in vitro characterization of psychoactive substances at...

11
1521-0103/357/1/134144$25.00 http://dx.doi.org/10.1124/jpet.115.229765 THE JOURNAL OF PHARMACOLOGY AND EXPERIMENTAL THERAPEUTICS J Pharmacol Exp Ther 357:134144, April 2016 Copyright ª 2016 by The American Society for Pharmacology and Experimental Therapeutics In Vitro Characterization of Psychoactive Substances at Rat, Mouse, and Human Trace Amine-Associated Receptor 1 s Linda D. Simmler, Danièle Buchy, Sylvie Chaboz, Marius C. Hoener, and Matthias E. Liechti Division of Clinical Pharmacology and Toxicology, Department of Biomedicine, University Hospital Basel, University of Basel, Basel, Switzerland (L.D.S., M.E.L.); and Neuroscience Research, Pharma Research and Early Development, Roche Innovation Center Basel, F. Hoffmann-La Roche Ltd., Basel, Switzerland (D.B., S.C., M.C.H) Received October 5, 2015; accepted January 19, 2016 ABSTRACT Trace amine-associated receptor 1 (TAAR1) has been implicated in the behavioral effects of amphetamine-type stimulant drugs in rodents. TAAR1 has also been suggested as a target for novel medications to treat psychostimulant addiction. We previously reported that binding affinities at TAAR1 can differ between structural analogs of psychostimulants, and species differences have been observed. In this study, we complement our previous findings with additional substances and the determination of functional activation potencies. In summary, we present here pharmacological in vitro profiles of 101 psychoactive substances at human, rat, and mouse TAAR1. p-Tyramine, b-phenylethylamine, and tryptamine were included as endogenous comparator compounds. Functional cAMP measurements and radioligand displacement assays were conducted with human embryonic kidney 293 cells that expressed human, rat, or mouse TAAR1. Most amphetamines, phenethylamine, and aminoindanes exhibited potentially physiologically relevant rat and mouse TAAR1 activation (EC 50 , 5 mM) and showed full or partial ( E max , 80%) agonist properties. Cathinone derivatives, including mephedrone and methylenedioxypyrovalerone, exhibited weak (EC 50 5 510 mM) to negligible (EC 50 . 10 mM) binding properties at TAAR1. Pipradrols, including methylphe- nidate, exhibited no affinity for TAAR1. We found considerable species differences in activity at TAAR1 among the highly active ligands, with a rank order of rat . mouse . human. This characterization provides information about the pharmacologi- cal profile of psychoactive substances. The species differences emphasize the relevance of clinical studies to translationally complement rodent studies on the role of TAAR1 activity for psychoactive substances. Introduction Trace amine-associated receptor 1 (TAAR1) is a relatively recently discovered G proteincoupled receptor (Borowsky et al., 2001; Bunzow et al., 2001), which is expressed in monoaminergic brain regions and throughout the limbic system (Borowsky et al., 2001; Lindemann et al., 2008; Espinoza et al., 2015). TAAR1 is thought to play a role in regulating the limbic network, reward circuits, cognitive processes, and mood states and has been proposed as a pharmacological target for the treatment of mental disorders (Wolinsky et al., 2007; Lindemann et al., 2008; Miller, 2011; Revel et al., 2013) and psychostimulant dependence (Di Cara et al., 2011; Pei et al., 2014; Cotter et al., 2015; Jing and Li, 2015). TAAR1 is stimulated by endogenous ligands, including b-phenylethylamine (b-PEA), p-tyramine, tryptamine, and 3-iodothyronamine (Scanlan et al., 2004; Zucchi et al., 2006). Many psychoactive compounds, including amphetamine and phenethylamine derivatives, also bind to TAAR1 (Bunzow et al., 2001; Wainscott et al., 2007; Simmler et al., 2013; Reese et al., 2014). The activation of TAAR1 results in elevations in intracellular cAMP (Bunzow et al., 2001; Xie and Miller, 2007). Amphetamines have structural similarity to the endoge- nous ligand b-PEA and were initially identified as TAAR1 ligands (Bunzow et al., 2001). We previously reported that many novel psychoactive substances are also ligands of rat and mouse TAAR1 (Simmler et al., 2013, 2014a,b; Rickli et al., 2015a,b,c). However, several novel psychoactive substances do not bind to TAAR1, and little has been reported on the activation of human TAAR1. The pharmacological and toxi- cological actions of novel psychoactive substances are also of interest because of the emergence of hundreds of these substances, referred to as legal highsor research chem- icals.These chemical compounds are recreationally used but have poorly known pharmacological properties. TAAR1 is implicated in the control of neuronal firing frequency and is thus likely to contribute to psychoactive and abuse-related drug effects. Ex vivo electrophysiology experiments that used slices from TAAR1 knockout (KO) mice (Lindemann et al., 2008) or pharmacological TAAR1 blockade (Bradaia et al., 2009) suggest that TAAR1 is This research was supported by the Federal Office of Public Health [Grant 13.006497] and F. Hoffmann-La Roche Ltd. and the University of Basel [Translational Medicine Hub Innovation Fund]. dx.doi.org/10.1124/jpet.115.229765. s This article has supplemental material available at jpet.aspetjournals.org. ABBREVIATIONS: b-PEA, b-phenylethylamine; DA, dopamine; 5-HT, 5-hydroxytryptamine (serotonin); KO, knockout; MDMA, 3,4-methylenedioxymethamphetamine; PBS, phosphate-buffered saline; RO5166017, (S)-4-[(ethyl-phenyl-amino)-methyl]-4,5-dihydro-oxazol- 2-ylamine; RO5203648, (S)-4-(3,4-dichlorophenyl)-4,5-dihydrooxazol-2-amine dihydrochloride; TAAR1, trace amine-associated receptor 1; WT, wild type. 134 http://jpet.aspetjournals.org/content/suppl/2016/01/20/jpet.115.229765.DC1 Supplemental material to this article can be found at: at ASPET Journals on January 11, 2020 jpet.aspetjournals.org Downloaded from

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Page 1: In Vitro Characterization of Psychoactive Substances at Rat,jpet.aspetjournals.org/content/jpet/357/1/134.full.pdf · transmitter release. Di Cara et al. (2011) supported the concept

1521-0103/357/1/134–144$25.00 http://dx.doi.org/10.1124/jpet.115.229765THE JOURNAL OF PHARMACOLOGY AND EXPERIMENTAL THERAPEUTICS J Pharmacol Exp Ther 357:134–144, April 2016Copyright ª 2016 by The American Society for Pharmacology and Experimental Therapeutics

In Vitro Characterization of Psychoactive Substances at Rat,Mouse, and Human Trace Amine-Associated Receptor 1s

