Catalysis Science & Technology
·
2019
·Vol. 10
·期 1
·138-146
·
IF 5.726
Ting Wang,Xueqin Tao,Yi Xiao,Ganhua Qiu,Yun Yang,Benxia Li
While heterogeneous photocatalysis is regarded as a sustainable strategy to achieve organic reactions for the production of high-value-added organics, photocatalytic efficiency is generally limited by poor charge separation, dull surface catalytic activity and the consequently caused insufficient generation of active species. Herein, the hybrid structures of metal–organic frameworks (MOFs) incorporated with Pd ultrasmall nanocrystals are synthesized, and their photocatalytic performance is evaluated by the oxidative coupling of benzylamine as a model reaction. The photocatalytic activity of the Pd/MIL-125-NH2 hybrid material with an optimal Pd loading is greatly superior to that of the pristine MIL-125-NH2, achieving a high benzylamine conversion rate of 3136 μmol h−1 gcat−1 at 94.08% conversion. The enhanced charge transfer and separation in Pd/MIL-125-NH2 are verified by photoluminescence spectroscopy and photoelectrochemical experiments. Photogenerated reactive oxygen species are probed by 3,3′,5,5′-tetramethylbenzidine (TMB) as an indicator and the reactive intermediates in the photocatalytic systems are identified by in situ ESR detection. The results confirm that the optimized Pd/MIL-125-NH2 hybrid catalyst possesses higher ability for molecule activation and that both superoxide radical (˙O2−) and singlet oxygen (1O2) are the dominant oxidative species in the present photocatalytic system. Therefore, the dual advantages of Pd/MIL-125-NH2 hybrid structures for promoting the photogenerated charge transfer/separation and providing highly catalytic sites for molecule activation contribute to higher photocatalytic activity.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Yang Lu,Zhenyi Wang,Wangxi Fang,Yuzhang Zhu,Yatao Zhang,Jian Jin
Porous polymeric support membranes with outstanding organic solvent resistance are highly required for fabricating thin-film composite (TFC) organic solvent nanofiltration (OSN) membranes. In this work, we report the fabrication of a high-permeance TFC-OSN membrane by the use of a polytetrafluoroethylene (PTFE) microfiltration membrane loaded with single-walled carbon nanotubes coated by a polydopamine (PD/SWCNT) network film (named the PD/SWCNT/PTFE composite membrane) as the support. Through interfacial polymerization between m-phenylenediamine and trimesoyl chloride, a polyamide (PA) thin film has successfully grown on the surface of the PD/SWCNT/PTFE composite membrane. The resulting PA TFC-OSN membrane exhibits a high methanol permeance up to 13.2 L m–2 h–1 bar–1 with a rejection rate of 89.6% to 6-hydroxy-2-naphthalenesulfonic acid sodium salt (HNSA, Mw = 246.21). Moreover, the rejection rates of the PA TFC-OSN membrane to various dyes remain unchanged before and after DMF activation, indicating that it possesses an excellent resistance to organic solvents.
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高影响因子
Frontiers of Materials Science
·
2023
·Vol. 17
·期 2
·1-10
·
IF 2.7
Liu Tianli,Zhang Jian,Xu Mingjie,Tian Chuanjin,Wang Chang-An
Sintering resistant noble metal nanoparticles are critical to the development of advanced catalysts with high activity and stability. Herein, we reported the construction of highly dispersed Pd nanoparticles loaded at the inner wall of ZrO 2 hollow spheres (Pd@HS-ZrO 2 ), which shows improved activity and thermal stability over references in the Pd-ZrO 2 (catalyst-support) system. Even after 800 °C high temperature calcination, the Pd nanoparticles and ZrO 2 hollow spheres did not undergo morphological changes. The Pd@HS-ZrO 2 manifests batter catalytic activity and thermal stability than the counterpart Pd/ZrO 2 catalysts. In comparison to Pd/ZrO 2 -800, Pd@ZrO 2 -800 exhibits a 25°C reduction in the temperature required for complete conversion of CO. The enhanced catalytic activity and thermal stability of Pd@HS-ZrO 2 can be attributed to the nanoconfinement effect offered by the 10 nm wall thickness of the ZrO 2 hollow spheres, which suppresses the coarsening of the Pd nanoparticles (active center for catalysis).
