Journal of the American Chemical Society
·
2026
·
IF 16.6
Jian-Hua Chen,Zi-Tong Long,Kun-Yu Cai,Hui-Jie Tu,Hong-Cai Wu,Fei-Qin Bian,Lin-Dong Liu
Fenton-like reactions are fundamental to environmental remediation, yet conventional electron-centric frameworks overlook critical proton transfer contributions. Here, we demonstrate that strategic modulation of proton transfer enhances heterogeneous Fenton-like reactivity by two orders of magnitude through validated proton-coupled electron transfer (PCET) mechanisms. Two complementary strategies emerged: modifying catalyst surface hydroxyl density and tuning solution pH. Mechanistic investigations revealed that hydroxyl modifications alter the surface O–H bond dissociation free energy (BDFE), while pH adjustments follow Brønsted–Evans–Polanyi (BEP) relationships. We developed electrochemical methods for quantifying BDFE alongside techniques for measuring net H• transfer rates involving surface hydroxyl groups. This paradigm transcends electron-centric approaches by establishing comprehensive theoretical frameworks for reaction enhancement and by providing transformative proton-transfer-based modulation strategies to overcome inherent activity limitations in practical Fenton-like applications.
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高影响因子
Science Bulletin
·
2026
·
IF 20.7
Ying Feng,Zhiquan Hou,Peijie Ma,Xiaohui Yu,Xun Wang,Kun Zheng,Yuxi Liu,Zhihua Wang,Zhenxia Zhao,Jiguang Deng,Hongxing Dai
The activation of C–H bonds is a fundamental process in various chemical reactions, while faces significant challenge under mild conditions due to the high bond energy and low polarity. An ultrathin (∼3 nm) amorphous oxygen-containing carbon layer inserted into Pt/TiO 2 yields C–O–M (M = Pt and Ti) dual interfaces. The photothermocatalytic consumption rate of n -heptane over Pt/C/TiO 2 at 140 ℃ is 8.8 and 61.8 times higher than that over Pt/TiO 2 and Pt/C, respectively. Temperature-programmed desorption (TPD) and density functional theory (DFT) calculations reveal that the constructed C–O–M interfaces significantly enhance the adsorption of hydrocarbon reactant, and decrease the C–H bond scission energy barrier. The photothermal X-ray photoelectron spectroscopy (XPS), femtosecond transient absorption (fs-TA) and electron paramagnetic resonance (EPR) experiments demonstrate that the C–O–Ti interface accelerates the electron migration and transforms the adsorbed oxygen into the superoxide species, thus efficiently oxidizing the reactant. Furthermore, introduction of an amorphous carbon layer to Pt/Al 2 O 3 , Pt/CeO 2 , Ce/TiO 2 or Cu/TiO 2 remarkably enhances the photothermal catalytic performance for propane, pentane, octane, toluene or hexanal oxidation. The unique effect of C–O–M dual interfaces induced via the ultrathin amorphous carbon layer provides a guideline for designing catalysts with efficient C–H bond activation ability.
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高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 2
·121666
·
IF 7.5
Jianjun Chen,Qian Zhao,Hongxing Shi,Ying Li,Limin Wang
The coexistence of cationic and anionic dyes in wastewater necessitates the development of amphoteric adsorbents. Herein, amphoteric hydrogel microspheres SA-S@PDA-H was successfully fabricated for their simultaneous removal. The microspheres were synthesized by crosslinking sodium alginate (SA) with Ca²⁺, followed by coating with polydopamine (PDA) and stearyl trimethyl ammonium chloride (STAC). The microspheres prepared through acid treatment to replace STAC was labeled SA-S@PDA-H, endowing the microspheres with enhanced adsorption capacity. FT-IR, SEM, zeta potential was utilized to characterize the structure and morphology of SA-S@PDA-H. The adsorption behavior and mechanism of SA-S@PDA-H for cationic and anionic dyes was investigated in depth. The results show SA-S@PDA-H exhibit 127.3 % of swelling ratio. The adsorption of SA-S@PDA-H for MB and MO reaches equilibrium at about 300 min followed by PSO model. The adsorption process of SA-S@PDA-H for MB and MO followed Temkin and Dubinin-Radushkevich model, respectively, and the maximum adsorption capacity displayed 869.1 mg/g at 45°C and 730.9 mg/g at 15°C, for MB and MO, respectively. MB adsorption increased with higher temperature and pH, while MO adsorption increased with lower temperature and pH. Adsorption of both dyes decreased at high ionic strength, and Cu 2 + and Fe 3+ had a significant inhibitory for MB than K + , while the inhibitory effects of SO 4 2- or CO 3 2- is more obvious for MO than Cl - . SA-S@PDA-H exhibited excellent adsorption performance for mixed cationic and anionic dyes through synergistic effects including electrostatic interactions, hydrogen bonds, π-π stacking and micropore filling. The microspheres maintained over 80 % removal efficiency after five consecutive adsorption-desorption cycles.
