CHINESE JOURNAL OF CATALYSIS
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2025
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IF 17.7
Zhenghao Mao,Wenjing Xu,Na Han,Yanguang Li
Aldehydes are valuable intermediates with widespread industrial applications, and their traditional synthesis relies on chemical oxidation that is often hazardous and environmentally unfriendly. Electrochemical oxidation offers a more sustainable and milder alternative; however, it faces challenges such as aldehyde overoxidation and susceptibility to base-catalyzed Cannizzaro disproportionation. Electrochemical glycerol oxidation to glyceraldehyde is a representative example, which typically requires precious metal-based electrocatalysts but still suffers from low selectivity and activity. Here, we report a metal-free oxidation strategy mediated by 2,2,6,6-tetramethylpiperidine-1-oxyl. By systematically investigating the redox thermodynamics and kinetics of TEMPO across a broad pH range, we construct a Pourbaix diagram and elucidate the relative kinetics of each reaction step. These insights allow us to explain the anomalously high apparent Faradaic efficiency (~200%) observed under acidic conditions, and identify neutral media as the optimal environment for selective glyceraldehyde production. Under optimized conditions, our system achieves a glyceraldehyde Faradaic efficiency exceeding 93% and a partial current density of 23.3 mA cm –2 at 0.57 V — more than doubling the performance of the best reported precious metal-based systems. Furthermore, the versatility of this strategy extends to the selective oxidation of other primary alcohols to their corresponding aldehydes with near-unity selectivity.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2025
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IF 7.8
Tianjian Dang,Guanghua Lu,Min Wang,Yuhao Ji,Yufang Chen,Runren Jiang
The lifetime of free radicals limits the effectiveness of catalytic degradation reactions and the efficient utilization of transient free radicals remains a significant challenge in current research. In this paper, we have developed MIL-125 MOF derivatives, which can influence the morphology and structure of the materials by controlling the calcination time. The CT3 system significantly enhanced the activation performance of persulfate (PDS) and enabled the complete degradation of acetaminophen (ACT) within 20 min. The electron acceptor effect of the C C double bond accelerates the generation of singlet oxygen in the CT3 system, and rapidly acts on ACT, thereby improving the degradation performance of the CT3 system. Product analysis and soybean seed germination experiments confirmed that the toxicity of the degradation products was significantly reduced, and the degraded solution did not affect soybean growth. This study offers novel approaches and insights for utilizing MOF derivatives to activate PDS for the degradation of organic contaminants.
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CELLULOSE
·
2025
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IF 4.8
Zhang Qian,Hao Sufen,Zhang Wenrui,Ding Zitian,Wang Xin,Huang Jintian
This paper presents a novel inside-out, layer-by-layer assembly process that combines the sol–gel transphase with pH inversion to prepare cellulose-reinforced sodium alginate (SA) gel microspheres (Q-ACCs). The use of oxidized cellulose (TOCN) in the inner layer resulted in a petal-like morphology and increased the specific surface area of the microspheres. The outermost layer of regenerated cellulose (RC) improved the mechanical properties and water absorption capacity of the hydrogel microspheres. Notably, the microspheres exhibited good encapsulation properties. Remarkable results were achieved when encapsulating fertilizer and Fe 3 O 4 . This study offers promising prospects for the preparation of gel microspheres and the development of functional synergies for producing multifunctional encapsulated materials in various fields. Graphical abstract
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Small
·
2025
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IF 12.1
Juan Hu,Yahui Zhang,Yingqi He,Zhitao Su,Wanli Lao,Shaodi Zhang,Yanglun Yu,Wenji Yu,Yuxiang Huang
Bamboo is an ideal candidate to replace traditional plastics, reduce environmental pollution, and promote harmony between nature and humanity owing to its rapid growth and renewability. However, achieving arbitrary shape-shifting of bamboo while retaining its high strength and degradability remains challenging. This study uses multiscale interface engineering to transform bamboo into a robust, biodegradable, and moldable bamboo cellulose-based material. First, natural bamboo is deconstructed into cellulose fibers, including macro- and nanofibers. Subsequently, the fibers are constructed into high-performance materials using physical and chemical methods, such as surface charge treatment, ion cross-linking, and dense hydrogen bonding networks. The prepared multiscale bamboo cellulose-based materials exhibit excellent properties, with a high specific strength (≈271.8 kN m kg −1 ), high impact toughness (≈58 kJ m −2 ), low thermal expansion coefficient (1.19 × 10 −6 K −1 ), excellent formability and biodegradability, and minimal environmental impacts. These properties are superior to those of current commercial plastics and other biomass-derived structural materials. Furthermore, the mechanical properties of the materials can be customized by adjusting the layup configuration, enabling a transition from anisotropic to isotropic characteristics. This transformation demonstrates the significant potential of bamboo for plastic substitution and advances the development of environmentally friendly materials.
