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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ACS Applied Energy Materials
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2021
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IF 6.024
Chuanliang Li,Yangyang Ren,Fan Gao,Baosong Li,Lanlan Li,Xinghua Zhang,Zunming Lu,Xiaojing Yang,Xiaofei Yu
Pt-based nanoframes with unique morphologies are one of the most promising catalysts for the oxygen reduction reaction (ORR). In this study, stacked Pd@PtPd core–shell rhombic dodecahedrons (Pd@PtPd RDs) were obtained by a solvothermal method, and then PtPd nanonets (PtPd NNs) were formed by etching of Pd@PtPd RDs with Fe(NO3)3 and HNO3. Combining the time-dependent changes of morphology, atomic ratio, and elemental distribution, the formation mechanism of PtPd NNs was explored. According to the electrochemical tests, the mass and specific activities of PtPd NNs were 4.7 and 7.6 times higher than those of Pt/C and 2.5 and 2.2 times as large as those of Pd@PtPd RDs in an alkaline solution, respectively. Meanwhile, PtPd NNs displayed higher stability than Pd@PtPd RDs and Pt/C. The enhanced catalytic performance might result from the unique open structures, the compressive strain, and the electron transfer from Pd to Pt atoms.
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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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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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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2020
·Vol. 412
·期 25
·6849-6858
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IF 3.637
Li Zhi,Qian Weina,Guo Hui,Song Xiao,Yan Hao,Jin Ruyi,Zheng Jianbin
In this study, novel Pd nanowire networks (PdNW) grown on three-dimensional polyaniline hydrogel (3D-PANI) were prepared via a facile one-step electrodeposition approach at a constant potential of − 0.2 V and further utilized as an electrochemical sensing material for sensitive determination of glucose in alkaline medium. Compared with the sensor based on Pd nanofilm (PdNF)/3D-PANI prepared by electrodeposition at − 0.9 V, the sensor based on PdNW/3D-PANI presented substantially enhanced electrocatalytic activity towards glucose oxidation, with an excellent sensitivity of 146.6 μA mM −1 cm −2 , a linear range from 5.0 to 9800 μM, and a low detection limit of 0.7 μM and was, therefore, demonstrated to be available for the determination of glucose in human serum. These findings are likely attributed to the combination of advantages of both PdNW and 3D-PANI, which outperformed most other Pd-based non-enzymatic glucose sensors reported earlier. Moreover, this non-enzymatic electrochemical sensor based on PdNW/3D-PANI may serve as an alternative tool for the assay of glucose and possibly other biomolecules.
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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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BULLETIN OF MATERIALS SCIENCE
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2020
·Vol. 43
·期 1
·1-7
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IF 1.392
Xiao Meng,Peng Yu,Pang Mengting,Hao Baicun,Wang Yujia,Zhang Yulian,Liao Yang,Mao Hui
Heterogeneous Pd catalysts were developed by immobilizing Pd nanoparticles (Pd NPs) onto plant polyphenol (bayberry tannin, BT) decorated γ-Al 2 O 3 . The abundant hydroxyls of plant polyphenols were capable of stabilizing the Pd NPs. Transmission electron microscopy observation confirmed that the Pd NPs with the diameter of 3.75 ± 0.5 nm were highly dispersed in the catalyst. The as-prepared Al 2 O 3 –BT–Pd catalysts were found to be highly active in mild hydrodechlorination (HDC) of 2,4-dichlorophenols (DCPs) using formic acid as a hydrogen source. The 2,4-DCPs were completely dechlorinated in 4 h at 30°C and under atmospheric pressure. During the catalytic HDC, the stabilizing capability of BT successfully prevented the leakage and aggregation of Pd NPs, thus ensuring a high cycling stability with stable and high catalytic activity. The Al 2 O 3 –BT–Pd catalysts were recycled six times, without obvious loss of activity. In the sixth cycle, the catalytic HDC yield still reached 98.29% under the same reaction conditions, superior to the control catalysts, including γ-Al 2 O 3 supported Pd NPs (Al 2 O 3 –Pd) and powdered activated carbon supported Pd NPs (AC–Pd). Furthermore, the Al 2 O 3 –BT–Pd also showed high activity in the mild catalytic HDC of 2,4,6-trichlorophenols and chlorobenzene derivatives. Our results demonstrated efficient catalysts to address the environmental issue of chlorophenol pollution.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
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IF 4.939
Yuan Zhou,Xun Zhu,Biao Zhang,Ding-Ding Ye,Rong Chen,Qiang Liao
Formic acid as a renewable fuel can be converted to clean electricity in fuel cells by high-efficient electrochemical oxidation . The conversion rate is fundamentally dictated by the synergy of interactive aspects: catalytic activity , accessibility to active sites, electron transfer , and anti-poisoning stability. For the first time, ordered mesoporous carbon (OMC) is used as the substrate for Pd–PdO catalyst for fuel cells. The unique ordered pore-channel network of OMC can enhance the spatial dispersion of Pd nanoparticles on the pore-channel wall, while the hollow pore-channel can facilitate reactant transport. Microwave and annealing treatments are found to enhance the chemical reduction and to strengthen the anchoring of Pd–PdO catalyst on OMC substrate, respectively. The OMC supported Pd–PdO catalyst (Pd–PdO/OMC) shows 1.7-fold and an order of magnitude higher mass activity and stability as compared to commercial Pd/C catalyst. For fuel cell testing, the Pd–PdO/OMC catalyst is applied to an air-breathing microfluidic fuel cell and achieves a maximum power density of 63.0 mW cm −2 , at least one-fold higher than similar previous reports.
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Green Energy & Environment
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2020
·
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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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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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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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
·
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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