APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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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.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Zhengjie Gong,Tao Ma,Feng Liang
Organic dyes and nitrophenols in the textile industry are wastewater pollutants. In order to develop an efficient nanocatalysts to remove organic pollutants in wastewater, the trimetallic Ni@Cu@Pd nanoparticles (Ni@Cu@Pd NPs) with a blackberry-like structure was successfully prepared by a seed mediated growth method for the first time. The blackberry-like structure and the presence of Ni, Cu and Pd have been confirmed through TEM, SEM, EDS and XPS characterizations. Owing to the charge interaction between metal species along with blackberry-like structure, trimetallic Ni@Cu@Pd NPs delivered a record high catalytic activity toward the reduction of rhodamine B (RhB), with an apparent rate constant of 7.20 min −1 . Ni@Cu@Pd NPs also exhibited high activity for the catalytic reduction of methylene blue (MB) and 4-nitrophenol (4-NP). Moreover, the Ni@Cu@Pd NPs catalyst showed excellent stability and reusability.
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JOURNAL OF NANOBIOTECHNOLOGY
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2021
·Vol. 19
·期 1
·1-18
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IF 10.435
Zhao Bonan,Dong Zhipeng,Liu Weixing,Lou Fangning,Wang Qiyan,Hong Hao,Wang Yue
Background According to data estimated by the WHO, primary liver cancer is currently the fourth most common malignant tumor and the second leading cause of death around the world. Hepatocellular carcinoma (HCC) is one of the most common primary liver malignancies, so effective therapy is highly desired for HCC. Results In this study, the use of poly( l -Aspartic acid)-poly(ethylene glycol)/combretastatin A4 (CA4-NPs) was aimed to significantly disrupt new blood vessels in tumor tissues for targeted hepatic tumor therapy. Here, PEG-b-PAsp-g-CA4 showed significantly prolonged retention in plasma and tumor tissue. Most importantly, CA4-NPs were mainly distributed at the tumor site because of the triple target effects—enhanced permeability and retention (EPR) effect, acid-sensitive (pH = 5.5) effect to the tumor microenvironment (TME), and good selectivity of CA4 for central tumor blood vessel. Considering that CA4-NPs might induce severe hypoxic conditions resulting in high expression of HIF-1α in tumor tissues, which could induce the overexpression of PD-L1, herein we also used a programmed death-ligand 1 antibody (aPD-L1) to prevent immunosuppression. This way of complementary combination is able to achieve an ideal treatment effect in tumor site where CA4-NPs and aPD-L1 could respond to the inner area and peripheral area, respectively. As a result, a significant decrease in tumor volume and weight was observed in the combination group of CA4-NPs plus aPD-L1 compared with CA4-NPs or aPD-L1 monotherapy in subcutaneous Hepa1-6 hepatic tumor models. Conclusions We presented a new idea that co-administration of CA4-NPs and aPD-L1 possessed notable anti-tumor efficacy for HCC treatment. Graphic abstract
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高影响因子
Catalysts
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2021
·Vol. 11
·期 2
·287
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IF 4.146
Jianguo Liu,Mingyue Zhang,Longlong Ma
Dibenzylamine motifs are an important class of crucial organic compounds and are widely used in fine chemical and pharmaceutical industries. The development of the efficient, economical, and environmentally friendly synthesis of amines using transition metal-based heterogeneous catalysts remains both desirable and challenging. Herein, we prepared the covalent organic framework (COF)-supported heterogeneous reduced COF-supported Pd-based catalyst and used it for the one-pot reductive amination of aldehydes. There are both Pd metallic state and oxidated Pdσ+in the catalysts. Furthermore, in the presence of the reduced COF-supported Pd-based catalyst, many aromatic, aliphatic, and heterocyclic aldehydes with various functional groups substituted were converted to their corresponding amines products in good to excellent selectivity (up to 91%) under mild reaction conditions (70 °C, 2 h, NH3, 20 bar H2). This work expands the covalent organic frameworks for the material family and its support catalyst, opening up new catalytic applications in the economical, practical, and effective synthesis of secondary amines.Keywords:COF;reduced COF-supported Pd-based catalyst;reductive amination;secondary amines
