Chem Catalysis

Online Now: High-efficiency plasma reforming of CO2-rich natural gas using rotating arc #catalysis

Online Now: Selenide-based catalysts containing platinum-group metals for electrochemical applications #catalysis

Bismuth-based catalysts for #electrocatalytic CO2 reduction to formate in aqueous media This review highlights key strategies to develop efficient bismuth-based electrocatalysts and attempts to build effective electrochemical systems with them, giving a comprehensive presentation of this representative type of formic acid-production catalyst from the fundamental mechanistic advances to their industrial implementation potential, which offers insights into advancing CO2-to-HCOOH conversion toward carbon-neutral technologies.

Online Now: Bismuth-based catalysts for #electrocatalytic CO2 reduction to formate in aqueous media #catalysis

Techno-economic assessment of non-aqueous CO2 reduction CO2 reduction is typically carried out in aqueous electrolytes. Non-aqueous systems can suppress hydrogen evolution but increase cell voltages. This techno-economic assessment of non-aqueous CO2 reduction shows that oxalic acid, a two-electron product, could be commercially viable via this process. Oxalic acid would cost $2.87/kg at small scale and $1.56/kg at commercial scale, near current market prices. This levelized cost is dominated by product separation, stack replacement, and electricity costs. We also propose a technical roadmap toward cost-competitive non-aqueous CO2R.

Online Now: Techno-economic assessment of non-aqueous CO2 reduction #catalysis

Pressure-pulsed flow triples mass transport in aqueous CO2 electrolysis CO2 electrolysis in fully aqueous conditions is currently strongly limited by mass transport of CO2. Fast pressure pulses enhance the mass transport of CO2 substantially, reaching partial current densities >80 mA/cm2. We find that this is due to both vibration of gas bubbles and flow oscillations.

Online Now: Pressure-pulsed flow triples mass transport in aqueous CO2 electrolysis #catalysis

Covalent organic frameworks with protonation control for selective photocatalytic nitroaromatic reduction This work provides a fundamental advance in controlling #catalytic selectivity through precise microenvironment engineering rather than relying on precious metals. By simply protonating a covalent organic framework, we achieved near-perfect selectivity for a previously elusive chemical transformation under mild, sustainable conditions. This strategy of tailoring the catalyst’s electronic environment to guide reaction pathways is a powerful and generalizable concept that can be applied to overcome long-standing challenges in synthetic chemistry and catalysis.

Online Now: Covalent organic frameworks with protonation control for selective photocatalytic nitroaromatic reduction #catalysis

Kinetic analysis of Fe leaching and stability in Fe–N–C catalysts during oxygen reduction This work introduces a sequential decoupling-recoupling framework to model the degradation of Fe–N–C catalysts under operation conditions. By quantifying iron leaching kinetics and proposing dual-atom stabilization strategies, the work bridges atomic-scale mechanisms with macroscopic durability, providing design principles for durable and active electrocatalysts.

Online Now: Kinetic analysis of Fe leaching and stability in Fe–N–C catalysts during oxygen reduction #catalysis

Affinity-induced upcycling of palladium nanoclusters in COF membranes for #catalytic water treatment This study proposes a strategy for recovering palladium into covalent organic framework membranes for #catalytic water treatment. The resulting #catalytic membranes loaded with Pd nanoclusters demonstrate excellent sieving of organic pollutants and high #catalytic activity. The work presents a versatile platform for creating highly active and stable #catalytic membranes for advanced water treatment.

Online Now: Affinity-induced upcycling of palladium nanoclusters in COF membranes for #catalytic water treatment #catalysis

Intermediate regulation strategies in tandem #electrocatalysis for small-molecule conversion Electrochemical tandem catalysis relies on the precise regulation of intermediates to achieve efficient small-molecule conversion. This review highlights the pivotal roles of ∗CO, ∗NO2−, ∗H, and ∗NH2 in CO2 reduction, NO3− reduction, and C–N coupling. By correlating intermediate pathways with catalyst-design strategies, we provide mechanistic insights and guidance for developing advanced tandem systems toward sustainable energy and green-chemical production.

Online Now: Intermediate regulation strategies in tandem #electrocatalysis for small-molecule conversion #catalysis

Electrochemical benzaldehyde carboxylation for sustainable mandelic acid synthesis via radical intermediates This work looked at the sustainable synthesis of mandelic acid—an important precursor in the synthesis of pharmaceuticals and plastics—via electrochemical coupling of benzaldehyde and CO2. After optimization of reaction parameters to maximize selectivity and efficiency, mechanistic analysis was performed using spectroscopic and electrochemical methods. The reaction was determined to proceed via a ketyl radical intermediate. Insights from this work not only inform future catalyst and reactor design efforts but can also be broadly applied toward related electrochemical syntheses.

