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      Photocatalytic manipulation of Ca 2+ signaling for regulating cellular and animal behaviors via MOF-enabled H 2O 2 generation

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          Abstract

          The in situ generation of H 2O 2 in cells in response to external stimulation has exceptional advantages in modulating intracellular Ca 2+ dynamics, including high controllability and biological safety, but has been rarely explored. Here, we develop photocatalyst-based metal-organic frameworks (DCSA-MOFs) to modulate Ca 2+ responses in cells, multicellular spheroids, and organs. By virtue of the efficient photocatalytic oxygen reduction to H 2O 2 without sacrificial agents, photoexcited DCSA-MOFs can rapidly trigger Ca 2+ outflow from the endoplasmic reticulum with single-cell precision in a repeatable and controllable manner, enabling the propagation of intercellular Ca 2+ waves (ICW) over long distances in two-dimensional and three-dimensional cell cultures. After photoexcitation, ICWs induced by DCSA-MOFs can activate neural activities in the optical tectum of tadpoles and thighs of spinal frogs, eliciting the corresponding motor behaviors. Our study offers a versatile optical nongenetic modulation technique that enables remote, repeatable, and controlled manipulation of cellular and animal behaviors.

          Abstract

          Photocatalytic generation of H 2O 2 could efficiently control cellular Ca 2+ response and animal behaviors.

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          Most cited references85

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          A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu.

          Stefan Grimme, Jens Antony, Stephan Ehrlich … (2010)
          The method of dispersion correction as an add-on to standard Kohn-Sham density functional theory (DFT-D) has been refined regarding higher accuracy, broader range of applicability, and less empiricism. The main new ingredients are atom-pairwise specific dispersion coefficients and cutoff radii that are both computed from first principles. The coefficients for new eighth-order dispersion terms are computed using established recursion relations. System (geometry) dependent information is used for the first time in a DFT-D type approach by employing the new concept of fractional coordination numbers (CN). They are used to interpolate between dispersion coefficients of atoms in different chemical environments. The method only requires adjustment of two global parameters for each density functional, is asymptotically exact for a gas of weakly interacting neutral atoms, and easily allows the computation of atomic forces. Three-body nonadditivity terms are considered. The method has been assessed on standard benchmark sets for inter- and intramolecular noncovalent interactions with a particular emphasis on a consistent description of light and heavy element systems. The mean absolute deviations for the S22 benchmark set of noncovalent interactions for 11 standard density functionals decrease by 15%-40% compared to the previous (already accurate) DFT-D version. Spectacular improvements are found for a tripeptide-folding model and all tested metallic systems. The rectification of the long-range behavior and the use of more accurate C(6) coefficients also lead to a much better description of large (infinite) systems as shown for graphene sheets and the adsorption of benzene on an Ag(111) surface. For graphene it is found that the inclusion of three-body terms substantially (by about 10%) weakens the interlayer binding. We propose the revised DFT-D method as a general tool for the computation of the dispersion energy in molecules and solids of any kind with DFT and related (low-cost) electronic structure methods for large systems.
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            Balanced basis sets of split valence, triple zeta valence and quadruple zeta valence quality for H to Rn: Design and assessment of accuracy.

            Florian Weigend, Reinhart Ahlrichs (2005)
            Gaussian basis sets of quadruple zeta valence quality for Rb-Rn are presented, as well as bases of split valence and triple zeta valence quality for H-Rn. The latter were obtained by (partly) modifying bases developed previously. A large set of more than 300 molecules representing (nearly) all elements-except lanthanides-in their common oxidation states was used to assess the quality of the bases all across the periodic table. Quantities investigated were atomization energies, dipole moments and structure parameters for Hartree-Fock, density functional theory and correlated methods, for which we had chosen Møller-Plesset perturbation theory as an example. Finally recommendations are given which type of basis set is used best for a certain level of theory and a desired quality of results.
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              Calcium signaling.

              David E Clapham, Md. Islam (2008)
              Calcium ions (Ca(2+)) impact nearly every aspect of cellular life. This review examines the principles of Ca(2+) signaling, from changes in protein conformations driven by Ca(2+) to the mechanisms that control Ca(2+) levels in the cytoplasm and organelles. Also discussed is the highly localized nature of Ca(2+)-mediated signal transduction and its specific roles in excitability, exocytosis, motility, apoptosis, and transcription.
              Article 0 comments Cited 1246 times – based on 0 reviews     Review now
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                Author and article information

