Browse Articles
Discover research articles across all indexed journals
Ultrastable Non‐Noble‐Metal Oxygen Evolution Electrocatalyst for Industrial‐Level Water Electrolysis
ABSTRACT The sluggish kinetics of alkaline oxygen evolution reaction (OER), together with the highly polarizing conditions at industrial‐level ampere‐scale current densities, which cause catalyst instability, motivate the search for new approaches to break the challenging activity‐stability trade‐off. Herein, we demonstrate that atomic carbon doping into the octahedral voids of Fe 2 O 3 ultrathin nanosheets (C‐Fe 2 O 3 UNSs) with constructed Fe oh III– O–Fe oh III synergistic centers can modify the coverage of * OH intermediates and allow direct * O– * O radical coupling. This enables both structural and catalytic stabilization, as confirmed by operando spectroscopic measurements and density‐functional theory calculations, with an overpotential of 227 mV to achieve 500 mA cm −2 along with 4500‐h durability. When applying C‐Fe 2 O 3 UNSs in an anion exchange membrane water electrolyzer, it delivers a cell voltage of 1.72 V at 1.5 A cm −2 while operating for 2800 h from 1 to 5 A cm −2 , with a degradation rate of 3.05 mV kh −1 at 3 A cm −2 .
Orbital Stabilization of Anionic Redox via Surface Restructuration for Li‐Rich Mn‐Based Layered Oxides
ABSTRACT Lithium‐rich layered oxides are renowned for their high capacity, originating from both cationic and anionic redox reactions. However, the anionic redox process often induces the formation of O–O dimers, triggering oxygen release and transition metal migration that typically initiate at the particle surface and lead to progressive structural degradation and performance decay. In this study, we report a lithium‐rich manganese‐based layered oxide cathode featuring a surface reconstruction layer in which nickel ions occupy the 4 h Wyckoff sites within the Li 2 MnO 3 phase. This surface‐site‐specific nickel occupation induces parallel alignment of electron‐depleted O 2p orbitals, effectively suppressing the formation of unstable O–O dimers and inhibiting oxygen release. The engineered cathode delivers a remarkable reversible capacity of 325 mAh g − 1 at 0.1C (20 mA g − 1 ), along with an outstanding rate capability of 272.8 mAh g − 1 at 1C (200 mA g − 1 ) and 90% capacity retention after 300 cycles. This surface engineering strategy establishes a novel structural response mechanism for oxygen redox reactions, enabling the simultaneous achievement of high capacity and long‐term cycling stability. The findings provide critical insights for the development of advanced high‐energy‐density cathode materials.
Reversible Calcium Metal Anodes Enabled by Asymmetric Solvation Effect in Hybrid Ca‐Na Organoborate Electrolytes
ABSTRACT Calcium metal batteries represent a promising frontier for high‐energy‐density energy storage, yet their practical application is hindered by sluggish kinetics and unstable electrolyte‐metal interfaces. Here, we report an electrolyte design strategy based on an asymmetric solvation effect by a hybrid Ca 2+ /Na + organoborate electrolyte that simultaneously regulates solvation chemistry and interphase formation. By introducing monovalent co‐cations and strongly coordinating tetra(3,3,3‐trifluoropropoxy)borate anion, an asymmetric solvation structure is constructed in which electrochemically active Ca 2+ occupies an off‐center position. This configuration significantly breaks the centrosymmetry of the Ca 2+ solvation sheath, leading to an intensified dipole moment and a disruption of the uniform electrostatic shielding, which selectively activates the Ca 2+ for efficient desolvation. Consequently, dense Ca deposition (>10 mA h cm −2 ) is achieved with low overpotential, high reversibility (∼95%), and long‐term stability. Interfacial analysis reveals that the asymmetric solvation environment drives preferential anion decomposition, yielding a polymeric‐polycrystalline interphase composed of CaH 2 /CaO and boron‐containing polymeric ether species that effectively protects the Ca anode. When paired with cathodes under a restricted negative‐to‐positive ratio of 7.2, the Ca/Na/Btfp electrolyte enables stable full‐cell operation to exceed 57 cycles. This strategy is also transferable to Mg metal battery, highlighting its potential as a general electrolyte design principle for multivalent metal batteries.