Online Now: Electrochemical benzaldehyde carboxylation for sustainable mandelic acid synthesis via radical intermediates #catalysis

Non-leaching cerium oxide evolved from Laves phase enables iron-retentive oxygen evolution The surface of Laves-phase CeFe2 intermetallics transform into α-FeOOH during alkaline OER, creating a pseudo-periodic coupling with concurrently formed CeO2. This partial transformation stabilizes active Fe sites, inhibits particle aggregation, alters the electronic structure, and enhances charge-transfer ability, leading to significantly improved OER performance.

Online Now: Non-leaching cerium oxide evolved from Laves phase enables iron-retentive oxygen evolution #catalysis

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Integrating micelle catalysts with living cells for recyclable photoenzymatic cascades Through an efficient and non-covalent micelle-cell integration approach, charged polymeric micelles encapsulating the photocatalyst 2-hydroxymethyl anthraquinone were loaded onto the surface of benzaldehyde lyase-expressing E. coli. The micelle-coated cells retained enzymatic activity and enabled an efficient one-pot photoenzymatic cascade with high recyclability, thereby providing a versatile platform for sustainable chemoenzymatic bioconversions.

Online Now: Integrating micelle catalysts with living cells for recyclable photoenzymatic cascades #catalysis

Online Now: #catalytic resonance theory for parametric uncertainty of programmable catalysis #catalysis

Design of electrolyzers for sustainable H2O2 electrosynthesis This commentary discusses emerging electrolyzer designs—ranging from simple batch cells to flow-cell and solid-state systems—for H2O2 electrosynthesis via the two-electron oxygen reduction reaction. Particular emphasis is placed on innovations such as gas diffusion electrodes (GDEs), membrane-free configurations, bubble-shielding strategies, and solid electrolytes. This commentary offers a clear framework for rationalizing the design of next-generation H2O2 electrosynthesis systems.

Online Now: Design of electrolyzers for sustainable H2O2 electrosynthesis #catalysis

Hydroxyl anchoring and electron transfer behaviors of atomic single-layer Pt in NH3 oxidation Pt atomic single layers (ASLs) are valuable catalysts due to their interaction with support materials, such as Al2O3 and TiO2, which influences their efficiency and product outcomes. This study investigates how various attachment methods between Pt ASLs and supports impact NH3 oxidation. The research underscores a straightforward concept: adjusting the attachment of Pt ASLs to supports allows for customized catalyst performance. This approach is beneficial for designing more effective catalysts for reactions like NH3 oxidation.

Online Now: Hydroxyl anchoring and electron transfer behaviors of atomic single-layer Pt in NH3 oxidation #catalysis

Dual-polarity engineering breaks charge transfer kinetic balances to enhance H2O2-mediated nitrate photosynthesis from air Traditional fertilizer production is energy intensive. This work pioneers a sustainable, solar-powered method to synthesize nitrate fertilizer directly from air (N2 and O2) using water and light. By ingeniously designing a metal-free carbon-based catalyst with built-in “electron highways” and “hole superchannels,” we overcome a major hurdle—carrier imbalance—that plagues such reactions. This breakthrough enables simultaneous capture and conversion of atmospheric nitrogen and oxygen into nitrate with record efficiency, offering a promising green alternative to the energy-hungry Haber-Bosch process.

Online Now: Dual-polarity engineering breaks charge transfer kinetic balances to enhance H2O2-mediated nitrate photosynthesis from air #catalysis

Access to chiral spiroketals via #catalytic enantioselective halogenation of racemic olefinic hemiketals We report an enantio- and diastereoselective synthesis of bromo-spiroketals via #catalytic asymmetric halocyclization of racemic olefinic hemiketals. A cross-assembled bifunctional catalyst system, comprising a chiral phosphoric acid and an achiral quinoline base, enables satisfactory stereocontrol. The resulting bromo-spiroketals serve as versatile precursors for late-stage functionalization into spiroketal diphosphine ligands, useful in metal-catalyzed asymmetric transformations.

Online Now: Access to chiral spiroketals via #catalytic enantioselective halogenation of racemic olefinic hemiketals #catalysis

Breaking the conversion-selectivity trade-off through a plasma reaction-separation coupling process Plasma for the selective oxidation of methane allows for the generation of more oxygenate compounds than the traditional selective oxidation of methane. Coupling the high-space-velocity cyclic process with plasma technology can further increase the yield of liquid fuel and reduce the formation of the overoxidation product CO2. This advancement strengthens the economic viability of plasma for the selective oxidation of methane for industrial applications.

Online Now: Breaking the conversion-selectivity trade-off through a plasma reaction-separation coupling process #catalysis

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Designing ionomers to control water content for low-voltage ethylene production from CO2 electrolysis Tunable quaternary ammonium ionomers show that the water content of ionomers steers the selectivity of ethylene for CO2 electrolysis in a Cu-based system. By combining tailored polymer chemistry, electrochemical experiments, and continuum modeling, we can understand how water uptake at different current densities can boost C2+ selectivity while keeping the cell voltage low.

Online Now: Designing ionomers to control water content for low-voltage ethylene production from CO2 electrolysis #catalysis

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Divergent contiguous stereocenters via asymmetric conjugate additions to cycloalkenyl ketones This study introduces a new, versatile chemical method for building complex ring-shaped molecules in one step with high precision. The approach works for crowded structures, where established techniques tend to fail, and could help speed up the discovery and development of new medicines.

