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Lipshultz Group

@lipshultzsbu.bsky.social

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Lipshultz Group@lipshultzsbu.bsky.social · 3mo ago

Thrilled to share great news! The group has received an NSF CAREER award! This grant will support our efforts in the development of rationally-designed photoactive Ti catalysts, as we seek to develop new synthetic transformations operating in catalyst-controlled paradigms!

Lipshultz Group@lipshultzsbu.bsky.social · 3mo ago

Congratulations to our undergrads! Returning for the summer Jialin Li awarded Mitchell Wortzman Undergraduate Research Award! 👩‍🔬👨‍🔬And our joining undergrad Matthew Serrano awarded Exploration in STEM scholar! Excited to see them in the lab this summer! 🥼🥽🧪

Lipshultz Group@lipshultzsbu.bsky.social · 3mo ago

Congrats to our two undergrads leaving us for the summer! 🥽 Joshua Griffin who will be working with Prof. Jacqueline Smith at Howard! And Mahir Hossain whos joining Prof. Andrew Zahrt at UPenn! 🥽🚗🍀

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Lipshultz Group@lipshultzsbu.bsky.social · 6mo ago

🎉 Thrilled to share our latest work on Ti-LMCT photocatalysis, out now in @jacs.acspublications.org. We show how Ti-catalysts bearing electronically-differentiated ligands can be leveraged for divergent reaction pathways from the LMCT excited state. Read it here: pubs.acs.org/doi/10.1021/....

Leveraging Divergent Ligand-to-Metal Charge-Transfer Excited State Pathways for Catalyst Control over Alkoxyl Radical Reactivity

Ligand-to-metal charge-transfer (LMCT) excitation has emerged in recent years as a powerful modality in organic synthesis, namely for the generation of heteroatom-centered radicals through formal metal–ligand bond homolysis from the LMCT excited state. However, the exploitation of alternative LMCT excited state processes has been extremely limited. Here, we describe a general strategy for tuning the reaction course from LMCT excited states of titanium alkoxides. This reactivity paradigm has been exploited for tandem β-scission/Giese addition reactions of both scission-amenable and scission-recalcitrant alcohols under divergent reaction pathways of metal–ligand bond homolysis and excited state β-scission through judicious choice of electronically tuned Ti catalysts. Through intramolecular competition studies, catalyst-controlled scission is shown to facilitate a rate enhancement of up to 103-fold over the intrinsic scission of free alkoxyl radicals, highlighting the impact of accessing the excited state scission paradigm. Computations support the relevance of a scission-promoting LMCT excited state with stereoelectronically aligned alkoxyl radical cation character to enable direct, selective β-scission.

pubs.acs.org

Lipshultz Group@lipshultzsbu.bsky.social · last yr.

Sharing our 1st preprint on our work on organo-Ti photocatalysis! We've found that titanocenes are photoactive catalysts for alcohol activation by LMCT excitation, enabling β-scission of alkoxyl radicals for degradative functionalization. Congrats Jagrut, Ashley & the whole team!

Degradative Alcohol Functionalization by Titanocene Photocatalysis

Organotitanium complexes are scarcely employed in photocatalytic reactions despite their robust ligand-to-metal charge-transfer photo-chemistry. Herein, we describe the development of titanocene pho-t...

chemrxiv.org