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Polymers
·
2026
·Vol. 18
·期 5
·578
·
IF 5.8
Wei Wang,Xueping Gao,Zhimin Li,Yishi Wang,Bo Zhu
Carbon-fiber-reinforced polymer (CFRP) composites possess outstanding specific stiffness and strength but typically exhibit low intrinsic damping, which limits vibration attenuation in lightweight dynamic structures. Herein, a hybrid toughening strategy combining carboxyl-terminated butadiene nitrile rubber (CTBN) and hexagonal boron nitride (h-BN) is developed to enhance the damping of CFRP laminates while preserving cure feasibility and thermomechanical stability. An E51/DICY/accelerator epoxy system (100:6.5:1.2, mass ratio) is used as the baseline matrix. Differential scanning calorimetry shows that both CTBN and h-BN shift the cure peak temperature upward (Tp: 160.6 → 170.3 °C) and reduce the reaction enthalpy (ΔH:386.5 → 255.1 J/g), indicating dilution/transport effects and altered cure kinetics. Dynamic mechanical analysis (DMA) reveals that CTBN exhibits an optimum damping enhancement at 25 phr (tan δ_max= 0.300), whereas h-BN provides a stronger monotonic increase up to 25 phr (tan δ_max= 0.437). Notably, the CTBN/h-BN hybrid (25/25 phr) delivers a hightan δ_maxof 0.468 together with the broadest effective damping window (ΔT_half= 28.6 °C), exceeding 85% of the linear additivity criterion proposed herein. When the materials are transferred into CFRP laminates, free-vibration tests (using the logarithmic decrement method) demonstrate a clear structural damping improvement (ζ:0.021 → 0.035;δ:0.132 → 0.221; t1/2: 0.48 → 0.27 s). Overall, the results suggest that the damping enhancement arises from a combination of EPBN-mediated ductile energy dissipation and h-BN-related interfacial/interlayer frictional losses, which can be jointly tuned to balance processability, thermal response, and damping performance in CFRPs.
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ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Zhenzhen Wu,Xiaoyu Wu,Wenting Liu,Songfeng Liang,Jiaming Luo,Mengyang Li,Yang Wang
Zinc-air batteries, widely regarded as a frontrunner in sustainable energy storage solutions, struggle with performance constraints stemming from the insufficient activity and durability of bifunctional oxygen electrocatalysts. This research presents a composite catalyst (FeCo@Fe-N-CNTs) synthesized through a straightforward in situ growth method, effectively integrating FeCo alloys with Fe single atoms incorporated in nitrogen-doped carbon nanotubes (N-CNTs). Theoretical and experimental studies show that FeNx atoms weaken the interaction between active iron sites and reactants, enhancing the reaction energy optimization. The optimization improves the characteristics of the intermediates’ adsorption and desorption, enabling the catalyst to exhibit remarkable bifunctional activity under alkaline conditions, achieving an overall overpotential as low as 0.67 V, with overpotential of merely 290 mV for the oxygen evolution process. The performance boost stems from a 38% larger electrochemical surface area (ECSA) combined with an 18% lower charge transfer resistance (Rct), pointing to gains in both active site numbers and intrinsic catalytic efficiency. We also employed X-ray absorption spectroscopy (XAS) and in situ Raman measurements to probe the Fe–Nx bonding configuration and track how the surface changes under the working conditions. Notably, zinc-air batteries using dual-function catalyst reached a peak energy density of 894 mAh g–1, maintained stable cycling for over 3000 h, and exhibited consistent charge–discharge capabilities in flexible quasi-solid-state devices (with voltage fluctuation remaining under 5% during bending strain), highlighting its immense potential for practical use in creating compact, high-capacity rechargeable batteries that can be worn or carried around. It is like giving us the keys to unlock a world where we can seamlessly incorporate portable energy solutions for renewable energy projects.
