JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Hao Lei,Qibo Zhang
Construction of strong metal-support interaction (SMSI) is of fundamental interest in the preparation of supported metal nanoparticle catalysts with enhanced catalytic activity. Herein, we report a facile in situ electrochemical redox tuning approach to build strong interactions between metals and supports. As for a typical example, a composite electrocatalyst of Pd-Co hybrid nanoparticles directly developed on Ni substrate is found to follow a distinct surface self-reconstruction process in alkaline media via an in situ electrochemical redox procedure, which results in structural transition from the original nanoparticles (NPs) to nanosheets (NSs) coupled with a phase transformation of the Co component, Co → CoO/Co(OH) 2 . The SMSI is observed in the electrochemically tuned Pd-Co hybrid system and leads to significantly enhanced catalytic activity for methanol oxidation reaction (MOR) due to the modified atomic/electronic structure, increased surface area, and more exposed electroactive sites. Compared with commercial Pd/C catalyst, the electrochemically tuned Pd-Co hybrid catalyst with SMSI exhibits superior catalytic activity (2330 mA∙mg Pd −1 ) and much better stability (remains 503 mA∙mg Pd −1 after 1000 cycles and 172 mA∙mg Pd −1 after 5000 s), and therefore has great potential in practical applications.
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高影响因子
BIOELECTROCHEMISTRY
·
2020
·
IF 4.722
Qingshan Yang,Ping Wang,Enhui Ma,Haoxuan Yu,Kaiwei Zhou,Chunyuan Tang,Jie Ren,Yueyun Li,Qing Liu,Yunhui Dong
In this work, a sandwich-type electrochemical immunosensor was fabricated to the effective detection of hepatitis B surface antigen (HBsAg). The designed electrochemical immunosensor was based on Au core and Pd shell nanodendrites loaded on amino functionalized molybdenum dioxide nanosheets (Au@Pd NDS/NH 2 –MoO 2 NSs) as the secondary antibody (Ab 2 ) label and silver nanoparticles were loaded by electrodeposited (D-Ag NPs) on the surface of electrode as the platform. Because of the synergistic effect and abundant catalytic activity sites provided by surface dendrite structure, Au@Pd NDs were more effective than single gold and palladium nanoparticles in catalytic reduction of hydrogen peroxide (H 2 O 2 ). MoO 2 had the good catalytic capacity for reduction of H 2 O 2 and favourable electrical conductivity . Hence, the obtained Au@Pd NDS/NH 2 –MoO 2 NSs were more effective than Au@Pd NDs and NH 2 –MoO 2 NSs in catalytic reduction of hydrogen peroxide attribute to a synergistic effect. Also, Ag NPs with admirable electrical conductivity and biocompatibility were used as sensing platforms and primary antibodies (Ab 1 ) carriers, which can accelerate the electron transfer and improve the sensitivity of the immunosensor. Here, the proposed electrochemical immunosensor offered a wide linear interval from 10 fg mL −1 to 100 ng mL −1 and the lower limit of detection of 3.3 fg mL −1 (S/N = 3) for detection of HBsAg under optimal experimental conditions. Furthermore, the accuracy of the actual serum sample analysis was satisfactory, which showed that the electrochemical immunosensor possessed a good application prospect in clinical detection.
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APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Fangke Zhan,Juanjuan Yin,Anqi Zhang,Jingxin Zhou,Mingli Wang,Tifeng Jiao
A seed-mediated co-reduction (SMCR) method that is simple to operate and produces heterogeneous components by the simultaneous co-reduction strategy to grow crystal was used to prepare a bimetallic nanomaterial, composed of two components of uniform metal elements. In this work, three different cationic surfactants were studied to control the morphology of bimetallic compound materials: cetyltrimethylammonium bromide (CTAB), cetyltrimethylammonium chloride (CTAC), and cetylpyridinium bromide (C16Py). Three mature and stable palladium crystal particles and the same number of Pd–Cu bimetallic nanomaterials (BNMs) products were obtained. The system of Pd and Cu bimetallic components, which has a large lattice mismatch, was grown uniformly by atomic layer-by-layer deposition under the SMCR method. The experimental results of BNMs for two nitro compounds (2-NA and 4-NP) were obtained by UV–vis spectral characterization. The prepared BNMs showed excellent catalytic ability in the reduction reaction and completed the catalytic reaction within 93 s. After eight consecutive catalytic cycles, the conversion of the catalytic reaction reached more than 90%. A set of surface-enhanced Raman scattering (SERS) experiments were also used to test the Raman enhancement properties of these BNMs, demonstrating a good SERS enhancement effect and good uniformity. These research results provide a new research topic for the exploration of morphology-controlled bimetal nanomaterials.
