Selective hydrogenation of nitrobenzene to aniline is an environmentally relevant transformation for converting hazardous nitroaromatic compounds into value-added chemical intermediates under mild conditions. However, nitrobenzene hydrogenation over single-atom catalysts is often limited by the kinetic mismatch between H₂ activation at isolated metal sites and the sustained supply of reactive hydrogen to adsorbed nitro groups. Herein, we report a defect-rich boron nitride-supported Pd single-atom catalyst, Pd₁/u-d-BN, prepared via a urea-assisted ball-milling strategy. Isolated Pd atoms are stabilized in a well-defined Pd₁–N₄ coordination environment, enabling efficient nitrobenzene hydrogenation to aniline under ambient conditions with a turnover frequency of 3672 molNB·molPd−1·h⁻¹ , an aniline selectivity of 99.5%, and an apparent activation energy of 36.2 kJ mol−1. The catalyst also shows broad applicability toward substituted nitroarenes, affording the corresponding aminoarenes with high selectivity. Kinetic analysis, in situ spectroscopic characterization, and theoretical calculations reveal that Pd₁–N₄ sites promote H₂ dissociation and nitro-group activation, while adjacent vacancy defects act as transient reservoirs for spillover H species and mediate their local delivery to adsorbed nitro intermediates. This activation–spillover–buffering mechanism addresses the coupled limitations of H₂ activation and reactive hydrogen utilization in single-atom hydrogenation catalysis.

Catalytic hydrogenation of aromatic carboxylic esters (ACE) makes them intrinsic safe and environmentally friendly, meanwhile endowing with tailored functionalities (e.g., flexibility or weatherability). In this work, a Ru catalyst supported on porous boron nitride (Ru/p-BN) were prepared and applied in the hydrogenation of dimethyl terephthalate (DMT) to dimethyl 1,4-cyclohexanedicarboxylate (DMCD). The p-BN with rich B/N vacancies and boron-oxygen defects promoted the dispersion of Ru. The 2Ru/p-BN catalyst harbored Ru clusters with an average particle size of 1.86 nm, featured abundant Ru edge sites and a high proportion of Ru0. With this unique structure, its catalytic performance and stability were significantly enhanced, with a DMT conversion over 99 %, and a DMCD selectivity of 99.7 %, under 50 degrees C and 5 MPa. The initial reaction rate was 252 molDMT center dot molRu-1 center dot h-1 with a low activation energy of 21.2 kJ/mol. The edge sites Ru clusters were identified as the dominant active sites for the DMT hydrogenation based on further study. Besides, the catalyst showed wide applicability, providing guidance regarding future catalyst design to the hydrogenation of a range of ACE.

Diesel engines represent a major source of NOₓ and soot emissions in China, which are among the primary contributors to air pollution and pose substantial risks to public health. However, the efficient catalytic oxidation of soot particles, especially under NOx-assisted conditions, remains a critical challenge. Against this backdrop, the core objective of this work is to construct SnCo solid solution catalysts with precisely modulated morphologies to achieve efficient low-temperature soot oxidation under NOx-containing conditions. For this purpose, we adopted three different strategies to realize the controllable synthesis of SnCo composite oxides with targeted morphologies: complexation method for 1D nanorods, coprecipitation method for 2D nanosheets, and hydrothermal method for 3D nanoparticle aggregates. Our experimental results confirm that the SnCo solid solution obtained via the hydrothermal route (SC9–1-H) possesses a unique three-dimensional porous network framework formed by the aggregation of abundant ultrafine nanoparticles. Benefiting from this structural feature, the sample exhibits the highest specific surface area, richest mesoporous channels, as well as the maximum concentrations of oxygen vacancies, surface Co3+ active species, and acidic sites among all catalysts in this work. The structural characteristics endow SC9–1-H with optimal catalytic activity in both O2 and NO+O2 atmospheres. Particularly under NOx-assisted conditions, T50 reaches as low as 332 °C, coupled with the lowest apparent activation energy and the greatest reducibility. Mechanistic studies demonstrate that a dual-pathway reaction scheme involving active oxygen species and NO2 substantially accelerates low-temperature soot combustion. These findings provide meaningful guidance for the design and development of highly efficient low-temperature catalysts for diesel soot oxidation.

