Jonas Wuyts

Science requires reproducibility. However, the replication crisis in medical, psychological, biological, and social sciences has revealed that satisfactory reproducibility is only achieved when it is measured, investigated, and critically discussed. Despite the inherent sensitivity and complexity of heterogeneous electrocatalysis, little is known about the reproducibility of its experimental protocols. Herein, we present a global interlaboratory study of nickel-iron-based oxygen evolution electrocatalysts, revealing substantial reproducibility challenges. Using a process characterization tool of the pharmaceutical industry, we identify that these reproducibility challenges originate from undescribed but critical process parameters. Finally, we discuss solution approaches to address electrocatalysis’ inherent experimental complexity without affecting academia’s explorative nature. This report sets a data-based foundation for a critical discussion of reproducibility and a following credibility revolution in heterogeneous catalysis research.

Mechanochemistry has become a powerful and sustainable approach in synthetic chemistry, yet the fundamental principles governing energy transfer during milling remain poorly understood. In particular, the trajectory of the milling ball has been largely overlooked in mechanistic studies. To address this, we employed high-speed recordings to precisely track ball motion, enabling accurate calculation of kinetic energies and their comparison with theoretical values. The use of hollow and solid balls of varying sizes further allowed us to disentangle the effects of altered trajectories in both the Finkelstein reaction and the direct mechanocatalyzed Suzuki coupling. This work underscores the critical importance of milling ball trajectory in mechanochemistry and highlights the need to consider this parameter in future mechanistic studies and in the development of optimized milling protocols.

Pt, Ni, and Pt–Ni/HY catalysts were prepared through mechanochemistry, without solvent. Upon optimization of the milling parameters, Pt–Ni/HY showed improved catalytic performance with less metal contents, which can be attributed to an improved metal distribution and interaction with the acid sites of HY zeolite.

Abstract

The global need to decrease CO₂ emissions led to the exploration of biomass-based fuels. However, the need to upgrade bio-oil through hydrodeoxygenation (HDO) reaction led to the search for more effective and environmentally sustainable bifunctional catalysts. Mechanochemistry, without any solvent, was chosen as a method to prepare metal-loaded (Pt, Ni, or both Pt–Ni) HY catalyst for the hydrodeoxygenation of guaiacol, which was used as model molecule. Under optimized milling conditions of 30 min and 200 rpm, the simultaneous addition of Pt and Ni allowed to reduce the metal contents when compared with solely Pt- or Ni-loaded catalysts, with improved catalytic performance for the hydrogenation of guaiacol. This can be attributed to the favorable effect of the mechanochemistry approach used to introduce the metallic function, reducing the size of zeolite clusters and promoting an effective metal dispersion, which is expected to favor the interactions of the metal sites with the more accessible acid sites in the zeolite.

Nature Chemistry, Published online: 04 September 2025; doi:10.1038/s41557-025-01922-9

Thomas Schlatzer and Véronique Gouverneur discuss why the chemistry of calcium fluoride is challenging, and how imaginative thinking based on fundamental principles can create positive change for the fluorochemical industry.

This mini review presents an overview on the catalytic conversion of plastic wastes toward value-added products and their original monomers. The most widely used plastics such as polyethylene (PE), polypropylene (PP) are chosen as the examples that converted to valuable products including cyclic hydrocarbons, liquid alkanes and gaseous olefins. Polyesters (PET), Nylon-6 (PA6), and poly bisphenol A carbonate (PC) are the representatives that depolymerized into their monomers.

Abstract

Plastic products have become integral to every facet of human life. However, the environmental pollution caused by plastic wastes has been an unavoidable problem nowadays. Catalytic depolymerization of plastic waste provides a sustainable and economic alternative to solve the environmental issue. Herein, we summarize different types of catalytic depolymerization based on the compositions and structures of plastics. One catalog is the conversion of plastics into monomers, i.e., polyethylene terephthalate, nylon, and polycarbonate. Then, we focus on the conversion of polyolefins to gaseous and liquid hydrocarbons, value-added products. Selective oxidation of polystyrene and transition to functional polymers are also discussed. Ongoing challenges and opportunities are discussed at the end of this review, in order to offer guidance for the synthesis of valuable products from plastic wastes as new feedstocks.

