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Article ; Online: Guest editorial for special issue on imaging mass spectrometry.

Castellino, Stephen

2020 Volume 55, Issue 4, Page(s) e4507

Language	English
Publishing date	2020-04-08
Publishing country	England
Document type	Editorial
ZDB-ID	1221763-3
ISSN	1096-9888 ; 1076-5174
ISSN (online)	1096-9888
ISSN	1076-5174
DOI	10.1002/jms.4507
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Zs.MO 220: Show issues

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Article ; Online: The emergence of imaging mass spectrometry in drug discovery and development: Making a difference by driving decision making.

Castellino, Stephen / Lareau, Nichole M / Groseclose, Mark Reid

Journal of mass spectrometry : JMS

2021 Volume 56, Issue 8, Page(s) e4717

Abstract: The pharmaceutical industry is a dynamic, science-driven business constantly under pressure to innovate and morph into a higher performing organization. Innovations can include the implementation of new technologies, adopting new scientific methods, ... ...

Abstract	The pharmaceutical industry is a dynamic, science-driven business constantly under pressure to innovate and morph into a higher performing organization. Innovations can include the implementation of new technologies, adopting new scientific methods, changing the decision-making process, compressing timelines, or making changes to the organizational structure. The drivers for the constant focus on performance improvement are the high cost of R&D as well as the lengthy timelines required to deliver new medicines for unmet needs. Successful innovations are measured against both the quality and quantity of potential new medicines in the pipeline and the delivery to patients. In this special feature article, we share our collective experience implementing matrix-assisted laser desorption/ionization imaging mass spectrometry (MALDI IMS) technology as an innovative approach to better understand the tissue biodistribution of drugs in the early phases of drug discovery to establish pharmacokinetic-pharmacodynamic (PK-PD) relationships, as well as in the development phase to understand pharmacology, toxicology, and disease pathogenesis. In our experience, successful implementation of MALDI IMS in support of therapeutic programs can be measured by the impact IMS studies have on driving decision making in pipeline progression. This provides a direct quantifiable measurement of the return to the organization for the investment in IMS. We have included discussion not only on the technical merits of IMS study conduct but also the key elements of setting study objectives, building collaborations, data integration into the medicine progression milestones, and potential pitfalls when trying to establish IMS in the pharmaceutical arena. We categorized IMS study types into five groups that parallel pipeline progression from the earliest phases of discovery to late stages of preclinical development. We conclude the article with some perspectives on how we see MALDI IMS maintaining relevance and becoming further embedded as an essential tool in the constantly changing environment of the pharmaceutical industry.
MeSH term(s)	Decision Making ; Drug Discovery ; Humans ; Mass Spectrometry ; Pharmacokinetics ; Tissue Distribution
Language	English
Publishing date	2021-03-16
Publishing country	England
Document type	Journal Article
ZDB-ID	1221763-3
ISSN	1096-9888 ; 1076-5174
ISSN (online)	1096-9888
ISSN	1076-5174
DOI	10.1002/jms.4717
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Zs.MO 220: Show issues

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Article ; Online: An Investigation into Retigabine (Ezogabine) Associated Dyspigmentation in Rat Eyes by MALDI Imaging Mass Spectrometry.

Groseclose, M Reid / Castellino, Stephen

Chemical research in toxicology

2019 Volume 32, Issue 2, Page(s) 294–303

Abstract: Retigabine (RTG) is an antiepileptic drug approved as an adjunctive treatment for refractory partial-onset seizures in adults. In April 2013, the Food and Drug Administration issued a warning that RTG could cause changes in retinal pigmentation and ... ...

