LANGMUIR
·
2025
·
IF 3.9
Chen Shen,Binyu Zhang,Haiyong Wang,Mi Luo,Tianhan Zhu,Tianyu Gao,Tong Zhang,Xiaoli Chen,Chenguang Wang
Precise modulation of interfacial electronic structures is crucial for enhancing the catalytic activity and selectivity in heterogeneous catalysis. The electron penetration effect (EPE), involving electron transfer from a metal core through a protective shell to surface active sites, has emerged as an effective strategy for tuning surface electronic properties and promoting catalytic performance. However, controlled manipulation of EPE remains challenging, particularly in regulating the phase structure of the metal core and the characteristics of the encapsulating shell. In this work, nitrogen-doped graphene-coated Ni nanoparticles were synthesized from a Ni-based metal–organic framework (Ni-MOF-T/t) by systematically adjusting the reduction temperature (T) and time (t). Subsequent deposition of Pd species yielded Pd/Ni-MOF-T/t catalysts. Among them, the optimized Pd/Ni-MOF-400 °C/2 h catalyst, featuring a hexagonal Ni core, exhibited enhanced electron penetration across the graphitic shell to the Pd sites, effectively modulating the surface electronic structure and boosting catalytic activity. The catalyst demonstrated excellent performance in both thermocatalytic hydrogenation of benzonitrile (90% conversion, 99.0% selectivity) and electrochemical hydrogenation of 4-nitrophenol (96.5% conversion, 90.5% Faradaic efficiency). These findings highlight that phase-controlled electron penetration provides a versatile and generalizable approach for constructing multifunctional catalysts with superior activity under mild conditions. This work establishes phase engineering of MOF-derived metal–carbon interfaces as an effective strategy to manipulate electron penetration effects and optimize catalytic performance.
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Journal of Cleaner Production
·
2025
·
IF 10
Tao Jiang,Ming Cheng,Yujiao Wang,Shaoqiang Guo,Wentao Zhou,Yafei Wang
The selective removal of neutron-absorbing fission products from spent nuclear fuel is critical for enhancing neutron economy and enabling efficient recycling. In this work, we present a novel two-step dry reprocessing strategy that integrates NH 3 /HCl gas mixture treatment with liquid Sn extraction to achieve phase-selective separation of Sm, Nd, Ru, Rh, and Pd from simulated U 3 O 8 -based spent fuel. Thermodynamic analysis and experimental validation reveal that decomposition of NH 4 Cl at elevated temperatures serves as the generator of NH 3 /HCl gas mixture capable of selectively chlorinating Sm 2 O 3 and Nd 2 O 3 into soluble chlorides while reducing U 3 O 8 to UO 2 and converting RuO 2 , Rh 2 O 3 , and PdO to their metallic states (Ru, Rh, Pd). Subsequent dissolution tests in LiCl-KCl confirm that Sm and Nd are almost completely removed, with chlorination efficiencies of nearly 100%, while uranium loss can be minimized by controlling direct NH 4 Cl contact. The coupled liquid Sn extraction at 1173 K enabled the recoveries of metallic Rh, Rh, and Pd with a promising extraction efficiency. This integrated approach significantly simplifies the partitioning of key neutron poisons (Sm, Nd, Ru, Rh, Pd) compared to conventional aqueous or pyrochemical routes, reduces secondary waste, and preserves uranium in its UO 2 form.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
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IF 5.816
Xiang Gong,Shuyi Guo,Zhao Jiang,Bolun Yang,Tao Fang
Hydrogen is a promising candidate to substitute the fossil fuels. However, the efficient hydrogen storage technologies restrict the commercial applications. Developing new catalysts with high activity and selectivity is important for the dehydrogenation reaction in N-ethylcarbazole/dodecahydro-N-ethylcarbazole (NECZ/12H-NECZ) hydrogen storage system. In this work, a series of Pd-M/Al 2 O 3 (M = Co, Ni and Cu) bimetallic catalysts are synthesized successfully and show good performance in the dehydrogenation reaction of 12H-NECZ than the commercial Pd/Al 2 O 3 catalyst. The Pd 1 Co 1 /Al 2 O 3 catalyst (Practical Pd content = 2.4136 wt%) showed the highest catalytic performance with 95.34% H 2 release amount, TOF of 230.5 min −1 and 85.4% selectivity of NECZ. Combined with the characterization analysis, it can be proposed that the dehydrogenation performance of 12H-NECZ is dependent on the alloy phases , reasonable electronic structures and nanoparticle size of catalysts. The fine-tuned alloy degree and appropriate nanoparticle size of Pd 1 Co 1 /Al 2 O 3 bring the 17.7% increase of H 2 release amount and 99.5% increase of NECZ selectivity than those of Pd/Al 2 O 3 . For the bimetallic catalysts, the enhancement of selectivity of NECZ is mainly from the increase of the kinetic constant of rate-limiting step.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