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ACS Sustainable Chemistry & Engineering
·
2025
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IF 7.3
Xu Chen,Wenjun Zhang,Yanmei Zheng,Lin Dong,Zupeng Chen
The photocatalytic oxidation of 5-hydroxymethylfurfural (5-HMF) to 2,5-furandicarboxylic acid (FDCA) represents a sustainable strategy for the conversion of biomass-based platform compounds into high-value chemicals. In this work, a supramolecular self-assembly strategy is employed to synthesize tubular carbon nitride (T-MCN), and sodium ion-doped carbon nitride (Na-T-MCN) is obtained via sodium chloride-assisted thermal polymerization. The optimized catalyst demonstrates superior activity in the oxidation of 5-HMF, achieving a high yield of FDCA (90%) within 8 h. The exceptional photocatalytic performance of Na-T-MCN is attributed to the incorporation of Na+ ions and cyanamide groups, which facilitate the separation of photogenerated charges and holes. To elucidate the underlying mechanism, intermediate trapping experiments and electron paramagnetic resonance (EPR) spectroscopy are employed to investigate the dynamics of photoinduced charge separation, electron transfer, and the reaction pathway of photocatalytic oxidation of 5-HMF. The findings reveal that the key active species in the oxidation reaction are the •O2– and h+ species. This study provides a viable and efficient strategy for converting biomass platform compounds into high-value-added products.
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SENSORS AND ACTUATORS B-CHEMICAL
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2025
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IF 7.7
Jianhong Liu,Xinyue Zhao,Li Zhang,Haowen Zhou,Xudong Li,Guorui Zheng,Xibin Zhou,Yongjin Peng,Jie Zhang
Rheumatoid arthritis (RA) is a chronic autoimmune disorder characterized by progressive joint destruction, where early diagnosis is crucial for impeding disease progression. Peroxynitrite (ONOO⁻), a key reactive nitrogen species, is critically involved in the pathogenesis of RA and represents a promising diagnostic target for early detection. Herein, we developed MRN, a mitochondria-targeting ratiometric fluorescent probe based on a Förster resonance energy transfer (FRET) mechanism for the dynamic monitoring of ONOO⁻ in RA inflammatory models. The probe integrates a rhodamine-naphthalimide FRET pair and a hydrazide group as the specific recognition unit, which facilitates a rapid, ONOO⁻-triggered ratiometric response within 30 seconds and achieves a detection limit of 7.5 nM. Furthermore, the conjugation of a triphenylphosphonium group ensures precise mitochondrial localization. Cellular assays demonstrated excellent biocompatibility and specific mitochondrial targeting. We successfully applied MRN for real-time ratiometric imaging of both endogenous and exogenous ONOO⁻ fluctuations in live BV-2 cells. Importantly, in a Complete Freund's Adjuvant (CFA)-induced rheumatoid arthritis mouse model, MRN enabled in situ ratiometric fluorescence imaging of ONOO⁻ at articular sites, revealing a strong positive correlation between the fluorescence signal intensity and the degree of inflammatory severity. This work establishes MRN as a novel and robust molecular tool for the early diagnosis of RA.
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Acta Biomaterialia
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2025
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IF 9.6
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.