Nature Communications, Published online: 28 August 2025; doi:10.1038/s41467-025-62409-2

Carbon dioxide is ubiquitous and is used in telomerization reactions with butadiene to create a monomer for polymer applications, but it is challenging to telomerize it with naturally occurring 1,3-dienes. Here the authors report a palladium-catalyzed telomerization reaction of carbon dioxide and isoprene.

A zeolite-catalyzed strategy enables size-selective monoacetalization of sugars and polyols in a single step by leveraging pore confinement to distinguish between mono- and multi-substituted species. This broadly applicable method avoids protection steps and excess reagents, opening new routes to bio-based amphiphiles with strong surface activity and hard-water resistance.

Abstract

Diol functionalization with acetals in carbohydrates and polyols is ubiquitously used in protection chemistry and in the manufacture of several platform chemicals. However, the selective functionalization of molecules where multiple acetalization reactions can occur typically involves multiple protection/deprotection steps. Here, we show that zeolites can be used to size-selectively acetalize sugars and polyols in a single step, and we demonstrate the potential of this approach for producing functional chemicals and materials. We show that high selectivity is dependent on effective pore confinement, which is achieved by a careful pairing of the substrate size and the zeolite morphology. This zeolite-catalyzed strategy exhibited consistently good-to-excellent yields (70%–95%) of novel polyol/sugar monoacetals, notably offering an easy route to bio-based amphiphiles. These resulting xylose-based surfactants exhibited similar or superior surface activity and, remarkably, hard-water resistance compared to their nonrenewable ethoxylated analogues, which illustrates the potential for practical applications of this approach.

Nature Synthesis, Published online: 17 July 2025; doi:10.1038/s44160-025-00839-y

The selectivity of a catalytic reaction is manipulated by straining a polymer support to which the catalyst is covalently bound. Enantioselective rhodium-catalysed hydrogenation of a series of 2-acetamidoacrylates is shown to increase with macroscopic strain, with enantiomeric ratios reaching twice their initial values.

A chlorine-modified ZrO₂ supported Pd catalyst (Pd-Cl/ZrO₂) has been designed and exhibited remarkable selectivity in the one-step catalytic hydroprocessing of lignin monomer oil and its model compound guaiacol to cyclohexanones under optimized conditions (200–240 °C, 2 MPa H₂, 430 ppm HCl), achieving a cyclohexanones yield of 34.3 wt%.

Abstract

Cyclohexanones, as critical biopolymer precursors, could be produced from lignin yet rarely reported due to the formidable challenge of simultaneously removing oxygen-containing functional groups (e.g., methoxy, hydroxyl) and achieving selective C═O bond retention during catalytic hydrogenation. Herein, we demonstrate a chlorine-modified ZrO₂ supported Pd catalyst (Pd-Cl/ZrO₂) efficiently converting lignin to cyclohexanones under optimized reaction conditions, based on poplar RCF (reductive catalytic fractionation) lignin oil. Notably, the addition of trace HCl enables the catalytic process to proceed under milder conditions (200 °C), achieving a cyclohexanones yield of 34.3 wt% (relative to lignin content in poplar biomass). The acidity (H⁺) from HCl promotes dehydroxylation of lignin oil. Moreover, studies on model compound guaiacol reveal that Cl species may partially block Pd to suppress aromatic ring hydrogenation and promote electron transfer from Pd to the ZrO₂ support, collectively promoting ketone yield. This study presents a novel catalytic approach for the efficient and selective conversion of lignin, advancing biorefineries toward the direct synthesis of ketone derivatives.

An Fe-N₃ single-atom catalyst embedded in nitrogen-doped hollow carbon spheres enables the electrochemical upcycling of polyethylene terephthalate (PET)-derived ethylene glycol into organosulfur compounds under ambient conditions. This sustainable process achieves >60% faradaic efficiency for hydroxymethanesulfonate formation, highlighting its potential in waste valorization and green carbon–sulfur (C─S) bond synthesis.

