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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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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CATALYSIS LETTERS
·
2018
·Vol. 148
·期 9
·2799-2811
·
IF 2.911
Huang Qifu,Li Wenzhi,Lei Yanyan,Guan Shengnan,Zheng Xusheng,Pan Yang,Wen Wu,Zhu Junfa,Zhang Haitao,Lin Qizhao
Abstract In this work, NiCo 2 O 4 with a hierarchical porous flower-like structure was fabricated and used as catalyst support for Pd nanoparticles. The NiCo 2 O 4 was composed of porous nanoplates without overlapping, and the Pd nanoparticles were uniformly distributed on these nanoplates. Pd–NiCo 2 O 4 with the Pd loading of 2.0 wt% showed extremely high activity and stability, methane (1.0% CH 4 /Air) can be totally oxidized at 330 °C and the T 90 is 309 °C, which is much lower than that of pure NiCo 2 O 4 (T 90 = 405 °C). At wet condition with the presence of 10 vol% water vapor, the catalytic activity was still acceptable with the T 90 of 366 °C, and no activity decrease or permanent damage for the catalyst was observed after 35 h reaction, showing high stability. A series of techniques including TEM, SEM, XRD, H 2 -TPR, BET and especially quasi in situ XPS combined with in situ MS were used to characterize the catalysts and investigate the catalysis mechanism. Two pathways of CHO evolution were proved by the quasi in situ XPS and in situ MS results: OCHO intermediate dehydrogenation pathway at lower temperature and CO oxidation pathway of CHO at higher temperature. Graphical Abstract
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ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Dongxing Tan,Jianling Zhang,Jinbiao Shi,Shaopeng Li,Bingxing Zhang,Xiuniang Tan,Fanyu Zhang,Lifei Liu,Dan Shao,Buxing Han
To develop photocatalysts with desirable compositions and structures for improving the efficiency and selectivity of CO2 conversion to CH4 under mild conditions is of great importance. Here, we design an effective photocatalyst of bimetal (Ag/Pd) nanoalloys supported on nitrogen-doped TiO2 nanosheet for CO2 conversion. Such a novel photocatalyst combines multiple advantages of abundant Ti3+ ions, oxygen vacancies, and substitutional nitrogen that are favorable for catalyzing CO2 reduction. It was found that CO2 could be efficiently transformed to CH4 under mild conditions, i.e., in aqueous solution and at atmospheric pressure and room temperature. The maximum production rate of CH4 can reach 79.0 μmol g–1 h–1. Moreover, the Ag/Pd bimetals supported on N-doped TiO2 nanosheet exhibit high selectivity to CH4. The as-synthesized photocatalyst can be well recycled for CO2 reduction.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
·
IF 3.141
Yunpeng Zhou,Yangqiang Huang,Bo Jin,Xiao Luo,Zhiwu Liang
Pd nanoclusters supported on Schiff base modifying graphitic carbon nitride (Pd/u-CN100) had been successfully synthesized using urea and terephthalaldehyde as precursors by an impregnation approach. The resulting sheet materials exhibited high catalytic activity that turnover frequency rose to 98.9 h–1 and stability in CO2 hydrogenation. Various factors affecting formate production including the addition amount of TPAL, reaction pressure, reaction temperature, and catalyst stability testing were studied to achieve favorable catalytic conversion. An amount of characterization methods were applied to investigate the structure–activity relationship, including TEM, XRD, XPS, FTIR, HETEM, EDS, and BET. The high activity and stability might be resulted from the electronic modification, the relatively high dispersion of noble metal nanoclusters and the formation of intensely anchored metal-carrier bonds. More concretely, the scattered Schiff base loci and multiple nitrogen species were of great significance in the efficient and durable CO2 hydrogenation system.
