This work presents a generalizable computer vision (CV) and machine learning model that is used for automated real-time monitoring and control of a diverse array of workup processes. Our system simultaneously monitors multiple physical outputs (e.g., liquid level, homogeneity, turbidity, solid, residue, and color), offering a method for rapid data acquisition and deeper analysis from multiple visual cues. We demonstrate a single platform (consisting of CV, machine learning, real-time monitoring techniques, and flexible hardware) to monitor and control vision-based experimental techniques, including solvent exchange distillation, antisolvent crystallization, evaporative crystallization, cooling crystallization, solid–liquid mixing, and liquid–liquid extraction. Both qualitative (video capturing) and quantitative data (visual outputs measurement) were obtained which provided a method for data cross-validation. Our CV model's ease of use, generalizability, and non-invasiveness make it an appealing complementary option to in situ and real-time analytical monitoring tools and mathematical modeling. Additionally, our platform is integrated with Mettler-Toledo's iControl software, which acts as a centralized system for real-time data collection, visualization, and storage. With consistent data representation and infrastructure, we were able to efficiently transfer the technology and reproduce results between different labs. This ability to easily monitor and respond to the dynamic situational changes of the experiments is pivotal to enabling future flexible automation workflows.

Ordered M1Zn1 intermetallic phases with structurally isolated atom sites offer unique electronic and geometric structures for catalytic applications, but lack reliable industrial synthesis methods that avoid forming a disordered alloy with ill-defined composition. We developed a facile strategy for preparing well-defined M1Zn1 intermetallic nanoparticle (i-NP) catalysts from physical mixtures of monometallic M/SiO2 (M = Rh, Pd, Pt) and ZnO. The Rh1Zn1 i-NPs with structurally isolated Rh atom sites had a high intrinsic selectivity to ethylene (91%) with extremely low C4 and oligomer formation, outperforming the reported intermetallic and alloy catalysts in acetylene semihydrogenation. Further studies revealed that the M1Zn1 phases were formed in situ in a reducing atmosphere at 400 °C by a Zn atom emitting–trapping–ordering (Zn-ETO) mechanism, which ensures the high phase-purity of i-NPs. This study provides a scalable and practical solution for further exploration of Zn-based intermetallic phases and a new strategy for designing Zn-containing catalysts.

Correction for ‘A high affinity pan-PI3K binding module supports selective targeted protein degradation of PI3Kα’ by Werner Theodor Jauslin et al., Chem. Sci., 2024, https://doi.org/10.1039/D3SC04629J.

In this study, we employed a 3d metal complex as a catalyst to synthesize alkenyl boronate esters through the dehydrogenative coupling of styrenes and pinacolborane. The process generates hydrogen gas as the sole byproduct without requiring an acceptor, rendering it environmentally friendly and atom-efficient. This methodology demonstrated exceptional selectivity for dehydrogenative borylation over direct hydroboration. Additionally, it exhibited a preference for borylating aromatic alkenes over aliphatic ones. Notably, derivatives of natural products and bioactive molecules successfully underwent diversification using this approach. The alkenyl boronate esters served as precursors for the synthesis of various pharmaceuticals and potential anticancer agents. Our research involved comprehensive experimental and computational studies to elucidate the reaction pathway, highlighting the B–H bond cleavage as the rate-determining step. The catalyst's success was attributed to the hemilability and metal–ligand bifunctionality of the ligand backbone.

Electrocatalytic and thermocatalytic CO2 conversions provide promising routes to realize global carbon neutrality, and the development of corresponding advanced catalysts is important but challenging. Hollow-structured carbon (HSC) materials with striking features, including unique cavity structure, good permeability, large surface area, and readily functionalizable surface, are flexible platforms for designing high-performance catalysts. In this review, the topics range from the accurate design of HSC materials to specific electrocatalytic and thermocatalytic CO2 conversion applications, aiming to address the drawbacks of conventional catalysts, such as sluggish reaction kinetics, inadequate selectivity, and poor stability. Firstly, the synthetic methods of HSC, including the hard template route, soft template approach, and self-template strategy are summarized, with an evaluation of their characteristics and applicability. Subsequently, the functionalization strategies (nonmetal doping, metal single-atom anchoring, and metal nanoparticle modification) for HSC are comprehensively discussed. Lastly, the recent achievements of intriguing HSC-based materials in electrocatalytic and thermocatalytic CO2 conversion applications are presented, with a particular focus on revealing the relationship between catalyst structure and activity. We anticipate that the review can provide some ideas for designing highly active and durable catalytic systems for CO2 valorization and beyond.

Dynamic covalent synthesis aims to precisely control the assembly of simple building blocks linked by reversible covalent bonds to generate a single, structurally complex, product. In recent years, considerable progress in the programmability of dynamic covalent systems has enabled easy access to a broad range of assemblies, including macrocycles, shape-persistent cages, unconventional foldamers and mechanically-interlocked species (catenanes, knots, etc.). The reversibility of the covalent linkages can be either switched off to yield stable, isolable products or activated by specific physico-chemical stimuli, allowing the assemblies to adapt and respond to environmental changes in a controlled manner. This activatable dynamic property makes dynamic covalent assemblies particularly attractive for the design of complex matter, smart chemical systems, out-of-equilibrium systems, and molecular devices.

