Small Methods
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2026
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IF 8.7
Xiaochen Feng,Zihao Huang,Mingwei Fang,Meiling Wang,Jinyue Ma,Zewen Wang,Ying Zhu,Lei Jiang
Electrochemical CO 2 reduction (CO 2 RR) to ethanol offers a sustainable route for carbon utilization and energy storage, yet achieving high ethanol selectivity under limited CO 2 availability remains a significant challenge. The central issue is the lack of quantitative understanding of how the interfacial * CO and * H intermediates jointly govern product selectivity. Here, we establish an interfacial coverage regulation strategy by embedding Cu nanoparticles into an imine-functionalized covalent organic framework (Cu/Im-COF). The imine-rich interface enriches CO 2 adsorption while modulating proton transfer, enabling a balanced surface coverage of * CO and * H, identified as the key selectivity descriptor ( θ *CO/*H ) for ethanol formation. Operando Raman spectroscopy, density functional theory calculations, confirms that an optimized θ *CO/*H stabilizes the * HCCHOH intermediate and lowers its formation barrier. Quantitative integration of Raman features allows direct determination of θ *CO/*H , revealing a volcano-type dependence of ethanol selectivity on this descriptor. A maximum ethanol Faradaic efficiency of 56% is achieved at log( θ *CO/*H ) ≈ 3.0, a current density of 700 mA cm − 2 , and a 15% CO 2 feed. This work establishes θ *CO/*H as a quantitative bridge between intermediate coverage and reaction kinetics, providing a mechanistic framework for rational design of CO 2 RR catalysts with high ethanol selectivity under CO 2 -constrained conditions.
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2026
·Vol. 123
·期 9
·e2533803123
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IF 9.5
Guobin Wen,Haiqi Liang,Shuxuan Liu,Ningce Zhang,Shuai Chen,Guoqiang Shen,Tehua Wang,Ru Chen,Li Tao,Bohua Ren,Shuangyin Wang
Electrochemical hydrogen isotope separation has been constrained for decades by the similar energy barriers of the rate-determining O–H and O–D bond cleavage step in water isotopologues. Herein, we compact H-bond connectivity through screening a series of additives to stimulate electrochemical proton quantum tunneling (QT) behaviors of “through-barrier”, which are virtually impossible for heavier D-relevant motions. The average H-bond length of H2O⋯OH− is 3.4% shorter (2.78 Å) with isopropanol additive at the engineered interface. Fundamentally, QT effects are magnified by selectively promoting proton transfer-involved reactions through strengthening the H-bond and filling the H-bond gap, which are further proved by both experimental Arrhenius plots with near small-curvature tunneling approximation and a stronger proton excursion in path integral molecular dynamics simulations. Hence, a record-high H2O separation factor of 276 is realized at room temperature with a three-order-of-magnitude growth of H/D kinetic isotope effect constant up to 10,165. Significantly, a large-scale multistage reactor is engineered to obtain continuous enrichment of heavy water with a deuterium atomic fraction over 80%.
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MATERIALS CHEMISTRY AND PHYSICS
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2022
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IF 4.778
Yuhong Nong,Licai Fu,Jiajun Zhu,Wulin Yang,Deyi Li,Lingping Zhou
To meet the criteria of high specific power thermal battery development, all-lithium molten salt electrolytes (LiF–LiCl–LiBr) are often employed in thermal batteries. In this work, a hexagonal boron nitride binding molten salt electrolyte (h-BN-E) was synthesized using a straightforward liquid nitrogen mixing process and high temperature calcination , which using h-BN as a binder in electrolyte. The h-BN-E has a low internal resistance (0.21 Ω) and a high discharge voltage (2.5 V), which is close to the theoretical discharge voltage (2.64 V). The h-BN-E with high specific capacity (329 mAhg −1 ) and specific energy (700 W h kg −1 ) at the same time. It can be demonstrated that h-BN has the capacity to more effectively immobilize the electrolytes at high temperature discharge when combined with the discharge overflow diagram. The investigation of h-BN as a binder for thermal batteries with low internal resistance can be started with the help of this work.
