MICROCHIMICA ACTA
·
2020
·Vol. 187
·期 8
·1-11
·
IF 6.232
Li Fang,Hu Yuting,Zhao Anqi,Xi Yachao,Li Zimu,He Jianbao
β -cyclodextrin-functionalized porous
Pd@Au nanostructures ( β -CD-Pd@Au) with intrinsic
and enhanced peroxidase-like activity were successfully synthesized by a two-step
method. The synthesized β -CD-Pd@Au can
efficiently catalyze the oxidation of various substrates, such as
3,3′,5,5′-tetramethylbenzidine (TMB), mixture of 4-amino antipyrine (4-AAP) and
3,5-dichloro-2-hydroxy acid sodium (DHBS) (4-AAP/DHBS), and mixture of 4-AAP and
N-Ethyl-N-(3-sulfopropyl)-3-methyl-aniline sodium salt (TOPS) (4-AAP/TOPS), by
H 2 O 2 to generate visual blue,
purple, and pink color, respectively. The UV-vis absorbance peak of the three β -CD-Pd@Au catalyzed the chromogenic reaction
system located at 650 nm, 510 nm, and 550 nm, respectively. The β -CD-Pd@Au-catalyzed
TMB-H 2 O 2 chromogenic reaction
exhibited higher absorbance intensity, catalytic efficiency, and color stability in
comparison to 4-AAP/DHBS-H 2 O 2 and
4-AAP/TOPS-H 2 O 2 chromogenic
reactions. The catalytic activity of β -CD-Pd@Au
was enhanced about 4-fold compared to that of Pd@Au in terms of
K cat for
H 2 O 2 . Using TMB as chromogenic
substrate, a colorimetric assay was fabricated for the determination of
H 2 O 2 with a detection limit of
2.78 μM (absorbance at 650 nm). The colorimetric determination of glucose with a
detection limit of 9.28 μM was further achieved by coupling with glucose oxidase
enzymatic reaction, indicating the versatility of the β -CD-Pd@Au-based detection strategy. A paper-based detection method
coupled with smartphone for fast visual and instrument-free detection of glucose was
further developed. Finally, the developed colorimetric assay and paper-based
detection method were successfully applied to the determination of glucose in human
serum sample.
Graphical abstract
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SENSORS AND ACTUATORS B-CHEMICAL
·
2020
·
IF 7.1
Yun-Zhi Dai,Shu-Yu Liang,Chao Lv,Gong Wang,Hong Xia,Tong Zhang,Hong-Bo Sun
Micro/nanoscale gas sensors attracted more attention because of their potential application in the emerging areas such as electronic capsules, wearable devices, and microdrone detectors. However, it is still a challenge to achieve micro/nanoscale sensors with controllable processing parameters of active components and fast response and recovery capability. Here, a flexible and high precision femtosecond laser direct-writing technology is selected to print various semiconductor metal oxides nanoparticles into microscale designable patterns with mask-free. And by using Pd-doped WO 3 • x H 2 O nanoparticles we have fabricated single Pd-WO 3 • x H 2 O microwire (SPWM) as gas sensors, which represented high sensitivity, faster response and recovery. Especially, for ammonia gas sensing the SPWM with pre-designed lengths can possess ultrafast response with response/recovery time of 1.4/3.3 s in 50 ppm NH 3 , or low limit-of-detection of 1 ppm at room temperature. This kind of micro-scale gas sensor is expected to be applied to human health monitoring, environmental air detection and other integrated intelligent devices.