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ACS Nano
·
2026
·
IF 17.3
Tian Tong,Min Xu,Entian Cui,Zhongye Cao,Qiu Wan,Fangmu Wang,Shuai Yin,Meng Tian,Gazi Hao,Wei Jiang,Jinhua Ye,Guigao Liu
Photocatalytic methanol coupling holds great promise for the sustainable production of value-added ethylene glycol (EG) and hydrogen yet remains challenging due to the difficulty in achieving selective C–H activation associated with spin-state transitions. Here, we develop a spin-polarized photocatalyst (sp-Mo1/ZCS) by anchoring asymmetric spin-state Mo single-sites onto ZnCdS, enabling selective C–H activation through quantum spin exchange interactions. Consequently, it demonstrates exceptional EG selectivity (97.6%), yield (236.2 mmol g–1), turnover number (1417.2 molEG molMo–1), and catalytic durability (over 100 h) in photocatalytic methanol coupling, with the EG production rate outperforming standalone ZnCdS by over an order of magnitude. We reveal that the spin-polarized Mo single-sites enhance surface polarization, thereby accelerating charge-carrier separation and migration. More importantly, they facilitate the spin-state transition of C–H activation to generate •CH2OH and the subsequent C–C coupling, consequently improving the selectivity and efficiency of EG synthesis. This study highlights the pivotal role of spin-implantation in steering C–H activation for efficient photocatalytic methanol coupling and related reactions.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·123598
·
IF 7.5
Di Li,Huimin Zhu,Yuan Zhang,Shaofei Yang,Ruiyu Zhu,Jiaoe Dang,Fang Song,Jun Zhou
The escalating global energy crisis and environmental pollution has drawn increasing attention. As a green and sustainable alternative, photocatalytic H 2 O 2 synthesis has attracted widespread interest. In this study, we has designed a novel exciton-regulated photocatalyst (Bi@g-C 3 N 4 /ST-NS) by integrating bismuth-doped graphitic carbon nitride with porphyrin-based supramolecular nanostructures (ST-NS). The composite was synthesized through a sequential process involving solvothermal reaction, high-temperature calcination, and solution-phase self-assembly. We systematically investigated its crystal structure, photoelectronic properties, and the mechanistic basis of photocatalytic H 2 O 2 production. Characterization results confirmed the successful incorporation of Bi single atoms into the sixfold cavities of g-C 3 N 4 , forming a p-n heterojunction with ST-NS while preserving the crystallinity of the host matrix. The built-in interfacial electric field not only promoted efficient charge separation but also extended the visible-light absorption range and prolonged the carrier lifetime. Performance evaluations revealed that Bi@g-C 3 N 4 /ST-NS exhibited significantly enhanced H 2 O 2 generation activity compared to pristine Bi@g-C 3 N 4 , with optimal performance achieved at a 10:1 mass ratio. Under visible-light irradiation, the H 2 O 2 concentration reached 1134 μM in the reaction solution, representing a 2.5-fold improvement over Bi@g-C 3 N 4 . Mechanistic studies indicated that the heterojunction facilitated efficient intersystem crossing from singlet to triplet excitons. Rather than following the conventional superoxide radical (·O 2 - ) pathway, these triplet excitons activated ground-state oxygen to generate singlet oxygen ( 1 O 2 ) via resonance energy transfer. The subsequent highly selective two-electron reduction of 1 O 2 yielded H 2 O 2 , effectively circumventing the high-energy barrier steps associated with traditional pathways. This work thus presented a promising strategy for the rational design of high-efficiency photocatalytic systems through exciton regulation.
