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Dicyanodithioquinoline‐Based Donor Polymers With Large Dipole Moments for Efficient Organic Solar Cells Exceeding 20% Power Conversion Efficiency

ABSTRACT Constructing efficient donor polymers is a crucial strategy to break through the bottleneck of organic solar cells (OSCs). Herein, a new acceptor unit dicyanodithioquinoline (TQCN) with large dipole moment (12.90 Debye) was first used to construct high performance polymeric donor PCN7. Theoretical calculations and experimental results confirm that, compared to PM6, the TQCN block suppresses exciton‐vibration coupling through enhanced intermolecular interactions and reduced exciton reorganization energy. The PCN7/L8‐BO binary OSCs yielded a remarkable power conversion efficiency (PCE) of 19.45%, representing one of the highest values among binary OSCs. It exhibits an open‐circuit voltage ( V OC ) of 0.910 V and a non‐radiative recombination energy loss (Δ E 3 ) of 0.216 eV, which are significantly superior to those of the PM6‐based device (0.883 V, 0.252 eV) and the D18‐based device (0.903 V, 0.221 eV). Multiple batches of PCN7 exhibited excellent PCE with good reproducibility. In addition, the D18:PCN7/L8‐BO ternary device exhibits an improved efficiency of 20.06%. These results confirm the potential of the TQCN acceptor block in suppressing exciton‐vibration coupling, providing a viable route toward designing donor materials with both low energy loss ( E loss ) and high PCE.

Heterocycle‐Linked Covalent Organic Frameworks With Indazole Units for Cooperative H ₂ O ₂ Photosynthesis and Biomass Valorization

ABSTRACT Developing artificial photosynthesis systems that couple hydrogen peroxide (H 2 O 2 ) production with organic valorization remains challenging due to rapid carrier recombination. Herein, indazole‐linked covalent organic frameworks (COFs) were constructed via Cadogan reductive cyclization of nitro‐functionalized imine‐linked precursors, which converts labile imine linkages into robust indazole linkages while preserving high crystallinity and enhancing visible‐light harvesting ability. Remarkably, in a synergistic system coupling H 2 O 2 production with furfuryl alcohol oxidation, indazole‐linked COFs exhibited a nearly 5.6‐fold enhancement in photocatalytic performance compared to its imine‐linked counterpart. Combined in situ DRIFTS and DFT calculations revealed that the indazole linkage optimizes interfacial reaction kinetics and facilitates substrate adsorption through polarized nitrogen sites. This work establishes heterocyclic linkage engineering as an effective strategy for designing advanced crystalline photocatalysts toward integrated solar energy conversion.

Templated Synthesis of Heterobimetallic Nd─Co Clusters

ABSTRACT Heterometallic clusters are typically realized through the design of metal site‐specific coordination environments. Their unusual metal‐metal interactions and potentially synergistic effects toward small‐molecule activation and catalysis are two of the many attributes of fundamental importance. Synthetic heterometallic clusters containing f‐ and d‐block metals are challenging to design and synthesize, and lag far behind those only containing transition metals. To this end, we used compound LH 5 Nd ( 1 ), where LH 8 = cyclen(1,4,7,10‐tetra‐ o ‐NH 2 C 6 H 4 ) 4 , and subjected it to metalation with Co 2 (HMDS) 4 (HMDS = hexamethyldisilazide) resulting in LH 3 NdCo 2 (HMDS) 2 ( 2 ). Cluster 2 displays a Nd─Co distance of 3.276(12) Å, which is under the shortest distance previously reported for a Nd─Co interaction (3.294(4) Å). Exposing 2 to dry dioxygen results in a dimeric species containing a single oxygen atom in a pseudo‐planar geometry across two Nd and two Co atoms, (LH 3 ) 2 Nd 2 Co 2 (µ 4 ‐O) ( 5 ). The Nd─Co distance in 5 shortens significantly to 2.993(6) Å. X‐ray photoelectron spectroscopic studies reveal 5 to be best described as [Nd III 2 Co III 2 ], where the Co(III) centers remain high spin based on local structural metrics ( d avg (Co─N) = 2.02(4) Å and d avg (Co─O) = 1.920(2) Å). Overall, we report the design and synthesis of well‐defined heterobimetallic Nd─Co clusters and their metal‐metal interaction synergy to activate dioxygen.

