Polymer Chemistry
·
2015
·Vol. 6
·期 35
·6351-6357
·
IF 5.52
Xiaoyu Jiang,Wuxue Zhao,Wei Wang,Fan Zhang,Xiaodong Zhuang,Sheng Han,Xinliang Feng
Two novel Pd-loaded heteroatom-linked microporous polymers Pd@NP and Pd@NPO were effectively synthesized by one-pot Pd-catalyzed Heck coupling reactions of tris(4-vinylphenyl)amine with tris(4-bromophenyl)phosphine and tris(4-bromophenyl)phosphine oxide, respectively. The Pd atoms loaded into the networks of the resulting porous polymers originated from the Pd-catalyst used in the polymerization, which was achieved under moderate reaction conditions. Besides the nitrogen atoms, the trivalent phosphorus atoms bearing one lone pair of electrons and the pentavalent phosphorus atoms of the phosphoryl groups were used as the linkers for the formation of the frameworks of the porous polymers Pd@NP and Pd@NPO, respectively. The phosphorus atoms with different oxidation states in the networks caused a dramatic variation in the physical and catalytic properties of the as-prepared porous polymers. Pd@NP and Pd@NPO exhibit surface areas of 381 m2 g−1 and 684 m2 g−1, respectively. Both Pd-loaded porous polymers enable efficient Suzuki–Miyaura coupling reactions featuring short reaction times and good yields, with the catalysts being highly stable and easy to recycle. The catalytic activity of Pd@NPO is higher than that of Pd@NP.
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CARBON
·
2013
·
IF 5.868
Xingyun Li,Xiulian Pan,Yonghua Zhou,Xinhe Bao
A C–SiC composite with a thin layer of carbon surrounding the SiC substrate has been produced by the reaction of SiC with CCl 4 . The pore structures , graphitization levels and the chemical compositions can be finely modulated by the synthesis temperature, and atmosphere. A higher synthesis temperature accelerates the chlorination rate, increases the thickness of carbon layers and enhances their graphitization. Mesopores can be generated in C–SiC composites in comparison to predominant micropores in commercial activated carbon (AC), particularly in the presence of reactive atmosphere such as CO 2 and NH 3 . Furthermore, with cofeeding of NH 3 with CCl 4 , N heteroatoms can be incorporated into the carbon layer and the N content varies in a range of 4.7–9.5 at.%, depending on the synthesis conditions. Both increased fraction of mesopores and their sizes, as well as N doping facilitate significantly hydrogenation of 4-carboxybenzaldehyde. The activity of Pd catalyst supported on N-doped C–SiC is five times that on commercially used AC under the same conditions.
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Advanced Healthcare Materials
·
2026
·
IF 11
Peng-Wei Chen,Yu-Meng Zhang,Lin-Song Li,Bang-Bang Liu,Han-Lu Sun,Liping Chen,Xiaojing Yang,Mei-Xia Zhao
The combination of phototherapy with oxaliplatin (OXA) represents a potent strategy for triggering immunogenic cell death (ICD) and elicit robust antitumor immunity. In this study, we construct IROTD nanoparticles (IROTD NPs) through self-assembly of a norcantharidin (NCTD)-OXA-conjugated polymer (P2) and the near-infrared (NIR) photosensitizer DTIR780. Under 808 nm laser irradiation, IROTD NPs generate heat and reactive oxygen species (ROS) while release OXA and NCTD, result in severe DNA damage and potent induction of ICD within tumor cells. Concurrently, NCTD inhibits DNA repair mechanisms and down-regulates PD-L1expression, thereby increase the infiltration of cytotoxic T-cell and amplify systemic antitumor immunity. Leverage the enhanced permeability and retention (EPR) effect, IROTD NPs efficiently accumulate at tumor sites, result in remarkable inhibition of tumor growth and recruitment of CD4 + and CD8 + T lymphocytes, which collectively contribute to the activation of a systemic antitumor immunity. In a bilateral tumor model, IROTD NPs effectively inhibit both primary and distant tumor growth. Overall, this work presents a rationally designed combinatorial nanoplatform that effectively ignites systemic immune response, thus establish a prospective chemo-immunotherapeutic stratagem for cancer treatment.
