He W, Xing X, Li Y
… +3 more, Zheng Z, Liu X, Cui D
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42360146
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Developing new approaches to fabricate polysiloxane with versatile structures is a challenging project. Meanwhile, sustainable plastic upcycling is an essential issue that needs to be solved urgently. We reported herein...Developing new approaches to fabricate polysiloxane with versatile structures is a challenging project. Meanwhile, sustainable plastic upcycling is an essential issue that needs to be solved urgently. We reported herein a new strategy for synthesizing polysiloxanes by B(CF)-catalyzed hydrosilylation deoxygenation polymerization, which simultaneously degraded the oxygenated polymers like polyethers and polyesters to alkanes. Steric hindrance around the C-O/C = O bonds of these polymers and their solubility, as well as the reaction conditions affected the efficiency of Si-O bond construction and the degree of C-O/C = O bond cleavage. This synthon exhibited generality, enabling the synthesis of various polysiloxanes with adjustable M (up to 79.6 kDa) and broad T values (-19.9 to -133.9°C), which are difficult to access with the current methods. Moreover, it is tolerant to functional groups that vinyl-modified polysiloxanes have been obtained via the tandem hydrosilylation/deoxygenation and Piers-Rubinsztajn reaction. These vinyl-modified polymers can further transform into re-processable materials with excellent mechanical properties through constructing a dynamically crosslinking bond of borate ester. Density functional theory (DFT) studies revealed that the deoxygenation polymerization proceeds via alkoxysilane intermediates to generate siloxanes, which was confirmed by NMR spectrum monitoring of the model reactions. This work establishes an unprecedented polymer-to-polymer upcycling and provides a platform for fabricating polysiloxanes, bypassing tedious monomer synthesis and purification.
Wang J, Fan W, Duan J
… +3 more, Cui L, Chen T, Sui K
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42360141
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Creating anisotropic networks with spatially programmed, pronounced swelling gradients to advance the morphological complexity and functionality of self-morphing hydrogels is crucial, yet remains a formidable challenge....Creating anisotropic networks with spatially programmed, pronounced swelling gradients to advance the morphological complexity and functionality of self-morphing hydrogels is crucial, yet remains a formidable challenge. Here, we present a polymerization kinetics-mediated strategy to spatially modulate both topological entanglement and interchain interactions, generating localized domains with vastly different swelling ratios for high-contrast 3D shape transformation. This approach leverages the kinetic competition between chain growth and mass transport during polymerization. Unlike rapid polymerization, slow polymerization allows substantial inward diffusion of unreacted monomers and formation of interpenetrating polymer networks, resulting in densely entangled chain architectures across multiple polymerization stages. Critically, such entanglements not only act as physical crosslinks but also enhance interchain hydrogen bonding, weakening polymer-water interactions and reducing osmotic pressure. By introducing hydrogen-bonding or polyelectrolyte effects, we significantly amplify differences in interchain interactions and equilibrium swelling ratio between rapidly and slowly polymerized hydrogels. Consequently, by spatially modulating ultraviolet light intensity, a pronounced disparity in entanglement density and interchain interactions is achieved between adjacent regions, yielding a striking 23-fold difference in swelling ratio. This sharp local swelling contrast enables intricate, high-cavity 3D morphologies unattainable with conventional self-morphing hydrogels, broadening the architectural versatility and application potential of hydrogel-based adaptive materials.
Wu Y, Wang G, Wu Y
… +7 more, Zhang Q, Wang Z, Liu Y, Zheng Z, Cheng H, Huang B, Wang P
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42360131
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Perovskite-based photocatalytic hydrogen bromide (HBr) splitting offers a promising route for solar-driven hydrogen production. However, the accumulation of the oxidation product bromine often impedes reaction kinetics d...Perovskite-based photocatalytic hydrogen bromide (HBr) splitting offers a promising route for solar-driven hydrogen production. However, the accumulation of the oxidation product bromine often impedes reaction kinetics due to its sluggish oxidation, which faces a substantial energy barrier of 1.09 V versus NHE. This study introduces acetaldehyde as a stable and highly reductive agent in a perovskite-saturated HBr system, enabling simultaneous high-performance H evolution and oxidative upgrading of acetaldehyde to valuable acetic acid. Using a Pt single-atom-modified FAPbBr perovskite with exposed (100) and (111) facets, which is different from the traditional morphology of perovskites and provides efficient charge separation, the system achieves remarkable production rates of 1033.13 µmol h for H and 1017.20 µmol h for acetic acid. High apparent quantum efficiencies of 30.62% at 450 nm and 31.78% at 520 nm are attained, with acetaldehyde conversion exceeding 90%. The process demonstrates stability over 15 h, recovering 0.8 mL of acetic acid at an 85% extraction efficiency. This strategy effectively utilizes both electrons and holes to simultaneously produce clean energy hydrogen and high-value organic products.
