International Journal of Molecular Sciences

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Open AccessEditorial

PET Molecular Imaging: Old Habits Do Not Die, They Only Evolve into New Applications

by Ferdinando F. Calabria

Int. J. Mol. Sci. 2024, 25(1), 403; https://doi.org/10.3390/ijms25010403 - 28 Dec 2023

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Abstract

The first studies on human applications of radioisotopes for the in vivo targeting of pathophysiological processes began in the late 1930s in Western Europe and the USA with ^99mTc [...] Full article

(This article belongs to the Special Issue Novel PET Radiopharmaceuticals: Molecular Probes for Personalized Imaging)

Research

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11 pages, 1637 KiB

Open AccessArticle

Beyond Visual Assessment of Basal Ganglia Uptake: Can Automated Method and Pineal Body Uptake Assessment Improve Identification of Nigrostriatal Dysfunction on ¹⁸F-DOPA PET/CT?

by Shir Hazut Krauthammer, Dan Cohen, Einat Even-Sapir and Hedva Lerman

Int. J. Mol. Sci. 2023, 24(6), 5683; https://doi.org/10.3390/ijms24065683 - 16 Mar 2023

Cited by 2 | Viewed by 2201

Abstract

The interpretation of ¹⁸F-DOPA PET/CT performed for assessing nigrostriatal dysfunction (NSD) is usually based on visual assessment of the uptake in the basal ganglia (VA-BG). In the present study, we evaluate the diagnostic performance of an automated method that assesses BG uptake [...] Read more.

The interpretation of ¹⁸F-DOPA PET/CT performed for assessing nigrostriatal dysfunction (NSD) is usually based on visual assessment of the uptake in the basal ganglia (VA-BG). In the present study, we evaluate the diagnostic performance of an automated method that assesses BG uptake (AM-BG) and of methods that assess pineal body uptake, and examine whether these methods can enhance the diagnostic performance of VA-BG alone. We retrospectively included 112 scans performed in patients with clinically suspected NSD who also had a subsequent final clinical diagnosis provided by a movement disorder specialist (69 NSD and 43 non-NSD patients). All scans were categorized as positive or negative based on (1) VA-BG, (2) AM-BG, and (3) qualitative and semiquantitative assessment of pineal body uptake. VA-BG, AM-BG, assessment of pineal body ¹⁸F-DOPA uptake by VA (uptake > background), by SUVmax (≥0.72), and by pineal to occipital ratio (POR ≥ 1.57) could all significantly differentiate NSD from non-NSD patients (Pv < 0.01 for all five methods). Of these methods, VA-BG provided the highest sensitivity (88.4%) and accuracy (90.2%). Combining VA-BG with AM-BG did not improve diagnostic accuracy. An interpretation algorithm that combines VA-BG with pineal body uptake assessment by POR calculation increased sensitivity to 98.5%, at the expense of decreased specificity. In conclusion, an automated method that assesses ¹⁸F-DOPA uptake in the BG and assessment of pineal body ¹⁸F-DOPA uptake can significantly separate NSD from non-NSD patients, with apparent inferior diagnostic performance when applied alone compared with VA-BG. When VA-BG categorizes a scan as negative or equivocal, assessment of the ¹⁸F-DOPA uptake in the pineal body has the potential to minimize the rate of false negative reports. Further research is essential to validate this approach and to study the pathophysiologic relationship between ¹⁸F-DOPA uptake in the pineal body and nigrostriatal dysfunction. Full article

(This article belongs to the Special Issue Novel PET Radiopharmaceuticals: Molecular Probes for Personalized Imaging)

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7 pages, 1272 KiB

Open AccessCommunication

Superiority of [¹¹C]methionine over [¹⁸F]deoxyglucose for PET Imaging of Multiple Cancer Types Due to the Methionine Addiction of Cancer

by Yutaro Kubota, Toshihiko Sato, Chihiro Hozumi, Qinghong Han, Yusuke Aoki, Noriyuki Masaki, Koya Obara, Takuya Tsunoda and Robert M. Hoffman

Int. J. Mol. Sci. 2023, 24(3), 1935; https://doi.org/10.3390/ijms24031935 - 18 Jan 2023

Cited by 20 | Viewed by 2585

Abstract

Positron emission tomography (PET) is widely used to detect cancers. The usual isotope for PET imaging of cancer is [¹⁸F]deoxyglucose. The premise of using [¹⁸F]deoxyglucose is that cancers are addicted to glucose (The Warburg effect). However, cancers are more [...] Read more.

