New horizons for catalysis disclosed by supramolecular chemistry

The adoption of a supramolecular approach in catalysis promises to address a number of unmet challenges, ranging from activity (unlocking of novel reaction pathways) to selectivity (alteration of the innate selectivity of a reaction, e.g. selective functionalization of C-H bonds) and regulation (swi...

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Published inChemical Society reviews Vol. 5; no. 13; pp. 7681 - 7724
Main Authors Olivo, Giorgio, Capocasa, Giorgio, Del Giudice, Daniele, Lanzalunga, Osvaldo, Di Stefano, Stefano
Format Journal Article
LanguageEnglish
Published England Royal Society of Chemistry 05.07.2021
Subjects
carbon-hydrogen bond activation
Catalysis
catalysts
catalytic activity
fields
Molecular machines
Recognition
researchers
Selectivity
selectivity (chemistry)
Stoichiometry
Online AccessGet full text
ISSN0306-0012
1460-4744
1460-4744
DOI10.1039/d1cs00175b

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Abstract The adoption of a supramolecular approach in catalysis promises to address a number of unmet challenges, ranging from activity (unlocking of novel reaction pathways) to selectivity (alteration of the innate selectivity of a reaction, e.g. selective functionalization of C-H bonds) and regulation (switch ON/OFF, sequential catalysis, etc. ). Supramolecular tools such as reversible association and recognition, pre-organization of reactants and stabilization of transition states upon binding offer a unique chance to achieve the above goals disclosing new horizons whose potential is being increasingly recognized and used, sometimes reaching the degree of ripeness for practical use. This review summarizes the main developments that have opened such new frontiers, with the aim of providing a guide to researchers approaching the field. We focus on artificial supramolecular catalysts of defined stoichiometry which, under homogeneous conditions, unlock outcomes that are highly difficult if not impossible to attain otherwise, namely unnatural reactivity or selectivity and catalysis regulation. The different strategies recently explored in supramolecular catalysis are concisely presented, and, for each one, a single or very few examples is/are described (mainly last 10 years, with only milestone older works discussed). The subject is divided into four sections in light of the key design principle: (i) nanoconfinement of reactants, (ii) recognition-driven catalysis, (iii) catalysis regulation by molecular machines and (iv) processive catalysis. Recent advancements in supramolecular catalysis are reviewed, which show the potential of related tools when applied to organic synthesis. Such tools are recognized as innovative instruments that can pave the way to alternative synthetic strategies.
AbstractList The adoption of a supramolecular approach in catalysis promises to address a number of unmet challenges, ranging from activity (unlocking of novel reaction pathways) to selectivity (alteration of the innate selectivity of a reaction, e.g. selective functionalization of C-H bonds) and regulation (switch ON/OFF, sequential catalysis, etc.). Supramolecular tools such as reversible association and recognition, pre-organization of reactants and stabilization of transition states upon binding offer a unique chance to achieve the above goals disclosing new horizons whose potential is being increasingly recognized and used, sometimes reaching the degree of ripeness for practical use. This review summarizes the main developments that have opened such new frontiers, with the aim of providing a guide to researchers approaching the field. We focus on artificial supramolecular catalysts of defined stoichiometry which, under homogeneous conditions, unlock outcomes that are highly difficult if not impossible to attain otherwise, namely unnatural reactivity or selectivity and catalysis regulation. The different strategies recently explored in supramolecular catalysis are concisely presented, and, for each one, a single or very few examples is/are described (mainly last 10 years, with only milestone older works discussed). The subject is divided into four sections in light of the key design principle: (i) nanoconfinement of reactants, (ii) recognition-driven catalysis, (iii) catalysis regulation by molecular machines and (iv) processive catalysis.