Dou R, Song R, Xie K
… +6 more, Lei J, Li J, Ge M, He H, Huang Y, Xu H
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42360124
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Artificial solid electrolyte interphases (ASEIs) are widely used to stabilize lithium metal anodes, yet their protection inevitably degrades because polymer coatings crack under repeated volume fluctuation and inorganic...Artificial solid electrolyte interphases (ASEIs) are widely used to stabilize lithium metal anodes, yet their protection inevitably degrades because polymer coatings crack under repeated volume fluctuation and inorganic SEI components detach during cycling. Herein, we present a dynamic crosslinked fluoropolymer (DCF) artificial interphase that simultaneously enables autonomous polymer crack healing and continuous replenishment of inorganic SEI components. The dynamic interphase is constructed from a layer of poly (2,2,2-trifluoroethyl acrylate) cross-linked by ureido-pyrimidinone, whose reversible quadruple hydrogen bonds enable rapid self-healing of the polymer network and effective closure of interfacial cracks. Additionally, the fluorine-rich polymer matrix serves as a persistent source for LiF formation, continuously replenishing the inorganic inner layer to compensate for detachment during cycling. Benefiting from this dual regenerative mechanism of polymer self-healing and inorganic component self-replenishment, lithium metal anodes protected by the dynamic interphase exhibit highly stable plating and stripping for over 4000 h in symmetric cells. In full cells, a LiFePO||Li cell retained 90.67% of its capacity after 1000 cycles, while a high-loading LiNiCoMnO (NCM622) pouch cell maintained 70% capacity after 700 cycles at 1C.
Zha X, Zuo M, Jiang Z
… +8 more, Zou Q, Xin Y, Xiong Y, Liu Y, Liu L, Luo M, Li M, Wang D
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42360114
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The construction of crystalline covalent organic frameworks (COFs) with strong and tunable chiroptical responses remains challenging due to rapid crystallization that limits effective chirality induction. Here, we report...The construction of crystalline covalent organic frameworks (COFs) with strong and tunable chiroptical responses remains challenging due to rapid crystallization that limits effective chirality induction. Here, we report a pre-crosslinked network-mediated dual-exchange strategy that enables both amplified chiroptical activity and decoupled multilevel chirality in β-ketoenamine-linked COFs. In this approach, monomers are first immobilized within a pre-crosslinked amorphous imine network, which kinetically regulates subsequent framework formation. The crystallization proceeds through a dual-exchange process involving concurrent amine and aldehyde exchange, thereby retarding reaction kinetics and prolonging the chirality induction window. As a result, the obtained COFs exhibit pronounced propeller-like conformational chirality with dissymmetry factors (|g|) up to 0.071, representing an order-of-magnitude enhancement over conventional systems. Furthermore, by integrating supramolecular transcription, mesoscopic helicity and molecular chirality are decoupled and independently incorporated within a single framework. Their cooperative or antagonistic interplay leads to enhanced or attenuated chiroptical responses. This work provides a general strategy for boosting chiroptical activity and programming multilevel chirality in crystalline frameworks.