Linda D. Simmler, Danièle Buchy, Sylvie Chaboz, Marius C. Hoener, and Matthias E. LiechtiDivision of Clinical Pharmacology and Toxicology, Department of Biomedicine, University Hospital Basel, University of Basel,Basel, Switzerland (L.D.S., M.E.L.); and Neuroscience Research, Pharma Research and Early Development, Roche InnovationCenter Basel, F. Hoffmann-La Roche Ltd., Basel, Switzerland (D.B., S.C., M.C.H)

Received October 5, 2015; accepted January 19, 2016

ABSTRACTTrace amine-associated receptor 1 (TAAR1) has been implicatedin the behavioral effects of amphetamine-type stimulant drugs inrodents. TAAR1 has also been suggested as a target for novelmedications to treat psychostimulant addiction. We previouslyreported that binding affinities at TAAR1 can differ betweenstructural analogs of psychostimulants, and species differenceshave been observed. In this study, we complement our previousfindings with additional substances and the determination offunctional activation potencies. In summary, we present herepharmacological in vitro profiles of 101 psychoactive substancesat human, rat, andmouseTAAR1.p-Tyramine,b-phenylethylamine,and tryptamine were included as endogenous comparatorcompounds. Functional cAMP measurements and radioliganddisplacement assays were conducted with human embryonickidney 293 cells that expressed human, rat, or mouse TAAR1.

Most amphetamines, phenethylamine, and aminoindanesexhibited potentially physiologically relevant rat and mouseTAAR1 activation (EC50 , 5 mM) and showed full or partial(Emax , 80%) agonist properties. Cathinone derivatives,including mephedrone and methylenedioxypyrovalerone,exhibited weak (EC50 5 5–10 mM) to negligible (EC50 . 10 mM)binding properties at TAAR1. Pipradrols, including methylphe-nidate, exhibited no affinity for TAAR1. We found considerablespecies differences in activity at TAAR1 among the highly activeligands, with a rank order of rat . mouse . human. Thischaracterization provides information about the pharmacologi-cal profile of psychoactive substances. The species differencesemphasize the relevance of clinical studies to translationallycomplement rodent studies on the role of TAAR1 activity forpsychoactive substances.

IntroductionTrace amine-associated receptor 1 (TAAR1) is a relatively

recently discovered G protein–coupled receptor (Borowskyet al., 2001; Bunzow et al., 2001), which is expressed inmonoaminergic brain regions and throughout the limbicsystem (Borowsky et al., 2001; Lindemann et al., 2008;Espinoza et al., 2015). TAAR1 is thought to play a role inregulating the limbic network, reward circuits, cognitiveprocesses, and mood states and has been proposed as apharmacological target for the treatment of mental disorders(Wolinsky et al., 2007; Lindemann et al., 2008; Miller, 2011;Revel et al., 2013) and psychostimulant dependence (Di Caraet al., 2011; Pei et al., 2014; Cotter et al., 2015; Jing and Li,2015). TAAR1 is stimulated by endogenous ligands, includingb-phenylethylamine (b-PEA), p-tyramine, tryptamine, and3-iodothyronamine (Scanlan et al., 2004; Zucchi et al., 2006).Many psychoactive compounds, including amphetamine and

phenethylamine derivatives, also bind to TAAR1 (Bunzowet al., 2001; Wainscott et al., 2007; Simmler et al., 2013; Reeseet al., 2014). The activation of TAAR1 results in elevations inintracellular cAMP (Bunzow et al., 2001; Xie and Miller,2007).Amphetamines have structural similarity to the endoge-

nous ligand b-PEA and were initially identified as TAAR1ligands (Bunzow et al., 2001). We previously reported thatmany novel psychoactive substances are also ligands of ratandmouse TAAR1 (Simmler et al., 2013, 2014a,b; Rickli et al.,2015a,b,c). However, several novel psychoactive substances donot bind to TAAR1, and little has been reported on theactivation of human TAAR1. The pharmacological and toxi-cological actions of novel psychoactive substances are also ofinterest because of the emergence of hundreds of thesesubstances, referred to as “legal highs” or “research chem-icals.” These chemical compounds are recreationally used buthave poorly known pharmacological properties.TAAR1 is implicated in the control of neuronal firing

frequency and is thus likely to contribute to psychoactiveand abuse-related drug effects. Ex vivo electrophysiologyexperiments that used slices from TAAR1 knockout (KO)mice (Lindemann et al., 2008) or pharmacological TAAR1blockade (Bradaia et al., 2009) suggest that TAAR1 is

This research was supported by the Federal Office of Public Health [Grant13.006497] and F. Hoffmann-La Roche Ltd. and the University of Basel[Translational Medicine Hub Innovation Fund].

dx.doi.org/10.1124/jpet.115.229765.s This article has supplemental material available at jpet.aspetjournals.org.

ABBREVIATIONS: b-PEA, b-phenylethylamine; DA, dopamine; 5-HT, 5-hydroxytryptamine (serotonin); KO, knockout; MDMA,3,4-methylenedioxymethamphetamine; PBS, phosphate-buffered saline; RO5166017, (S)-4-[(ethyl-phenyl-amino)-methyl]-4,5-dihydro-oxazol-2-ylamine; RO5203648, (S)-4-(3,4-dichlorophenyl)-4,5-dihydrooxazol-2-amine dihydrochloride; TAAR1, trace amine-associated receptor 1; WT, wild type.

134

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constitutively active to control dopamine (DA) and serotonin[5-hydroxytryptamine (5-HT)] tone.Compared with wild-type (WT) mice, TAAR1 KO mice

were shown to consume more ethanol and be more suscepti-ble to its sedating effects (Lynch et al., 2013). The TAAR1partial agonist RO5203648 [(S)-4-(3,4-dichlorophenyl)-4,5-dihydrooxazol-2-amine dihydrochloride] reduced cocaine self-administration and cocaine-induced hyperlocomotion in rats(Revel et al., 2012b). Both selective TAAR1 partial agonistsand selective TAAR1 full agonists reduced cocaine self-administration and the reinstatement of drug-seeking behaviorin rats (Pei et al., 2014, 2015) and decreased cocaine-mediatedintracranial self-stimulation (Pei et al., 2015). Reductions ofhyperlocomotion, self-administration, and reinstatement byTAAR1 partial agonism have also been reported for metham-phetamine (Cotter et al., 2015; Jing andLi, 2015). These studiesestablished TAAR1 as a promising target for therapeutics totreat substance use disorders, regardless of the TAAR1binding properties of the abused substances themselves. Bydirectly interacting with TAAR1, psychoactive substancesmay also modulate their own pharmacological effects. Forexample, amphetamine induces markedly more striatalmonoamine release in TAAR1 KO mice than in WT mice(Lindemann et al., 2008). Methamphetamine and amphet-amine increase locomotor activity to a greater extent inTAAR1 KO mice compared with WT mice (Achat-Mendeset al., 2012). TAAR1 also plays a role in contingent oralmethamphetamine intake (Harkness et al., 2015). Similar toamphetamine and methamphetamine, 3,4-methylenedioxy-methamphetamine (MDMA) significantly increased extra-cellular striatal DA and 5-HT levels to a greater extent inTAAR1 KO mice compared with WT mice (Di Cara et al.,2011). TAAR1 KO mice are hypersensitive to psychoactivesubstances that are also TAAR1 ligands. By contrast, TAAR1overexpression in mice reduced locomotor activity inresponse to amphetamine (Revel et al., 2012a). BecauseMDMA, methamphetamine, and amphetamine are TAAR1ligands, they possibly autoinhibit their own effects on neuro-transmitter release. Di Cara et al. (2011) supported theconcept of the autoregulation of TAAR1-activating psychostim-ulants, showing that the TAAR1 ligand o-phenyl-3-iodotyraminedecreased the DA release response to p-chloroamphetamine,which is a psychostimulant that is inactive at TAAR1, in WTmice but not in TAAR KO mice.Because TAAR1might be significantly involved in the mode

