Featured
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Article |
A photochemical dehydrogenative strategy for aniline synthesis
A dual cobalt and photocatalysis system provides a way to assemble anilines from cyclohexanones and amines by progressively dehydrating the intermediate imine.
- Shashikant U. Dighe
- , Fabio Juliá
- & Daniele Leonori
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Article |
Vacancy-enabled N2 activation for ammonia synthesis on an Ni-loaded catalyst
Ammonia is synthesized using a dual-site approach, whereby nitrogen vacancies on LaN activate N2, which then reacts with hydrogen atoms produced over the Ni metal to give ammonia.
- Tian-Nan Ye
- , Sang-Won Park
- & Hideo Hosono
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Article |
Photoenzymatic enantioselective intermolecular radical hydroalkylation
A transformation in which an ‘ene’ reductase catalyses the visible-light-induced intermolecular radical hydroalkylation of alkenes gives carbonyl compounds with a remote stereocentre in high yield and enantioselectivity.
- Xiaoqiang Huang
- , Binju Wang
- & Huimin Zhao
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Article |
Desymmetrization of difluoromethylene groups by C–F bond activation
Enantioselective activation of a single C–F bond in a difluoromethylene group is achieved using a chiral transition metal catalyst and a fluorophilic activator.
- Trevor W. Butcher
- , Jonathan L. Yang
- & John F. Hartwig
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Article |
Accelerated discovery of CO2 electrocatalysts using active machine learning
Machine learning predicts Cu-Al electrocatalysts provide better efficiency and productivity than copper when using intermittent renewable electricity to convert carbon dioxide to useful chemicals and fuels.
- Miao Zhong
- , Kevin Tran
- & Edward H. Sargent
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Article |
An engineered PET depolymerase to break down and recycle plastic bottles
Computer-aided engineering produces improvements to an enzyme that breaks down poly(ethylene terephthalate) (PET) into its constituent monomers, which are used to synthesize PET of near-petrochemical grade that can be further processed into bottles.
- V. Tournier
- , C. M. Topham
- & A. Marty
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Article |
Copper-mediated synthesis of drug-like bicyclopentanes
A one-step, three-component radical coupling of [1.1.1]propellane by a photoredox reaction mediated by a copper catalyst produces drug-like bicyclopentanes.
- Xiaheng Zhang
- , Russell T. Smith
- & David W. C. MacMillan
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Article |
Synthesis of rare sugar isomers through site-selective epimerization
Various rare sugars that cannot be isolated from natural sources are synthesized using light-driven epimerization, a process which may find application in other synthetic scenarios.
- Yong Wang
- , Hayden M. Carder
- & Alison E. Wendlandt
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Article |
Lactonization as a general route to β-C(sp3)–H functionalization
Pd-catalysed β-C(sp3)–H lactonization of aliphatic acids enabled by a mono-N-protected β-amino acid and tert-butyl hydrogen peroxide is reported, achieving high β-position selectivity without the use of a directing group.
- Zhe Zhuang
- & Jin-Quan Yu
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Article |
Domino electroreduction of CO2 to methanol on a molecular catalyst
Individual cobalt phthalocyanine derivative molecules immobilized on carbon nanotubes effectively catalyse the electroreduction of CO2 to methanol via a domino process with high activity and selectivity and stable performance.
- Yueshen Wu
- , Zhan Jiang
- & Hailiang Wang
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Article |
Molecular tuning of CO2-to-ethylene conversion
Electrocatalytic reduction of CO2 over copper can be made highly selective by ‘tuning’ the copper surface with adsorbed organic molecules to stabilize intermediates for carbon-based fuels such as ethylene
- Fengwang Li
- , Arnaud Thevenon
- & Edward H. Sargent
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Article |
Site-specific allylic C–H bond functionalization with a copper-bound N-centred radical
A Cu-bound nitrogen-centred radical is used to control site-specific and enantioselective allylic C–H cyanations of molecules with synthetic and medicinal relevance, such as tri- and tetrasubstituted alkenes.
- Jiayuan Li
- , Zhihan Zhang
- & Guosheng Liu
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Letter |
Low-barrier hydrogen bonds in enzyme cooperativity
Structural and biophysical studies reveal that low-barrier hydrogen bonds enable long-range communication between the active sites of multimeric enzymes and synchronise catalysis.