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42360111
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A promising strategy to valorize polyethylene is its oxidation to dicarboxylic acids with O and NO. However, it remains unclear whether and how the formation of dicarboxylic acids from polyethylene can be increased throu...A promising strategy to valorize polyethylene is its oxidation to dicarboxylic acids with O and NO. However, it remains unclear whether and how the formation of dicarboxylic acids from polyethylene can be increased through catalyst design and reaction parameters adjustment. In this work, it was found that through proper reaction condition selection and in the absence of a catalyst the yield toward dicarboxylic acids could reach ∼29 mol% with only little overoxidation to undesired CO and CO. At high NO partial pressure, the formation of gaseous products is suppressed, yielding an excellent carbon recovery for a variety of polyethylene types. The yield toward dicarboxylic acids can be further enhanced through the addition of a Cu/V catalyst up to ∼51 mol% (>90% wt.% diacid), while the excellent carbon recovery can be maintained. It was found that the catalyst system was both robust and tolerant as the use of post-consumer plastic waste, a mixture of polyethylene and polypropylene, yielded a similar product slate.
Bendtsen MK, Møllebjerg A, Peña-Díaz S
… +15 more, Graham R, Petersen NC, Isaksen BN, Carstensen M, Johansen MB, Sommerfeldt A, Petersen AR, Chuma IK, Ryberg C, Wittenborn TR, Gichuru V, Wang H, Scavenius C, Sandahl A, Otzen DE
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42360106
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Better enzymes are needed to develop sustainable methods to recycle plastics with C-X heterobonds such as polyurethane (PUR) and nylon, for which no industrial-scale solutions exist. Current methods rely largely on seque...Better enzymes are needed to develop sustainable methods to recycle plastics with C-X heterobonds such as polyurethane (PUR) and nylon, for which no industrial-scale solutions exist. Current methods rely largely on sequence mining based on a small number of known enzymes. Here, we expand the pool of PURases and nylonases by bioprospecting legacy plastic waste with fluorophore plastic mimics combined with fluorescence-assisted cell sorting (FACS). We identify 29 plastic-degrading bacteria, from which 12 enzymes are identified by mass spectrometry and homology searches. Compared to existing enzymes, these enzymes show higher thermostability and hydrolytic activities against different high-molecular weight PUR polymers and nylon textiles compared to previously described wildtype enzymes. To our knowledge, this is the first reported example of enzymes capable of hydrolyzing longer chains of untreated PUR and nylon as well as crosslinked PUR. This study significantly increases the number of known PURases and nylonases and provides starting points for optimization campaigns through protein engineering and for in silico discovery.
Li J, Ye Y, Wang R
… +7 more, He X, Shi X, Qiu M, Chen W, Ji S, Dang L, Li MD
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42360081
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Room temperature phosphorescence (RTP) materials with long luminescence lifetimes and tunable properties are highly desirable for applications in optoelectronics, information encryption, and bioimaging. Although host-gue...Room temperature phosphorescence (RTP) materials with long luminescence lifetimes and tunable properties are highly desirable for applications in optoelectronics, information encryption, and bioimaging. Although host-guest doping is an effective strategy to achieve high-performance RTP in most systems, the RTP originates from the guest through host confinement and charge/energy transfer. Activating RTP from the host remains a significant challenge due to inefficient triplet exciton manipulation. Here, we successfully achieved ultralong host RTP (224 ms) in the host-guest doped systems with a controlled triplet state energy gap (ΔE) of 0.36-0.44 eV, which facilitates an endothermic reverse triplet-triplet energy transfer (rTTET) process from the guest to the host, and thereby promotes the repopulation of host triplet excitons. This process establishes a dynamic thermal equilibrium between forward triplet-triplet energy transfer (TTET) and rTTET, leading to thermally activated delayed phosphorescence from the host. As a result, the lifetime of the host's RTP is extended by 1120-fold (from 0.2 to 224 ms). More importantly, the photoluminescence properties of the host's RTP can be systematically and predictably tuned by varying the ΔE, temperature, and doping ratio. This work provides a mechanistic insight and paradigm into the design of RTP materials through intermolecular exciton dynamics.