of action of many psychoactive drugs, we determined theTAAR1 binding and activation properties of a series of mostlynovel substances and found considerable differences inTAAR1 binding properties within and between substanceclasses. Our data set provides evidence of significant speciesdifferences in ligand/receptor interactions between rodent andhuman TAAR1.

Materials and MethodsChemicals. The compounds were purchased from Lipomed

(Arlesheim, Switzerland) or Cayman Chemicals (Ann Arbor, MI)as racemic mixtures, with the exception of D-amphetamine,D-methamphetamine, (1)-ephedrine, and (2)-ephedrine. A list ofgeneric or full chemical names is provided in (Supplemental Table 1).5-EAPB, diclophensine, diphenidine, ethylphenidate,methoxphenidine,and N-methyl-2-AI were obtained from the Forensic Institute Zürich

(Zürich, Switzerland). Naphyrone and MDAI were synthesized inour laboratory as reported previously (Simmler et al., 2013, 2014b).Radiochemicals (3H-isotopes) were purchased from PerkinElmer(Schwerzenbach, Switzerland), with the exception of [3H]RO5166017[(S)-4-[(ethyl-phenyl-amino)-methyl]-4,5-dihydro-oxazol-2-ylamine],which was synthesized at Roche (Basel, Switzerland).

Cell Culture and Membrane Preparation. Human embryonickidney 293 cells that stably expressed human, rat, or mouse TAAR1were used as described previously (Revel et al., 2011). All of the celllines were maintained at 37°C and 5% CO2 in high-glucose Dulbecco’smodified Eagle’s medium that contained 10% fetal calf serum (heat-inactivated for 30 minutes at 56°C), 1% penicillin/streptomycin, and375 mg/ml Geneticin (Gibco, Zug, Switzerland). For membranepreparation, the cells were released from culture flasks usingtrypsin/EDTA, harvested, washed twice with ice-cold phosphate-buffered saline (PBS; without Ca21 andMg21), pelleted at 1000� g for5 minutes at 4°C, frozen, and stored at 280°C. Frozen pellets weresuspended in buffer A [20 ml HEPES-NaOH (20 mM, pH 7.4) thatcontained 10 mM EDTA] and homogenized with a Polytron (PT 6000;Kinematica, Luzern, Switzerland) at 14,000 rpm for 20 seconds. Thehomogenate was centrifuged for 30 minutes at 48,000 � g at 4°C. Thesupernatant was removed and discarded, and the pellet was resus-pended in buffer A using the Polytron (20 seconds at 14,000 rpm). Thecentrifugation and removal of the supernatant was repeated, andthe final pellet was resuspended in buffer A and homogenized usingthe Polytron. Typically, 2-ml aliquots of membrane portions werestored at 280°C. With each new membrane batch, the dissociationconstant (Kd) was determined by a saturation curve.

Radioligand Binding Assay. For the competitive binding assays,the TAAR1 agonist [3H]RO5166017 was used as a TAAR1 radioligandat a concentration equal toKd values, which was usually around 0.7 nM(mouse TAAR1) and 2.3 nM (rat TAAR1). Nonspecific binding wasdefined as the amount of radioligand bound in the presence of 10 mMRO5166017. Compoundswere tested at a broad range of concentrations(10 pM to 10mM) in duplicate. Compounds (20ml/well) were transferredto a 96-deep-well plate (TreffLab, Degersheim, Switzerland), and 180mlbinding buffer (20mMHEPES-NaOH, 10mMMgCl2, and 2mMCaCl2,pH 7.4), 300 ml radioligand, and 500 ml membranes (resuspended at60 mg protein/ml) were added. The plates were incubated at 4°C for90 minutes. Incubations were terminated by rapid filtration throughUnifilter-96 plates (Packard Instrument Company, PerkinElmer) andglass filtersGF/C (PerkinElmer) presoaked for 1 hour in polyethylenimine(0.3%) and washed three times with 1 ml cold binding buffer. After theaddition of 45 ml Microscint 40 (PerkinElmer), the Unifilter-96 platewas sealed. After 1 hour, radioactivity was counted using a TopCountMicroplate Scintillation Counter (Packard Instrument Company).IC50 values were determined by calculating nonlinear regressioncurves for a one-site model using at least three independent 10-pointconcentration-response curves, run in duplicate, for each compound.Ki (affinity) values, which correspond to the dissociation constants,were determined using the Cheng–Prusoff equation. Ki values arepresented as means 6 S.D. (in micromoles). For reasons of integrity,Table 1 includes severalKi values that we have previously publishedas indicated by the references in the table.

Functional TAAR1 Activity. Substances were tested for bindingaffinity at rat and mouse TAAR1 as described above. If relevantbinding was observed, then we also determined potencies for receptoractivation and maximal efficacy at rat, mouse, and human TAAR1 tocharacterize the compounds as full or partial agonists (Emax , 80%).The endogenous TAAR1 ligands b-PEA, p-tyramine, and tryptamineserved as reference substances for comparisons of affinity values andfunctional potency and efficacy. cAMPmeasurements were performedas described previously (Revel et al., 2011). In brief, cells that expressedrat or mouse TAAR1 were plated on 96-well plates (BIOCOAT 6640;Becton Dickinson, Allschwil, Switzerland) and incubated for 20 hoursat 37°C. Prior to stimulation of the cells with a broad concentra-tion range of agonists for 30 minutes at 37°C, the cells werewashed with PBS and preincubated with PBS that contained 1 mM

Psychoactive Substances and TAAR1 135

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TABLE

1Bindingaffinities,activa

tion

potenc

ies,

andefficacy

ofps

ychoa

ctivesu

bstanc

esan

den

doge

nous

compa

ratorcompo

unds

atrat,mou

se,a

ndhu

man

TAAR1

Value

saregivenas

mea

ns6

S.D.K

iva

lues

ofhu

man

TAAR1wereno

tde

term

ined

becaus

eof

thelack

ofarelia

bleradioligan

dne

eded

forthein

vitroassay.

