Mark R. Crimmin
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View article: A heterometallic σ-silane adduct from cooperative reactivity of an iron–aluminium complex
A heterometallic σ-silane adduct from cooperative reactivity of an iron–aluminium complex Open
Protonation of a heterometallic silanide complex with an alcohol led to formation of a σ-silane complex. This reaction does not require a strong acid or weakly coordinating anion.
View article: Defluoroalkylation of Trifluoromethane with Organolithium Reagents: Mechanism and Synthesis of Fluoroalkenes
Defluoroalkylation of Trifluoromethane with Organolithium Reagents: Mechanism and Synthesis of Fluoroalkenes Open
Trifluoromethane (HCF 3 , HFC‐23) is a byproduct of fluoropolymer production that has limited applications. It is often stored or destroyed at the point of production, but if released into the environment is a potent greenhouse gas with a …
View article: Defluoroalkylation of Trifluoromethane with Organolithium Reagents: Mechanism and Synthesis of Fluoroalkenes
Defluoroalkylation of Trifluoromethane with Organolithium Reagents: Mechanism and Synthesis of Fluoroalkenes Open
Trifluoromethane (HCF 3 , HFC‐23) is a byproduct of fluoropolymer production that has limited applications. It is often stored or destroyed at the point of production, but if released into the environment is a potent greenhouse gas with a …
View article: Chemical Recycling of Hydrofluorocarbons by Transfer Fluorination
Chemical Recycling of Hydrofluorocarbons by Transfer Fluorination Open
Fluorochemicals improve our quality of life, there is however increasing concern over how they are made and their negative impacts on health and the environment. Here we report an approach to the recycling of fluorochemicals. Treatment of …
View article: An accessible and efficient 3D printed modular ‘M-Arc’ photoreactor
An accessible and efficient 3D printed modular ‘M-Arc’ photoreactor Open
An accessible, 3D printable modular photoreactor is presented and benchmarked against commercial products using actinometry and kinetic analysis of 4CzIPN catalysed transformations.
View article: A Heterometallic σ-Silane Adduct from Cooperative Reactivity of an Fe–Al Complex
A Heterometallic σ-Silane Adduct from Cooperative Reactivity of an Fe–Al Complex Open
Protonation of an Fe–Al heterometallic silanide complex with an alcohol led to selective formation of the corresponding σ-silane complex. This reaction does not require the use of a weakly coordinating anion, but rather the synergistic act…
View article: Defluoroalkylation of Trifluoromethane with Organolithium Reagents: Mechanism and Synthesis of Fluoroalkenes
Defluoroalkylation of Trifluoromethane with Organolithium Reagents: Mechanism and Synthesis of Fluoroalkenes Open
Trifluoromethane (HCF3) is a byproduct of fluoropolymer production that has limited applications. It is often stored or destroyed at the point of production, but if released into the environment is a potent greenhouse gas with a global war…
View article: C(sp <sup>2</sup> )─H Bond Activation with a Heterometallic Nickel–Aluminium Complex
C(sp <sup>2</sup> )─H Bond Activation with a Heterometallic Nickel–Aluminium Complex Open
Herein we present a ligand‐catalyzed bond‐breaking and making process that occurs with a Ni–Al heterometallic complex. While combinations of Ni pre‐catalysts and Al additives are known for site‐selective C─H functionalization, detailed stu…
View article: Synthesis, Properties, and Chemoselective Reactions of an AlH–BH Functional Group
Synthesis, Properties, and Chemoselective Reactions of an AlH–BH Functional Group Open
A new alumaborane compound containing a {AlH–BH} functional group has been prepared by reaction of the aluminium(I) complex [{(ArCMeN)2CH}Al] (Ar = 2,6-i-Pr2C6H3) with a boron dihydride species supported by an anionic chelating kappa-2-N,N…
View article: C(sp <sup>2</sup> )─H Bond Activation with a Heterometallic Nickel–Aluminium Complex
C(sp <sup>2</sup> )─H Bond Activation with a Heterometallic Nickel–Aluminium Complex Open
Herein we present a ligand‐catalyzed bond‐breaking and making process that occurs with a Ni–Al heterometallic complex. While combinations of Ni pre‐catalysts and Al additives are known for site‐selective C─H functionalization, detailed stu…
