JOURNAL OF CONTROLLED RELEASE
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2025
·
IF 11.5
Jiadong Pang,Xiaoyu Chen,Zhijun Lin,Shuo Yao,Wanyan Wang,Hong Wu,Wei Xing,Jiang Yang
Anaplastic lymphoma kinase (ALK) oncogenic fusions are an infamously evolving target in ALK fusion-positive (ALK + ) non-small cell lung cancer (NSCLC). RNA interference (RNAi) is a potential alternative to small-molecule ALK inhibitors but suffers from poor cellular delivery and low stability, restricting sustained on-target therapeutic efficacy. To attain non-invasive direct RNAi at target sites in the lungs, inhalable vehicles are demanded to shield unstable siRNA from degradation in alkaline pleural fluid and to shuttle siRNA in the acidic tumor microenvironment. Here, we chemically synthesize a universal polyethylene glycol-poly(β-amino esters)-histidine(PEG-PBAE-His, PPH) system that enables siRNA-directed ALK gene silencing in ALK + NSCLC with controlled release. The rational design of PEGylated polycationic PPH integrates the non-ionic nature, inertness, stealth effect, and low immunogenicity of PEG coronae with dual positively-charged PBAE and His to encapsulate siRNA payloads through enhanced electrostatic complexations. The assembled polyplexes with low polydispersity are overall anionic in alkaline pleural fluid and reversed into cationic charges at acidic pH, facilitating cellular uptake and lysosomal pH-governed release. The PPH-directed delivery significantly improves siRNA stability and ALK sequence-specific knockdown in H3122 cells, with a transfection efficiency comparable to commercial polyethylenimine but with lower cytotoxicity. The ALK-centric RNAi therapy prohibits cancer clonogenicity, migration, and invasion and induces potent growth inhibition in ALK + NSCLC xenografts through inhalation. The inhalable polyplexes represent a transformative delivery platform that combines pH-responsive targeting, enhanced stability, and low toxicity, addressing critical limitations of existing siRNA delivery systems.
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高影响因子
LANGMUIR
·
2024
·
IF 3.7
Yirong Fan,Hui Sun
The morphological control and transformation of soft nanomaterials are critical for their physical and chemical properties, which can be achieved by dynamically regulating the hydrophilicity of amphiphilic polymers during self-assembly. Herein, an amphiphilic homopolymer poly(N-(2,2′-bipyridine)-4-acrylamide) (PBPyAA) with bipyridine pendants is synthesized, and the effect of various parameters including initial concentration, temperature, pH, and metal ion coordination on the self-assembly behavior and morphology of the assemblies is investigated. Upon changing the initial concentration of PBPyAA, bowl-shaped nanoparticles (BNPs) with precisely controlled diameter, opening size, and thickness are obtained. With the decrease of pH of the solution, the negatively charged surface of BNPs transforms to a positively charged state. Furthermore, the addition of divalent metal ions (Co2+, Mn2+, and Zn2+) induces the transformation of BNPs to vesicles and giant vesicles. The effect of the above factors on the morphology of the assemblies is essential to change the hydrophilicity of PBPyAA dynamically, leading to variation of the local viscosity during self-assembly. Overall, manipulation of the structural parameters of BNPs and transformation of BNPs to vesicles are achieved, providing fresh insights for the precise control of the morphologies of soft nanomaterials.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Xiong Jinqi,Mao Shanjun,Luo Qian,Ning Honghui,Lu Bing,Liu Yanling,Wang Yong
As a crucial industrial process for the production of bulk and fine chemicals, semi-hydrogenation of alkynes faces the trade-off between activity and selectivity due to undesirable over-hydrogenation. By breaking the energy linear scaling relationships, we report an efficient additive-free WO 3 -based single-atom Pd catalytic system with a vertical size effect of hydrogen spillover. Hydrogen spillover induced hydrophilic polar layer (HPL) with limited thickness on WO 3 -based support exhibits unconventional size effect to Pd site, in which over-hydrogenation is greatly suppressed on Pd 1 site due to the polar repulsive interaction between HPL and nonpolar C=C bonds, whereas this is invalid for Pd nanoparticles with higher altitudes. By further enhancing the HPL through Mo doping, activated Pd 1 /MoWO 3 achieves recorded performance of 98.4% selectivity and 10200 h −1 activity for semi-hydrogenation of 2-methyl-3-butyn-2-ol, 26-fold increase in activity of Lindlar catalyst. This observed vertical size effect of hydrogen spillover offers broad potential in catalytic performance regulation.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
