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ChemistrySelect · 2024 ·Vol. 9 ·期 45 ·e202404657 · IF 1.9

Synthesis of Diones via Visible Light-Induced Oxidation of α-Hydroxy Ketone Derivatives

Chenyue Zhao,Heran Yang,Shuo Hu,Yaqian Liu,Dongping Cheng,Xiaoliang Xu

Graphical In the presence of CBrCl3 and ruthenium photocatalyst, the corresponding dione was obtained by visible light induced oxidation of α-hydroxyl ketone derivatives with the yield of 49%–95%. It has the advantages of medium to excellent yield, good functional group tolerance, and mild reaction conditions. A visible light-induced oxidation of α-hydroxy ketone derivatives is reported, which is carried out in the presence of CBrCl 3 and ruthenium photocatalyst, and the corresponding diketones are obtained in 49-95% yields. This reaction has the advantages of moderate to excellent yields, good functional group tolerance, and mild reaction condition. The free radical reaction process was confirmed by the addition of radical scavenger 2,2,6,6-tetramethylpiperidi-1-oxy (TEMPO). The fluorescence quenching experiment indicated that CBrCl 3 was participated in the oxidation quenching cycle.

研究领域: 有机化学 · 光化学 · 合成化学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Multifunctional roles of TEMPO-oxidized cellulose nanofibrils on the enhancement of mechanical and conductive properties of acrylic-based hydrogels for temperature response and human motion sensing

Jintang Luo,Tao Song,Tingting Han,Haisong Qi,Qunhua Liu,Thomas Rosenau

Simultaneously having competitive mechanical properties, fatigue-resistant stability, temperature adaptability, excellent conductivity and sensitivity has been a challenge in the design of acrylic-based conductive hydrogels if they are meant for application in electronic skin mimics capable of sensory and stimulus responses. In this work, an acrylic-based conductive hydrogel with both excellent mechanical and electrical properties was prepared based on an integrated strategy employing the multifunctionality of TEMPO-oxidized CNFs (TOCNFs) and metal ion interaction. The TOCNFs with their abundant –COOH groups played a key role in the hydrogel by a) well-dispersing polyacrylic acid (PAA) chains in the hydrogel to form a homogeneous and porous multi-network, b) furnishing more –COOH to interact with Fe 3+ , c) forming more hydrogen bonds with PAA and glycerol, and d) offering high modulus to the final hydrogel. The obtained optimal hydrogel showed competitive mechanical properties (0.88 MPa at 70 % compressive strain; 0.24 MPa at 873 % tensile strain) and fatigue-resistant properties (56.5 % strength retention after 500 cycles of 50 % compression; 51.7 % strength retention after 20 cycles of 200 % tensile), high electrical conductivity (2.45 S m −1 ) and sensitivity (GF up to 2.62 for tensile strains over 100 %), while still maintaining a high electrical conductivity (1.67 S m −1 ) at −25 °C. Accordingly, the hydrogel prepared in this work was able to act as an electronic skin that responds to temperature variations and detect human body movement of pressing, writing, stretching and bending with highly sensitive conductive signals, which endows it great potential for applications in humanoid robotics and multi-scenario strain sensing.

CAS / MDL: 7727-54-0 110-26-9
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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

Boosting the catalytic activity of Cu2O via forming composite with both Cu and metal oxides MO2 (M = Mo and W) by tuning its band structure and Lewis acidity

Yi Pei,Jie Li,Zhaoyang Wang,Wei Zhong,Chunxin Lu,Zhongquan Shen,Nianlong Qian,Xiaoming Liu

In this work, composite materials (Cu-Cu 2 O/MO 2 , M = Mo and W) and their thermally treated form were prepared and characterized by using a variety of spectroscopic techniques (XRD, SEM, HRTEM, XPS and UPS) and cyclic voltammetry. Their catalytic performance on aerobic oxidation of various alcohols under mild conditions was investigated with N-methylimidazole (NMI) and 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) as the co-catalysts. Of the materials, the thermally treated MoO 2 -based material exhibited the best performance and durability. Compared to Cu-Cu 2 O, the involvement of MO 2 significantly enhances the catalytic activity on the oxidation. Our results suggest that the presence of MO 2 not only raises the energy level of VBM of Cu 2 O which is beneficial to O 2 activation and generates internal electric field pointing to the catalytic center (Cu 2 O) which would accelerate the electron transfer from the substrate to the catalyst through forming heterojunction with both Cu and MO 2 , but also disperses the catalytic center. Further, the Lewis acidity of MO 2 with appropriate strength can bring the substrate closer to the catalytic center via adsorption. But appropriate acidity is essential as easy on–off adsorption is desired in the catalysis. Thermal treatment generates oxidation state VI species of stronger acidity which offsets the effect of the raised VBM energy level.