Yao L, Wei Z, Zhao T
… +4 more, Wang Z, Wang G, Chi X, Liu Y
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42360078
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Aqueous zinc metal batteries (AZMBs) employing halogen- or manganese-based cathodes and anode-free design possess the highest energy density among the aqueous battery families. However, their performance is severely limi...Aqueous zinc metal batteries (AZMBs) employing halogen- or manganese-based cathodes and anode-free design possess the highest energy density among the aqueous battery families. However, their performance is severely limited by interfacial side reactions and anode-cathode cross-talk, which undermine energy density and cycle life. Conventional strategies focusing on a single interface are inadequate to address these systemic issues. The optimal strategy cluster from literature data mining guided the material system creation via a data-driven process of molecular descriptor screening. This guided the creation of an asymmetric dual-interphase separator, featuring a Zn-supplying interphase (ZSI) on the anode side that suppresses polyhalide shuttling and accelerates desolvation, and a composite conductive interphase (CCI) on the cathode side that enhances multi-electron reaction kinetics and active species utilization. Enabled by the asymmetric dual-interphase engineering, the constructed anode-free Zn||MnO full cell achieves a high voltage efficiency of 90% and stable cycling over 1000 cycles. Concurrently, a state-of-the-art anode-free Zn||I battery delivers an energy efficiency exceeding 90% at high areal loading of 38.14 mg cm. Furthermore, a universal zinc metal anode/electrolyte interphase descriptor (ZMAEID) was proposed, mechanistically linking interfacial electrochemical behavior with mechanical stability. This systematic, data-driven, and theory-guided strategy establishes a new paradigm for next-generation anode-free AZMBs.
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42360050
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Porous organic cages (POCs) have emerged as a distinct class of molecular porous materials featuring precisely tunable pore architectures and exceptional solution processability, positioning them as promising platforms f...Porous organic cages (POCs) have emerged as a distinct class of molecular porous materials featuring precisely tunable pore architectures and exceptional solution processability, positioning them as promising platforms for membrane-based ion separation. Their unique ability to synergistically combine structural confinement with tunable ion-channel interactions enables the selective separation of ions with closely similar sizes and physicochemical properties. This review provides a systematic overview of recent advances in POC-based ion separation membranes, with an emphasis on molecular design, membrane fabrication, interfacial engineering, and the underlying separation mechanisms. Furthermore, it offers critical insights into emerging design principles and key challenges for achieving high-performance membranes, thereby establishing a conceptual framework for the development of next-generation ion separation systems.
Zhang P, Cai Z, Wang H
… +4 more, Yu Y, Du Y, Xiao J, Yan Z
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42360040
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Scintillators are crucial for radiation detection and medical imaging, yet the simultaneous optimization of their luminescence efficiency, stability, and device compatibility via molecular design remains challenging. Her...Scintillators are crucial for radiation detection and medical imaging, yet the simultaneous optimization of their luminescence efficiency, stability, and device compatibility via molecular design remains challenging. Here, we propose and demonstrate "coordination-saturation isomerism" as a molecular-design paradigm for systematically tuning the luminescence and scintillation properties of copper-iodide clusters. By modulating the protonation state of a single A-site cation (N-methylpiperazine), we achieve three distinct structural modes: Ionic 1D chain (Ionic-type CuI-L) with excitation-dependent dual emission; organic-ligand saturation gives a rigid, highly symmetric 0D cluster (Coordination-type- CuIL) that exhibits efficient cyan emission (PLQY 86%) and outstanding scintillation performance (light yield 53,000 ph•MeV); and inorganic-iodide-assisted saturation results in a heterogeneous 0D cluster ("All-in-One" hybrid-type CuIL) with red-shifted emission and lower efficiency. This strategy surpasses conventional dimensionality engineering, clearly revealing how structural evolution from ionic to covalent bonding and from organic to inorganic-assisted saturation dictates excited-state properties and device performance. A flexible scintillation film based on CuIL enables high-resolution CT imaging, highlighting the potential of this material system for flexible x-ray detection and imaging. This work provides a novel molecular blueprint for the precise design and performance regulation of metal-halide optoelectronic materials.