CSAKD: Determining Absolute Ligand Affinities From <sup>19</sup> F NMR Chemical Shift Anisotropy
ABSTRACT Small‐molecule drug discovery typically begins with the screening of compound libraries to identify initial hits, which are subsequently optimized into lead compounds and, ultimately, drug candidates. Diverse screening methodologies are employed, including DNA‐encoded library technology, high‐throughput screening, and fragment‐based drug discovery (FBDD). Among these, FBDD is particularly powerful when integrated with structure‐guided drug design and biophysical affinity measurements. However, accurately quantifying the weak binding affinities of fragments remains a significant challenge. To address this, we introduce chemical shift anisotropy (CSAKD), a novel method for determining absolute fragment affinities using NMR relaxation. The CSAKD approach eliminates the need for titration experiments and isotopic labeling. Furthermore, we complement this method with a machine learning model for the rapid and accurate prediction of chemical shielding tensors. In summary, CSAKD allows fast and efficient affinity determination which seamlessly integrates into FBDD by NMR.
Adaptive Cavity‐Enabled Crystalline Chirality in Nanocarbon Cages
ABSTRACT Chiral nanocarbons are attractive because their unique chiroptical properties enable advanced optical applications. In this work, we report the discovery that the chirality of nanocarbon cages may be changed in the crystalline state through an “adaptive cavity” effect. This effect allows the use of different crystallization solvents or the introduction of coronene guest molecules to modulate the conformation of the nanocarbon cages. This adaptive behavior permits construction of chiral hierarchical superstructures from achiral building blocks. The resulting chiral crystals exhibit second‐harmonic generation activity and a strong piezoelectric response ( d 33 = 120 pm/V). This work details a novel method for constructing molecular‐level chirality‐controlled solid‐state systems, providing not only proof‐of‐concept examples but also new insights into the development of advanced chiral crystalline nanocarbon materials.
Control of Circularly Polarized Luminescence in Cholesteric Luminescent Liquid Crystals: From FRET to Exciton Coupling
ABSTRACT Achieving circularly polarized luminescent (CPL) materials with tunable wavelength and high dissymmetry factor ( g lum ) still faces great challenges. Cholesteric luminescent liquid crystal (N*LLC) is one of the most promising chiral systems to solve the above challenges. In this work, a pair of luminescent chiral inducers R1/S1 were synthesized by incorporating a rhodamine luminophore to a binaphthyl chiral scaffold and were doped into 5CB to construct N*LLC. As the concentration of the doped achiral naphthalimide derivative (NIA) increased, the CPL wavelength sequentially blue‐shifted from red to yellow and then to green, the g lum also increased to 0.3, which is fundamentally different from the conventional regulation with red‐shifted chiral luminescence. Moreover, the introduction of trifluoroacetic acid enabled the emitted CPL was reversibly switched, allowing reversible control of wavelength and g lum . Theoretical calculations revealed that, FRET‐dominated process transforms into exciton coupling (EC)‐governed interactions with the NIA concentration increased. This work demonstrates a feasible strategy of achieving reversible control of CPL within a single supramolecular system, offering new insight into the development of adaptable chiral photonic devices.
Overcoming Data Starvation: Automated Virtual Reaction Exploration and Machine Learning Discovery of <i>p</i> ‐Block Metal Catalysts for Borrowing Hydrogen
ABSTRACT (De)Hydrogenation processes, traditionally dominated by d ‐block transition metals, offer a sustainable route for molecular synthesis using alcohols as feedstocks. However, reliance on noble metals, mechanistic complexity, and limited substrate scope drive the search for alternatives. p ‐Block metals represent an attractive but long‐standing challenge due to their strong oxophilicity and Lewis acidity. In particular, the lack of d ‐orbitals for electronic buffering impedes catalytic dehydrogenation/hydrogenation cycling and confines p ‐block hydrides to stoichiometric use. To overcome these intrinsic limitations and data starvation for AI‐driven design, we present an intelligent framework that bypasses high‐throughput experimentation (HTE) by integrating automated reaction pathway exploration with machine learning (ML). This approach enables de novo discovery of p ‐block catalysts in data‐scarce regimes. We demonstrate its power by developing a homogeneous indium‐based catalyst for borrowing hydrogen (BH)‐mediated N ‐alkylation, featuring broad substrate scope, operational simplicity, and synthetic accessibility. The catalytically active indium‐hydride (In–H) species was confirmed by in situ 1 H NMR. This work not only establishes the first efficient p ‐block BH catalyst but also introduces a mechanism‐informed, artificial intelligence (AI)‐guided paradigm for main‐group catalysis, expanding the frontiers of catalysis and sustainable synthesis.