Positron emission tomography (PET) is widely used to detect cancers. The usual isotope for PET imaging of cancer is [¹⁸F]deoxyglucose. The premise of using [¹⁸F]deoxyglucose is that cancers are addicted to glucose (The Warburg effect). However, cancers are more severely addicted to methionine (The Hoffman effect). [¹¹C]methionine PET (MET-PET) has been effectively used for the detection of glioblastoma and other cancers in the brain, and in comparison, MET-PET has been shown to be more sensitive and accurate than [¹⁸F]deoxyglucose PET (FDG-PET). However, MET-PET has been limited to cancers in the brain. The present report describes the first applications of MET-PET to cancers of multiple organs, including rectal, bladder, lung, and kidney. The results in each case show that MET-PET is superior to FDG-PET due to the methionine addiction of cancer and suggest that the broad application of MET-PET should be undertaken for cancer detection. Full article

(This article belongs to the Special Issue Novel PET Radiopharmaceuticals: Molecular Probes for Personalized Imaging)

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15 pages, 20627 KiB

Open AccessArticle

Late-Stage Functionalization through Click Chemistry Provides GLUT5-Targeting Glycoconjugate as a Potential PET Imaging Probe

by Adelina Oronova and Marina Tanasova

Int. J. Mol. Sci. 2023, 24(1), 173; https://doi.org/10.3390/ijms24010173 - 22 Dec 2022

Cited by 4 | Viewed by 3003

Abstract

The targeting of facilitative sugar transporters (GLUTs) has been utilized in the development of tools for diagnostics and therapy. The interest in this area is promoted by the phenomenon of alterations in cellular metabolic processes that are linked to multitudes of metabolic disorders [...] Read more.

The targeting of facilitative sugar transporters (GLUTs) has been utilized in the development of tools for diagnostics and therapy. The interest in this area is promoted by the phenomenon of alterations in cellular metabolic processes that are linked to multitudes of metabolic disorders and diseases. However, nonspecific targeting (e.g., glucose-transporting GLUTs) leads to a lack of disease detection efficiency. Among GLUTs, GLUT5 stands out as a prominent target for developing specific molecular tools due to its association with metabolic diseases, including cancer. This work reports a non-radiolabeled fluoride (¹⁹F) coumarin-based glycoconjugate of 2,5-anhydro-D-mannitol as a potential PET imaging probe that targets the GLUT5 transporter. Inherent fluorescent properties of the coumarin fluorophore allowed us to establish the probe’s uptake efficiency and GLUT5-specificity in a GLUT5-positive breast cell line using fluorescence detection techniques. The click chemistry approach employed in the design of the probe enables late-stage functionalization, an essential requirement for obtaining the radiolabeled analog of the probe for future in vivo cancer imaging applications. The high affinity of the probe to GLUT5 allowed for the effective uptake in nutrition-rich media. Full article

(This article belongs to the Special Issue Novel PET Radiopharmaceuticals: Molecular Probes for Personalized Imaging)

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13 pages, 2698 KiB

Open AccessArticle

Oxidation-Cyclisation of Biphenyl Thioethers to Dibenzothiophenium Salts for Ultrarapid ¹⁸F-Labelling of PET Tracers

by Fatih Sirindil, Sinead Maher, Michael Schöll, Kerstin Sander and Erik Årstad

Int. J. Mol. Sci. 2022, 23(24), 15481; https://doi.org/10.3390/ijms232415481 - 7 Dec 2022

Cited by 1 | Viewed by 2370

Abstract

¹⁸F-labelled radiotracers are in high demand and play an important role for diagnostic imaging with positron emission tomography (PET). Challenges associated with the synthesis of the labelling precursors and the incorporation of [¹⁸F]fluoride with practical activity yields at batch scale [...] Read more.