Abstract	Retigabine (RTG) is an antiepileptic drug approved as an adjunctive treatment for refractory partial-onset seizures in adults. In April 2013, the Food and Drug Administration issued a warning that RTG could cause changes in retinal pigmentation and discoloration of skin, resulting in a blue appearance. As part of a larger preclinical effort to gain a mechanistic understanding as to the origins of retinal pigment changes associated with RTG, we conducted a long-term repeat dosing study in rats. Matrix-assisted laser desorption/ionization imaging mass spectrometry (MALDI IMS) was used to determine the distribution of RTG and its metabolites in the rat eye following 13 and 39 weeks of dosing. IMS revealed the presence of RTG, a previously characterized N-acetyl metabolite of RTG (NAMR), and several species structurally related through the dimerization of RTG and NAMR. These species were highly localized to the melanin-containing layers of the uveal tract of the rat eye including the choroid, ciliary body, and iris, suggesting that the formation of these dimers occurs from melanin bound RTG and NAMR. Furthermore, several of the RTG-related dimers have UV absorbance which give them a purple color in solution. We propose that the melanin binding of RTG and NAMR effectively concentrates the two compounds to enable mixed condensation reactions to occur when the binding provides the proper geometry in the redox environment of the uveal tissues. High lateral resolution images illustrate that the blood-retinal barrier effectively restricts retinal access to RTG-related compounds. The spatial information provided by MALDI IMS was critical in contextualizing the homogenate concentrations of key RTG-related compounds and helped provide a basis for the mechanism of dimer formation.
MeSH term(s)	Animals ; Carbamates/metabolism ; Carbamates/pharmacology ; Dimerization ; Male ; Melanins/chemistry ; Melanins/metabolism ; Phenylenediamines/metabolism ; Phenylenediamines/pharmacology ; Rats ; Rats, Long-Evans ; Retinal Pigments/analysis ; Spectrometry, Mass, Matrix-Assisted Laser Desorption-Ionization ; Uvea/drug effects ; Uvea/metabolism ; Uvea/pathology
Chemical Substances	Carbamates ; Melanins ; Phenylenediamines ; Retinal Pigments ; ezogabine (12G01I6BBU)
Language	English
Publishing date	2019-01-31
Publishing country	United States
Document type	Journal Article
ZDB-ID	639353-6
ISSN	1520-5010 ; 0893-228X
ISSN (online)	1520-5010
ISSN	0893-228X
DOI	10.1021/acs.chemrestox.8b00313
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Zs.A 2320: Show issues

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Article: The emergence of imaging mass spectrometry in drug discovery and development: Making a difference by driving decision making

Castellino, Stephen / Lareau, Nichole M. / Groseclose, Mark Reid

Journal of mass spectrometry. 2021 Aug., v. 56, no. 8

2021

Abstract: The pharmaceutical industry is a dynamic, science‐driven business constantly under pressure to innovate and morph into a higher performing organization. Innovations can include the implementation of new technologies, adopting new scientific methods, ... ...

Abstract	The pharmaceutical industry is a dynamic, science‐driven business constantly under pressure to innovate and morph into a higher performing organization. Innovations can include the implementation of new technologies, adopting new scientific methods, changing the decision‐making process, compressing timelines, or making changes to the organizational structure. The drivers for the constant focus on performance improvement are the high cost of R&D as well as the lengthy timelines required to deliver new medicines for unmet needs. Successful innovations are measured against both the quality and quantity of potential new medicines in the pipeline and the delivery to patients. In this special feature article, we share our collective experience implementing matrix‐assisted laser desorption/ionization imaging mass spectrometry (MALDI IMS) technology as an innovative approach to better understand the tissue biodistribution of drugs in the early phases of drug discovery to establish pharmacokinetic‐pharmacodynamic (PK‐PD) relationships, as well as in the development phase to understand pharmacology, toxicology, and disease pathogenesis. In our experience, successful implementation of MALDI IMS in support of therapeutic programs can be measured by the impact IMS studies have on driving decision making in pipeline progression. This provides a direct quantifiable measurement of the return to the organization for the investment in IMS. We have included discussion not only on the technical merits of IMS study conduct but also the key elements of setting study objectives, building collaborations, data integration into the medicine progression milestones, and potential pitfalls when trying to establish IMS in the pharmaceutical arena. We categorized IMS study types into five groups that parallel pipeline progression from the earliest phases of discovery to late stages of preclinical development. We conclude the article with some perspectives on how we see MALDI IMS maintaining relevance and becoming further embedded as an essential tool in the constantly changing environment of the pharmaceutical industry.
Keywords	decision making ; desorption ; drugs ; ionization ; mass spectrometry ; medicine ; organization of work ; pathogenesis ; pharmaceutical industry ; pharmacology ; therapeutics ; toxicology
Language	English
Dates of publication	2021-08
Publishing place	John Wiley & Sons, Ltd
Document type	Article
Note	JOURNAL ARTICLE
ZDB-ID	1221763-3
ISSN	1096-9888 ; 1076-5174
ISSN (online)	1096-9888
ISSN	1076-5174
DOI	10.1002/jms.4717
Database	NAL-Catalogue (AGRICOLA)