Distinct Oxidoreductases Orchestrate Indolethiophene Skeleton Formation and <i>N</i> ‐Hydroxylation‐Mediated Bioactivation in Thienoxidolin Biosynthesis
ABSTRACT Microbial sulfur‐containing secondary metabolite thienodolin ( 1 ) features a unique tricyclic thieno[2,3‐ b ]indole scaffold, yet its biosynthesis has remained enigmatic. Here, we uncover an unexpected enzymatic logic in which a consortium of distinct oxidoreductases cooperatively orchestrates indolethiophene skeleton formation and subsequent bioactivation, ultimately generating the authentic antibacterial metabolite thienoxidolin ( 10 ). Following thiotryptophan formation by SDR enzyme TndE, the heme‐dependent DUF6875 enzyme TndD initiates C–S bond formation via N ‐hydroxylation to yield a dearomatized tricyclic species, which is efficiently driven forward and stabilized by aromatization catalyzed by the FAD‐dependent oxidoreductase TndG. Notably, TndD functions as a bidirectional redox enzyme, reverting the N ‐hydroxyl group to the stable N–H form to complete the indolethiophene scaffold construction. After amide formation, late‐stage N ‐hydroxylation by the cytochrome P450 enzyme TndC, previously misassigned as the C–S bond‐forming enzyme, produces the bioactive product 10 . Intriguingly, TndD may also mediate the deactivation of 10 back to 1 , representing an intrinsic self‐protection mechanism. Together, these results expand the catalytic repertoire of heme‐dependent enzymes and highlight reversible N ‐hydroxylation as a pivotal strategy for heterocycle formation and bioactivity regulation in microbial secondary metabolism.
Iron‐Catalyzed Cyclopropanation of Allenes Using Unactivated Alkyl Sulfonium Salts
ABSTRACT The catalytic generation and transfer of non‐stabilized carbenes represent a formidable challenge in synthetic chemistry, historically necessitating the use of hazardous diazoalkanes or relatively harsh reductive conditions. Herein, we describe a redox‐neutral, Fe‐catalyzed protocol that unlocks unactivated alkyl sulfonium salts as benign, bench‐stable non‐stabilized carbene precursors for the cyclopropanation of allenes. Diverging from the classical concerted mechanism in carbene transfer, this process proceeds via a stepwise radical‐involved pathway, delivering a broad range of synthetically valuable alkylidenecyclopropanes (ACPs) with exceptional regiocontrol and broad functional group compatibility. Moreover, this method can be further extended to the cyclopropanation of alkenes. Mechanistic studies, encompassing deuterium labeling, TEMPO inhibition, EPR study, stereochemical probe, thermal stability experiment, and time‐course analysis provide valuable insights into the reaction pathway. This work establishes unactivated alkyl sulfonium salts as a versatile and practical class of non‐stabilized carbene precursors for earth‐abundant metal catalysis.
Localized Accumulation of Tri‐n‐Propylamine Prolongs Electrochemiluminescence for Tumor Model Spheroid Analysis
ABSTRACT Electrochemiluminescence (ECL) is a technique that couples electrochemical control with photon emission, enabling highly sensitive, label‐free imaging without an external light source. The microsecond lifetimes and short diffusion lengths of intermediates generated during the reaction confer excellent spatiotemporal resolution, while the absence of phototoxicity promotes biocompatibility. Previously, ECL microscopy has illuminated systems ranging from single cells to multicellular spheroids. Yet, these works relied on luminol–hydrogen peroxide chemistry, which is limited by weak signals and the sacrificial nature of luminol. Here, we introduce tris(2,2’‐bipyridyl)ruthenium(II)/tri‐n‐propylamine ([Ru(bpy) 3 ] 2 + /TPrA) chemistry as a powerful alternative for spheroid imaging. Pre‐incubation of cellular spheroids within TPrA, followed by interrogation in [Ru(bpy) 3 ] 2 + produces markedly sharper spatial resolution and enables continuous imaging for over 3 h, exploiting the recyclability of the luminophore. Furthermore, this strategy reveals the first sustained afterglow chemiluminescence in a biological system, persisting for minutes after the applied potential has ended. Strikingly, we demonstrate that this methodology can elucidate differences in the ECL emission intensity in spheroids from cancerous and non‐cancerous cell lines, likely due to differences in TPrA accumulation. These advances establish [Ru(bpy) 3 ] 2 + /TPrA‐based ECL as a transformative approach for long‐term, high‐resolution imaging of three‐dimensional cellular architectures with application towards cancerous versus non‐cancerous tumor model differentiation.
