Nano Research
·
2024
·
IF 9.5
Liu Weiruo,Zhu Yanbin,Wang Jiwei,Feng Haisong,Zhai Yunpu,Li Wei,Zhao Dongyuan
Highly dispersed Pd/N-doped carbon dots (Pd/NCDs) were successfully immobilized in the mesoporous channels of amino-functionalized dendritic mesoporous silica nanospheres (NMS). The synthesized Pd/NCDs@NMS catalyst exhibits outstanding performance in the catalytic reduction of 4-nitrophenol (4-NP), achieving a turnover frequency of 1461.8 mol·mol Pd −1 ·h −1 , with the conversion rate remaining above 80% after 11 cycles. Experiments and density functional theory calculations reveal that the NCDs significantly affect the electronic structure of Pd nanoparticles, leading to changes in the energy barriers for the adsorption of 4-NP at the Pd sites and the conversion of 4-NP reaction intermediates, which is a key factor contributing to the catalytic performance. This study offers a new strategy for synthesizing carbon-dot-modified metal-based catalysts.
✓ 已验证
产品关联
DOI
高影响因子
VACUUM
·
2025
·
IF 3.9
Xiaohua Wang,Yanwei Li,Xinhui Jin,Guang Sun,Jianliang Cao,Yan Wang
The pressing need for health and environmental protection has sparked significant interest among researchers in exploring gas sensors made from metal oxide semiconductors (MOSs). Herein, a co-modification approach involving palladium (Pd) and palladium oxide (PdO) is introduced to enhance the sensing properties of indium oxide (In 2 O 3 ) to hydrogen sulfide (H 2 S). Pd and PdO co-modified In 2 O 3 hierarchical porous nanocubes (Pd/PdO-In 2 O 3 HPNCs) were synthesized using a facile hydrothermal method. With the theoretical doping amount of 2 mol%, the synergistic effect of metal Pd and PdO-In 2 O 3 heterojunction made Pd/PdO-In 2 O 3 show excellent sensing performance to H 2 S compared to In 2 O 3 . Specifically, the material features a lower operating temperature (280 vs 300 °C), higher sensitivity (95.06 vs 28.59 to 20 ppm H 2 S; 2.28 vs 1.17–100 ppb H 2 S), and better selectivity (7.41 vs 2.32 times to triethylamine), while also demonstrating satisfactory reproducibility and stability. The synergistic sensitization mechanism of noble metal catalysis and heterojunction in Pd/PdO–In 2 O 3 HPNCs, along with their underlying mechanism, was discussed. Integrating noble metal modification with heterojunctions adds complexity to the structure and composition of the material. The synergistic effects of these two sensitization strategies on the H 2 S sensitization mechanism need further in-depth investigation.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Fangxu Shi,Fuxin Liang,Yulin Wei,Junyan Wu,Sai Huang,Honglei Wang,Zhi Wang,Guopu Shi
The hydrogenation-catalyzed synthesis of mirabellone, a drug for the treatment of overactive bladder (OAB), faces the challenge of catalytic efficiency and selectivity regulation of its core intermediate. In this study, we propose an innovative strategy for constructing a Pd/B-Al 2 O 3 composite catalytic system on a foam ceramic substrate using the impregnation method, and systematically investigate the modulation mechanism of different boron doping ratios on the catalyst's performance. Experimental and density functional theory studies demonstrate that the incorporation of boron synergistically enhances surface adsorption of reaction intermediates, facilitates the efficient reduction of PdO, and precisely modulates the distribution of acidic sites, thereby establishing a catalytic environment more favorable for the selective reduction of nitro groups. This catalyst, characterized by its unique three-dimensional pore structure and the interface synergistic effect resulting from boron modification, enables a uniform distribution of catalytically active centers and enhances the efficiency of reaction mass transfer. Through the optimization of process parameters, the yield of the target product was significantly improved, providing an innovative technological path for the preparation of the key intermediate of mirabilon.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Zhiliang Ma,Chao Xie,YueZhou Wei,Xiangbiao Yin,Caiwu Luo,Shunyan Ning,Qiang Wu,Tianjiao Jiang