Zero-dimensional (0D) hybrid metal halides have emerged as highly efficient luminescent materials, but integrated multifunction in a structural platform remains a significant challenge. Herein, a new hybrid 0D indium halide of (Im-BDMPA)InCl6·H2O was designed as a highly efficient luminescent emitter and X-ray scintillator toward multiple optoelectronic applications. Specifically, it displays strong broadband yellow light emission with near-unity photoluminescence quantum yield (PLQY) through Sb3+ doping, acting as a down-conversion phosphor to fabricate high-performance white light emitting diodes (WLEDs). Benefiting from the high PLQY and negligible self-absorption characteristics, this halide exhibits extraordinary X-ray scintillation performance with a high light yield of 55 320 photons per MeV, which represents a new scintillator in 0D hybrid indium halides. Further combined merits of a low detection limit (0.0853 μGyair s−1), ultra-high spatial resolution of 17.25 lp per mm and negligible afterglow time (0.48 ms) demonstrate its excellent application prospects in X-ray imaging. In addition, this 0D halide also exhibits reversible luminescence off–on switching toward tribromomethane (TBM) but fails in any other organic solvents with an ultra-low detection limit of 0.1 ppm, acting as a perfect real-time fluorescent probe to detect TBM with ultrahigh sensitivity, selectivity and repeatability. Therefore, this work highlights the multiple optoelectronic applications of 0D hybrid lead-free halides in white LEDs, X-ray scintillation, fluorescence sensors, etc.

Correction for ‘When SF5 outplays CF3: effects of pentafluorosulfanyl decorated scorpionates on copper’ by Anurag Noonikara-Poyil et al., Chem. Sci., 2021, 12, 14618–14623, https://doi.org/10.1039/D1SC04846E.

Correction for ‘Synthetic ramoplanin analogues are accessible by effective incorporation of arylglycines in solid-phase peptide synthesis’ by Edward Marschall et al., Chem. Sci., 2024, 15, 195–203, https://doi.org/10.1039/D3SC01944F.

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Liquid metals have recently emerged as promising catalysts that can outcompete their solid counterparts for many reactions. Although theoretical modelling is extensively used to improve solid-state catalysts, there is currently no way to capture the interactions of adsorbates with a dynamic liquid metal. We propose a new approach based on ab initio molecular dynamics sampling of an adsorbate on a liquid catalyst. Using this approach, we describe time-resolved structures for formate adsorbed on liquid Ga–In, and for all intermediates in the methanol oxidation pathway on Ga–Pt. This yields a range of accessible adsorption energies that take into account the at-temperature motion of the liquid metal. We find that a previously proposed pathway for methanol oxidation on Ga–Pt results in unstable intermediates on a dynamic liquid surface, and propose that H desorption must occur during the path. The results showcase a more accurate way to treat liquid metal catalysts in this emerging field.

The existence of the oxidation/reduction interface can promote the performance of a photocatalyst, due to its effect on the separation of photogenerated carriers and the surface reactivity. However, it is difficult to construct two sets of oxidation/reduction interfaces in a single crystal and compare their separation efficiency for photogenerated carriers. Introducing a high proportion of active facets into the co-exposed facets is even more challenging. Herein, a hollow anatase TiO2 tetrakaidecahedron (HTT) with two sets of oxidation/reduction interfaces ({001}/{101} and {001}/{110}) is synthesized by directional chemical etching. Theoretical and experimental results indicate that the {001}/{110} interface is a dominant oxidation/reduction interface, showing a better promotion on the separation of photogenerated carriers than the {001}/{101} interface. In the HTT, the ratio of dominant {001}/(110) is increased and the proportion of the active {110} facet is about 40% (generally about 15%). Therefore, the HTT shows excellent catalytic activity for photocatalytic reductive (hydrogen production) and oxidative (selective oxidation of sulfides) reactions. The HTT also demonstrates favorable photocatalytic activity for the cross-dehydrogenative coupling reaction, where both photogenerated electrons and photogenerated holes are involved, further verifying its high separation efficiency of photogenerated carriers and surface reactivity. This work provides an important guideline for developing advanced structures with a predetermined interface toward desired applications.

The methoxime group has emerged as a versatile directing group for a variety of C–H functionalizations. Despite its importance as a powerful functional handle, conversion of methoximes to the parent ketone, which is often desired, usually requires harsh and functional group intolerant reaction conditions. Therefore, the application of methoximes and their subsequent conversion to the corresponding ketone in a late-stage context can be problematic. Here, we present an alternative set of conditions to achieve mild and functional group tolerant conversion of methoximes to the parent ketones using photoexcited nitroarenes. The utility of this methodology is showcased in its application in the total synthesis of cephanolide D. Furthermore, mechanistic insight into this transformation obtained using isotope labeling studies as well as the analysis of reaction byproducts is provided.