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IF 9.4
Yong Xu,Yue Wang,Ping Wang,Yishun Wang,Weili Dai,Jianping Zou,Xubiao Luo
Employing electric energy to convert carbon dioxide (CO 2 ) into valuable small molecules is a potentially practical method in energy storage and greenhouse gas alleviation. A huge challenge for electrocatalytic CO 2 reduction is to reduce overpotential to improve energy efficiency. Herein, we demonstrate that doping alloy Pd 49 Ag 30 Te 4 (PAT) with rare-earth element Tb is beneficial for selective exposure of (1 1 1) crystal plane, which is a highly active crystal plane for producing carbon monoxide (CO). The as-prepared Tb 2.9 PAT exhibited high electrocatalytic performance with 95.7 % CO faradic efficiency at − 0.8 V (vs RHE), far exceeding that of PAT, and coupled with good durability. In situ spectral study and theoretical calculations disclose that the introduction of Tb regulates the d-band center of PAT alloy, weakens the Pd − C bonding ability, and promotes the desorption of *CO in the rate-determining step. This study provides a method for doping induced selective exposure of crystal face, which provides new idea for improving catalytic performance.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Siyuan Meng,Fangnan Lv,Jieqing Chen,Linlin Tao,Hao Guo,Danhui Wang,Jie Sun,Jian Li,Ning Liu,Wei Xu,Meirong Huo
A biomimetic antigen outpost is engineered to sustainably co-deliver tumor antigens, siSOCS1, and Mn 2+ adjuvant. • Plasma gel recruits DCs to the injection site, while CRT on nanovaccines acts as an "eat-me" signal to enhance antigen uptake. • SOCS1 silencing and PD-L1 blockade synergistically empower DCs to more effectively prime and activate cytotoxic T lymphocytes (CTLs). • PD-L1 blockade further protects activated CTLs from tumor cell-mediated exhaustion, enabling sustained tumor killing and potent antitumor immunity in TNBC models. Tumor vaccines represent a promising immunotherapy approach but are challenged by rapid systemic clearance, low immunogenicity, and various immunosuppressive mechanisms. To overcome these issues, we created a biomimetic antigen outpost system to enhance vaccine delivery and immune activation. This system uses cationic 1,2-dihydroxybenzene-modified poly- l -lysine to co-load small interfering RNA targeting cytokine-suppressing factor 1 (siSOCS1) and immunoadjuvant (Mn 2+ ) as the core. This core is further coated with calreticulin (CRT)-enriched tumor cell membranes to form a nanovaccine (CRTM/PBM siSOCS1 ), which is ultimately encapsulated in a plasma gel (PG@CRTM/PBM siSOCS1 ). This design prolongs the vaccine's in vivo retention, recruits dendritic cells (DCs) by simulating subcutaneous hemorrhage signals, and enhances effective antigen uptake through CRT-mediated “eat me” signals. Upon DC internalization, the nanovaccine undergoes non-lysosomal trafficking, avoiding siSOCS1 degradation. The efficient SOCS1 silencing alleviates intracellular immunosuppressive feedback and, together with synergistic DC activation by antigens and Mn 2+ , further promotes DC maturation and antigen cross-presentation. In a triple-negative breast cancer model, the combination with anti-PD-L1 antibody simultaneously blocked PD-L1 on both mature DCs and tumor cells, significantly enhancing cytotoxic T lymphocyte function at both the immune priming and effector stages, and demonstrating potent antitumor efficacy. This multi-level intervention strategy provides a promising platform for enhancing cancer immunotherapy. Download: Download high-res image (112KB) Download: Download full-size image
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International Journal of Nanomedicine
·
2026