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JOURNAL OF POWER SOURCES
·
2026
·
IF 8.4
Zhengnan Li,Bin Zhang,Xiang Xu,Han Lin,Tuo Ji,Liwen Mu,Xiaohua Lu,Jiahua Zhu
The requirement for surface wetting to enhance efficient electrolysis reactions, along with the need for dewetting to accelerate H 2 desorption from the electrode surface, creates a paradox in effective electrode design. In this study, we created an asymmetric hydrogen evolution reaction (HER) electrode that synergizes mass transfer and reaction processes on both sides. Using plasma-enhanced chemical vapor deposition (PECVD) and atomic layer deposition (ALD), we fabricated an asymmetric self-supported electrode (CW-GNs-Pd) on carbonized cedar wood. This electrode features a graphene-coated side with high roughness, enhancing superhydrophobicity for efficient hydrogen bubble desorption, while the uncoated side retains the natural porous structure for rapid mass transfer. Pd single atoms and nanoclusters were deposited on the graphene surface via ALD,modifying the electronic structure of the Pd active sites, as confirmed by XPS (Pd 3d peaks) and XAS (Pd K-edge absorption). The CW-GNs-Pd electrode demonstrates exceptional HER performance in both alkaline and acidic environments, achieving low overpotentials of 29 mV and 45 mV at 10 mA cm −2 , with Tafel slopes of 24.73 mV dec −1 and 10.11 mV dec −1 , respectively. It also shows remarkable stability over 120 h. The unique design, which separates mass transfer and catalytic zones, addresses traditional electrode limitations and presents a promising strategy for developing cost-effective, high-performance HER electrodes.
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APPLIED CATALYSIS A-GENERAL
·
2026
·
IF 4.8
Haodong Huang,Bo Chen,Zhiwei Zheng,Changyi Chen,Ruifeng Luo,Haijun Guo,Zhili Li,Xinde Chen
1,2-propanediol (1,2-PDO) and ethylene glycol (EG), as key precursors for high-value fine chemicals, represent one of the core challenges in green chemical engineering through the development of biomass-directed conversion systems. This study constructed a bifunctional x%NiO@Hβ-1%Pd hierarchical porous catalyst through an interfacial engineering strategy: utilizing the confinement effect of two-dimensional mesoporous nickel silicate nanosheets to load Ni onto Hβ zeolite, and anchored highly dispersed Pd nanoparticles on the NiO@Hβ surface through NaBH 4 -induced in situ reduction, systematically investigated the structure-activity relationship of this catalyst for sorbitol hydrogenolysis in Ca(OH) 2 alkaline aqueous systems. Combined NH 3 -TPD and N 2 adsorption-desorption characterization revealed that, the introduction of Hβ zeolite significantly modulated the catalyst acidity and pore structure—the total acid amount of 25%NiO@Hβ-1%Pd reached 4.13 mmol/g (representing a 104% enhancement compared to the support-free system), the desorption peak at 550°C corresponds to strong Lewis acid sites formed by Ni-O-Si bonds, the pore system with 69% mesopore content (BET specific surface area of 541.6 m 2 /g) provides efficient transport pathways for reactant diffusion. Mechanistic studies revealed that, the Brønsted acid sites of Hβ selectively adsorb sorbitol C-O bonds through hydrogen bonding interactions, while spillover hydrogen species at the Pd-Ni interface synergistically induce selective C-C bond cleavage in cooperation with strong Lewis acid sites, ultimately achieved a total diol carbon yield of 80.3 C% for 1,2-PDO/EG under conditions of 220°C and 3 MPa H 2 . This work provides new insights into the “acid-metal-mass transfer” ternary synergistic mechanism for precise hydrogenolysis of biomass polyols.
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International Journal of Electrochemical Science
·
2023
·Vol. 7
·期 1
·106-119
·
IF 1.5
Yun Zhi Fu,Yun Yang
Nanostructured Pd networks were synthesized in high yield through the reduction of Pd (acac) 2 using oleylamine as the solvent, reductant and capping agent. The formation of the network Pd nanostructure is due to oriented attachment among the formed primary particles at high temperature. By adjusting the reaction time, concentration of Pd precursor and reaction temperature, their thickness and interconnectivity can be tuned. The prepared nanostructured Pd networks exhibit efficient electrocatalytic activities toward the oxidation of formic acid in acid media. The enhanced electrocatalytic properties of Pd networks can be attributed to the interconnectivity and presence of a large number of active sites on their surfaces.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Yiran Sun,Xingyue Zhou,Sikai Dai,Yu Fan,Chengkun Xie,Ruoqi Wang,Jun Qian,Lingzhi Nie,Peiyuan Zuo,Qixin Zhuang
High-entropy alloys (HEAs) are promising electromagnetic absorbers owing to tunable magneto-dielectric properties, yet severe particle agglomeration and grain coarsening severely degrade their wave-absorbing capacity. Herein, a Pd-mellitic acid ligand-induced strategy is developed to immobilize uniform FeCoNiCuPd quinary HEA nanoparticles on one-dimensional hollow mesoporous carbon nanorods (CPMO@5 A). Multidentate carboxyl groups of mellitic acid serve as universal coordination sites for synchronous multi-metal nucleation, effectively restraining HEA aggregation and triggering prominent grain refinement and lattice distortion driven by high configurational entropy. Benefiting from hierarchical porous architecture, uniform-dispersed HEA nanoparticles and abundant heterogeneous crystal defects, CPMO@5 A achieves superior electromagnetic wave absorption. It delivers a minimum reflection loss of −76.6 dB at 2.7 mm and an ultra-wide effective absorption bandwidth of 8.4 GHz, covering the entire Ku-band and most X-band. Meanwhile, it exhibits infrared absorptivities of 98.2%, 98.9% and 97.7% in long-wave, mid-wave and short-wave infrared regions, outperforming most reported HEA absorbers. Dielectric loss from Cu and carbon matrix, coupled with magnetic loss of Fe, Co, Ni and Pd, synergistically promotes electromagnetic energy dissipation. This work provides a facile universal route for fabricating HEA-based electromagnetic materials for high-performance radar-infrared compatible stealth materials.