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Journal of Environmental Chemical Engineering
·
2025
·Vol. 14
·期 1
·120662
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IF 7.2
Bin Ou,Hongwei Rong,Baihui Cui,Jie Zhang,Fang Zhang,Dabin Guo
The coordination calcination method is used to form a coordination complex between Co 2 + and thiophene, which is adsorbed on carbon black (CB) and then calcined to prepare Co-S-C/CB single atom catalyst. Co-S-C/CB could efficiently activate peroxymonosulfate (PMS) by forming Co-S 3 coordination structure and Co-S 3 is the active site for activating PMS. Electron rich region was formed on the Co atom and the Co atom could keep in a low valence state during the catalytic process and donate electrons to PMS to produce radicals (•OH and SO 4 •- ) through a single-electron-reduction. Co-S-C/CB could not only promote PMS to generate •OH and SO 4 •- , but also inhibit the generation of 1 O 2 and O 2 •- . The radical pathway has the lowest Gibbs free energy (ΔG) compared to the 1 O 2 pathway and the Co(IV)=O pathway. Therefore, Co-S-C/CB could regulate the radical pathway of PMS. •OH and SO 4 •- are mainly responsible for the removal of Rhodamine B (RhB). Co-S-C/CB could be applied to efficiently degrade various organic pollutants and has good stability. Macro preparation of Co-S-C/CB could be achieved from both the preparation process and raw material aspects.
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ACS Applied Polymer Materials
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2025
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IF 4.7
Qi Xu,Yuwen Gai,Shuang Wang,Xinmeng Li,Weixiao Ding,Jian Cui,Peng Zhou,Luyu Yang,Lei Zhang,Dongping Sun
In recent years, the development of flexible wearable materials and electromagnetic shielding materials has progressed rapidly. The demand for monitoring movement data and providing protection against electromagnetic waves has also increased significantly. However, there is currently a lack of materials suitable for applications in high-humidity and underwater environments, which limits their ability to meet the needs of users in special conditions. In this study, we designed an aerogel sensor based on MXene and bacterial cellulose (BC) capable of monitoring movement in both dry and wet states while also exhibiting good electromagnetic wave absorption properties.The sensor showed a sensitivity of −6.43 with excellent linearity (99.8%) and stability. The sensor exhibits a high compressive strength of up to 15 kPa in the dry state, with a resistance change rate reaching 50% under 8% strain, and can undergo 710 cycles, demonstrating high sensitivity and stability. Under water-induced conditions, the sensor demonstrates high flexibility, shape-memory performance, and a wide strain range (0–80%) as a wet-state sensor, maintaining good structural stability and sensing performance throughout the dry–wet transition process. The BCNF/MXene sensor also demonstrates good resistance to electromagnetic interference. The RLmin of the BCNF/MXene-30% sensor reaches −45.60 dB, with an electromagnetic wave absorption rate of 99.99% and a relatively broad effective absorption bandwidth (4 GHz). This resistive sensor can be applied in electronic skins, human–machine interactions, smart wearable devices, and personalized health monitoring. Our work successfully demonstrated the application of water-sensitive shape-memory materials in electronic skins, health monitoring components, and electromagnetic wave protection.
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CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
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2025
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IF 10.3
Weixia Wang,Yongji Zhang,Fei Zhao,Libo Wang,Fanpeng Meng,Shuchao Qin,Jinsheng Zhao
Carrier recombination in polymer photocatalysts involves both undissociated exciton decay and charge recombination, which are the main obstacles limiting their photocatalytic activity. Achieving efficient charge generation and separation in a polymer system is a fundamental strategy for the potential success of solar energy conversion to hydrogen, but it remains a huge challenge. In this study, we propose an innovative intermolecular π–π stacking strategy to construct a π-delocalized all-polymer S-scheme heterojunction for photocatalytic hydrogen evolution. Two conjugated porous polymers (CPPs)—PyB, composed of benzo[1,2-b:4,5-b′]dithiophene (BDT) and pyrene units, and PhB, composed of BDT and benzene—were synthesized and integrated with CN nanosheets. The highly planar and π-extended structure of PyB facilitated strong interfacial π–π stacking with CN, forming an extended π-delocalized network that enhanced the internal electric field (IEF), improved charge separation, and boosted visible-light absorption. As a result, the optimized PyB/CN-20 composite achieved a remarkable hydrogen evolution rate (HER) of 23.84 mmol⋅h −1 ⋅g −1 under visible light, approximately 287 times higher than that of pristine CN. This work underscores the critical role of polymer planarity and π-conjugation in heterojunction efficiency, and provides new insights into the rational design of π-delocalized S-scheme systems and establishes a general strategy for developing highly efficient, metal-free photocatalysts by leveraging molecular-level structural control.
