000856172 001__ 856172 000856172 005__ 20210129235247.0 000856172 0247_ $$2doi$$a10.1038/s41598-018-33050-5 000856172 0247_ $$2Handle$$a2128/19820 000856172 0247_ $$2pmid$$apmid:30297855 000856172 0247_ $$2WOS$$aWOS:000446577500037 000856172 0247_ $$2altmetric$$aaltmetric:49999795 000856172 037__ $$aFZJ-2018-05799 000856172 082__ $$a600 000856172 1001_ $$0P:(DE-HGF)0$$aOtte, Maik$$b0 000856172 245__ $$aHydrophobic alkyl chains substituted to the 8-position of cyclic nucleotides enhance activation of CNG and HCN channels by an intricate enthalpy - entropy compensation 000856172 260__ $$a[London]$$bMacmillan Publishers Limited, part of Springer Nature$$c2018 000856172 3367_ $$2DRIVER$$aarticle 000856172 3367_ $$2DataCite$$aOutput Types/Journal article 000856172 3367_ $$0PUB:(DE-HGF)16$$2PUB:(DE-HGF)$$aJournal Article$$bjournal$$mjournal$$s1539780064_27723 000856172 3367_ $$2BibTeX$$aARTICLE 000856172 3367_ $$2ORCID$$aJOURNAL_ARTICLE 000856172 3367_ $$00$$2EndNote$$aJournal Article 000856172 520__ $$aCyclic nucleotide-gated (CNG) and hyperpolarization-activated cyclic nucleotide-gated (HCN) channels are tetrameric non-specific cation channels in the plasma membrane that are activated by either cAMP or cGMP binding to specific binding domains incorporated in each subunit. Typical apparent affinities of these channels for these cyclic nucleotides range from several hundred nanomolar to tens of micromolar. Here we synthesized and characterized novel cAMP and cGMP derivatives by substituting either hydrophobic alkyl chains or similar-sized more hydrophilic heteroalkyl chains to the 8-position of the purine ring with the aim to obtain full agonists of higher potency. The compounds were tested in homotetrameric CNGA2, heterotetrameric CNGA2:CNGA4:CNGB1b and homotetrameric HCN2 channels. We show that nearly all compounds are full agonists and that longer alkyl chains systematically increase the apparent affinity, at the best more than 30 times. The effects are stronger in CNG than HCN2 channels which, however, are constitutively more sensitive to cAMP. Kinetic analyses reveal that the off-rate is significantly slowed by the hydrophobic alkyl chains. Molecular dynamics simulations and free energy calculations suggest that an intricate enthalpy - entropy compensation underlies the higher apparent affinity of the derivatives with the longer alkyl chains, which is shown to result from a reduced loss of configurational entropy upon binding. 000856172 536__ $$0G:(DE-HGF)POF3-342$$a342 - Disease Mechanisms and Model Systems (POF3-342)$$cPOF3-342$$fPOF III$$x0 000856172 536__ $$0G:(DE-HGF)POF3-511$$a511 - Computational Science and Mathematical Methods (POF3-511)$$cPOF3-511$$fPOF III$$x1 000856172 536__ $$0G:(DE-HGF)POF3-561$$a561 - Biological Key Regulators and Small Chemical Compounds (POF3-561)$$cPOF3-561$$fPOF III$$x2 000856172 536__ $$0G:(DE-Juel1)hkf7_20170501$$aForschergruppe Gohlke (hkf7_20170501)$$chkf7_20170501$$fForschergruppe Gohlke$$x3 000856172 536__ $$0G:(DE-Juel1)hdd17_20170501$$aDisinhibition and inhibition of HCN2 channel function by ligand binding to the cyclic nucleotide bin (hdd17_20170501)$$chdd17_20170501$$fDisinhibition and inhibition of HCN2 channel function by ligand binding to the cyclic nucleotide bin$$x4 000856172 588__ $$aDataset connected to CrossRef 000856172 7001_ $$0P:(DE-HGF)0$$aSchweinitz, Andrea$$b1 000856172 7001_ $$00000-0003-4411-7342$$aBonus, Michele$$b2 000856172 7001_ $$0P:(DE-HGF)0$$aEnke, Uta$$b3 000856172 7001_ $$0P:(DE-HGF)0$$aSchumann, Christina$$b4 000856172 7001_ $$0P:(DE-Juel1)172663$$aGohlke, Holger$$b5 000856172 7001_ $$0P:(DE-HGF)0$$aBenndorf, Klaus$$b6$$eCorresponding author 000856172 773__ $$0PERI:(DE-600)2615211-3$$a10.1038/s41598-018-33050-5$$gVol. 8, no. 1, p. 14960$$n1$$p14960$$tScientific reports$$v8$$x2045-2322$$y2018 000856172 8564_ $$uhttps://juser.fz-juelich.de/record/856172/files/171.pdf$$yOpenAccess 000856172 8564_ $$uhttps://juser.fz-juelich.de/record/856172/files/171.pdf?subformat=pdfa$$xpdfa$$yOpenAccess 000856172 909CO $$ooai:juser.fz-juelich.de:856172$$pdnbdelivery$$pdriver$$pVDB$$popen_access$$popenaire 000856172 9101_ $$0I:(DE-588b)5008462-8$$6P:(DE-Juel1)172663$$aForschungszentrum Jülich$$b5$$kFZJ 000856172 9131_ $$0G:(DE-HGF)POF3-342$$1G:(DE-HGF)POF3-340$$2G:(DE-HGF)POF3-300$$3G:(DE-HGF)POF3$$4G:(DE-HGF)POF$$aDE-HGF$$bGesundheit$$lErkrankungen des Nervensystems$$vDisease Mechanisms and Model Systems$$x0 000856172 9131_ $$0G:(DE-HGF)POF3-511$$1G:(DE-HGF)POF3-510$$2G:(DE-HGF)POF3-500$$3G:(DE-HGF)POF3$$4G:(DE-HGF)POF$$aDE-HGF$$bKey Technologies$$lSupercomputing & Big Data$$vComputational Science and Mathematical Methods$$x1 000856172 9131_ $$0G:(DE-HGF)POF3-561$$1G:(DE-HGF)POF3-560$$2G:(DE-HGF)POF3-500$$3G:(DE-HGF)POF3$$4G:(DE-HGF)POF$$aDE-HGF$$bKey Technologies$$lBioInterfaces in Technology and Medicine$$vBiological Key Regulators and Small Chemical Compounds$$x2 000856172 9141_ $$y2018 000856172 915__ $$0StatID:(DE-HGF)0200$$2StatID$$aDBCoverage$$bSCOPUS 000856172 915__ $$0StatID:(DE-HGF)1050$$2StatID$$aDBCoverage$$bBIOSIS Previews 000856172 915__ $$0LIC:(DE-HGF)CCBY4$$2HGFVOC$$aCreative Commons Attribution CC BY 4.0 000856172 915__ $$0StatID:(DE-HGF)0600$$2StatID$$aDBCoverage$$bEbsco Academic Search 000856172 915__ $$0StatID:(DE-HGF)1040$$2StatID$$aDBCoverage$$bZoological Record 000856172 915__ $$0StatID:(DE-HGF)0100$$2StatID$$aJCR$$bSCI REP-UK : 2017 000856172 915__ $$0StatID:(DE-HGF)0501$$2StatID$$aDBCoverage$$bDOAJ Seal 000856172 915__ $$0StatID:(DE-HGF)0500$$2StatID$$aDBCoverage$$bDOAJ 000856172 915__ $$0StatID:(DE-HGF)0110$$2StatID$$aWoS$$bScience Citation Index 000856172 915__ $$0StatID:(DE-HGF)0111$$2StatID$$aWoS$$bScience Citation Index Expanded 000856172 915__ $$0StatID:(DE-HGF)0150$$2StatID$$aDBCoverage$$bWeb of Science Core Collection 000856172 915__ $$0StatID:(DE-HGF)9900$$2StatID$$aIF < 5 000856172 915__ $$0StatID:(DE-HGF)0510$$2StatID$$aOpenAccess 000856172 915__ $$0StatID:(DE-HGF)0030$$2StatID$$aPeer Review$$bASC 000856172 915__ $$0StatID:(DE-HGF)1150$$2StatID$$aDBCoverage$$bCurrent Contents - Physical, Chemical and Earth Sciences 000856172 915__ $$0StatID:(DE-HGF)0310$$2StatID$$aDBCoverage$$bNCBI Molecular Biology Database 000856172 915__ $$0StatID:(DE-HGF)0300$$2StatID$$aDBCoverage$$bMedline 000856172 915__ $$0StatID:(DE-HGF)0320$$2StatID$$aDBCoverage$$bPubMed Central 000856172 915__ $$0StatID:(DE-HGF)0199$$2StatID$$aDBCoverage$$bClarivate Analytics Master Journal List 000856172 920__ $$lyes 000856172 9201_ $$0I:(DE-Juel1)JSC-20090406$$kJSC$$lJülich Supercomputing Center$$x0 000856172 9201_ $$0I:(DE-Juel1)ICS-6-20110106$$kICS-6$$lStrukturbiochemie $$x1 000856172 9201_ $$0I:(DE-Juel1)NIC-20090406$$kNIC$$lJohn von Neumann - Institut für Computing$$x2 000856172 9801_ $$aFullTexts 000856172 980__ $$ajournal 000856172 980__ $$aVDB 000856172 980__ $$aUNRESTRICTED 000856172 980__ $$aI:(DE-Juel1)JSC-20090406 000856172 980__ $$aI:(DE-Juel1)ICS-6-20110106 000856172 980__ $$aI:(DE-Juel1)NIC-20090406 000856172 981__ $$aI:(DE-Juel1)IBI-7-20200312