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Zs.A 4254: Show issues			Location: Je nach Verfügbarkeit (siehe Angabe bei Bestand) bis Jg. 1994: Bestellungen von Artikeln über das Online-Bestellformular Jg. 1995 - 2021: Lesesall (2.OG) ab Jg. 2022: Lesesaal (EG)
Zs.MO 220: Show issues

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Article ; Online: MALDI imaging MS analysis of drug distribution in tissue: the right time!(?).

Castellino, Stephen

Bioanalysis

2012 Volume 4, Issue 21, Page(s) 2549–2551

MeSH term(s)	Drug Discovery ; Pharmaceutical Preparations/analysis ; Pharmaceutical Preparations/metabolism ; Spectrometry, Mass, Matrix-Assisted Laser Desorption-Ionization ; Tissue Distribution ; Tissue Fixation
Chemical Substances	Pharmaceutical Preparations
Language	English
Publishing date	2012-11
Publishing country	England
Document type	Editorial
ISSN	1757-6199
ISSN (online)	1757-6199
DOI	10.4155/bio.12.251
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Mapping the Lipids of Skin Sebaceous Glands and Hair Follicles by High Spatial Resolution MALDI Imaging Mass Spectrometry.

Xie, Fang / Groseclose, Mark Reid / Tortorella, Sara / Cruciani, Gabriele / Castellino, Stephen

Pharmaceuticals (Basel, Switzerland)

2022 Volume 15, Issue 4

Abstract: Matrix-assisted laser desorption/ionization (MALDI) imaging mass spectrometry (IMS) is a technology that utilizes the high sensitivity and specificity of mass spectrometry, combined with a high spatial resolution to characterize the molecular species ... ...

Abstract	Matrix-assisted laser desorption/ionization (MALDI) imaging mass spectrometry (IMS) is a technology that utilizes the high sensitivity and specificity of mass spectrometry, combined with a high spatial resolution to characterize the molecular species present in skin tissue. In this article, we use MALDI IMS to map specific lipids characteristic of two important skin appendages in minipig skin: the sebaceous glands and hair follicles. A set of specific lipid markers linked to the synthesis of sebum, stages of sebum production, and the secretion of sebum for two different sebaceous gland subzones, the peripheral and central necrotic, were identified. Furthermore, biochemical pathway analysis of the identified markers provides potential drug-targeting strategies to reduce sebum overproduction in pathological conditions. In addition, specific lipid markers characteristic of the different layers in the hair follicle bulge area, including the outer root sheath, the inner root sheath, and the medulla that are associated with the growth cycles of the hair, were determined. This research highlights the ability of MALDI IMS to link a molecular distribution not only to the morphological features in skin tissue but to the physiological state as well. Thus, this platform can provide a basis for the investigation of biochemical pathways as well as the mechanisms of disease and pharmacology in the skin, which will ultimately be critical for drug discovery and the development of dermatology-related illnesses.
Language	English
Publishing date	2022-03-28
Publishing country	Switzerland
Document type	Journal Article
ZDB-ID	2193542-7
ISSN	1424-8247
ISSN	1424-8247
DOI	10.3390/ph15040411
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Article ; Online: Quantification and assessment of detection capability in imaging mass spectrometry using a revised mimetic tissue model.