Louka A, Kalaitzaki EE, Panousis A
… +8 more, Bonoras S, Livas C, Froudakis G, Drygiannakis I, Damianaki A, Kolios G, Valatas V, Eleftheriadis N
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42360035
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Photopharmacology offers powerful opportunities for the spatiotemporal control of biological processes, yet the rational design of photoswitchable enzyme inhibitors remains challenging. Here, we report a target-guided st...Photopharmacology offers powerful opportunities for the spatiotemporal control of biological processes, yet the rational design of photoswitchable enzyme inhibitors remains challenging. Here, we report a target-guided strategy for the development of diazo-based photoswitchable inhibitors of human 15-lipoxygenase-1 (15-LOX-1), a key enzyme in inflammatory signaling, ferroptosis, and cancer. Guided by the structural features of known ligands, we developed three complementary photoswitch classes: reversible azobenzenes (ABs), azo-heteroarenes (HAs), and covalent azo-bis-alkynes (BAs). These compounds exhibit efficient E/Z photoisomerization and high bistability, supported by single-crystal x-ray diffraction and density functional theory calculations. Enzymatic inhibitory and kinetic studies revealed distinct activity and selectivity profiles within the tested substrates/isoenzyme: AB and HA derivatives function as E-ON/Z-OFF inhibitors, whereas BA derivatives display Z-ON/E-OFF behavior, enabling programmable light-controlled modulation. We validated 15-LOX-1 as a therapeutic target in cellular and in vivo mouse models of colonic inflammation, where inhibition suppressed IL-8 expression. Finally, using our reversible and covalent photoswitches, we demonstrate photoisomer-dependent suppression of IL-8. Beyond 15-LOX-1, this work establishes a generalizable framework for the rational development of selective photoswitchable inhibitors with tunable biological outcomes.
Ge T, Cheng B, Zhang D
… +5 more, Chai DF, Chu D, Sui G, Li J, Guo D
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42360029
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Enhancing the selectivity and capacity of chloride capture is a fundamental challenge for high-performance capacitive deionization (CDI). Here, a coordination engineering strategy guided by selective orbital coupling (SO...Enhancing the selectivity and capacity of chloride capture is a fundamental challenge for high-performance capacitive deionization (CDI). Here, a coordination engineering strategy guided by selective orbital coupling (SOC) theory is proposed for the rational design of superior chloride capture electrodes. A heterostructured FeCoSe/TiC featuring coexisting tetrahedral Fe and octahedral Co sites is synthesized as a model platform. This unique dual-site geometry triggers significant charge transfer and electronic modulation, which synergistically tailors the discrete d-orbital states of the active Co sites. The resulting optimization in orbital energy and symmetry enhances selective hybridization with Cl 3p orbitals, while the concurrently increased soft-acid character of the Co sites further promotes specific charge-transfer interactions. Consequently, the FeCoSe/TiC electrode delivers outstanding desalination performance, including a high salt adsorption capacity of 140.5 mg g, a fast average salt adsorption rate of 5.8 mg g min, a remarkable charge efficiency of 97.3% (in 2000 mg L NaCl), and excellent long-term stability. This work not only validates SOC as a powerful design principle for selective CDI electrodes but also establishes a generalizable paradigm to circumvent scaling relations through atomic-scale coordination engineering, paving the way for precisely regulated ion-adsorption energetics in advanced desalination technologies.
Oftadeh E, Ortiz M, Rodriguez KD
… +2 more, Yang J, Lipshutz BH
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42360028
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A new approach to Pd-catalyzed C─N bond formation is disclosed based on observations from Nature, where its use of an "on water" phenomenon allows for variations in its pH and content. By employing highly basic condition...A new approach to Pd-catalyzed C─N bond formation is disclosed based on observations from Nature, where its use of an "on water" phenomenon allows for variations in its pH and content. By employing highly basic conditions generated from addition of a certain amount of KOH (i.e., the "dirt") to the water, aminations take place quickly. This "on dirty water" approach also provides the needed base, further simplifying reactions. The viscosity of the KOH/water (i.e., 30% KOH) presumably prevents dissolution of the organic coupling partners; hence, base-sensitive groups (e.g., esters, nitriles, etc.) are readily accommodated, thereby broadening the scope of this process. Recycling of this highly basic medium is also illustrated, resulting in a very low complete E-Factor. Several comparisons with recent literature routes are made using not only Pd catalysis, but also with aminations based on earth-abundant metals such as Ni and Cu, which tend to be carried out in various organic solvents. Water-based sequences are also shown, including chemoenzymatic catalysis. Prospects for extending this discovery to several other types of valuable bond formations in synthetic chemistry are also presented.