Henning Hopf (1940–2026): A Role Model in Chemistry and Beyond

Mechanistic Diversity in Photoexcited Radical Redox Chemistry: A Critical Evaluation

ABSTRACT “Photoexcited Radical Redox”, a subset of photoredox reactions in which electron transfer occurs via excitation of an already oxidized or reduced radical form of the photocatalyst, has been a cause of both great excitement and confusion in recent years. While the ability of photoexcited radical redox to access extreme redox potentials has led to a string of exciting, high‐profile, challenging new transformations, serious doubts have been raised as to the feasibility of the mechanisms proposed, leading to an extensive debate over a diversity of different mechanistic rationales. While these discussions are supported by a steadily growing body of experimental evidence, overall understanding of photoexcited radical redox remains murky at best. Each mechanistic model struggles to account for at least some important observations, and many important general questions remain unanswered. In this review, we comprehensively summarize the various mechanistic models that have been proposed to account for observations of (apparent) photoexcited radical redox, provide a detailed, critical assessment of the evidence for and against each of them, and highlight continuing gaps in collective understanding and directions for future investigations.

Harnessing Synergistic Enthalpy‐Entropy Regulation: An I‐Motif‐Based Modulating Design for Programming Stimulus‐Responsive DNA Switches

ABSTRACT DNA switches with target‐induced allostery show great potential in biomedical application, yet often remain unprogrammable responses and limited accuracy. Existing designs also lack adaptability beyond predefined response windows and offer limited sensitivity tuning. Herein, we present an i‐motif‐based modulating design that leverages enthalpy‐entropy synergy to engineer programmable, tunable pH‐responsive DNA switches applicable to diverse aptamers. The design couples target‐binding aptamers with split i‐motif structures through variable‐length linkers that act as dual thermodynamic regulators. Linker‐length modulation permits collective control over critical parameters of switches, including target responsiveness, functional pH window, and the magnitude of pH‐dependent affinity shifts. An auxiliary sequestration mechanism further allows independent fine‐tuning of individual parameters. This design successfully converts aptamers targeting ATP, cortisol, Zn 2+ , and PTK7 into programmable switches, demonstrating versatility across different binding characteristics. Practical validation in tumor microenvironment profiling confirms the design’ capability for multi‐analyte detection with enhanced sensitivity. By establishing fundamental thermodynamic perspective and achieving cross‐platform adaptability, this strategy represents a paradigm shift from trial‐and‐error methods to rational molecular switch engineering, opening new avenues for responsive biosensing and diagnostic applications.

Netanel Shpigel

Easily Accessible and Highly Active Heterogeneous Nickel Catalyst Supported by Covalent Organic Framework for In Situ Ethylene Polymerization

ABSTRACT The heterogenization of homogeneous transition‐metal catalysts is a well‐established strategy for enabling oriented synthesis and precise morphological control of high‐molecular‐weight polyolefins. To date, however, the development of covalent organic framework (COF)‐supported late‐transition‐metal catalysts has remained unexplored. Herein, we report the facile construction of a heterogeneous Ni@PY‐COF catalyst via straightforward coordinated post‐synthetic modification of a dipyridyl‐functionalized COF. This system delivers highly active (10 6  g mol −1 h −1 ) and thermally stable (up to 100°C) Ni catalytic sites without requiring bulky steric substituents on the ligand. The catalyst produces semicrystalline, predominantly methyl‐branched polyethylene featuring high molecular weight (29–297 kg mol −1 ), high melting points (121°C–128°C), low branching density (≤ 25/1000 C), and well‐controlled particle morphology. Structural analysis reveals that the confined nanoscale environment of the highly porous COF framework suppresses β ‐H elimination, the dominant chain transfer and termination pathway in late‐transition‐metal‐catalyzed olefin polymerization. This work demonstrates the feasibility of integrating late‐transition‐metal active sites into an atomically precise COF material to enable heterogeneous olefin polymerization rather than oligomerization, thereby establishing a transformative paradigm for advancing high‐performance and industrially relevant polyolefin catalysts.