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Small
·
2026
·
IF 11.8
Chao Ma,Xinxin Liang,Yongqian Cui,Xinyu Yang,Qibing Dong,Abdelkader Labidi,Chuanyi Wang
Photocatalytic upcycling of polylactic acid (PLA) via a two-step process-hydrothermal depolymerization to a lactic acid (LA)-rich hydrolysate followed by selective photocatalytic oxidation to form value-added chemicals-presents a sustainable pathway for plastic waste upgrading. However, the efficient activation of LA molecules and effective generation of key intermediates remain significant challenges. Herein, Pd nanoparticle-modified ZnIn 2 S 4 (Pd-ZIS) nanosheets were developed to promote selective conversion of PLA hydrolysate to acetic acid (AA). In situ FTIR spectral analysis indicates that Pd nanoparticles promote electron transfer and O 2 dissociation, accelerating the generation of hydroxyl radicals via proton-coupled electron transfer (PCET). Furthermore, in situ electron paramagnetic resonance (EPR) results reveal that Pd nanoparticles effectively activate the C α ─C COOH bond in LA molecules, promoting the formation of acetyl radical intermediates that subsequently couple with hydroxyl radicals to yield AA. Consequently, the optimized 0.5 wt% Pd-ZIS catalyst exhibits superior performance, achieving an AA production rate of 4.2 mmol g −1 h −1 with a selectivity of 88.7% and an apparent quantum yield of 1.31% ( λ = 380 nm). These performance metrics surpass those reported in most previous studies. This work offers novel insights into catalyst design for waste plastic upcycling, deepening the understanding of the mechanisms to effectively regulate the underlying complex reaction pathways.
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Molecular Catalysis
·
2026
·
IF 4.3
Haonan Ying,Zheng Xiong,Xinwei Yang,Min Ding,Li Wang,Yun Guo,Yanglong Guo,Wangcheng Zhan,Jihang Yu,Aiyong Wang
Co 3 O 4 is a promising catalyst for propane combustion but is limited by poor water resistance and insufficient high-temperature stability. Noble metal loading is widely employed to enhance its performance, however, the metal-specific effects remain poorly understood. In this work, Co 3 O 4 -supported Pt, Pd, and Ru catalysts were systematically investigated for propane oxidation. It was found that all noble metals decreased the surface Co 2+ content and oxygen vacancies, leading to modified redox behavior and propane activation ability. Among them, Ru incorporation enhanced the catalytic activity (T 90 = 266 °C) of Co 3 O 4 (T 90 = 286 °C) and significantly improved its water resistance and thermal stability. These improvements are mainly attributed to the abundant partially oxidized RuO x species, which provide additional active sites and facilitate propane adsorption and activation. In contrast, Pt and Pd modification inhibited propane oxidation due to the intrinsically low activity of highly oxidized Pt species and PdO, as well as the coverage of Co 3 O 4 active sites caused by highly dispersed Pt and particulate PdO. The findings offer mechanistic insights for the rational design of efficient catalysts for propane combustion and VOCs abatement.
