INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2018
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IF 3.141
Dongyue Zhao,Zhongnan Gao,Hui Xian,Lingli Xing,Yuexi Yang,Ye Tian,Tong Ding,Zheng Jiang,Jing Zhang,Lirong Zheng,Xingang Li
Herein, we report the function of Pd species in the Pd-added La0.7Sr0.3CoO3 perovskite for removal of NOx (NO+NO2) in the lean-burn NOx traps (LNT) process. The addition of Pd significantly improves the De-NOx activity of the perovskite-based catalysts. The Pd-supported catalyst has an excellent NOx removal efficiency of 90.4%, which is higher than the Pd-doped catalyst (74.4%) and pure La0.7Sr0.3CoO3 (51.6%). Our results show that the addition of Pd species enhances both the NOx desorption behaviors to regenerate the NOx storage sites and NOx reduction ability of the catalysts in the fuel-rich period, which induces the improved NOx trapping performance in the followed lean-burn period. These achievements result in the enhanced De-NOx activity of the Pd-added catalyst in the alternative NOx storage and reduction operations. Compared with the Pd-doped catalyst, the Pd-supported catalyst possesses the higher utilization efficiency of the Pd, thus exhibiting a higher catalytic activity.
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Journal of the Taiwan Institute of Chemical Engineers
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2018
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IF 3.849
Fengxia Wang,Xiaobo Niu,Wei Wang,Wangli Jing,Yulong Huang,Ji Zhang
A green innovation strategy is performed to synthesize palladium nanoparticles (Pd NPs) using Cynomorium songaricum polysaccharide (CSP). The structure and properties of the as-prepared Pd NPs are characterized by a set of techniques, including transmission election microscopy, X-ray photoelectron spectroscopy, powder X-ray diffraction and cyclic voltammetry. The results show that Pd NPs are well dispersed with a mean size of 4.2 nm. As-obtained Pd–CSP/C electrode exhibits good stability and anti-interference ability for glucose detection in electrochemical studies. It can completely cover the normal blood glucose concentration with high sensitivities of 17.7 µA mM −1 cm −2 , and excellent stability during long-term electrochemical detection. Compared with the commercial glucometer, the relative deviation of the measured samples was equal to 5.0%. Significantly, this study offers an environmental friendly polysaccharide way for fabricating nanomaterials, which would develop more nanomaterials for various application fields in future.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2017
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IF 2.843
Lei Yang,Yuzhuo Jin,Xiangchen Fang,Zhenmin Cheng,Zhiming Zhou
Magnetic core–shell structured Pd-based catalysts (Fe3O4@M/Pd, M = SiO2, AlOOH, TiO2, Cu3(BTC)2, and ZIF-8) were prepared and applied to semihydrogenation of phenylacetylene. The catalysts were characterized by various techniques, and it was found that the predominant chemical state of Pd species on the catalyst surface was PdO2, which was stable under the reaction condition (40 °C and 0.1 MPa H2). Among all the catalysts studied, Fe3O4@ZIF-8/Pd showed the highest selectivity to styrene, which was also superior to conventional catalysts such as Pd/C, Pd/Al2O3 and Lindlar catalyst. The high selectivity of Fe3O4@ZIF-8/Pd was mainly ascribed to the electronic effect between PdO2 and ZIF-8. Further investigation revealed that the phenylacetylene hydrogenation on Fe3O4@ZIF-8/Pd was solvent-dependent with the activity increasing with the solvent polarity. Among eight solvents tested, methanol was the most effective, with high and stable selectivity to styrene (around 92%) at complete conversion of phenylacetylene (≥99.5%) during five consecutive cycles.
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Scientific Reports
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2017
·Vol. 7
·期 1
·1-8
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IF 4.259
Yang Zi-Rui,Wang Shang-Qing,Wang Jing,Zhou Ai-Ju,Xu Chang-Wei
Carbon material containing nickel, nitrogen and sulfur (Ni-NSC) has been synthesized using metal-organic frameworks (MOFs) as precursor by annealing treatment with a size from 200 to 300 nm. Pd nanoparticles supported on the Ni-NSC (Pd/Ni-NSC) are used as electrocatalysts for ethanol oxidation in alkaline media. Due to the synergistic effect between Pd and Ni, S, N, free OH radicals can form on the surface of Ni, N and S atoms at lower potentials, which react with CH 3 CO intermediate species on the Pd surface to produce CH 3 COO − and release the active sites. On the other hand, the stronger binding force between Pd and co-doped N and S is responsible for enhancing dispersion and preventing agglomeration of the Pd nanoparticles. The Pd(20 wt%)/Ni-NSC shows better electrochemical performance of ethanol oxidation than the traditional commercial Pd(20 wt%)/C catalyst. Onset potential on the Pd(20 wt%)/Ni-NSC electrode is 36 mV more negative compared with that on the commercial Pd(20 wt%)/C electrode. The Pd(20 wt%)/Ni-NSC in this paper demonstrates to have excellent electrocatalytic properties and is considered as a promising catalyst in alkaline direct ethanol fuel cells.
