Catalysts
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2025
·Vol. 15
·期 6
·544
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IF 4
Tingting Hu,Baozeng Ren,Liang Zhao
Hydrogen peroxide (H2O2) is an important industrial chemical that is widely applied in many areas. The direct synthesis of H2O2from H2and O2has proved to be a green and economic pathway. Pd-based bimetallic catalysts, due to their superior catalytic performances in this reaction, have attracted intensive attention. Herein, Tetrakis(hydroxymethyl)phosphonium chloride (THPC) was adopted as the protective ligand to immobilize Pd-Au alloy nanoparticles onto activated carbon (AC). The varied Pd/Au molar ratios demonstrated homogeneously distributed Pd-Au nanoalloys with average particle sizes ranging from 3.51 to 5.75 nm. The optimal ratio was observed over the Pd3Au1/AC-THPC catalyst with a maximum H2O2productivity of 165 mol/(kgPd·h) and selectivity of 82.3% under ambient pressure. The relationship between the electronic structure and catalytic activity indicated Pd0was the active site, while the presence of Au inhibited H2O2degradation rate. This research could help in the design efficient bimetallic catalysts for the direct synthesis of H2O2.
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高影响因子
APPLIED CATALYSIS A-GENERAL
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2016
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IF 4.012
Hui Wang,Wei Yang,Penghui Tian,Jie Zhou,Rui Tang,Shengji Wu
Catalytic combustion has been identified as one of the most efficient and economically feasible routes for removing volatile organic compounds. In this work, supported noble-metal (Pd and Pt) catalysts for catalytic combustion of toluene were prepared by an improved incipient wetness impregnation method. Controlled amounts of oleic acid (OA) were introduced into the aqueous solution of metal salts in this new preparation method, which improved Pd and Pt dispersion remarkably on SiO 2 , as confirmed by XRD and TEM. XPS results showed that introduction of OA in the catalyst preparation resulted in increased proportion of metallic palladium. All of the activities in catalysts with OA were much higher than those of the catalysts without OA in the same catalyst system. Among the catalysts prepared, the 0.25%Pd-0.25%Pt/SiO 2 –OA catalyst exhibited the best catalytic activity for toluene oxidation, and the T 98 of toluene was only 160 °C under the conditions of toluene concentration at 1000 ppm and SV at 60,000 mL/(g h). Furthermore, the 0.25%Pd-0.25%Pt/SiO 2 –OA catalyst maintained high catalytic activity in the active stability test at 160 °C, and the result of TG indicated that no coke was formed on the spent catalyst.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2016
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IF 2.653
Man Qiao,Junze Jiang,Jidong Yang,Shaopu Liu,Zhongfang Liu,Xiaoli Hu
Based on l -tryptophan-Pd(II) system, a sensitive and selective fluorimetric assay for the quantification of ceftriaxone (CTRX) had been developed. The experimental results showed that in pH 4.0 Britton–Robinson (BR) buffer medium, the fluorescence of l -tryptophan ( l -Trp) ( λ ex / λ em = 276 nm/352 nm) could be efficiently quenched by Pd(II). When CTRX was added to the mixed solution of the l -tryptophan and Pd(II), the fluorescence of l -Trp recovered. The reaction mechanism and the reasons for the fluorescence recovery were also discussed. Pd(II) reacted with l -Trp to form a 1:1 chelate complex, and then, after CTRX was added in l -Try-Pd(II) system, the ligand exchange reaction occurred between l -Trp and CTRX, which resulted in the fluorescence recovery. Under the optimized experimental conditions, the recovered fluorescence intensities at 352 nm showed excellent linear relationship with the concentration of CTRX over the range of 6.0 × 10 − 8 –2.4 × 10 − 6 mol L − 1 (0.040–1.59 μg mL − 1 ). The correlation coefficient (R) was 0.9997 and the detection limit was 1.8 × 10 − 8 mol L − 1 (11.9 ng mL − 1 ). Furthermore, the assay had been applied to determine trace amount of CTRX human urine samples with satisfactory results.
