Chem by Cell Press

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Proton-coupled electrochemical reduction of a phosphine oxide A redox-active π-acceptor scaffold enables proton-coupled electrochemical reduction of a phosphine oxide P=O bond to the corresponding phosphine at mild potentials, producing water as the only byproduct. This main-group PCET strategy suggests a blueprint for sustainable phosphine oxide recycling and broader activation of strong p-block element bonds.

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Splint RNA-mediated single-stranded DNA-encoded library construction and label-free live-cell selection An efficient and precise short-splint RNA-mediated single-stranded DNA (ssDNA) ligation system has been developed. This system demonstrates superior discrimination of single-base mismatches at oligonucleotide ligation junctions and achieves optimal ligation efficiency with as few as 12–14 nucleotides. Leveraging these advantages, we have established a concise ssDEL-encoding platform and developed a SplintR ligase-mediated proximity ligation (SIMPL)-based PCR method for label-free live-cell selection.

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Multiply entangled receptors for high-affinity anion recognition in water Selective sulfate binding in water remains challenging despite its importance in biological and environmental processes. Here, multiply entangled macrocycles are designed to achieve strong sulfate binding in aqueous solution. The performance of these receptors is enhanced by structural entanglement, which enforces three-dimensional preorganization. This study suggests that such receptors could represent a promising platform for anion sensing and capture in water.

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SAM molecular stacking with heterogeneous orientation for high-performance perovskite photovoltaics This study developed a molecular packing strategy with heterogeneous orientation for self-assembled monolayer (SAM) materials in perovskite photovoltaics. Thermal-evaporated SAM thick films spontaneously form a vertical-to-horizontal gradient in molecular orientation with excellent surface coverage. This heterogeneity gives rise to a gradient energy barrier that optimally facilitates hole transport. The newly proposed strategy is readily applicable for fabricating large-area, uniform SAM films, thereby overcoming a key challenge in achieving homogeneous SAM deposition for scalable production with traditional solution-based techniques.

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Inorganic backbone polymer This perspective defines inorganic backbone polymers, a class of materials that breaks the carbon-centric paradigm of traditional polymer science. Constructing inorganic backbones at the sub-nanometer scale enables these materials to synergize the processability of organic polymers with the exceptional properties of inorganic elements. The authors outline synthesis and interfacial engineering strategies, providing a roadmap for the rational design of next-generation functional materials with tunable mechanical, optical, catalytic, and other advanced properties.

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Ultracapacitive bioactive-ion pumps The detection of ion dynamics in carbon nanopores and bulk solutions is achieved through the molecular integration of UV-absorbing cations and anions with distinct signatures, alongside in situ spectroscopic techniques. This innovation provides a new understanding of the process by which ions enter carbon nanopores and shows that co-ion desorption is the dominant pathway in the case of pre-equilibrated electrodes. These findings form the technological basis for rationally designing ultracapacitive bioactive-ion pumps, enabling electrically controlled ion release and delivery.

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Integrated transient chromophores for efficient photo-induced radiofluorination While traditional photoredox catalysis is highly dependent on bimolecular collisions between the excited photoredox catalyst and substrate, in this work, we introduce a strategy that integrates a chromophore directly into the substrate, significantly enhancing substrate activation and reducing precursor loading. By exploiting the dual properties of the chromophore as both a photocatalyst and a charged leaving group, we not only accelerate the reaction rate but also simplify the purification step. Application of this approach is further demonstrated by the synthesis of 18F-labeled arenes containing PET tracers.

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DNA-mediated force transmission for precise and efficient mechanochemical activation Kim et al. establish DNA as a mechanochemical scaffold, achieving efficient bond scission (99.9% within 15 min) under ultrasound. Sequencing and mass spectrometry enable precise mechanophore characterization, advancing both fundamental mechanochemistry and potential therapeutic applications.

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A modular genetic code expansion approach to site-specific lysine acylations A modular strategy combining genetic code expansion with a selective amide bond-forming reaction enables the site-specific installation of lysine acylations on folded proteins. Acylboronates react selectively with genetically encoded hydroxylamines and provide precise access to site-specifically acylated proteins, thereby expanding the toolkit for studying the regulatory roles of these important posttranslational modifications.

