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.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2017
·
IF 4.233
Wenhao Dong,Yipeng Ren,Zhixue Bai,Jun Jiao,Yuan Chen,Bingkai Han,Qiang Chen
An innovative epinephrine sensor was fabricated by integrating tetrahexahedral (THH) Au-Pd core–shell nanocrystals on reduced graphene oxide (rGO) nanosheets . Furthermore, the nanocomposites combined the large specific areas of rGO with the high-index facets and excellent electrocatalytic activity of the THH Au-Pd nanocrystals, and the nanocomposites were an essential adapter for detecting epinephrine. In the present work, transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FTIR) and X-ray diffraction (XRD) were used to identify and characterize these unique nanocomposites, and the results revealed that a unique THH Au-Pd/rGO core–shell nanostructure was synthesized successfully. To further explore the electrochemical behaviors of these nanomaterials at a GC electrode, we applied cyclic voltammetry (CV), differential pulse voltammetry (DPV) and amperometry to study the conductivity and electrocatalytic activity of the proposed sensor, and the results suggested that the sensor based on Au-Pd/rGO presented a lower limit of detection (0.0012 μM at a signal to noise ratio of 3), wide linear detection range (0.001 µM to 1000 µM), and extraordinary selectivity and reproducibility. Moreover, the data showed that the sensor possessed good stability and acceptable accuracy to detect epinephrine in human serum samples. In summary, this work is not only a potential way to manufacture various nonenzymatic sensors but also a significant contribution to further studies in catalysis, cell fuel cells and other relevant applications.
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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 .
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Applied Catalysis O: Open
·
2024
·
IF 0
Zhe Zhang,Weiting Xiao,Yufei He,Dianqing Li,Xiaodong Zhao
During the manufacture of Al 2 O 3 , sulfate would be inevitably introduced when aluminum sulfate is used as raw material, but its effect has received little attention. In this work, Al 2 O 3 supports with different sulfate content were synthesized and used to prepare Pd/Al 2 O 3 catalyst. Sulfates in all samples exist as surface sulfate, and would be partially removed during the preparation process. Sulfate existing in Al 2 O 3 supports had little impact on the electric structure of Pd, but would partially block pores and also consume surface hydroxyl groups. As a result, higher sulfate content in support would lead to lower Pd dispersion in catalysts and slower reaction rate towards the hydrogenation of amyl-anthraquinone.
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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.
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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.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2020
·Vol. 22
·期 11
·6222-6230
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IF 3.43
Xiao Yan,Yafei Luo,Wei Liu,Li Liang,Ya Gan,Zhongzhu Chen,Zhigang Xu,Hua Wan,Dianyong Tang,Hubing Shi,Jianping Hu
Unveiling the reaction mechanism is significant for developing high-performance catalysts. In this paper, a series of precisely controlled PdxM147−x (M = Cu, Pt, Au, Rh, Ru) dendrimer encapsulated nanoparticles (DENs) has been successfully synthesized. The mechanisms of PdxM147−x as catalysts for Suzuki cross-coupling reactions were investigated by combining experimental and theoretical methods. The experimental results indicate that Pd74Cu73 DEN shows similar activity to Pd147 DEN and excellent substrate adaptability under mild reaction conditions. Moreover, the Cu component can play an important role in tuning the catalytic activity of PdxCu147−x DEN. Density functional theory (DFT) calculations illustrate that the similar activities of the Pd147 and Pd74Cu73 DENs originate from the comparable energy barriers of the rate-determining steps. The partial density of states (PDOS) and electron density differences demonstrate that Cu decreases the intensities of the valence orbitals of the top and edge Pd atoms and weakens orbital interactions between the intermediates and Pd74Cu73 DEN, leading to low desorption energies of the products. This work can provide a promising strategy to reduce the cost of Pd catalysts in Suzuki cross-coupling reactions.