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Molecular Catalysis
·
2026
·
IF 4.3
Jinwei Wu,Junfei Chen,Lining Fang,Mingkang Zhang,Zebao Rui
H-Beta supported InO x -IrO x dual-function active sites with abundant acid sites are designed. • Synergy of InO x -IrO x regulates surface redox properties and InO⁺ species generation. • InO⁺ species and acid sites facilitates NO conversion while IrO x sites promote CH₄ activation. • IrIn/H-Beta demonstrates superior CH 4 -SCR performance. In the field of selective catalytic reduction of nitrogen oxides with methane (CH 4 -SCR), achieving a balance between high CH 4 -SCR selectivity and high CH 4 activation ability remains challenging. Herein, InO x -IrO x dual-function active sites anchored on the H-Beta zeolite with abundant acid sites are rationally designed. The InO x -IrO x bimetallic oxide structures and the confinement effect of the zeolite framework effectively suppress the migration and sintering of IrO x species, while the electron transfer between In and Ir facilitates the formation of Ir-O-In bond and the generation of InO⁺ species. The In sites, together with the acid sites of H-Beta, assist the conversion of NO into NO 3 - and NO⁺ species, while the CH 4 is predominantly dissociated on Ir sites to form In-CH 3 species via the Ir-O-In bond. These In-CH 3 species react with nitrate species on adjacent InO⁺ sites to form reactive intermediates such as CH 3 NO 2 , which further interact with NO⁺ to produce N 2 , CO 2 , and H 2 O. Owing to the dual functionality of InO x -IrO x active sites, the as-designed IrIn/H-Beta simultaneously achieves superior performance of 81% NO x conversion and 100% CH 4 conversion at 500°C under a gas velocity of 120,000 mL g -1 h -1 . Such proposed dual-function bimetallic catalyst design strategy demonstrates potential for developing a catalyst with high activity and high selectivity in CH 4 -SCR reactions. The as-proposed dual-function bimetallic IrIn/H-Beta catalyst demonstrates high activity and high selectivity in CH 4 -SCR reactions. Download: Download high-res image (193KB) Download: Download full-size image
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ACS Omega
·
2026
·Vol. 11
·期 30
·45485-45493
·
IF 5.2
Ye Zhixuan,Chen Xingshu,Zhang Linxin,Wang Jun,Chen Hanxian,Zhang Xinxiang,Zhao Weiwei,Yuan Zhanhui
The abundant hydrophilic
hydroxyl groups and porous structure make
wood highly susceptible to moisture absorption from the environment,
leading to issues such as deformation and decay. This work aims to
in situ construct a multifunctional organosilicon/organic hybrid resin
coating on the wood surface derived from the click reaction of polymethylhydrosiloxane
(PMHS), using PMHS, divinylbenzene (DVB), and the Karstedt catalyst.
At room temperature, through the Si–H addition click reaction
between PMHS and DVB, a cross-linked and rigid hybrid resin coating
with a hardness of 94.00 HA is fabricated on the wood surface. Simultaneously,
a dehydrogenation click reaction takes place between the Si–H
groups of PMHS and the –OH groups on the wood surface, anchoring
the hybrid resin coating to the wood via covalent bonds. These endow
the hybrid resin coating with excellent mechanical stability. The
low surface energy of organosilicon resin in the hybrid coating affords
the modified wood with good waterproofness by decreasing the 24 h
water absorption rate from 78.6% to 13.9%. Most importantly, the coating
remains hydrophobic even after being immersed in an alkaline solution
(pH = 13) for 24 h. SEM images of the coating after alkaline corrosion
indicate that while the Si–O–Si skeleton of the organosilicon
component is partially dissolved due to its susceptibility to alkali,
the hydrophobic organic resin skeleton remains intact, imparting good
alkali resistance to the hybrid resin coating. In summary, the organosilicon/organic
hybrid coating constructed via the click reaction of PMHS on the wood
surface effectively addresses the issue of poor alkali resistance
commonly associated with traditional organosilicon coatings.