·
IF 8.7
Jing Zhang,Xiaoqiang Kong,Xiangping Wu,Dongyun Tao,Xiang Li,Huimin Cheng
Introduction Triple-negative breast cancer (TNBC) is an aggressive malignancy with poor prognosis, and Fusobacterium nucleatum (Fn) colonization further aggravates tumor progression, immunosuppression and therapeutic resistance. Conventional monotherapies are limited by insufficient tumor targeting, rapid drug clearance and failure to reverse immune suppression. Here, we fabricated cRGD-modified nanoparticles (Ag@GQDs/QUE-siP-c-L) for co-delivery of AgNPs, quercetin (QUE) and PD-L1 siRNA (siP).Methods The morphology, particle size, surface metal elements, drug content and QUE entrapment efficiency of Ag@GQDs/QUE-siP-c-L were obtained using particle size analysis, SEM, inductively coupled plasma-optical emission spectrometry (ICP-OES) and HPLC. We further detected cellular uptake, in vitro drug release, cytotoxicity, intracellular reactive oxygen species level, PD-L1 gene silencing efficiency and in vitro anti-Fn activity. Pharmacokinetics and tissue distribution of Ag and QUE were analyzed by ICP-OES and LC-MS/MS, and in vivo antitumor efficacy and biosafety were tested in Fn-colonized orthotopic 4T1 tumor mice.Results Ag@GQDs/QUE-siP-c-L exhibited uniform spherical morphology (195.87± 15.96 nm) with high encapsulation of QUE. cRGD modification enhanced Ag/QUE cellular uptake in 4T1 cells, with pH-responsive release accelerated under tumor acidic conditions. The nanoparticles exhibited selective tumor cytotoxicity, induced oxidative stress, downregulated PD-L1 mRNA, and exerted potent anti-Fn activity in vitro. Pharmacokinetics revealed increased AUC0-t and reduced clearance compared with free drugs, and cRGD modification promoted tumor accumulation and retention of drugs. In vivo preliminary experiments proved the Ag@GQDs/QUE-siP-c-L formulation suppressed tumor growth with a tumor inhibition rate of 45%, and effectively modulated the tumor immune microenvironment: it increased tumor-infiltrating CD3⁺CD4⁺ T cells, reduced PD-L1⁺CD11c⁺ dendritic cells, and decreased the proportions of immunosuppressive Tregs and MDSCs. Hematoxylin-eosin staining and serum liver-kidney biochemistry confirmed no obvious systemic toxicity.Conclusion Ag@GQDs/QUE-siP-c-L serves as a multimodal nanoplatform for Fn-associated TNBC with combined in vitro antibacterial, gene silencing and in vivo antitumor immunomodulatory effects, showing great potential for future translational research.
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Interdisciplinary Medicine
·
2026
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IF 14.5
Bo Pan,Shicui Hong,Xinyue Wang,Yanghang Li,Cai Wang,Yaxiao Liu,Ying Chen,Chen Fang,Yifeng Zheng,Shengqi Wang,Juping Zhang,Neng Wang,Zhiyu Wang
Triple-negative breast cancer (TNBC) remains a clinical challenge due to its high risk of recurrence and metastasis, coupled with limited responses to immunotherapy. Tumor-associated macrophages (TAMs) contribute to immunosuppression in the tumor microenvironment (TME) through C-X-C motif ligand 1 (CXCL1) secretion, but their targeting is hindered by poor drug delivery efficiency and physical barriers imposed by cancer-associated fibroblasts (CAFs). To address this, we developed a TAM-targeting black phosphorus nanosystem (αM2-BP-BHS, MBB) loaded with Baohuoside I (BHS), a known inhibitor of TAM polarization and CXCL1 secretion. In vitro and in vivo studies demonstrated that MBB efficiently targets TAMs and penetrates CAF barriers via photothermal activation under 808 nm near-infrared (NIR) irradiation, significantly enhancing BHS-mediated suppression of TAM/CXCL1 signaling. Furthermore, MBB-mediated photothermal therapy (PTT) boosted the memory T cell population, CD8 + T-cell infiltration and cytotoxic cytokine expression. When combined with anti-PD-L1 therapy, MBB synergistically suppressed TNBC progression and metastasis while establishing durable anti-cancer immunity to prevent recurrence. Notably, MBB exhibited excellent biocompatibility with minimal off-target effects, underscoring its potential as a precision delivery platform for BHS. Our findings highlight MBB as a promising adjuvant to potentiate immunotherapy in TNBC by concurrently overcoming stromal resistance and reprogramming immunosuppressive TME.