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高影响因子
FUEL
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2022
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IF 8.035
Hua Yan,Xiaowei Liu,Junhong Zhou,Dawei Li,Xiaoye Yang,Yiming Gu,Hongjiu Su,Shudong Wang
The development of anthraquinone (AQ) hydrogenation catalysts with high activity and selectivity remains a challenge, but it is critical in industrial applications from both economic and environmental perspectives. In this work, an amine-modified catalyst, i.e., Pd/A/SiO 2 , was designed and synthesized via grafting 3-aminopropyltrimethoxysilane (APTMS) onto silica support and then loading Pd via the Shiff-base reaction. Multiple techniques were used to thoroughly characterize and analyze the catalysts' structural and electronic properties, such as transmission electron microscopy (TEM), H 2 temperature-programmed reduction (H 2 -TPR), and X-ray photoelectron spectroscopy (XPS), etc. The Pd particle size (3.86 nm) in Pd/A/SiO 2 was found to be very close to the reported optimal value, which balances well between the number of active sites and the required size for AQ adsorption; also, the residual carbon species from APTMS improves the hydrophobic properties of the support, which benefits AQ adsorption and anthrahydroquinone (AQH 2 ) desorption; and furthermore, the electron transferred from N to Pd increases the electron density of the latter, favoring the activation of the C O bond in AQ. These factors combine to give a very superior performance of Pd/A/SiO 2 for AQ hydrogenation, including a hydrogenation efficiency as high as 15.7 g/L with an intriguing selectivity of 96.1 %, and a good reusability merit within a six-run test, all of which are among the best results reported so far. This work, we believe, provides food for thought in the development of a highly efficient catalyst for AQ hydrogenation.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2023
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IF 8.2
Qiuyang Huang,Xiaoling Zang,Zhiwei Zhang,Hang Yu,Baoyan Ding,Zhuangzhuang Li,Simin Cheng,Xin Zhang,Mustafa R.K. Ali,Xue Qiu,Zhihua Lv
The discovery of new anti-cancer drugs targeting the PD-1/PD-L1 pathway has been a research hotspot in recent years. In this study, biological affinity ultrafiltration (BAU), UPLC-HRMS, molecular dynamic (MD) simulations and molecular docking methods were applied to search for endogenous active compounds that can inhibit the binding of PD-L1 to PD-1. We screened dozens of potential cancer related endogenous compounds. Surprisingly, cyclic adenosine monophosphate (cAMP) was found to have a direct inhibitory effect on the PD-1/PD-L1 binding with an in vitro IC 50 value of about 36.4 ± 9.3 μM determined by homogeneous time-resolved fluorescence (HTRF) assay. cAMP could recover the proliferation of Jurkat T cells co-cultured with DU-145 cells and may suppress PD-L1 expression of DU-145 cells. cAMP was demonstrated to bind and induce PD-L1 dimerization by FRET assay, and also predicted by MD simulations and molecular docking. The finding of cAMP as a potential inhibitor directly targeting the PD-1/PD-L1 interaction could advance our understanding of the activity of endogenous compounds regulating PD-L1.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
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2022
·Vol. 23
·期 22
·14072
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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
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Xiao-Chen Ma,Chun Pu,Yue-Xing Zhang,Gang-Gang Chang,Ge Tian,Si-Ming Wu,Jia-Wen Liu,Zhi-Yi Hu,Li-Ying Wang,Yi-Xia Yin,Christoph Janiak,Xiao-Yu Yang
Efficient regeneration of Pd catalysts is a challenge and has a very high technological importance. Herein, we report confined Pd clusters with the ultrafine size (1.2 nm) and ultralow loading amount (0.14 wt%) in a metal–organic framework (MOF), which could potentially allow for the successive realization of the cascade-type catalytic reaction from starting reagents to final desired products, and thus to avoid the excessive processes, save energy and reduce waste. Experiments and theoretical computations have been conducted to study the strong host–guest interaction between the Pd clusters and the MOF support, leading to the high catalytic activity and dynamic of the Pd clusters. A unique dynamic structure from active disordered arrangement to deactive crystalline arrangement and then back to the active disordered arrangement (>99% of activity after regeneration by simple H 2 reduction). The MOF-confined Pd shows excellent catalytic activity (>99% activity), selectivity (around 100%) and stability (>99% activity after recycling) under mild reaction conditions (atmospheric temperature and pressure).
