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Therapeutic Radionuclides in Nuclear Medicine

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A special issue of Pharmaceuticals (ISSN 1424-8247). This special issue belongs to the section "Radiopharmaceutical Sciences".

Deadline for manuscript submissions: closed (31 January 2024) | Viewed by 14847

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Dr. Marc Pretze

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Guest Editor

1 Department of Nuclear Medicine, University Hospital Carl Gustav Carus, Technical University Dresden, 01307 Dresden, Germany
2 Molecular Imaging and Radiochemistry, Department of Radiology and Nuclear Medicine, Medical Faculty Mannheim, Heidelberg University, 68167 Mannheim, Germany
Interests: radiolabelling; quality control; imaging; therapy; automation; clinical translation

Prof. Dr. Jörg Kotzerke

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Guest Editor

1 Department of Nuclear Medicine, University Hospital Carl Gustav Carus, Technical University Dresden, 01307 Dresden, Germany
2 Helmholtz-Zentrum Dresden-Rossendorf, PET Center, Institute of Radiopharmaceutical Cancer Research, 01328 Dresden, Germany
Interests: radiolabelling; quality control; imaging; therapy; automation; clinical translation

Special Issue Information

Dear Colleagues,

Sodium iodide is the first example of a theranostic radiopharmaceutical wherein diagnostic (¹²³I, ¹²⁴I) and therapeutic (¹³¹I) radionuclides are used, respectively for diagnostic imaging and subsequent radiotherapy. It has been in clinical application since the 1940s and received the first FDA approval for the use of radioactive material for cancer treatment. The visualization of regional distribution in the context of pretherapeutic dosimetry and post therapeutic biodistribution is a prerequisite for robust methodology and broad clinical use.

Recently, the theranostic principle has been used with tumor receptor-specific radiopharmaceuticals containing therapeutic nuclides, such as ¹⁶¹Tb, ¹⁷⁷Lu, ¹⁸⁸Re, ²¹²Pb, ²²⁵Ac. The production mode, availability, and costs of radionuclides have a significant impact on their clinical use and is often a bottleneck for broad application. Therefore, cyclotron-produced neutrons could open a new era for producing relevant radionuclides.

Identification of tumor-specific binding sites, development of tumor-addressing conjugates, and opportunities for enhanced target enrichment and the protection of critical organs define the potential of therapeutic radiopharmaceuticals. The combination of radiotherapeutics with other pharmaceuticals to modulate the target or repair systems exploits synergistic effects. Combining radiotherapeutics with the body's immune system or immunotherapeutics raises hopes for immunization against cancer and could explain the success of targeted alpha therapy vs. targeted beta therapy. The value of diverse radiation qualities including options such as photodynamic therapy using Cherenkov light must be systematically investigated in vitro and in preclinical models before they can be used in clinical trials and patient care.

The path from radioisotope to targeted radionuclide therapy encompasses a multitude of aspects like availability, costs, dosimetry, waste management, which will be highlighted in this issue.

Dr. Marc Pretze
Prof. Dr. Jörg Kotzerke
Guest Editors

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Keywords

targeted Alpha therapy (TαT)
targeted Beta therapy (TβT)
Thorium-229
Actinium-225
Lead-212
Terbium-161
radio immune response
cherenkov
nanoparticle
Dosimetry
Waste management

Published Papers (11 papers)

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Research

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12 pages, 1072 KiB

Open AccessArticle

Safety and Efficacy of Selective Internal Radionuclide Therapy with ⁹⁰Y Glass Microspheres in Patients with Progressive Hepatocellular Carcinoma after the Failure of Repeated Transarterial Chemoembolization

by Alexander Bellendorf, Nicolai Mader, Stefan P. Mueller, Samer Ezziddin, Andreas Bockisch, Hong Grafe, Jan Best, Juliane Goebel, Thorsten D. Pöppel and Amir Sabet

Pharmaceuticals 2024, 17(1), 101; https://doi.org/10.3390/ph17010101 - 11 Jan 2024