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RSC Advances
·
2017
·Vol. 7
·期 40
·24822-24827
·
IF 3.108
Ting Yu,Guoxing Yin,Peng Yin,Ying Zeng,Haitao Li,Youyu Zhang,Shouzhuo Yao
We have synthesized a novel long-wavelength fluorescent probe MFC for detection of palladium (Pd0). This probe not only shows high selectivity for palladium, but also could quickly discriminate different palladium species (Pd0, Pd2+, Pd4+) in phosphate buffered solution. After the reaction with Pd(PPh3)4, the UV absorption of the probe MFC shifts from 334 nm to 594 nm within a few minutes. The probe MFC conjugated with alkyl carbamate, which destroys the principle of intramolecular charge transfer (ICT) and shows weak fluorescence. Based on the Pd0-catalyzed Tsuji–Trost deallylation reaction, the fluorogen was released and the fluorescence intensity at 612 nm was observed with 13-fold enhancement along with an obvious color change from yellow to purple with low detection limit.
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ACTA PHYSICO-CHIMICA SINICA
·
2017
·Vol. 33
·期 7
·1453-1461
·
IF 0.767
LIU Jing-Wei,YANG Na-Ting,ZHU Yan
We report an efficient catalyst composed of ternary components prepared by inlaying Pd/Co3O4 nanoparticles in alkaline Al2O3 nanosheets for catalytic oxidation of methane. Pd/Co3O4 inlaid in alkaline Al2O3
exhibited a higher ability to break the C-H bond of methane than Pd/Co3O4 supported on SiO2, ZrO2, CeO2, and acidic or neutral Al2O3. Our results show more oxygen vacancies and higher amounts of surface adsorbed oxygen
on the surface of Pd/Co3O4/alkaline Al2O3 than on other catalysts, which is responsible for methane activation and conversion. Further, the Pd/Co3O4/alkaline Al2O3 catalyst can almost restore to its initial
value in the absence of water when 5% (volume fraction) vapor water was cut off, although a decrease in activity occurred when water vapor was introduced to the reaction system. Even under a condition similar to the exhaust of a lean-burn natural gas engine, the catalytic performance of the
Pd/Co3O4/alkaline Al2O3 catalyst is excellent, that is, methane could be completely converted when the sample temperature in the reaction atmosphere was ramped to 400°C.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2017
·
IF 5.401
Hong Li,Hongli Zhao,Haiyan He,Libo Shi,Xuan Cai,Minbo Lan
In this work, an ultrasensitive microelectrode for hydrogen peroxide (H 2 O 2 ) detection was constructed. The carbon fiber microelectrode (CFME) was modified with Pt-Pd nanocoral (Pt-Pd/CFME) by using a one-step electrochemical deposition method. Compared to Pt/CFME and Pd/CFME, the Pt-Pd/CFME has larger active surface area and faster electron transfer efficiency, thus exhibiting higher electrocatalytic activity for H 2 O 2 sensing. Under the optimal condition, the Pt-Pd/CFME presents fast response time (≤5 s), high selectivity (11.6 mA mM −1 cm −2 ), wide linear range (5–3920 μM) and low detection limit (0.42 μM, S/N = 3) for H 2 O 2 detection. Furthermore, the proposed sensor was successfully employed to monitor H 2 O 2 released from A549 living cells, and the detection of H 2 O 2 in milk was also realized. With the above attractive electrocatalytic properties and convenient fabrication process, the as-prepared microelectrode provides unique advantages in the monitor of H 2 O 2 in biological samples, especially in cellular environment.