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From “heavy” water to “heavy” boron clusters In this issue of Chem, Liang et al. report a general and operationally straightforward strategy for the perdeuteration of closo-borane clusters. By employing palladium catalysis, the authors demonstrate efficient catalytic late-stage transfer of deuterium from heavy water (D2O) to B–H vertices across a broad range of boron cluster frameworks.

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CO2 capture with post-modified nitrile and styrene-butadiene-styrene rubbers Using carbon capture to abate climate change is an immense challenge due to the current gigaton-per-year scale CO2 emissions, which will require enormous amounts of CO2-sorbing materials from readily available and low-cost feedstocks. Substantial waste fractions, such as single-use nitrile gloves or related rubbers, are shown here to be converted into effective adsorbents for potential use within point-source CO2 capture, such as from flue gases. This work shows a proof of concept to upcycle waste to be used for carbon capture.

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Online now: Unstructured protein mimics have enzymatic activity

Understanding and mitigating degradation in amine-based sorbents for CO2 direct air capture Direct air capture of CO2 via amine-based sorbents is currently limited by sorbent degradation. This review connects mechanisms of degradation to sorbent chemistry and process conditions, discusses design strategies for more durable materials, and outlines future directions for improving sorbent lifetime.

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p-p orbital hybridization enables durable aqueous zinc-iodine batteries Orbital engineering of p-p hybridization in iodine host materials is demonstrated to enable efficient and durable AZIBs. By incorporating a rationally designed p-block element of Bi SACs with strong interaction between the 6p orbital of Bi and the 5p orbital of iodine, the target Bi-NC catalysts favor rapid redox kinetics and a suppressed polyiodide shuttle effect, delivering exceptional durability with negligible capacity decay at an ultra-high current density of 16 A g−1 over 100,000 cycles.

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A redesigned aldehyde dehydrogenase enables intermolecular biocatalytic amide formation from aldehydes and amines Amide formation represents a key reaction in pharmaceutical synthesis, for which more environmentally friendly methods are sought. In Science, Gao et al. report a biocatalytic oxidative strategy exploiting a redesigned aldehyde dehydrogenase that allows the coupling of aldehydes with amines at the expense of an oxidant [NAD(P)+, molecular oxygen].

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Data-driven copper catalysis enables stereoselective fluorocyclopropanation Stereoselective construction of fluorinated cyclopropanes is historically difficult. We present a data-driven copper-catalyzed platform that pairs automated high-throughput experiments with machine learning informed by carbene mechanistic descriptors. The workflow reliably produces highly enantio- and diastereoselective fluorocyclopropanes, scales to gram quantities, and accelerates access to fluorinated drug-like scaffolds—showing how AI and automation can make stereochemical optimization faster and more predictive.

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Reimagining metal-organic framework discovery: Integrating experiment, computation, and artificial intelligence The convergence of automated synthesis, computational materials design, and artificial intelligence (AI) is reshaping metal-organic framework (MOF) discovery. This perspective highlights advances in automated MOF synthesis, high-throughput characterization, and computational screening, and explores how these tools can be integrated with AI into autonomous workflows. Key challenges in instrumentation, data infrastructure, and experiment-theory alignment are discussed as guiding considerations for the MOF laboratories of the future.

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Light-controlled colloidal crystallization Light-sensitive molecules are used for controlling both the attraction and repulsion between microscopic particles. This light control enables the local self-assembly of well-ordered crystal-like microstructures, and controlling light intensity and local illumination can achieve “colloidal crystallization” with excellent precision.

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Catalysis, replication, and non-equilibrium behavior: Key determinants for life-like complexity realized using short peptides A short peptide-based system is shown that can integrate self-replication with catalytic competence to exhibit complex non-equilibrium behavior. Substrate-driven self-replicators demonstrate an antagonistic relationship where the catalytic self-degradation of one replicating set enables the system to adapt and select a new set of fitter successor replicators exclusively out of equilibrium.

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Selective recognition of quaternary ammonium cations Conventional interaction models predict that less substituted ammonium cations should be more strongly recognized by synthetic receptors because of their enhanced hydrogen-bond donation and cation-π interactions. Here, we overturn this paradigm by integrating supramolecular recognition with solid-phase abstraction to achieve thermodynamically controlled and highly selective isolation of quaternary ammonium cations. Our adaptive BINOL·counterion networks operate across diverse scaffolds and in aqueous environments, redefining substitution-dependent selectivity in ammonium recognition.