                Contributors
                Zherui Zhang:
                ORCID: https://orcid.org/0009-0000-3385-6161
                Role: ConceptualizationRole: Formal analysisRole: InvestigationRole: MethodologyRole: Project administrationRole: SoftwareRole: ValidationRole: VisualizationRole: Writing - original draftRole: Writing - review & editing
                Yuhao Luo:
                ORCID: https://orcid.org/0000-0002-9392-5760
                Role: Formal analysisRole: InvestigationRole: MethodologyRole: Project administrationRole: ResourcesRole: ValidationRole: Writing - review & editing
                Yuanhong Ma: Role: InvestigationRole: MethodologyRole: ResourcesRole: Validation
                Yaofeng Zhou: Role: Writing - review & editing
                Dingcheng Zhu:
                ORCID: https://orcid.org/0000-0002-5636-4976
                Role: ConceptualizationRole: Data curationRole: Formal analysisRole: Funding acquisitionRole: InvestigationRole: MethodologyRole: Project administrationRole: ResourcesRole: SoftwareRole: SupervisionRole: ValidationRole: VisualizationRole: Writing - original draftRole: Writing - review & editing
                Wanhua Shen:
                ORCID: https://orcid.org/0000-0002-5178-9561
                Role: ConceptualizationRole: Data curationRole: Formal analysisRole: Funding acquisitionRole: InvestigationRole: MethodologyRole: Project administrationRole: ResourcesRole: SupervisionRole: ValidationRole: VisualizationRole: Writing - original draftRole: Writing - review & editing
                Junqiu Liu:
                ORCID: https://orcid.org/0000-0003-1608-7908
                Role: ConceptualizationRole: Data curationRole: Formal analysisRole: Funding acquisitionRole: InvestigationRole: MethodologyRole: Project administrationRole: ResourcesRole: SoftwareRole: SupervisionRole: ValidationRole: VisualizationRole: Writing - original draftRole: Writing - review & editing
                Journal
                Journal ID (nlm-ta): Sci Adv
                Journal ID (iso-abbrev): Sci Adv
                Journal ID (publisher-id): sciadv
                Journal ID (hwp): advances
                Title: Science Advances
                Publisher: American Association for the Advancement of Science
                ISSN (Electronic): 2375-2548
                Publication date Collection: 19 April 2024
                Publication date (Electronic, pub): 19 April 2024
                Volume: 10
                Issue: 16
                Electronic Location Identifier: eadl0263
                Affiliations
                [ 1 ]College of Material, Chemistry, and Chemical Engineering, Key Laboratory of Organosilicon Chemistry and Material Technology, Ministry of Education, Hangzhou Normal University, Hangzhou 311121, China.
                [ 2 ]Zhejiang Key Laboratory of Organ Development and Regeneration, College of Life and Environmental Sciences, Hangzhou Normal University, Hangzhou, Zhejiang 310036, China.
                [ 3 ]Westlake University, Shilongshan Rd. Cloud Town, Xihu District, Hangzhou, Zhejiang, China.
                Author notes
                [* ]Corresponding author. Email: shen@ 123456hznu.edu.cn (W.S.); zhudc@ 123456hznu.edu.cn (D.Z.); junqiuliu@ 123456hznu.edu.cn (J.L.)
                [†]

                These authors contributed equally to this work.

                Author information
                https://orcid.org/0009-0000-3385-6161
                https://orcid.org/0000-0002-9392-5760
                https://orcid.org/0000-0002-5636-4976
                https://orcid.org/0000-0002-5178-9561
                https://orcid.org/0000-0003-1608-7908
                Article
                Publisher ID: adl0263
                DOI: 10.1126/sciadv.adl0263
                PMC ID: 11029810
                PubMed ID: 38640246
                SO-VID: c8a4cf08-1645-4974-a598-fc543a3a73b6
                Copyright © Copyright © 2024 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).
                License:

                This is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license, which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited.

                History
                Date received : 25 September 2023
                Date accepted : 18 March 2024
                Funding
                Funded by: FundRef http://dx.doi.org/10.13039/501100001809, National Natural Science Foundation of China;
                Award ID: 22105055
                Funded by: FundRef http://dx.doi.org/10.13039/501100003787, Natural Science Foundation of Hebei Province;
                Award ID: F2021203102
                Funded by: FundRef http://dx.doi.org/10.13039/501100004731, Natural Science Foundation of Zhejiang Province;
                Award ID: LQ22E03001
                Funded by: National Natural Sciences Foundation of China;
                Award ID: 31871041
                Funded by: National Natural Sciences Foundation of China;
                Award ID: 22161142015
                Funded by: Scientific Research Start up Foundation of Hangzhou Normal University;
                Award ID: 2021QDL015
                Funded by: Hangzhou Leading Innovation and Entrepreneurship Team Project;
                Award ID: TD2022001
                Funded by: National KeyR&D Program of China;
                Award ID: 2020YFA0908503
                Funded by: Scientific Research Start-up Foundation of Hangzhou Normal University;
                Award ID: 2019QDL026
                Categories
                Subject: Research Article
                Subject: Physical and Materials Sciences
                Subject: SciAdv r-articles
                Subject: Materials Science
                Subject: Signal Transduction
                Subject: Materials Science
                Custom metadata
                Copyeditor Michael Sabado

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