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42360027
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Publisher ↗
Cells can form open compartments, known as biomolecular condensates, which possess distinct environments and concentrations compared to their surroundings. These biomolecular condensates can modulate biochemical processe...Cells can form open compartments, known as biomolecular condensates, which possess distinct environments and concentrations compared to their surroundings. These biomolecular condensates can modulate biochemical processes, including protein aggregation. Notably, they have been reported to both accelerate and inhibit protein aggregation. Since protein aggregation is often associated with pathological conditions like neurodegenerative diseases, it is crucial to understand the molecular mechanisms underlying the interplay between phase separation and fibril formation. In this review, we discuss how, contrary to intuition, aggregation within the bulk of condensates can be inhibited rather than promoted, even in the presence of elevated local protein concentration. However, biomolecular condensates can still facilitate fibril formation by generating an interface between the dense and dilute phases, where molecular and mesoscale properties are optimal for the nucleation of protein aggregation.
Yang Y, Kırtel O, Badino SF
… +8 more, Strother LH, Rotilio L, Lauridsen JMV, Neun S, Morth JP, Lee JW, Welner DH, Westh P
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42360017
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Aqueous monoethanolamine (MEA) solutions can absorb CO from industrial point sources via amine scrubbing. Mechanistically, CO diffuses in and reacts with MEA or hydroxide to form a mixture of carbamate and carbonate/bica...Aqueous monoethanolamine (MEA) solutions can absorb CO from industrial point sources via amine scrubbing. Mechanistically, CO diffuses in and reacts with MEA or hydroxide to form a mixture of carbamate and carbonate/bicarbonate. Subsequently, CO is released for storage or utilization via an energy-intensive thermal solvent-regeneration process. Here, we explored biocatalytic acceleration of the solvent regeneration step, which accounts for the dominant energy cost of carbon dioxide removal (CDR) processes. We conducted a sequence mining campaign based on urethane-degrading Amidase Signature superfamily enzymes and discovered amidases that hydrolyze MEA carbamate, thereby increasing the overall release rate of CO. The most promising candidate, an amidase from Parageobacillus caldoxylosilyticus (PcAmd), showed good thermostability (T around 70°C) and a specific activity against MEA carbamate of about 1 U/mg (20 nKat/mg). We found that PcAmd accelerated the regeneration of MEA sorbent. Specifically, PcAmd at 1 µM increased the initial CO release rate by about 20%, and the time required to release 80% of the captured CO was reduced by approximately half compared to enzyme-free solutions. These results identified a novel potential of amidases in carbon capture and motivated further efforts to discover or engineer enzymes with better stability and activity for industrial CDR applications.
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42360014
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Publisher ↗
Despite their privileged status in pharmaceutical chemistry, the sustainable synthesis of cyclopropanes remains a fundamental challenge. Conventional methods rely on hazardous diazo precursors or pre-functionalized subst...Despite their privileged status in pharmaceutical chemistry, the sustainable synthesis of cyclopropanes remains a fundamental challenge. Conventional methods rely on hazardous diazo precursors or pre-functionalized substrates that generate stoichiometric byproducts. Here, we report an overall endergonic, catalytic route to cyclopropanes from abundant, renewable starting materials. Furan oxetanes, readily formed by photochemical [2 + 2] cycloaddition of aldehydes and furan, undergo an intramolecular S-type rearrangement under Lewis acid catalysis, producing cyclopropanes with ideal atom economy. The strategy enables access to meso-cyclopropane dicarbaldehydes, which are versatile intermediates that streamline the preparation of otherwise challenging bioactive motifs. By harnessing photogenerated oxetanes as cyclopropane precursors, this work offers a sustainable way to densely functionalized cyclopropanes from simple feedstocks under mild conditions.