Abstract

Cycling and electrochemical upgrading of plastics present a sustainable approach to transforming waste into high-value chemicals, yet the focus has predominantly been on carbohydrate production, leaving the potential of organosulfur compounds largely unexplored. In this study, we introduced an efficient electrochemical strategy to convert polyethylene terephthalate (PET)-derived ethylene glycol (EG) into organosulfur compounds with high yields. A specially designed iron single-atom catalyst (SAC) supported on nitrogen-doped hollow carbon spheres (NHCS), which feature high catalytic activity of the Fe-N₃ motifs, was employed, which facilitates the C─C bond cleavage during EG oxidation, and generates formaldehyde (CH₂O) species. These intermediates subsequently react with S-containing nucleophiles, that is, SO₃ ²⁻, to form hydroxymethanesulfonate (HMS) via C─S bond formation. Our method achieves a remarkable faradaic efficiency of over 60% and an unprecedented production rate of 1800 µmol cm⁻² h⁻¹ for HMS. Additionally, we validate the use of PET as feedstock for C─S bond formation, achieving a considerable faradaic efficiency of over 25% and an unprecedented production rate of 900 µmol cm⁻² h⁻¹. Our approach promises to enhance sustainability and profitability in plastic value chain management and revolutionize the production of pharmaceuticals, textile chemicals, and agrochemicals.

Palladium supported on carbon nitride sheets was developed to decompose formic acid under mild conditions. The obtained results revealed a clear structure–activity relationship between the Pd-exposed crystallographic planes and the catalytic performance. This study evidences the potential of these catalytic systems for effective application of formic acid as an energy vector.

Abstract

Carbon nitride, C₃N₄, was synthesized through thermal polycondensation of melamine with varying temperature and time conditions. This approach represents a cost-effective, straightforward, and environmentally friendly synthetic method with lower energy consumption to obtain hierarchically structured carbon nitride. The resulting materials were subjected to comprehensive characterization to analyze their crystalline structure, textural properties, composition, and light absorption characteristics. To evaluate their catalytic potential, the supports were impregnated with different loadings of palladium (1, 5, and 10 wt%) as the active phase and tested in the decomposition of formic acid for hydrogen production in liquid phase at mild conditions. This study revealed that the structure and composition of the C₃N₄ were highly dependent on the degree of polycondensation, which in turn was influenced by the temperature and the thermal synthesis process. The most promising catalytic performance was achieved with a support prepared by decomposing melamine at 650 °C for 4 h, followed by impregnation with 10 wt% Pd. Furthermore, a mechanistic study was conducted using operando DRIFTS-MS to explore the plausible catalytic pathways for synthesizing formic acid via CO₂ hydrogenation using the aforementioned catalyst. This investigation highlights the potential of C₃N₄ as a support, further demonstrating its versatility in the circular economy of formic acid.

This work investigates the selective catalytic transfer hydrogenation (CTH) of muconic acid and muconates using ethanol as a hydrogen source. Here we provide the first system selective for hexenedioic acid (HDA) production via CTH, with RuCl₃ hydrate. A mechanistic investigation and reaction model are provided in the work, giving vital insights into this reaction toward a promising biobased compound.

Abstract

The hydrogenation of muconic acid (MA), a biobased platform molecule, offers a sustainable pathway to adipic acid (AA), a key industrial dicarboxylic acid. In this study, we explore the catalytic transfer hydrogenation (CTH) of muconic acid and muconates using ionic ruthenium complexes. Unlike previous approaches, our method aims to selectively hydrogenate MA toward the monounsaturated compound hexenedioic acid (HDA) or its ester. Alcohols (methanol and ethanol) are employed as a hydrogen donor, providing a safer and more moderate alternative to H₂ gas. Using hydrated RuCl₃ as the catalyst, the reaction successfully produces HDA, with no over-hydrogenation toward AA observed. The resulting product mixture comprises up to four different HDA isomers, which were all identified and distinguished by GC, GC-MS-FID, and ¹H-NMR methods. The trans-2 isomer was the most abundant, which was supported by mechanistic investigation using isotopically labeled experiments. A 2,5-hydrogenation mechanism following a monohydride reaction cycle could be suggested. Furthermore, a kinetic model is presented to provide a deeper understanding of the various reaction pathways.

Base-metal-catalyzed (Mn, Fe, Co, Ni, and Cu) transfer hydrogenation of unsaturated N-containing organic compounds (such as imines, N-heteroarenes, nitriles, carboxamides, and nitroaromatic compounds) allows access to a variety of synthetically valuable amines. This review highlights advances and challenges of such transformations with a focus on the substrate scope, selectivity, and mechanisms of catalytic reactions.

