2D Materials
·
2019
·Vol. 7
·期 1
·015001
·
IF 7.343
Hong Jiang,Na Zhou,Ze-Xian Low,Yefei Liu,Weihong Xing,Huanting Wang,Rizhi Chen
A novel sheet-on-sheet Pd-ZIF/GO (Pd/ZG) catalyst is synthesized by constructing ZIF-L with GO and PVP-Pd nanoparticles (NPs) via a facile in situ method. The in situ introduction of GO promotes the formation of ZIF-L, leading to a higher yield of Pd/ZG, about three times higher than Pd/ZIF-L. We ascribe this to the possible interaction of the oxygen-containing groups on the GO surface with the Zn2+ cations in ZIF nodes and the PVP wrapped on the Pd surface, resulting in the formation of sheet-on-sheet Pd-ZIF/GO with good Pd dispersion. The Pd/ZG shows superior catalytic performance in the reduction of nitroarenes, and its turnover frequency (TOF) value is five times higher than Pd/ZIF-L. The superior catalytic activity can be ascribed to the uniformly dispersed tiny Pd NPs between ZIF-L and GO nanosheets, fast mass transfer in porous structure, and excellent electron conductivity due to strong interactions among ZIF-L, GO and PVP-Pd. These findings provide new opportunities for rational design of catalysts and their applications in the reduction of nitroarenes, important processes for industrial synthesis of pesticides, dyes, medicines, etc.
研究领域:
材料科学
·
催化化学
·
工业化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2025
·
IF 6.2
Wanchen Zhu,Zhongyang Luo,Feiting Miao,Longyi Liu
Biomass hydropyrolysis vapor upgrading (HPVU) is a promising approach for biofuel production, where metallic catalysts play a key role in oxygen removal and aromatic hydrocarbon formation. In this study, Pd/HZSM-5 and Mo/γAl 2 O 3 catalysts were prepared and utilized individually or in combination to investigate their effects on poplar HPVU in a continuous-flow reactor. Meanwhile, the influence of upgrading temperature on hydrodeoxygenation (HDO) reactions was studied. At an upgrading temperature of 400 ℃, combination of Pd/HZSM-5 and Mo/γAl₂O₃ resulted in an organic phase yield of 9.19 wt%. The mass yield and selectivity of aromatic hydrocarbons reached 8.13 wt% and 93.4 %, respectively, with selectivity of C8 + monocyclic aromatic hydrocarbons accounting for 56.7 %. The overall mass balance was 96.2 %. The presence of Pd promotes hydrogenation and hydroalkylation reactions, while Mo/γAl₂O₃ enhances deoxygenation. Additionally, its mesoporous structure facilitates reactant diffusion. The density functional theory calculations confirmed that Pd could efficiently activate H 2 and thus provide hydrogen radicals for HDO on Mo/γAl₂O₃ surface, which revealed the synergistic effect of these two catalysts. This study highlights that noble-metal catalyst aided by oxophilic metal catalyst can make a significant contribution to biomass HPVU.