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CHEMICAL PHYSICS LETTERS
·
2020
·
IF 2.029
Chunhui Yue,Pan Yang,Jingchuan Wang,Xiaochong Zhao,Yuqi Wang,Lijun Yang
Development of low-cost and high-efficiency catalysts for hydrogen generation represents the significant challenge for realizing hydrogen economy. NiCo and nano-Pd loaded NiCo microfibers with high surface area has been successfully developed by electrospinning and following vacuum thermal treatment. Towards hydrogen generation, the catalyst exhibits efficient TOF as high as 350 and 680 mL min −1 gcat −1 for NiCo and nano-Pd loaded NiCo microfibers, providing superior performance compared with the most promising reported catalysts. The excellent catalytic activity remain above 90% confirming the remarkable durability. The insights uncovered here inspire and guide the rational design of advanced catalysts for the rapidly developing hydrogen energy applications.
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APPLIED CATALYSIS A-GENERAL
·
2020
·
IF 5.006
Peng Zhang,Ziyan Wang,Yan Zhang,Jian Wang,Wenqing Li,Lina Li,Peiping Zhang,Cundi Wei,Shiding Miao
In this work a Pd/Fe-Co-Ni layered double hydroxide (LDH) composite was prepared and investigated in the semi-hydrogenation of 2-methyl-3-butyn-2-ol (MBY). Hollow nanocages of ternary Fe-Co-Ni LDH were constructed by stacking the LDH nanosheets edge-to-face which inherited the rhombic dodecahedral structure of ZIF-67 templates. Uniform palladium (Pd) nanocrystals with cubic shapes were imbedded in the LDH nanocages via a solvothermal method. The hydroxyl groups on LDH supports were critical to inhibit the association of excess hydrogen atoms on the catalyst, so less MBY molecules were converted to 2-methyl-2-butanol (MBA) during the hydrogenation catalysis. Under optimized reaction conditions the hydrogenation activity of Pd/Fe-Co-Ni LDH was significantly improved, and the conversion of MBY was higher than 99% with selectivity of 2-methyl-3-buten-2-ol (MBE) exceeding 99%. The catalyst was easily recovered and had little reduction in catalytic performance during the cycling reactions.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Ming Lei,Zhiying Wang,Yao Tang,Huimin Wang,Lihua Zhu,Heqing Tang
The use of palladium deposited TiO 2 (Pd/TiO 2 ) as catalysts yielded complete debromination of 2,2′,4,4′-tetrabromodiphenyl ether (BDE47) in isopropanol solution containing NaOH at 40 °C within 60 min. The final organic products were diphenyl ether and dibenzofuran. It was disclosed that two competing reduction paths (hydro-debromination and coupling-debromination) occurred over Pd nanoparticles . The hydro-debromination was dependent on the participation of active H atom species generated by catalytic transfer hydrogenation on metallic Pd. The coupling-debromination proceeded via the oxidative addition of Pd(0) to B r 2 C 12 H 8 OB r 2 ′ , leading to an transition state of B r 2 Pd II C 12 H 8 OB r 2 ′ , the reductive dissociation of which resulted in the elimination of Br − ions, producing a new transition state Pd 0 C 12 H 8 OB r 2 ′ − . A further oxidative addition of Pd 0 C 12 H 8 OB r 2 ′ − generated B r 2 ′ Pd II C 12 H 8 O − , and its final reductive elimination provided dibenzofuran, leading to the regeneration of Pd(0). The integration of the catalytic coupling and hydrogenation reaction on Pd nanoparticles greatly accelerated the removal of the halogenated organic pollutants.