Solid‐Phase Engineered Metal‐Free Carbonized Polymer Dots With Auto‐Generated Rigid Amorphous Network Enabled High‐Temperature Liquid‐Phase Phosphorescence

ABSTRACT While organic phosphorescent materials hold immense promise, their application is severely hampered by limited emission tunability, short lifetimes, and environmental instability. Herein, we report a facile solid‐phase engineering strategy to achieve the large‐scale synthesis of metal‐free carbonized polymer dots (CPDs) from a single precursor. These CPDs feature tunable phosphorescence wavelengths (∼472 to 545 nm) and lifetimes (∼646.49 µs to 65.56 ms), coupled with extraordinary resilience to thermal and moisture stress. Experimental surveys and theoretical calculations reveal that high‐temperature solid‐phase reaction drive the structural evolution of CPDs from amorphous molecules to ordered heptazine structures, enabling the CPDs with progressive singlet‐triplet energy splitting for tunable phosphorescence wavelengths. Concurrently, the auto‐generated rigid amorphous network and hydrophobic groups of CPDs synergistically mitigate triplet exciton quenching triggered by dissolved oxygen and thermal deactivation, endowing the tunable high‐temperature liquid‐phase phosphorescence. With the unique optical characteristics, these CPDs show great promise for applications in aqueous‐phase illumination, displays under harsh conditions, and three‐dimensional information encryption. This work paves a new approach to polymeric phosphorescent materials, significantly contributing to the advanced lighting and information technologies.

Total Synthesis of <i>ent</i> ‐Kaurenoic Acid Diterpenoids Enabled by Distal Conformational Control in Photoredox Radical Polyene Cyclization

ABSTRACT We report a divergent synthesis of ent ‐kaurenoic acid‐derived diterpenoids enabled by a stereoselective photoredox radical polyene cyclization directed by distal conformational control. A chiral bicyclo[3.2.1]octane unit biases the reactive polyene conformation and controls stereochemical outcome remotely during cascade cyclization. This substrate‐encoded process enables highly diastereoselective construction of the 6/6/6/5 ent ‐kaurenoic acid framework under visible‐light conditions. A convergent nickel‐catalyzed reductive cross‐electrophile coupling rapidly assembles the cyclization precursor. Late‐stage oxidation‐state and stereochemical editing from a common intermediate provide access to seven structurally distinct diterpenoids, including the first total synthesis of noueinsiancin D.

Dynamic Dual‐Site Relay Catalysis Enables Selective Solar‐Driven CO ₂ Reduction Toward Ethanol

ABSTRACT Photocatalytic CO 2 reduction to ethanol (C 2 H 5 OH) offers a sustainable carbon recycling route but is limited by inefficient C−C coupling under visible light irradiation. Here, we report a defect‐engineered WO 3‐x /In SAs (SAs, single atoms) photocatalyst with a dynamic dual‐site relay mechanism, where electron‐rich W−V O (V O , oxygen‐vacancy) and electron‐deficient In single atom sites cooperatively drive selective ethanol synthesis. The W−V O site acts as a persistent *CO supply hub for CO 2 ‐to‐*CO conversion, while In site functions as an ethanol‐selective coupling center for targeted *CO−*CO coupling. This relay enables exceptional ethanol production and high selectivity (97.43% electrons selectivity and 86.35% yield‐based selectivity). Notably, the photocatalyst maintains efficient CO 2 ‐to‐ethanol conversion efficiency under natural sunlight illumination in scaled‐up experiments using a reactor equipped with a 20 × 20 cm 2 plate coated with WO 3‐x /In SAs . Combined in situ spectroscopy and DFT calculations reveal that W−V O orchestrates CO 2 ‐to‐*CO feeding and relays electrons to In SAs , reducing the C−C coupling barrier via asymmetric electron distribution. Electron‐trapping at oxyphilic In stabilizes *CO via O‐lone‐pair donation; subsequent W d‐orbital hybridization anchors *OCCO, dictating ethanol selectivity. Our work provides a design strategy for efficient photogenerated carrier utilization in CO 2 ‐to‐ethanol conversion, with implications for scalable solar fuel synthesis.