研究领域:
能源与催化
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Wei Guo,Yao Qin,Cheng Liu,Binbin Guo,Junhua Zou,Zenghong Xie,Ling Wu
This work reports the rapid and effective photocatalytic dechlorination of 3,3′,4,4′-trtrachlorobiphenyl (PCB77) with highly dispersed Pd nanoclusters loaded two-dimensional (2D) TiO 2 (B) nanosheets (Pd/TiO 2 (B)) under visible light irradiation, achieving a dechlorination efficiency of 100 % with H 2 O used as an H-donor source. The ultra-thin TiO 2 (B) nanosheets provide a good platform for studying the dechlorination intermediates/pathways of PCB77 at the molecular level. It is proved that the dechlorination of PCB77 is a stepwise process, in which chlorines at the para positions are much more susceptible than those at the meta positions due to the activation of the C Cl bond in the presence of Pd nanoclusters. Furthermore, in-situ FTIR results of D 2 O absorption suggest that the TiO 2 (B) nanosheets with abundant surface defects greatly promote the activation of water molecules via the formation of surficial complexes by hydrogen bonds. Finally, a synergistic mechanism is proposed for photocatalytic dechlorination of PCB77 over Pd/TiO 2 (B). The study provides an efficient method for complete dechlorination of PCB77 and an in-depth understanding photocatalyzed dechlorination reaction mechanism at the molecular level, which may extend to other photocatalytic dehalogenation reactions of halogenated pollutants.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Bio Materials
·
2018
·
IF 0
Yu Liu,Lei Ding,Dandan Wang,Min Lin,Haizhu Sun,Hao Zhang,Hongchen Sun,Bai Yang
Photothermal therapy (PTT) is successfully integrated with photodynamic therapy (PDT) to effectively improve the curative effect of cancer. The therapy nanoplatform is based on hollow Pd (H–Pd) nanospheres conjugated with Ce6 (Pd@Ce6). H–Pd nanospheres and Ce6 work as PTT and PDT agents, respectively. The H–Pd nanospheres with tunable surface plasmon resonance (SPR) properties effectively absorb light with near-infrared (NIR) emission and then convert the light to heat, selectively killing tumor cells. The experimental results show that H–Pd nanospheres with a size of 90 nm have the strongest absorbance and exhibit a high photothermal conversion efficiency (η) of 70%. Moreover, the absorption intensity and photothermal properties of H–Pd nanospheres do not show any decrease after 6 months of storage at room temperature, showing their excellent stability. Furthermore, after Ce6 is conjugated onto the surface of H–Pd nanospheres using polyethylenimine (PEI) as a linker, Pd@Ce6 not only exhibits the capabilities of photothermal conversion but also generates singlet oxygen (1O2), realizing the integration of PDT and PTT. In cell experiments, 86% of HeLa cells are killed after Pd@Ce6 is simultaneously irradiated with 660 and 808 nm lasers for 5 min with a power of 0.5 and 2 W cm–2, respectively. This successful combination of PTT with PDT to eradicate cancer provides a noninvasive and harmless way for cancer therapy.
研究领域:
生物医学工程
·
肿瘤学
✓ 已验证
DOI
ACS Applied Materials & Interfaces
·
2016
·
IF 7.145
Wenhui Wang,Ting He,Xuehua Liu,Weina He,Hengjiang Cong,Yangbin Shen,Liuming Yan,Xuetong Zhang,Jinping Zhang,Xiaochun Zhou
Hydrogen is regarded as a future sustainable and clean energy carrier. Formic acid is a safe and sustainable hydrogen storage medium with many advantages, including high hydrogen content, nontoxicity, and low cost. In this work, a series of highly active catalysts for hydrogen production from formic acid are successfully synthesized by controllably depositing Pd onto Ag nanoplates with different Ag nanofacets, such as Ag{111}, Ag{100}, and the nanofacet on hexagonal close packing Ag crystal (Ag{hcp}). Then, the Pd–Ag nanoplate catalysts are supported on Vulcan XC-72 carbon black to prevent the aggregation of the catalysts. The research reveals that the high activity is attributed to the formation of Pd–Ag alloy nanofacets, such as Pd–Ag{111}, Pd–Ag{100}, and Pd–Ag{hcp}. The activity order of these Pd-decorated Ag nanofacets is Pd–Ag{hcp} > Pd–Ag{111} > Pd–Ag{100}. Particularly, the activity of Pd–Ag{hcp} is up to an extremely high value, i.e., TOF{hcp} = 19 000 ± 1630 h–1 at 90 °C (lower limit value), which is more than 800 times higher than our previous quasi-spherical Pd–Ag alloy nanocatalyst. The initial activity of Pd–Ag{hcp} even reaches (3.13 ± 0.19) × 106 h–1 at 90 °C. This research not only presents highly active catalysts for hydrogen generation but also shows that the facet on the hcp Ag crystal can act as a potentially highly active catalyst.