Viewed by 833

Abstract

Transarterial chemoembolization (TACE) is currently the standard of care in patients with unresectable hepatocellular carcinoma (HCC), and selective internal radionuclide therapy (SIRT) with ⁹⁰Y microspheres is mainly used as an alternative modality in patients considered poor candidates for TACE. Treatment with sorafenib is the recommended option for patients with progressive disease after TACE. This study aims to evaluate the safety and efficacy of SIRT with glass microspheres in patients with progressive HCC after repeated TACE who are not eligible for treatment with sorafenib. Forty-seven patients with progressive HCC after a median of three TACE sessions (range 2–14) underwent SIRT (3.5 ± 1.5 GBq; liver target dose 110–120 Gy). Toxicity was recorded 4 and 12 weeks after treatment and reported according to the Common Terminology Criteria for Adverse Events Version 5.0. Treatment response was assessed three months after SIRT using multiphase computed tomography and modified criteria in solid tumors (mRECIST). Survival analyses were performed using Kaplan–Meier curves and a Cox proportional hazards model for uni- and multivariate analyses. Significant but reversible hepatotoxicity (≥grade 3) occurred in five patients (11%). No radioembolization-induced liver disease (REILD) was observed. The number of previous TACE sessions and cumulative administered activity did not predict the incidence of post-SIRT significant hepatotoxicity. Treatment responses consisted of partial responses in 26 (55%), stable disease in 12 (26%), and progressive disease in 9 (19%) patients. The median overall survival (OS) was 11 months (95% confidence interval (CI), 9–13), and objective responses to SIRT were associated with a longer OS (p = 0.008). Significant hepatotoxicity (≥grade 3) after SIRT was a contributor to impaired survival (median OS 6 months (95% CI, 4–8) vs. 12 months (95% CI, 10–14), p < 0.001). SIRT with glass microspheres is a safe and effective salvage treatment for patients with progressive HCC refractory to TACE who are considered poor candidates for sorafenib treatment. Full article

(This article belongs to the Special Issue Therapeutic Radionuclides in Nuclear Medicine)

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12 pages, 1567 KiB

Open AccessArticle

Combining Cisplatin with Different Radiation Qualities—Interpretation of Cytotoxic Effects In Vitro by Isobolographic Analysis

by Roswitha Runge, Falco Reissig, Nora Herzog, Liane Oehme, Claudia Brogsitter and Joerg Kotzerke

Pharmaceuticals 2023, 16(12), 1720; https://doi.org/10.3390/ph16121720 - 12 Dec 2023

Viewed by 879

Abstract

Background: The combination of platinum-containing cytostatic drugs with different radiation qualities has been studied for years. Despite their massive side effects, these drugs still belong to the therapeutic portfolio in cancer treatment. To overcome the disadvantages of cisplatin, our study investigated the cytotoxic effects of combining radionuclides with cisplatin. Methods: FaDu cells were treated with cisplatin (concentration ≈ 2 µM) and additionally irradiated after two hours with the alpha-emitter ²²³Ra, the beta-emitter ¹⁸⁸Re as well as external X-rays using dose ranges of 2–6 Gy. Cell survival was followed by colony formation assays and plotted against cisplatin concentration and radiation dose. The results were interpreted by isobolograms. Results: Isobolographic analyses revealed a supra-additive cytotoxic effect for the combination of cisplatin and ²²³Ra. A sub-additive effect was observed for the combination of cisplatin and ¹⁸⁸Re, whereas a protective effect was found for the combination with X-rays. Conclusions: The combination of cisplatin and ²²³Ra may have the potential to create a successfully working therapy scheme for various therapy approaches, whereas the combination with ¹⁸⁸Re as well as single-dose X-ray treatment did not lead to a detectable radiosensitizing effect. Thus, the combination with alpha-emitters might be advantageous and, therefore, should be followed in future studies when combined with cytostatic drugs. Full article

(This article belongs to the Special Issue Therapeutic Radionuclides in Nuclear Medicine)