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Catalysts
·
2020
·Vol. 10
·期 3
·303
·
IF 3.52
Yaodan Wang,Hongyan Pan,Qian Lin,Yongyong Shi,Jiesong Zhang
Hydrogen peroxide (H2O2), as a clean and green oxidant, is widely used in many fields. The direct synthesis of H2O2(DSHP) from H2and O2has attracted most research interest because it relates to a facile, environmentally friendly, and economic process. Yolk–shell Pd-M@HCS (hollow carbon sphere) (M = Co, Ni, Cu) nanocatalysts, in which the bimetal nanoparticle is the core and porous carbon works as the shell layer, are reported in this work. It was found that catalytic activities were enhanced because of the introduced M metals. Additionally, the different mass ratios of Pd to Co (mPd/mCo) were further investigated to improve the catalytic performance for the DSHP. When mPd/mCo was 4.4, the prepared Pd-Co@HCS-(4.4) catalyst, with an average Pd nanoparticle size of 7.30 nm, provided the highest H2O2selectivity of 87% and H2O2productivity of 1996 mmolgPd−1·h−1, which were increased by 24% and 253%, respectively, compared to Pd@HCS.Keywords:direct synthesis of hydrogen peroxide;Pd-based catalyst;yolk–shell structure
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ACS Omega
·
2020
·
IF 2.87
Yao Feng,Juanjuan Yin,Shufeng Liu,Yuying Wang,Bingfan Li,Tifeng Jiao
Poly(ethylene imine) (PEI) has abundant amino groups in a macromolecular chain and can be used as a graft source for metal nanocomposites, which shows excellent ability to form stable complexes with heavy metal ions. In this work, a simple and convenient method was used to make PEI into a stable hydrogel with 1-ethyl-3-(3-dimethylaminopropyl)carbodiimide-N-hydroxysuccinimide and subsequently coprecipitate with silver nitrate solution or palladium chloride solution to form metal-loaded composite hydrogels. In addition, the characterizations of composite hydrogels were investigated by scanning electron microscopy, specific surface area tests (Brunauer–Emmett–Teller), X-ray photoelectron spectroscopy, and ultraviolet spectroscopy. The properties of composite hydrogels on the catalytic reduction of 4-nitrophenol were studied. The results showed that the composite hydrogels could be easily separated from the water environment, which indicated the large-scale potential application in organic catalytic degradation and wastewater treatment.
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NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 7
·3087-3096
·
IF 3.288
Gang Li,Peng Sun,Fanggen Wu,Jie Zhao,Dongxue Han,Guofeng Cui
4-Aminophenol (4-AP) is a highly toxic environmental pollutant and contaminant of medicine, which is widely used in industries and daily life. Therefore, the development of a reliable sensor for determining the amount of 4-AP is of great importance for the protection of human and environmental health. Herein, by fabricating a Pd@CeO2 composite on a nanoporous gold-coated carbon fiber paper (NPG/CFP), the sensing properties for 4-AP can be largely enhanced. Combining the significant increase in the catalytic activity of the Pd@CeO2 composite (derived from the strong interactions between Pd and CeO2) with the NPG and NPG/CFP hierarchical porous structure having a high electrochemically active surface area, the electrode achieved excellent detection of 4-AP. It manifested an extremely high sensitivity of 75.4 μA μM−1 and 56.5 μA μM−1 in the concentration range from 0.005 μM to 0.03 μM and 0.03 μM to 9 μM, respectively. The detection limit reached as low as 4 nM under optimized conditions (S/N = 3). The electrode also possesses long-term stability and presents great anti-interference ability. All these results demonstrate that the electrode is a promising candidate for future sensors for monitoring 4-AP in water and pharmaceuticals.
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Biomaterials Science
·
2019
·Vol. 8
·期 5
·1418-1430
·
IF 5.251
Tiankuan Li,Zhongqian Hu,Chao Wang,Jian Yang,Chuhui Zeng,Rui Fan,Jinhe Guo
Immunotherapy is gradually becoming as important as traditional therapy in the treatment of cancer, but adverse drug reactions limit patient benefits from PD1/PD-L1 checkpoint inhibitor drugs in the treatment of non-small cell lung cancer (NSCLC). As a chemotherapeutic drug for NSCLC, docetaxel (DTX) can synergize with PD1/PD-L1 checkpoint inhibitors but increase haematoxicity and neurotoxicity. Herein, anti-PD-L1 monoclonal antibody (mAb)-conjugated and docetaxel-loaded multifunctional lipid-shelled microbubbles (PDMs), which were designed with biologically safe phospholipids to produce synergistic antitumour effects, reduced the incidence of side effects and promoted therapeutic effects under ultrasound (US) irradiation. The PDMs were prepared by the acoustic-vibration method and then conjugated with an anti-PD-L1 mAb. The material features of the microbubbles and their cytotoxic effects, cellular apoptosis and cell cycle inhibition were studied. A subcutaneous tumour model was established to test the drug concentration-dependent and antitumour effects of the PDMs combined with US irradiation, and an orthotopic lung tumour model simultaneously confirmed the antitumour effect of this synergistic treatment. The PDMs achieved higher cellular uptake than free DTX, especially when combined with US irradiation. The PDMs combined with US irradiation also induced an increased rate of cellular apoptosis and an elevated G2-M arrest rate in cancer cells, which was positively correlated with PD-L1 expression. An in vivo study showed that synergistic treatment had relatively strong effects on tumour growth inhibition, increased survival time and decreased adverse effect rates. Our study possibly provides a well-controlled design for immunotherapy and chemotherapy and has promising potential for clinical application in NSCLC treatment.