Barry, Jeremy A / Groseclose, Mark Reid / Castellino, Stephen

Bioanalysis

2019 Volume 11, Issue 11, Page(s) 1099–1116

Abstract: Aim: ...

Abstract	Aim:
MeSH term(s)	Animals ; Brain ; Chlorpropamide/analogs & derivatives ; Chlorpropamide/analysis ; Clozapine/analysis ; Liver/chemistry ; Male ; Mass Spectrometry ; Models, Biological ; Nucleosides/analysis ; Rats ; Rats, Wistar ; Skin/chemistry ; Swine
Chemical Substances	API 2 ; NSC 177223 ; Nucleosides ; Clozapine (J60AR2IKIC) ; Chlorpropamide (WTM2C3IL2X)
Language	English
Publishing date	2019-07-08
Publishing country	England
Document type	Journal Article
ISSN	1757-6199
ISSN (online)	1757-6199
DOI	10.4155/bio-2019-0035
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Mapping the Lipids of Skin Sebaceous Glands and Hair Follicles by High Spatial Resolution MALDI Imaging Mass Spectrometry

Fang Xie / Mark Reid Groseclose / Sara Tortorella / Gabriele Cruciani / Stephen Castellino

Pharmaceuticals, Vol 15, Iss 4, p

2022 Volume 411

Abstract	Matrix-assisted laser desorption/ionization (MALDI) imaging mass spectrometry (IMS) is a technology that utilizes the high sensitivity and specificity of mass spectrometry, combined with a high spatial resolution to characterize the molecular species present in skin tissue. In this article, we use MALDI IMS to map specific lipids characteristic of two important skin appendages in minipig skin: the sebaceous glands and hair follicles. A set of specific lipid markers linked to the synthesis of sebum, stages of sebum production, and the secretion of sebum for two different sebaceous gland subzones, the peripheral and central necrotic, were identified. Furthermore, biochemical pathway analysis of the identified markers provides potential drug-targeting strategies to reduce sebum overproduction in pathological conditions. In addition, specific lipid markers characteristic of the different layers in the hair follicle bulge area, including the outer root sheath, the inner root sheath, and the medulla that are associated with the growth cycles of the hair, were determined. This research highlights the ability of MALDI IMS to link a molecular distribution not only to the morphological features in skin tissue but to the physiological state as well. Thus, this platform can provide a basis for the investigation of biochemical pathways as well as the mechanisms of disease and pharmacology in the skin, which will ultimately be critical for drug discovery and the development of dermatology-related illnesses.
Keywords	MALDI imaging mass spectrometry ; sebaceous glands ; hair follicles ; Medicine ; R ; Pharmacy and materia medica ; RS1-441
Subject code	571
Language	English
Publishing date	2022-03-01T00:00:00Z
Publisher	MDPI AG
Document type	Article ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Article ; Online: Multimodal imaging distribution assessment of a liposomal antibiotic in an infectious disease model.

Cheng, Shih-Hsun / Groseclose, M Reid / Mininger, Cindy / Bergstrom, Mats / Zhang, Lily / Lenhard, Stephen C / Skedzielewski, Tinamarie / Kelley, Zachary D / Comroe, Debra / Hong, Hyundae / Cui, Haifeng / Hoover, Jennifer L / Rittenhouse, Steve / Castellino, Stephen / Jucker, Beat M / Alsaid, Hasan

Journal of controlled release : official journal of the Controlled Release Society

2022 Volume 352, Page(s) 199–210

Abstract: Liposomes are promising targeted drug delivery systems with the potential to improve the efficacy and safety profile of certain classes of drugs. Though attractive, there are unique analytical challenges associated with the development of liposomal drugs ...