¹⁸F-labelled radiotracers are in high demand and play an important role for diagnostic imaging with positron emission tomography (PET). Challenges associated with the synthesis of the labelling precursors and the incorporation of [¹⁸F]fluoride with practical activity yields at batch scale are the main limitations for the development of new ¹⁸F-PET tracers. Herein, we report a high-yielding and robust synthetic method to access naked dibenzothiophenium salt precursors of complex PET tracers and their labelling with [¹⁸F]fluoride. C-S cross-coupling of biphenyl-2-thioacetate with aryl halides followed by sequential oxidation-cyclisation of the corresponding thioethers gives dibenzothiophenium salts in good to excellent yields. Labelling of neutral and electron-deficient substrates with [¹⁸F]fluoride is ultrarapid and occurs under mild conditions (1 min at 90 °C) with high activity yields. The method enables facile synthesis of complex and sensitive radiotracers, as exemplified by radiofluorination of three clinically relevant PET tracers [¹⁸F]UCB-J, [¹⁸F]AldoView and [¹⁸F]FNDP, and can accelerate the development and clinical translation of new ¹⁸F-radiopharmaceuticals. Full article

(This article belongs to the Special Issue Novel PET Radiopharmaceuticals: Molecular Probes for Personalized Imaging)

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12 pages, 1399 KiB

Open AccessArticle

[⁶⁸Ga]Ga-DATA^5m-LM4, a PET Radiotracer in the Diagnosis of SST₂R-Positive Tumors: Preclinical and First Clinical Results

by Panagiotis Kanellopoulos, Berthold A. Nock, Lukas Greifenstein, Richard P. Baum, Frank Roesch and Theodosia Maina

Int. J. Mol. Sci. 2022, 23(23), 14590; https://doi.org/10.3390/ijms232314590 - 23 Nov 2022

Cited by 5 | Viewed by 2401

Abstract

Radiolabeled somatostatin subtype 2 receptor (SST2R)-antagonists have shown advantageous profiles for cancer theranostics compared with agonists. On the other hand, the newly introduced hybrid chelator (6-pentanoic acid)-6-(amino)methyl-1,4-diazepinetriacetate (DATA^5m) rapidly binds Ga-68 (t_1/2: 67.7 min) at much lower temperature, thus [...] Read more.

Radiolabeled somatostatin subtype 2 receptor (SST2R)-antagonists have shown advantageous profiles for cancer theranostics compared with agonists. On the other hand, the newly introduced hybrid chelator (6-pentanoic acid)-6-(amino)methyl-1,4-diazepinetriacetate (DATA^5m) rapidly binds Ga-68 (t_1/2: 67.7 min) at much lower temperature, thus allowing for quick access to “ready-for-injection” [⁶⁸Ga]Ga-tracers in hospitals. We herein introduce [⁶⁸Ga]Ga-DATA^5m-LM4 for PET/CT imaging of SST₂R-positive human tumors. LM4 was obtained by 4Pal³/Tyr³-substitution in the known SST₂R antagonist LM3 (H-DPhe-c[DCys-Tyr-DAph(Cbm)-Lys-Thr-Cys]-DTyr-NH₂) and DATA^5m was coupled at the N-terminus for labeling with radiogallium (Ga-67/68). [⁶⁷Ga]Ga-DATA^5m-LM4 was evaluated in HEK293-SST₂R cells and mice models in a head-to-head comparison with [⁶⁷Ga]Ga-DOTA-LM3. Clinical grade [⁶⁸Ga]Ga-DATA^5m-LM4 was prepared and injected in a neuroendocrine tumor (NET) patient for PET/CT imaging. DATA^5m-LM4 displayed high SST₂R binding affinity. [⁶⁷Ga]Ga-DATA^5m-LM4 showed markedly higher uptake in HEK293-SST₂R cells versus [⁶⁷Ga]Ga-DOTA-LM3 and was stable in vivo. In HEK293-SST₂R xenograft-bearing mice, it achieved longer tumor retention and less kidney uptake than [⁶⁷Ga]Ga-DOTA-LM3. [⁶⁸Ga]Ga-DATA^5m-LM4 accurately visualized tumor lesions with high contrast on PET/CT. In short, [⁶⁸Ga]Ga-DATA^5m-LM4 has shown excellent prospects for the PET/CT diagnosis of SST₂R-positive tumors, further highlighting the benefits of Ga-68 labeling in a hospital environment via the DATA^5m-chelator route. Full article

