Malcolmson, Steven - Duke University - Department of Chemistry

个人简介

Steven Malcolmson was born and raised in Boston, MA and received a B.A. in Chemistry from Boston University in 2004. He attended Boston College for graduate school, developing new Mo-based catalysts for stereoselective olefin metathesis under the mentorship of Prof. Amir Hoveyda in collaboration with Prof. Richard Schrock (MIT). After obtaining a Ph.D. in 2010, Steve studied natural product biosynthesis as an NIH postdoctoral fellow with Prof. Chris Walsh at Harvard Medical School. He began his independent career at Duke University in 2013 as an Assistant Professor of Chemistry and was promoted to Associate Professor in 2020.

研究领域

The discovery of catalysts is of great importance to the practice of modern synthetic chemistry, both to improve upon the existing catalog of chemical transformations and to generate new modes of reactivity. Research in the Malcolmson lab focuses on the discovery of novel methods for the efficient and selective synthesis of small molecule scaffolds through the design and development of new catalysts. In these transformations, we seek to realize new synthetic bond disconnections while also controlling some aspect of selectivity (e.g., enantio-, and/or site selectivity). The catalysts and methods developed in the group are being applied to the synthesis of biologically active molecules to drive the development of new chemistry as well as help to address problems in human health.

近期论文

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2-Azadienes as Reagents for Preparing Chiral Amines: Synthesis of 1,2-Amino Tertiary Alcohols by Cu-Catalyzed Enantioselective Reductive Couplings with Ketones. We introduce a new strategy for synthesis of chiral amines: couplings of α-aminoalkyl nucleophiles generated by enantioselective migratory insertion of 2-azadienes to a Cu-H. Bipyridine Adducts of Molybdenum Imido Alkylidene and Imido Alkylidyne Complexes. Seven bipyridine adducts of molybdenum imido alkylidene bispyrrolide complexes of the type Mo(NR)(CHCMe(2)R')(Pyr)(2)(bipy) (1a-1g; R = 2,6-i-Pr(2)C(6)H(3) (Ar), adamantyl (Ad), 2,6-Me(2)C(6)H(3) (Ar'), 2-i-PrC(6)H(4) (Ar(iPr)), 2-ClC(6)H(4) (Ar(C Catalyst-Controlled Stereoselective Olefin Metathesis © 2015 Wiley-VCH Verlag GmbH & Co. KGaA. All rights reserved. This chapter covers the advances made since 2003 in the development of catalysts that can control the stereochemical outcome of olefin metathesis reactions. Catalytic enantioselective olefin metathesis in natural product synthesis. Chiral metal-based complexes that deliver high enantioselectivity and more. Chiral olefin metathesis catalysts enable chemists to access enantiomerically enriched small molecules with high efficiency; synthesis schemes involving such complexes can be substantially more concise than those that would involve enantiomericall Cover Picture: Diazirines as Potential Molecular Imaging Tags: Probing the Requirements for Efficient and Long-Lived SABRE-Induced Hyperpolarization (Angew. Chem. Int. Ed. 40/2017) Design and stereoselective preparation of a new class of chiral olefin metathesis catalysts and application to enantioselective synthesis of quebrachamine: catalyst development inspired by natural product synthesis. A total synthesis of the Aspidosperma alkaloid quebrachamine in racemic form is first described. Development and Mechanistic Investigations of Enantioselective Pd-Catalyzed Intermolecular Hydroaminations of Internal Dienes © 2018 American Chemical Society. We report the development of highly enantio- and regioselective Pd-catalyzed intermolecular hydroaminations of challenging 1,4-disubstituted acyclic dienes. Diastereoselective and Enantiospecific Synthesis of 1,3-Diamines via 2-Azaallyl Anion Benzylic Ring-Opening of Aziridines. The 1,3-diamine motif appears in numerous complex molecules, yet there are few methods for the stereoselective construction of this moiety. Diazirines as Potential Molecular Imaging Tags: Probing the Requirements for Efficient and Long-Lived SABRE-Induced Hyperpolarization Diazirines are an attractive class of potential molecular tags for magnetic resonance imaging owing to their biocompatibility and ease of incorporation into a large variety of molecules. Dihydrophenylalanine: a prephenate-derived Photorhabdus luminescens antibiotic and intermediate in dihydrostilbene biosynthesis. 2,5-Dihydrophenylalanine (H(2)Phe) is a multipotent nonproteinogenic amino acid produced by various Actinobacteria and Gammaproteobacteria. Direct and cost-efficient hyperpolarization of long-lived nuclear spin states on universal 15N2-diazirine molecular tags Conventional magnetic resonance (MR) faces serious sensitivity limitations which can be overcome by hyperpolarization methods, but the most common method (dynamic nuclear polarization) is complex and expensive, and applications are limited by shor Direct Hyperpolarization of Nitrogen-15 in Aqueous Media with Parahydrogen in Reversible Exchange. Signal amplification by reversible exchange (SABRE) is an inexpensive, fast, and even continuous hyperpolarization technique that uses para-hydrogen as hyperpolarization source. Enantioselective Intermolecular Addition of Aliphatic Amines to Acyclic Dienes with a Pd-PHOX Catalyst. We report a method for the catalytic, enantioselective intermolecular addition of aliphatic amines to acyclic 1,3-dienes. Enantioselective Intermolecular Pd-Catalyzed Hydroalkylation of Acyclic 1,3-Dienes with Activated Pronucleophiles. We report a highly enantioselective Pd-PHOX-catalyzed intermolecular hydroalkylation of acyclic 1,3-dienes. Enantioselective Synthesis of anti-1,2-Diamines by Cu-Catalyzed Reductive Couplings of Azadienes with Aldimines and Ketimines. Here we report highly efficient and chemoselective azadiene-imine reductive couplings catalyzed by (Ph-BPE)Cu-H that afford anti-1,2-diamines. Enantioselective synthesis of cyclic enol ethers and all-carbon quaternary stereogenic centers through catalytic asymmetric ring-closing metathesis. The first examples of catalytic asymmetric ring-closing metathesis (ARCM) reactions of enol ethers are reported. To identify the most effective catalysts, various chiral Mo- and Ru-based catalysts were screened. Enantioselective synthesis of P-stereogenic phosphinates and phosphine oxides by molybdenum-catalyzed asymmetric ring-closing metathesis.