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22 pages, 5540 KiB

Open AccessArticle

Radiosynthesis of Stable ¹⁹⁸Au-Nanoparticles by Neutron Activation of α_vβ₃-Specific AuNPs for Therapy of Tumor Angiogenesis

by Güllü Davarci, Carmen Wängler, Klaus Eberhardt, Christopher Geppert, Ralf Schirrmacher, Robert Freudenberg, Marc Pretze and Björn Wängler

Pharmaceuticals 2023, 16(12), 1670; https://doi.org/10.3390/ph16121670 - 30 Nov 2023

Viewed by 938

Abstract

This paper reports on the development of stable tumor-specific gold nanoparticles (AuNPs) activated by neutron irradiation as a therapeutic option for the treatment of cancer with high tumor angiogenesis. The AuNPs were designed with different mono- or dithiol-ligands and decorated with different amounts of Arg-Gly-Asp (RGD) peptides as a tumor-targeting vector for α_vβ₃ integrin, which is overexpressed in tissues with high tumor angiogenesis. The AuNPs were evaluated for avidity in vitro and showed favorable properties with respect to tumor cell accumulation. Furthermore, the therapeutic properties of the [¹⁹⁸Au]AuNPs were evaluated in vitro on U87MG cells in terms of cell survival, suggesting that these [¹⁹⁸Au]AuNPs are a useful basis for future therapeutic concepts. Full article

(This article belongs to the Special Issue Therapeutic Radionuclides in Nuclear Medicine)

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11 pages, 2460 KiB

Open AccessArticle

Influence of the Molar Activity of ^203/212Pb-PSC-PEG₂-TOC on Somatostatin Receptor Type 2-Binding and Cell Uptake

by Marc Pretze, Enrico Michler, Roswitha Runge, Kerstin Wetzig, Katja Tietze, Florian Brandt, Michael K. Schultz and Jörg Kotzerke

Pharmaceuticals 2023, 16(11), 1605; https://doi.org/10.3390/ph16111605 - 14 Nov 2023

Cited by 1 | Viewed by 793

Abstract

(1) Background: In neuroendocrine tumors (NETs), somatostatin receptor subtype 2 is highly expressed, which can be targeted by a radioactive ligand such as [¹⁷⁷Lu]Lu-1,4,7,10-tetraazacyclododecane-N,N′,N″,N‴,-tetraacetic acid-[Tyr³,Thr⁸]-octreotide (¹⁷⁷Lu-DOTA-TOC) and, more recently, by a lead specific chelator (PSC) containing ^203/212Pb-PSC-PEG₂-TOC (PSC-TOC). The molar activity (A_M) can play a crucial role in tumor uptake, especially in receptor-mediated uptake, such as in NETs. Therefore, an investigation of the influence of different molar activities of ^203/212Pb-PSC-TOC on cell uptake was investigated. (2) Methods: Optimized radiolabeling of ^203/212Pb-PSC-TOC was performed with 50 µg of precursor in a NaAc/AcOH buffer at pH 5.3–5.5 within 15–45 min at 95° C. Cell uptake was studied in AR42 J, HEK293 sst2, and ZR75-1 cells. (3) Results: ^203/212Pb-PSC-TOC was radiolabeled with high radiochemical purity >95% and high radiochemical yield >95%, with A_M ranging from 0.2 to 61.6 MBq/nmol. The cell uptake of ²⁰³Pb-PSC-TOC (A_M = 38 MBq/nmol) was highest in AR42 J (17.9%), moderate in HEK293 sstr (9.1%) and lowest in ZR75-1 (0.6%). Cell uptake increased with the level of A_M. (4) Conclusions: A moderate A_M of 15–40 MBq/nmol showed the highest cell uptake. No uptake limitation was found in the first 24–48 h. Further escalation experiments with even higher A_M should be performed in the future. It was shown that A_M plays an important role because of its direct dependence on the cellular uptake levels, possibly due to less receptor saturation with non-radioactive ligands at higher A_M. Full article

