JOURNAL OF CATALYSIS
·
2024
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IF 6.5
Mengyuan Zhang,Jian Ye,Nana Lu,Xiaoyan Lu,Kongliang Luo,Jiali Dong,Qiang Niu,Pengfei Zhang,Sheng Dai
CO 2 methanation at low temperatures is still a challenge. Herein, Ni n CeO x (n = 1–3) and Ni 2.5 Pd 0.1 CeO x nanofibers by electrospinning is reported. The main advantage of this method is to obtain the highly dispersed precursor of palladium, nickel, and cerium, overcoming the difficulty of uniform mixing in conventional preparation methods. The Ni 2.5 Pd 0.1 CeO x nanofiber catalyst exhibited outstanding catalytic performance at low temperatures (CO 2 conversion rate = 90.4 %, CH 4 selectivity = 99.6 % at 230 °C) along with exceptional stability over 300 h. EPR, Raman, and O 1s XPS confirmed that Pd 2+ doping increased oxygen vacancy concentration. In-situ infrared spectroscopy indicated that CO 2 methanation on Ni 2.5 CeO x and Ni 2.5 Pd 0.1 CeO x catalysts followed the formate pathways. Pd 2+ doping increased the number of surface oxygen vacancies and hydroxyl groups, thus increasing the amount of bicarbonates and formates. DFT calculations suggested that Pd 2+ doping increased CO 2 adsorption energy, and confirmed surface hydroxyl groups and bicarbonate being beneficial for CO 2 methanation, consequently enhancing the activity of Ni 2.5 Pd 0.1 CeO x catalyst especially at low temperatures.
研究领域:
材料科学
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催化化学
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Analytical Methods
·
2019
·Vol. 11
·期 47
·6053-6061
·
IF 2.378
Man Du,Yue Zhang,Yifeng Yu,Hua Zhao,Yue Guo,Yunxu Yang
A novel “off–on” fluorescent probe ACBT, using a readily available dye 2-(2′-aminophenyl) benzothiazole as the fluorophore, for the determination of Pd2+ was designed and synthesized in this work. Based on a palladium triggered cleavage reaction, the probe ACBT exhibited rapid response time (<2 min), and high selectivity and sensitivity towards Pd2+ in aqueous solution under mild conditions. The detection limit of probe ACBT towards Pd2+ was estimated to be as low as 2.6 nM. Furthermore, fabrication of probe ACBT test strips was achieved for a convenient visual detection of palladium. In addition, it also has been successfully applied to detect Pd2+ in environmental water samples with satisfactory results, indicating that the use of probe ACBT could be a potential and feasible method to detect Pd2+ in environmental systems.
研究领域:
化学
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环境科学
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高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2022
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IF 5.141
Hanqing Wu,Liangbin Lin,Lingyi Zheng,Hongyu Guo,Fafu Yang
Although the fluorescence sensors for Cu 2+ or Pd 2+ had been prepared, the sensor of in-situ detecting both Cu 2+ ion and Pd 2+ ion in aqueous media was rarely concerned. Herein, a bis-tetraphenylimidazole Schiff-base ( Bis-TPI ) with aggregation-induced emission was designed and prepared in yield of 88%. Bis-TPI displayed strong red fluorescence at 550–650 nm in aqueous media and selectively response on detecting Cu 2+ and Pd 2+ with quenched fluorescence. The detection limits attained 8.3 × 10 -7 M for Cu 2+ and 9.2 × 10 -7 M for Pd 2+ , respectively. The mutual interference on detecting Cu 2+ and Pd 2+ in their coexistence system was eliminated by the masking reagent of adenosine triphosphate for Cu 2+ , realizing the detection of Cu 2+ and Pd 2+ sequentially. The sensing mechanism of 1:1 binding system was supported by FT-IR spectra, binding MS spectra, 1 H NMR spectra and fluorescence Job’s plot. Moreover, Bis-TPI showed good fluorescence bioimaging property and achieved in-situ detection on Cu 2+ and Pd 2+ in living-cell system, implying the application prospect on in-situ sensing Cu 2+ and Pd 2+ in both vitro environment and vivo assay.
研究领域:
分析化学
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生物成像
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环境科学
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2017
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IF 7.504
Wenli Gao,Haohan Song,Xiao Wang,Xiaoqiang Liu,Xiaobin Pang,Yanmei Zhou,Bin Gao,Xiaojun Peng
Red emissive carbon dots (CDs) have drawn more and more attention due to their good organ penetration depth and slight biological tissue photodamage. Herein, the fluorescent CDs with red emission were synthesized by the facile one-pot hydrothermal treatment of citric acid and neutral red and they show red fluorescence both in aqueous solution and solid state. The solution of CDs exhibits the quantum yield of 12.1%, good stability against photobleaching, and low cytotoxicity. As-prepared CDs can be used as a fluorescent probe for peculiar detection of Pt2+, Au3+, and Pd2+. Furthermore, the CDs show excellent biocompatibility, which were successfully used as hopeful bioimaging and biosensing of noble metal ions in PC12 cells and zebrafish.