The efficient separation and recovery of palladium (Pd) from high-level liquid waste (HLLW) are critical for promoting resource sustainability and advancing the nuclear fuel cycle. In this study, a novel silica-based sorbent (HT-paPBI@SiO 2 ) enriched with nitrogen adsorption sites was synthesized via a polymerization–vacuum impregnation–high-temperature optimization strategy to address the challenges of Pd(II) recovery in highly acidic and ionically complex environments. HT‑paPBI@SiO 2 was systematically characterized using SEM, EDS, TG‑DSC, BET, and FT‑IR analyses, which confirmed its rigid framework, abundant porosity, high loading efficiency, and excellent thermal stability. Static batch adsorption experiments demonstrated that HT‑paPBI@SiO 2 efficiently adsorbs Pd(II) over a broad acidity range (0.1–9 M HNO 3 ). In simulated HLLW at 6 M HNO 3 , the material exhibited outstanding selectivity ( SF Pd/other metal ions > 1.05 × 10 3 ) and a high saturation adsorption capacity of 128.2 ± 1.8 mg/g. Furthermore, the adsorption kinetics fit well with a pseudo‑second‑order model, while the equilibrium data conform to the Langmuir isotherm and van’t Hoff thermodynamic models, indicating a spontaneous, endothermic, monolayer chemical adsorption process. Furthermore, dynamic adsorption experiments successfully achieved the selective recovery of Pd(II) from simulated HLLW, highlighting the potential of HT-paPBI@SiO 2 for industrial-scale applications. Mechanistic investigations, supported by FT-IR, XPS, and DFT calculations, revealed that the benzene ring in paPBI was oxidized to a quinone structure under high-temperature treatment. The electron-rich regions resulting from the interaction of the C=O group in quinone with the C=N − C moiety in imidazole enhance the affinity for Pd(II). This interaction facilitates the coordination of nitrogen and oxygen atoms with Pd(II), while NO 3 − ions coordinate to balance the charge.
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES B-BIOINTERFACES
·
2025
·
IF 5.6
Feng Lin,Hong Huang,Jie Long,Renchuan Liang,Yunxi Huang,Xiaoling Luo
Cancer remains a major global health burden due to its high rates of recurrence and resistance to conventional therapies. Although PD-L1/PD-1 immune checkpoint inhibitors (ICIs) have emerged as promising treatments by restoring T cell function and enhancing anti-tumor immunity, their efficacy is often limited by immunosuppressive tumor microenvironment (ITM) and metabolic adaptations that impair T cell activity. To address these challenges, we developed a novel intelligent drug delivery platform that integrates PANoptosis induction, metabolic modulation and targeted nanotherapy. Specifically, hollow mesoporous manganese dioxide (H-MnO 2 ) nanoshells were synthesized and co-loaded with SOAT1 inhibitor avasimibe (Ava). Trop2-specific targeting ligands were further conjugated to enable precise tumor localization, resulting in the multifunctional nanoplatform Ava@HM/Trop2. Upon tumor accumulation via Trop2-mediated targeting, acidic pH conditions and TME stimuli trigger rapid degradation of the H-MnO 2 nanoshells, releasing Ava and inducing PANoptosis. This process activates the cGAS-STING pathway, remodels immunosuppressive TME, mitigates lipid-induced T cell senescence, and synergizes with PD-1 blockade to potentiate anti-tumor immunity. Both in vitro and in vivo experiments demonstrate that Ava@HM/Trop2 achieves efficient tumor targeting, robust tumor cell apoptosis, and improved therapeutic outcomes. This innovative multi-modal strategy highlights a promising avenue for overcoming immunotherapy resistance and advancing the clinical management of solid tumors.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CANCER LETTERS
·
2021
·
IF 8.679
Ya-Nan Tan,Yong-Peng Li,Jian-Dong Huang,Min Luo,Shan-Shan Li,Anne Wing-Mui Lee,Fu-Qiang Hu,Xin-Yuan Guan
The response rate of anti-PD therapy in most cancer patients remains low. Therapeutic drug and tumor-infiltrating lymphocytes (TILs) are usually obstructed by the stromal region within tumor microenvironment (TME) rather than distributed around tumor cells, thus unable to induce the immune response of cytotoxic T cells. Here, we constructed the cationic thermosensitive lipid nanoparticles IR780/DPPC/BMS by introducing cationic NIR photosensitizer IR-780 iodide (IR780) modified lipid components, thermosensitive lipid DPPC and PD-1/PD-L1 inhibitor BMS202 (BMS). Upon laser irradiation, IR780/DPPC/BMS penetrated into deep tumor, and reduced cancer-associated fibroblasts (CAFs) around tumor cells to remodel the spatial distribution of TILs in TME. Interestingly, the cationic IR780/DPPC/BMS could capture released tumor-associated antigens (TAAs), thereby enhancing the antigen-presenting ability of DCs to activate cytotoxic T lymphocytes. Moreover, IR780/DPPC/BMS initiated gel-liquid crystal phase transition under laser irradiation, accelerating the disintegration of lipid bilayer structure and leading to the responsive release of BMS, which would reverse the tumor immunosuppression state by blocking PD-1/PD-L1 pathway for a long term. This combination treatment can synergistically exert the antitumor immune response and inhibit the tumor growth and metastasis.