(This article belongs to the Special Issue Therapeutic Radionuclides in Nuclear Medicine)

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15 pages, 2197 KiB

Open AccessArticle

The Importance of Uncertainty Analysis and Traceable Measurements in Routine Quantitative ⁹⁰Y-PET Molecular Radiotherapy: A Multicenter Experience

by Marco D’Arienzo, Emilio Mezzenga, Amedeo Capotosti, Oreste Bagni, Luca Filippi, Marco Capogni, Luca Indovina and Anna Sarnelli

Pharmaceuticals 2023, 16(8), 1142; https://doi.org/10.3390/ph16081142 - 11 Aug 2023

Viewed by 1135

Abstract

Molecular Radiation Therapy (MRT) is a valid therapeutic option for a wide range of malignancies, such as neuroendocrine tumors and liver cancers. In its practice, it is generally acknowledged that there is a need to evaluate the influence of different factors affecting the accuracy of dose estimates and to define the actions necessary to maintain treatment uncertainties at acceptable levels. The present study addresses the problem of uncertainty propagation in ⁹⁰Y-PET quantification. We assessed the quantitative accuracy in reference conditions of three PET scanners (namely, Siemens Biograph mCT, Siemens Biograph mCT flow, and GE Discovery DST) available at three different Italian Nuclear Medicine centers. Specific aspects of uncertainty within the quantification chain have been addressed, including the uncertainty in the calibration procedure. A framework based on the Guide to the Expression of Uncertainty in Measurement (GUM) approach is proposed for modeling the uncertainty in the quantification processes, and ultimately, an estimation of the uncertainty achievable in clinical conditions is reported. Full article

(This article belongs to the Special Issue Therapeutic Radionuclides in Nuclear Medicine)

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12 pages, 3934 KiB

Open AccessArticle

Image-Based Dosimetry in Dogs and Cross-Reactivity with Human Tissues of IGF2R-Targeting Human Antibody

by Kevin J. H. Allen, Ohyun Kwon, Matthew R. Hutcheson, Joseph J. Grudzinski, Stuart M. Cain, Frederic A. Cruz, Remitha M. Vinayakamoorthy, Ying S. Sun, Lindsay Fairley, Chandra B. Prabaharan, Ryan Dickinson, Valerie MacDonald-Dickinson, Maruti Uppalapati, Bryan P. Bednarz and Ekaterina Dadachova

Pharmaceuticals 2023, 16(7), 979; https://doi.org/10.3390/ph16070979 - 08 Jul 2023

Cited by 2 | Viewed by 1231

Abstract

Background: Osteosarcoma (OS) represents the most common primary bone tumor in humans and in companion dogs, being practically phenotypically identical. There is a need for effective treatments to extend the survival of patients with OS. Here, we examine the dosimetry in beagle dogs and cross-reactivity with human tissues of a novel human antibody, IF3, that targets the insulin growth factor receptor type 2 (IGF2R), which is overexpressed on OS cells, making it a candidate for radioimmunotherapy of OS. Methods: [⁸⁹Zr]Zr-DFO-IF3 was injected into three healthy beagle dogs. PET/CT was conducted at 4, 24, 48, and 72 h. RAPID analysis was used to determine the dosimetry of [¹⁷⁷Lu]Lu-CHXA”-IF3 for a clinical trial in companion dogs with OS. IF3 antibody was biotinylated, and a multitude of human tissues were assessed with immunohistochemistry. Results: PET/CT revealed that only the liver, bone marrow, and adrenal glands had high uptake. Clearance was initially through renal and hepatobiliary excretion in the first 72 h followed by primarily physical decay. RAPID analysis showed bone marrow to be the dose-limiting organ with a therapeutic range for ¹⁷⁷Lu calculated to be 0.487–0.583 GBq. Immunohistochemistry demonstrated the absence of IGF2R expression on the surface of healthy human cells, thus suggesting that radioimmunotherapy with [¹⁷⁷Lu]Lu-CHXA”-IF3 will be well tolerated. Conclusions: Image-based dosimetry has defined a safe therapeutic range for canine clinical trials, while immunohistochemistry has suggested that the antibody will not cross-react with healthy human tissues. Full article