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MACROMOLECULES
·
2025
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IF 5.2
Shengli Chen,Xuelei Dong,Yuhong Cui,Mingxue Xing,Min Wang,Xiongwei Qu,Fenfen Wang
Stimuli-responsive nanoparticles capable of reversible morphological transformations is a challenge in the field of intelligent polymers. This work presents a novel strategy termed “thermo-driven dynamic reversible self-assembly”, which enables efficient and reversible interconversion between polymersomes and worms, with over 95.0% structural retention after three cycles. This was achieved by grafting crystalline polycaprolactone (PCL) side chains onto the backbone of poly(4-vinylpyridine)-b-polystyrene via polymerization-induced self-assembly. Multiscale mechanistic analysis reveals that the crystallization and melting behavior of brush PCL side chains dynamically modulates the hydrophilic–hydrophobic balance. At low temperatures, the crystalline domains function as physical cross-linking points that stabilize the vesicles. Upon heating, the melting of these domains enhances chain segment mobility, thereby promoting a transition to low-curvature worms. Leveraging this temperature responsiveness, a radical inhibitor was encapsulated within the vesicle cavity, achieving a loading capacity of 13.4%, and constructed an active safety protection system. When applied to an acrylic acid polymerization system, the abrupt temperature increase caused by a runaway reaction triggered the vesicle-to-worm transition, resulting in the rapid release of 98.0% of the inhibitor and effectively preventing gelation. This work demonstrates thermo-driven reversible self-assembly of micelles, and integrates this capability with chemical safety protocols, offering a self-triggered, energy-free protective mechanism.
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SENSORS AND ACTUATORS A-PHYSICAL
·
2025
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IF 4.9
Wei Chen,Xiuchuan Jing,Zhuang Li,Yongxi Ma,Hongda Gu,Haiqing Miao,Zhong Wang,Guohe Wang
Attaching flexible resistive strain sensors to human skin enables response detection of behaviours towards real-time physiological monitoring. However, current flexible resistive strain sensors hinder themselves from practical applications due to their low sensitivity, small linear working range, and poor wearing comfort. In this research, a conductive thermoplastic polyurethane (TPU) membrane is fabricated using TEMPO modified nanocellulose (TNC) decorated with carbon quantum dots (CQDs) to prepare flexible highly sensitive, and breathable strain sensors. Results show that the mechanical property and strain response range of the TPU membrane is significantly enhanced by CQDs-TNC. The TPU membrane also exhibits the highest sensitivity (GF= 49.4 in the 30∼80 % strain range) and a wide response range (0–80 %). At 5 %wt of CQDs-TNC, the membrane displays the highest elongation at break (389.8 %) with maximum breaking stress approaching 9.7 MPa. The CQDs-TNC/TPU membrane exhibits fast response and recovery times (85 ms and 93 ms), low hysteresis (8.9 %), and excellent dynamic cyclic strain performance (1000 stretch/release cycles). The CQDs/TMC/TPU-resistive strain sensor (CTT-RSS) sensor well conforms to human joints, and accurately produces real-time regular resistance strain responses based on human movements. In all, this study contributes a novel research design for fabricating flexible and sensitive sensor to the development of smart textiles.
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危险品化学品经营许可证（带存储）