Sun R, Lu M, Wang Z
… +7 more, Gao W, Chen J, Liu X, Zhang H, Bednarkiewicz A, Zhang F, Sun L
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42360008
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High-resolution biological imaging in deep tissues holds substantial importance for advancing precision medicine. Currently, the lanthanide-doped nanoparticles enable in vivo near-infrared imaging but face a critical tra...High-resolution biological imaging in deep tissues holds substantial importance for advancing precision medicine. Currently, the lanthanide-doped nanoparticles enable in vivo near-infrared imaging but face a critical trade-off: Er -based emission at around 1530 nm enables high optical resolution yet suffers from limited tissue penetration due to water absorption, whereas nanoprobes emitting at approximately 980/1060 nm offer deeper penetration with high brightness but compromised resolution due to higher tissue scattering at shorter wavelength. This fundamental contradiction between imaging depth and resolution remains a key challenge. Herein, we introduce the concept of energy traps to actively regulate energy distribution within lanthanide nanoparticles via excitation-wavelength switching and directional energy transfer modulation. This strategy enables controlled access to either sensitizers (Yb, Nd) self-emission or efficient sensitization of activators (Er), thereby allowing selective enhancement of emission channels. By integrating the deep-tissue penetration capability of short-wavelength sensitizers (980 and 1060 nm) with the high-resolution emission of long-wavelength activators (1530 nm) through a deep-learning-based network, we successfully achieved a 93% enhancement in imaging performance for short-wavelength probes, offering a robust and adaptable platform for high-contrast deep-tissue bioimaging and future point-of-care diagnostics.
Sánchez-Férez F, Khobotov-Bakishev A, Ortín-Rubio B
… +10 more, von Baeckman C, Hernández-López L, Cortés-Martínez A, Paraoan RAI, Boada R, Juanhuix J, Gándara F, Goodwin AL, Carné-Sánchez A, Maspoch D
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42360004
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Publisher ↗
Controlling the spatial distribution of defects in metal-organic frameworks (MOFs) remains a fundamental challenge in defect engineering. Here, we report a cage-directed assembly strategy that enables the programmed intr...Controlling the spatial distribution of defects in metal-organic frameworks (MOFs) remains a fundamental challenge in defect engineering. Here, we report a cage-directed assembly strategy that enables the programmed introduction of topologically correlated defects and induces aperiodicity in HKUST-1-type frameworks. Pre-synthesised Rh(II) metal-organic cages or polyhedra (MOPs) act as persistent cavities that template the formation of HKUST-1-based networks containing linker-induced Cu-vacancy domains confined within discrete cuboctahedral cavities. The use of dicarboxylate linkers, in which one carboxylate group is missing compared to the original 1,3,5-benzenetricarboxylate linker, gives rise to nine distinct local defect configurations that are independently distributed throughout the lattice. This results in an aperiodic framework with preserved long-range crystallinity. The resulting materials exhibit hierarchical micro-mesoporosity, reversible loss and recovery of crystallinity, and a pronounced solvent-induced breathing response. This work demonstrates that combining pre-formed cages with linkers with reduced connectivity can be a new strategy to localise defects and access aperiodic MOFs with emergent structural adaptability.
Zhou S, Shi XL, Li M
… +7 more, Chen W, Cao T, Li NH, Zhang M, Sonar P, Liu Q, Chen ZG
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42360003
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Publisher ↗
Carbon-based materials, particularly single-walled carbon nanotubes (SWCNTs), are promising candidates for flexible thermoelectric applications due to their excellent electrical conductivity and mechanical robustness. Ho...Carbon-based materials, particularly single-walled carbon nanotubes (SWCNTs), are promising candidates for flexible thermoelectric applications due to their excellent electrical conductivity and mechanical robustness. However, severe self-aggregation of SWCNTs leads to suboptimal and degraded thermoelectric performance. Conventional dispersion strategies have proved largely ineffective in overcoming this limitation. Here, we present a pioneered radical-mediated dispersion (RMD) strategy, enabled by a rationally designed small molecule, OTN, which incorporates a donor-acceptor conjugated backbone and pendant free-radical terminals. The RMD strategy mechanism functions through dual interactions: The donor-acceptor backbone enhances π-interactions with SWCNTs, while the pendant radicals facilitate radical-radical interactions to further suppress nanotube aggregation. This synergistic molecular design enables OTN-SWCNT hybrid films to achieve a high power factor of 30.1 µW cm K, far exceeding previous reports, while maintaining excellent free-standing mechanical flexibility. Furthermore, a nine-leg thermoelectric device assembled from these films delivers a normalized power density of 0.653 µW cm K, representing one of the best performances for CNT-based thermoelectrics to date. This pioneering molecular design, together with the derived innovative RMD strategy overcomes the long-standing aggregation of SWCNTs and is anticipated to open new avenues for advancing carbon-based thermoelectric materials toward practical, flexible energy-harvesting applications.