The merger of photoredox catalysis with transition metal catalysis, termed metallaphotoredox catalysis, has become a mainstay in synthetic methodology over the past decade. Metallaphotoredox catalysis has combined the unparalleled capacity of transition metal catalysis for bond formation with the broad utility of photoinduced electron- and energy-transfer processes. Photocatalytic substrate activation has allowed the engagement of simple starting materials in metal-mediated bond-forming processes. Moreover, electron or energy transfer directly with key organometallic intermediates has provided novel activation modes entirely complementary to traditional catalytic platforms. This Review details and contextualizes the advancements in molecule construction brought forth by metallaphotocatalysis.

Metallaphotoredox: The Merger of Photoredox and Transition Metal Catalysis.

In recent years, visible light-induced transition metal catalysis has emerged as a new paradigm in organic photocatalysis, which has led to the discovery of unprecedented transformations as well as the improvement of known reactions. In this subfield of photocatalysis, a transition metal complex serves a double duty by harvesting photon energy and then enabling bond forming/breaking events mostly via a single catalytic cycle, thus contrasting the established dual photocatalysis in which an exogenous photosensitizer is employed. In addition, this approach often synergistically combines catalyst-substrate interaction with photoinduced process, a feature that is uncommon in conventional photoredox chemistry. This Review describes the early development and recent advances of this emerging field.

Visible Light-Induced Transition Metal Catalysis.

The development of transition metal (TM) catalysis for organic synthesis under visible light without recourse to typical photoredox catalysts has become a rapidly growing area of research and has b...

Transition Metal-Catalyzed Organic Reactions under Visible Light: Recent Developments and Future Perspectives

The emerging field of organometallic catalysis has shifted towards research on Earth-abundant transition metals due to their ready availability, economic advantage, and novel properties. In this case, manganese, the third most abundant transition-metal in the Earth's crust, has emerged as one of the leading competitors. Accordingly, a large number of molecularly-defined Mn-complexes has been synthesized and employed for hydrogenation, dehydrogenation, and hydroelementation reactions. In this regard, catalyst design is based on three pillars, namely, metal-ligand bifunctionality, ligand hemilability, and redox activity. Indeed, the developed catalysts not only differ in the number of chelating atoms they possess but also their working principles, thereby leading to different turnover numbers for product molecules. Hence, the critical assessment of molecularly defined manganese catalysts in terms of chelating atoms, reaction conditions, mechanistic pathway, and product turnover number is significant. Herein, we analyze manganese complexes for their catalytic activity, versatility to allow multiple transformations and their routes to convert substrates to target molecules. This article will also be helpful to get significant insight into ligand design, thereby aiding catalysis design.

Manganese-catalyzed hydrogenation, dehydrogenation, and hydroelementation reactions.

A simple and efficient protocol to generate amidyl radicals from amine functionalities through a manganese-mediated atom-transfer reaction has been developed. This approach employs an earth-abundant and inexpensive manganese complex, Mn2 (CO)10 , as the catalyst and visible light as the energy input. Using this strategy, site-selective chlorination of unactivated C(sp3 )-H bonds of aliphatic amines and intramolecular/intermolecular chloroaminations of unactivated alkenes were readily realized under mild reaction conditions, thus providing efficient access to a range of synthetically valuable alkyl chlorides, chlorinated pyrrolidines, and vicinal chloroamine derivatives. These practical reactions exhibit a broad substrate scope and tolerate a wide array of functional groups, and complex molecules including various marketed drug derivatives.

Generation and Reactivity of Amidyl Radicals: Manganese‐Mediated Atom‐Transfer Reaction

Visible-Light-Initiated Manganese-Catalyzed E-Selective Hydrosilylation and Hydrogermylation of Alkynes.

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Visible-Light-Initiated Manganese-Catalyzed E-Selective Hydrosilylation and Hydrogermylation of Alkynes.