EC50

was

determ

ined

forsu

bstanc

eswithreleva

ntbind

ing(K

iva

lue,

10mM).

Kiva

lues

from

ourpr

eviouspu

blicationsareinclude

dan

dreferenced.

Thege

neric

orfullch

emical

nam

esforab

brev

iatedsu

bstancesarelisted

inSupp

lemen

talTab

le1.

Subs

tance

Rat

TAAR1

Mou

seTAAR1

Human

TAAR1

Recep

tor

BindingKi

Activation

Poten

cyEC50

Emax

Recep

tor

BindingKi

ActivationPoten

cyEC50

Emax

Activation

Poten

cyEC50

Emax

mM

%mM

%mM

%

Endo

genou

sliga

nds

b-PEA

0.24

60.12

0.11

60.08

1006

110.31

60.15

0.20

60.09

1026

80.26

60.09

1046

10p-Tyram

ine

0.05

96

0.02

00.03

60.02

194

611

0.38

60.13

0.28

60.17

886

90.99

60.29

916

8Tryptam

ine

0.13

60.05

0.41

60.15

916

81.46

0.4

2.76

0.5

1176

221

613

736

16Phen

ethylam

ines

25B-N

B2O

Me

0.28

60.00

2a1.26

0.4

376

194.56

1.7a

6.16

2.5

476

4.10

25C-N

B2O

Me

0.52

60.10

a1.66

0.4

296

515

62a

6.76

1.6

486

6.30

25D-N

B2O

Me

0.81

60.10

a1.56

0.4

346

413

64a

4.06

0.6

676

12.30

25E-N

B2O

Me

0.26

60.03

a0.65

60.39

376

151.16

0.3a

1.86

0.3

466

10.10

25H-N

B2O

Me

1.56

0.2a

3.06

1.4

376

11.20

a6.16

2.6

536

10.10

25I-NB2O

Me

0.44

60.07

a1.86

1.0

326

173.46

0.9a

5.26

2.2

176

9.10

25N-N

B2O

Me

2.26

0.14

a1.56

0.3

346

9.20

a.30

.10

25P-N

B2O

Me

0.05

56

0.00

4a0.51

60.20

346

170.24

60.03

a1.36

0.2

406

26.10

25T2-NB2O

Me

0.35

60.02

a0.93

60.38

246

144.26

0.6a

2.96

0.6

306

23.10

25T4-NB2O

Me

0.12

60.02

a1.16

0.6

316

121.56

0.4a

4.76

2.1

336

12.10

25T7-NB2O

Me

0.08

86

0.03

2a0.55

60.17

526

231.06

0.2a

2.16

0.5

686

23.10

2C-B

0.07

96

0.00

8a0.24

60.16

576

162.26

0.3a

2.36

0.4

696

133.36

0.9

106

22C

-B-Fly

0.02

96

0.00

8b0.27

60.16

486

10.71

60.23

b1.86

0.7

496

6.30

2C-C

0.11

60.02

a0.34

60.15

516

144.16

0.3a

2.36

1.5

576

23.10

2C-D

0.15

60.03

a0.49

60.14

556

103.56

0.1a

2.06

0.2

616

19.10

2C-E

0.06

66

0.00

9a0.18

60.14

726

131.26

0.1a

1.16

0.2

646

23.10

2C-H

0.96

0.16

a1.56

0.7

806

711

62a

7.56

3.3

566

146.56

0.7

536

52C

-I0.12

60.02

a0.19

60.11

506

193.36

0.1a

2.46

0.8

516

21.10

2C-N

0.34

60.02

a0.25

60.12

596

16.20

a15

612

286

13.10

2C-P

0.02

06

0.00

5a0.03

06

0.02

284

68

0.28

60.03

a0.56

60.23

916

274.26

0.5

726

112C

-T2

0.04

36

0.00

6a0.09

66

0.05

186

617

2.26

0.6a

4.36

2.8

546

14.10

2C-T4

0.05

36

0.00

8a0.08

36

0.05

067

611

4.56

0.9a

3.76

2.2

516

21.10

2C-T7

0.03

36

0.00

5a0.07

96

0.03

483

611

0.56

60.12

a0.91

60.67

676

4.10

Mescaline

3.36

0.5a

3.76

1.8

376

1811

64a

4.86

3.7

256

20.10

Mescaline-NB2O

Me

136

6a.30

.20

a.30

.10

Amph

etam

ines

Amph

etam

ine

0.23

60.18

c0.66

60.61

916

200.08

96

0.05

9c0.53

60.67

906

302.86

0.8

916

154-APB

0.11

60.02

b0.16

60.09

756

92.16

0.1b

0.85

60.78

726

124.16

2.1

506

215-APB

0.04

26

0.00

6b0.06

76

0.04

088

612

0.11

60.00

2b0.13

60.07

676

116.16

2.3

436

166-APB

0.05

26

0.01

7b0.04

26

0.02

990

614

0.05

66

0.01

5b0.06

76

0.03

993

613

7.26

0.3

476

77-APB

0.06

66

0.00

6b0.05

86

0.03

310

96

130.13

60.02

b0.11

60.07

956

170.63

60.13

896

45-APDB

0.49

60.05

b1.46

0.7

936

200.77

60.06

b1.56

1.2

646

14.10

6-APDB

1.06

0.04

b1.06

0.97

836

170.21

60.04

b0.51

60.27

956

19.10

5-EAPB

0.81

60.08

b1.16

0.6

396

10.15

b13

67

266

11.10

N-E

thylam

phetam

ine

2.56

1.4d

0.88

60.05

626

10.10

d.10

.10

4-Fluoroa

mph

etam

ine

0.08

16

0.04

1e0.06

96

0.00

478

612

0.32

60.1e

0.13

60.02

776

123.56

0.6

676

94-Fluorom

etham

phetam

ine

0.24

60.09

e0.16

60.02

766

111.76

0.9e

0.46

60.05

696

66.26

2.2

446

115-IT

0.15

60.02

0.20

60.01

666

40.36

60.15

0.34

60.07

636

5.30

5-MAPDB

0.67

60.09

b1.16

0.9

656

113.56

0.1b

4.36

3.0

596

11.10

MBDB

1.26

0.1c

1.76

1.2

756

83.66

1.1c

4.16

1.1

346

28.30

MDA

0.25

60.04

b0.74

60.16

866

50.16

60.01

b0.58

60.08

1026

113.66

0.4

116

4MDEA

2.76

1.0c

1.56

0.9

666

246.66

3.1c

6.26

3.4

356

33.30

MDMA

0.37

60.12

c1.06

0.7

566

102.46

1.1c

4.06

1.0

716

1635

621

266

8

(con

tinu

ed)