In this study, epsilon-MnO2 was modified via silver (Ag) loading and chemical reduction for catalytic ozone decomposition under extremely-low temperatures. The effects of various modification strategies on surface chemistry and catalytic performance were systematically investigated. At temperatures as low as -50 degrees C, oxygen vacancies (O-v) were identified as the primary active sites for ozone decomposition. Reduction modification significantly increased the concentration of oxygen vacancies, thereby enhancing catalytic performance. In particular, the NaBH4-reduced sample (MnO2-NaBH4) maintained a high ozone conversion (>90%) for up to 318 min. However, rapid catalyst deactivation remained a challenge due to the difficulty of oxygen-vacancy regeneration. Ag modification facilitated the regeneration of oxygen vacancies by promoting the desorption of peroxide intermediates. Density functional theory (DFT) calculations revealed that the introduction of Ag reduced the desorption energy barrier of peroxide species from 0.98 eV to 0.68 eV. However, excess Ag species will repair oxygen vacancies and cause channel blockage. By integrating NaBH4 reduction with an optimal Ag loading (1 wt.%), the resulting 1Ag-MnO2-NaBH4 catalyst achieved a synergistic balance between abundant active sites and efficient vacancy regeneration, maintaining over 80% ozone removal efficiency for 600 min at -50 degrees C.

Developing highly active catalysts for low-temperature ammonia decomposition is crucial for generating COx-free hydrogen, yet the reaction is fundamentally limited by sluggish N2 desorption kinetics. This study systematically uncovers the facet-dependent electronic interplay between Ru and CeO2 supported by tuning their nanoscale morphologies into five distinct shapes: rod, hollow sphere, broom, irregular particle, and cube. Among these, the rod-shaped Ru/CeO2 catalyst (Ru/CeO2-r) demonstrates exceptional low-temperature activity, achieving 100% NH3 conversion at 450 degrees C and a remarkable hydrogen production rate of 840 mmol & centerdot;gcat -1 & centerdot;h-1. Combined experimental characterizations and Density Functional Theory (DFT) calculations identify N2 desorption as the rate-determining step and reveal the underlying catalytic mechanism. The preferential exposure of the (110) facet on the rod morphology features a lower oxygen vacancy formation energy, which facilitates the transfer of abundant electrons from the CeO2 support to the Ru active sites, thereby lowering the valence state. This localized enhancement of the electron cloud density upon Ru effectively accelerates the recombinative desorption of N2, thereby unlocking superior catalytic performance. These findings provide a compelling structural and electronic design rationale for developing highly efficient Ru-based catalysts for hydrogen energy applications.

The development of eco-friendly, low-carbon materials from biomass resources has emerged as a strategic priority, driving the sustainable bio-based evolution of thermoplastic polyurethane elastomers (TPUs). However, the currently developed bio-based TPUs still face critical challenges including insufficient bio-based carbon content and compromised mechanical performance compared to conventional petroleum-based materials. Herein, a series of multifunctional fully biobased polyurethanes were developed using bio-based aliphatic 1,5pentamethylene diisocyanate (PDI), bio-based diols, linear 1,5-pentanediol (PDO), and rigid bicyclic isosorbide (ISO) by molecular design. The synthesized TPUs exhibit exceptional mechanical properties, including an ultimate tensile strength of 36.3-37.6 MPa, an elongation at break of 826 similar to 864 %, and excellent toughness (104-123 MJ/m(3)). As amorphous polyurethanes, these materials also demonstrate ultrahigh optical transmittance (>90 %). Furthermore, the resulting PCDL-ISO films displayed recoverable tensile properties, recyclability, thermally-induced shape memory functionality, enabled by the synergistic effects of reversible dynamic hydrogen-bonding networks, microphase separation between hard and soft domains, and thermally activated chain mobility. Notably, the comprehensive properties of these synthesized TPUs are comparable to those of petroleum-derived counterparts. This work provides a novel design strategy for the fabrication of highperformance intelligent materials from biomass resources, which is conducive to the development of biobased TPUs in the direction of eco-friendly and multifunctionality.