(This article belongs to the Special Issue Novel PET Radiopharmaceuticals: Molecular Probes for Personalized Imaging)

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9 pages, 3910 KiB

Open AccessArticle

¹⁸F-Fluoroethylcholine PET/CT Radiomic Analysis for Newly Diagnosed Prostate Cancer Patients: A Monocentric Study

by Daniele Antonio Pizzuto, Elizabeth Katherine Anna Triumbari, David Morland, Luca Boldrini, Roberto Gatta, Giorgio Treglia, Riccardo Bientinesi, Marco De Summa, Marina De Risi, Carmelo Caldarella, Eros Scarciglia, Angelo Totaro and Salvatore Annunziata

Int. J. Mol. Sci. 2022, 23(16), 9120; https://doi.org/10.3390/ijms23169120 - 14 Aug 2022

Cited by 4 | Viewed by 2367

Abstract

Aim: The aim of this study is to assess whether there are some correlations between radiomics and baseline clinical-biological data of prostate cancer (PC) patients using Fluorine-18 Fluoroethylcholine (¹⁸F-FECh) PET/CT. Methods: Digital rectal examination results (DRE), Prostate-Specific Antigen (PSA) serum levels, [...] Read more.

Aim: The aim of this study is to assess whether there are some correlations between radiomics and baseline clinical-biological data of prostate cancer (PC) patients using Fluorine-18 Fluoroethylcholine (¹⁸F-FECh) PET/CT. Methods: Digital rectal examination results (DRE), Prostate-Specific Antigen (PSA) serum levels, and bioptical-Gleason Score (GS) were retrospectively collected in newly diagnosed PC patients and considered as outcomes of PC. Thereafter, Volumes of interest (VOI) encompassing the prostate of each patient were drawn to extract conventional and radiomic PET features. Radiomic bivariate models were set up using the most statistically relevant features and then trained/tested with a cross-fold validation test. The best bivariate models were expressed by mean and standard deviation to the normal area under the receiver operating characteristic curves (mAUC, sdAUC). Results: Semiquantitative and radiomic analyses were performed on 67 consecutive patients. tSUVmean and tSkewness were significant DRE predictors at univariate analysis (OR 1.52 [1.01; 2.29], p = 0.047; OR 0.21 [0.07; 0.65], p = 0.007, respectively); moreover, tKurtosis was an independent DRE predictor at multivariate analysis (OR 0.64 [0.42; 0.96], p = 0.03) Among the most relevant bivariate models, szm_2.5D.z.entr + cm.clust.tend was a predictor of PSA levels (mAUC 0.83 ± 0.19); stat.kurt + stat.entropy predicted DRE (mAUC 0.79 ± 0.10); cm.info.corr.1 + szm_2.5D.szhge predicted GS (mAUC 0.78 ± 0.16). Conclusions: tSUVmean, tSkewness, and tKurtosis were predictors of DRE results only, while none of the PET parameters predicted PSA or GS significantly; ¹⁸F-FECh PET/CT radiomic models should be tested in larger cohort studies of newly diagnosed PC patients. Full article

(This article belongs to the Special Issue Novel PET Radiopharmaceuticals: Molecular Probes for Personalized Imaging)

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Review

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22 pages, 15758 KiB

Open AccessReview

Recent Advances of ⁶⁸Ga-Labeled PET Radiotracers with Nitroimidazole in the Diagnosis of Hypoxia Tumors

by Anh Thu Nguyen and Hee-Kwon Kim

Int. J. Mol. Sci. 2023, 24(13), 10552; https://doi.org/10.3390/ijms241310552 - 23 Jun 2023

Cited by 3 | Viewed by 1551

Abstract

Positron emission tomography (PET) is a noninvasive molecular imaging method extensively applied in the detection and treatment of various diseases. Hypoxia is a common phenomenon found in most solid tumors. Nitroimidazole is a group of bioreducible pharmacophores that selectively accumulate in hypoxic regions [...] Read more.