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高影响因子
ENERGY CONVERSION AND MANAGEMENT
·
2022
·
IF 11.533
Zechang Wei,Chenyang Cai,Yu Fu
To reach global carbon neutralization, the use of clean energy and biomaterials has become a trend to reduce CO 2 emission. With the increasing concerns about freshwater shortage and crude oil pollution, water purification and sewage treatment have become particularly urgent. Solar energy is an environment-friendly energy to mitigate freshwater shortage stress and reduce crude oil pollution. However, how to make solar energy applied to effectively drive freshwater generation and crude oil pollution remedy is crucial. Herein, the electrospun membrane was explored as sustainable matrix with desirable solar-to-thermal performance. The strategy of spectrum-tailoring was proposed to tailor bandgap energy of vanadium disulfide (VS 2 ) for photothermal conversion promotion and interfacial evaporation efficiency. Inspired by mussel, dopamine was polymerized on surface of VS 2 (VS 2 @PDA) for spectrum tailoring (Solar absorptance, α, is 89.34 %). Bandgap energy of the complex favorably decreased from 2.06 to 1.41 eV. Combining the dual H-bonding networks, water evaporation enthalpy of the membranes dramatically decreased from 2370 to 1990.2 J/g and the resulted evaporators showed excellent salt resistance, with evaporation rate of 1.40 kg m -2 h −1 (enhancement factor is 2.032) and extraordinary cyclic evaporation performance. Additionally, sunflower-inspired tilting model was architectured to eliminate disturbance of sun irradiation incident angles for effective solar-driven interfacial generation. The resulted membrane effectively treated the seawater and decreased high viscosity of the super-viscous crude oil under the sun irradiation, thus showing great potential in seawater treatment and crude oil pollution remedy. The designs maximized utilization of solar energy and evaporation rates by treating seawater and reducing crude oil pollution without consuming additional energy, thus contributing to carbon neutralization. Therefore, the integration of dual H-bonding networks and spectrum-tailoring strategies would facilitate the structure-functional unification and desirable photothermal capabilities, and bring about an application potential in the development of composite evaporators for carbon neutralization.
研究领域:
材料科学
·
环境科学
·
能源科学
·
化学工程
·
可持续技术
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高影响因子
FUEL
·
2018
·
IF 4.908
Peng Lu,Dongming Shen,Shilin Cheng,Emmerson Hondo,Linet Gapu Chizema,Chengwei Wang,Xikun Gai,Chengxue Lu,Ruiqin Yang
Liquefied petroleum gas (LPG, C3 and C4 paraffins) from syngas have attracted much attention recently due to the growing demand of non-oil resource as well as its environmentally friendly features, but the catalytic reaction process controlled by thermodynamics and CO conversion rate is low with many side reactions. Here we report a catalyst with core shell structure for LPG synthesis from syngas. Zeolite as shell was synthesized by hydrothermal method firstly and then coated on Cu/ZnO core with Ludox (CZ@Z), the Cu/ZnO core was prepared by co-precipitation method. The unique core shell structure had efficient synergistic effect. The reaction equilibrium favored forward reaction because methanol as an intermediate was directly transformed to dimethyl ether. The zeolite type in the core shell structure catalyst had great effects on the activity and selectivity. The catalysts have been characterized by XRD, NH 3 -TPD and SEM. The activities were determined after in situ H 2 reduction. CZ@H-β catalyst showed a more effective catalytic activity compared with the traditional hybrid catalyst. The excellent catalytic performance was attributed to the combined contribution of both unique core shell structure and proper zeolite type. At these reaction conditions, temperature of 350 °C, pressure of 3.0 MPa and flow rate of 40 ml min −1 , CO conversion and hydrocarbons selectivity achieved 61.8% and 64.2%, respectively. LPG selectivity in hydrocarbons was 70.2%.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2022
·Vol. 139
·期 24
·52335
·
IF 3.057
Hao Zhang,Ying Jun Li,Jun Zeng,Hui Ping Liu,Yuan Lin Zhou
In order to solve the problem of poor thermal conductivity of polymer-based radiation shielding composite materials, h-BN@PDA@PbWO 4 hybrid powders were prepared by combining h-BN with high thermal conductivity and PbWO 4 with γ shielding. With the assistance of polydopamine, PbWO 4 particles were synthesized in situ on the h-BN surface. The effects of h-BN@PDA@PbWO 4 on thermal conductivity, γ-ray shielding, and mechanical properties of chloroprene rubber were studied. The results showed that the hybrid particles had better dispersibility than the pure mixing of h-BN and PbWO 4 in chloroprene rubber and significantly improved the thermal conductivity gamma-ray shielding performance and mechanical properties of CR composites. When the filler content of the hybrid powder reaches 40 wt%, the thermal conductivity of the composite is about 3.16 times that of the pure CR. The γ shielding rates at 86.5 KeV and 105.3 KeV photon energies increase by 14.14% and 17.61% compared with the pure CR. Compared with pure CR, the tensile strength of the composites increased by 4.79 MPa, and the elongation at break decreased slightly. These were because h-BN@PDA@PbWO 4 shows had an excellent synergistic effect in CR substrate. The new kind of CR/h-BN@PDA@PbWO 4 composite can be used for thermal management and gamma shielding.
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