The synthesis of N-substituted carbamates through the carbonylation of amines with alkyl carbamates represents a green and promising route, yet it is hindered by insufficient catalytic efficiency and a lack of mechanistic understanding. In this work, a single-atom Bi-doped TiO2 (Bi1-TiO2) catalyst was synthesized using MIL-125(Ti) as the precursor for the carbonylation of amines with ethyl carbamate (EC). The optimized 5% Bi1-TiO2 catalyst demonstrated exceptional performance, achieving a high space-time yield of ethyl propyl carbamate (EPC) at 833 mmol center dot gcat-1 center dot h-1 with 99% selectivity, surpassing most reported catalysts. Mechanistic studies revealed that the 5% Bi1-doped TiO2 possessed a high density of Lewis acid sites of 256 mu mol/gcat. Dipropylurea (DPU) was identified as the key reaction intermediate. Both DPU and ethanol were preferentially activated on the Lewis acidic Bi delta+ sites. Further evidence indicated that electrons were populated into the anti-bonding orbitals of DPU from Bi, leading to significant activation of the N-(C=O) bond. This activation dramatically enhanced the carbonylation process by facilitating the alcoholysis of DPU. Additionally, the catalyst exhibited excellent stability for over 250 h and substrate universality across a range of amines for the synthesis of various N-substituted carbamates.

The efficient hydrogenation of nitroaromatics under mild conditions remains a significant challenge, particularly while retaining sensitive functional groups. Herein, we report a cobalt-based catalyst supported on nitrogen-doped carbon (10% Co@NC), which achieved 100% conversion and >99% selectivity in the hydrogenation of nitrobenzene at mild temperature (30 °C) and pressure (10 bar). The catalyst exhibited an exceptional space-time yield of up to 1.89 g·gcat-1·h-1, surpassing most reported cobalt-based catalysts. The catalyst demonstrated remarkable stability for over 400 h. The outstanding performance originated from the synergistic effect between the nitrogen-doped carbon support and the metallic cobalt particles. Such efficient hydrogenation under ambient temperatures is exceedingly rare among non-noble metal-based catalysts. In situ DRIFTS experiments and Density Functional Theory (DFT) calculations revealed that the nitrogen vacancy (Nv) in the carbon matrix played a pivotal role by giving rise to the spontaneous hydrogenation of the nitro group, thereby enabling the high-performance catalysis under mild conditions.

Heterogeneous catalysts for transesterification reaction are highly desirable, but normally suffer from low activity or severe deactivation. Here we report a Bi1-ceria catalyst for transesterification that exhibits catalytic activity of 2499 g1,2-BC gcat.-1 h-1 and stability for 800 h, in the synthesis of 1,2-butylene carbonates from 1,2-butanediol and dimethyl carbonate. Our study reveals that the constructed Bi1 does not serve as the conventional catalytic centre but regulates the acidity-basicity of the active sites through remote catalysis, realized by the induced delocalization of the f electron of Ce3+ and the remote propagation of electrons via the conductive lattice oxygen. The highly active sites lead to the Bi1 centred re-construction into BiOx during the reaction, which triggers tardily decline in catalytic activity. Nevertheless, the catalyst can be readily regenerated with thermal treatment by restoring the migrated oxygen. These findings open an avenue for the rational design of single-atom catalysts for transesterification reactions.

The selective hydrogenolysis of furfuryl alcohol (FFA) to 1,2-pentanediol (1,2-PeD) represents a promising route for biomass valorization, yet it remains challenging due to the competing over-hydrogenation of the furan ring and the recalcitrant C5-O bond cleavage. Herein, we report a highly efficient bimetallic Pt-Y catalyst supported on a MgO-AlO(OH) mixed oxide (MAO) that enables the selective hydrogenolysis of FFA to 1,2-PeD under remarkably mild conditions (140 °C, 0.8 MPa H2). Structural characterizations (AC-HAADF-STEM, XPS) confirm the formation of Pt-Y mixed clusters, which induce electron transfer from Pt to Y. This electronic modulation, combined with the tailored basicity of the MAO support, effectively suppresses the over-hydrogenation pathway while promoting the activation of the target C-O bond. In situ Fourier transform infrared spectroscopy shows that after the introduction of Y, FFA adsorbs on the catalyst surface in a vertical adsorption configuration through its O-H and C-O-C bonds, promoting the selective ring-opening. Consequently, the optimized 0.75Pt0.45Y/MAO catalyst achieves complete FFA conversion with an exceptional 1,2-PeD selectivity of 80.3% (110 mol 1,2-PeD·mol Pt per h), significantly outperforming its monometallic counterparts. Furthermore, the catalyst demonstrates outstanding stability in a continuous-flow reactor for over 200 hours without obvious deactivation. This work provides a strategy for designing synergistic bimetallic catalysts for the sustainable production of 1,2-PeD under mild conditions.