研究领域:
催化化学
·
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Pingping Wu,Lei Song,Yue Wang,Xuehua Liu,Zhengke He,Peng Bai,Zifeng Yan
Achieving the balance between the catalytic activity and product selectivity still remains a challenge in partial oxidation processes, because the products are prone to be over-oxidized. Lewis acids (such as AlCl 3 ) have previously been identified to interact with C O groups, which can prevent the ketone products from further transformation. In this work, ZrO 2 promoted Au-Pd/γ-Al 2 O 3 catalyst was designed to enhance the benzaldehyde selectivity by generating more surface Lewis acid site on ZrO 2 -modified alumina. Results show that the introduction of ZrO 2 (5%) resulted in the formation of more surface Lewis acid sites, which improved the benzaldehyde selectivity through the strengthened interaction between the Lewis acid sites and C O groups in benzaldehyde. Besides, the addition of small amount of ZrO 2 enhanced the noble metal dispersion and led to the formation of more active sites to improve the oxygen transfer during the reaction.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Jia-Fang Xie,Jie-Jie Chen,Yu-Xi Huang,Xing Zhang,Wei-Kang Wang,Gui-Xiang Huang,Han-Qing Yu
In this work, a novel Cu-Pd heterostructure, derived from CuCl-PdO x hexagonal microplates, was prepared to tune selective single hydrocarbon production from electrochemical CO 2 reduction. The CuCl-PdO x hexagonal microplates were synthesized by a dual-potential electrodeposition technique, followed by electrochemical reduction to form Cu-Pd heterostructure. This Cu-Pd heterostructure exhibited a much higher CO 2 -to-CH 4 selectivity (32 % Faradaic efficiency, FE) compared to pure Cu or Pd. Moreover, Cu-Pd heterostructure showed excellent suppression on C 2 H 4 generation (below 1 % FE). The density functional theory calculations suggested that the hollow site of Pd region in the Cu-Pd heterostructure could stablize CO* intermediate and selectively lowered the energy demand for CH 4 formation rather than C 2 H 4 . This work provides new opportunities of designing Cu-based electrocatalysts for selective CO 2 reduction to single hydrocarbon.
研究领域:
材料科学
·
电化学
·
催化
·
理论化学
✓ 已验证
产品关联
DOI
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
·
催化
·
材料科学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2022
·Vol. 23
·期 22
·14072
·
IF 6.208
Shiyue Chen,Yujun Yang,Mingjun Zhang,Xiaohong Ma,Xiaoxiao He,Teng Wang,Xi Hu,Xiang Mao
Dye degradation is a key reaction in organic decomposition production through electron donor transferring. Palladium (Pd) is the best-known element for synthesis Pd-based catalyst, the surface status determines the scope of relative applications. Here we first prepare Pd-Cu alloy nanoparticles (NPs) by co-reduction of Cu(acac)2(acac = acetylacetonate) and Pd(C5HF6O2)2in the presence of sodium borohydride (NaBH4) and glutathione (GSH). The obtained Pd-Cu is about ~10 nm with super-hydrophilicity in aqueous mediums. The structural analysis clearly demonstrated the uniform distribution of Pd and Cu element. The colloidal solution keeps stability even during 30 days. Bimetallic Pd-Cu NPs shows biocompatibility in form of cell lines (IMEF, HACAT, and 239 T) exposed to colloidal solution (50 µg mL−1) for 2 days. It shows the catalytic multi-performance for dye degradation such as methyl orange (MO), rhodamine B (RhB), and methylene blue (MB), respectively. The as-synthesized nanoparticles showed one of the best multiple catalytic activities in the industrially important (electro)-catalytic reduction of 4-nitrophenol (4-NP) to corresponding amines with noticeable reduced reaction time and increased rate constant without the use of any large area support. In addition, it exhibits peroxidase-like activity in the 3, 3′, 5, 5′-Tetramethylbenzidine (TMB) color test and exhibit obvious difference with previous individual metal materials. By treated with high intensity focused ultrasound filed (HIFU), Pd-Cu NPs might be recrystallized and decreased the diameters than before. The enhancement in catalytic performance is observed obviously. This work expedites rational design and synthesis of the high-hierarchy alloy catalyst for biological and environment-friendly agents.Keywords:Pd-Cu NPs;hydrophilic;biocompatibility;catalytic agent;dye degradation