MOF‐Derived Hollow CoFe@NC Nanocages for Highly Efficient Degradation of Textile Fibers

ABSTRACT The accelerated accumulation of synthetic textile fibers, particularly 100% polyester (PET), poses a persistent environmental challenge due to their chemical inertness and resistance to degradation. Herein, hollow CoFe@NC nanocages were synthesized through a cyanometalate‐assisted transformation of ZIF‐67 nanocubes followed by reductive calcination, producing metallic CoFe alloy domains confined within an N‐doped graphitic carbon framework. The optimized CoFe@NC‐600 catalyst exhibited a hollow architecture, abundant accessible active sites, and strong metal–carbon interfacial coupling for efficient peroxymonosulfate (PMS) activation. Under visible‐light irradiation, the CoFe@NC‐600/PMS system achieved 99.2% degradation efficiency toward real PET textile substrates, confirmed by gravimetric analysis, total organic carbon (TOC) measurement, and degradation product identification. Beyond conventional semiconductor photocatalysis, this work demonstrates that metallic alloy–carbon interfaces can efficiently utilize visible light through coupled photothermal conversion, interfacial electronic activation and CoFe redox mediation to drive PMS oxidation. X‐ray photoelectron spectroscopy (XPS), electrochemical impedance spectroscopy (EIS), radical quenching experiments and density functional theory (DFT) calculations reveal that the CoFe/N‐doped carbon interface facilitates PMS adsorption, electron transfer and O─O bond activation, promoting the generation of radical and nonradical reactive species. This study provides new insights into metal–carbon hybrid catalysts for advanced oxidation processes and offers a sustainable approach for the remediation of persistent polymer wastes.

Sulfur‐Modulated Covalent Organic Framework Superstructures With Highly Dense and Fully Accessible Protophilic Sites for High‐Performance All‐Organic Proton Batteries

ABSTRACT Covalent organic frameworks (COFs) have emerged as competitive battery materials by solving the solubility and/or kinetics limitations of small molecules and polymers, while offering structure‐function merits over inorganics. However, a tricky trade‐off remains between active‐site density and accessibility. Here we describe a trade‐off‐breaking design of sulfur‐modulated COF superstructures (TD‐COFS) via synergistic geometric‐electronic structure engineering. Flower‐shaped TD‐COFS is constructed by intermolecular H‐bonding and π‐π stacking self‐assembly of tricarbonyl‐benzothiazole motifs, maximizing exposure of well‐organized multi‐protophilic active sites and π‐electron delocalization routes. Electron‐rich S‐heterocyclic benzothiazole (replacing N‐containing bipyridine, TM‐COFS) increases the electronegativity of TD‐COFS and reduces the redox barrier (S &lt; N), enabling synchronous optimization of molecular charge distribution and electronic bandgap (−0.75/1.82 vs. −0.52/2.47 eV of TM‐COFS). Furthermore, sulfur modulation boosts proton‐transfer redox activity with a low activation energy (0.23 eV), and achieves full accessibility of highly dense protophilic sites in TD‐COFS (99.3% vs. 0.34 eV/84.7% of TM‐COFS), liberating high capacity (356 mAh g −1 ) and cycling stability (70 000 cycles). Besides, the assembled soft‐packed all‐organic proton batteries deliver state‐of‐the‐art capacity (161 mAh g −1 ), energy density (81 Wh kg −1 cell ), and life (3000 cycles). This work broadens the design philosophy of structured‐tailored COFs with highly dense and accessible protophilic sites for better proton batteries.

Upcycling Poly(ethylene terephthalate) Into High‐Efficient Epoxy Toughener: Hyperbranched Oligomer Induced Nano‐Structural Heterogeneities

ABSTRACT The post‐consumer recycling efficacy of poly(ethylene terephthalate) (PET) has attracted considerable attention. Current chemical recycling of PET predominantly targets monomers, specialty chemicals, and functional materials, yet faces hurdles of costly purification/decolorization and limited market capacity. Here, we report an upcycling paradigm to directly transfer waste PET into highly efficient epoxy tougheners. Through a one‐pot process, PET is converted into hyperbranched oligomers (HBO) bearing a compact architecture and abundant terminal hydroxyl groups. This unique structure enables uniform dispersion and covalent integration into the epoxy network during curing, resulting in the formation of chemically seamless and homogeneous rigid nano‐structural heterogeneities. And these nano‐structural heterogeneities act as stress concentrators that activate localized plastic deformation, promote crack deflection and bridging, and induce microcracking, collectively establishing a multi‐scale energy dissipation network, rather than the cavity‐induced shear deformation process characteristic of conventional hyperbranched polymers. Remarkably, merely 0.3 wt.% incorporation enhances impact strength by 98.9% without compromising intrinsic processability, mechanical and thermal stability. Moreover, this method demonstrates strong feedstock versatility and has been validated at the kilogram scale, offering a viable and integrated pathway for high‐value plastic circularity.