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Molecular Biomedicine
·
2026
·Vol. 7
·期 1
·129
·
IF 13
Wang Zhengshi,Jia Chengyou,Liu Yongqiang,Rixiati Youlutuziayi,Zhang Wentao,Mao Shiyu,Chen Haotian,Zou Libin,Ye Chen,Shen Bing,Yao Xudong
Prostate cancer (PCa) is one of the most common cancers in males, and its treatment remains challenging due to the tumor microenvironment (TME) with immunosuppressive properties and limited response to anti-PD-1 therapy. Gut microbiota-derived metabolites have recently emerged as modulators of cancer immunometabolism, however, their role in PCa progression and immunotherapy is poorly understood. Here we found that indole-3-lactic acid (ILA), a metabolite produced by Lactobacillus plantarum , exerted dual anti-tumor effects on PCa cells and the TME. Mechanistically, ILA activates the aryl hydrocarbon receptor (AHR), and the resulting AHR/ARNT heterodimer translocates into the nucleus and binds to the promoter of ASF1B. This heterodimer then recruits the HDAC1/2-NuRD complex to reduce H3K27ac levels and suppress ASF1B expression. ASF1B binds to specific residues of ENO1 via its N-terminal core domain and enhances ENO1 enzymatic activity. ILA-induced downregulation of ASF1B impairs this interaction, reduces ENO1 activity, and suppresses the PI3K/Akt pathway, thereby inhibiting the malignant phenotypes of PCa cells. Concurrently, ILA decreased CXCL8 secretion by inhibiting the PI3K/Akt/NF-κB pathway, enhancing CD8 + T cell infiltration and M1 macrophage polarization, thereby remodeling the TME. Additionally, ILA synergized with anti-PD-1 therapy to more effectively suppress tumor growth. These findings reveal a novel mechanism by which gut microbiota-derived metabolites regulate PCa progression and immunometabolism, positioning ILA as a potential therapeutic agent to improve PCa treatment.
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Nanoscale
·
2023
·Vol. 15
·期 8
·3772-3779
·
IF 6.7
Qiaoli Chen,Hui Jin,Tianchun Cheng,Zhi Wang,Yaoyao Ren,Jinshu Tian,Yihan Zhu
Proton-exchange membrane fuel cells are considered as promising energy-conversion devices. Alloying 3d transition metals with noble metals not only highly improves the performance of noble metal-based catalysts towards electrocatalytic reactions in fuel cells due to d–d hybridization interaction but also decreases the total cost. However, the rapid leaching of transition metal atoms leads to a fast decay of the activity, which seriously affects the performance of the fuel cell. Herein, alloyed Pd-main group metal (e.g. Pb, Bi, Sn) ultrathin nanowires were realized by a facile one-step wet-chemical strategy. The content of the main group metal could be tuned in a certain range while maintaining the same one-dimensional ultrathin nanowire morphology, which provided a large surface area and many more active sites. These Pd-based alloys showed a significant improvement in electrocatalytic activity and durability towards the oxygen reaction reaction as well as ethanol oxidation reaction. Optimal activity occurred when a small amount of main group metal existed, which could be explained through calculations by a strong p–d hybridization interaction between the main group metal and Pd to optimize the surface electronic structure collaboratively. Besides, high stability was achieved, which could be ascribed to the increased antioxidant activity of Pd by the main group metal. Furthermore, the low amount of the main group metal atoms also prevented them from leaching out of the crystal lattice.