136 Simmler et al.

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TABLE

1—Con

tinued

Subs

tance

Rat

TAAR1

Mou

seTAAR1

Human

TAAR1

Recep

tor

BindingKi

Activation

Poten

cyEC50

Emax

Recep

tor

BindingKi

ActivationPoten

cyEC50

Emax

Activation

Poten

cyEC50

Emax

Metha

mph

etam

ine

0.35

60.12

c0.85

60.38

736

100.55

60.24

c0.73

60.47

786

75.36

2.3

706

214-Methy

lamph

etam

ine

0.10

60.01

0.11

60.02

936

170.15

60.07

0.07

16

0.01

394

68

.30

4-MTA

0.28

60.04

d0.26

60.03

566

100.04

36

0.00

7d0.08

96

0.01

679

619

.10

PMA

0.66

60.02

d0.34

60.13

836

80.14

60.10

d0.24

60.14

916

5.30

PMMA

1.36

0.2d

0.63

60.29

756

150.26

60.11

d1.06

0.1

826

13.30

Cathinon

es4-Bromom

ethcathinon

e1.86

0.1e

5.26

2.5

286

1213

63e

156

750

612

.30

Buph

edrone

.10

d.10

d

Bupr

opion

.20

.20

Butylone

.20

c.20

c

Cathino

ne

2.26

0.7c

1.26

0.3

286

82.16

0.7c

1.26

0.3

666

316.96

3.2

536

16N,N

-Dim

ethy

lcathino

ne

.10

d.10

d

Ethcathinon

e.10

d.10

d

4-Ethylmethcathinon

e.20

e.20

e

Ethylon

e.20

c.20

c

Fleph

edrone

5.46

1.7c

156

346

68

.10

c.20

.30

3-Fluorom

ethcathinon

e.10

d.10

d

MDPBP

.20

e.50

e

MDPPP

166

7e.20

e

MDPV

7.26

1.1c

5.96

2.7

626

14.10

c.30

.30

Mep

hedr

one

4.36

2c9.06

4.3

526

3.10

c20

67

876

16.30

Methcathinon

e4.16

1.2c

8.26

2.5

416

10.10

c6.86

2.7

646

16.30

Methe

dron

e18

64d

.20

d

Methy

lened

ioxy

cath

inon

e4.86

0.9b

5.76

0.9

536

206.56

2.8b

7.86

2.4

576

2.30

3-Methy

lmethc

athinon

e5.76

1.4

.10

116

13.86

0.04

256

7.10

4-Methy

lethcathinon

e.20

d.20

d

Methylon

e.13

c.10

c

Nap

hyron

e.20

c.20

c

Pen

tedr

one

.10

d.10

d

Pen

tylone

.10

d.10

d

a-PVP

166

6e.20

e

Pyrov

aleron

e.13

c.10

c

Eph

edrine

s(2

)-Eph

edrine

3.76

0.9

2.56

0.7

426

5.15

146

231

67

.10

(+)-Eph

edrine

5.26

1.7

106

629

69

.15

196

1021

616

.10

4-Fluoroeph

edrine

2.66

1.2e

2.26

0.8

406

1818

68e

236

810

06

10.30

Tryptam

ines

5-MeO

-aMT

1.16

0.2

2.36

0.2

386

64.86

0.9

3.76

1.6

556

5.10

4-HO-D

iPT

.15

.15

4-HO-M

ET

3.16

0.2

2.16

0.3

716

912

63

2.56

1.1

786

4.10

5-MeO

-MiPT

.15

.15

DiPT

.15

.15

N,N

-DMT

2.26

0.2

1.56

0.1

816

153.36

0.4

1.26

0.2

736

1.10

Psilocin

1.46

0.2

0.92

60.58

856

717

62

2.76

2.5

806

9.30

Aminoinda

nes

2-AI

0.31

60.09

5f0.11

60.04

906

52.16

0.4f

0.33

60.06

546

151.56

0.1

1106

5N-M

ethy

l-2-AI

0.53

60.04

0.37

60.21

636

52.66

0.1

0.94

60.09

1086

143.36

0.2

546

85-IA

I0.03

06

0.00

7f0.03

36

0.01

396

624

1.16

0.4f

0.41

60.00

236

610

3.26

0.8

336

5MDAI

0.57

60.19

f0.22

60.13

956

151.86

0.1f

0.52

60.24

996

144.16

0.5

306

7Piperaz

ines

Ben

zylpiperaz

ine

.20

f.20

f

m-C

PP

0.05

46

0.01

0f0.15

60.11

606

136.66

1.1f

3.26

1.2

406

20.30

(con

tinu

ed)

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3-isobutyl-1-methylxanthine for 10 minutes at 37°C and 5% CO2.Stimulation with 0.2% dimethylsulfoxide was set as the basal level,and the effect of 30 mM b-PEA was set as the maximal response.Subsequently, the cells were lysed, and cAMP assays were performedaccording to the manufacturer’s instructions (cAMP kit; Upstate/Millipore, Schaffhausen, Switzerland). Finally, the plates were readwith a luminometer (1420 Multilabel Counter; PerkinElmer), and theamount of cAMP was calculated. The results were obtained from atleast three independent experiments. Experiments were run induplicate or triplicate. EC50 values are presented as means 6 S.D.(in micromoles). The Emax value for the functional activity data atTAAR1 describes the degree of functional activity compared with100% for the endogenous ligand and full agonist b-PEA.

ResultsThe binding affinity values (Ki), receptor activation poten-

cies (EC50), and maximal efficacy (Emax) of 104 substances aresummarized in Table 1. These substances represent thecollection of compounds in our laboratory that have been usedto characterize the in vitro pharmacology of novel designerdrugs (for review, see Liechti, 2015). The substances for thesestudies were chosen based on the availability of pure chemicalcompounds and the reported abuse of these substances. For asubset of compounds, we have previously published rat andmouse TAAR1 affinities as indicated by references in Table 1,but no human, rat, and mouse activity data. All substanceswere grouped according to their basic chemical structure(Fig. 1) as phenethylamines, amphetamines, cathinones,ephedrines, tryptamines, aminoindanes, pipradrols, andpiperazines. A few psychoactive substances, such as cocaineand lysergic acid diethylamide, were added but not classi-fied because of the lack of common basic structures.TAAR1 Binding and Functional TAAR1 Activation.