研究领域:
储能技术
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材料科学
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电化学
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热电池
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COMPOSITES COMMUNICATIONS
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2026
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IF 7.7
Yujie Yang,Huixing Lin,Jiaqi Li,Yang Gao,Xiaogang Yao,Haiyi Peng
Efficient thermal management is a critical challenge for next-generation electronics, where conventional polymer-based materials suffer from inherently low thermal conductivity. Inspired by natural honeycomb structures, we developed a freeze-casting strategy to fabricate high-performance hexagonal boron nitride (h-BN)/polysilylaryl-enyne (PSAE) composites exhibiting enhanced thermal conductivity. By leveraging the unidirectional crystallization of tert-butyl alcohol (TBA), a highly ordered h-BN honeycomb scaffold was constructed, facilitating the formation of efficient phonon conduction pathways. The composites, with a low h-BN (10 μm) ratio of 23 vol%, exhibit an outstanding omni-directional thermal conductivity of 4.71 W/(m·K) along the z-axis and 3.44 W/(m·K) along the x-axis, significantly outperforming conventional polymer composites. Moreover, dielectric characterization confirms that the honeycomb structure enhances anisotropic dielectric behavior ( ε rz = 3.68, ε rx = 3.32, for h-BN (10 μm) at 23 vol%). The proposed bioinspired approach presents a scalable and effective route for developing lightweight, thermally conductive composites for advanced electronic applications.
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MOLECULES
·
2026
·Vol. 31
·期 15
·2595
·
IF 5.1
Jie Chen,Ying Zhou,Yishao Wang,Fujing Huang,Fangming Zou,Shunmei He,Xianwen Song
Small-molecule blending is an effective strategy for improving the mechanical properties of poly(vinyl alcohol) (PVA). However, the influence of structural differences among phenolics on the toughening mechanism remains unclear. In this study, we systematically investigated the reinforcing effects of three trihydroxy-phenolics (apigenin, galangin, and baicalein) on PVA hydrogels by combining molecular simulations with experimental validation. Molecular simulations predicted that H-bonding crosslinking between phenolics and PVA chains is the central reinforcement mechanism, and that the spatial arrangement of hydroxyl groups and the competition between intermolecular H-bonding ultimately determine the performance. Structural characterization and experimental validation showed that apigenin, owing to the dispersed spatial distribution of its three hydroxyl groups, exhibits stronger H-bonding crosslinking ability and achieves the most significant reinforcement. After a single freeze–thaw cycle, all trihydroxy-phenolics/PVA composite hydrogels exhibited markedly better mechanical properties than pure PVA hydrogels, with the following strength order: apigenin/PVA > galangin/PVA ≈ baicalein/PVA. This study provides a rapid and efficient theoretical model and a reference case for small-molecule toughened PVA hydrogels.
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CHINESE JOURNAL OF CATALYSIS
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2026
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IF 17.2
Yiwei Zhao,Zuhang Jin,Cheng Tao,Rui Du,Yongzheng Shi,Chao Zhang
The synthesis of KA oil (a cyclohexanone-cyclohexanol mixture) from guaiacol through mild electrocatalytic approach represents a sustainable strategy for biomass valorization. Herein, we report the electrocatalytic conversion of guaiacol to KA oil over the reduced Pt/TiO 2 catalysts. The TiO 2 -induced hydrogen spillover effect facilitates strategic modulation of H ads (H*) coverage on Pt surfaces, thereby effectively suppressing competitive aromatic ring hydrogenation and excessive hydrogen evolution reactions. Comparative studies of electrocatalysis and thermocatalysis have demonstrated that Pt active sites serve as the dominant catalytic centers. However, H spillover significantly influences reactivity and selectivity, particularly in the electrocatalytic pathways. The electrocatalytic system demonstrates preferential C–O bond cleavage with KA oil selectivity around 70%. This work provides valuable insights into the regulation of metal-support interactions in the design of electrocatalysts.
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Materials Today Chemistry
·
2026
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IF 7.4
Mengjiao Zhao,Xianjie Xu,Sheng Huang,Xiuquan Gu,Wufan Xuan
The CsCu 2 I 3 /ZnO-heterojunction-based sensor enables H 2 S detection with a response value of 0.83 at 1 ppm, with response and recovery times of 240 s and 834 s. • The CsCu 2 I 3 /ZnO heterojunction improves structural stability and ensures continuous and stable sensor response. • The CsCu 2 I 3 /ZnO-heterojunction-based sensor achieves self‐calibration for different H 2 S concentrations with 99% detection accuracy. Hydrogen sulfide (H 2 S), a colorless and toxic gas, poses serious health risks upon prolonged exposure, including damage to respiratory and cardiovascular systems, which can be fatal in severe cases. Current H 2 S sensors suffer from limited response, particularly in detecting ultra‐low concentrations. To overcome this limitation, we developed a CsCu 2 I 3 /ZnO heterojunction‐based gas sensor via vacuum evaporation. This composite material enables highly responsive H 2 S detection at room temperature. The heterojunction not only improves structural stability but also ensures continuous and stable sensor response. At 1 ppm H 2 S, the sensor exhibits a sensitivity of 0.72, the response value of 0.83, the limit of detection (LOD) of 14.25 ppb, with response and recovery times of 240 s and 834 s, respectively. Furthermore, an intelligent calibration framework was developed by integrating Gramian Angular Summation Fields with the AlexNet algorithm, operating as a robustness enhancer. The sensor achieves self‐calibration for different H 2 S concentrations with 99.33% detection accuracy through 5-Fold Cross-Validation, significantly enhancing quantification capability. These results demonstrate the excellent potential of our CsCu 2 I 3 /ZnO-heterojunction-based sensor in H 2 S monitoring. The combination of responsive materials with machine learning offers a robust strategy for advancing ultra‐low concentration gas detection technologies.