Decoding Atypical G‐Quadruplexes and Their Interactome in Liquid Biopsies via Integrated Electroanalytical–Proteomic Technologies

ABSTRACT A multipurpose electroanalytical biotechnology to advance the role of atypical G‐quadruplex (G4) structures as emerging, multifunctional DNA biomarkers is reported. The technology presented enables determination, selective isolation, and in‐depth characterization of G4 motifs from liquid and solid biopsy samples obtained from oncology patients. The strategy relies on magnetic immunocaptors operating in a competitive assay between endogenous G4 targets and a homologous biotinylated G4 sequence labeled with an enzyme conjugate, coupled with amperometric transduction at screen‐printed electrodes. Beyond G4 determination and evaluation of the interaction of G4‐ligands using electroanalytical transduction, the strategy allows efficient G4 capture, facilitating their downstream structural and molecular characterization using complementary omics techniques. The analytical performance is validated in synthetic models and clinically relevant samples from colorectal cancer (CRC) patients, demonstrating the direct detection of G4 structures in plasma from oncology patients without prior nucleic acid extraction. Furthermore, by integrating magnetic immunocapture with PCR and DNA sequencing, and advanced proteomics, we confirm the selective isolation of endogenous G4‐forming DNA regions and show that CRC induces a stage‐dependent remodeling of the plasma G4 protein interactome beyond global G4 level changes, respectively. Notably, we identified a CRC‐associated G4‐binding protein linked to poor survival.

Separation and Valorization of Chlorine From Tail Gas Streams

ABSTRACT The chemical industry generates chlorine‐containing tail gas streams on a million‐ton scale. Following the established linear approach, these streams are neutralized, consuming large quantities of caustic soda (NaOH), thereby producing waste streams of lower value. To overcome this unsustainable linear approach, we developed a circular process to recycle chlorine from tail gas streams. The process is enabled by an ion exchange resin [IEx]Cl that selectively adsorbs chlorine in the presence of other gases, including oxygen, nitrogen, carbon dioxide, and hydrogen, while forming the corresponding trichloride [IEx][Cl 3 ] by halogen bonding. Upon application of heat (80°C) and reduced pressure the adsorbed chlorine is efficiently released, and the ion exchange resin [IEx]Cl is regenerated. Importantly, the adsorbed chlorine can also be directly converted with ethylene or carbon monoxide into the base chemicals 1,2‐dichloroethane or phosgene, respectively. In this way, chlorine from tail gas streams can be recycled and valorized in an integrated process supporting the transformation of the chemical industry toward a more circular economy.

Chemoenzymatic Radiosynthesis of a Gluconate Transporter‐Targeted In Vivo Bacterial Sensor From Clinical [ ¹⁸ F]FDG

ABSTRACT Many bacteria, but not mammalian cells, can directly import and metabolize extracellular gluconate via gluconate permease (GntP) and kinase (GntK). We hypothesized that fluorine‐18 labeled gluconic acid ([ 18 F]FGA) could leverage unique bacterial gluconate metabolism for pathogen‐specific PET imaging. Here, we report [ 18 F]FGA as a new PET tracer targeting bacterial gluconate metabolism. The chemoenzymatic radiosynthesis of [ 18 F]FGA was simple, only requiring readily available [ 18 F]FDG and glucose oxidase. [ 18 F]FGA showed broad detection sensitivity across multiple bacterial species, including multidrug‐resistant clinical isolates. Staphylococcus aureus transposon mutant studies showed substantial loss of [ 18 F]FGA uptake in GntP and GntK mutants, supporting high specificity for bacterial gluconate metabolism. [ 18 F]FGA PET selectively highlighted live bacterial infection, with high target‐to‐nontarget ratios in S. aureus (36‐fold) and Escherichia coli (30‐fold) in a murine model of myositis. Unlike [ 18 F]FDG, no appreciable uptake of [ 18 F]FGA was detected at sites of sterile inflammation. In a Klebsiella pneumoniae pneumonia model, [ 18 F]FGA showed significantly higher accumulation in the infected lung (5.2 ± 0.8%IA/cc) than in the uninfected lung (0.1 ± 0.0%IA/cc), further supporting its potential for imaging challenging clinical infections. Taken together, [ 18 F]FGA PET may be a useful tool for pathogen‐targeted imaging in clinical practice.