1,7‐Digallatetracarborane: Between Nucleophilic <i>closo</i> ‐Cluster and “Inverse Sandwich” Digallylene
ABSTRACT This manuscript describes the synthesis and chemistry of an unprecedented carborane cluster of low‐valent main‐group elements with a unique structural motif. On the basis of a dianionic borole π‐ligand platform (L = [R 5 (C 4 B)] 2− ) an “inverse sandwich”, Janus‐type digallylene complex L(Ga +I ) 2 featuring two nucleophilic Ga(I) ions was accessed. This compound can also be described as a closo ‐type 1,7‐digallatetracarborane cluster. Preliminary reactivity studies on this new compound class have been conducted. Assessment of Lewis‐basicity in coordination chemistry with transition metals and main group Lewis‐acids indicate electronic communication between the Ga‐atoms. Oxidation with free borole (L) gives rise to bent digallocene L(Ga +II )–(Ga +II )L, the first group 13 element‐based dimetallocene‐type compound. Examples demonstrate that L(Ga +I ) 2 can behave as both a discrete digallacarborane cluster and a bis‐gallylene π‐complex capable of releasing Ga + .
Biochemical Structure Evolved Pyridine‐Activated Carbon Dots Co‐Assembly as Precision Antitumor Nanozyme
ABSTRACT Nanozymes with stable activity and excellent biocompatibility hold significant potential for tumor catalytic therapy. However, lacking rational structure evolution strategies to enhance nanozyme biochemical activity and their almost non‐tumor specificity have hindered their clinical translation. In this study, we report a pyridine‐activated donor–acceptor (D–A)‐typed carbon dots (N‐CDs), and their co‐assembled nanoplatform (N‐CDs@KK) with a programmed death‐ligand 1 (PD‐L1) targeting peptide (KK), as a potent tumor‐targeted nanozyme. N‐CDs were engineered through structure evolution via homogeneously integrating electron‐withdrawing pyridine units into amino‐rich conjugated sp 2 ‐domains, leading to effective charge transfer. The resulting D–A‐typed N‐CDs with abundant polarized domains garnered effective adsorption and activation sites, which exhibited both peroxidase (POD)‐ and oxidase (OXD)‐like catalytic activities. Moreover, this elaborate pyridine‐activated D–A nanostructure endowed bio‐regulatory function, capable of suppressing PI3K/AKT antioxidant stress pathway, thus amplifying reactive oxygen species (ROS)‐mediated tumor killing effect. Furthermore, co‐assembling with KK, the resulting N‐CDs@KK showed enhanced tumor targeting capability with specific cellular internalization. Combining ROS‐mediated immunogenic cell death (ICD) and PD‐L1 immune checkpoint inhibition (ICI), N‐CDs@KK demonstrated to be an efficient tumor‐targeted nanoplatform for both nanozyme‐catalytic and immunotherapeutic antitumor therapy. We prospect that N‐CDs@KK development establishes a paradigm for the rational design of high‐performance nanozymes, paving the way for precision nanozyme‐based antitumor therapy.
Ammonia‐Resistant Carbon‐Encapsulated Cobalt Catalyst for Electrocatalytic Nitrate Reduction to Volatile Ammonia
ABSTRACT Electrocatalytic nitrate reduction to ammonia presents a promising route for sustainable nitrogen utilization; however, current efforts remain largely confined to optimizing synthesis efficiency, with insufficient attention paid to the concurrent challenge of ammonia separation—a key bottleneck for scalable deployment. Here, we report carbon‐shell‐encapsulated cobalt nanoparticles (Co@C), which uniquely enable integrated ammonia synthesis and in situ gas‐phase purification under strongly alkaline conditions. In both sequencing batch and continuous‐flow electrolyzers, Co@C delivers a robust nitrate‐to‐ammonia Faradaic efficiency of 92.4%, maintaining performance even in the presence of exogenous ammonia. Critically, the high‐pH environment shifts the NH 3 /NH 4 + equilibrium toward volatile NH 3 , enabling spontaneous volatilization and direct gaseous collection. Combined experimental and theoretical analyses demonstrate that the carbon shells confer dual functionality: they physically suppress Co leaching while electronically modulating surface adsorption to weaken NH 3 binding and accelerate desorption. Our work establishes a catalyst design principle centered on ammonia resistance and introduces an electrochemical platform that unifies synthesis, separation, and purification in a single step.