研究领域: 催化 · 材料科学 · 化学工程 · 物理化学
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JOURNAL OF CATALYSIS · 2025 · IF 6.5

Electron-rich Cuδ+-O-Con+ boosts active site reconfiguration to trigger multi-pathway C-O bond hydrogenolysis activation in lignin

Zong-Pin Fu,Qi-Jie Zhou,Yun-Peng Zhao,Yu-Fa Wu,Fang-Jing Liu,Mei Zhong,Jian Li,Jing Liang,Jing-Pei Cao

The abundant bridging bonds and side chains in lignin make the selective cleavage of its C-O bonds a promising approach for achieving efficient conversion. Herein, Cu/CoOx-CeO 2 catalysts were prepared and the effects of their physical and chemical structures on C-O bond hydrogenolysis activity were investigated. The results indicated that incorporating an appropriate amount of CeO 2 as a support facilitated the doping of Co n+ cations into the CeO 2 lattice, enhancing oxygen vacancy concentration. Additionally, the Cu K-edge X-ray absorption near-edge structure (XANES) spectra revealed that Cu exists in a mixed valence state (Cu δ+ , 0 < δ < 2) within the catalyst. Reaction pathway regulation was achieved through strategic modulation of reaction conditions. When isopropanol was used as the solvent under a N 2 atmosphere, 2-phenoxy-1-phenylethanol (2-PPE-ol) was completely converted at 180 °C within 2 h, yielding ethylbenzene and cyclohexanol with 100 % selectivity. Conversely, when n -hexane was employed as the solvent, dehydrogenation of the C α -OH group generated hydrogen radicals, which promoted cleavage of the C β -O bond in the β-O-4 ketone intermediate, resulting in phenol and 1-phenylethanol with 100 % selectivity. Isotopic labeling and active hydrogen tracking experiments revealed that the active hydrogen in catalyst transfer hydrogenolysis (CTH) originated from the solvent, whereas self-hydrogen-transfer hydrogenolysis (SHTH) relied on hydrogen derived from the C α -OH group of 2-PPE-ol. This work provides valuable insights into the directional conversion of lignin into high-value chemicals and efficient energy utilization.

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Journal of Energy Chemistry · 2025 · IF 14.9

Dynamic covalent bond-mediated suppression of phase segregation in wide-bandgap perovskites

Xiyue Wang,Na Wang,Xinyu Yuan,Mengyao Guo,Jinling Zhang,Yanlin Song,Ziqiu Ren

Phase segregation triggered by illumination is a typical stimulus response in wide-bandgap perovskites, and addressing it is vital for overcoming the stability bottleneck of perovskite devices by mitigating phase segregation and implementing dynamic management. To tackle this, a dynamic covalent bond-mediated approach is proposed to deal with phase segregation in wide-bandgap perovskites. Results show that adding dynamic disulfide and diselenide bonds effectively suppresses phase segregation while keeping halogen homogeneity. A 1.77 eV wide-bandgap perovskite device attains a peak conversion efficiency of 21.02% and retains over 90% of its initial efficiency after 1200 h of continuous illumination at the maximum power point. A fabricated perovskite/perovskite tandem device reaches an optimal conversion efficiency of 28.45%. Incorporating dynamic covalent bonds presents a new strategy for mitigating phase segregation in wide-bandgap perovskites and is expected to drive further progress in this area.