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JOURNAL OF CATALYSIS
·
2019
·
IF 7.723
Jiaxuan Fan,Lingxiang Cheng,Yanan Liu,Yufei He,Yanfei Wang,Dianqing Li,Junting Feng
Photocatalytic reduction of CO 2 with H 2 O into CH 4 is a promising way to realize solar energy utilization and CO 2 conversion, in which the key issue is how to enhance and couple CO 2 reduction as well as H 2 O oxidation. In this work, we precisely fabricated a binary functional photocatalyst by loading Au@Pd nanoparticles onto V O -rich TiO 2 through a surfactant-free deposition-reduction method, whose fine structure was confirmed by aberration-corrected HAADF-STEM, EELS, EPR and XPS. Combining photocatalytic performance with a series of in situ FTIR measurements, we clarified the role of metallic sites and semiconductor support in coupling CO 2 reduction and H 2 O oxidation. Specifically, H 2 O oxidation process was facilitated by the V O -rich TiO 2 to contribute more protons, followed by the activation of CO 2 and protons primarily by the metallic Au@Pd sites to form the surface bounded Au@Pd-CO 2 − and Au@Pd-H species. By adjusting the ratio of Au@Pd nanoparticles and V O concentration to manipulate the Au@Pd-CO 2 − /Au@Pd-H ratio, CH 4 yield of 26.32 μmol/(g·h) and selectivity of electron toward CH 4 of 96% can be observed with minimal concomitant H 2 generation. These findings could open a feasible and universal route to enhance the photocatalytic efficiency of CO 2 conversion.
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JOURNAL OF MOLECULAR LIQUIDS
·
2019
·
IF 4.561
Jiling Zhao,Chen Wang,Shixing Wang,Yang Zhou,Bing Zhang
Palladium wastewater is produced from various industrial activities and seriously pollutes the environment. In here, a new adsorbent (PMDA-PGMA) was manufactured by functionalizing poly(glycidyl methacrylate) microspheres with pyromellitic acid and introduced to recover Pd(II) from wastewater. The main influencing factors including pH, palladium ionic content, reaction time and temperature were evaluated. The selectivity , reusability and sorption mechanism have been systematically examined. The pH 2 was optimal for Pd(II) adsorption and only 300 min was required to reach maximum adsorption capacity about 206.71 mg/g. The experimental data were is in tune with pseudo-secondary kinetics and Langmuir model well. So, the Pd(II) adsorption process was monolayer chemical adsorption. Thermodynamic parameters indicate that Pd(II) adsorption on PMDA-PGMA was an endothermic reaction . The main adsorption mechanism is ion exchange, electrostatic attraction and coordination between palladium ions and pyromellitic acid groups. Additionally, PMDA-PGMA can be easily regenerated by 10% thiourea and can be recycled at least five times. PMDA-PGMA exhibited good selective extraction ability for Pd(II) and effectively separated Pd(II) (≥95%) from laboratory wastewater in the presence divers metal ions . Density functional theory calculations show that PMDA-PGMA combines with Pd(II) through monodentate N atoms and bidentate O groups. The application prospect of PMDA-PGMA is encouraging in removing palladium from wastewater due to its high adsorption capacity and better reusability.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2019
·Vol. 34
·期 2
·e5364
·
IF 3.259
Yizhu Lei,Wenchao Zhu,Yali Wan,Renshu Wang,Hailong Liu
Developing efficient and recyclable heterogeneous catalysts for organic reactions in water is important for the sustainable development of chemical industry. In this work, Pd nanoparticles supported on DABCO-functionalized porous organic polymer was successfully prepared through an easy copolymerization and successive immobilization method. Characterization results indicated that the prepared catalyst featured big surface area, hierarchical porous structure, and excellent surface amphiphilicity. We demonstrated the use of this amphiphilic catalyst in two case reactions, i.e. the aqueous hydrodechlorination and Suzuki-Miyaura coupling reactions. Under mild reaction conditions, the catalyst showed high catalytic activities for the two reactions. In addition, the catalyst could be easily recovered and reused for several times. Also, no obvious Pd leaching and aggregation of Pd nanoparticles occurred up during the consecutive reactions.