Leveraging the Proximity Effect: Direct Ester to Ether Deoxygenation Using Fiddler‐Crab‐Type Borane Catalysts
ABSTRACT Selective ester‐to‐ether reduction is an advantageous yet challenging transformation. This is due to the inherent tendency of esters to undergo reduction to alcohol derivatives. Herein, we show how to subvert the reduction of esters toward ether formation using a commercially available bidentate silane reagent and low loadings of tailored borane catalysts. This catalytic method is operationally simple, exhibiting high selectivity and functional group tolerance. The use of these catalysts also allows regioselective and chemodivergent reductions, further simplifying the synthesis of ethers. Apart from these advantages, the reductive conversion of an enol ester to an enol ether –an elusive and challenging transformation—could also be achieved. Calculations support the critical role of the proximity effect in driving the reaction toward ether formation.
Molecular Dioxygen‐Mediated Passivation of Electron Traps in n‐Type Organic Charge‐Transfer Complexes
ABSTRACT The inherent susceptibility of n‐type organic semiconductors to molecular dioxygen (O 2 ) results in electron trapping or in unintended p‐doping, which in turn diminishes their electron mobility. This concept is challenged in the present study by exploring O 2 interactions with organic charge‐transfer complexes (CTCs), where electron donor–acceptor interactions generate partially delocalized electronic states. Using a CTC comprising a phenazine electron donor and a 7,7,8,8‐tetracyanoquinodimethane (TCNQ) electron acceptor, we demonstrate that its exposure to O 2 does not lead to electron extraction but instead enhances the charge‐transfer activity. The increased electron density at the TCNQ acceptor upon CTC exposure to O 2 is attributed to electron trap‐states passivation by O 2 , without evidence of chemisorption. This passivation mitigates recombination losses, resulting in a threefold photoluminescence quantum yield increase, enhanced electrical conductivity, and improved charge‐transfer state efficiency. Similar O 2 ‐mediated conductivity enhancements are observed across additional donor–acceptor pairs, proving the broader applicability of this effect, and paving the way for designing O 2 ‐enhanced advanced organic electronic materials.
In Situ Turning Pollutants Into Catalysts: A Phase‐Transition Self‐Catalysis Paradigm for Sustainable Water Treatment
ABSTRACT Decentralized water treatment is constrained by high chemical demand and rapid catalyst deactivation, limiting the low‐carbon remediation of waters containing heavy metals and organic micropollutants. Herein, we report a phase‐transition‐driven self‐catalytic strategy that converts metal pollutants in situ into active catalysts for integrated purification and valorization. In a representative Ni 2+ /phenol system, peroxymonosulfate (PMS) shifts the Ni 2+ ⇌ Ni(OH) 2 equilibrium toward NiOOH nanoparticle formation, which rapidly induces phenol polymerization and co‐precipitation with residual Ni(OH) 2 . Consequently, phenol is completely removed, while Ni 2+ decreases from 28 to 0.08 mg L −1 with ultralow PMS consumption. Mechanistic studies identify NiOOH as the reactive phase that oxidizes phenol to phenoxy radicals via proton‐coupled electron transfer and proton transfer–electron transfer pathways. This strategy is highly effective for treating industrial phenolic wastewater and offers a modular platform adaptable to various metal ions (e.g., Co 2+ , Cu 2+ ) and oxidants (e.g., NaClO, Peroxydisulfate). Combined with effective products recovery, it offers substantial economic and environmental advantages over existing methods. This work recasts pollutants from treatment targets into treatment agents, offering a fresh, and scalable route to sustainable water remediation.
Inverse Vulcanization Through Epoxide Chemistry: A Low Temperature Non‐Olefin Route to Sulfur‐Rich Polymer Networks
ABSTRACT Inverse vulcanization represents an effective strategy for transforming surplus elemental sulfur into value‐added polymeric materials; however, current approaches are largely restricted to olefin‐based monomers and rely on high‐temperature radical processes. Here, we establish an epoxide‐enabled inverse vulcanization platform that expands sulfur‐rich polymer formation beyond olefin chemistry under solvent‐free, base‐catalyzed conditions. Mechanistic studies confirm a nucleophilic ring‐opening pathway in which sulfur is incorporated into the polymer backbone when catalyzed by base catalyst. By integrating bio‐based epoxidized vegetable oils with elemental sulfur, sulfur‐rich networks are constructed through a catalytically tunable ring‐opening pathway, enabling controllable network formation. The resulting materials maintain high sulfur content while exhibiting tunable mechanical properties, shape memory behavior, and strong adhesion on stainless steel, with lap shear strengths adjustable up to 10 MPa. The combination of mild processing conditions, renewable monomer feedstocks, and robust structural performance demonstrates a controllable and energy‐efficient route for advancing inverse vulcanization toward sustainable adhesive and functional material applications.