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APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Jin-Tao Du,Meng Qiao,Yuan Pu,Jie-Xin Wang,Jian-Feng Chen
The reduction of nitroarenes is usually catalyzed by heterogeneous catalysts. In this work, highly stable aqueous dispersions of monodisperse Pt, Pd, and Au nanoparticles stabilized by thermosensitive polymer, poly(N-isopropylacrylamide) (PNIPAM), are conveniently synthesized with the average sizes of 2.3, 3.1, and 2.3 nm, respectively. The modulation of the hydrophilic-hydrophobic nano-environments of the catalysts can be selectively provided by utilizing the temperature-responsive characteristics of PNIPAM. They are effective and thermosensitive pseudohomogeneous catalysts for nitroarenes reduction. The decreasing trend of catalytic activity is as follows: PNIPAM-Au > PNIPAM-Pd > PNIPAM-Pt. The catalytic reduction of nitrobenzene (NB), 4-nitrophenol (4-NP), and o-nitroaniline (o-NA) follow the pseudo-first-order kinetics, and the catalytic rates can be tuned by utilizing their temperature-responsive behavior. PNIPAM-Au nanocatalysts exhibit high turnover frequencies (TOF) up to 84, 12.9, and 40 min −1 for catalytic reduction of NB, 4-NP, and o-NA at 20 °C, respectively, which are one of the highest values ever reported.
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Applied Nanoscience
·
2021
·Vol. 13
·期 2
·1495-1506
·
IF 3.674
Zhang Xian-bing,Hu Ya-ping,Yang Wei,Feng Ming-bao
For the efficient disposal of organic pollutants and Escherichia coli ( E. coli ) in water, Ag-loaded and Pd-loaded ZnO nanofibers (NFs) were prepared through electrospinning (e-spin), followed by the alcohol-thermal method. The NFs were prepared in membrane form to promote their separation, recovery, and reuse in practical applications. The complete decolorizations of three types of dyes (i.e., azo, triarylmethane, and heterocyclic dyes) were observed when the Ag-loaded or Pd-loaded ZnO nanofiber membrane (NFM) was first applied as photocatalyst under 30-min UV irradiation. The characterization of the catalysts and the decolorization performance of dyes both demonstrated that the optimal loading rates of Ag and Pd were 12% and 6%, respectively. Moreover, the 12%-Ag/ZnO NFM displayed excellent recyclability over five cycles than the 6%-Pd/ZnO NFM. The E. coli disinfection test demonstrated that the photocatalytic inactivation rates with the 12%-Pd/ZnO NFM and the 6%-Ag/ZnO NFM were significantly improved under solar or UV irradiation, and hydroxyl radicals (∙OH) was primarily responsible for the antibacterial performance. Therefore, the presented 12%-Ag/ZnO NFM and 6%-Pd/ZnO NFM can be used for the efficient photocatalytic treatment of dyes and E. coli in water.
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ENERGY
·
2021
·
IF 7.147
Xiuquan Li,Zhongqing Yang,Li Zhang,Ziqiang He,Ruiming Fang,Ziqi Wang,Yunfei Yan,Jingyu Ran
The catalytic reaction of C 2 H 6 with CO 2 provides an opportunity to use shale gas and the greenhouse gas as source materials to produce ethylene through oxidative dehydrogenation or produce syngas through dry reforming . In this work, the reaction characteristics of ethane with CO 2 on Fe/Co/Ni/Cu monometallic catalysts and Pd-doped bimetallic catalysts were studied through activity test, kinetic analysis , catalyst characterization and DFT calculation. It is found that Pd–Fe 6 /CeO 2 has a high and stable C 2 H 4 selectivity of 80.4%, which is suitable for oxidative dehydrogenation reaction, while Ni 6 /CeO 2 has a large ethane/CO 2 conversion and a high CO selectivity of 96.5%, which is suitable for dry reforming reaction. For Fe-based catalyst, the doping of Pd form double active component structure. It only reduces the energy barrier of ethylene formation and CO 2 direct activation to provide O∗, but also increases the energy barrier of ethylene deep dehydrogenation, thus increasing the conversion of reactants and selectivity of C 2 H 4 . For Ni-based catalysts, the doping of Pd forms the alloy structure, which reduces the energy barrier of O∗-assisted dehydrogenation reaction and increases the conversion of reactants, but increases the energy barrier of C–C bond cleavage and CO 2 activation reaction, which reduces the selectivity of reforming to syngas.