The adoption of a supramolecular approach in catalysis promises to address a number of unmet challenges, ranging from activity (unlocking of novel reaction pathways) to selectivity (alteration of the innate selectivity of a reaction, e.g. selective functionalization of C-H bonds) and regulation (switch ON/OFF, sequential catalysis, etc. ). Supramolecular tools such as reversible association and recognition, pre-organization of reactants and stabilization of transition states upon binding offer a unique chance to achieve the above goals disclosing new horizons whose potential is being increasingly recognized and used, sometimes reaching the degree of ripeness for practical use. This review summarizes the main developments that have opened such new frontiers, with the aim of providing a guide to researchers approaching the field. We focus on artificial supramolecular catalysts of defined stoichiometry which, under homogeneous conditions, unlock outcomes that are highly difficult if not impossible to attain otherwise, namely unnatural reactivity or selectivity and catalysis regulation. The different strategies recently explored in supramolecular catalysis are concisely presented, and, for each one, a single or very few examples is/are described (mainly last 10 years, with only milestone older works discussed). The subject is divided into four sections in light of the key design principle: (i) nanoconfinement of reactants, (ii) recognition-driven catalysis, (iii) catalysis regulation by molecular machines and (iv) processive catalysis. Recent advancements in supramolecular catalysis are reviewed, which show the potential of related tools when applied to organic synthesis. Such tools are recognized as innovative instruments that can pave the way to alternative synthetic strategies.
The adoption of a supramolecular approach in catalysis promises to address a number of unmet challenges, ranging from activity (unlocking of novel reaction pathways) to selectivity (alteration of the innate selectivity of a reaction, e.g. selective functionalization of C–H bonds) and regulation (switch ON/OFF, sequential catalysis, etc. ). Supramolecular tools such as reversible association and recognition, pre-organization of reactants and stabilization of transition states upon binding offer a unique chance to achieve the above goals disclosing new horizons whose potential is being increasingly recognized and used, sometimes reaching the degree of ripeness for practical use. This review summarizes the main developments that have opened such new frontiers, with the aim of providing a guide to researchers approaching the field. We focus on artificial supramolecular catalysts of defined stoichiometry which, under homogeneous conditions, unlock outcomes that are highly difficult if not impossible to attain otherwise, namely unnatural reactivity or selectivity and catalysis regulation. The different strategies recently explored in supramolecular catalysis are concisely presented, and, for each one, a single or very few examples is/are described (mainly last 10 years, with only milestone older works discussed). The subject is divided into four sections in light of the key design principle: (i) nanoconfinement of reactants, (ii) recognition-driven catalysis, (iii) catalysis regulation by molecular machines and (iv) processive catalysis.
The adoption of a supramolecular approach in catalysis promises to address a number of unmet challenges, ranging from activity (unlocking of novel reaction pathways) to selectivity (alteration of the innate selectivity of a reaction, e.g. selective functionalization of C-H bonds) and regulation (switch ON/OFF, sequential catalysis, etc.). Supramolecular tools such as reversible association and recognition, pre-organization of reactants and stabilization of transition states upon binding offer a unique chance to achieve the above goals disclosing new horizons whose potential is being increasingly recognized and used, sometimes reaching the degree of ripeness for practical use. This review summarizes the main developments that have opened such new frontiers, with the aim of providing a guide to researchers approaching the field. We focus on artificial supramolecular catalysts of defined stoichiometry which, under homogeneous conditions, unlock outcomes that are highly difficult if not impossible to attain otherwise, namely unnatural reactivity or selectivity and catalysis regulation. The different strategies recently explored in supramolecular catalysis are concisely presented, and, for each one, a single or very few examples is/are described (mainly last 10 years, with only milestone older works discussed). The subject is divided into four sections in light of the key design principle: (i) nanoconfinement of reactants, (ii) recognition-driven catalysis, (iii) catalysis regulation by molecular machines and (iv) processive catalysis.The adoption of a supramolecular approach in catalysis promises to address a number of unmet challenges, ranging from activity (unlocking of novel reaction pathways) to selectivity (alteration of the innate selectivity of a reaction, e.g. selective functionalization of C-H bonds) and regulation (switch ON/OFF, sequential catalysis, etc.). Supramolecular tools such as reversible association and recognition, pre-organization of reactants and stabilization of transition states upon binding offer a unique chance to achieve the above goals disclosing new horizons whose potential is being increasingly recognized and used, sometimes reaching the degree of ripeness for practical use. This review summarizes the main developments that have opened such new frontiers, with the aim of providing a guide to researchers approaching the field. We focus on artificial supramolecular catalysts of defined stoichiometry which, under homogeneous conditions, unlock outcomes that are highly difficult if not impossible to attain otherwise, namely unnatural reactivity or selectivity and catalysis regulation. The different strategies recently explored in supramolecular catalysis are concisely presented, and, for each one, a single or very few examples is/are described (mainly last 10 years, with only milestone older works discussed). The subject is divided into four sections in light of the key design principle: (i) nanoconfinement of reactants, (ii) recognition-driven catalysis, (iii) catalysis regulation by molecular machines and (iv) processive catalysis.