Positron emission tomography (PET) is a noninvasive molecular imaging method extensively applied in the detection and treatment of various diseases. Hypoxia is a common phenomenon found in most solid tumors. Nitroimidazole is a group of bioreducible pharmacophores that selectively accumulate in hypoxic regions of the body. Over the past few decades, many scientists have reported the use of radiopharmaceuticals containing nitroimidazole for the detection of hypoxic tumors. Gallium-68, a positron-emitting radioisotope, has a favorable half-life time of 68 min and can be conveniently produced by ⁶⁸Ge/⁶⁸Ga generators. Recently, there has been significant progress in the preparation of novel ⁶⁸Ga-labeled complexes bearing nitroimidazole moieties for the diagnosis of hypoxia. This review provides a comprehensive overview of the current status of developing ⁶⁸Ga-labeled radiopharmaceuticals with nitroimidazole moieties, their pharmacokinetics, and in vitro and in vivo studies, as well as PET imaging studies for hypoxic tumors. Full article

(This article belongs to the Special Issue Novel PET Radiopharmaceuticals: Molecular Probes for Personalized Imaging)

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19 pages, 5121 KiB

Open AccessReview

Diagnostic Performance of Positron Emission Tomography with Fibroblast-Activating Protein Inhibitors in Gastric Cancer: A Systematic Review and Meta-Analysis

by Alessio Rizzo, Manuela Racca, Federico Garrou, Elisabetta Fenocchio, Luca Pellegrino, Domenico Albano, Francesco Dondi, Francesco Bertagna, Salvatore Annunziata and Giorgio Treglia

Int. J. Mol. Sci. 2023, 24(12), 10136; https://doi.org/10.3390/ijms241210136 - 14 Jun 2023

Cited by 10 | Viewed by 2388

Abstract

Various papers have introduced the use of positron emission tomography (PET) with [⁶⁸Ga]Ga-radiolabeled fibroblast-activation protein inhibitor (FAPi) radiopharmaceuticals in different subtypes of gastric cancer (GC). Our aim was to assess the diagnostic performance of this novel molecular imaging technique in GC [...] Read more.

Various papers have introduced the use of positron emission tomography (PET) with [⁶⁸Ga]Ga-radiolabeled fibroblast-activation protein inhibitor (FAPi) radiopharmaceuticals in different subtypes of gastric cancer (GC). Our aim was to assess the diagnostic performance of this novel molecular imaging technique in GC with a systematic review and meta-analysis. A straightforward literature search of papers concerning the diagnostic performance of FAP-targeted PET imaging was performed. Original articles evaluating this novel molecular imaging examination in both newly diagnosed GC patients and GC patients with disease relapse were included. The systematic review included nine original studies, and eight of them were also eligible for meta-analysis. The quantitative synthesis provided pooled detection rates of 95% and 97% for the assessment of primary tumor and distant metastases, respectively, and a pooled sensitivity and specificity of 74% and 89%, respectively, for regional lymph node metastases. Significant statistical heterogeneity among the included studies was found only in the analysis of the primary tumor detection rate (I² = 64%). Conclusions: Beyond the limitations of this systematic review and meta-analysis (i.e., all the included studies were conducted in Asia, and using [¹⁸F]FDG PET/CT as a comparator of the index test), the quantitative data provided demonstrate the promising diagnostic performance of FAP-targeted PET imaging in GC. Nevertheless, more prospective multicentric studies are needed to confirm the excellent performances of FAP-targeted PET in this cluster of patients. Full article

(This article belongs to the Special Issue Novel PET Radiopharmaceuticals: Molecular Probes for Personalized Imaging)

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20 pages, 410 KiB

Open AccessReview

A Comparison of PET Tracers in Recurrent High-Grade Gliomas: A Systematic Review

by Sankar Muthukumar, Jordan Darden, James Crowley, Mark Witcher and Jackson Kiser

Int. J. Mol. Sci. 2023, 24(1), 408; https://doi.org/10.3390/ijms24010408 - 27 Dec 2022

Cited by 3 | Viewed by 2478

Abstract

Humans with high-grade gliomas have a poor prognosis, with a mean survival time of just 12–18 months for patients who undergo standard-of-care tumor resection and adjuvant therapy. Currently, surgery and chemoradiotherapy serve as standard treatments for this condition, yet these can be complicated [...] Read more.