This study investigated the effects of zero-valent iron (ZVI) on the leaching behavior of selenium (Se), chromium (Cr), arsenic (As), and boron (B) from fly ash, which was utilized as the cementitious material in cement systems. Toxicity characteristic leaching procedure (TCLP) tests were conducted under acidic and alkaline conditions, with or without amino acids. In the acidic leaching test, ZVI prohibited the leaching of Cr through redox reactions, whereas alkaline conditions predominantly facilitated stabilization via hydrocalumite and ettringite formation. The reduction of Cr(VI) to Cr(III) through ZVI occurred preferentially, and the transformation of Se (IV) to Se(0) seemed not to be promoted due to the limited redox-active sites and surface passivation of ZVI. The role played by ZVI in anions leaching behavior was not affected by amino acids. From the perspective of the existence of amino acids, the stabilization of anions was enhanced by amino acids. H2Asp improved Se and Cr retention, while H2Cys enabled Cr leaching below the maximum contaminant level value through reductive dissolution, even in ZVI-containing systems. Notably, ZVI showed negligible immobilization effects on As and B. These findings demonstrate that ZVI combined with Ca-based additives effectively enhances Cr(VI) immobilization in fly ash-blended cement blocks, rather than Se(IV). This work provides a valuable reference for applying iron-based reductants in multi-anion containment systems.

Diesel engines represent a major source of NOR and soot emissions in China, which are among the primary contributors to air pollution and pose substantial risks to public health. However, the efficient catalytic oxidation of soot particles, especially under NOx-assisted conditions, remains a critical challenge. Against this backdrop, the core objective of this work is to construct Sn-Co solid solution catalysts with precisely modulated morphologies to achieve efficient low-temperature soot oxidation under NOx-containing conditions. For this purpose, we adopted three different strategies to realize the controllable synthesis of Sn-Co composite oxides with targeted morphologies: complexation method for 1D nanorods, coprecipitation method for 2D nanosheets, and hydrothermal method for 3D nanoparticle aggregates. Our experimental results confirm that the Sn-Co solid solution obtained via the hydrothermal route (SC9-1-H) possesses a unique three-dimensional porous network framework formed by the aggregation of abundant ultrafine nanoparticles. Benefiting from this structural feature, the sample exhibits the highest specific surface area, richest mesoporous channels, as well as the maximum concentrations of oxygen vacancies, surface Co3+ active species, and acidic sites among all catalysts in this work. The structural characteristics endow SC9-1-H with optimal catalytic activity in both O2 and NO+O2 atmospheres. Particularly under NOx-assisted conditions, T50 reaches as low as 332 degrees C, coupled with the lowest apparent activation energy and the greatest reducibility. Mechanistic studies demonstrate that a dual-pathway reaction scheme involving active oxygen species and NO2 substantially accelerates low-temperature soot combustion. These findings provide meaningful guidance for the design and development of highly efficient lowtemperature catalysts for diesel soot oxidation.

Methyl diphenylmethane dicarbamate (MDC) was synthesized by condensation of methyl phenylcarbamate (MPC) using trioxane as methylenation reagents over sulfonic acid resin catalyst. The effect of Brønsted's acid amount on the condensation reaction was investigated, and the optimal sulfonic acid resin (NKC-9) with an acid amount of 4.57 was determined. 2-MDC, featuring a methylene-bridged biphenyl structure, achieved 91.6% selectivity and 83.2% yield after response surface methodology optimization. In situ FTIR spectroscopy was employed to monitor the condensation process. The spectroscopic results unequivocally demonstrate that trioxane undergoes catalytic depolymerization to formaldehyde over NKC-9 resin, which subsequently reacts with MPC to form MDC. After sulfuric acid regeneration, NKC-9 maintains its catalytic performance after 4 cycles.

