ACS Applied Nano Materials
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2020
·
IF 0
Wei Zhao,Shuang Liu,Huishu Wang,Jun Yang,Xinhan Chen
Heterogeneous Pd has been developed as a well-known catalyst for debenzylation reactions via hydrogenative C–N bond cleavage. However, the extensive applications are still limited owing to a high loading and usage amount of the noble metal. Herein, well-dispersed Pd nanocatalysts over TiO2 were explored with a deposition–precipitation method and characterized by FESEM, physical adsorption, XRD, TEM, and XPS. It was proposed that the ultrasmall and electron-rich Pd nanoparticles can be enhanced over TiO2 rather than C, Al2O3, or SiO2. As representatives, the debenzylations of hexabenzylhexaazaisowurtzitane (HBIW) and tetraacetyldibenzylhexaazaisowurtzitane (TADBIW), which are key steps for the synthesis of CL-20 with the highest energy and density, were selected to evaluate the catalytic performances. It was found that Pd/TiO2 exhibited considerably low usage with high yields in the debenzylation processes of not only HBIW (1 wt ‰) but also TADBIW (4 wt ‰). Meanwhile, the superior catalytic activities can be maintained in the different reaction scales and can be repeated for TADBIW hydrodebenzylation. Hence, Pd nanoparticles supported on TiO2 can be considered to be suitable catalysts for highly efficient catalytic synthesis for hydrogenative C–N bond cleavage.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Wenjie Xue,Hongxia Liu,Baohua Mao,Honglei Liu,Minghuang Qiu,Chengguang Yang,Xinqing Chen,Yuhan Sun
Hydrogen is a promising candidate to replace the exhausting fossil fuels. However, it is still a big challenge for hydrogen storage. Liquid organic hydrogen carrier (LOHC), which possesses high safety and purity, easy transport and reversibility, is highly attractive for hydrogen storage. Herein we report a new reusable bimetallic Pd-Rh nanoparticles (NPs) catalyst with synergy effect, boosting both the hydrogenation of N-ethylcarbazole (NEC) and dehydrogenation of dodecahydro-N-ethylcarbazole (12H-NEC), which allows multiple cycles of reversible high-weight% hydrogen storage and uptake in short reaction time. Various ex- and in-situ characterizations evidenced that the superior activity was attributed to the bimetallic Pd-Rh NPs cluster structure on the surface of γ-Al 2 O 3 support. The mechanism of NEC hydrogenation over the Pd-Rh catalyst was proposed and verified by density functional theory (DFT) calculations. Such a strategy can be extended to other LOHCs and sheds light onto the development of LOHCs as energy vectors.
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Functional Materials Letters
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2020
·
IF 2
Kaicheng Yue,Zhaoqian Yan,Zhihao Sun,Anran Li,Lei Qian
In this work, graphitic carbon nitride (g-C 3 N 4 ) was modified by Pd nanoparticles (Pd-CN) to prepare an efficient cathode catalyst for Li-O 2 batteries. The specific surface area of g-C 3 N 4 was improved to 239.56 m 2 /g by two-steps thermal polymerization. Pd nanoparticles were loaded onto the g-C 3 N 4 by K 2 PdCl 4 reduction with NaBH 4 . The resulted Pd-CN composites were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, field emission scanning electron microscope, and transmission electron microscope. The results proved that g-C 3 N 4 showed three-dimensional layered and porous structure, and Pd nanoparticles were successfully supported on it. The Li-O 2 batteries using Pd-CN composites as cathode catalysts were assembled and tested. The maximum initial discharge specific capacity reached 26,614 mAh g − 1 at current density of 100 mA g − 1 . The electrodes remained large capacity under high current density, meaning excellent rate capability. Li-O 2 batteries containing Pd-CN cathode were continuously cycled for 70 cycles with no loss of capacity and obvious change in the terminal voltage. These electrochemical results indicated that the loading Pd nanoparticles effectively increased specific capacity, reduced overpotential and improved the cyclic stability. The Pd-CN composites are proved to be the promising cathode catalysts for Li-O 2 batteries.
