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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ORGANIC & BIOMOLECULAR CHEMISTRY
·
2026
·
IF 2.8
Lin Chen,Shuang Xu,Zhiming Chen
Direct α-C(sp3)−H arylation of 4-aminopyrazolones involving arynes, enabled by dual phase-transfer catalysis and ultraviolet irradiation, has been developed. The dual phase-transfer catalytic pathway powered by triaminocyclopropenium salts gave rise to the generation of structurally diverse 4-amino-4-arylpyrazolones in moderate to excellent yields, while the photochemical protocol furnished the products with moderate yields. Notably, these products are tentatively proposed as candidates for carbamate pesticides based on the preliminary structural analysis. The synthetic potentials of the methods were shown by gram-scale reactions, and the possibilities for greater structural diversity of the product were highlighted by derivatizations. The results of control experiments indicated that the timely capture of the transient arynes by the activated 4-aminopyrazolone nucleophiles is the key to the success of the reactions.
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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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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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PHOSPHORUS SULFUR AND SILICON AND THE RELATED ELEMENTS
·
2017
·
IF 0.809
Huili Ma,Shuyun Liu,Shaohua Zhu,Wenzhu Bi,Xiaolan Chen,Yufen Zhao
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POLYMER COMPOSITES
·
2026
·
IF 4.9
Jie Chen,Qingjun Ding,Gai Zhao,Huafeng Li,Lin Yang,Guoqing Wang
Polyimide (PI)-based tribological composites containing carbon fiber (CF), molybdenum disulfide (MoS 2 ), and other solid lubricants have been extensively studied. However, the role of hexagonal boron nitride (h-BN) in regulating interfacial interactions and wear mechanisms in PI/CF/MoS 2 systems remains insufficiently understood. In this study, the effects of h-BN incorporation on the mechanical and tribological behaviors of PI/CF/MoS 2 composites were systematically investigated through experimental characterization combined with molecular dynamics (MD) simulations. The results revealed that h-BN addition improved hardness while reducing tensile strength and ductility due to the enhanced interfacial restriction and increased stress concentration. The tribological performance exhibited a non-monotonic dependence on h-BN content, with the optimal performance achieved at 5 wt.% h-BN. Scanning electron microscopy (SEM) and energy-dispersive X-ray spectroscopy (EDS) analyses suggested that an appropriate h-BN content facilitated the formation of a relatively continuous transfer film, whereas excessive h-BN promoted filler agglomeration and interfacial degradation, leading to accelerated wear. Furthermore, MD simulations suggested that the reduced molecular mobility and fractional free volume at the optimal h-BN content were consistent with enhanced interfacial stability. The combined experimental and simulation results provide qualitative insights into the role of h-BN in regulating filler dispersion, interfacial interactions, and molecular chain dynamics. These findings establish a structure–property relationship for designing high-performance multi-filler PI-based tribological composites. Highlights Hexagonal boron nitride improves the hardness but reduces tensile strength. Friction and wear are minimized at 5 wt.% hexagonal boron nitride loading. Excess hexagonal boron nitride triggers agglomeration and abrasive wear. Molecular dynamics simulations corroborate experimental wear mechanisms.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Shuai Wang,Yue Gu,Yu Feng,Ziru Zhao,Shufeng Shen
Nonaqueous amine-based absorbents offer advantages over aqueous monoethanolamine (MEA), but they inevitably evolve into water-lean systems when treating humid flue gas, presenting a challenge for long-term performance stability. In this work, a formulated water-lean absorbent, 50B-40BE-10 W, was evaluated for CO 2 capture from simulated humid flue gas in an upgraded lab-scale continuous plant over 720 h, benchmarking it against 30 mass% MEA. Key operational parameters and water balance behavior were systematically investigated to inform rational process design. Under a framework of absorbent-tailored regeneration strategy coupled with dynamic water-balance control, the 50B-40BE-10 W solvent achieved a remarkably low desorber heat duty, about 50–65% reduction compared to MEA. Critically, a dynamic water-management strategy was proposed and demonstrated, involving controlled discharge of desorber overhead condensate following a membrane dehydration process. This approach successfully maintained stable water content of ∼10 wt% in the solvent over a 100-h period, effectively addressing the challenge of water accumulation in water-lean systems. Furthermore, NMR analysis of the absorbent after ∼1700 h of operation, even under high‑oxygen exposure, indicated no catastrophic degradation. The compelling performance and stability demonstrated at the bench-scale pave a solid pathway for further development of this advanced water-lean capture technology.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Hao Yu,Jiakai Shi,Jiaqi Wen,Shi Liu,Jingyu Cai,Linxi Hou
Permittivity is a key parameter characterising the polarisation capacity of a dielectric, and directly influences a material’s signal transmission and energy storage properties. As electronic devices evolve towards higher frequencies and greater integration, there is an increasing demand for polymer materials that combine low dielectric constant with excellent thermal and environmental stability. In this study, a aluminium-based metal-organic framework material CAU-10-H, which exhibits negative thermal expansion, was synthesised using the hydrothermal method and incorporated into PEEK matrix by hot-press to prepare CAU-10-H/PEEK composite films. The as-obtained CAU-10-H is relatively well dispersed within the PEEK matrix at low-to-moderate filler loadings, while its incorporation is associated with a reduction in the dielectric constant of the composite. The reduced dielectric response is mainly attributed to the introduction of low-polarity nanoporous domains, while the increase in free volume fraction may also contribute to this behaviour. When the filler content is 5 wt%, the composite exhibits a low die This may be attributed to the following factors:lectric constant across the 2–18 GHz frequency range, with an average value as low as 2.45, whilst the thermal decomposition temperature is above 500℃. In addition, this composite material offers moisture resistance, excellent dimensional stability, outstanding frequency stability and good signal integrity. This study provides new insights into the regulation of the high-frequency dielectric properties and stability of polymer composites using microporous materials with negative thermal expansion characteristics. Download: Download high-res image (181KB) Download: Download full-size image Owing to the inherent microporous structure of MOFs and their interaction with the polymer matrix, this composite material achieves a dual reduction in both the dielectric constant and dielectric loss at high frequencies, whilst exhibiting excellent thermal stability and superior moisture resistance.
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Small
·
2026
·
IF 11.8
Jiacheng Zheng,Yulong Deng,Wenting Chen,Chengliao Deng,Xiaoming Cai,Jinming Cai,Honglin Tan
Zinc indium sulfide (ZnIn 2 S 4 , ZIS), a visible-light-responsive photocatalyst, has garnered significant attention due to its facile synthesis, high stability, suitable band gap, and abundant active sites. This study innovatively constructed a CNT@Ag@ZIS tubular structure, introducing Ag mediators as electron donors at the CNT-ZIS interface. Results demonstrate that the Ag mediators establish clear interfacial contact with both hexagonal ZIS and CNT. Consequently, ZIS exhibits markedly enhanced photocurrent response and improved separation efficiency of photogenerated charge carriers. The catalyst achieved a remarkable hydrogen evolution rate of 18.44 mmol g −1 h −1 , representing an 8.7-fold enhancement over pristine ZIS. The study revealed that Ag, with its high Fermi level, facilitates interfacial electron transfer to ZIS. This induces a downshift of the p-band center (3p orbitals of S) in ZIS, simultaneously prolonging the H─S bond length and increasing the antibonding orbital occupation. This electron restructuring creates electron-rich S (2+δ)− active sites, substantially lowering the H 2 desorption energy barrier. Thus, the surface reaction kinetics of the sulfide are optimized through a regulation strategy targeting antibonding orbitals.
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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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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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