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
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IF 3.573
Fengnan Wang,Jiuxuan Zhang,Yanhua Shao,Hong Jiang,Yefei Liu,Rizhi Chen
Covalent organic frameworks (COFs) have emerged as an excellent support for heterogeneous catalysis due to their regular pore structure and high specific surface area. Herein, a series of porous TpPa-1 with different morphologies and structures were achieved by adjusting the ratio of water to acetic acid in the solvent-thermal process, and Pd@TpPa-1 catalysts were obtained with Pd solution impregnation. Notably, Pd@TpPa-1-100 prepared with 100 wt % water as the catalyst has superior catalytic properties in the phenol hydrogenation to cyclohexanone, and its turnover frequency (TOF) of 33.1 h–1 is about 7 times higher than that of Pd@TpPa-1-0 synthesized with 100 wt % acetic acid as the catalyst. The two-dimensional (2D) nanosheet structures, highly dispersed Pd nanoparticles (NPs) with small particle size, and superhydrophilicity should be responsible for the superior catalytic performance of Pd@TpPa-1-100. Furthermore, Pd@TpPa-1-100 also has better catalytic performance in the hydrogenation of catechol, resorcinol, and hydroquinone than Pd@TpPa-1-0 and exhibits superior catalytic stability. This study provides a new approach for the structural regulation of metal-based COF catalysts.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2020
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IF 5.162
Yuqing Yu,Shilin Liu,Ying Pei,Xiaogang Luo
Dyeing industry highly contributes to environmental pollution and this needs to be addressed on priority. Pd NPs/CMs, a highly efficient and reusable catalyst for methylene blue (MB) decolorization , were fabricated by in-situ reduction method based on the cellulose microspheres (CMs). Pd NPs/CMs were characterized for the structure and catalytic performance by spectroscopic techniques such as SEM, EDS, XRD, IR, XPS, porosity, zeta potential , MS, and UV–visible spectroscopy, which all demonstrated that Pd NPs were distributed on the cellulose microspheres uniformly and exhibited excellent catalytic performances to decolorize a model organic dye MB in the presence of NaBH 4 with catalytic efficiency higher than 99.8%. More importantly, Pd NPs/CMs were proven to show excellent reusability for at least five cycles. Decolorization mechanism of MB, via the destruction of the chromophores (C N and S ) of MB, was established with the help of MS combined with IR and XPS. Blank experiments using pure cellulose microspheres were carried out simultaneously to estimate the level of catalytic capacity achieved to Pd NPs/CMs. These materials proved themselves having great potential in large scale applications to treat dye-containing wastewater.
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Green Energy & Environment
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2020
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IF 6.395
Revanasiddappa Manjunatha,Li Dong,Zibo Zhai,Jianyi Wang,Qianru Fu,Wei Yan,Jiujun Zhang
Rational design and synthesis of low-cost trifunctional electrocatalysts with improved stability and superior electrocatalytic activity for oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER) are highly desirable but remain as the bottlenecks at the current state of technology. In this paper, the cobalt-iron (Co–Fe) composite supported on nitrogen-doped carbon nanotubes (CoFe composite/NCNTs) is synthesized. The intrinsic OER and HER catalytic activities of this CoFe composite/NCNTs composite are significantly improved with palladium (Pd) nanocluster decoration [Pd-coated (CoFe composite/NCNTs)]. The as-prepared Pd-coated (CoFe composite/NCNTs) catalyst exhibits