(This article belongs to the Special Issue Therapeutic Radionuclides in Nuclear Medicine)

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Review

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26 pages, 2598 KiB

Open AccessReview

Towards Effective Targeted Alpha Therapy for Neuroendocrine Tumours: A Review

by Paul M. D. Gape, Michael K. Schultz, Graeme J. Stasiuk and Samantha Y. A. Terry

Pharmaceuticals 2024, 17(3), 334; https://doi.org/10.3390/ph17030334 - 04 Mar 2024

Viewed by 1461

Abstract

This review article explores the evolving landscape of Molecular Radiotherapy (MRT), emphasizing Peptide Receptor Radionuclide Therapy (PRRT) for neuroendocrine tumours (NETs). The primary focus is on the transition from β-emitting radiopharmaceuticals to α-emitting agents in PRRT, offering a critical analysis of the radiobiological basis, clinical applications, and ongoing developments in Targeted Alpha Therapy (TAT). Through an extensive literature review, the article delves into the mechanisms and effectiveness of PRRT in targeting somatostatin subtype 2 receptors, highlighting both its successes and limitations. The discussion extends to the emerging paradigm of TAT, underlining its higher potency and specificity with α-particle emissions, which promise enhanced therapeutic efficacy and reduced toxicity. The review critically evaluates preclinical and clinical data, emphasizing the need for standardised dosimetry and a deeper understanding of the dose-response relationship in TAT. The review concludes by underscoring the significant potential of TAT in treating SSTR2-overexpressing cancers, especially in patients refractory to β-PRRT, while also acknowledging the current challenges and the necessity for further research to optimize treatment protocols. Full article

(This article belongs to the Special Issue Therapeutic Radionuclides in Nuclear Medicine)

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20 pages, 2930 KiB

Open AccessReview

Alpha-Emitting Radionuclides: Current Status and Future Perspectives

by Matthias Miederer, Martina Benešová-Schäfer, Constantin Mamat, David Kästner, Marc Pretze, Enrico Michler, Claudia Brogsitter, Jörg Kotzerke, Klaus Kopka, David A. Scheinberg and Michael R. McDevitt

Pharmaceuticals 2024, 17(1), 76; https://doi.org/10.3390/ph17010076 - 08 Jan 2024

Cited by 1 | Viewed by 2208

Abstract

The use of radionuclides for targeted endoradiotherapy is a rapidly growing field in oncology. In particular, the focus on the biological effects of different radiation qualities is an important factor in understanding and implementing new therapies. Together with the combined approach of imaging and therapy, therapeutic nuclear medicine has recently made great progress. A particular area of research is the use of alpha-emitting radionuclides, which have unique physical properties associated with outstanding advantages, e.g., for single tumor cell targeting. Here, recent results and open questions regarding the production of alpha-emitting isotopes as well as their chemical combination with carrier molecules and clinical experience from compassionate use reports and clinical trials are discussed. Full article

(This article belongs to the Special Issue Therapeutic Radionuclides in Nuclear Medicine)

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9 pages, 1764 KiB

Open AccessReview

Radiopharmaceuticals for Treatment of Adrenocortical Carcinoma

by Kerstin Michalski, Wiebke Schlötelburg, Philipp E. Hartrampf, Aleksander Kosmala, Andreas K. Buck, Stefanie Hahner and Andreas Schirbel

Pharmaceuticals 2024, 17(1), 25; https://doi.org/10.3390/ph17010025 - 23 Dec 2023