✓ 已验证
DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Xin-Hao Shen,Feng Liu,Qin-Qin Chen,Ying Gao,Xiao-Wen Wang,Xin Liu
The efficient degradation of emerging pollutants in water, represented by CBZ, is receiving increasing attention from all sectors of society. Although advanced oxidation reactions represented by Fenton reaction can efficiently degrade emerging pollutants, the problem of iron sludge that comes with it is hindering the further promotion of this technology. Herein, UiO-66(Zr)-2OH material was synthesized by hydrothermal method and loaded with Pd 0 NPs on the surface of the material by in situ reduction. The MOFs-H 2 -Accelerated Catalytic Fenton system was constructed by accelerating the regeneration of Fe(II) in the system by activating the [H] produced by H 2 introduced into the system at room temperature and pressure. Within 180 min, the removal of the target pollutant CZB could reach more than 99 % under the condition of only 25 µmol of Fe(II) and 25 mmol of H 2 O 2 .
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Jiamin Shi,He Wang,Han Wang,Qun Yan,Athanasia Tekerlekopoulou,Dimitris V. Vayenas,Bin Huang
Nitrate pollution threatens ecological environment and human health. Electrochemical reduction of nitrate to ammonia using metal-doped modified cathode is a promising technique for nitrate removal. In this work, a bimetallic Ru/Pd-doped Cu foam (CF) electrode was developed for nitrate reduction using cation exchange method. Confirmed by various physio-chemical characterization, it was found that the Ru/Pd-Cu Spongy Copper Foam (SCF) was successfully prepared. In addition, nearly 100 % nitrate removal, 94.07 % NH 3 selectivity, and 84.9 % Faradaic efficiency (FE) could be achieved, under the optimized conditions as 100 mg L −1 of initial NO 3 - -N concentration, 0.3 mol L −1 of Na 2 SO 4 as electrolyte and the applied current of 5.42 mA cm −2 . Through electrochemical testing and DFT calculation, it was revealed that the bimetallic doping of Ru/Pd facilitate electrocatalytic nitrate reduction reaction (NO 3 RR) by reducing the energy barriers of the NO 3 - -to-NH 3 pathway from 0.81 to 0.56 eV. Besides, the electrode showed excellent stability and anti-toxicity even after 10 repeated NO 3 RR cycles, since the NH 3 yield rate and NH 3 selectivity ranged from 0.206 to 0.231 mg h −1 cm −2 , 87–96.87 % respectively. After NO 3 RR, an extended electrochemical oxidation process was implemented to remove ammonia, and nearly 100 % of NH 3 was oxidized to N 2 without byproducts. Thereby, this study provides a new option for the electrochemical reduction of nitrate to ammonia via cathode modification, to achieve the substantial nitrate removal from nitrate-containing water.
✓ 已验证
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Xiao-Chao Chen,Wen-Di Guo,Guo-Sheng Zhang,Long-Gen Hu,Yong Lu,Ye Liu
Pd-catalyzed hydroxycarbonylation of alkynes with CO and H 2 O is a promising alternative for one-step synthesis of α,β-unsaturated carboxylic acids advantageous with 100 % atom-economy, but suffering from rapid catalyst deactivation and unavoidable side reactions like polymerization and hydration while the auxiliary acid-additive is required as a co-catalyst. Herein, free of any auxiliary acid-additive and under mild conditions (0.5 MPa, 60 °C, 3 h), a flexible zwitterionic phosphine of L1 containing a mono-phosphino-fragment and a hydrophilic sulfonate group (–SO 3 - ) conferred to Pd(OAc) 2 catalyst efficient performance for hydroxycarbonylation of terminal alkynes, affording the branched α,β-unsaturated carboxylic acids in the yields of 85 ∼ 91 % with 100 % regioselectivity. In addition, the developed L1 -Pd(OAc) 2 system was so stable that it could be recycled for 30 runs with well-maintained activity and selectivity, which proved the most active and stable to date under acid-additive-free condition.