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CHINESE JOURNAL OF CATALYSIS
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2026
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IF 17.2
Chengyang Sun,Haochen Zhang,Xiaohui Liu,Yanqin Wang
Catalytic hydrogenolysis offers a promising route for plastic waste upcycling. Herein, we demonstrate that oxygen vacancies (O V ) in CeO 2 supports dramatically enhanced this process. Reduction-engineered Ru/CeO 2 -NH 3 -800 exhibits 40% higher activity at 800 °C than untreated counterparts. Comprehensive characterization revealed unchanged Ru metal sites after treatment, but significantly increased oxygen vacancy content in the CeO 2 support. Isotopic C 6 –D 2 temperature-programmed surface reaction studies revealed that higher O V concentrations correlate with lower C–H bond activation temperatures, directly aligning with observed activity trends. We propose a novel Ru–Ce interfacial mechanism: O V -adjacent Ce 3+ –O sites activate C–H bonds to form *RCCR* intermediates, while dual Ru sites cleave C–C bonds via C–Ru coordination. This work establishes an O V -driven structure-activity relationship for the first time and reveals support-mediated C–H activation as crucial for advanced catalyst design.
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TURKISH JOURNAL OF CHEMISTRY
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2026
·Vol. 50
·期 3
·285-299
·
IF 2
LI JUANHONG,WANG SUQIN,LIU XIN,LIU FENG
A [H]-accelerated catalytic Fenton system was developed using Pd/UiO-66(Zr)-F4 as the catalyst. This system enabled the regeneration of Fe²⁺ and facilitated the continuous generation of both ·OH and 1O2 through [H]-mediated electron transfer at ambient temperature and pressure. Under the conditions of 0.2 g L−1 catalyst (Pd loading 0.516 wt%), 25 μM Fe2+, 60 mL min−1 H2 flow (as the [H] source), 20 mM H2O2, and pH 3, approximately 89% of carbamazepine (initial concentration 20 mg L−1) was degraded within 3 h using trace iron. However, the catalytic activity of Pd/UiO-66(Zr)-F4 gradually declined from 89% to 53% over six reaction cycles. This decrease was likely due to loss of specific surface area caused by microstructural degradation associated with hydrogen spillover effects.
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CERAMICS INTERNATIONAL
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2026
·
IF 6
Peng Chu,Lindong Ma,Hongli Liu,Zongwei Zhang,Yuhao Liu,Weiqiang Xie,Wenshuo Cao,Mingwei Li,Yuanhang Zhou
Aluminum borate fibers are promising candidates for high-temperature thermal insulation owing to their excellent thermal stability, good chemical resistance, and relatively low density. Herein, we report a simple method for preparing porous Al 18 B 4 O 33 /h-BN composite fibers via electrospinning and stepwise heat treatment, using an aluminum isopropoxide/aluminum nitrate (AIP-AN) complex as the aluminum source and nanoscale h-BN as the boron source. The incorporation of h-BN not only promotes the in-situ formation of the Al 18 B 4 O 33 phase but also affects the fiber's pore structure. Meanwhile, the heterogeneous interface formed between h-BN and the Al 18 B 4 O 33 may introduce additional interfacial thermal resistance, thereby synergistically reducing thermal conductivity and improving thermal insulation performance. The resulting composite fibers exhibited a highly porous structure, with a high specific surface area of 53.9175 m 2 g −1 , a low density of 0.025 g cm −3 , and a low thermal conductivity of 0.0417 W m −1 K −1 . The porous Al 18 B 4 O 33 /h-BN composite fibers demonstrate significant potential for thermal insulation in extreme environments, offering a viable approach to developing high-performance ceramic fiber insulation materials.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Mohan Zhang,Yu Zhang,Jiayi Meng,Jiajie Wang,Jiaqi Du,Hongwei Chen,Yifan Liao,Yuchen Wei,Quanmei Zhou,Yuying Hu,Yakun Song,Hongyan Zhao,Wei-Lin Dai