We found marked differences in affinities at TAAR1 andthe functional activation of TAAR1 among the variouspsychoactive substances. The ligand properties varied con-siderably within substance classes, with the exception ofcathinones and pipradrols, which generally exhibited noneto very weak binding to TAAR1. We also observed speciesdifferences in TAAR1 activation. At the human TAAR1, only19 substances had EC50 values that indicated functionalactivation (,10 mM), whereas the EC50 values were , 10 mMfor 52 and 68 substances at the mouse and rat TAAR1,respectively. Therefore, below we present the properties ofthe psychoactive compounds compared with the endogenousTAAR1 ligands b-PEA, p-tyramine, and tryptamine sepa-rately for each species.Human TAAR1. b-PEA and p-tyramine activated the

human TAAR1 with EC50 values of 0.26 and 0.99 mM,respectively, and showed full agonistic properties (Emax 5104% and 91%, respectively). Amphetamine, 7-APB, and 2-AIhad potency (EC50 5 0.6–2.8 mM) and agonist efficacy (Emax .89%) that were comparable to b-PEA and p-tyramine athuman TAAR1. Methamphetamine exhibited an EC50 of5.3 mM and 70% efficacy. The endogenous ligand tryptamineexhibited weak activation of human TAAR1, with an EC50 of21 mM (Emax 5 73%). Generally, most of the psychoactivecompounds that were tested were weak human TAAR1ligands, and none of them were more potent than theendogenous ligand b-PEA.Rat TAAR1. At the rat TAAR1, b-PEA had a Ki of 0.24 mM

and showed full agonism, with an EC50 of 0.11 mM, whereasTABLE

1—Con

tinued

Subs

tance

Rat

TAAR1

Mou

seTAAR1

Human

TAAR1

Recep

tor

BindingKi

Activation

Poten

cyEC50

Emax

Recep

tor

BindingKi

ActivationPoten

cyEC50

Emax

Activation

Poten

cyEC50

Emax

TFMPP

0.38

60.06

f0.75

60.18

596

162.36

0.6f

3.86

0.2

446

4.30

Pipradr

ols

2-DPMP

.10

f.10

f

D2P

M.10

f.10

f

Ethylph

enidate

.15

.15

Methox

phen

idine

.15

.15

Methylph

enidate

.15

f15

610

586

9.30

f29

63

446

15.30

Others

Cocaine

.10

c.10

c

Diclofensine

1.36

0.1

116

0.1

306

16.96

0.7

.30

.10

Diphen

idine

.15

.15

LSD

0.45

60.05

a1.46

0.4

296

810

63a

9.76

3.5

136

4.20

Methylhex

anam

ine

.15

.15

Mod

afinil

.15

.30

.15

.30

.30

aKiva

lues

forratan

dmou

seTAAR1pr

eviouslypu

blished

inRickliet

al.(20

15c).

bKiva

lues

forratan

dmou

seTAAR1pr

eviouslypu

blished

inRickliet

al.(20

15b).

c Kiva

lues

forratan

dmou

seTAAR1pr

eviouslypu

blished

inSim

mleret

al.(201

3).

dKiva

lues

forratan

dmou

seTAAR1pr

eviouslypu

blished

inSim

mleret

al.(201

4a).

e Kiva

lues

forratan

dmou

seTAAR1pr

eviouslypu

blished

inRickliet

al.(201

5a).

f Kiva

lues

forratan

dmou

seTAAR1pr

eviouslypu

blished

inSim

mleret

al.(201

4b).

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p-tyramine was more potent, with a Ki of 0.06 mM and EC50 of0.03 mM, with full agonist properties (Emax 5 94%). The thirdendogenous ligand tested, tryptamine, showed similar affinity(Ki 5 0.13 mM) to b-PEA and p-tyramine and slightly lowerfunctional activity (EC50 5 0.41 mM). Several of the screenedamphetamines (5-APB, 6-APB, 7-APB, and4-fluoroamphetamine)and phenethylamines (2C-P, 2C-T2, 2C-T4, and 2C-T7) andthe aminoindane 5-IAI had affinities and EC50 values thatwere comparable to p-tyramine, the most potent of the threeendogenous ligands at rat TAAR1, but none of these had amore potent EC50 than p-tyramine. The majority of thesepotent novel psychoactive substances exhibited full agonistproperties (Emax . 80%) at rat TAAR1. The Emax values of4-fluoroamphetamine and 2C-T4 were 78% and 67%, suggestingpartial agonism.The piperazine m-CPP and several amphetamines (4-APB,

4-fluoromethamphetamine, 5-IT, 4-methylamphetamine, and4-MTA), phenethylamines (2C-B, 2C-B-Fly, 2C-C, 2C-E, 2C-I,and 2C-N), and aminoindanes (2-AI, N-methyl-2-AI, andMDAI) were comparable to the less potent endogenous ligandsb-PEA and tryptamine in their affinities and functionalpotencies at rat TAAR1. The majority of these compoundswere partial agonists. Amphetamine and the well knownamphetamine derivatives methamphetamine, MDMA, andMDA were slightly less active than the structurally relatedendogenous ligand b-PEA.Mouse TAAR1. b-PEA and p-tyramine had equal affini-

ties at mouse TAAR1, with Ki values of 0.31 and 0.38 mM,respectively, and full agonist properties, with EC50 values of0.2 and 0.28 mM, respectively. Various amphetamines (am-phetamine, 6-APDB, 4-fluoroamphetamine, 5-IT, MDA, andPMA) and one phenethylamine (2C-P) showed similar bindingaffinities and functional potencies to these endogenousTAAR1 ligands, whereas some amphetamines were evenmorepotent (5-APB, 6-APB, 7-APB, 4-methylamphetamine, and 4-MTA), with mostly full agonist properties. The endogenousligand tryptamine was slightly weaker than b-PEA and

p-tyramine, and many phenethylamines (25E-NB2OMe,25P-NB2OMe, 25T7-NB2OMe, 2C-E, and 2C-T7), amphet-amines (4-APB, 4-fluoroamphetamine, 5-IT, methamphet-amine, and PMMA), and aminoindanes (2-AI, N-methyl-2-AI,and MDAI) were similarly active as b-PEA and p-tyramine,although all of them were partial agonists (Emax 5 36%–78%),with the exception of PMMA and MDAI (Emax 5 82% and99%, respectively). Interestingly, binding affinity did notalways predict functional potency, such as with the amino-indanes, which showed functional activities similar to am-phetamine but exhibited much lower binding affinities thanamphetamine.Differences in Activation Potencies at Human versus

Rat and Mouse TAAR1. Our results suggest significantspecies differences in TAAR1 affinities and activationpotencies for most of the substances with relevant bindingproperties in the rat. Importantly, although the endogenousligands p-tyramine and tryptamine activated TAAR1 with apotency rank order of rat . mouse . human, like manypsychostimulant compounds, b-PEA had similar EC50

values across the three species. This is relevant because acomparison of activation potencies across species with invitro assays could be biased by assay-specific variables, suchas expression levels of the transporters in the respective celllines. However, b-PEA can serve as a reference compoundfor species comparisons. Wainscott et al. (2007) also report-ed comparable EC50 values for b-PEA at rat and humanTAAR1 and species differences for other compounds. Toquantify the extent of species differences in TAAR1 activa-tion potencies, we calculated human/rat EC50 ratios andhuman/mouse EC50 ratios for substances with low tosubmicromolar (,10 mM) potencies for human TAAR1activation. The human/rat ratios ranged from 171 to 2.4,demonstrating the lower activity of the compounds at hu-man versus rat TAAR1 (Table 2). This broad range of ratiosshowed that the extent of species differences varied sub-stantially between compounds. The endogenous ligand

Fig. 1. Chemical structures of basic compounds (in bold) and location for derivatization (indicated by “R”) for compounds included in the data set.Residues for each compound are specified in Fig. 2 and Supplemental Table 1. Structural analogs were grouped according to the basic chemicalstructures for presentation of the data in tables and heat maps (Fig. 2). The generic or full chemical names for abbreviated substances are listed inSupplemental Table 1.