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PubMed
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2024
·
IF 3.7
Junbo Feng,Junyan Wu,Dongdong Yan,Yadong Zhang
Porous silica nano-flowers (KCC-1) immobilized Pt-Pd alloy NPs (Pt-Pd/KCC-1) with different mass ratios of Pd and Pt were successfully prepared by a facile in situ one-step reduction, using hydrazinium hydroxide as a reducing agent. The as-synthesized silica nanospheres possess radial fibers with a distance of 15nm, exhibiting a high specific surface area (443.56 m 2 ·g –1 ). Meanwhile, the obtained Pt-Pd alloy NPs are uniformly dispersed on the silica surface with a metallic particle size of 4–6 nm, which exist as metallic Pd and Pt on the surface of monodisperse KCC-1, showing the transfer of electrons from Pd to Pt. The as-synthesized 2.5%Pt-2.5%Pd/KCC-1 exhibited excellent catalytic activity and stability for the continuous dehydrogenation of 2-methoxycyclohexanol to prepare guaiacol. Compared with Pt or Pd single metal supported catalysts, the obtained 2.5%Pt-2.5%Pd/KCC-1 shows 97.2% conversion rate of 2-methoxycyclohexanol and 76.8% selectivity for guaiacol, which attributed to the significant synergistic effect of bimetallic Pt-Pd alloy NPs. Furthermore, turn over frequency value of the obtained 2.5%Pt-2.5%Pd/KCC-1 NPs achieved 4.36 s –1 , showing higher catalytic efficiency than other two monometallic catalysts. Reaction pathways of dehydro-aromatization of 2-methoxycyclohexanol over the obtained catalyst are proposed. Consequently, the obtained 2.5%Pt-2.5%Pd/KCC-1 NPs prove their potential in the dehydrogenation of 2-methoxycyclohexanol, while the kinetics and mechanistic study of the dehydrogenation reaction over the catalyst in a continuous fixed-bed reactor may provide valuable information for the development of green, outstanding and powerful synthetic pathway of guaiacol.
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Catalysts
·
2025
·Vol. 15
·期 5
·442
·
IF 4
Zhe Wang,Xiaoliang Li
A series of Pd/g-C3N4catalysts were synthesized using different graphitic carbon nitride precursors, and were found to exhibit significant variations in catalytic performance for solvent-free selective catalytic oxidation of benzyl alcohol. Through comprehensive characterization (XRD, N2-BET, ICP-AES, TEM, and XPS), the experimental results found that the nitrogen chemical configuration and surface Pd2+concentration critically determined the catalytic efficiency. Among the various nitrogen species, N-(C)3-type nitrogen demonstrated the strongest influence on catalytic activity, which was positively correlated with its abundance in g-C3N4matrices. In particular, g-C3N4derived from dicyandiamide contained the highest N-(C)3type nitrogen content. When serving as Pd nanoparticle support, this material simultaneously achieved the best Pd2+surface concentration and catalytic performance compared to the other g-C3N4-supported catalysts.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Dali Wu,Yile Shi,Xiang Liu,Chenggong Zhang,Min Hua,Xuhai Pan
In the study of WO 3 -based gasochromic materials, the color-change rate and contrast are key indicators for evaluating sensor performance, while long-term stability is equally critical, as it directly determines the service life and reliability of the material in practical applications. In this work, h-WO 3 /m-WO 3 gasochromic materials with a hexagonal–monoclinic mixed-phase structure were successfully synthesized by regulating the annealing temperature. Pd nanoparticles were introduced as essential catalysts to enable room-temperature hydrogen-induced coloration of WO 3 . The Pd–WO 3 –400 sample exhibits excellent response to 1 % hydrogen at room temperature, with a rapid response time of only 13 s and a maximum total color difference (ΔE) of 8.1. Moreover, after one year of cyclic testing, this sample shows the slowest performance degradation, demonstrating outstanding long-term stability. In the mixed-phase structure, the open ionic diffusion channels of the hexagonal phase synergize with the structural stability of the monoclinic phase, while phase interfaces further enhance electron and hydrogen-ion transport. These combined effects significantly improve the gasochromic response. This study provides a strategy for designing gasochromic materials that balance high sensitivity and long-term stability, supporting the practical application of visual hydrogen-leak detection.
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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.
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PubMed
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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.
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PubMed
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