View article: Phosphine-Catalyzed C(sp2)–H Bond Activation with a Heterometallic Nickel---Aluminum Complex
Phosphine-Catalyzed C(sp2)–H Bond Activation with a Heterometallic Nickel---Aluminum Complex Open
Herein we present the discovery of a ligand-catalyzed bond breaking and making processes that occurs in the coordination sphere of a novel Ni–Al heterometallic complex. While combinations of Ni pre-catalysts and Al additives are known for …
View article: Synthetic Methodologies for the Chemical Recycling of Fluorocarbons
Synthetic Methodologies for the Chemical Recycling of Fluorocarbons Open
In this review, we describe synthetic methods that harvest fluoride (F–) from fluorocarbons and deliver it to other molecules through either transfer fluorination or fluoride shuttling. We also summarise related approaches, transfer hydrof…
View article: Synthetic Methodologies for the Chemical Recycling of Fluorocarbons
Synthetic Methodologies for the Chemical Recycling of Fluorocarbons Open
In this review, we describe synthetic methods that harvest fluoride (F–) from fluorocarbons and deliver it to other molecules through either transfer fluorination or fluoride shuttling. We also summarise related approaches, transfer hydrof…
View article: Reactions of a Zn–Zn bond with main group carbene analogues as a prototypical case of reductive addition
Reactions of a Zn–Zn bond with main group carbene analogues as a prototypical case of reductive addition Open
Oxidative addition most commonly involves the addition of a substrate to a metal centre. This reaction is fundamental across synthetic chemistry and underpins numerous catalytic methods. In the textbook description of oxidative addition re…
View article: Chemical Recycling of Hydrofluorocarbons by Transfer Fluorination
Chemical Recycling of Hydrofluorocarbons by Transfer Fluorination Open
The production of fluorochemicals is currently achieved through a linear manufacturing process starting from fluorspar (CaF2). While fluorochemicals improve our quality of life, there is increasing concern over their negative impact on hea…
View article: Homocoupling of C1 Building Blocks by a Heterometallic Mg–Al Complex
Homocoupling of C1 Building Blocks by a Heterometallic Mg–Al Complex Open
A heterometallic magnesium–aluminium hydride complex is reported for the selective homologation of C1 building blocks (CO and CNXyl, Xyl = 2,6-dimethylphenyl) to form products containing C2 and C3 chains. CO reacts to form known deltate or…
View article: Boron, Aluminum, and Gallium Fluorides as Catalysts for the Defluorofunctionalization of Electron-Deficient Arenes: The Role of NaBAr<sup>F</sup><sub>4</sub> Promoters
Boron, Aluminum, and Gallium Fluorides as Catalysts for the Defluorofunctionalization of Electron-Deficient Arenes: The Role of NaBAr<sup>F</sup><sub>4</sub> Promoters Open
A series of boron, aluminum, and gallium difluoride complexes [{(ArNCMe)2CH}MF2] (M = B, Al, Ga) are reported as catalysts for the defluorofunctionalization of electron-deficient arenes. Thiodefluorination reactions b…
View article: Flash Communication: Pd<sub>2</sub>Zn<sub>2</sub> Clusters from the Reduction of Palladium(II) Dichloride Precursors with Metallic Zinc
Flash Communication: Pd<sub>2</sub>Zn<sub>2</sub> Clusters from the Reduction of Palladium(II) Dichloride Precursors with Metallic Zinc Open
We report the synthesis and solid-state characterization of two unusual Pd2Zn2 clusters formed from the partial reduction of [PdL2Cl2] precursors (L2 = dcpe or dppe) with metallic zinc…
View article: Homocoupling of C<sub>1</sub> building blocks by a heterometallic Mg–Al complex
Homocoupling of C<sub>1</sub> building blocks by a heterometallic Mg–Al complex Open
A heterometallic magnesium–aluminium hydride complex is reported for the selective homologation of C 1 building blocks (CO and CNXyl, Xyl = 2,6-Me 2 C 6 H 3 ) to form products containing C 2 and C 3 chains.
View article: Electrochemical dehydrogenative intramolecular C–C coupling for expedient carbazole synthesis
Electrochemical dehydrogenative intramolecular C–C coupling for expedient carbazole synthesis Open
A metal/oxidant-free electrochemical method enables regioselective carbazole synthesis via dehydrogenative aryl–aryl coupling of arylamines. Reactivity and selectivity are supported by cyclic voltammetry and DFT studies.