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tryptamine exhibited a high human/rat ratio (51). Metham-phetamine and amphetamine presented relatively lowhuman/rat ratios of 6.2 and 4.2, respectively, whereas thehuman/rat ratio for MDMA was significantly higher (35). Thehuman/mouse ratios were lower than their respective human/rat ratios for all substances, with human/rat ratios $ 8.9.Calculations of ratios for substances that were inactive athuman TAAR1 (EC50 . 10 mM) were not meaningful, butsubstantial differences between human/rat and human/mouseratios were observed among the substances that were active atrat and mouse TAAR1.Species differences and differences across substances in

TAAR1 activation potencies are presented as a heat map inFig. 2, in which the substances were sorted according totheir EC50 values for the activation of rat TAAR1. Clearly,there was an overall rank order of rat . mouse . humanacross the psychoactive substances. Figure 2 also shows thatTAAR1 binding and activation was greater for certain sub-stance classes than for others. Amphetamines, cathinones,and phenethylamines represented the three largest substanceclasses in our screen. Amphetamines and phenethylamineswere well represented among the potent TAAR1 ligands,with EC50 values within a range that could be physiologi-cally relevant (30 nM to 5 mM), whereas the activity ofcathinone derivatives was low (EC50 . 5 mM, except forcathinone). None of the pipradrols exhibited significantbinding properties. Interestingly, tryptamine derivativeswere weak agonists or did not bind to TAAR1 at all, althoughtryptamine itself is an endogenous rat and mouse TAAR1ligand, with activation potency that is comparable to b-PEAand full efficacy.

DiscussionFor this in vitro study, we determined the binding affinities

and activation potencies of a large set of psychoactivecompounds at the human, rat, and mouse TAAR1 in heterol-ogous expression systems. We also characterized the ligandsas full or partial agonists. None of the active compounds hadfull antagonist properties. As indicated by our previousstudies (Simmler et al., 2013, 2014a), cathinone derivativesstood out as poor TAAR1 ligands. Most of the other psychoac-tive compounds were potent to moderate rat and mouseTAAR1 agonists but exhibited generally weak or no activityat human TAAR1. The active compounds showed full orpartial TAAR1 agonist properties, with generally no distinctpatterns related to their chemical structure.To our knowledge, our screening is the most extensive

published data set to date, which included 101 psychoactivesubstances and 3 endogenous ligands as comparator com-pounds. The in vitro pharmacology of comparator com-pounds and some psychoactive substances (amphetamine,methamphetamine, MDMA) were previously determined byus and others (Borowsky et al., 2001; Bunzow et al., 2001;Reese et al., 2007; Wainscott et al., 2007; Lindemann et al.,2008; Lewin et al., 2011). The replication of those datafor this study was an important validation of our assays.Furthermore, because we determined binding affinities forsome novel psychoactive substances in earlier studies, weincluded these data in this study. As a result, all datadetermined by our laboratory are conveniently summarizedhere in Table 1.Species differences in TAAR1 activation between rodent

and human receptors have been reported previously forphenethylamine analogs (Wainscott et al., 2007), p-tyramine,and methamphetamine (Reese et al., 2007). These compoundshave consistently exhibited lower potencies for human TAAR1activation than for rodent TAAR1 activation. Structure-activity correlations for b-PEA derivatives with regard tohuman TAAR1 activation have shown that bulky residues onthe amine or phenyl ring reduced ligand potency (Lewin et al.,2008). Reduced human TAAR1 activity could be expected fornovel psychoactive substances for which substantial derivati-zation is typical. Together with previous reports on speciesdifferences, the data provide evidence that many psychoactivesubstances are considerably less potent at human TAAR1than at mouse or rat TAAR1. In rodents, psychoactivecompounds could reduce neuronal firing via TAAR1 activation,comparable to the endogenous TAAR1 ligand p-tyramine,which has been shown to reduce the DA neuron firingrate (Bradaia et al., 2009). Consequently, the psychoactiveTAAR1 ligands likely exert autoregulatory effects on theirTAAR1-independent effects, such as reducing drug-inducedDA release in the striatum (Di Cara et al., 2011). Given thatstudies in rodents have reported autoregulatory effects of thepsychostimulant TAAR1 ligands amphetamine, methamphet-amine, and MDMA (Lindemann et al., 2008; Di Cara et al.,2011; Achat-Mendes et al., 2012; Harkness et al., 2015), thesespecies differences at TAAR1 could be relevant to the trans-lational validity of preclinical studies. Particularly for novelpsychoactive substances with large TAAR1 species differ-ences, the abuse liability that is evaluated in rodent modelsmay actually underestimate the risk for addiction that isposed by the drugs in humans.

TABLE 2EC50 ratios calculated for all substances with EC50 values , 10 mM forthe human TAAR1Ratios are ranked according to the human/rat ratio. Values . 1 indicate lowerpotency at the human TAAR1 versus the rat or mouse TAAR1.

Substance

EC50 Ratio

Structure ClassHuman/Rata

Human/Mouse

6-APB 171 107 Amphetamines2C-P 140 7.5 Phenethylamines5-IAI 97 7.8 Aminoindanes5-APB 91 47 AmphetaminesTryptamine 51 7.8 Endogenous

ligandsb

4-Fluoroamphetamine 51 27 Amphetamines4-Fluoromethamphetamine 39 13 AmphetaminesMDMA 35 8.6 Amphetaminesp-Tyramine 33 3.5 Endogenous

ligandsc

4-APB 26 4.8 AmphetaminesMDAI 19 7.9 Aminoindanes2C-B 14 1.4 Phenethylamines2-AI 14 4.5 Aminoindanes7-APB 11 5.7 AmphetaminesN-Methyl-2-AI 8.9 3.5 AminoindanesMethamphetamine 6.2 7.3 AmphetaminesCathinone 5.8 5.8 CathinonesMDA 4.9 6.2 Amphetamines2C-H 4.3 0.9 PhenethylaminesAmphetamine 4.2 5.3 Amphetaminesb-PEA 2.4 1.3 Endogenous

ligandsc

aSubstances are sorted according to human/rat ratios.bStructure class: tryptamines.cStructure class: phenethylamines.