Efficient and cost-effective electrocatalysts for the hydrogen oxidation/evolution reaction (HOR/HER) are essential for commercializing alkaline fuel cells and electrolyzers. The sluggish HER/HOR reaction kinetics in base is the key issue that requires resolution so that commercialization may proceed. It is also quite challenging to decrease the noble metal loading without sacrificing performance. Herein, we report improved HER/HOR activity as a result of hydrogen spillover on platinum-supported MoO3 (Pt/MoO3-CNx-400) with a Pt loading of 20%. The catalyst exhibited a decreased over-potential of 66.8 mV to reach 10 mA cm−2 current density with a Tafel slope of 41.2 mV dec−1 for the HER in base. The Pt/MoO3-CNx-400 also exhibited satisfactory HOR activity in base. The mass-specific exchange current density of Pt/MoO3-CNx-400 and commercial Pt/C are 505.7 and 245 mA mgPt−1, respectively. The experimental results suggest that the hydrogen binding energy (HBE) is the key descriptor for the HER/HOR. We also demonstrated that the enhanced HER/HOR performance was due to the hydrogen spillover from Pt to MoO3 sites that enhanced the Volmer/Heyrovsky process, which led to high HER/HOR activity and was supported by the experimental and theoretical investigations. The work function value of Pt [Φ = 5.39 eV) is less than that of β-MoO3 (011) [Φ = 7.09 eV], which revealed the charge transfer from Pt to the β-MoO3 (011) surface. This suggested the feasibility of hydrogen spillover, and was further confirmed by the relative hydrogen adsorption energy [ΔGH] at different sites. Based on these findings, we propose that the H2O or H2 dissociation takes place on Pt and interfaces to form Pt–Had or (Pt/MoO3)–Had, and some of the Had shifted to MoO3 sites through hydrogen spillover. Then, Had at the Pt and interface, and MoO3 sites reacted with H2O and HO− to form H2 or H2O molecules, thereby boosting the HER/HOR activity. This work may provide valuable information for the development of hydrogen-spillover-based electrocatalysts for use in various renewable energy devices.

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Organic small molecules exhibiting both thermally activated delayed fluorescence (TADF) and wide-ranging piezochromism (Δλ > 150 nm) in the near-infrared region have rarely been reported in the literature. We present three emitters MeTPA-BQ, tBuTPA-BQ and TPPA-BQ based on a hybrid acceptor, benzo[g]quinoxaline-5,10-dione, that emit via TADF, having photoluminescence quantum yields, ΦPL, of 39–42% at photoluminescence (PL) maxima, λPL, of 625–670 nm in 2 wt% doped films in 4,4′-bis(N-carbazolyl)-1,1′-biphenyl (CBP). Despite their similar chemical structures, the PL properties in the crystalline states of MeTPA-BQ (λem = 735 nm, ΦPL = 2%) and tBuTPA-BQ (λem = 657 nm, ΦPL = 11%) are significantly different. Further, compounds tBuTPA-BQ and TPPA-BQ showed a significant PL shift of ∼98 and ∼165 nm upon grinding of the crystalline samples, respectively. Deep-red organic light-emitting diodes with MeTPA-BQ and tBuTPA-BQ were also fabricated, which showed maximum external quantum efficiencies, EQEmax, of 10.1% (λEL = 650 nm) and 8.5% (λEL = 670 nm), respectively.

Hydroxyapatite-based materials have been widely used in countless applications, such as bone regeneration, catalysis, air and water purification or protein separation. Recently, much interest has been given to controlling the aspect ratio of hydroxyapatite crystals from bulk samples. The ability to exert control over the aspect ratio may revolutionize the applications of these materials towards new functional materials. Controlling the shape, size and orientation of HA crystals allows obtaining high aspect ratio structures, improving several key properties of HA materials such as molecule adsorption, ion exchange, catalytic reactions, and even overcoming the well-known brittleness of ceramic materials. Regulating the morphogenesis of HA crystals to form elongated oriented fibres has led to flexible inorganic synthetic sponges, aerogels, membranes, papers, among others, with applications in sustainability, energy and catalysis, and especially in the biomedical field.

Developing accurate tumor-specific molecular imaging approaches holds great potential for evaluating cancer progression. However, traditional molecular imaging approaches still suffer from restricted tumor specificity due to the “off-tumor” signal leakage. In this work, we proposed light and endogenous APE1-triggered plasmonic antennas for accurate tumor-specific subcellular molecular imaging with enhanced spatial resolution. Light activation ensures subcellular molecular imaging and endogenous enzyme activation ensures tumor-specific molecular imaging. In addition, combined with the introduction of plasmon enhanced fluorescence (PEF), off-tumor signal leakage at the subcellular level was effectively reduced, resulting in the significantly enhanced discrimination ratio of tumor/normal cells (∼11.57-fold) which is better than in previous reports, demonstrating great prospects of these plasmonic antennas triggered by light and endogenous enzymes for tumor-specific molecular imaging at the subcellular level.