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INTERNATIONAL JOURNAL OF PHOTOENERGY
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2020
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IF 1.88
Jing Yan,Xiaojuan Li,Bo Jin,Min Zeng,Rufang Peng
A series of TiO2, TiO2/Pd, and TiO2/PdO hollow sphere photocatalysts was successfully prepared via a combination of hydrothermal, sol-immobilization, and calcination methods. The structure and optical properties of the as-prepared samples were characterized by X-ray diffraction, field emission scanning electron microscopy, transmission electron microscopy, Brunauer-Emmett-Telleranalysis, Barrett-Joyner-Halenda measurement, and UV-Vis diffuse reflectance spectroscopy. The photocatalysis efficiencies of all samples were evaluated through the photocatalytic degradation of rhodamine B under visible light irradiation. Results indicated that TiO2/PdO demonstrated a higher photocatalytic activity (the photocatalytic degradation efficiency could reach up to 100% within 40 min) than the other samples and could maintain a stable photocatalytic degradation efficiency for at least four cycles. Finally, after using different scavengers, superoxide and hydroxyl radicals were identified as the primary active species for the effectiveness of the TiO2/PdO photocatalyst.
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PHARMACOLOGICAL RESEARCH
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2020
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IF 5.893
Linxin Teng,Kaiyuan Wang,Weiping Chen,Yun-shan Wang,Lei Bi
Traditional Chinese medicine (TCM) plays a vital part in cancer treatment due to its unique superiority. Huoxue Yiqi Recipe-2 (HYR-2) was supposed to have therapeutic effect on lung cancer, which came from Ze Qi Decoction in one of the four great classics of TCM called "Synopsis of Prescriptions of the Golden Chamber". Network pharmacology demonstrated that the targets of active components from HYR-2 were significantly enriched in the signaling pathways, which were closely associated with non-small cell lung cancer (NSCLC) and programmed death ligand 1 (PD-L1). Then, data about NSCLC was downloaded from Gene Expression Omnibus database (GEO). The Cancer Genome Atlas (TCGA) and DisGeNET was analyzed by bioinformatics, and 214 biomarkers for NSCLC were obtained, containing 14 targets of active components from HYR-2 (which were significantly enriched in the PD-L1 related signaling pathway). In vivo and in vitro experiments showed that HYR and HYR-2 could inhibit the growth of lung cancer and down-regulate the expression of PD-L1, which might be related to the blocking effect of HYR-2 on the PI3K/Akt signaling pathway. Furthermore, HYR-2 promoted the transformation of M2 macrophages into M1 macrophages as well. It is deserved to be mentioned that the level of Akkermansia muciniphila was also significantly elevated by HYR-2, which was believed to enhance the therapeutic effect of PD-L1 antibodies. To sum up, HYR-2 might play an anti-lung cancer effect by down-regulating PD-L1 together with up-regulating Akkermansia muciniphila.