excellent trifunctional electrocatalytic activity and stability due to the interfacial coupling between Pd and (CoFe composite/NCNTs). This catalyst is successfully employed in the water electrolysis cell as both OER and HER electrode catalysts, flexible rechargeable Zn-air battery as the bifunctional ORR and OER electrode catalyst. The cell voltage of this catalyst-coated electrodes requires only 1.60 V to achieve 10 mA cm −2 current density for water electrolysis cell, which is comparable to and even better than that of Pt/C and Ir/C based cell. The primary Zn-air battery using this catalyst shows a constant high open-circuit voltage (OCV) of 1.47 V and a maximum power density of 261 mW cm −2 in the flooded mode configuration. Most importantly, a flexible Zn-air battery with this catalyst runs very smoothly without a change in voltage gap during flat, bending, and twisting positions.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Amir Mahmoud Makin Adam,Madeha Ishag Adam,Chunmiao Zhang,Baffa Haruna,Mingzhu Chi,Xiong Li,Jia Kang Wan,Mujtaba Aminu,Girum Girma Bizuneh,Min Deng,Aimei Zhu,Qiugen Zhang,Qinglin Liu
Developing highly active Pd-based nanocatalysts with a well-organized structure is desired for direct alcohol fuel cell commercialization. In this study, room temperature seed mediated growth strategy has been successfully developed to prepare ternary Pd@Cd x -Ag y core-shell as advanced novel non-Pt anode nanocatalysts for ethanol oxidation reaction EOR in alkaline electrolyte . The introduction of oxophilic Cd and Ag metals into Pd nanocatalysts can reduce the adsorption energy of OH ads on the Pd@Cd x -Ag y nanocatalysts and inhibit the CO ads on the Pd surface. Morphological characterization demonstrates that the as-synthesized Pd@Cd x -Ag y nanocatalysts are well-organized core-shell nanostructure with Pd NPs as the core and Cd-Ag alloy as the shell. Moreover, electrochemical results indicate that the Pd@Cd 1 -Ag 1 core-shell catalyst exhibit a remarkable electrochemical activity ( 2995.76 mA mg Pd − 1 ), excellent CO tolerance and long-term durability compared to those of Pd@Cd ( 1285.9 mA mg Pd − 1 ), Pd@Ag ( 2423.52 mA mg Pd − 1 ) and commercial Pd/C (JM) ( 477.4 mA mg Pd − 1 ) nanocatalysts. The excellent catalytic activity and stability of Pd@Cd 1 -Ag 1 nanocatalyst can be associated to their huge electrochemical active surface area, positive influence of Cd-Ag NPs on Pd NPs and the unique well-organized core-shell nanostructure. These results suggested that the as-synthesized Pd@ C d x -Ag y core-shell could serve as advanced catalysts towards alkaline DEFCs.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Yanju Chen,Zhi Liu,Shoujie Liu,Yuansheng Cheng,Chao Zhang,Jiqing Jiao,Yukun Lu,Wenhong Wang,Kaian Sun,Xiaolong Bi,Aiyan Han,Bin Liu,Yuan Pan,Yunqi Liu,Chenguang Liu
Developing catalysts with high activity and high atom utilization as well as exploring catalytic active sites are the biggest challenges for the electrocatalytic hydrodechlorination technology. Herein, a novel strategy of Pd crystal transformation induced by in-situ doping was proposed, and a series of amorphous Pd–P nanoparticles (NPs) with controllable coordination environment were synthesized successfully. The amorphous Pd–P NPs catalyst exhibits the highest activity for electrocatalytic hydrodechlorination and good cycling stability when the Pd–P coordination number is 3 and the Pd–Pd coordination number is 4. The 4-chlorophenol hydrodechlorination efficiency of Pd–P-60 NPs reaches 100 % within 2 h, and the mass activity is 8.58 min −1 g −1 , which is 5.57 times as high as that for crystalline Pd NPs catalyst. Theoretical calculation shows that Pd–P catalyst facilitates the desorption of phenol and weakens the toxic effect on active sites. Density of states indicate that the doping of P results in a downshift of d -band center, facilitating the desorption of phenol. This work discovers the crystal effect and coordination effect of amorphous Pd–P NPs for electrocatalytic hydrodechlorination, which lays an important theoretical foundation for the design and development of high-performance Pd-based catalysts for electrocatalytic hydrodechlorination.