- Shaobo Dai
- , Lisa-Marie Funk
- & Kai Tittmann
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Letter |
Design and evolution of an enzyme with a non-canonical organocatalytic mechanism
A hydrolytic enzyme with a non-canonical organocatalytic mechanism was generated by introducing Nδ-methylhistidine into a designed active site using engineered translation components, allowing optimization of enzyme performance using laboratory evolution.
- Ashleigh J. Burke
- , Sarah L. Lovelock
- & Anthony P. Green
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Letter |
A rigorous electrochemical ammonia synthesis protocol with quantitative isotope measurements
A protocol for the electrochemical reduction of nitrogen to ammonia enables isotope-sensitive quantification of the ammonia produced and the identification and removal of contaminants.
- Suzanne Z. Andersen
- , Viktor Čolić
- & Ib Chorkendorff
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Letter |
Molybdenum-catalysed ammonia production with samarium diiodide and alcohols or water
The molybdenum-catalysed reduction of nitrogen to ammonia is achieved under ambient conditions, using samarium(ii) diiodide in combination with either simple alcohols or water as the proton source.
- Yuya Ashida
- , Kazuya Arashiba
- & Yoshiaki Nishibayashi
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Letter |
Site-selective and versatile aromatic C−H functionalization by thianthrenation
A highly site-selective aromatic C–H functionalization reaction that does not require a particular directing group or arene substitution pattern provides functionalized arenes that can participate in various transformations.
- Florian Berger
- , Matthew B. Plutschack
- & Tobias Ritter
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Letter |
Atomically dispersed iron hydroxide anchored on Pt for preferential oxidation of CO in H2
Atomically dispersed iron hydroxide deposited on silica-supported platinum nanoparticles enables complete and selective carbon monoxide removal through preferential oxidation in hydrogen in the temperature range from 198 to 380 kelvin.
- Lina Cao
- , Wei Liu
- & Junling Lu
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Letter |
Deacylative transformations of ketones via aromatization-promoted C–C bond activation
Aromatization-driven C–C bond activation through iridium/phosphine catalysis enables deacylative transformations in various ketone substrates.
- Yan Xu
- , Xiaotian Qi
- & Guangbin Dong
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Letter |
Photoredox catalysis using infrared light via triplet fusion upconversion
Photoredox transformations are achieved with infrared light by using triplet fusion upconversion that converts infrared into visible light, enabling the use of photoredox chemistry on larger scales and through barriers that are impenetrable by visible light.
- Benjamin D. Ravetz
- , Andrew B. Pun
- & Luis M. Campos
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Letter |
Enzymatic assembly of carbon–carbon bonds via iron-catalysed sp3 C–H functionalization
Evolved iron-containing enzymes based on cytochrome P450 achieve selective intermolecular alkylation of sp3 C–H bonds through a carbene C–H insertion strategy.
- Ruijie K. Zhang
- , Kai Chen
- & Frances H. Arnold
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Letter |
Desymmetrization of cyclohexanes by site- and stereoselective C–H functionalization
Unactivated cyclohexane derivatives can be desymmetrized by site- and stereoselective C–H functionalization using carbene-insertion chemistry.
- Jiantao Fu
- , Zhi Ren
- & Huw M. L. Davies
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Letter |
Base-free nickel-catalysed decarbonylative Suzuki–Miyaura coupling of acid fluorides
This nickel-catalysed Suzuki–Miyaura coupling of aryl boronic acids with in-situ-generated acid fluorides does not require an exogenous base and is applicable to a range of base-sensitive boronic acids and bioactive carboxylic acids.
- Christian A. Malapit
- , James R. Bour
- & Melanie S. Sanford
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Letter |
Catalytic enantioconvergent coupling of secondary and tertiary electrophiles with olefins
Nickel-catalysed coupling of racemic alkyl electrophiles and olefins in the presence of a hydrosilane is achieved with good enantioselectivity and yield under very mild reaction conditions.
- Zhaobin Wang
- , Haolin Yin
- & Gregory C. Fu
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Letter |
A protein functionalization platform based on selective reactions at methionine residues
This methionine-selective functionalization strategy uses hypervalent iodine reagents to introduce new groups via the formation of a sulfonium intermediate, which can then undergo further visible-light-mediated reactions to form a diverse range of protein conjugates.