CAS / MDL: 2564-83-2 882-33-7
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Materials Today Chemistry · 2025 · IF 6.7

The application of dual-function ionic liquids-hydrogel in the bidirectional non-interference effect of benzoylurea insecticides extraction and dye degradation

Hongmei Liu,Boyue Zheng,Zhengxue Ge,Mengyun Liu,Caihong Tao,Fangbin Fan

The analysis and treatment of hazardous substances in food have long been constrained by the dual challenges of limited single-target recognition capability and low resource utilization efficiency. To overcome these limitations, this study developed an ionic liquid-hydrogel material using a polymerization technique. The material featured a stable porous nanostructure and exhibited dual functionality, enabling highly efficient photo-catalytic degradation and adsorptive extraction. Under optimized conditions, it achieved a degradation rate of over 90 % for the dye Amaranth and extraction recovery exceeding 85 % for three benzoylurea pesticides. Mechanistic studies using in-situ IR spectroscopy revealed that the material's efficient and synergistic pretreatment capability for the two distinct classes of pollutants was attributed to the high substrate specificity of its active sites, which ensured that the two pathways operated independently without interference, guaranteeing the reliability of the treatment process. In conclusion, the developed dual-functional material combining with the advantages of low cost, ease of preparation and environmental friendliness provided an innovative strategy for the simultaneous pretreatment of multiple food contaminants and represented a significant advancement in this field.

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JOURNAL OF MEMBRANE SCIENCE · 2025 · IF 9

Photoinduced passivation-directed growth of δ-MnO2 nanosheets with excellent hydrophilicity for advanced pervaporation desalination membranes

Runzhang Tao,Jian Lu,Shilong Li,Weihu Zhang,Zhongkai Shan,Yuqing Sun,Wenheng Jing

Designing stable, high-performance two-dimensional (2D) MnO 2 membranes for pervaporation (PV) desalination remains challenging. Herein, we present a photoinduced surface passivation strategy for the controlled growth of ultrathin single-layer δ-MnO 2 nanosheets, combined with layer-by-layer assembly to fabricate robust PV membranes. The e − / h +  dual-path mechanism of photoinduced synthesis of MnO 2 was firstly proposed. Comprehensive structural characterizations and DFT simulations reveal that h +  drives surface passivation stabilizes the thermodynamic configuration, while e − modulating growth kinetics to achieve narrow lateral size distributions of nanosheets. Moreover, the process generates Mn 3+ states (Mn (III) ≈ 49.96 %), abundant oxygen vacancies and surface hydroxyls, imparting exceptional hydrophilicity (water contact angle ≈ 10°) and enabling ultrafast water transport through the 2D channels during PV. The resulting MnO 2 membranes exhibit nearly complete salt rejection (99.9 %) and an impressive water flux of 36.53 kg m −2  h −1 in high-salinity feeds, outperforming state-of-the-art membranes. This work establishes photoinduced facet passivation as an effective route for precision-controlled growth of 2D nanosheets, opening promising avenues for next-generation PV membranes and other water purification technologies in harsh environments.

CAS / MDL: 2564-83-2 7722-64-7
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Biomimetic adhesive-free self-splicing enables scalable wood film for programmable hygromorphic soft actuators

Wenbo Che,Yufeng Miao,Yifan Liu,Runxuan Wang,John Moyo,Youming Yu,Wenhui Bao,Yunyan Peng

Stimulus-responsive actuators play a crucial role in the next-generation intelligent systems. However, challenges such as complex fabrication processes, limited sustainability, and poor tolerance to complex deformations remain. This study introduces a sustainable “top-down” self-splicing strategy to fabricate spliced transparent wood film (TWF) for programmable hygromorphic soft actuators. Natural wood was subjected to delignification followed by TEMPO-mediated oxidation, yielding TWF with exceptional hygroscopicity. Two adhesive-free self-splicing methods: biomimetic “Mortise and Tenon” interlocking and self-adhesion using oxidized wood fibers enable arbitrary shaping and large-scale integration of spliced TWF. Since hydrogen bonding dominates interfacial bonding strength, the self-spliced TWF exhibits excellent tensile strength (up to 131.8 MPa), surpassing most plastic films and TWF joined with commercial adhesives. Interestingly, benefiting from the hygroscopicity and designability of self-splicing TWF, the resulting hygromorphic soft actuator achieves continuous rapid deformation and recovery, and programmable morphing into complex configurations ( e.g. , spirals, biomimetic mimosa and petals). This adhesive-free self-splicing approach enables the scalable production of TWF and yielding soft actuators with versatile morphing capabilities, low production cost, and sustainability, highlighting their potential in soft robotics and smart materials.