✓ 已验证
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Yinan Wang,Xuteng Zhao,Ting Chen,Zuwei Zheng,Rijing Zhan,He Lin
Pd/SSZ-13 with different Al distributions were hydrothermally synthesized and utilized as passive NOx adsorbers (PNA). The characterization results indicated that more concentrated Al distribution can not only improve the ion-exchanged level of Pd but also generated more Z 2 Pd 2+ sites at six-member rings. Thus, as revealed by NOx adsorption experiments, samples with more Z 2 Pd 2+ sites showed high NOx storage capacity as well as stronger water resistance. Besides, 84.8 % adsorption capacity of this sample was retained after hydrothermal aging treatment. On the other side, Pd existed as [Pd(OH)] + sites on SSZ-13 with isolated Al as the majority. These sites were vulnerable to H 2 O and less stable. Seriously Pd agglomerated was observed on the aged Pd/SSZ-13 with less paired Al. This study revealed that proper Al distribution on SSZ-13 could significantly improve the performance and stability of the catalyst and provided a new direction for the design of PNA catalysts.
✓ 已验证
DOI
高影响因子
ACS Catalysis
·
2019
·
IF 12.221
Xueping Qin,Lulu Zhang,Gui-Liang Xu,Shangqian Zhu,Qi Wang,Meng Gu,Xiaoyi Zhang,Chengjun Sun,Perla B. Balbuena,Khalil Amine,Minhua Shao
Improving the reaction kinetics of hydrogen evolution and oxidation reactions (HER/HOR) in alkaline media is critical to promote the development of alkaline fuel cells and electrolyzers. Here, we prepared Pd3Ru alloy nanocatalysts with Ru segregated on the surfaces, forming adatoms and clusters. This structure dramatically lowered the overpotential of Pd toward HER in 1 M KOH by 104 mV at 10 mA cm–2. The HER activity was even higher than that of Pt (6 mV improvement at 10 mA cm–2). Theoretical simulation results revealed that Ru adatoms/clusters on the surface could weaken the hydrogen-binding energy and promote the OH adsorption, consequently lowering the reaction barrier of the rate-determining step in HER. Our findings are of significance for clarifying the role of Ru in bimetallic catalysts and rational design of more active catalysts for HER/HOR.
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
He Jiang,Haoliang Wei,Xinkai Li,Yijun Zhang,Tingjiang Lu,Feili Li,Shuang Song,Yan Yu,Meilan Pan,Weiting Yu
The widespread discharge of halogenated organic pollutants (HOPs) in wastewater brings significant risks to the environment and human health due to potent high toxicity, antibacterial activity, and strong biodegradation resistance. Adsorbed atomic hydrogen (H* ads )-mediated electrocatalytic hydrodehalogenation (EHDH) has been recognized as an efficient strategy for HOPs removal through selectively breaking carbon-halogen bonds. In this work atomic Pd uniformly anchored on molybdenum disulfide (denoted as Pd-MoS 2 ) was synthesized through a facile hydrothermal method and found with state-of-the-art specific activity in florfenicol (FLO) removal via the H* ads -mediated EHDH process. Pd-MoS 2 completely dehalogenated (∼100 %) FLO within 30 min at a rate constant of 0.15 min −1 , which was 6.0, 6.5 and 33.1 times the value of MoS 2 , Pd/C and carbon paper samples, respectively. Notably, the toxicity of the wastewater was reduced to 1/6 of its original value after the treatment. Moreover, Pd-MoS 2 presented superior catalytic stability in five successive cycles. Furthermore, Pd-MoS 2 was also robust in complex water environment with practical applicability for industrial wastewater treatment. A dual-active-center mechanism with enhanced H* ads production capacity and the improved H* ads utilization efficiency was contributed to the increased EHDH activity on Pd-MoS 2 .
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）