JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
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.
✓ 已验证
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2018
·Vol. 9
·期 2
·286-301
·
IF 5.365
Mengyuan Zhang,Shipeng Wu,Longchun Bian,Qiue Cao,Wenhao Fang
Ce–Ni mixed oxides with different Ni/Ce molar ratios, promoted by a rather low amount of Pd (0.2 wt%), were prepared by a simple one-pot precipitation method. The thus-synthesized CeNiXOY and Pd–CeNiXOY catalysts were applied respectively to the direct N-alkylation of amine and alcohol via oxidative coupling, under O2 in the absence of basic additives. The CeNiXOY catalyst could provide a >99% yield of imine in the model alkylation reaction of aniline with benzyl alcohol at 100 °C. The Pd-promoted Pd–CeNiXOY catalyst surprisingly showed an enhanced imine yield (>99%) at a mild temperature of 60 °C. This catalyst exhibited good reusability, and moreover, demonstrated high performance towards imine synthesis from various amines with alcohols. The presence of Pd species and the Ni/Ce molar ratio showed a synergistic impact on the conversion of aniline, as well as on the product selectivity, which was believed to be related to the improvement on the intrinsic activity of the oxidation of benzyl alcohol to benzaldehyde. Various physicochemical techniques, including ICP-MS, XRD, N2 adsorption–desorption, UV-Raman, H2-TPR, TEM, EPMA and XPS, were employed to study mainly the composition, structure and redox properties of the catalysts. The proportion of Ce3+ species and oxygen vacancies, which can be manipulated by the Ce–Ni redox system and the interaction between Ce and Ni, was crucial to the selective activation of alcohols in the presence of reactive amines. The activation of alcohol on the highly reactive Pd0 species was the other crucial factor.
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Kaihao Li,Yongwang Li,Yang Qin,Zheng Wang,Bingxin Zhu,Yancong Yin,Fumin Wang,Xubin Zhang
The production of high-purity hydrogen chloride from petrochemical by-product hydrogen chloride gas represents the primary industrial approach for manufacturing electronic-grade hydrogen chloride. However, trace acetylene and ethylene impurities in the feedstock severely compromise product quality. This study innovatively proposes a "stepwise conversion-deep chlorination" synergistic mechanism and successfully develops a bimetallic catalyst (10 %Fe/0.5 %Pd/AC). By tailoring the preparation processes, we precisely controlled the distribution of Fe and Pd active sites, while systematically comparing the performance between Single-metal tandem catalytic system (Pd/AC + Fe/AC) and the bimetallic catalyst. Experimental results combined with DFT calculations demonstrate the superior performance of the 10 %Fe/0.5 %Pd/AC catalyst and confirm the cascade reaction mechanism based on the synergistic tandem effect of Fe/Pd active sites: Acetylene preferentially undergoes hydrochlorination at Pd sites to form vinyl chloride, while ethylene and the resultant vinyl chloride are subsequently converted to chloroethane and more easily removable 1,1-dichloroethane at Fe sites. Under optimized conditions (120 °C, GHSV=180 h −1 ), removal efficiencies exceeding 99 % for both acetylene and ethylene were achieved, with 1,1-dichloroethane selectivity surpassing 99 %. Comprehensive characterizations demonstrated the outstanding stability of the 10 %Fe/0.5 %Pd/AC catalyst. This study presents an innovative catalytic approach for high-efficiency purification of industrial hydrogen chloride.
✓ 已验证
产品关联
DOI
高影响因子
Coatings
·
2025
·Vol. 15
·期 9
·1027
·
IF 2.8
Minglei Yang,Zhenhong Xu,Chongjun Tang,Shuaijie Wang,Zhourong Xiao,Fei Ye
This research introduces a synergistic photoelectrocatalytic (PEC) system designed for the effective degradation of tetracycline (TC), integrating a PO43−-grafted Mo-doped BiVO4(PO43−-Mo:BiVO4) photoanode with a Pd-loaded ordered mesoporous carbon (Pd/CMK-3) cathode. The incorporation of Mo doping and PO43−modification significantly improved the photoanode’s charge separation efficiency, achieving a photocurrent density of 2.9 mA cm−2, and fine-tuned its band structure to enhance hydroxyl radical (·OH) generation. Meanwhile, the Pd/CMK-3 cathode promoted a two-electron oxygen reduction reaction pathway, producing hydrogen peroxide (H2O2) and facilitating molecular oxygen activation via atomic hydrogen (H*) intermediates. Under optimized conditions—1.0 V vs. Ag/AgCl of anodic potential, pH 6.58, and oxygen saturation—the combined system accomplished 80% TC degradation within 60 min, markedly surpassing the performance of the photoanode (72%) or cathode (71%) alone. Notably, this synergistic approach also reduced energy consumption to 0.0065 kWh m−3, outperforming individual components. Radical quenching experiments and liquid chromatography–mass spectrometry (LC-MS) analysis revealed that the photogenerated holes (h+) and ·OH were the key reactive species responsible for TC mineralization. The system demonstrated remarkable stability, with only a 2.96% decline in activity, and effectively degraded other contaminants, such as phenol, 4-chlorophenol, and ciprofloxacin. This study highlights an energy-efficient PEC strategy that harnesses the combined strengths of anodic oxidation and cathodic molecular oxygen activation to significantly enhance the removal of organic pollutants.