Helium-3 (He-3), an important isotope, serves as a crucial working substance and raw material in various scientific fields. However, its extremely low natural abundance poses a significant challenge for efficient extraction. Cryogenic distillation is a promising method but its operation near the superfluid transition temperature of helium-4 (He-4) risks disruption by superfluidity. This study investigates the enrichment characteristics of trace He-3 under total reflux using a 2 K cryogenic distillation. The experiments show that, under the present operating conditions, when the column is entirely within the superfluid helium (He-II) regime (T < 2.176 K), no stable axial temperature gradient can be established, and effective distillation is not observed. This behavior is attributed to the exceptionally high effective thermal conductivity and film-flow effect of He-II, which suppress temperature gradients and disturb the vapor-liquid countercurrent structure. In contrast, upon entering the normal-fluid (He-I) regime, stable thermodynamic gradients can be formed, enabling effective distillation. With a feed concentration of He-4 /He-4 = 0.15 & times; 10(-7), the system could stably maintain a top enrichment factor of 150-270 in the He-I regime. This work clarifies the decisive role of superfluidity in the distillation process, defines the feasible operating window, and lays an experimental foundation for the cryogenic distillation test of helium isotopes.

The further development of forward osmosis (FO) technology has been constrained by intrinsic limitations including low water flux and pronounced concentration polarization. To improve this, three nanostructured materials MOF-801(Zr), CAU-1(Al), and their hierarchical nanocomposite MOF-801(Zr)@CAU-1(Al) were synthesized with superior hydrothermal stability and precisely tunable porosity. These nanomaterials were subsequently incorporated into cellulose acetate (CA) FO membrane through phase inversion and the optimal synthesis conditions were explored, yielding three distinct mixed-matrix membranes (MMMs) including CA/MOF-801(Zr) FO-MMM, CA/CAU-1(Al) FO-MMM, and CA/MOF-801(Zr)@CAU-1(Al) FO-MMM. Comparative evaluation of separation performance demonstrated that the nanomaterials modified membrane achieved optimal performance enhancements, with higher water flux and reverse salt flux relative to pristine CA membrane. Notably, the CA/MOF-801(Zr)@CAU-1(Al) FO-MMM exhibited superior antifouling characteristics with an optimal value of 84.26 L/(m2∙h) in water flux and 1.65 g/(m2∙h) in reverse salt flux. In seawater desalination applications, the nanocomposite integration significantly reduced flux loss and enhanced the performance recovery ability of CA membranes after fouling, with a flux recovery rate of over 90%. The CA/MOF-801(Zr)@CAU-1(Al) FO-MMM performed the highest water flux. Although its salt rejection rate was lower than that of commercial FO membrane supplied by Hydration Technology Innovations, LLC (HTI, Albany, OR, USA), it remained higher than those of the CA/MOF-801(Zr) FO-MMM and CA/CAU-1(Al) FO-MMM. Therefore, this work provides a reference to select advanced additives which promoting the desalination performance and anti-fouling property for FO membrane in seawater desalination.

Helium isotope separation is essential for both producing ultra-high-purity 4He required in precision low-temperature physics experiments and recovering scarce 3He for advanced technological applications. Superleak filtration provides a simple method for continuous, high-throughput helium isotope separation; however, reliable in situ measurements of the downstream flow rate and investigations of upstream 3He enrichment remain limited. In this work, a visualized cryogenic superleak filtration system was developed to investigate the flow and separation behavior of helium isotopes. A coaxial superleak element packed with compacted Al2O3 powder was innovatively coupled to a collecting pot and a glass-tube level indicator, enabling real-time monitoring of the downstream liquid-level rise. At a fixed bath temperature, the flow rate increased linearly from 0.03 to 0.05 g/s as the heating power at the downstream end of the superleak increased from 0 to 30 mW. The measured flow rates agree well with theoretical predictions, indicating that the superfluid flow remained in the laminar regime under the tested conditions. Full-volume recovery experiments further showed that superleak filtration can reduce the 3He concentration in the feed gas by approximately one order of magnitude, from the 10-8 level to the 10-9 level. These results demonstrate that the proposed visualized system provides an effective platform for quantifying superleak flow regulation and evaluating helium isotope separation performance.

The carbonylation of amines offers a promising route for synthesizing N-substituted carbamates with high atom economy. However, conventional catalysts exhibit limited catalytic efficiency, and the underlying proton transfer mechanism remains elusive. Herein, we reported a metal-free, room-temperature strategy utilizing 1,5,7-triazabicyclo[4.4.0]dec-5-ene (TBD) as a dual hydrogen bond catalyst to synergistically activate propylamine (PA) and dimethyl carbonate (DMC). This green catalytic system achieves a 10-fold acceleration in reaction rate compared to other hydrogen bonding catalysts under mild conditions. This is enabled by dual hydrogen bonding of TBD with PA and DMC, which facilitates rapid proton transfer and stabilizes tetrahedral intermediates. Theoretical calculations confirm that the dual hydrogen bond system significantly lowers activation energy compared to single hydrogen bond analogs. Furthermore, it was revealed that the hydrogen bonding network within the product is the primary factor responsible for the sluggish reaction rate. This study demonstrates the effectiveness of a dual hydrogen bond system in accelerating the carbonylation of amines and provides a green route to access carbamates.