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Scientific Reports
·
2026
·
IF 4.9
Zhou Kun,Yuan Wei,Zhang Fan
Radix Bupleuri-Radix Paeoniae Alba (RB-RPA) has the potential to ameliorate the immune microenvironment in hepatocellular carcinoma (HCC). The interactions between various cells influence the immune microenvironment. However, the effects of the active components (saikosaponin D (SSD) and paeoniflorin) of RB-RPA on HCC and the cell interactions within its microenvironment warrant further investigations. We established orthotopic mouse models of HCC using Hepa 1–6 cells (a hepatoma cell line) to investigate the infiltration of cancer-associated fibroblasts (CAFs). Following this, we knocked down CLCF1 in the CAFs to explore their interactions with Hepa 1–6 cells. We subsequently treated CAFs with SSD-paeoniflorin. In T-cell activation assays, we overexpressed PD-L1 in Hepa 1–6 cells and co-cultured these cells with T cells. Additionally, we treated HCC mice with SSD-paeoniflorin and induced the overexpression of CLCF1 in vivo. In mice with HCC, tumors were characterized by substantial infiltration of CAFs, which displayed elevated levels of the protein CLCF1. These CAFs play a role in suppressing the HCC immune microenvironment and elevating PD-L1 levels through the production of CLCF1. At the cellular level, SSD-paeoniflorin inhibited the growth of CAFs and the expression of CLCF1 and also suppressed the PD-L1 level in Hepa 1–6 cells through CAF-derived CLCF1. Mechanistically, CLCF1 may promote PD-L1 expression via the JAK/STAT3 signaling pathway. Furthermore, the overexpression of PD-L1 in Hepa 1–6 cells suppressed T cell proliferation and activation. In animal studies, SSD-paeoniflorin improved the HCC immune microenvironment by enhancing the interaction between CAFs and Hepa 1–6 cells through CLCF1. Collectively, SSD-paeoniflorin inhibits CLCF1 secretion in CAFs to downregulate PD-L1 expression in Hepa 1–6 cells and may reactivate the anti-tumor immune microenvironment in HCC.
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ACS ES&T Water
·
2026
·
IF 4.5
Jingjing Liu,Liyu Shi,ShuoShuo Mao,Fang Li,Juan Zhou
The remediation of aquatic environments cocontaminated with halogenated organics and phenolic pollutants poses a significant challenge to conventional single-mode treatment technologies. To address this, we engineered a bifunctional Pd–CoFe2O4 catalyst that orchestrates a synergistic reductive–oxidative (R–O) cascade for the simultaneous elimination of monoiodoacetic acid (MIAA) and bisphenol A (BPA). This system operates on a novel converting reduction byproducts into catalytic resources strategy: initially, favorable hydrodeiodization of MIAA occurs on Pd sites using NaBH4 as a hydrogen source, releasing iodide ions (I–). Crucially, rather than persisting as waste, these I– ions serve as in situ mediators that activate peroxymonosulfate (PMS) in the subsequent oxidative stage. The rapidly generated reactive iodine species (RIS, e.g., I•, IO3–) facilitate the ultrafast degradation of BPA within 5 min, significantly outperforming standalone advanced oxidation processes. Mechanistically, the Pd0/Pdn+ species determine the reductive efficiency, while the Co2+/Co3+ redox cycle on the spinel support amplifies PMS activation. Consequently, this integrated R–O system achieves a 67% total organic carbon (TOC) removal efficiency, far exceeding the 17% of the molecular oxidation alone. This work establishes a transformative paradigm for converting reduction byproducts into catalytic assets for the efficient treatment of complex wastewater.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Chengxun Li,Fei Chen,Jianing Wu,Jun Ren,Yingzhu Li,Shengjie Li,Zuguang Xia
Antibody drug conjugates (ADCs) offer targeted cancer therapy but face limitations in drug loading, stability, and immune modulation. Here, antibody DNA nanostructure conjugates (ADNCs) is reported as a next-generation platform that overcomes these challenges. By leveraging the programmable architecture of DNA nanostructures, ADNCs achieve high, tunable drug payloads without inducing antibody aggregation—a major drawback of conventional ADCs. In CT26 cells, gemcitabine-loaded ADNCs trigger dual cell death pathways—caspase-3-mediated apoptosis and RIP3-mediated necroptosis—enhancing tumor cell killing. In the CT26 syngeneic model, ADNCs suppress tumor growth with no observable toxicity and, notably, activate anti-tumor immunity without upregulating PD-1, suggesting avoidance of T-cell exhaustion. Critically, ADNCs maintain efficacy in patient-derived xenograft (PDX) models despite tumor heterogeneity. The study presents a novel, stable, and scalable antibody-drug conjugate (ADC)-inspired platform that integrates high payload delivery capacity with enhanced and adjustable drug-loading capabilities—characteristics that are seldom achieved in existing ADC technologies—thereby demonstrating translational potential for applications in precision oncology.
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