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JOURNAL OF POWER SOURCES
·
2013
·
IF 4.675
Shan-Shan Li,Jing-Jing Lv,Yuan-Yuan Hu,Jie-Ning Zheng,Jian-Rong Chen,Ai-Jun Wang,Jiu-Ju Feng
In this study, a simple, facile, and effective wet-chemical strategy was developed in the synthesis of uniform porous Pt–Pd nanospheres (Pt–Pd NSs) supported on reduced graphene oxide nanosheets (RGOs) under ambient temperature, where octylphenoxypolye thoxyethanol (NP–40) is used as a soft template, without any seed, organic solvent or special instruments. The as-prepared nanocomposites display enhanced electrocatalytic activity and good stability toward methanol oxidation , compared with commercial Pd/C and Pt/C catalysts. This strategy may open a new route to design and prepare advanced electrocatalysts for fuel cells.
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FUEL
·
2025
·
IF 7.5
Zhenzhen Wang,Shufeng Lin,Liujun Wang,Zhe Wang,Bing Lu,Zhonghua Sun,Zhihui Zhang,Mingyang He,Junfeng Qian
The hydrogenation of CO 2 to formic acid (FA) represents a sustainable route for carbon utilization and chemical production, yet it faces challenges in catalytic efficiency, selectivity, and process scalability. Herein, we report a highly efficient catalytic system based on Pd supported on amine-functionalized Zr-SBA-15 (Pd/Zr-SBA-15-AP) for continuous FA synthesis in a fixed-bed reactor. The flake-shaped Zr-SBA-15 support with short mesoporous channels facilitates superior mass transfer. Meanwhile, amine functionalization was identified to serve a dual function: significantly enhancing CO 2 adsorption capacity and modulating the electronic state of Pd to form electron-enriched sites conducive to H 2 activation. The optimized catalyst, 0.3Pd/Zr-SBA-15-AP 3.0 , achieved an exceptional turnover number (TON) of 160 and a turnover frequency (TOF) of 80 h −1 , outperforming the state-of-the-art catalyst under similar continuous-flow conditions. Furthermore, the catalyst demonstrated stable performance over 32 h of continuous operation, underscoring its practical potential. This work provides a scalable strategy for sustainable FA production, effectively bridging laboratory-scale research and industrial application.
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产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2025
·Vol. 156
·期 1
·27
·
IF 2.4
Tian Hongkun,Hu Yuqi,Li Hao
Diisobutyl ketone (DIBK), a high-value chemical with growing market demand, is currently produced as a by-product in methyl isobutyl ketone (MIBK) synthesis, leading to high costs and limited output. This study investigates the one-step synthesis of DIBK from acetone condensation and hydroconversion using Pd/Beta zeolite catalysts. A series of catalysts were prepared via impregnation and systematically characterized by XRD, BET, NH₃-TPD, Py-IR, and XPS. The effects of zeolite type, SiO₂/Al₂O₃ ratio, Pd loading, and reaction conditions on catalytic performance were thoroughly examined. Results demonstrate that Pd/Beta-25, possessing the highest acid site density, optimal Brønsted-to-Lewis acid ratio, and superior Pd dispersion, achieved the best performance: 98.4% acetone conversion and 64% DIBK selectivity under optimal conditions (210 °C, 3 MPa H₂, 9 h). The synergy between abundant acid sites (facilitating condensation) and well-dispersed Pd nanoparticles (enabling hydrogenation) is crucial for promoting the consecutive reaction pathway to DIBK. This work provides fundamental insights and an efficient catalytic system for direct DIBK production, highlighting the advantage of zeolite-based catalysts over conventional Pd/resin systems. Graphical
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MOLECULES
·
2019
·Vol. 24
·期 4
·674
·
IF 3.06
Haodong Tang,Bin Xu,Meng Xiang,Xinxin Chen,Yao Wang,Zongjian Liu