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ELECTROCHIMICA ACTA
·
2026
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IF 5.8
Xiaoyan Ma,Qixian Xu,Kejin Zhou,Hailong Xu,Kunming Wei,Su Jiang,Jing Deng,Qingsong Li,Xueyan Li,Stefanos Giannakis
Haloacetic acids (HAAs), which are characterized by their persistence in tap water, are major contributors to the carcinogenic risk posed by disinfection byproducts (DBPs). This study introduces a Pd/Cu x O porous carbon composite electrode, synthesized via a metal-doping modulation strategy and immobilized on a steel electrode for the electrocatalytic dechlorination of trichloroacetic acid (TCAA). The Pd/Cu x O/St electrode demonstrated outstanding dechlorination efficiency, achieving up to 95.2% TCAA removal, surpassing that of other experimental transition metals. Material characterization confirmed the successful formation of a Pd-Cu x O heterostructure on the Pd/Cu x O/St composite electrode. Electrochemical analysis revealed that the optimized Pd/Cu x O/St system displayed a significantly higher current density and enhanced reaction kinetics than their undoped counterparts. The optimal mass ratio of Pd/Cu x O for doping was determined to be 0.075:1, achieving TCAA removal efficiency of 95.2%. Our Pd/Cu x O/St electrode combined rapid kinetics, dual-pathway mechanisms, and metal-doping synergy to efficiently convert the persistent and toxic DBPs into harmless products. Quenching experiments with tert-butanol and EDTA-2Na identified atomic hydrogen (H*), Cu, and Pd ions as the dominant active species, leading to the conversion of TCAA to less toxic acetic acid. This work not only advances TCAA dechlorination technology but also provides vital insights for developing effective end-of-pipe treatments for DBPs, a significant step towards safer drinking water.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Xuehan Gao,Weifeng Zhi,Dongmei Huang,Wenyu Pan,Xinhang Ma,Liyi Pan,Zequan Li,Shuangliang Zhao
Hydrogenated nitrile butadiene rubber (HNBR) is a crucial material for high-performance sealing applications; however, conventional solution hydrogenation is often limited by high noble-metal consumption and the challenges in simultaneously achieving high activity, selectivity and stability. Herein, a synergistic design strategy integrating mass transfer enhancement, bimetallic electronic synergy, and support interface stabilization is proposed for efficient NBR hydrogenation. A Pd-Ni bimetallic-doped TiO 2 -Al 2 O 3 porous composite catalyst was synthesized through a sol–gel method, in which the pore size distribution was tuned to 15–18 nm by using an F127 template to facilitate macromolecular diffusion. Partial substitution of Pd with Ni modulates the electronic structure of Pd sites, promoting H 2 dissociation and selective C=C bond hydrogenation, while the TiO 2 -Al 2 O 3 composite support provides Lewis acid–base sites and oxygen vacancies that enhance metal dispersion and catalyst stability. The optimized Pd–1Ni catalyst achieves a hydrogenation degree of 92% at 120 °C and 4 MPa, and retains over 80% of its activity after five consecutive cycles. This work demonstrates an effective strategy for balancing catalytic activity, noble-metal utilization, and operational stability in heterogeneous NBR hydrogenation systems, providing a practical reference for catalyst design in polymer hydrogenation processes.
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SENSORS AND ACTUATORS B-CHEMICAL
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2014
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IF 3.84
Shan-Shan Li,Yuan-Yuan Hu,Ai-Jun Wang,Xuexiang Weng,Jian-Rong Chen,Jiu-Ju Feng
In this work, we developed a simple wet-chemical method for fabrication of worm-like Au–Pd nanostructures uniformly supported on reduced graphene oxide (Au–Pd/rGO), only with the assistance of polyethylene glycol monooleyl ether (Brij-35) as a growth-directing agent, a stabilizing agent, and a mild reducing agent. The as-prepared nanocomposites showed improved analytical performance for nitrite detection, which was further explored to construct a nitrite sensor with fast response, wide linear range from 0.05 to 1000.0 μM, low detection limit of 0.02 μM ( S / N = 3), good reproducibility, and long-term stability.
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CHEMOSPHERE
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2019
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IF 5.108
Yuan Chen,Keqiang Hu,Yuancai Chen
In this study, we screened a new aerobic bacterium ( Bacillus megaterium Y-4) that can efficiently reduce Pd(II) with different electron donors. The best electron donor was sodium formate and the best reduction of Pd(II) were by log growth phase cells. The high removal capacity of Pd(II) (1658.3 mg/g) was obtained with 30 mg/L dry cell weight and 50 mg/L Pd (II) in the presence of 5 mM sodium formate. The removal amount of Pd(II) increased with initial Pd(II) concentrations ranging from 50 to 200 mg/L with 100 mg/L Pd(II) being completely removed by 148 mg/L dry cell weight in 6 h. The cell wall, periplasmic space and intracellular contents of B . megaterium Y-4 contains different kinds of enzymes for reducing Pd(II). In addition, the activity of extracellular and periplasmic enzymes was more sensitive to temperature than intracellular enzymes . XRD and XPS analysis revealed that the enzyme for reducing Pd(II) in B. megaterium Y-4 can tolerate a broad range of temperatures (20–60 °C) and pH (2.0–7.0) but was sensitive to oxygen. TEM analysis showed that biogenic palladium nanoparticles (Pd-NPs) were mainly distributed evenly in the periplasmic space of the live cells and were released from cells into aqueous solution, which reduced the toxicity of Pd(II), allowing Pd-NP recovery without cell destruction. B. megaterium Y-4 is a potential bacterium for efficient treatment and reclamation of Pd(II) pollution and formation of Pd-NPs.
