bicarbonate, diluted with water (10 mL) and extracted with EtOAc (15 mL). The organic layer was isolated, and the aqueous layer re-extracted with EtOAc (2 x 15 mL). The combined organic layer was washed with brine (10 mL), passed through a hydrophobic frit and concentrated under reduced pressure to give a crude mixture of the title compounds (232 mg). LCMS (Method C): Rt = 0.67 min, MH+ 313. Crude material was taken forward to the next reaction step without further purification. Intermediate 14. tert-Butyl 4-((4-(2-(2-methoxypyrimidin-5-yl)-4.5.7.8-tetrahydro-2W- oxepinor4.5-c1pyrazol-3-yl)-lW-pyrazol-l-yl)methyl)piperidine-l-carboxylate and tert- butyl 4-((4-(l-(2-methoxypyrimidin-5-yl)-4,5,7,8-tetrahydro-lH-oxepinor4,5-c1pyrazol- 3-yl)-lH-pyrazol-l-yl)methyl)piperidine-l-carboxylate A crude mixture of the 2-(2-methoxypyrimidin-5-yl)-3-(lH-pyrazol-4-yl)-4,5,7,8-tetrahydro-2H- oxepino[4,5-c]pyrazole and l-(2-methoxypyrimidin-5-yl)-3-(lH-pyrazol-4-yl)-4,5,7,8-tetrahydro-lH- oxepino[4,5-c]pyrazole (232 mg) was dissolved in DMF (2 mL) and placed under an atmosphere of nitrogen. The mixture was treated with NaH (17 mg, 0.423 mmol, 60percent suspension in mineral oils) and stirred for 30 min then treated with tert-butyl 4-(bromomethyl)piperidine-l-carboxylate (86 mg, 0.310 mmol) and stirred for a further 24 h. The reaction mixture was acidified to pH 5 using a 2 M solution of HCI and diluted with water (25 mL) then partitioned with EtOAc (25 mL). The organic layer was isolated and the aqueous layer re-extracted with EtOAc (25 mL). The combined organic layer was washed with LiCI (5percent solution in water, 2 x 25 mL) and brine (25 mL), and passed through a hydrophobic frit then concentrated under reduced pressure to give a crude mixture of the title compounds (90 mg). LCMS (Method A): Rt = 1.08 min, MH+ 510. Crude material was taken forward to the next reaction step without further purification. Intermediate 15. 2-(2-Methoxypyrimidin-5-yl)-3-(l-(piperidin-4-ylmethyl)-lH-pyrazol-4-yl)-4,5.7,8-tetrahydro-2H-oxepinor4,5-c1pyrazole and l-(2-methoxypyrimidin-5-yl)-3-(l-(piperidin-4-ylmethyl)-lH-pyrazol-4-yl)-4,5,7,8-tetrahydro-lH-oxepinor4,5- clpyrazole A mixture of tert-butyl 4-((4-(l-(2-methoxypyrimidin-5-yl)-4,5,7,8-tetrahydro-lH-oxepino[4,5- c]pyrazol-3-yl)-lH-pyrazol-l-yl)methyl)piperidine-l-carboxylate and tert-butyl 4-((4-(2-(2- methoxypyrimidin-5-yl)-4,5,7,8-tetrahydro-2H-oxepino[4,5-c]pyrazol-3-yl)-lH-pyrazol-l- yl)methyl)piperidine-l-carboxylate (90 mg) was dissolved in DCM (2 mL). The reaction mixture was placed under an atmosphere of nitrogen and treated with TFA (0.068 mL, 0.883 mmol) then stirred for 1 h. The reaction mixture was treated with saturated aqueous sodium carbonate solution (5 mL) and partitioned with EtOAc (15 mL). The organic layer was isolated and the aqueous layer re-extracted with EtOAc (2 x 15 mL). The combined organic layer wa... |
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