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IF 5.8
Haili Zhao,Qi Wang,Hang Li,Han Li,Tianhang Han,Aozhou Wang,Kaisheng Yao
Developing a simple and mild one-step method for the preparation of bimetallic nanomaterials with both free-standing features and excellent catalytic performance is highly desirable but remains technically difficult. Herein, a facile liquid-liquid interface route is exploited to grow the wheat-like PdAg nanostructures at the interface of chloroform and water under mild conditions without the use of any surfactants and supports. To implement this scheme, Na 2 PdCl 4 and AgNO 3 as precursors are dissolved in aqueous phase and α-naphthol as reducing agent in chloroform phase to build up the interfacial reaction system. At 40°C, the PdAg nanowheats are orderly grown, fused and assembled by many newly generated nanoparticles at the interface region, which have uniform shapes with the length of about 340 nm and the diameter of about 45 nm, abundant defects and strong electronic interaction between Au and Pd, as well as free-standing features. In the hydrogenation reaction of 4-nitrobenzaldehyde, PdAg-1 nanowheats exhibit excellent catalytic activity, selectivity and durability. Within 60.0 min of reaction at 35°C under atmospheric pressure, 99.8 % conversion of 4-nitrobenzaldehyde and 99.5 % selectivity toward 4-aminobenzaldehyde can be realized. After 5 cycles, 99.4 % conversion of 4-nitrobenzaldehyde and 98.0 % selectivity toward 4-aminobenzaldehyde can be maintained.
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ACS Applied Energy Materials
·
2024
·
IF 5.4
Tao Chen,Manli Wang,Donghang Hu,Qianlin Ju,Kaige Zhao,Liang Fu,Zelin Chen,Xiaolong Yu,Changjiu Li
The mainstream electrocatalysts for direct ethanol fuel cells (DEFCs) are Pt- or Pd-based nanomaterials, which are severely hampered by CO intermediate poisoning and the relatively low selectivity of the C1 pathway in anodic ethanol oxidation reaction (EOR), thereby impeding the efficiency enhancement and practical application of DEFCs. Herein, we report a Pt-decorated amorphous PdS nanowire [denoted as a-Pd(S)NWs/Pt] catalyst with abundant crystalline/amorphous heterogeneous interfacial active sites for alkaline EOR. The a-Pd(S)NWs/Pt was demonstrated a superior EOR mass activity of 6.16 A·mgPd+Pt–1, which is 22.81 times over that of commercial Pt/C (0.27 A·mgPt–1) and 34.22 times over that of commercial Pd/C (0.18 A·mgPd–1). Additionally, the a-Pd(S)NWs/Pt exhibited considerable stability, significantly enhanced resistance to CO poisoning and enhanced selectivity for the EOR C1 pathway. Density functional theory calculations and experimental results further revealed that the optimized COads and OHads binding energies due to the decoration of Pt nanoclusters can be responsible for the enhanced CO resistance and C1 selectivity of a-Pd(S)NWs/Pt. Furthermore, benefiting from its optimized electronic configuration at the interfacial active sites and the appropriate intermediate adsorption capacity, the a-Pd(S)NWs/Pt electrocatalyst was successfully extended to the electrocatalytic methanol and ethylene glycol oxidation reaction systems.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Haiyang Xie,Dan Tang,Yanjuan Zhang,Zuqiang Huang,Huayu Hu,Qian He,Hongbing Ji,Tao Gan
The design of non-noble metal single-atom catalysts (SACs) with superior performance for semi-hydrogenation of alkynol to alkenol is remarkable but challenging. Herein, fluorine-tuned Fe SACs supported on N, F-codoped carbon (Fe 1 -NFC) with a Fe-N 4 F 1 structure is successfully prepared via a complexation method. The axial F-doping can modulate the electronic structure of the metalloporphyrin-like active sites (Fe-N 4 ), promoting the transfer of electrons from Fe atoms to F atoms to form electron-deficient Fe δ+ species. As a result, the Fe 1 -NFC catalyst shows a remarkable activity for the semi-hydrogenation of 2-methyl-3-butyn-2-ol to 2-methyl-3-buten-2-ol under mild conditions, with a TOF of 9163 h −1 and a selectivity of 96 % at 97 % conversion, both much higher than that of the Fe SACs supported on N-doped carbon (Fe 1 -NC). Density functional theory (DFT) calculations reveal that the excellent catalytic activity is attributed to the interfacial electronic effect of Fe species induced by axial F-doping, thereby enhancing the exothermic adsorption of alkynol on the Fe-N 4 F 1 structures and accelerating the desorption of alkenol to against the overhydrogenation.