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Desalination and Water Treatment
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2024
·
IF 1
Qiuxiang Liu,Jinhui Fang,Sulin Ni,Shasha Tang,Zhiqiao He
A hybrid electrode comprised of Pd and Co 3 O 4 supported on Ni foam (Pd-Co 3 O 4 /Ni foam) was applied toward the dechlorination of 2,4-dichlorophenoxyacetic acid (2,4-D). The effects of the reaction condition, such as Co 3 O 4 and Pd loading, current density, initial concentration of 2,4-D, temperature and dissolved anions, on the electrochemical dechlorination process were investigated and interpreted based on an indirect reduction mechanism via active atomic H*. The optimal Pd and Co 3 O 4 loading were determined to be 0.47 and 0.51 mg/cm 2 , respectively. A highest current efficiency of 12.10% was obtained at a current density of 1.50 mA/cm 2 , an initial 2,4-D concentration of 50 mg/L and reaction temperature of 298 K, and the apparent activation energy of 2,4-D dechlorination by the Pd-Co 3 O 4 /Ni foam electrode was calculated to be 42.33 × 10 3 J/mol. In addition, dissolved anions such as S 2- , SO 3 2- and NO 3 - suppress the catalytic activity, whereas HCO 3 - and Cl - have a negligible effect on the reaction process. The Pd-Co 3 O 4 /Ni foam electrode can also be applied to the dechlorination of 2,4-D in natural water bodies as well as other chlorinated organic compounds, such as chlorophenols.
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CHEMICAL ENGINEERING JOURNAL
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2013
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IF 3.473
Bo Yang,Yunfei Zhang,Shubo Deng,Gang Yu,Yonghong Lu,Jinhua Wu,Jianzhong Xiao,Gang Chen,Xiaobing Cheng,Lili Shi
The Pd/Al nanoparticles (NPs) prepared by aqueous cementation were employed to probe hydrodechlorination (HDC) efficiencies of 4-chlorophenol (4-CP) in aqueous solution and 2-chlorobiphenyl (2-PCB) in surfactant solution. Major factors affecting HDC performance were investigated including acidic types, pH conditions, and surfactant types and their concentrations. Among HCl, H 2 SO 4 , H 3 PO 4 , formic acid, and acetic acid, only HCl was the proper pH adjustor to initiate HDC reaction of 4-CP with Pd/Al NPs at pH 3.0 due to the particular penetration function of active Cl − on the compact oxide film of Al. Aqueous pH states obviously influenced HDC efficiency and its values stable at pH 3–4 were the optimum range for HDC with HCl adjustor. 0.389 mM of 4-CP could be almost completely dechlorinated into phenol after 30-min reaction using 2 g/L of Pd/Al NPs with 1.2 wt.% of Pd loading. In addition, the effect of surfactants on HDC process of highly hydrophobic 2-PCB was explored, which were employed for its better solubilization. The addition of surfactants including SDS, CTAB, Tween 80, or Brij 30 had adverse effect on HDC activity of Pd/Al NPs due to their inhibiting effect on Al corrosion. The adverse effect was closely related with the concentrations of surfactants especially for each CMC level and molecular structures.