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Species differences in TAAR1/ligand interactions have beenpredicted from sequence alignment studies that compared thecritical residues for the binding of b-PEA, showing that aminoacids that correspond to the critical residues differ betweenrat, mouse, and human TAAR1 (Kratochwil et al., 2011). Site-directed mutagenesis studies have identified two locations inTAAR1 transmembrane domains 6 and 7, where amino acidsubstitutions markedly reduce or increase methamphetamineTAAR1 activation potencies in the rat and mouse TAAR1(Reese et al., 2014). Docking studies with a homologymodel forthe human TAAR1 (Cichero et al., 2013, 2014) could serve tofurther elucidate the essential amino acids that are requiredfor ligand binding and discover structural determinants forthe TAAR1 activity or inactivity of psychoactive substances.

Importantly, TAAR1 is a promising target for therapeuticdrugs for the treatment of substance use disorders, regardlessof species differences in the direct TAAR1 agonism propertiesof psychoactive substances. TAAR1 agonists that have beenreported in the literature are similarly potent at both humanand rat TAAR1. Furthermore, the efficacy that has beenreported in animal models is comparable to the efficacy thathas been reported in in vitro expression systems, which mayprovide a basis for predicting effective doses in humans. TheTAAR1 partial agonist RO5203648 effectively reduced cocaineself-administration and relapse to drug-seeking behavior inrats (Revel et al., 2012b; Pei et al., 2014), although cocaineis not a TAAR1 ligand itself. TAAR1 partial agonism mark-edly reduced cocaine-induced DA overflow in the nucleus

Fig. 2. Heat map illustrating the diversity of TAAR1 activity between individual substances and between human, rat, and mouse TAAR1. Thesubstances are sorted according to their rat TAAR1 activity (EC50 values). The compounds were split into the 52more active (A) and the 51 less active (B)rat TAAR1 ligands. Next to the substance names, the respective substance classes are specified by color code and basic chemical structures are definedby numbers. The residues R2–R11 refer to the chemical structures presented in Fig. 1. Underlined residues indicate ring structures between twolocations for derivatization. The generic or full chemical names for abbreviated substances are listed in Supplemental Table 1.

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accumbens (Pei et al., 2014). Because TAAR1 is involved in theconstitutive regulation of neuronal firing (Bradaia et al.,2009), pharmacological TAAR1 activation with a therapeuticdrug may regulate neuronal firing and result in hyposensi-tivity to drugs, similar to the overexpression of TAAR1 in atransgenic mouse model (Revel et al., 2012a). Moreover, theefficacy of these potentially therapeutic compounds could beeven greater in humans than in rodents. In rodents, but not orless so in humans, TAAR1-mediated negative feedback thatis induced by the abused substances could be present andattenuate the extent of therapeutic drug effects.Ex vivo electrophysiology experiments in the ventral teg-

mental area and dorsal raphe nuclei showed that both partialagonists and antagonists enhanced DA and 5-HT neuron

firing rates in WT mice (Bradaia et al., 2009; Revel et al.,2012b), whereas full agonists like p-tyramine decreased firingrates (Revel et al., 2011, 2012b). However, both full and partialagonists have been shown to be protective against the re-warding and reinforcing effects of the psychostimulant cocaine(Pei et al., 2015), but the opposing effects of full and partialagonists on firing rates suggest that psychoactive substancesthat are full agonists would exert effects that are differentfrom partial agonists. Data on the full or partial agonistproperties of TAAR1 ligands are thus important. Whereas fullagonists such as amphetamine induce negative feedback toblunt their own effect on DA and 5-HT systems (Lindemannet al., 2008; Di Cara et al., 2011), partial agonists mightincrease their effect on neuronal signal transmission by

Fig. 2. Continued.

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increasing firing rates via TAAR1. This is an assumption thatwould be based on findings with selective TAAR1 ligands andrequires further investigation.In our data set and based on data reported previously by two

different laboratories (Reese et al., 2007; Wainscott et al.,2007), the activation potencies of b-PEA at rat, human, andmouse TAAR1 exhibited similar EC50 values between species,whereas p-tyramine was more potent at rat TAAR1, followedby mouse and human TAAR1. Given that these data weregenerated in independent laboratories that used differentassay conditions and expression systems, the similarities ofthe pharmacological profiles suggest good consistency of thedata and support the validity of the comparisons betweenspecies.In this study, we simply determined activity at specific

targets, which is common with interpretations of in vitro data,and we did not take into account that the processes that allowa substance to interact with TAAR1 in vivo depend on morevariables than solely substance/receptor interactions. Thelocation of TAAR1 expression is mostly intracellular inneurons (Miller, 2011) and also in glial cells (Cisneros andGhorpade, 2014). Because the substances need to reach thelocation of expression of TAAR1 to bind to the receptor, theintracellular availability of the ligands is also relevant.Certain psychoactive substances, such as amphetamine de-rivatives, are substrates of monoaminergic transporters andcarried into the cell (Zaczek et al., 1991). These substrate-typesubstances, therefore, might be more likely available tointracellular TAAR1 than substances that are not trans-porter substrates, including, for example, cocaine, MDPV, otherpyrovalerone cathinones, methylphenidate, and other pipra-drols (Simmler et al., 2013, 2014b). One limitation of our studyis that we did not consider stereoselectivity of the compoundsby screening racemic mixtures for most substances. As withactivity at other psychostimulant targets, such as monoamin-ergic reuptake transporters, TAAR1 has a stereoselective bind-ing site, and the assessment of racemates could underestimatethe activity of the more active isomer (Lewin et al., 2011).In conclusion, we provide an extensive data set on the ligand

properties of psychoactive substances at TAAR1. With differ-ences between activity at rodent and human TAAR1, weprovide evidence of significant species differences in interac-tions between TAAR1 and psychoactive drugs, which could berelevant to the translational validity of preclinical studies toclinical applications.

Acknowledgments

The authors thank Lipomed for providing the 2C andNBOMedrugsat no cost, Michael Arends for text editing, and Roger Norcross forhelpful discussions.

Authorship Contributions

Participated in research design: Hoener, Liechti.Conducted experiments: Buchy, Chaboz.Performed data analysis: Simmler, Buchy, Chaboz, Hoener.Wrote or contributed to the writing of the manuscript: Simmler,

Hoener, Liechti.

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Address correspondence to: Dr. Matthias E. Liechti, Division of ClinicalPharmacology and Toxicology, Department of Biomedicine, University Hospi-tal Basel, Hebelstrasse 2, CH-4031 Basel, Switzerland. E-mail: [email protected]

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