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Green Energy & Environment
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2020
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IF 6.395
Difan Li,Xiuge Zhao,Qingqing Zhou,Bingjie Ding,Anna Zheng,Qingpo Peng,Zhenshan Hou
Selective oxidation of glycerol provides a feasible route towards the sustainable synthesis of high value-added chemicals. Herein, the hydroxyapatite (HAP) supported palladium (Pd) species were fabricated by impregnation and subsequent calcination. The as-obtained heterogeneous Pd catalyst afforded not only excellent selectivity to glyceric acid (GLA) up to 90% with 59% conversion of glycerol but also good recyclability by using molecular oxygen as an oxidant under mild conditions. The characterization of catalysts indicated that both the surface basicity and Pd sites on the catalyst played a crucial role in promoting glycerol oxidation. Notably, it demonstrated that the presence of the vicinal hydroxyl group of glycerol molecule can assist the oxidation reaction via forming a coordination between the vicinal hydroxyl group and Ca 2+ sites on HAP-derived catalysts. In this catalytic process, the secondary hydroxyl of glycerol kept untouched and the primary hydroxyl of glycerol was converted into carboxyl group, while the Pd species acted as active centers for cooperatively promoting the subsequent oxidation to generate GLA. Additionally, this catalytic system can be extended widely for the oxidative conversion of other vicinal diols into the corresponding α-hydroxycarboxylic acids selectively. Isotope labeling experiment using H 2 18 O confirmed that H 2 O not only acted as solvent but also was involved in the catalytic cycles. On the basis of the results, a possible reaction mechanism has been proposed. The HAP-supported Pd catalytic system has been shown to serve as an effective approach for the upgrading of bio-derived vicinal diols to high value-added chemicals.
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COMPOSITES SCIENCE AND TECHNOLOGY
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2020
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IF 7.094
Junjun Huang,Chengmei Gui,Haodong Ma,Peng Li,Wangping Wu,Zhenming Chen
Electroless nickel plating provides a rapid and low-cost approach to prepare surface-metallization material, but complicated technology would increase cost and restrict its application. In this work, a new kind of Pd nanoparticle/polymer brush (Pd/ PB ) catalytic solution ( AS ) with a mixture of deionized water, ethanol, 3-aminopropyltriethoxysilane ( KH550 ), PdCl 2 solution was designed to modify and activate polyethylene terephthalate ( PET ) simultaneously. Pd nanoparticle could be adsorbed by PB with –NH 2 , Si–O–Si groups from hydrolyzed KH550. An activated layer with Pd/PB structure established on PET surface after coating AS solution. The generated Ag/PB that served as seed to catalyze the electroless nickel plating. As a result, a facile route for electroless nickel plating was achieved. The maximum effective thickness, rupture work and adhesion of Ni-plated coating were about 0.8 μm, 0.4 J/m 2 , and 5B, respectively, and it maintained considerable conductivity even after 1000 times of cyclical bending. This dependable technology has great potential application in the preparation of metal-polymer material.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
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IF 4.939
Ying-Hua Zhou,Xingyun Cao,Jingzhu Ning,Changchun Ji,Yong Cheng,Jing Gu
To exploit the low-cost and efficient catalyst for the hydrolytic dehydrogenation of ammonia borane , trace amount of palladium-doped transition metal (Cu, Ni, Co, Fe and Zn) nanoparticles have been incorporated into the interior of metal-organic frameworks named ZIF-8, ZIF-67, ZIF-67/ZIF-8 and core-shell ZIF-67@ZIF-8 by a double-solvent approach. The optimized catalyst of CuPd 0.01 @ZIF-67@ZIF-8 composite exhibited an excellent activity with a turnover frequency (TOF) value of 30.15 mol H 2 (mol metal ) −1 min −1 at 298 K and a relatively low activation energy of 38.78 kJ mol −1 . It might attributed to both ultrafine size of metal nanoparticles (~3 nm) induced by the confinement of core-shell ZIF-67@ZIF-8 and the synergistic effect between Pd and Cu. Moreover, the detailed kinetic study has manifested that this catalytic reaction is first-order in regards to the catalyst amount while zero-order as for the concentration of ammonia borane. In addition, the durability and recyclability of CuPd 0.01 @ZIF-67@ZIF-8 have been demonstrated to be great.
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