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CATALYSIS TODAY
·
2024
·
IF 5.2
Min Qiao,Jiansu Ran,Tianyi Yang,Zhaohui Liu,Kexin Yao
Resorcinol 1,4-phthalaldehyde resin (RPR) was successfully synthesized using a solvent-free self-assembly method employing a template (F127) and a mixture of resorcinol and 14-phthalaldehyde. After the removal of the template (F127) by heating, the PRR exhibited an ordered mesoporous structure with a size of approximately 5.8 nm. After impregnating with Pd species, a RPR supported Pd catalyst (Pd/RPR) was finally obtained, which demonstrated outstanding catalytic performance and good stability in the hydrodeoxygenation of vanillin . With an optimal catalyst, 100% conversion of vanillin and 96.7% selectivity for 2-methoxy-4-methylphenol were achieved under the reaction conditions of 2 MPa H 2 in ethanol at 90 ℃ over 4 hours. The superior catalytic properties of Pd/RPR with high activity and stability are anticipated to be significant for future biofuel upgrades.
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Small
·
2024
·Vol. 20
·期 52
·2408373
·
IF 13
Xiaotong Zhou,Songliang Liu,Huaifang Teng,Kun Ma,Weixin Miao,Xuejing Cui,Xin Zhou,Luhua Jiang
Reasonable construction of high activity and selectivity electrocatalysts is crucial to achieve efficient ethanol oxidation reaction (EOR). However, the oxidation of ethanol tends to produce CO species that poison the active centers of the EOR electrocatalysts. Herein, a unique amorphous CrO x -protected defect-rich ultrafine Pd nanowires (CrO x -Pd NWs) is developed. On the one hand, the CrO x layer can act as a protective layer to maintain the structure of the nanowire. On the other hand, it can play the role of OH regulator to optimize the adsorption energy barrier of intermediate species in Pd nanowire, thereby enhancing the ability of the catalyst to resist CO poisoning. The CrO x -Pd NWs exhibit excellent EOR performance with 3.64 times higher mass activity and 50 mV lower CO electro-oxidation potential than commercial Pd black. The results show that the CrO x layer promotes the dissociation of H 2 O into OH ads , while the CrO x transfers electrons to neighboring Pd atoms optimizing the electronic configuration of Pd, thus selectively oxidizing ethanol to acetate and preventing the formation of toxic * CO. This work provides an effective strategy for the synthesis of nanowire materials with oxide/metal interfaces and offers new ideas for the design of catalysts that can efficiently drive EOR.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2025
·
IF 2.8
Yun Hong,Chunjie Li,Feng Zhang,Xiaoye Ma,Dingxiao Jiang,Rizhe Jin,Chuanqing Kang
The incorporation of fillers into waterborne polyurethane (WPU) can endow the composites with improved physicochemical and physiological properties for biomedical applications. Silk fibroin possesses excellent mechanical properties and biocompatibility owing to its unique hierarchical structure comprising β-sheet crystallites and amorphous matrix. To mimic its structure, a crystalline tetrapeptide Gly-Ala-Gly-Ala (GAGA) derived from the repetitive segments of the primary sequence of fibroins was grafted onto the WPU backbone. The tetrapeptides aggregated via additional hydrogen bonds to form crystalline domains, which served as physical crosslinking points to significantly improve the mechanical properties of WPU. Compared with the pristine WPU, the modification enhanced the maximum tensile strength (from 13.1 to 25.4 MPa) and hydrophilicity (the water contact angle from 80.6° to 38.8°). In addition, the modified WPU with the optimal proportion of the tetrapeptide remained structurally stable under physiological environments and showed improved biocompatibility including good cell and protein adhesion, noncytotoxicity, and nonhemolysis. The excellent performance confirms the effectiveness of peptides in WPU modification and sheds light on the potential of modified WPU in biomedical applications.