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CATALYSIS TODAY
·
2018
·
IF 4.667
Lingcong Li,Xiaojun Liu,Hong He,Ningqiang Zhang,Ziwen Liu,Guizhen Zhang
The MgO-doped hexagonal boron nitride (MgO-h-BN) nanomaterials were designed as a support for Palladium (Pd) catalysts for CO oxidation reaction. The catalytic properties of Pd/MgO(5)-h-BN catalyst was investigated and compared with Pd/h-BN catalyst. Transmission electron microscopy (TEM) results suggested that the PdO nanoparticles with small grain sizes (ca. 8 nm) were effectively dispersed on the surface of MgO, and the MgO were deposited on the h-BN nanosheets in the Pd/MgO(5)-h-BN catalyst. X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) analyses revealed that a small amount of Mg 2+ embedded into the B vacancies of h-BN nanosheets in the Pd/MgO(5)-h-BN catalyst. More significantly, a large amount of adsorbed oxygen appeared near the B vacancies of Pd/MgO(5)-h-BN catalyst. The experiments outcomes of diffuse reflectance fourier transform spectra analysis of CO (CO-DRIFT) indicated that the carbonate/formate species were easily decomposed to CO 2 on the Pd/MgO(5)-h-BN catalyst than Pd/h-BN catalyst, which might be a reason why the Pd/MgO(5)-h-BN catalyst had high CO oxidation activity. According to above analyses, we provide a new insight for the MgO-h-BN nanomaterials for Pd catalysts for application in CO oxidation reaction.
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EUROPEAN JOURNAL OF PHARMACEUTICAL SCIENCES
·
2018
·
IF 3.466
Xian Tang,Jingdong Rao,Sheng Yin,Jiaojie Wei,Chunyu Xia,Man Li,Ling Mei,Zhirong Zhang,Qin He
The Cancer-Immunity Cycle is a series of anticancer immune responses initiated and allowed to proceed and expand iteratively. Paclitaxel (PTX) is a classic chemotherapeutic agent, which could induce immunogenic cell death (ICD) to trigger the Cancer-Immunity Cycle. However, the Cycle is severely impaired by tumor cell immunosuppression of host T cell antitumor activity through the programmed cell death receptor 1 (PD-1) and programmed cell death ligand 1 (PD-L1) (PD-1/PD-L1) immune checkpoint pathway. Here, we demonstrated that PTX mediated the Cancer-Immunity Cycle could be enhanced by PD-L1 knockdown (KD) and followed mTOR pathway inhibition in tumor cells. PD-L1 siRNA (siP) and the hydrophobic chemotherapy drug PTX were co-delivered with a rationally designed hybrid micelle (HM). We showed clear evidence that the HM-siP/PTX is capable of delivering siP and PTX simultaneously to the B16F10 cells both in vitro and in vivo . We demonstrated that HM-PTX/siP reduced the expression of PD-L1 and p-S6K (a marker of mTOR pathway activation) both in vitro and in melanoma-bearing mice and attenuated synergistically tumor growth by chemical toxicity , promoting cytotoxic T-cell immunity and suppressing the mTOR pathway.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2014
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IF 2.235
Miao Liang,Rongxin Su,Wei Qi,Yi Zhang,Renliang Huang,Yanjun Yu,Libing Wang,Zhimin He
Efficient immobilization of catalytic active metal nanoparticles into porous supporting materials is of important scientific interest in practice. We report on the fabrication of novel bionanocomposites, comprising a three-dimensional porous eggshell membrane (ESM) bioscaffold decorated with catalytic active metal (Pt, Pd) nanoparticles, to reduce highly toxic Cr(VI). Procyanidin (Pro), a natural plant polyphenol with abundant phenolic hydroxyls, was first covalently grafted on the ESM fiber surface to provide stable binding sites for chelating metal precursors. Highly dispersed Pt and Pd nanoparticles with small size were facilely generated and stably immobilized onto the surface of ESM followed by NaBH4 reduction. These metal nanoparticle-incorporating ESM composites were active heterogeneous catalysts for the reduction of toxic Cr(VI) to Cr(III) by employing formic acid as the reducing agent. Notably, it is easy to recover and recycle the catalysts, revealing the good stabilization of procyanidin-grafted ESM for nanoparticles.