- Michael T. Taylor
- , Jennifer E. Nelson
- & Matthew J. Gaunt
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Letter |
Multicomponent synthesis of tertiary alkylamines by photocatalytic olefin-hydroaminoalkylation
Complex tertiary alkylamines are prepared in one step from readily available amines, carbonyls and alkenes, via the visible-light-mediated reduction of in-situ-generated iminium ions to form alkyl-substituted α-amino radicals.
- Aaron Trowbridge
- , Dominik Reich
- & Matthew J. Gaunt
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Letter |
Cooperative asymmetric reactions combining photocatalysis and enzymatic catalysis
A cooperative chemoenzymatic reaction combines photocatalytic alkene isomerization with enzymatic reduction to generate enantioenriched products in a stereoconvergent manner.
- Zachary C. Litman
- , Yajie Wang
- & John F. Hartwig
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Letter |
Enantioselective remote meta-C–H arylation and alkylation via a chiral transient mediator
Remote, enantioselective C–H activation reactions can be achieved by relaying ortho-C–H activation to the meta position, using a chiral norbornene as the mediator.
- Hang Shi
- , Alastair N. Herron
- & Jin-Quan Yu
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Letter |
Velocity-resolved kinetics of site-specific carbon monoxide oxidation on platinum surfaces
The catalytic oxidation of carbon monoxide over platinum proceeds through two distinct channels: it is dominated at low temperatures by the more active step sites and at high temperatures by the more abundant terrace sites of the platinum surface.
- Jannis Neugebohren
- , Dmitriy Borodin
- & Theofanis N. Kitsopoulos
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Article |
Quaternary stereocentres via an enantioconvergent catalytic SN1 reaction
Cooperation between a chiral hydrogen-bond-donor catalyst and a strong Lewis-acid promoter in an SN1-type reaction mediates the formation of tertiary carbocations and enables control over enantioselectivity and product distribution.
- Alison E. Wendlandt
- , Prithvi Vangal
- & Eric N. Jacobsen
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Letter |
Palladium-catalysed electrophilic aromatic C–H fluorination
An approach for the direct electrophilic C–H fluorination of arenes is reported, using a palladium catalyst and mild fluorinating reagents.
- Kumiko Yamamoto
- , Jiakun Li
- & Tobias Ritter
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Review Article |
Enhancing the potential of enantioselective organocatalysis with light
This Review discusses recent developments in the combination of organocatalysis and photochemistry for the activation of molecules, which has enabled previously inaccessible reaction pathways and influenced many fields of chemical research.
- Mattia Silvi
- & Paolo Melchiorre
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Article |
Synthesis of E- and Z-trisubstituted alkenes by catalytic cross-metathesis
An approach for the synthesis of E- and Z- trisubstituted alkenes in high stereoisomeric purity is developed by merging catalytic cross-metathesis and cross-coupling processes.
- Thach T. Nguyen
- , Ming Joo Koh
- & Amir H. Hoveyda
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Letter |
Mild oxidation of methane to methanol or acetic acid on supported isolated rhodium catalysts
Single-site isolated rhodium species anchored on zeolites or titanium dioxide are shown to catalyse the direct conversion of methane to methanol and acetic acid, using oxygen and carbon monoxide under mild conditions.
- Junjun Shan
- , Mengwei Li
- & Maria Flytzani-Stephanopoulos
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Letter |
Site-selective and stereoselective functionalization of non-activated tertiary C–H bonds
The functionalization of specific inert C–H bonds avoids the need for functional groups in organic synthesis and here the challenges of this approach are overcome using a dirhodium catalyst that is capable of C–H bond site-selectivity.
- Kuangbiao Liao
- , Thomas C. Pickel
- & Huw M. L. Davies
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Letter |
Ligand-accelerated non-directed C–H functionalization of arenes
Using a ligand as a promoter enhances the reactivity of the palladium catalyst in non-directed C–H functionalization of arenes, enabling the arene to be used as the limiting reagent.
- Peng Wang
- , Pritha Verma
- & Jin-Quan Yu
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Letter |
Direct instrumental identification of catalytically active surface sites
Scanning tunnelling microscopy is used to distinguish between different active sites of a catalyst—such as boundaries between different materials—during a reaction, allowing the contributions of these sites to be evaluated.
- Jonas H. K. Pfisterer
- , Yunchang Liang
- & Aliaksandr S. Bandarenka
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Letter |
Visible-light-driven methane formation from CO2 with a molecular iron catalyst
An iron tetraphenylporphyrin complex is shown to catalyse the reduction of carbon dioxide to methane upon visible light irradiation at ambient temperature and pressure.