Humans with high-grade gliomas have a poor prognosis, with a mean survival time of just 12–18 months for patients who undergo standard-of-care tumor resection and adjuvant therapy. Currently, surgery and chemoradiotherapy serve as standard treatments for this condition, yet these can be complicated by the tumor location, growth rate and recurrence. Currently, gadolinium-based, contrast-enhanced magnetic resonance imaging (CE-MRI) serves as the predominant imaging modality for recurrent high-grade gliomas, but it faces several drawbacks, including its inability to distinguish tumor recurrence from treatment-related changes and its failure to reveal the entirety of tumor burden (de novo or recurrent) due to limitations inherent to gadolinium contrast. As such, alternative imaging modalities that can address these limitations, including positron emission tomography (PET), are worth pursuing. To this end, the identification of PET-based markers for use in imaging of recurrent high-grade gliomas is paramount. This review will highlight several PET radiotracers that have been implemented in clinical practice and provide a comparison between them to assess the efficacy of these tracers. Full article

(This article belongs to the Special Issue Novel PET Radiopharmaceuticals: Molecular Probes for Personalized Imaging)

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31 pages, 2259 KiB

Open AccessReview

Recent Advances in Cardiovascular Diseases Research Using Animal Models and PET Radioisotope Tracers

by Weronika Wargocka-Matuszewska, Witold Uhrynowski, Natalia Rozwadowska and Zbigniew Rogulski

Int. J. Mol. Sci. 2023, 24(1), 353; https://doi.org/10.3390/ijms24010353 - 26 Dec 2022

Cited by 3 | Viewed by 3560

Abstract

Cardiovascular diseases (CVD) is a collective term describing a range of conditions that affect the heart and blood vessels. Due to the varied nature of the disorders, distinguishing between their causes and monitoring their progress is crucial for finding an effective treatment. Molecular [...] Read more.

Cardiovascular diseases (CVD) is a collective term describing a range of conditions that affect the heart and blood vessels. Due to the varied nature of the disorders, distinguishing between their causes and monitoring their progress is crucial for finding an effective treatment. Molecular imaging enables non-invasive visualisation and quantification of biological pathways, even at the molecular and subcellular levels, what is essential for understanding the causes and development of CVD. Positron emission tomography imaging is so far recognized as the best method for in vivo studies of the CVD related phenomena. The imaging is based on the use of radioisotope-labelled markers, which have been successfully used in both pre-clinical research and clinical studies. Current research on CVD with the use of such radioconjugates constantly increases our knowledge and understanding of the causes, and brings us closer to effective monitoring and treatment. This review outlines recent advances in the use of the so-far available radioisotope markers in the research on cardiovascular diseases in rodent models, points out the problems and provides a perspective for future applications of PET imaging in CVD studies. Full article

(This article belongs to the Special Issue Novel PET Radiopharmaceuticals: Molecular Probes for Personalized Imaging)

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41 pages, 8621 KiB

Open AccessReview

Synthesis of Radioiodinated Compounds. Classical Approaches and Achievements of Recent Years

by Stanislav A. Petrov, Mekhman S. Yusubov, Elena K. Beloglazkina and Valentine G. Nenajdenko

Int. J. Mol. Sci. 2022, 23(22), 13789; https://doi.org/10.3390/ijms232213789 - 9 Nov 2022

Cited by 22 | Viewed by 3732

Abstract

This review demonstrates the progress in the synthesis of radioiodinated compounds over the past decade. The possibilities and limitations of radiopharmaceuticals with different iodine isotopes, as well as the synthesis of low and high molecular weight compounds containing radioiodine, are discussed. An analysis [...] Read more.

This review demonstrates the progress in the synthesis of radioiodinated compounds over the past decade. The possibilities and limitations of radiopharmaceuticals with different iodine isotopes, as well as the synthesis of low and high molecular weight compounds containing radioiodine, are discussed. An analysis of synthesis strategies, substrate frameworks, isolation methods, and metabolic stability, and the possibility of industrial production of radioiodinated organic derivatives which can find applications in the synthesis of drugs and diagnostics are presented. Full article

(This article belongs to the Special Issue Novel PET Radiopharmaceuticals: Molecular Probes for Personalized Imaging)

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