研究领域:
分析化学
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生物医学
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材料科学
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 18
·8785-8796
·
IF 3.3
Jiaxin Zhang,Xianlang Chen,Jinhua Yu,Zheng Fang,Lele Yan,Zijian Wang,Zhengyu Pan,Rongrong Li,Li Zhang
Catalytic hydrodechlorination (HDC) is considered as one of the most promising strategies for the treatment of chlorinated environmental pollutants. Here we proposed a strategy for rapid complete dechlorination by exploiting a B–N co-doped hierarchically porous carbon material (BNC) to immobilize Pd NPs, which makes use of not only the micro/meso porous structure to accelerate the mass transport and to provide enormous active sites, but also the synergistic effect for codoping of B–N to enhance the interaction between Pd NPs and support and thus to stabilize and disperse the small size of the Pd particle. Ascribed to these combined advantages, Pd/BNC exhibited more distinctive catalytic dehalogenation activity (k = −0.14 min−1) and better stability (about 90.0% activity retention after 5 cycles) than Pd/C (k = −0.0070 min−1). Additionally, density functional theory (DFT) calculation indicates that the incorporation of N and B atoms in the carbon skeleton will reduce the adsorption energy of Cl− and thus Pd/BNC exhibits more remarkable stability than Pd/C during long-term HDC reactions. As a result, ultrafine Pd particles and high Pd2+/(Pd2+ + Pd0) ratios were found in Pd/BNC.
研究领域:
环境科学
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材料科学
·
催化
·
化学工程
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Xin Song,Wenjie Pan,Fangjun Shao,Zijiang Zhao,Xiaonian Li,Zhongzhe Wei,Jianguo Wang
The development of alkyne semihydrogenation catalysts with high conversion and selectivity under mild conditions is extremely challenging. Here, the modulation of Pd by different crystalline aluminas was investigated to improve the reaction performance. XPS confirmed that different crystalline aluminas modified the electronic structure of palladium. The Pd0.5/γ-Al2O3 catalyst with a Pd loading of 0.48 wt % attained 98% conversion and 91% selectivity. Stronger interaction of the γ-Al2O3 support with the loaded Pd nanoparticles resulted in electron deflection toward the support. The electronic structure of Pd was altered by modulating the crystallographic shape of the support, resulting in metal nanoparticles containing more Pd2+. Electron-deficient Pd2+ adsorbs more strongly on an electron-rich C≡C, which in turn modulates the competitive adsorption of alkenes and alkynes. Finally, the effective semihydrogenation of phenylacetylene was realized at low temperature and pressure.
研究领域:
化学工程
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催化
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材料科学
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DOI
高影响因子
ChemCatChem
·
2024
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IF 3.8
Gao Li,Liang Yuan,Fatimah Kehinde Busari,Yue Li,Zhangjie Li,Wen Xu,Yongdong Chen
Three-way catalysis represents a pivotal technology for converting automobile exhaust pollutants into non-toxic gases. Substituting some noble metals with transition metals is considered a promising way to reduce catalyst costs. Herein, we have investigated the catalytic potential of different configurations of Pd-Cu catalysts prepared by impregnation (PdCu/MA), sol-gel (PdCu-MA), impregnation with physical mixing (Pd/Cu/MA) and sol-gel with physical mixing (Pd/Cu-MA) to modify the interaction of Pd/Cu and MgAl1.82Ce0.18O4 (MA) spinel in this comparative study. The different structures in these catalysts lead to different catalytic performances. PdCu/MA exhibits the best three-way catalytic performance, which owe to the small-sized PdCu particles with high Pd2+ content (45.3%) and optimal interaction of Pd/Cu particles and MgAl1.82Ce0.18O4 support. Furthermore, comprehensive CO-DRIFTS, H2-TPR, and O2-TPD analyses discover that the metal-support interaction is beneficial to enhance the catalytic performance in three-way catalysis. Overall, we demonstrated that the interaction between PdCu bimetals and support can regulate the electronic state of Pd, thereby enhancing the use and efficiency of noble metals.
研究领域:
催化化学
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材料科学
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环境科学
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高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2023
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IF 3.8
Pan He,Xianyu Huang,Pingting Zhuang,Hongyu Guo,Fafu Yang
Although some Pd 2+ sensors were presented, the in-situ and real-time examination of Pd 2+ based on fluorescent sensor is still a challenging task. In this work, a novel thiourea-cyanostilbene derivative ( TCS ) was designed and synthesized as the effective fluorescent sensor on in-situ and real-time sensing Pd 2+ in aqueous media. TCS possessed good AIE fluorescence in THF/H 2 O solution. The fluorescence was selectively quenched by Pd 2+ among all kinds of metallic ions . The sensing mechanism of 1:1 stoichiometry ratio for TCS with Pd 2+ was confirmed by Job's plot, 1 H NMR and MS spectra. The detection limit was as low as 4.32 × 10 −8 M. TCS exhibited the good sensing application for Pd 2+ in tested paper and simulated samples with low errors. TCS had the excellent fluorescence imaging performance in living cells with the fluorescence imaging response on Pd 2+ . This research not only reported an effective fluorescence sensor for Pd 2+ , but also suggested the good application prospect on in-situ and real-time sensing Pd 2+ in complicated environment.