Abstract	Liposomes are promising targeted drug delivery systems with the potential to improve the efficacy and safety profile of certain classes of drugs. Though attractive, there are unique analytical challenges associated with the development of liposomal drugs including human dose prediction given these are multi-component drug delivery systems. In this study, we developed a multimodal imaging approach to provide a comprehensive distribution assessment for an antibacterial drug, GSK2485680, delivered as a liposomal formulation (Lipo680) in a mouse thigh model of bacterial infection to support human dose prediction. Positron emission tomography (PET) imaging was used to track the in vivo biodistribution of Lipo680 over 48 h post-injection providing a clear assessment of the uptake in various tissues and, importantly, the selective accumulation at the site of infection. In addition, a pharmacokinetic model was created to evaluate the kinetics of Lipo680 in different tissues. Matrix-assisted laser desorption/ionization (MALDI) imaging mass spectrometry (IMS) was then used to quantify the distribution of GSK2485680 and to qualitatively assess the distribution of a liposomal lipid throughout sections of infected and non-infected hindlimb tissues at high spatial resolution. Through the combination of both PET and MALDI IMS, we observed excellent correlation between the Lipo680-radionuclide signal detected by PET with the GSK2485680 and lipid component signals detected by MALDI IMS. This multimodal translational method can reduce drug attrition by generating comprehensive biodistribution profiles of drug delivery systems to provide mechanistic insight and elucidate safety concerns. Liposomal formulations have potential to deliver therapeutics across a broad array of different indications, and this work serves as a template to aid in delivering future liposomal drugs to the clinic.
MeSH term(s)	Animals ; Mice ; Humans ; Liposomes/chemistry ; Tissue Distribution ; Anti-Bacterial Agents ; Spectrometry, Mass, Matrix-Assisted Laser Desorption-Ionization/methods ; Positron-Emission Tomography ; Multimodal Imaging ; Lipids ; Communicable Diseases
Chemical Substances	Liposomes ; Anti-Bacterial Agents ; Lipids
Language	English
Publishing date	2022-10-20
Publishing country	Netherlands
Document type	Journal Article
ZDB-ID	632533-6
ISSN	1873-4995 ; 0168-3659
ISSN (online)	1873-4995
ISSN	0168-3659
DOI	10.1016/j.jconrel.2022.08.061
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Zs.A 2055: Show issues

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Article ; Online: A mimetic tissue model for the quantification of drug distributions by MALDI imaging mass spectrometry.

Groseclose, M Reid / Castellino, Stephen

Analytical chemistry

2013 Volume 85, Issue 21, Page(s) 10099–10106

Abstract: The full potential of imaging mass spectrometry (IMS) as a tool in drug development will not be realized until reliable quantitative information can be integrated with the molecular distributions. Here we report a novel method for the quantification of ... ...

Abstract	The full potential of imaging mass spectrometry (IMS) as a tool in drug development will not be realized until reliable quantitative information can be integrated with the molecular distributions. Here we report a novel method for the quantification of drugs in tissue sections using matrix-assisted laser desorption/ionization (MALDI) IMS. This method uses a mimetic tissue model consisting of a set of tissue homogenates spiked with a range of different drug concentrations that have been frozen into a polymer support mold. The goal of this model is to mimic a dosed tissue in its effects on analyte extraction and ion suppression. Parallel preparation and analysis of sections from the tissue model and the dosed tissues allow for the quantification of a drug's distribution. Here we detail the steps involved in constructing the model and provide proof of concept data to highlight the potential of this approach. Several figures of merit are evaluated including linearity of response, variability, and section-to-section reproducibility. Finally, the tissue model is used to quantify two different drugs, lapatinib and nevirapine, in dosed tissues from nonclinical species and the results are compared with those generated by LC-MS quantification.
MeSH term(s)	Animals ; Female ; Mice ; Models, Theoretical ; Pharmaceutical Preparations/analysis ; Rats ; Spectrometry, Mass, Matrix-Assisted Laser Desorption-Ionization/methods
Chemical Substances	Pharmaceutical Preparations
Language	English
Publishing date	2013-11-05
Publishing country	United States
Document type	Journal Article
ZDB-ID	1508-8
ISSN	1520-6882 ; 0003-2700
ISSN (online)	1520-6882
ISSN	0003-2700
DOI	10.1021/ac400892z
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