研究领域: 材料科学 · 软体机器人 · 智能材料 · 可持续工程 · 仿生学
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CARBOHYDRATE POLYMERS · 2025 · IF 12.5

3D-printing of hierarchical porous monoliths using emulsion gels stabilized by lignin-containing cellulose nanofibrils for thermal insulation

Chuhang Liu,Xiaojie Shi,Bo Lin,Zekun Song,Feng jiang,Mei-Chun Li,Chaozheng Liu,Changtong Mei

3D printing of cellulose-based porous materials with tailored architecture is of significant interest for advanced thermal insulation applications. However, most existing approaches lack internal hierarchical porosity, thereby limiting their insulation efficiency. Here, we propose an emulsion gel ink strategy based on high internal phase Pickering emulsions (HIPPEs) stabilized by lignin-containing cellulose nanofibrils (LCNFs) and reinforced with sodium alginate (SA). This approach integrates emulsion templating with direct ink writing (DIW), enabling simultaneous control of macroscopic geometry and microscopic pore structure. LCNFs with tunable lignin content and surface charge effectively stabilize oil–water interfaces, while SA provides a viscoelastic matrix, ensuring high printability. After freeze-drying, the printed porous monoliths exhibit low density (~17.7 mg·cm −3 ), high porosity (> 98 %), and hierarchical pores templated by emulsified droplets and LCNF-SA network. The resulting structures combine excellent mechanical resilience and low thermal conductivity (~0.031 W·m −1 ·K −1 ). This work provides a scalable route to bio-based 3D-printed porous materials with programmable porosity and multifunctional performance.

研究领域: 材料科学 · 增材制造 · 高分子科学 · 热工工程 · 可持续材料
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Acta Biomaterialia · 2025 · IF 9.6

A Kneading-Responsive Hyaluronic Acid-based Hydrogel for On-Demand Local Anesthesia in Osteoarthritis

Wenjin Dai,Mengjun Zeng,Lu Zhang,Guangwei Shi,Hong Wang,Chengyi Xu,Riguang Zhao,Cong Zhang,Jiu Wang,Liqun Jiang

An intelligent hydrogel system that can rapidly release local anesthetics in response to simple mechanical kneading offers a patient-friendly solution for managing osteoarthritis (OA) pain during acute flare-ups. Conventional stimuli-responsive hydrogels often require specialized devices (e.g., near-infrared emitters and ultrasound generators), limiting their accessibility in real-world settings. A kneading-responsive hydrogel composed of oxidized hyaluronic acid (OHA) and carboxymethyl chitosan, incorporating pressure-sensitive multivesicular liposomes (pMVLs) loaded with phosphoric acid and benzocaine covalently linked to OHA, was developed in this study. Mechanical kneading (0.25 ±0.03 kg/cm²) ruptured the pMVLs, releasing acid to lower the gel pH from 7.4 to 6.7, thereby cleaving Schiff base bonds and accelerating benzocaine release by 2.26-fold in vitro . In OA-rat models, periarticular injection of the hydrogel significantly increased pain thresholds, and kneading raised benzocaine accumulation in the synovial fluid by 3.88-fold, improving locomotor activity and joint function. The release was gated by a predefined pressure threshold : the hydrogel remained quiescent under physiological interstitial pressures but was activated by conscious kneading (0.25 ± 0.03 kg/cm²), allowing for patient-controlled, on-demand analgesia. This kneading-responsive hydrogel enables self-controlled, on-demand analgesia without the need for specialized equipment, providing a convenient strategy for precision pain management in OA. Statement of Significance Many pain-relief options rely on clinic devices or fixed depots that patients cannot control. We report an equipment-free, kneading-responsive hyaluronic-acid hydrogel that converts gentle finger pressure (0.25 kg·cm⁻², measured) into on-demand local anesthesia for osteoarthritis flares. The reservoir combines a pH-sensitive OHA/CMS network with pressure-sensitive multivesicular liposomes that release phosphoric acid, transiently lowering the pH to cleave imine (Schiff-base) bonds and accelerate benzocaine release. In OA rats, a single kneading produced ∼48 h of drug elevation, while the depot persisted for up to 14 days; once-daily kneading maintained effective analgesia for up to 6 days, improving pain, mobility, and cartilage preservation. Benchmarking versus NIR/ultrasound highlights the trade-off between remote triggering and simple, patient-directed use. This self-managed platform enables localized, repeat-dosing pain control.