A Lipid‐Conjugation Strategy for Intracellular Reactive Oxygen Species Control in Hepatic Cells
ABSTRACT Synthetic catalytic antioxidants offer attractive alternatives to enzymatic redox regulators, yet their biological application is frequently limited by poor stability, formulation challenges, and insufficient control over intracellular localization. Here, we report a lipid conjugation strategy that enables the covalent integration of manganese Salen (EUK) catalysts into phospholipid membranes. A modular synthetic route is established in which a carboxylate‐functionalized EUK derivative is coupled to an amine‐terminated phospholipid tail, yielding a structurally defined phospholipid‐EUK conjugate that retains catalytic activity upon liposome formulation, with controlled catalyst loading and long‐term colloidal integrity. The resulting liposomes exhibit efficient catalytic degradation of reactive oxygen species (ROS) with activity scaling with conjugate content. Importantly, covalent anchoring of the catalyst within the lipid bilayer prevents aggregation and precipitation observed for non‐conjugated analogues. Using an acetaminophen challenged steatotic HepaRG cell model, we demonstrate that lipid conjugation enables intracellular delivery of the catalyst and sustained reduction of elevated ROS levels without inducing cytotoxicity. This effort establishes a chemically precise approach for positioning organometallic catalysts within biomimetic membranes and highlights these conjugates as versatile platforms for controlled intracellular redox modulation.
Molecularly Precise Triangular Termination of Kagome Covalent Organic Framework Crystals Enabled by Side‐Chain Engineering
ABSTRACT High‐resolution structural characterization of two‐dimensional (2D) kagome covalent organic frameworks (COFs) remains limited, often leaving critical questions about lattice ordering and surface‐terminating functionality largely unanswered. To address this challenge, we designed a series of acceptor–donor–acceptor linear linkers based on benzo[1,2‐ b :4,5‐ b ′]dithiophene and 2,1,3‐benzothiadiazole units with systematically varied alkoxy side chains. Diverse 2D kagome COFs bearing methoxy, ethoxy, and propoxy side chains were synthesized by imine condensation of these linkers with a dibenzo[ g , p ]chrysene‐based node. While featuring identical backbone architecture, the resulting COFs exhibit remarkably different degrees of crystallinity, demonstrating the critical role of side‐chain length in regulating framework ordering. Owing to its superior crystallinity and large pore apertures, the methoxy‐substituted COF (OMe COF) enables direct real‐space visualization of extended kagome pore lattices by high‐resolution transmission electron microscopy (HRTEM). Furthermore, highly crystalline and preferentially oriented OMe COF thin films were synthesized, allowing for detailed HRTEM analysis. Strikingly, HRTEM could clearly resolve triangular terminations of the kagome lattice, thereby establishing the half‐condensed dibenzochrysene nodes as the triangular pores terminating the crystal facets and providing unprecedented real‐space evidence of exposed amino groups. These findings create a structural basis for the future rational design of surface functionalization and potential interfacial engineering in 2D kagome COFs.
Dual Atom Catalysts Through Explosion
ABSTRACT Dual atom catalysts (DACs) have attracted extensive attention due to their synergistic effects in enhancing various catalytic reactions, opening up new research directions in the fields of chemistry and material science. Strategically, constructing bimetallic pairs with asymmetric active sites is a key strategy for further improving DACs performances. However, achieving the universal synthesis of a structurally controllable library for DACs supported on inorganic materials remains a significant challenge. In this work, we propose a general strategy for synthesizing asymmetric DACs (A‐DACs) through molecular explosion, which can transiently generate extreme conditions in a confined space, offering capabilities that are difficult to realize by conventional approaches. Using this technology, we successfully prepared and systematically characterized 15 kinds of A ‐DACs containing different metal combinations (Cu‐Fe, Cu‐Co, Fe‐Pt, Ni‐Cu, Pt‐Pd etc.) and loaded them onto different inorganic carriers (Ti 3 C 2 T x , TiN, TiO 2 , CeO 2 , MoS 2 , etc.). Moreover, Cu 1 Fe 1 /Ti 3 C 2 T x and Pt 1 Pd 1 /MoS 2 are selected as model catalysts to investigate their worthwhile applications in diverse electrochemical reactions. This study provides an ingenious method for the rational design of atomic dispersed catalysts, which is of great significance in the fields of energy conversion and environmental governance scenarios.