Online Now: Divergent contiguous stereocenters via asymmetric conjugate additions to cycloalkenyl ketones #catalysis

#photocatalysis as a mechanistic probe for the Staudinger β-lactam synthesis The presence of high-energy zwitterionic intermediates is commonly postulated in many thermal transformations, with the Staudinger β-lactam synthesis being one of the most famous examples. Here, we demonstrate that, using triplet energy transfer catalysis, the same intermediates can be accessed indirectly, providing a powerful mechanistic probe for interrogating these species. Using a combination of experimental and computational methodologies, we were able to gain a deeper insight into the Staudinger β-lactam synthesis.

Online Now: #photocatalysis as a mechanistic probe for the Staudinger β-lactam synthesis #catalysis

Decoupling size and surface effects of intermetallic CuPd nanocrystals for #electrocatalytic nitrate reduction to ammonia Modulating the crystal structure, size, and morphology of CuPd nanocrystals reveals the critical role of the intermetallic CuPd (100) surface facet in catalyzing the conversion of nitrate to ammonia. This study offers key insights into structure-property relationships, advancing the design of nanocrystal catalysts for sustainable ammonia production and nitrogen-cycle remediation.

Online Now: Decoupling size and surface effects of intermetallic CuPd nanocrystals for #electrocatalytic nitrate reduction to ammonia #catalysis

Artificial-intelligence-enabled catalysis via standardized batch data This commentary advocates for advancing artificial intelligence (AI)-enabled catalysis research through improved data quality, the integration of multimodal data frameworks, and the implementation of closed-loop workflows by focusing on the importance of standardized batch data. Jiang et al. emphasize that such datasets are essential for building interpretable and transferable AI models that can accelerate catalyst discovery, enhance mechanistic understanding, and ultimately support the shift from intuition-driven to data-driven catalysis research.

Online Now: Artificial-intelligence-enabled catalysis via standardized batch data #catalysis

Photothermal reforming of polylactic acid plastics into pyruvic acid with 92.8% selectivity at S-scheme Ov-BiVO4/CdS heterostructures The developed Ov-BiVO4/CdS exhibits higher local charge accumulation on Bi sites, which enhances the energy barrier of Cα−CCOOH bond cleavage from −0.34 to 0.44 eV and lowers that of α-OH bonds in LA by transferring electrons to the C atoms, thus contributing to the generation of ⋅OR radicals. Induced by O vacancies, Ov-BiVO4/CdS shows a favorable photothermal effect that not only promotes the reaction kinetics but also facilitates the desorption of PA, thus suppressing its overoxidation.

Online Now: Photothermal reforming of polylactic acid plastics into pyruvic acid with 92.8% selectivity at S-scheme Ov-BiVO4/CdS heterostructures #catalysis

Enantioselective polymerization of racemic lactide for stereocomplex poly(lactic acid) Stereocomplex poly(lactic acid) (PLA)—a mixture of poly(l-lactic acid) and poly(d-lactic acid)—offers superior physico-mechanical properties over other degradable poly(lactic acid) forms. However, the direct synthesis of stereocomplex PLA from racemic lactide was previously impossible due to a lack of enantioselective catalysts. Chiral aluminum catalysts are developed to enable enantioselective polymerization of each enantiomer in racemic lactide through enantiomorphic-site control, thus allowing for the single-step production of stereocomplex PLA that is tougher and more ductile than poly(l-lactic acid) and conventionally blended stereocomplex PLA.

Online Now: Enantioselective polymerization of racemic lactide for stereocomplex poly(lactic acid) #catalysis

Accessing planar chiral ferrocenes via transient directing group-enabled C–H alkenylation under Pd(II) catalysis Ferrocene is an important skeleton widely used in catalysis, medicine, and materials. Planar chiral ferrocene derivatives are especially valuable but traditionally require extra steps to install and remove directing groups. In this work, we developed a transient directing strategy that enables efficient and selective synthesis of planar chiral ferrocenes without permanent modifications, offering a simpler and more effective route to complex chiral molecules.

Online Now: Accessing planar chiral ferrocenes via transient directing group-enabled C–H alkenylation under Pd(II) catalysis #catalysis

Controllable partial self-sacrifice of metal-organic frameworks for enhancing nitrate electroreduction to ammonia A controlled partial self-sacrifice strategy for metal-organic frameworks by leveraging the pronounced disparity in the coordination capacity of hybrid ligands and Cu nodes was designed. The resulting composite catalyst containing both ultrafine Cu2O and coordination-unsaturated Cu nodes exhibits superior electrochemical nitrate reduction to ammonia performance through the synergistic catalysis involving electron transfer from the electron-rich unsaturated Cu2+ nodes to the encapsulated nanoparticles.

Online Now: Controllable partial self-sacrifice of metal-organic frameworks for enhancing nitrate electroreduction to ammonia #catalysis