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PubMed
高影响因子
CATALYSIS LETTERS
·
2020
·Vol. 150
·期 9
·2703-2708
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IF 2.482
Zhao Zhaohui,Wang Yanhua
Abstract Thermoregulated phase-transfer Pd nanocatalyst was firstly employed in the selective hydrogenation of 1,5-cyclooctadiene (1,5-COD) at atmospheric hydrogen pressure. Under the optimal conditions, > 99% conversion and 95% selectivity to cyclooctene (COE) were obtained. The Pd nanocatalyst can be easily separated from products and directly reused. The turnover frequency (TOF) of 1411 h −1 is the highest value ever reported among Pd nanocatalysts at atmospheric hydrogen pressure. Graphic Abstract
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ENERGY & FUELS
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2020
·
IF 3.421
Jun Hu,Mingxing Zhao,Bingxing Jiang,Shiliang Wu,Ping Lu
Direct hydrogenolysis of native lignin in biomass into monomeric phenols has received increasing attention. In this work, catalytic transfer hydrogenolysis of native lignin from birch, pine, and corn stalk was studied over a Ni–Pd bimetallic catalyst using isopropanol as the in situ hydrogen source. The bimetallic Ni50Pd50/SBA-15 exhibited higher activity than the monometallic counterparts in catalytic transfer hydrogenolysis of native birch lignin, affording 37.2 wt % monophenols at 245 °C after 4 h. 4-Propylsyringol had the highest yield of 18.9 wt % with a selectivity of 51%. Among the three biomass feedstocks, native lignin in birch gave the highest monophenol yield, which is 2.2 times that of native pine lignin (16.9 wt %) and 4.6 times that of native corn stalk lignin (8.1 wt %). FTIR and Py–GC MS analyses of the starting biomasses and the depolymerization solid products revealed that native birch lignin has the highest depolymerization efficiency with the least active lignin remaining.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Ningning Wang,Yaxin Zhou,Yuwen Xu,Xiaomeng Ren,Shiyao Zhou,Qi Shang,Yue Jiang,Yuxia Luan
Immune checkpoint blockade (ICB) strategy based on suppressing programmed death-1 (PD-1)/programmed death-ligand 1 (PD-L1) pathway has been proved to be promising and effective in cancer immunotherapy. However, its potential risk of immune-related adverse events (irAEs) places stringent requirements on the precise loading of anti-PD-L1 agent in nanomedicine. Precise control of the loading content of anti-PD-L1 antibody is a difficult task since physical encapsulation has inevitable drawbacks like batch-to-bath variation and chemical modification is limited by the low stability of the antibody. Herein, we proposed a molecular engineering strategy to develop the nanomedicine with precise control of anti-PD-L1 agent content by using anti-PD-L1 peptide (APP) as the substitute to anti-PD-L1 antibody. The APP was chemically bonded with a photosensitizer IR780 to obtain IR780-M-APP, a molecule able to self-assemble into nanoparticles (NPs) with a precise APP loading (48.4 wt%) determined by the molecular structure. Specifically, the IR780 moiety in IR780-M-APP NPs endows the nanoparticles with photodynamic therapeutic effect as well as the ability to trigger immunogenic cell death (ICD), while the APP moiety can block the PD-1/PD-L1 pathway for promoting immunotherapy. The proposed photodynamic-immunotherapy nanoplatform not only killed primary tumors directly but also eradicated the metastatic and invasive tumors effectively. The present molecular engineering strategy combined with anti-PD-L1 peptide might provide more opportunities for the design of advanced nanoplatforms for cancer therapy.
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高影响因子
CATALYSIS COMMUNICATIONS
·
2020
·
IF 3.612
Baining Lin,Yuxin Zhang,Yifan Zhu,Yingping Zou,Yingjie Hu,Xuhong Du,Huasheng Xie,Kang Wang,Yonghua Zhou
Developing the highly active Pd catalyst via facile synthesis technique for alkenes hydrogenation is a long-term goal to pursuit. Here, Pd catalyst with phosphor-doped g-C 3 N 4 as support was fabricated by calcination and impregnation technique. XRD and XPS indicated that phosphor was doped into the framework of g-C 3 N 4 ,resulting in the highly dispersed Pd loaded thereon. The resultant Pd catalyst exhibited an unprecedentedly high activity for styrene hydrogenation of 856.89 mmol Styrene ·min −1 ·g Pd −1 and TOF value of 18,974 h −1 attributed to the enhanced Pd dispersion, more Pd 0 species and the intrinsic advantages of the support. This work provides a new avenue for the fabrication of highly effective Pd catalyst over alkenes hydrogenation.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
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2019
·
IF 4.527
Jinghao Wang,Sijing Bi,Yuancai Chen,Yongyou Hu
Gram-negative Citrobacter freundii with high Pd (II) reduction capacity was isolated from electroplating wastewater, and the electron transfer involved in Pd (II) bio-reduction by C. freundii JH was investigated in phosphate buffer saline solution with sodium formate as sole electron donor under anaerobic condition . FTIR spectra indicated that hydroxyl and amine groups on cell wall participated Pd (II) bio-sorption. TEM , XRD, XPS results confirmed that Pd (0) nanoparticles (NPs) could be bio-synthesized intra/extracellularly. Meanwhile, pH turn-over were observed owing to the reduction of cytochrome c (c-Cyt) in bio-reduction process. EPR spectra indicated that free radicals ( OH) was generated from high concentration Pd (II), which would cause seriously damage to cell. Despite of the lower tolerance to Pd (II), the cells at logarithmic phase exhibited higher Pd (II) reduction capacity (72.21%) than that at stationary phase (56.21%), which might be related to the relatively stronger proton motive force (PMF) created by the substrate oxidation and the electron transfer, as evidenced by electrochemical experiments (CV, DPV, amperometric I-t curves) and protein denaturalization experiments. Additionally, c-Cyt and riboflavin were confirmed to be important participants in electron transfer. Finally, a putative synthesis mechanism of Pd (0)-NPs was deduced. This study contributed to further understanding the electron transfer in Pd (II) reduction, and provided more information for the bio-synthetic of metal nanoparticles.