✓ 已验证
产品关联
DOI
高影响因子
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
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
Interdisciplinary Medicine
·
2026
·
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.
✓ 已验证
DOI
高影响因子
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.
✓ 已验证
DOI
高影响因子
Gland Surgery
·
2022
·
IF 2.16
Meili Zhang,Jialei Gu,Wendong Wang,Kejing Wang,Linfeng Zheng,Jianguo Feng,Jinbiao Shang
Background Identifying the high recurrence group of patients with early-stage papillary thyroid cancer (PTC) is the greatest challenge in the management of this disease. It has been noted that B-type Rafkinase (BRAF) V600E mutation and programmed death ligand 1 (PD-L1) are associated in PTC and highly expressed in PTC, correlating in PTC as potential prognostic biomarkers. However, whether they can be used to predict the aggressiveness and recurrence of early PTC remains unclear. Methods Clinicopathological data of 137 patients with early PTC [tumor-node-metastasis (TNM) stage I–II] who underwent surgery in Zhejiang Cancer Hospital between 2008 and 2010 were retrospectively analyzed. BRAF V600E mutation and PD-L1 was detected by immunohistochemistry. The median follow-up time was 136 months (interquartile range 5.8). The presence of tumor confirmed by imaging or pathology or lymph node metastasis was considered as tumor recurrence. The association of both alone and in combination with clinicopathological features and recurrence was statistically analyzed respectively. The risk of recurrence was assessed using Cox regression models. Results Most of the 137 early PTC were female (78.1%). The mean age was 43.2±12.1 years. The median tumor size was 1.4 cm; 14 patients developed recurrence during follow-up period; 56 patients (40.9%) were detected positive for BRAF V600E mutation; 76 patients (55.5%) were detected positive for PD-L1. Patients with both BRAF V600E mutation and PD-L1 expression had larger tumors (P=0.038), were more likely to have extrathyroidal invasion (P=0.045), and had a lower rate of cervical lymph node metastasis (P=0.046). The recurrence rate was 17.5% (7/40) in patients with BRAF V600E mutation and PD-L1 double expression compared to 8.9% (4/45) in patients with BRAF V600E mutation and PD-L1 double negative [hazard ratio (HR) =1.267; 95% CI: 0.841–1.909; P=0.257]. Survival curves showed flatter recurrence-free survival (RFS) curves in positive BRAF V600E mutation only and PD-L1 expression only, whereas decreased sharply in positive expression of both BRAF V600E mutation and PD-L1; however, the differences were not significant (P>0.05). Conclusions The combination of BRAF V600E mutation and PD-L1 to identify group at higher risk of recurrence in early PTC has insufficient clinical evidence and should be used with caution in the clinical management of PTC.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
Arabian Journal of Chemistry
·
2023
·
IF 6
Yongyong Shi,Donghai Jiang,Liming Zhou,Jingyun Zhao,Jun Ma,Qian Lin,Hongyan Pan
Directly synthesizing H 2 O 2 from H 2 and O 2 at atmospheric pressure requires a highly efficient Pd catalyst, which poses a challenge for reasonable design and simple synthesis of Pd catalyst. In this study, a series of Pd/NPCS catalysts were synthesized by various methods with mono-disperse, uniform-size and N-doped porous carbon sphere named NPCS as the support and PdCl 2 as the palladium precursor. The results indicated that the ultrasonic-assisted-microwave quick synthesis method significantly reduced the synthesis time of Pd catalyst. The Pd nanoparticles obtained via this method were well-distributed on the NPCS support, with a smaller particle size, a narrower particle size distribution range, and more exposed Pd active sites, which leading to improved H 2 O 2 generation rate compared to traditional preparation methods. Additionally, N-doped, high specific surface area, and abundant mixed micro-mesoporous pore structure of NPCS support improved the transfer and diffusion performance of Pd/NPCS catalysts, facilitating the adsorption of reactants and desorption of H 2 O 2 from Pd active sites, and effectively inhibited hydrogenation and decomposition side reactions caused by the breaking of the O-O bond. The ultrasonic-assisted-microwave quick synthesis method and excellent NPCS support synergistically improved the catalytic activity and stability of Pd/NPCS catalyst. These findings provide insight into the design and preparation of efficient Pd catalysts for directly synthesizing H 2 O 2 at atmospheric pressure.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）