研究领域:
材料科学
·
环境科学
·
生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Binbin Jin,Xin Ye,Heng Zhong,Fangming Jin
Efficient conversion of CO2/bicarbonate into chemicals using solar energy as driving force is meaningful to alleviate global warming caused by excessive CO2 emission. In this work, a direct light-driven method of bicarbonate hydrogenation into formate over a nanocatalyst Pd/TiO2 is proposed. Formic acid has recently attracted increasing attention as a promising hydrogen storage carrier. By using the Pd/TiO2, the reaction system achieved a self-heating effect under irradiation, promoting the hydrogenation of bicarbonate. Owing to its extraordinary photothermal conversion ability and efficient light utilization, the 5 wt % Pd/TiO2 exhibited a high photothermal conversion efficiency of 30.9% under experimental illumination. The desirable performance of the Pd/TiO2 catalyst for hydrogenation of bicarbonate is attributed to the elevated temperature from the localized surface plasmon resonance effect of nano-Pd and the direct participation of photogenerated carriers in hydrogenation of bicarbonate. This study combined the merits of photocatalysis and thermocatalysis, providing a promising method for light-driven conversion of CO2 using the photothermal synergistic effect.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
RSC Advances
·
2019
·Vol. 9
·期 59
·34581-34588
·
IF 3.049
Li Wang,Yue Zhang,Qingqing Ma,Zhiyong Pan,Baoning Zong
Organosilane-functionalized mesoporous silica SBA-15 was prepared by the co-condensation method and then applied as a support of Pd catalysts for hydrogenation of 2-alkyl-anthraquinone (AQ, alkyl = ethyl, tert-butyl and amyl). The as-prepared Pd catalysts were characterized by X-ray diffraction, Fourier transform infrared spectroscopy, thermogravimetric analysis, N2 adsorption–desorption, zeta potential, water contact angles measurement and transmission electron microscopy. By extending the pre-hydrolysis time of the silica source, the content of functional groups in the catalysts slightly increases. However, there is an initial increase in zeta potential and water contact angles up to a maximum at 2 h, followed by a decrease as the pre-hydrolysis time was further prolonged. The hydrophobicity created by organic functionalization has positive effects on AQ hydrogenation. The catalyst with the highest hydrophobicity exhibits the highest catalytic activity, with increments of 33.3%, 60.0% and 150.0% for hydrogenation of ethyl-, tert-butyl- and amyl-anthraquinone compared with the unfunctionalized one.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Fangxu Lu,Song Wen,Jie Jiang,Jinchong Zhao,Changsheng Zhang,Junjie Feng,Jing Zhang,Bing Sun,Wei Xu
It is generally acknowledged that the crystal structure of the support plays a crucial role in the catalytic performance, however, the exact role of crystal structure in the catalytic system remains controversial. The Pd/TiO2 catalysts designed in this study with different crystals (rutile (r) and anatase (a)) were employed to study the effects of the crystal structure via a probe reaction for oxygen removal under a hydrogen atmosphere. Under the same reaction conditions, the temperature to achieve 90% O2 conversion on Pd/a-TiO2 could reach up to 150 °C, which is ∼1.4 times (107 °C) that of the Pd/r-TiO2 catalyst. Based on the various characterization results, it is found that strong metal support interactions (SMSIs) are dominant on the Pd/r-TiO2 catalyst, which could facilitate the formation of oxygen vacancies and Pd2+ species in the active sites, resulting in excellent catalytic performance. This study not only improves the understanding of the distinctive structural properties of TiO2 crystal support but also offers an effective strategy to design efficient heterogeneous catalysts via tuning SMSIs.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）