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Arabian Journal of Chemistry
·
2022
·
IF 6.212
Donghai Jiang,Yongyong Shi,Liming Zhou,Jun Ma,Hongyan Pan,Qian Lin
Nitrogen-doped porous carbon is potential support for directly synthesizing H 2 O 2 from H 2 and O 2 . Here, density functional theory (DFT) was used to study the effect of N -doped porous carbon on H 2 O 2 directly synthesized. The theoretical calculation results showed that N -doped improved H 2 O 2 productivity and H 2 conversion by increasing the dispersion of Pd nanoparticles and the Pd 0 /Pd 2+ ratio. However, N -doped decreased H 2 O 2 selectivity by reducing oxygen's dissociation energies. The experimental results showed that adjusting the pore structure of N -doped porous carbon could improve the adverse effects of N -doping for H 2 O 2 selectivity. The H 2 O 2 productivity and selectivity of Pd/C catalyst with a macropore-mesoporous-microporous hierarchical porous structure were up to 328.4 mol H2O2 ·kg cat -1 ·h −1 and 71.9 %, respectively, at ambient pressure. The macropore structure enhances the transfer and diffusion performance of the catalyst and effectively inhibits the effect of N -doping on O O bond dissociation, which improves H 2 O 2 productivity and selectivity. This research provides a possible solution for designing a high-performance Pd/C catalyst to directly synthesize H 2 O 2 from H 2 and O 2 at ambient pressure.
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FOOD CONTROL
·
2022
·
IF 6.652
Chengyuan Wu,Xiangchuan Wu,Fan Hou,Lina Wu,Guangxia Liu
An ultrasensitive electrochemical aptasensor was established based on metalloporphyrin metal organic frameworks ( [email protected] ) with peroxidase-like activity and exonuclease III-assisted recycling magnification for the detection of ochratoxin A (OTA). [email protected] showed well peroxidase-like activities due to Fe-tetrakis (4-carboxyphenyl) porphyrin (Fe-TCPP) as a heme-like ligand and in situ supported with palladium nanoparticle, which could be used for the label of ssDNA instead of nature enzyme. The designed exonuclease III-assisted recycling magnification further improve the sensitivity for the detection. Based on this, the proposed aptasensor showed a well linear relationship within the scope of 1 × 10 −5 ng mL −1 to 10 ng mL −1 and a low detection limit of 6.79 fg mL −1 . Additionally, the application in the real spiked oil samples confirmed the dependability and veracity of the aptasensor. Hence, the designed aptasensor has comprehensive application prospects for the detection of OTA in food .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Ningfan Song,Zihan Chen,Jinghua Shi,Dezhi Shi,Li Gu
In the present study, a Pd/Cu bimetallic catalyst supported on a chelating resin (TP207) was prepared in order to selectively reduce nitrate to N 2 with ZVI (zero valent iron) as a reductant. The effects of Pd/Cu mass ratio, temperature, and initial solution pH on the removal of nitrate and TN were then examined. The highest nitrate (63.2%) removal was obtained under neutral conditions at a ratio of Pd/Cu 2:1, in which 57.8% of TN was removed and N 2 accounted for more than 90% of the final products. Additional ammonia (30–40%) were formed when the reaction was conducted at a higher temperature (313 K) compared to when performed at 303 K. The mechanism study for nitrate reduction indicated that this catalyst could broaden the suitable pH range and improve the selectivity of N 2 without the generation of other intermediate compounds or by-products in comparison to ZVI and its combination with a non-supported Pd/Cu catalyst. The slow rate of ZVI corrosion, high Fe(Ⅱ) proportion in corrosion products and high N/H ratio at neutral pH conditions may serve as reasons for the high N 2 selectivity. The chelating resin also played a key role via its load capacity and dispersion ability to Pd/Cu particles in enhancing N 2 selectivity. Accordingly, the proposed method may have great potential application for nitrate reduction to N 2 , which warrants further study.
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