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Surfaces and Interfaces
·
2025
·
IF 6.3
Junjing Li,Xu Liu,Zilin Tan,Liang Wang
In order to enhance the catalytic activity of Pd nanoparticles and reduce the amount of Pd, the present study was carried out to construct nanowire structures by surfactant-directed hydration method to further increase the active sites on the surface of Pd and improve the yield of atomic hydrogen (H ⁎ ). The introduction of cheap metal Ni effectively reduced the Pd dosage and increased the utilization of Pd. Nitrogen-doped ordered mesoporous carbon (NOMC) was incorporated to facilitate the dispersion of Pd particles and improve the stability of the catalyst while ensuring the catalytic activity. The prepared palladium-nickel nanowires/nitrogen-doped ordered mesoporous carbon/carbon (Pd-Ni NWs/NOMC/C) electrodes showed excellent efficiency for the removal of halogenated pharmaceuticals and personal care products (PPCPs). The combination of palladium-nickel nanowires (Pd-Ni NWs) with NOMC enhanced the electron transfer capability at the electrode surface and improved the H ⁎ yield. The results showed that the removal efficiency of this electrode for lornoxicam reached 97.2 % at 270 min. The electrode reduced the amount of Pd while stabilizing the electrocatalytic effect. The dechlorination mechanism of Pd-Ni NWs/NOMC/C electrode for lornoxicam was also proposed, and the reaction products and their toxicity were analyzed. This study provided a new idea for designing and synthesizing metal composite catalysts, reduced the cost of catalyst preparation, and had a good application prospect in the treatment of wastewater containing halogenated organic compounds.
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GREEN CHEMISTRY
·
2024
·
IF 9.3
Shumin Huang,Xiaolin Luo,Ji Li,Sibao Liu,Li Shuai
High-density fuel additives are important for heavy transportation. Production of high-density fuel additives from renewable resources has been receiving increasing attention in recent years. Despite the progress in the depolymerization of lignin, cellulose, and hemicelluloses, there are limited studies on integrating lignin and carbohydrates to make value-added products. Here we design a route to synthesize high-density fuel additives with lignin-derived monophenolics and carbohydrate-derived furanics. We performed Brønsted base-catalyzed C–C coupling of phenolics and furanics followed by hydrodeoxygenation catalyzed by a synthesized Ir–ReOx/SiO2 catalyst. Under optimized reaction conditions, the coupling product of phenolics and furanics, bicyclic furyl phenyl precursors, reached a yield of over 90%, and was further hydrodeoxygenated to bicyclohexyl alkanes with a yield of over 98%. The current two-step strategy demonstrates high-selectivity of preparing high-density hydrocarbon fuels from lignocelluloses and provides a possible way to utilize all components of lignocellulosic biomass in an integrated upgrading pathway.
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Materials Today Chemistry
·
2024
·
IF 6.7
Xiangfeng Sun,Xuan Song,Dongxia Li,Yuxin Xue,Yulin Fu,Yuanhao Shi,Zhiqi Li,Chongxian Luo,Qiong Lin,Xuefeng Gui,Jiwen Hu,Kai Xu
Lithium-sulfur batteries (LSBs) have been considered as ideal candidates for next-generation energy storage equipment. However, its development has been hindered by the shuttle effect exhibited by the intermediate lithium polysulfides (LiPSs). To address this problem, covalent organic frameworks (COFs) show great promises as sulfur hosts for LSBs. We devised and synthesized a covalent organic framework (TPAS–TPB–COF) that is rich in redox sites by solution polymerization. The reactive groups in the covalent organic framework nano–channels not only inhibit the shuttling of polysulfides, but also promote the migration of Li ions. Meanwhile, the abundant cavities as well as redox sites in the COF nano–channels achieve a high sulfur loading capacity (∼71 wt%), a strong LiPS adsorption capacity, and facilitate ion diffusion. Based on these advantages, when it is used as a sulfur host for LSBs, our COF system provides a high capacity of 1134 mAh g −1 at 0.2 C (1 C = 1675 mA g −1 ), an outstanding rate capability (560 mAh g −1 at 4 C), and excellent stability.
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