研究领域:
环境化学
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纳米修复
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水处理
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催化
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污染物降解
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高影响因子
International Journal of Nanomedicine
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2026
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IF 6.5
Zhiqiang Lin,Hui Jiang,Yingying Zhou,Li Xu,Lixin Jiang,Jing Du
Purpose Triple-negative breast cancer (TNBC) is prone to relapse and metastasis due to the immunosuppressive state of the tumor microenvironment and limited exposure to relevant antigens, and chemotherapy alone has poor efficacy. We have developed a novel theranostic nanoplatform to address these problems: multifunctional nanocapsules (NCs) with a PD-L1-mediated gold shell induce immunogenic cell death (ICD) to remodel the immune microenvironment. PD-L1 and NLG919 dual immune checkpoints are programmed to synergistically sensitize photothermal therapy and chemotherapy, and photoacoustic imaging (PAI) is used to visualize and localize TNBC tissues for identification.Methods DOX-NLG919@PLGA@Au-antiPD-L1 NCs (DNPA-aPD-L1 NCs) were prepared using an improved single emulsion water-in-oil (O/W) solvent evaporation method, electrostatic adsorption, gold seed surface-induced crystallization reduction method, and carbodiimide method. A series of animal models were established to focus on the in vivo PAI of NCs, the effects of photochemotherapy combined with immunotherapy and antitumor therapy, ICD induced by NCs, the metabolic distribution of NCs, and toxicity tests.Results This project successfully constructed gold nanoshell-PLGA core NCs with PD-L1 antibody co-loaded with chemotherapeutic drugs doxorubicin and indoleamine 2,3-dioxygenase inhibitor NLG919. Laser-triggered release of DOX, NLG919, and photothermal therapy can synergistically induce immunogenic cell death (ICD), thereby enhancing tumor immunogenicity, inhibiting IDO, and reshaping the tumor immune microenvironment. This can effectively eliminate the primary TNBC lesions, inhibit recurrence and metastasis, significantly prolong the survival of tumor-bearing mice, and NCs have good in vivo biosafety. This diagnostic and therapeutic agent can be used for photochemotherapy, immunotherapy, and PAI to visualize and identify TNBC.Conclusion The photochemotherapy mediated by the DNPA-aPD-L1 NCs we developed, combined with tumor microenvironment remodeling and immune activation, shows great promise for the diagnosis and treatment of TNBC.
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Science China-Chemistry
·
2026
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IF 9.7
Zheng Xia,Fu Yaoqiang,Ning Jing,Wang Haorui,Liu Hongfei,Cui Chunhua
Direct formate fuel cells (DFFCs) are becoming one of the most promising next-generation energy devices owing to their high energy density, low toxicity, and carbon neutrality. However, their practical application is hindered by the sluggish kinetics of the formate oxidation reaction (FOR) on conventional palladium (Pd)-based catalysts due to the strong adsorption of hydrogen intermediates (H ads ) that block the active sites. Herein, we tackled the above problem by tailoring the Pd electrocatalytic properties through the interfacial interaction with the hydroxyl group-abundant and oxophilic Co(OH) 2 substrate. This resulted in an impressive mass activity of 5.02 A mg
−1 Pd
for the synthesized Pd/Co(OH) 2 , approximately three times that of commercial Pd/C. Moreover, under high formate concentration, Pd/Co(OH) 2 exhibits significantly improved stability, i.e. , up to 24000 s sustainable current density with 100% selectivity toward CO 2 (CO 2 is actually converted to carbonate in alkaline media). Kinetic isotope effect (KIE) analysis and in situ Raman spectroscopy based mechanistic study reveal the excellent FOR performance of Pd/Co(OH) 2 originates from the partially oxidized Pd facilitated H ads oxidative removal and the more hydrophilic surface induced competitive HCOO − adsorption over H ads . This study demonstrates a rational strategy to optimize the Pd-based FOR electrocatalysts through the electronic and interfacial interactions with appropriate substrate to modulate the key intermediate adsorption-reaction kinetics.
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Nature Communications
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2026
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IF 18.1
Ren Lijuan,Hu Xiuli,Wang Shuyu,Shi Jiaqi,Gong Jiaxing,Wang Manyun,Zhou Ji,Wang Jianzu,Lv Xian-Wei,Bielawski Christopher W.,Geng Jianxin
Zinc−air batteries are promising devices for use in safe and cost-effective energy storage applications. However, their practical utility is hindered by sluggish oxygen evolution and oxygen reduction reactions. We show that hybridizing electronically coupled Co single atoms and a CoPd alloy within a three-dimensional macroporous N-doped carbon (CoPd/Co@3D NC) enables high-performance N 2 H 4 -assisted zinc−air batteries, where the oxygen evolution reaction is replaced with the thermodynamically more favorable hydrazine oxidation reaction. Experimental and theoretical data reveal that electronic coupling between the Co single atoms and the CoPd alloy mutually modifies their electronic structures, which, in turn, weakens oxygen adsorption on the Co single atoms and enhances N 2 H 4 adsorption on the Pd sites. The electronic-coupling effect accelerates the rate-limiting steps of the oxygen evolution and hydrazine oxidation reactions. Consequently, N 2 H 4 -assisted zinc−air batteries employing CoPd/Co@3D NC exhibit a small charging/discharging voltage gap of 0.52 V at 100 mA cm −2 , a peak specific power of 151 mW cm −2 , and a specific capacity of 810 mAh g −1 at 10 mA cm −2 ; these values are competitive when compared to those exhibited by conventional zinc−air batteries.
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