Nitrogen-doped activated carbon (N-AC) obtained through the thermal treatment of a mixture of HNO3-pretreated activated carbon (AC) and urea under N2atmosphere at 600 °C was used as the carrier of Pd catalyst for both liquid-phase hydrodechlorination of 2,4-dichlorophenol (2,4-DCP) and gas-phase hydrodechlorination of chloropentafluoroethane (R-115). The effects of nitrogen doping on the dispersion and stability of Pd, atomic ratio of Pd/Pd2+on the surface of the catalyzer, the catalyst’s hydrodechlorination activity, as well as the stability of N species in two different reaction systems were investigated. Our results suggest that, despite no improvement in the dispersion of Pd, nitrogen doping may significantly raise the atomic ratio of Pd/Pd2+on the catalyst surface, with a value of 1.2 on Pd/AC but 2.2 on Pd/N-AC. Three types of N species, namely graphitic, pyridinic, and pyrrolic nitrogen, were observed on the surface of Pd/N-AC, and graphitic nitrogen was stable in both liquid-phase hydrodechlorination of 2,4-DCP and gas-phase hydrodechlorination of R-115, with pyridinic and pyrrolic nitrogen being unstable during gas-phase hydrodechlorination of R-115. As a result, the average size of Pd nanocrystals on Pd/N-AC was almost kept unchanged after liquid-phase hydrodechlorination of 2,4-DCP, whereas crystal growth of Pd was clearly observed on Pd/N-AC after gas-phase hydrodechlorination of R-115. The activity test revealed that Pd/N-AC exhibited a much better performance than Pd/AC in liquid-phase hydrodechlorination of 2,4-DCP, probably due to the enhanced stability of Pd exposed to the environment resulting from nitrogen doping as suggested by the higher atomic ratio of Pd/Pd2+on the catalyst surface. In the gas-phase hydrodechlorination of R-115, however, a more rapid deactivation phenomenon occurred on Pd/N-AC than on Pd/AC despite a higher activity initially observed on Pd/N-AC, hinting that the stability of pyridinic and pyrrolic nitrogen plays an important role in the determination of catalytic performance of Pd/N-AC.Keywords:activated carbon;hydrodechlorination;nitrogen doping;Pd
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Riyang Shu,Ying Xu,Longlong Ma,Qi Zhang,Chao Wang,Ying Chen
Many effective methods have been proposed to achieve lignin depolymerization, while controllable product distribution is still hard to realize. Herein, an efficient lignin hydrogenolysis process with controllable product distribution was put forward using Pd/C catalyst cooperated with metal chloride. Results showed that lignin produced a high amount of guaiacols in the presence of ZnCl 2 , while a high amount of phenols in the presence of CrCl 3 . Guaiacylglycerol-β-guaiacyl ether was used as the model compound to carry out the mechanistic investigation. A synergetic catalysis effect between Pd/C and metal chloride was exhibited in this process. And the Lewis acidity was an important factor to determine the product distribution. With the synergetic catalysis of Pd/C and metal chloride, the dissociation energy of β-O-4 bond was reduced significantly, which made the cleavage easier to realize. The phenolic monomer product of guaiacols was produced in the initial stage. Then CrCl 3 catalyst with strong Lewis acidity could further promote the occurrence of demethoxylation and alkylation, converting the guaiacols into phenols. This work figures out the mechanism of product control in the hydrogenolysis process and displays a clear potential for the controllable valorization of lignin.
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APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Hui Chen,Jie He,Jinsheng Sun
The production of cyclohexanone, of industrial importance, is at a distance to environment friendly and efficiency. As a solution, a mild sustainable catalytic hydrogenation is presented herein, of phenol into cyclohexanone on Pd/C with potassium formate the hydrogen donor under open atmosphere. Some important reaction conditions, such as temperature, reaction time, catalyst, amount of potassium formate, etc. were investigated and analyzed. The positive growth was found to accelerate the conversion rate of phenol while reducing cyclohexanone selectivity by weakening the protection of phosphotungstic acid. Phosphotungstic acid was confirmed to be the co-catalyst exhibiting the highest activity under given conditions. Based on experiments, we have made reasonable assumptions about the reaction mechanism, while the reaction kinetics proves high reaction rates within a wide temperature range, indicating the reaction to be quick process. Furthermore, the good reusability and recyclability of Pd/C catalyst is verified to benefit future industrial applications.
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