研究领域: 生物医学工程 · 药物递送 · 疼痛管理 · 生物材料 · 骨关节炎治疗
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY · 2025 · IF 2.4

Efficient activation of peroxymonosulfate by MoSe2-based bimetallic composite selenides for the degradation of levofloxacin

Taiping Xie,Shengli Xie,Yuxuan He,Kailin Xu,Jin Qian

BACKGROUND Antibiotic pollution in aquatic environments poses significant threats to human health and ecosystems by promoting the spread of antibiotic resistance. RESULTS This study investigates the use of MoSe 2 -based bimetallic composite selenides (MoSe 2 /CoSe 2 and MoSe 2 /MnSe) to activate peroxymonosulfate (PMS) for the oxidation of levofloxacin (LEF), a model fluoroquinolone antibiotic. The composites were synthesized via a solvothermal method and characterized using SEM, TEM, XRD, and XPS, confirming the formation of heterojunction interfaces and the presence of active metal sites. Catalytic performance tests demonstrated that MoSe 2 /CoSe 2 and MoSe 2 /MnSe significantly enhanced LEF degradation, achieving removal efficiencies of 92.98% and 89.4%, respectively, compared to 49.07% with MoSe 2 alone. Optimization of reaction parameters revealed that PMS dosage, catalyst dosage, and pH critically influence degradation efficiency. Reusability tests confirmed the catalysts' stability over multiple cycles with minimal loss in activity. Electron paramagnetic resonance (EPR) and radical quenching experiments identified sulfate radicals (SO 4 •- ) as the primary active species driving LEF degradation. CONCLUSION This work provides a robust theoretical foundation for the application of SR-AOPs in wastewater treatment, highlighting the potential of MoSe 2 -based composites in mitigating antibiotic contamination. © 2025 Society of Chemical Industry (SCI).

研究领域: 环境科学 · 材料化学 · 水处理 · 催化
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Advanced Science · 2025 · IF 14.1

A Tangentially Sensitive Tactile Sensor Reveals the Stick-Slip Mechanism and Enhances Robotic Tactile Sensing

Jinghui Wang,Xiaoyu Liu,Yujiao Du,Yepu Chen,Jieyi Guo,Linyuan Fan,Min Tang,Xiaofeng Qiao,Yuanjie Zhu,Zhiyang Zhang,Chaojie Dong,Lizhen Wang,Yubo Fan

The mechanism of human tactile perception offers inspiration for developing a high-performance artificial sensory system. Pacinian corpuscles (PCs) allowing high-frequency tangential sensitivity that endows humans with the ability to perceive multidimensional tactile stimuli. However, replicating similar high-frequency and tangential perception as that of PCs in artificial systems remains a significant challenge. Here, an artificial PC (APC) from ultralight aerogel with a multilayer-stacked and anisotropic structure analogous to that of PC via a multi-directional freeze-drying method is reported. The APC sensor with radial-axial anisotropy exhibits tangential sensitivity (1022 kPa −1 ), detects multidimensional tactile stimuli, and identifies stick-slip states with high precision. By mimicking PC clusters, the APC sensor system achieves spatiotemporal sensing capabilities for discriminating frictional patterns (static, sliding, or rolling) and tracking slip. A robot equipped with the APC sensory system possesses enhanced tactile perception for diverse tactile events in active (100% accuracy) and passive (98.18% accuracy) interaction with humans. It is found that high-frequency components are crucial for stick-slip detection, providing insights into the underlying tangential tactile sensing mechanisms of PCs. The work exemplifies a bidirectional enhancement of understanding between technological innovation and biological mechanisms.

研究领域: 机器人学 · 感知系统 · 仿生学 · 触觉传感 · 材料科学
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