Discrete Hf18 Metal‐oxo Cluster as a Heterogeneous Nanozyme for Site‐Specific Proteolysis
Само за регистроване кориснике
2020
Аутори
Moons, Jensde Azambuja, Francisco
Mihailović, Jelena
Kozma, Karoly
Smiljanić, Katarina
Amiri, Mehran
Ćirković-Veličković, Tanja
Nyman, May
Parac-Vogt, Tatjana
Чланак у часопису (Објављена верзија)
Метаподаци
Приказ свих података о документуАпстракт
The selective hydrolysis of proteins by non‐enzymatic catalysis is difficult to achieve, yet it is crucial for applications in biotechnology and proteomics. Herein, we report that discrete hafnium metal‐oxo cluster [Hf18O10(OH)26(SO4)13⋅(H2O)33] (Hf18), which is centred by the same hexamer motif found in many MOFs, acts as a heterogeneous catalyst for the efficient hydrolysis of horse heart myoglobin (HHM) in low buffer concentrations. Among 154 amino acids present in the sequence of HHM, strictly selective cleavage at only 6 solvent accessible aspartate residues was observed. Mechanistic experiments suggest that the hydrolytic activity is likely derived from the actuation of HfIV Lewis acidic sites and the Brønsted acidic surface of Hf18. X‐ray scattering and ESI‐MS revealed that Hf18 is completely insoluble in these conditions, confirming the HHM hydrolysis is caused by a heterogeneous reaction of the solid Hf18 cluster, and not from smaller, soluble Hf species that could leach into ...solution.
Кључне речи:
amino-acid-selective cleavage / artificial proteases / heterogeneous catalysis / metal-oxo clusters / protein hydrolysisИзвор:
Angewandte Chemie (International Edition), 2020, 59, 17, 1-9Издавач:
- Wiley
Финансирање / пројекти:
- Молекуларне особине и модификације неких респираторних и нутритивних алергена (RS-172024)
- Serbian Academy of Sciences and Arts GA No. F-26.
- FoodEnTwin-Twinning of research activities for the frontier research in the fields of food, nutrition and environmental omics (EU-810752)
- U.S. Department of Energy, Office of Basic Energy Sciences, Division of Material Sciences and Engineering, under award DE SC0010802.
Напомена:
- Peer-reviewed manuscript: https://cherry.chem.bg.ac.rs/handle/123456789/4850
- Supplementary material: https://cherry.chem.bg.ac.rs/handle/123456789/4851
Повезане информације:
DOI: 10.1002/anie.202001036
ISSN: 1433-7851
WoS: 000522270200001
Scopus: 2-s2.0-85082965044
Колекције
Институција/група
Hemijski fakultet / Faculty of ChemistryTY - JOUR AU - Moons, Jens AU - de Azambuja, Francisco AU - Mihailović, Jelena AU - Kozma, Karoly AU - Smiljanić, Katarina AU - Amiri, Mehran AU - Ćirković-Veličković, Tanja AU - Nyman, May AU - Parac-Vogt, Tatjana PY - 2020 UR - https://cherry.chem.bg.ac.rs/handle/123456789/3917 AB - The selective hydrolysis of proteins by non‐enzymatic catalysis is difficult to achieve, yet it is crucial for applications in biotechnology and proteomics. Herein, we report that discrete hafnium metal‐oxo cluster [Hf18O10(OH)26(SO4)13⋅(H2O)33] (Hf18), which is centred by the same hexamer motif found in many MOFs, acts as a heterogeneous catalyst for the efficient hydrolysis of horse heart myoglobin (HHM) in low buffer concentrations. Among 154 amino acids present in the sequence of HHM, strictly selective cleavage at only 6 solvent accessible aspartate residues was observed. Mechanistic experiments suggest that the hydrolytic activity is likely derived from the actuation of HfIV Lewis acidic sites and the Brønsted acidic surface of Hf18. X‐ray scattering and ESI‐MS revealed that Hf18 is completely insoluble in these conditions, confirming the HHM hydrolysis is caused by a heterogeneous reaction of the solid Hf18 cluster, and not from smaller, soluble Hf species that could leach into solution. PB - Wiley T2 - Angewandte Chemie (International Edition) T1 - Discrete Hf18 Metal‐oxo Cluster as a Heterogeneous Nanozyme for Site‐Specific Proteolysis VL - 59 IS - 17 SP - 1 EP - 9 DO - 10.1002/anie.202001036 ER -
@article{ author = "Moons, Jens and de Azambuja, Francisco and Mihailović, Jelena and Kozma, Karoly and Smiljanić, Katarina and Amiri, Mehran and Ćirković-Veličković, Tanja and Nyman, May and Parac-Vogt, Tatjana", year = "2020", abstract = "The selective hydrolysis of proteins by non‐enzymatic catalysis is difficult to achieve, yet it is crucial for applications in biotechnology and proteomics. Herein, we report that discrete hafnium metal‐oxo cluster [Hf18O10(OH)26(SO4)13⋅(H2O)33] (Hf18), which is centred by the same hexamer motif found in many MOFs, acts as a heterogeneous catalyst for the efficient hydrolysis of horse heart myoglobin (HHM) in low buffer concentrations. Among 154 amino acids present in the sequence of HHM, strictly selective cleavage at only 6 solvent accessible aspartate residues was observed. Mechanistic experiments suggest that the hydrolytic activity is likely derived from the actuation of HfIV Lewis acidic sites and the Brønsted acidic surface of Hf18. X‐ray scattering and ESI‐MS revealed that Hf18 is completely insoluble in these conditions, confirming the HHM hydrolysis is caused by a heterogeneous reaction of the solid Hf18 cluster, and not from smaller, soluble Hf species that could leach into solution.", publisher = "Wiley", journal = "Angewandte Chemie (International Edition)", title = "Discrete Hf18 Metal‐oxo Cluster as a Heterogeneous Nanozyme for Site‐Specific Proteolysis", volume = "59", number = "17", pages = "1-9", doi = "10.1002/anie.202001036" }
Moons, J., de Azambuja, F., Mihailović, J., Kozma, K., Smiljanić, K., Amiri, M., Ćirković-Veličković, T., Nyman, M.,& Parac-Vogt, T.. (2020). Discrete Hf18 Metal‐oxo Cluster as a Heterogeneous Nanozyme for Site‐Specific Proteolysis. in Angewandte Chemie (International Edition) Wiley., 59(17), 1-9. https://doi.org/10.1002/anie.202001036
Moons J, de Azambuja F, Mihailović J, Kozma K, Smiljanić K, Amiri M, Ćirković-Veličković T, Nyman M, Parac-Vogt T. Discrete Hf18 Metal‐oxo Cluster as a Heterogeneous Nanozyme for Site‐Specific Proteolysis. in Angewandte Chemie (International Edition). 2020;59(17):1-9. doi:10.1002/anie.202001036 .
Moons, Jens, de Azambuja, Francisco, Mihailović, Jelena, Kozma, Karoly, Smiljanić, Katarina, Amiri, Mehran, Ćirković-Veličković, Tanja, Nyman, May, Parac-Vogt, Tatjana, "Discrete Hf18 Metal‐oxo Cluster as a Heterogeneous Nanozyme for Site‐Specific Proteolysis" in Angewandte Chemie (International Edition), 59, no. 17 (2020):1-9, https://doi.org/10.1002/anie.202001036 . .