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HYDROMETALLURGY
·
2019
·
IF 3.465
Shunyan Ning,Shichang Zhang,Wei Zhang,Jie Zhou,Siyi Wang,Xinpeng Wang,Yuezhou Wei
The separation of fission products Ru, Rh, and Pd will benefit both the nuclear fuel cycle and enlarge the platinum group metals source. A silica-based iso Bu-BTP/SiO 2 -P adsorbent was used to separate Ru, Rh, and Pd from nitrate solution. It exhibited good adsorption towards Ru, Rh, and Pd with the uptake rates over 95% at 55 °C in 0.1 M HNO 3 –3 M NaNO 3 solution and no adsorption towards 238 U(VI). The adsorption towards Ru, Rh, and Pd matched well with pseudo-second-order model with the equilibrium obtained within 24 h, 24 h and 0.5 h and Langmuir adsorption isotherm model with the saturation adsorption amounts as high as 0.37 mmol/g, 0.34 mmol/g and 0.71 mmol/g respectively. The adsorbed Pd, Rh, and Ru can be desorbed by 0.1 M HNO 3 –0.1 M thiourea , 2 M HCl and NaClO solution (CP) which is expected to realize their mutual separation in desorption stage using the above-mentioned eluents successively. Both FT-IR and XPS revealed that C N C played key role during adsorption and the adsorption needed the participation of NO 3 − to keep charge balance. In a word, iso Bu-BTP/SiO 2 -P is a promising adsorbent for separation and recovery Ru, Rh, and Pd, especially in the case of separating them from other fission products and actinides from high level liquid waste .
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Yicheng Zhong,Yuelin Mao,Shunli Shi,Mingming Wan,Chong Ma,Shuhua Wang,Chao Chen,Dan Zhao,Ning Zhang
MNPs@MOF catalysts obtained by encapsulating metal nanoparticles (NPs) into metal–organic frameworks (MOFs) show fascinating performance in heterogeneous catalysis. The improvement of catalytic activity and reusability of MNPs@MOF catalysts has been a great challenge for a long time. Herein, we demonstrate well-designed Pd/MOFs, featuring hollow double-shell structure and magnetic property, exhibiting high reusability, efficient catalytic activity, and size selectivity for hydrogenation reaction. The as-synthesized Pd/MOF, denoted as Void nFe3O4@Pd/ZIF-8@ZIF-8, possesses diverse functional structural features. The hollow cavity can improve mass transfer; superparamagnetic Fe3O4 NPs embedded in the inner MOF shell can enhance the separation and recyclability; Pd NPs are highly dispersed in the matrix of the inner MOF shell, and the outer MOF shell acts as a protector to prevent the leaching of Pd NPs and a sieve to achieve size selectivity. As a proof of concept, the Void nFe3O4@Pd/ZIF-8@ZIF-8 catalyst exhibited excellent performance for the hydrogenation of styrene at room temperature. The activity only reduced 10% after 20 cycles for the higher conversions (>90%), and the lower conversion only decreased 3.6% (from 32.5 to 28.9% conversion) after twenty consecutive cycles, indicating the good and intrinsic reusability of the catalyst. The proposed structure in this work provides a strategy to effectively improve the reusability of MNPs@MOF catalysts, which would increase their practical applications.
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ENERGY & FUELS
·
2019
·
IF 3.021
Lingjun Ma,Caixia Yue,Liang Ye,Qihuang Huo,Lina Han,Liping Chang,Weiren Bao,Jiancheng Wang
Pd–Fe bimetallic sorbents were shown to be a great potential sorbent for Hg0 removal from coal-derived fuel gas. In this work, activated carbon (AC), Al2O3, and Beta molecular sieve were chosen as supports to disperse Pd–Fe bimetallic components. The effects of the supports on Hg0 removal of Pd–Fe bimetallic sorbents were evaluated using a fixed-bed reactor at 200 °C. The regeneration performance of sorbents was also investigated. The results showed that Hg0 removal activity and regeneration performance over Pd–Fe/AC was the best, followed by Pd–Fe/Beta, and Pd–Fe/Al2O3. The Hg0 removal efficiency of Pd–Fe/AC bimetallic sorbents remained above 80% within 400 min after regeneration 4 times. The Pd–Fe bimetallic sorbents were characterized by N2 adsorption–desorption, Fourier transform infrared spectroscopy, X-ray diffraction, CO pulse adsorption, Hg temperature-programmed thermal desorption, and X-ray photoelectron spectroscopy. The analysis results revealed that three sorbents had a similar Hg0 removal mechanism. Hg0 transformed to Pd–Hg amalgam and HgS after reacting with the sorbents. Pd0 and Fe2O3 were the active species for the removal of Hg0. The removal performance of Hg0 by Pd–Fe/Al2O3 sorbents was the lowest. It is because Pd–Fe/Al2O3 sorbents have the lowest specific surface area, surface content, and dispersion degree of the Pd component. Furthermore, Pd0 over Pd–Fe/Al2O3 sorbents was severely poisoned and transformed to PdS during the regeneration process.
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