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Dual-polarization fluorescent DNA framework nanomaterials DNA origami offers a programmable way to arrange fluorescent molecules into architectures with tailored optical behaviors. By encoding dye orientation and interactions within the DNA framework, we create structures that emit two distinct polarization signals whose balance can be precisely controlled. This built-in optical signature allows the 3D orientation of the DNA structures to be read out without complex instrumentation. Our approach provides a general strategy for designing fluorescent materials with customizable, structure-encoded properties for imaging and photonic applications.

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Electrified CO2 uptake in quinone-based covalent organic frameworks Electrochemical CO2 capture using molecular quinones is often limited by solubility and oxygen sensitivity in liquid systems. Embedding quinones into porous covalent organic frameworks (COFs) enhances stability, shifts reactivity into an oxygen-tolerant regime, and localizes redox activity to the solid sorbent. We developed a scalable synthesis of quinone-based COFs and validated their performance in a device operating under simulated flue gas, capturing CO2 efficiently for 80 h. This approach offers a promising, solid-state pathway toward electrochemical carbon-capture technologies.

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The ElectroChemputer: A digital infrastructure framework for programmable electrochemistry Electrochemical synthesis is a key technology for sustainable chemistry. The current lack of standardized methodologies makes reproducibility, scale-up, and transfer to industry a challenge. In this issue of Chem, Cronin and co-workers disclose the ElectroChemputer, a programmable, modular, digitally controlled platform that unifies electrochemical synthesis, monitoring, and data-driven reaction control.

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ElectroChemputer with integrated monitoring for programmable electrochemistry The ElectroChemputer is a programmable, modular platform that unifies automated electrochemical synthesis with real-time analytical feedback. By integrating nuclear magnetic resonance monitoring with electroanalysis, the system enables the parallel execution of diverse and complex synthetic protocols. This reproducible infrastructure sets a new standard for electrosynthesis.

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Aluminum redox catalysis has a ring to it Redox catalysis promoted by molecular aluminum complexes has not been previously documented. Now in Nature, Zhang and Liu report the use of an aluminum(I) redox catalyst for the regioselective assembly of 1,2,4-substituted benzenes from terminal alkynes. This work provides a foundational blueprint for designing redox-active aluminum complexes for future homogeneous catalysis.

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Vacancy-interface coupling in nanomaterials for photocatalytic energy and environmental applications Vacancy-interface coupling integrates defect chemistry with interfacial band modulation to steer charge separation, strengthen redox pathways, and enhance photocatalytic transformations. This strategy enables efficient photocatalytic H2 production, H2O2 evolution, CO2 reduction, and pollutant degradation while driving the photoreforming of plastics and biomass through synergistic vacancy-induced band restructuring and interfacial electric fields.

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A radical–polar crossover approach to complex nitrogen heterocycles via the triplet state Precisely positioning a leaving group has been shown to divert certain alkene photocyclizations from isomerization—the usual result of this type of reaction—to iminium salt formation. Trapping this ionic intermediate with nucleophiles enables the rapid assembly of structurally complex and chemically diverse nitrogen-containing ring systems.

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A donor-acceptor porous organic polymer anchoring a high density of cobalt single sites realizes full-spectrum photothermal CO2 hydrogenation The efficient utilization of the full solar spectrum in photothermal CO2 hydrogenation remains a major challenge in catalyst design. Here, a two-dimensional donor-acceptor porous organic polymer with high-density, atomically dispersed Co sites is developed for efficient full-spectrum CO2 hydrogenation. The Co single sites enhance charge separation and infrared absorption, achieving excellent photothermal conversion efficiency and CO production performance.

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TriCAN: A phase-transition molecular robot realizing closed-loop sense-compute-actuate control for inflammation-triggered bone regeneration Most drug carriers fire as soon as they see one signal, even if the tissue is not truly diseased. This work builds a peptide “nanorobot,” TriCAN (tri-phasic cell-adaptive nanorobot), that waits for three conditions: contact with a bone-forming stem cell, acidic pH, and excess oxidants. Only then does a gel-to-droplet-to-solution phase transition uncage a bone-regenerating peptide, repairing inflamed periodontal bone while sparing healthy sites.

Online now: TriCAN: A phase-transition molecular robot realizing closed-loop sense-compute-actuate control for inflammation-triggered bone regeneration