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高影响因子
Nanoscale
·
2019
·Vol. 12
·期 3
·2126-2132
·
IF 6.97
Hui Xu,Hongyuan Shang,Cheng Wang,Liujun Jin,Chunyan Chen,Yukou Du
Although great successes have been accomplished on the controlled synthesis of 2D and 3D Pd-containing nanomaterials, tapping into the novel Pd-containing electrocatalysts that combined the advantages of both 2D and 3D structures remains a significant challenge. Here, an approach to systematically produce porous Fe-doped Pd nanosheet assemblies (NSAs) with a geometry tuning from PdFe hollow nanospheres (HNSs), PdFe nanocages (NCs), to PdFe nanoplates (NPs) is reported. The inherent ultrathin and porous features endow these PdFe catalysts with excellent electrocatalytic performance. As a result, the optimized 3D PdFe NCs show a much-improved methanol oxidation reaction (MOR) and ethanol oxidation reaction (EOR) activities in comparison with PdFe HNSs, Pd NPs, and commercial Pd/C catalysts. Moreover, these PdFe nanocatalysts also display greatly enhanced electrocatalytic stability, which can endure 500 cycles with negligible activity loss and structural changes. The mechanism investigations reveal that the introduced Fe atom efficiently modulates the electronic structure of Pd, leading to the downshift of the d-band center of Pd, which is beneficial for the adsorption of reactants. Moreover, the porous nanosheet assembly structure can provide rich mass and electron transfer channels, further boosting the improvement of electrocatalytic performance.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2019
·
IF 5.107
Jian Lu,Yingying Qin,Chao Yu,Xinyu Lin,Minjia Meng,Yongsheng Yan,Hougang Fan,Yilin Wu,Chunxiang Li
Pd (II) from release-unbridled electroplating wastewater is causing great challenges, which is unfavourable either to human health or resource reutilization. Ion-imprinted membranes (IIMs) have recently drawn attentions for selective separation of specific ions from analogues. In this context, we have developed a facile strategy for fabrication of Pd (II)-imprinted membranes (Pd-IIMs) for the selective separation of Pd (II). The enhanced flux was obtained by three-dimensional macroporous structure on polydimethylsiloxane (PDMS). Then the Pd-IIMs were synthesized by a modification-imprinting strategy based on PDMS substrates. With the existence of Co (II), Cu (II), Cd (II) and Ni (II), the as-obtained Pd-IIMs showed superior adsorptive selectivity (3.32–5.06) and perm-selectivity (2.34–4.04) towards Pd (II), as well as the satisfactory regeneration performance (more than 92% of the initial rebinding capacities after 5 cycles of adsorption/desorption). Moreover, the as-prepared Pd-IIMs also displayed stability on separation factors even under ultrasonic treatment. Notably, the overused Pd-IIMs after applications for selective separation of Pd (II) showed a satisfactory performance for the treatment of methylene blue (99.87%), which displayed potentials for the “further applications”. The Pd-IIMs and preparation strategy developed in this work have shown a positive opportunity for the efficient treatment of electroplating wastewater and organic dyes.
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