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JOURNAL OF NANOBIOTECHNOLOGY
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2021
·Vol. 19
·期 1
·1-14
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IF 10.435
Guo Xiaoyang,Liu Jia,Jiang Lingdong,Gong Wanjun,Wu Huixia,He Qianjun
Background Photothermal therapy (PTT) frequently cause thermal resistance in tumor cells by inducing the heat shock response, limiting its therapeutic effect. Hydrogen sulfide (H2S) with appropriate concentration can reverse the Warburg effect in cancer cells. The combination of PTT with H2S gas therapy is expected to achieve synergistic tumor treatment.Methods Here, sulourea (Su) is developed as a thermosensitive/hydrolysable H2S donor to be loaded into Pd nanocubes through in-depth coordination for construction of the Pd-Su nanomedicine for the first time to achieve photo-controlled H2S release, realizing the effective combination of photothermal therapy and H2S gas therapy.Results The Pd-Su nanomedicine shows a high Su loading capacity (85 mg g−1), a high near-infrared (NIR) photothermal conversion efficiency (69.4%), and NIR-controlled H2S release by the photothermal-triggered hydrolysis of Su. The combination of photothermal heating and H2S produces a strong synergetic effect by H2S-induced inhibition of heat shock response, thereby effectively inhibiting tumor growth. Moreover, high intratumoral accumulation of the Pd-Su nanomedicine after intravenous injection also enables photothermal/photoacoustic dual-mode imaging-guided tumor treatment.Conclusion sThe proposed NIR-responsive heat/H2S release strategy provides a new approach for effective cancer therapy.Graphic abstract
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ACS Applied Nano Materials
·
2021
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IF 5.097
Haiping Li,Xue Wang,Yanan Liu,Yufei He,Junting Feng,Dianqing Li
The catalytic upgrading of phenolic derivatives is vital for the efficient utilization of biomass resources. Herein, we construct a reductive layered double oxide material (CoAlCe-LDO) with the Ce–Co interface and abundant oxygen vacancy (VO) via heat-treating layered double hydroxide (LDH) precursors. The support spontaneous in situ redox method is employed to prepare the supported catalyst using CoAlCe-LDO as a support and reductant. Interestingly, highly dispersed Pd nanoparticles prefer to distribute at the contact edge of the Ce–Co interface. Pd2+ is successfully reduced to Pd0 by the reductive Co/Ce sites. Due to the redox reaction between the support and Pd species, a strong metal–support interaction is introduced. The Pd/CoAlCe-LDO catalyst shows high activity for phenol hydrogenation under mild conditions and a low molar ratio of Pd to phenol. The kinetic study suggests that the highly dispersed Pd sites could preferably activate H2 molecules, thereby boosting the rapid phenol hydrogenation.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
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2021
·Vol. 22
·期 24
·13314
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IF 5.924
Feng Guo,Junfeng Ke,Zhengdong Fu,Wenzhao Han,Liping Wang
Cell penetrating peptides (CPPs) are peptides that can directly adapt to cell membranes and then permeate into cells. CPPs are usually covalently linked to the surface of nanocarriers to endow their permeability to the whole system. However, hybrids with lipids or polymers make the metabolism much more sophisticated and even more difficult to determine. In this study, we present a continuous sequence of 18 amino acids (FFAARTMIWY(d-P)GAWYKRI). It forms nanospheres around 170 nm, which increase slightly after loading with siRNA and DOX. Notably, it can be internalized by cancer cells mainly through electronic interactions and PD-L1-mediated endocytosis. Compared with poly-l-lysine and polyethyleneimine, it has a much higher efficiency (about four times) of gene transduction while lowering toxicity. In the treatment of cancer, it causes apoptosis (21%) and inhibits the expression of SURVIVIN protein in vitro. In vivo, it shows good biocompatibility as there are no changes in mice’s body weight. When administering peptide-siRNA-DOX, tumor growth is inhibited the most (about three times). These results above prove the sequence to be a good candidate for gene therapy and drug delivery.Keywords:peptide;self-assembly;gene therapy;PD-L1
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高影响因子
Nanomaterials
·
2021
·Vol. 11
·期 5
·1341
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IF 5.076
Qian Zhao,Decai Bu,Zhihui Li,Xiuling Zhang,Lanbo Di
Supported metal nanoparticles with small size and high dispersion can improve the performance of heterogeneous catalysts. To prepare graphene-supported Pd catalysts, graphene and PdCl2were used as support and Pd precursors, respectively. Pd/G-P and Pd/G-H catalysts were prepared by cold plasma and conventional thermal reduction, respectively, for the catalytic reduction of p-nitrophenol (4-NP). The reaction followed quasi-first-order kinetics, and the apparent rate constant of Pd/G-P and Pd/G-H was 0.0111 and 0.0042 s−1, respectively. The graphene support was exfoliated by thermal reduction and cold plasma, which benefits the 4-NP adsorption. Pd/G-P presented a higher performance because cold plasma promoted the migration of Pd species to the support outer surface. The Pd/C atomic ratio for Pd/G-P and Pd/G-H was 0.014 and 0.010, respectively. In addition, the Pd nanoparticles in Pd/G-P were smaller than those in Pd/G-H, which was beneficial for the catalytic reduction. The Pd/G-P sample presented abundant oxygen-containing functional groups, which anchored the metal nanoparticles and enhanced the metal-support interaction. This was further confirmed by the shift in the binding energy to a high value for Pd3d in Pd/G-P. The cold plasma method operated under atmospheric pressure is effective for the preparation of Pd/G catalysts with enhanced catalytic activity for 4-NP reduction.Keywords:cold plasma;Pd;graphene;reduction of 4-NP;catalytic hydrogenation
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