Articles in 2023

Elucidating the origin of light-induced reaction rate enhancement in plasmonic photocatalysis is very challenging. Now, bimetallic supercrystals are reported to boost photocatalytic hydrogen evolution from formic acid with the sole aid of intensified electric fields.

Iron–nitrogen–carbon (FeNC) catalysts are a viable alternative to platinum, but still lack the necessary performance. Now, pyrolysis under forming gas is found as a path to boosting their site density, activity and durability.

Enantioselective synthesis of chiral cyclobutanes via direct cycloaddition of C–C single bonds with C=C double bonds has remained an unmet challenge. Now, a photoelectrocatalytic system enabling asymmetric dehydrogenative [2+2] cycloaddition of alkyl ketones and alkenes has been developed.

With climate change concerns deepening, CO₂ fixation pathways to produce value-added chemicals are currently of interest. Now, synthetic biology and machine learning help developing such a pathway across modules that have been tested in vivo in Escherichia coli for the production of acetyl coenzyme A.

The search for novel biocatalysts for plastic degradation has recently become a hot topic. Now, multiple catalytic triads of well-known serine esterases were introduced into non-catalytic protein nanopores to enable the hydrolysis of PET nanoparticles.

Electrification offers a means to decarbonize the chemical industry. In this Editorial we reflect on opportunities in the area of catalysis that come with an increasing availability of renewable electricity.

Electrocatalytic NO_x reduction (NO_xR) to ammonia has recently become an increasingly popular alternative to the more challenging N₂ reduction. This Perspective critically assesses the possible ways NO_xR could contribute to the ammonia economy and clarifies the necessary steps for a rigorous experimental protocol.

Direct CO₂-to-C₂₊ and tandem CO₂-to-CO and CO-to-C₂₊ electrocatalytic systems have been proposed as strategies for sustainable fuel and chemical synthesis. This Perspective considers the role of acidic CO₂ gas on the cathodic microenvironment and local pH and draws connections between this and product selectivity in the electrochemical CO₂ reduction reaction and the electrochemical CO reduction reaction, focusing on the competition between two major pathways: ethylene/ethanol and acetate.

Thanks to a unique set of properties, liquid metal catalysts provide advantages compared to traditional solid systems, yet their potential in heterogeneous catalysis has not been fully explored. This Perspective identifies some of the key advances in the field of liquid metal catalysis, discussing areas where progress is expected through further fundamental understanding as well as reactor engineering.

Few synthetic CO₂-fixation pathways have been tested in vivo. Now, the new-to-nature THETA cycle is designed, realized in vitro and modular implemented in vivo. This cycle involves 17 enzymes, including the two most active carboxylases known so far, to produce the central building block acetyl-CoA using CO₂.

Merging photoredox and biocatalysis provides opportunities to address challenges in synthetic chemistry. Now the combination of a ruthenium photocatalyst for oxidative radical formation and ‘ene’-reductases for radical interception enables an enantiodivergent decarboxylative alkylation reaction.

Chiral lactams are important pharmacophores and strategies for their synthesis through direct C–H functionalization are highly sought after. Now, intramolecular C–H amidation of dioxazolones via biocatalytic nitrene transfer enables the synthesis of enantioenriched lactams with various ring sizes.

Low-carbon chemicals generated from CO₂ provide a possible path to improve the sustainability of microbial bioproduction of food and chemicals. Now, using a metabolic engineering approach, yeast is engineered to produce glucose, myo-inositol, glucosamine, sucrose and starch from C_1–3 molecules.

Fe–N–C catalysts are a promising alternative to precious metals in fuel cell cathodes, but they suffer from durability issues. Now, a preparation method is reported that allows increasing the active site density while also improving durability.

Plasmonic composites have potential for photocatalytic conversions using solar light; however, complex interactions between light and the components are poorly understood. Here, a highly ordered two-dimensional plasmonic bimetallic AuPt supercrystal demonstrates a high rate of H₂ generation from formic acid while providing insight into the interaction between plasmonic antenna and catalyst.