View article: Combined Kinetic and Computational Analysis of the Palladium-Catalyzed Formylation of Aryl Bromides
Combined Kinetic and Computational Analysis of the Palladium-Catalyzed Formylation of Aryl Bromides Open
Aryl aldehydes are key synthetic intermediates in the manufacturing of active pharmaceutical ingredients. They are generated on scale (>1000 kg) through the palladium-catalyzed formylation of aryl bromides using syngas (CO/H2). …
View article: Fluoroalkenes from the Defluoroalkylation of Trifluoromethane
Fluoroalkenes from the Defluoroalkylation of Trifluoromethane Open
Trifluoromethane (HCF3) is a byproduct of fluoropolymer production that has limited applications. It is often stored or destroyed at the point of production, but if released into the environment is a potent greenhouse gas with global warmi…
View article: Boron, Aluminium, and Gallium Fluorides as Catalysts for the Defluorofunctionalisation of Electron-Deficient Arenes: The Role of NaBArF4 Promoters
Boron, Aluminium, and Gallium Fluorides as Catalysts for the Defluorofunctionalisation of Electron-Deficient Arenes: The Role of NaBArF4 Promoters Open
A series of molecular boron, aluminium, and gallium difluoride complexes [{(ArNCMe)2CH}MF2] (M = B, Al, Ga) are reported as catalysts for the defluorofunctionalisation of electron-deficient arenes. Thiodefluorination reactions between TMS–…
View article: A Continuous Flow Process for the Defluorosilylation of HFC-23 and HFO-1234yf
A Continuous Flow Process for the Defluorosilylation of HFC-23 and HFO-1234yf Open
A continuous flow process has been developed for the defluorosilylation of trifluoromethane (HFC-23) and 2,3,3,3-tetrafluoropropene (HFO-1234yf) through reaction with lithium silanide reagents under inert conditions. Design of experiment o…
View article: A Continuous Flow Process for the Defluorosilylation of HFC-23 and HFO-1234yf
A Continuous Flow Process for the Defluorosilylation of HFC-23 and HFO-1234yf Open
A continuous flow process has been developed for the defluorosilylation of trifluoromethane (HFC-23) and 2,3,3,3-propene (HFO-1234yf) through reaction with lithium silanide reagents under inert conditions. Design of experiment optimization…
View article: A Combined Kinetic and Computational Analysis of the Palladium-Catalysed Formylation of Aryl Bromides
A Combined Kinetic and Computational Analysis of the Palladium-Catalysed Formylation of Aryl Bromides Open
Aryl aldehydes are key synthetic intermediates in the manufacturing of active pharmaceutical ingredients. They are generated on scale (>1000 kg) through the palladium-catalysed formylation of aryl bromides using syngas (CO:H2). The best-in…
View article: Reductive Addition of a Zn–Zn Bond to Main Group Carbene Analogues
Reductive Addition of a Zn–Zn Bond to Main Group Carbene Analogues Open
Oxidative Addition involves the addition of a substrate to a metal centre. This reaction is fundamental across synthetic chemistry and underpins numerous catalytic methods. In the textbook description of oxidative addition reactions, charg…
View article: A Paramagnetic Nickel–Zinc Hydride Complex
A Paramagnetic Nickel–Zinc Hydride Complex Open
Reaction of a molecular zinc–hydride [{(ArNCMe) 2 CH}ZnH] (Ar=2,6‐di‐isopropylphenyl) with 0.5 equiv. of [Ni(CO)Cp] 2 led to the isolation of a nickel–zinc hydride complex containing a bridging 3‐centre,2‐electron Ni−H−Zn interaction. This…
View article: A Paramagnetic Nickel–Zinc Hydride Complex
A Paramagnetic Nickel–Zinc Hydride Complex Open
Reaction of a molecular zinc–hydride [{(ArNCMe) 2 CH}ZnH] (Ar=2,6‐di‐isopropylphenyl) with 0.5 equiv. of [Ni(CO)Cp] 2 led to the isolation of a nickel–zinc hydride complex containing a bridging 3‐centre,2‐electron Ni−H−Zn interaction. This…
View article: Dyotropic Rearrangement of an Iron–Aluminium Complex
Dyotropic Rearrangement of an Iron–Aluminium Complex Open
Ligand exchange processes at metal complexes underpin their reactivity and catalytic applications. While mechanisms of ligand exchange at single site complexes are well established, occurring through textbook associative, dissociative and …