Abstract

Owing to the synthetic availability of imines, N-heteroarenes, nitriles, carboxamides, and nitroarenes, their catalytic hydrogenation is considered an attractive and atom-economical route to a diversity of amines, which find widespread applications specialty chemical industries. Although catalytic hydrogenation of unsaturated N-containing organic compounds with compressed H₂ gas is well-established, such transformations require expensive high-pressure equipment and have associated H₂ handling risks. In contrast, transfer hydrogenation protocols utilize nongaseous hydrogen sources, offering significant advantages in the operational cost and safety of transformations. Whereas many economical nonprecious metal catalysts have been described for efficient transfer hydrogenation of aldehydes and ketones, similar systems for selective transfer hydrogenation of unsaturated nitrogen-containing organic compounds have been developed relatively recently. This review aims to highlight current advances and challenges of base-metal-catalyzed (i.e., Mn, Fe, Co, Ni, and Cu) transfer hydrogenation of imines, N-heteroarenes, nitriles, nitro compounds, as well as carboxamides and related molecules to the corresponding amines. Mechanistic aspects of catalytic reactions, the substrate scope, and selectivity of the transformations are also discussed.

Nature, Published online: 09 July 2025; doi:10.1038/s41586-025-09184-8

An inventory of 16,325 known plastic chemicals, including >4,200 hazardous compounds, supports the development of safer plastics.

Self-driving laboratories (SDLs) have the potential to revolutionize chemical discovery and optimization, yet their widespread adoption remains limited by high costs, complex infrastructure, and limited accessibility. Here, we introduce RoboChem-Flex, a low-cost, modular self-driving laboratory platform designed to democratize autonomous chemical experimentation. The system combines customizable, in-house-built hardware with a flexible Python-based software framework that integrates real-time device control and advanced Bayesian optimization strategies, including multi-objective and transfer learning workflows. RoboChem-Flex supports both fully autonomous closed-loop operation and human-in-the-loop configurations, enabling seamless integration with shared analytical equipment and minimizing entry barriers. We validate the versatility of the platform across six diverse case studies, including photocatalysis, biocatalysis, thermal cross-couplings, and enantioselective catalysis, spanning both single and multi-objective optimizations. Through these campaigns, we demonstrate RoboChem-Flex’s ability to navigate large, complex chemical spaces, autonomously identify scalable high-performance reaction conditions, and flexibly adapt to a variety of analytical setups. By providing an affordable, scalable, and open platform, RoboChem-Flex offers a tangible step toward making SDLs accessible to resource-limited laboratories, fostering broader participation in automated chemical research.

Recent rapid developments in forest biomass valorisation have highlighted lignin as a key value driver for the economic sustainability of modern biorefining. Sugar-based biorefinery hydrolysis lignin (HL) from wood biomass has an immense potential as an alternative for fossil-based aromatic feedstock. However, impurities, heterogeneous structures and limited solubility in common solvents are the main challenges associated with HL functionalisation. Aqueous organic solvent fractionation represents a promising approach to improve on HL properties and subsequently increase its valorisation options. In this study, for the first time, biorefinery HL derived from birch was purified and fractionated with water-EtOH and -THF mixtures across the whole co-solvent concentration range at ambient temperature. The highest lignin solubility was achieved with 70 wt% THF mixture, which dissolved a remarkable 81 wt% of lignin available in HL. Moreover, fractionated lignin purity was further increased to 95 wt% when employing an extra water-washing step. In general, fractions soluble in THF mixtures had high dispersity, syringyl-to-guaiacyl (S/G) subunit ratio and aliphatic OH-groups, whereas EtOH fractions had narrower molecular weight distributions, lower S/G subunit ratio and higher concentration of phenolic OH-groups. A brief description of the solvent effects at the molecular level was given using molecular dynamics simulations which revealed specific solvation between the dissolved lignin and solvent mixture. Protocol presented in this paper enables to purify HL and control the physicochemical properties of the soluble lignin fractions by simply altering the composition of the solvent mixture, and therefore, expanding the possibilities in valorisation of HL.

Nature Chemistry, Published online: 23 June 2025; doi:10.1038/s41557-025-01863-3

Synthetic and biological chemistry are traditionally seen as separate fields. Now, a biocompatible chemical reaction enables an engineered microbe to convert plastic waste into valuable compounds under mild, cell-friendly conditions.