Hierarchical Surface‐to‐Bulk Architecture for High‐Performance O3‐Type Sodium Cathodes

ABSTRACT O3‐type layered oxide cathodes suffer from surface chemical instability and sluggish Na + transport within the O‐type framework, limitations that are aggravated by humid‐air exposure and fast‐charging operation, leading to severe interfacial degradation and rapid capacity decay. Herein, we propose a mild ethylene‐glycol–assisted treatment that in situ constructs a coherent surface‐to‐bulk architecture within NaNi 1/3 Fe 1/3 Mn 1/3 O 2 (NFM) particles, comprising a nanoscale surface rock‐salt layer, a depth‐dependent Na‐vacancy gradient, and a Na‐deficient bulk. This hierarchical configuration locks the surface chemistry while opening continuous Na + percolation pathways across the surface–bulk junction, thereby flattening radial (de)sodiation heterogeneity and steering a more uniform, highly reversible phase evolution during prolonged cycling. As a result, the modified sample exhibits outstanding fast‐charging performance, delivering 107.6 mAh g −1 at 5C (600 mA g −1 ) with 81.6% capacity retention after 400 cycles. This work highlights gradient interphase coupled with Na‐vacancy engineering as an effective strategy to develop high‐performance layered oxide cathodes for sodium‐ion batteries.

Harnessing Secondary Nucleation–Driven Supramolecular Bundled Fibers for Long‐Range One‐Dimensional Assembly of Semiconductor Nanocrystals

ABSTRACT Achieving long‐range 1D organization of semiconductor nanocrystals without altering their inherent optical properties is highly challenging, yet crucial for their applications. Herein, we report on the secondary‐nucleation‐triggered supramolecular polymerization of an alkyl chain‐tethered tetraphenylethylene derivative ( TPE‐A ) in dodecane, leading to the formation of ultralong, rigid, bundled and straight 1D fibers. Supramolecular polymerization of TPE‐A in dodecane proceeds through a nucleation–elongation mechanism, resulting in non‐emissive 1D nanofibers as the primary kinetic aggregates ( Aggr KP ). The non‐emissive characteristic of Aggr KP suggests that the tetraphenylethylene (TPE) units within Aggr KP are in a “monomer‐like” state. The TPE units and alkyl chains in Aggr KP enable their interaction with free monomers in solution, thereby acting as “seed” for catalyzing secondary nucleation. This process leads to the temporal evolution of highly fluorescent, ultralong, rigid bundled fibers as the stable thermodynamic product ( Aggr TP ). The enhanced fluorescence of Aggr TP is attributed to the aggregation‐induced emission from the TPE during the bundling of the nanofibers. As a result of secondary‐nucleation‐triggered bundling, Aggr TP creates multiple micrometer‐long, straight, parallel, 1D hydrophobic lanes. The potential of the hydrophobic lanes in Aggr TP to serve as a supramolecular template for the long‐range 1D organization of semiconductor nanocrystals without compromising their inherent optical properties is demonstrated.

Introducing Diradicaloid Thiele's Hydrocarbon Derivatives as Ligand in Transition Metal Chemistry

ABSTRACT Thiele's hydrocarbon (TH) derivatives, or p ‐quinodimethanes, are prototypical members of the organic diradicaloid family, predominantly explored in organic and main‐group organometallic chemistry. Herein, we introduce them to transition‐metal coordination by employing N‐doped TH derivatives as ligands. Pyridine‐ and pyrazine‐substituted p ‐quinodimethane ligands were synthesized, enabling the formation of mono‐ and dinuclear rhodium and cyclometalated iridium complexes ( Py∙Rh , Pz∙Rh , Py∙Ir , and Pz∙Ir ). We show the strong effects that simple metalation, and more importantly, orthometalation can have on the photophysical and electrochemical properties, as well as on singlet‐triplet gaps of these diradicaloids. Additionally, the metalated mixed‐valent forms are strongly electrochromic NIR absorbing dyes. Spectro‐electrochemical studies reveal distinct electronic interactions between the diradicaloid backbone and the metal centers, highlighting the potential of N‐doped TH derivatives as versatile redox‐active ligands in transition‐metal chemistry.