Author Lanzalunga, Osvaldo
Capocasa, Giorgio
Di Stefano, Stefano
Del Giudice, Daniele
Olivo, Giorgio
AuthorAffiliation Università degli Studi di Roma "La Sapienza"
Dipartimento di Chimica
Dipartimento di Chimica and ISB-CNR Sede Secondaria di Roma - Meccanismi di Reazione
AuthorAffiliation_xml – name: Dipartimento di Chimica and ISB-CNR Sede Secondaria di Roma - Meccanismi di Reazione
– name: Dipartimento di Chimica
– name: Università degli Studi di Roma "La Sapienza"
Author_xml – sequence: 1
  givenname: Giorgio
  surname: Olivo
  fullname: Olivo, Giorgio
– sequence: 2
  givenname: Giorgio
  surname: Capocasa
  fullname: Capocasa, Giorgio
– sequence: 3
  givenname: Daniele
  surname: Del Giudice
  fullname: Del Giudice, Daniele
– sequence: 4
  givenname: Osvaldo
  surname: Lanzalunga
  fullname: Lanzalunga, Osvaldo
– sequence: 5
  givenname: Stefano
  surname: Di Stefano
  fullname: Di Stefano, Stefano
BackLink https://www.ncbi.nlm.nih.gov/pubmed/34008654$$D View this record in MEDLINE/PubMed
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Notes Giorgio Olivo obtained his PhD in 2015 at "La Sapienza" university of Rome (Italy) with S. Di Stefano. Then, he moved to Girona (Spain) as a postdoctoral fellow in the QBIS group of M. Costas (2016-2020), working on a recognition-driven oxidation of remote aliphatic C-H bonds catalyzed by Fe and Mn catalysts. Recently (2021) he moved back to Rome, where his research interests lie in the design and implementation of a supramolecular approach to control selectivity in late-stage functionalization and in bioinspired metal catalysis.
Giorgio Capocasa was born in Rome in 1993. In 2017, he earned a master's degree in Chemistry at "La Sapienza" University of Rome (Italy) and enrolled in a PhD programme at the same university. In 2021, he gained his PhD with a thesis on supramolecular catalysis applied to hydrocarbon functionalization under the supervision of S. Di Stefano. He is currently working as a post-doc in the M. Costas group at "Universitat de Girona" (Catalunya, Spain) with a project on bioinspired C-H functionalization.
Osvaldo Lanzalunga received his PhD degree from the University of Rome "La Sapienza" in 1994. After postdoctoral experience in S. Steenken group at the Max Plank Institute fur Strahlenchemie, Mülheim (Germany) he became Researcher and is currently Full Professor in Organic Chemistry at the Dipartimento di Chimica of the University "La Sapienza". His scientific research is mainly focused on the chemistry of radicals and radical ions, on the role of structural and medium effects on hydrogen atom transfer (HAT) and electron-transfer (ET) reactions involving oxygen-centered radicals and on the role of ET processes in organic and bioorganic reactions.
Daniele Del Giudice was born in Latina in 1995. In 2019 he earned the master's degree in chemistry at the University of Rome La Sapienza, receiving the "Excellent Graduate" award from the same university. Master's degree internship was performed in the laboratory of S. Di Stefano, regarding the development of chemical fuels triggering the motion of acid-base operating molecular machines. Then he enrolled in a PhD programme under the supervision of the same professor, working on the employment of chemical fuels to obtain dissipative control on several kinds of supramolecular systems.
Stefano Di Stefano received his PhD in Chemical Sciences in 2000 at the University of Rome La Sapienza. After a period in the pharmaceutical industry, he came back to the same University where he is now an Associate Professor. His research interests lie in the field of supramolecular catalysis, dynamic covalent chemistry, and chemically driven molecular machines. For his research work, he received an award from Italian Chemical Society in 2020. He also received the prize for "Excellent University Teaching" in 2014, 2017 and 2018 from the Faculty Dean. He has been involved in many national and international scientific collaborations.
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Snippet The adoption of a supramolecular approach in catalysis promises to address a number of unmet challenges, ranging from activity (unlocking of novel reaction...
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SubjectTerms carbon-hydrogen bond activation
Catalysis
catalysts
catalytic activity
fields
Molecular machines
Recognition
researchers
Selectivity
selectivity (chemistry)
Stoichiometry
Title New horizons for catalysis disclosed by supramolecular chemistry
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