Viewed by 860

Abstract

Adrenocortical carcinoma (ACC) represents a rare tumor entity with limited treatment options and usually rapid tumor progression in case of metastatic disease. As further treatment options are needed and ACC metastases are sensitive to external beam radiation, novel theranostic approaches could complement established therapeutic concepts. Recent developments focus on targeting adrenal cortex-specific enzymes like the theranostic twin [^123/131I]IMAZA that shows a good image quality and a promising therapeutic effect in selected patients. But other established molecular targets in nuclear medicine such as the C-X-C motif chemokine receptor 4 (CXCR4) could possibly enhance the therapeutic regimen as well in a subgroup of patients. The aims of this review are to give an overview of innovative radiopharmaceuticals for the treatment of ACC and to present the different molecular targets, as well as to show future perspectives for further developments since a radiopharmaceutical with a broad application range is still warranted. Full article

(This article belongs to the Special Issue Therapeutic Radionuclides in Nuclear Medicine)

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0 pages, 1300 KiB

Open AccessReview

Targeted Alpha Therapy: All We Need to Know about ²²⁵Ac’s Physical Characteristics and Production as a Potential Theranostic Radionuclide

by Wael Jalloul, Vlad Ghizdovat, Cati Raluca Stolniceanu, Teodor Ionescu, Irena Cristina Grierosu, Ioana Pavaleanu, Mihaela Moscalu and Cipriana Stefanescu

Pharmaceuticals 2023, 16(12), 1679; https://doi.org/10.3390/ph16121679 - 02 Dec 2023

Cited by 2 | Viewed by 2227

Abstract

The high energy of α emitters, and the strong linear energy transfer that goes along with it, lead to very efficient cell killing through DNA damage. Moreover, the degree of oxygenation and the cell cycle state have no impact on these effects. Therefore, α radioisotopes can offer a treatment choice to individuals who are not responding to β− or gamma-radiation therapy or chemotherapy drugs. Only a few α-particle emitters are suitable for targeted alpha therapy (TAT) and clinical applications. The majority of available clinical research involves ²²⁵Ac and its daughter nuclide ²¹³Bi. Additionally, the ²²⁵Ac disintegration cascade generates γ decays that can be used in single-photon emission computed tomography (SPECT) imaging, expanding the potential theranostic applications in nuclear medicine. Despite the growing interest in applying ²²⁵Ac, the restricted global accessibility of this radioisotope makes it difficult to conduct extensive clinical trials for many radiopharmaceutical candidates. To boost the availability of ²²⁵Ac, along with its clinical and potential theranostic applications, this review attempts to highlight the fundamental physical properties of this α-particle-emitting isotope, as well as its existing and possible production methods. Full article

(This article belongs to the Special Issue Therapeutic Radionuclides in Nuclear Medicine)

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20 pages, 4305 KiB

Open AccessReview

Theranostic Imaging Surrogates for Targeted Alpha Therapy: Progress in Production, Purification, and Applications

by Bryce J. B. Nelson, John Wilson, Jan D. Andersson and Frank Wuest

Pharmaceuticals 2023, 16(11), 1622; https://doi.org/10.3390/ph16111622 - 17 Nov 2023

Cited by 2 | Viewed by 1311

Abstract

This article highlights recent developments of SPECT and PET diagnostic imaging surrogates for targeted alpha particle therapy (TAT) radiopharmaceuticals. It outlines the rationale for using imaging surrogates to improve diagnostic-scan accuracy and facilitate research, and the properties an imaging-surrogate candidate should possess. It evaluates the strengths and limitations of each potential imaging surrogate. Thirteen surrogates for TAT are explored: ¹³³La, ¹³²La, ¹³⁴Ce/¹³⁴La, and ²²⁶Ac for ²²⁵Ac TAT; ²⁰³Pb for ²¹²Pb TAT; ¹³¹Ba for ²²³Ra and ²²⁴Ra TAT; ¹²³I, ¹²⁴I, ¹³¹I and ²⁰⁹At for ²¹¹At TAT; ¹³⁴Ce/¹³⁴La for ²²⁷Th TAT; and ¹⁵⁵Tb and ¹⁵²Tb for ¹⁴⁹Tb TAT. Full article

(This article belongs to the Special Issue Therapeutic Radionuclides in Nuclear Medicine)

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