- Heng Rao
- , Luciana C. Schmidt
- & Marc Robert
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Letter |
Remote carboxylation of halogenated aliphatic hydrocarbons with carbon dioxide
A nickel catalyst that promotes carboxylation of halogenated hydrocarbons at remote aliphatic sites with carbon dioxide via tunable and controllable chain-walking is described.
- Francisco Juliá-Hernández
- , Toni Moragas
- & Ruben Martin
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Letter |
Decarboxylative alkenylation
Starting with alkyl carboxylic acids, a simple olefin synthesis using any substitution pattern or geometry, based on amide-bond synthesis with nickel- or iron-based catalysis, is described.
- Jacob T. Edwards
- , Rohan R. Merchant
- & Phil S. Baran
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Review Article |
Exploiting non-covalent π interactions for catalyst design
Our increasing understanding of non-covalent interactions involving aromatic systems is reviewed, and the use of these insights in the design of small-molecule catalysts and enzymes is surveyed.
- Andrew J. Neel
- , Margaret J. Hilton
- & F. Dean Toste
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Letter |
Low-temperature hydrogen production from water and methanol using Pt/α-MoC catalysts
As an alternative vehicle fuel, hydrogen can be generated in situ from methanol and water—a process that is shown here to occur under mild conditions using a catalyst that comprises platinum atomically dispersed on an α-molybdenum carbide substrate.
- Lili Lin
- , Wu Zhou
- & Ding Ma
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Letter |
Molybdenum chloride catalysts for Z-selective olefin metathesis reactions
Substitution of a ligand in molybdenum-based complexes enables typically inert hexafluorobutene to participate in Z-selective olefin cross-metathesis reactions.
- Ming Joo Koh
- , Thach T. Nguyen
- & Amir H. Hoveyda
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Letter |
High-spatial-resolution mapping of catalytic reactions on single particles
The chemical conversion of N-heterocyclic carbene molecules attached to catalytic particles is monitored at high spatial resolution using synchrotron-radiation-based infrared nanospectroscopy.
- Chung-Yeh Wu
- , William J. Wolf
- & Elad Gross
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Letter |
Kinetically E-selective macrocyclic ring-closing metathesis
Ring-closing metathesis is a widely used chemical transformation that can generate organic macrocycle compounds; here, an approach is described by which the E-stereoisomer of a macrocycle is generated selectively, exemplified by synthesizing the antibiotic recifeolide and the anti-cancer drug pacritinib.
- Xiao Shen
- , Thach T. Nguyen
- & Amir H. Hoveyda
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Letter |
Catalyst support effects on hydrogen spillover
The mechanism of hydrogen spillover is described using a precisely nanofabricated model system, explaining why it is slower on an aluminum oxide catalyst support than on a titanium oxide catalyst support.
- Waiz Karim
- , Clelia Spreafico
- & Jeroen A. van Bokhoven
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Letter |
Accessing non-natural reactivity by irradiating nicotinamide-dependent enzymes with light
hotoexcitation of a catalytic enzyme enzyme’s co-factor is shown to change the reactivity of the enzyme, enabling it to carry out a non-natural enantioselective dehalogenation of lactone molecules.
- Megan A. Emmanuel
- , Norman R. Greenberg
- & Todd K. Hyster
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Letter |
Catalytic activation of carbon–carbon bonds in cyclopentanones
In the chemical industry, it is often necessary to activate carbon–carbon bonds in order to synthesize complex organic molecules, but this is challenging when starting with simple five- or six-membered carbon rings; a new method uses a rhodium pre-catalyst and an amino-pyridine co-catalyst, enabling an overall energetically favourable reaction that involves activation of carbon–carbon bonds plus activation of carbon–hydrogen bonds.
- Ying Xia
- , Gang Lu
- & Guangbin Dong
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Letter |
Amide-directed photoredox-catalysed C–C bond formation at unactivated sp3 C–H bonds
The formation of carbon–carbon bonds is achieved via directed cleavage of traditionally non-reactive carbon–hydrogen bonds and their subsequent coupling with readily available alkenes.
- John C. K. Chu
- & Tomislav Rovis
Coupling dinitrogen and hydrocarbons through aryl migration