Bio-based pentamethylene dicarbamate (PDC) serves as a crucial intermediate in the synthesis of bio-based pentamethylene diisocyanate (PDI) via a non-phosgene route, and its carbonylation synthesis holds significant scientific and industrial importance. In this study, niobium-doped ceria (NbxCe) catalysts were designed and synthesized for the carbonylation reaction between pentanediamine (PDA) and methyl carbamate (MC). The catalytic performance of CeO2 on the carbonylation of PDA was promoted by the surface modulation by Nb doping. Nb0.06Ce achieved a space-time yield of PDC up to 32.4 gPDC·gcat.-1·h-1, which was 1.4 times higher than that of CeO2. The catalysts were characterized by XRD, BET, TEM, XPS, EPR, NH3/CO2-TPD, and Py-IR. Catalyst characterization results suggested that the superior catalytic performance of Nb0.06Ce may be attributed to the synergistic combination of high oxygen vacancy concentration, abundant surface-adsorbed oxygen species, plentiful acid-base sites, and a large specific surface area. In-situ FTIR analysis confirmed that the alcoholysis of polyurea intermediates was a key step in the synthesis of PDC, and this process was notably accelerated in the presence of the catalyst. In-situ DRIFTS further indicated the Nb0.06Ce facilitated the adsorption and activation of reactants. In the catalytic reaction, the polyurea intermediate was activated by the acid-base sites on the surface of NbxCe, generating the final product PDC. The Nb0.06Ce catalyst demonstrated excellent stability, maintaining its catalytic activity after multiple reaction cycles. Furthermore, it was successfully applied to the efficient carbonylation synthesis of various aliphatic carbamates, highlighting its broad applicability.

Single-atom catalysts for alkyne semi-hydrogenation have been extensively investigated due to their high metal utilization and improved olefin selectivity. However, their reactivity is hindered by the sluggish activation of reactants on isolated sites. Herein, a non-precise metal catalyst consisting of Ni-Cu hetero-diatomic pairs was prepared using a sequential deposition method. The diatomic sites catalyst exhibited an unprecedented activity among non-precious catalysts with over 98% conversion and 77 molC2H2 molmetal -1 h-1 at 180 degrees C, whereas the single-atom catalysts of Cu/C and Ni/C were almost inert under the same conditions. Experimental and theoretical results revealed the crucial diatomic synergy between the Ni-Cu pairs, wherein acetylene was adsorbed on Ni sites and hydrogen was adsorbed on Cu sites, and the diatomic site enabled spontaneous desorption of ethylene. The superior activity of the diatomic catalyst was observed, resulting from the enhanced dominance of d-electrons of Ni near the Fermi level. The research demonstrates an approach to designing non-precise metal catalysts with extraordinary catalytic performance for alkyne hydrogenation. (c) 2025 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.

ABSTRACT The development of high‐strength, on‐demand debondable, and recyclable adhesives from renewable resources remains a major challenge. Herein, we present a facile strategy to construct robust, low‐molecular‐weight adhesives with thermally and electrically triggered debonding from sustainably sourced tannic acid and DL‐carnitine hydrochloride. The adhesive exhibits outstanding adhesion on various substrates, with a maximum adhesion strength of 14.4 MPa on ceramics. This superior strength originates from dense interaction sites and rich noncovalent interactions, which facilitate the multidimensional synergistic enhancement of both cohesive and adhesive energies. Notably, ionic moieties reorganize the hydrogen‐bond network, generating additional interfacial donors and acceptors that strengthen substrate adhesion. Remarkably, the adhesive allows for on‐demand debonding either thermally (75°C) or electrochemically (10 V, 60 s), triggered by the disruption of noncovalent interactions and oxidation of catechol or pyrogallol to quinone, respectively. Moreover, the adhesive can be recovered by water immersion, and the monomers can be efficiently separated and recovered via ethanol treatment. This work proposes a novel strategy for regulating adhesion performance via ionic moieties and establishes a new paradigm for triggered debonding through electrochemical oxidation.