研究领域:
分析化学
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材料科学
·
生物医学工程
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Long Jiang,Yaojie Liu,Xu Meng,Mo Xian,Chao Xu
Removal of toxic heavy metals needs to be assured from drug substances and catalyst residues from waste streams at the ppm level which has sometimes proved difficult, causing irreversible harm to human health and environment. Herein, on basis of binding evaluation between isothiocyanate derivatives in Pd(MeCN) 2 Cl 2 model solution, the corresponding functional materials were prepared by efficiently nucleophilic substitution and isomerization reaction on polystyrene framework. The isomerization from thiocyanide to isothiocyanate gifted SCN-2-NCS excellent Pd 2+ adsorption capacity which could tolerate various composite solvent systems and was generally superior than the widely-used isothiourea modified material PSTU. Systematic thermodynamics and kinetics study indicated the complexation with Pd 2+ was kinetically hindered and the increase of temperature contributed to the adsorption process as the maximum adsorption capacity was evaluated as 4.995 mmol·g −1 . The breakthrough point for SCN-2-NCS was 385–390 BV in Pd(MeCN) 2 Cl 2 solution (1.000 mmol·L -1 ) and reached to 126–130 BV in Pd-catalyzed debenzylation waste stream (5.433 mmol·L -1 ). Subsequently, computational chemistry certified an electrophilic addition reaction occurred to generate a five-member Pd 2+ complex in adsorption process which could be converted to N-substituted thiocarboxylic acid in acid condition, and FTIR, NMR and XPS analysis were further employed to probe the proposed adsorption mechanism.
研究领域:
环境科学
·
材料科学
·
化学工程
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DOI
高影响因子
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.
研究领域:
催化化学
·
材料科学
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产品关联
DOI
高影响因子
Nature Communications
·
2026
·
IF 18.1
Hong Feng,Chen Hongqiu,Chen Jiawei,Ying Zhehan,Peng Mi,Zhang Jingwang,Yang Zuodong,Wen Guodong,Diao Jiangyong,Sun Bo,Sun Geng,Ma Ding,Liu Hongyang
Acetylene semihydrogenation is a critical process in the polyolefin industry by selectively removing trace acetylene from ethylene-rich reformate. However, this reaction is generally limited by the inherent activity-selectivity trade-off due to the thermodynamic advantage of overhydrogenation. Herein, we develop a facile and straightforward strategy to construct Pd 2 dual-atom sites anchored on defect-rich surface-graphitized nanodiamond (ND@G) via the solvent-mediated dispersion of palladium carboxylate driven by the chelation of palladium precursors via carboxylate anion. Cs-corrected HAADF-STEM images coupled with XAS analysis unambiguously manifest the successful architecting of Pd 2 dual-atom sites. Compared to Pd 1 single-atom sites, the obtained Pd 2 /ND@G sample demonstrates superior catalytic performance in acetylene semihydrogenation, with the corresponding TOF values increased from 0.151 s −1 to 1.953 s −1 , without the obvious decline of ethylene selectivity (93.2%, at full acetylene conversion). C 2 H 2 /C 2 H 4 -TPD, H 2 -D 2 exchange reaction, isotope-labeled TPSR combined with DFT calculations confirm the effective co-activation of C 2 H 2 /H 2 on Pd 2 dual-atom sites while maintaining the weak adsorption of ethylene similar to that on its single-atom sites, which can break the activity-selectivity trade-off in acetylene semihydrogenation.
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高影响因子
ACS Catalysis
·
2026
·
IF 13.1
Yihui Cai,Chunfa Li,Wenjing Guo,Qi Zhou,Xin Zhang,Saisai Wang,Chunxiao Jin,Renqin Chang,Yuxue Yue,Jia Zhao
Designing catalytic systems that overcome the intrinsic trade-off between activity and selectivity remains a fundamental challenge in selective alkyne hydrogenation. Here, we report a preconstruction strategy (PCS) to precisely assemble Pd2-Cu1 integrated clusters (ICs) stabilized by ionic liquids, achieving fully exposed active sites with 100% atomic utilization. This rational design enables nearly complete conversion of acetylene with >99% ethylene selectivity and durability over 800 h of continuous operation. Compared to conventional impregnation methods, the PCS ensures atomic-level control over the coordination environment and electronic structure, as validated by advanced spectroscopy and density functional theory calculations. The optimized C2H2/C2H4 adsorption behavior and the tailored hydrogenation pathway over Pd2-Cu1 ICs significantly lower the energy barriers for key intermediates while suppressing overhydrogenation. This work establishes a generalizable bottom-up design principle for constructing atom-efficient, stable, and selective hydrogenation catalysts, offering a transformative route for the development of next-generation heterogeneous catalysts.
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