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ACS Applied Materials & Interfaces
·
2014
·
IF 5.9
Long Zhang,Lianhuan Du,Xiang Yu,Shaozao Tan,Xiang Cai,Peihua Yang,Yu Gu,Wenjie Mai
Electron–hole recombination is one of the major factors limiting the efficiency of ZnO-based photocatalysts. In this work, a 2-fold enhancement strategy was employed to suppress electron–hole recombination and boost photocatalytic efficiency. First, significantly enhanced photocatalytic activity of ZnO by introducing graphene oxide (GO) was systematically investigated. Hybrid photocatalysts with different weight ratios of ZnO to GO (from 0.95:0.05 to 0.70:0.30) were synthesized and characterized. The results indicated that when the proportion ratio of ZnO to GO reached 0.85:0.15, the as-synthesized ZnO–GO nanocomposite exhibited the maximum photocatalytic efficiency on methylene blue with an apparent rate constant κapp almost 10 times faster than that of pure ZnO under UV illumination. GO was suggested to enhance the photocatalytic activity of ZnO because of its great capability in dye adsorption and charge separation. Second, Pd nanoparticles were introduced to decorate ZnO–GO to produce generally better photocatalyst ZnO–GO–Pd nanocomposites. The junction between Pd and ZnO was believed to also effectively separate the photogenerated charges due to the metal-semiconductor diode effect. These two systems of ZnO–GO and ZnO–GO–Pd nanocomposites are expected to have a broad range of applications in environmental conservation.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2015
·
IF 3.564
Xiao-ning Ye,Qiang Lu,Wen-tao Li,Pan Gao,Bin Hu,Zhi-bo Zhang,Chang-qing Dong
A new technique was proposed to selectively produce nicotyrine, a valuable alkaloidal product, from catalytic fast pyrolysis of tobacco mixed with the Pd/C catalyst. Pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) experiments were performed to investigate the effects of pyrolysis temperature and catalyst-to-tobacco ratio on the selective nicotyrine production. The actual nicotyrine yields under different reaction conditions were quantitatively determined. Moreover, the catalytic activity of the Pd/C catalyst was compared with those of the activated carbon (AC), Ru/C and Pd/SBA-15 catalysts. The results indicated that during the catalytic fast pyrolysis process, the Pd/C catalyst possessed promising dehydrogenation capability to selectively convert the nicotine in tobacco into the nicotyrine, and it performed much better than the other three catalysts. The maximal nicotyrine yield reached as high as 2.80 wt%, obtained at the pyrolysis temperature of 400 °C and catalyst-to-tobacco ratio of 2.
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Catalysis Science & Technology
·
2015
·Vol. 6
·期 6
·1913-1920
·
IF 5.426
Renfeng Nie,Hezhan Jiang,Xinhuan Lu,Dan Zhou,Qinghua Xia
N-doped active carbon (N-AC) has been synthesized via heat treatment of a mixture consisting of dicyandiamide as the nitrogen source and commercial active carbon as the precursor. This material is especially adapted for anchoring ultrafine Pd nanoparticles by a very clean strategy using H2 as the reductant. The physicochemical properties of materials were investigated by powder X-ray diffraction (XRD), Raman spectroscopy, Fourier transform infrared spectroscopy (FTIR), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). The results reveal that the variation of the treatment temperature can assist the tuning of the content of N and the dispersion of Pd on xN-AC, by which Pd nanoparticles with a narrow size distribution centered at around 1.8 nm can be obtained. These robust catalysts show very high catalytic activity for the aromatic ring hydrogenation of acidic substrates, such as electron-deficient benzoic acid or electron-rich phenol, under mild conditions in aqueous media. Excellent catalytic results (9.2 times higher activity in comparison to non-doped catalyst for benzoic acid hydrogenation), high stability and easy recyclability of the catalyst were achieved. The strong interaction between the pyridinic nitrogen group and Pd species will lower the reducibility of the Pd species and result in the formation of relatively electron-deficient and ultra-small sized Pd clusters, thus leading to high hydrogenation activity.
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Small
·
2015
·Vol. 11
·期 36
·4745-4752
·
IF 8.368
Yi Li,Wenxing Wang,Kaiyang Xia,Wenjun Zhang,Yingying Jiang,Yuewu Zeng,Hui Zhang,Chuanhong Jin,Ze Zhang,Deren Yang
Despite a few reports on the synthesis of ultrathin 2D nanosheets made of noble metals, it still remains a tremendous challenge to generate their ultrathin hollowed nanostructures, which are of particular interest in highly active catalysis due to their unique structural features. Here, the synthesis of ultrathin 2D Pd nanorings is reported with a hollow interior by selective epitaxial growth of Pd atoms on the periphery of the as-preformed Pd nanosheets in combination with oxidative etching. This approach can be extended to fabricate Pd-based bimetallic ultrathin nanorings such as Pd–Pt. The Pd nanorings exhibit substantially enhanced activity toward the hydrogenation of p -nitrophenol, which is 2.2 and 33.4 times higher than that of the Pd nanosheets and commercial Pd black, respectively. Significantly, the Pd nanorings are highly stable with only less than 11% loss in activity compared to 45.7% loss of the Pd nanosheets and 72.2% loss of the Pd black after ten cycles.
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