Organic/inorganic CdSe/TpBpy-COF S-scheme heterojunction for H 2 O 2 photosynthesis. • Molecularly intimate interface by in-situ solvothermal growth for rapid electron transfer. • Strong internal electric field and band bending drive the S-scheme charge transfer pathway. • An exceptional H 2 O 2 yield of 4349 mmol·g −1 ·h −1 in pure water without sacrificial agents. • DFT reveals thermodynamically spontaneous "downhill" 2e - oxygen reduction pathway. Photocatalytic H 2 O 2 production via oxygen reduction represents a sustainable pathway for solar-to-chemical energy conversion. However, constructing sacrificial-agent-free heterojunctions that simultaneously maximize charge separation and preserve redox ability remains a significant challenge. Herein, we report a molecular-level interfacial engineering strategy to anchor COF-TpBpy onto CdSe nanorods via in-situ solvothermal growth, fabricating a strongly coupled organic–inorganic S-scheme heterojunction. Benefiting from the intimate interfacial contact, the optimized 10CdSe/TpBpy composite achieves a remarkable H 2 O 2 yield of 4349 μmol·g⁻¹·h⁻¹ in pure water without any sacrificial agents, alongside an impressive apparent quantum yield (AQY) of 11.1% at 450 nm. Mechanistic investigations, combining Density Functional Theory (DFT) calculations, Kelvin probe force microscopy (KPFM), and in-situ irradiated X-ray photoelectron spectroscopy ( in-situ XPS), visually confirm a robust built-in internal electric field (IEF) driven by the work function difference. Furthermore, femtosecond transient absorption (fs-TA) spectroscopy reveals an ultrafast picosecond-scale interfacial charge transfer behavior, providing direct kinetic evidence for the S-scheme mechanism. This unique charge transfer pathway effectively preserves the strong reducing electrons in the CdSe conduction band to boost the oxygen reduction reaction (ORR) kinetics. This work offers a viable paradigm for designing robust hybrid S-scheme architectures for efficient photocatalysis. Download: Download high-res image (167KB) Download: Download full-size image
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Yuhui Lv,Xinyu Gao,Binghui Guo,Xinyi Li,Chenhui Sun,Suhang Wang,Rongshi Jing,Jiaxin Chen,Liying Pu,Min Zhang,Yanyan Liu,Gang Wang,Yucheng Ren,Tiantian Gu
Organic materials have attracted considerable attention in rechargeable aqueous zinc-ion batteries (AZIBs) due to their sustainability and structural tunability. However, the electrochemical performance of existing organic electrodes is severely constrained by limited redox-active sites, high solubility and short conjugated backbones. Herein, a conjugated N-heterocyclic anhydride-based framework, benzoquinone-fused dianhydride (NTBQ), was constructed via solid-state condensation to enable highly reversible Zn 2+ /H + storage. The strategic integration of C=O groups triggers intramolecular electrostatic potential reconstruction and activates adjacent C=N sites, enabling fast and thermodynamically spontaneous multi-electron Zn 2+ /H + co-insertion. The rational structural design endows the NTBQ cathode with a remarkable initial discharge specific capacity of 434.6 mAh g −1 at 0.05 A g −1 and excellent rate capability. Moreover, the extended π-electron delocalization significantly strengthens intermolecular π-π interactions, enhancing the dissolution resistance of NTBQ in aqueous electrolytes and affording long-lasting cycling durability (88.1% retention after 10,000 cycles at 10 A g −1 ). Systematic mechanistic studies demonstrate that the superior electrochemical performance originates from the synergistic redox chemistry of C=O/C=N dual-active centers within the anhydride-based skeleton. These findings demonstrate that intramolecular electronic modulation can effectively evoke multi-electron redox activity, providing an effective avenue for designing high-performance organic cathodes toward advanced AZIBs. Structural optimization from NTPH to NTBQ via incorporation of additional C O groups induces intramolecular electrostatic potential redistribution, enhancing π-electron delocalization and activating adjacent C N sites. This creates synergistic C O/C N dual-redox centers for efficient multi-electron Zn 2+ /H + co-insertion. Download: Download high-res image (130KB) Download: Download full-size image
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