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JOURNAL OF POROUS MATERIALS
·
2021
·Vol. 28
·期 6
·1737-1747
·
IF 2.496
Jiang Haoxi,Zhao Yingying,Lin Jing,Chen Yifei,Wang Sheng
Highly dispersed palladium nanoparticles (NPs) supported on UiO-66 as catalyst for CO 2 methanation were prepared by supercritical fluid deposition (SFD). As a result, the most suitable Pd precursor salt and co-solvent are Na 2 PdCl 4 and ethanol/DMF, respectively. The best SFD process condition to deposit the Pd precursor on UiO-66 is 40 °C, 10 MPa and 2 h. Under the above condition, 4% Pd/UiO-66 exhibits the highest activity with 53% of CO 2 conversion and 95% of CH 4 selectivity while the turnover frequency (TOF) value is 3669.4 h −1 . The catalysts were characterized by XRD, BET, TEM, XPS, TGA, CO-DRIFTS and ICP-OES to investigate the structure–activity relationship. The 4% Pd/UiO-66 with the average size of 2.2 nm of Pd prepared in assistance of supercritical fluid behaved the similar activity as the 6%Pd/UiO-66 with average size of 9.7 nm of Pd prepared by sol–gel method. It is showed prospect of technique for reducing noble metal loading resulting from high dispersion effect.
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BIOORGANIC CHEMISTRY
·
2021
·
IF 5.275
Gaochao Lv,Yinxing Miao,Yinfei Chen,Chunmei Lu,Xiuting Wang,Minhao Xie,Ling Qiu,Jianguo Lin
Programmed death ligand 1 (PD-L1) expression level is a reproducible biomarker for guiding stratification of patients to immunotherapy. However, the most widely used immunohistochemistry method is incompetent to fully understand the PD-L1 expression level in the whole body because of the highly complex PD-L1 expression in the tumor microenvironment. In this work, a novel small-molecular radiotracer [ 18 F]LG-1 based on the biphenyl active structure was developed to evaluate PD-L1 expression in tumors. [ 18 F]LG-1 was obtained by conjugating and radiolabeling with [ 18 F]FDG with high radiochemical purity (>98.0%) and high molar activity (37.2 ± 2.9 MBq/nmol). In vitro experimental results showed that [ 18 F]LG-1 could target PD-L1 in tumor cells and the cellular uptake in A375-hPD-L1 cells (PD-L1 + ) was clearly higher than that in A375 cells (PD-L1-). In vivo dynamic PET images of [ 18 F]LG-1 provided clear visualization of A375-hPD-L1 tumor with high tumor-to-background contrast, and the tumor uptake was determined to be 3.98 ± 0.21 %ID/g at 60 min, which was 2.6-fold higher than that of A375 tumor. These results suggested that [ 18 F]LG-1 had great potential as a promising PD-L1 radiotracer.
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ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Jiahui Kang,Jiahui Chen,Jiali Sheng,Jinqi Xie,Xian-Zhu Fu,Rong Sun,Ching-Ping Wong
To meet the ever-growing clean energy technology, developing effective catalysts for the oxygen evolution reaction (OER) is imperative for boosting the efficiency of electrochemical water splitting. This work reports Pd nanoparticle-interspersed nickel cobalt hydroxide carbonate nanothorn-coated copper hydroxide nanotube arrays grown on a copper foam (CH@NCHC NT-Pd/CF) as highly efficient OER electrocatalytic electrodes. The nanothorns and open-structured nanotubes have large surface areas and plenty of active sites. Particularly, the interfacial interaction between Pd nanoparticles and NCHC nanothorns causes charge transfer and redistribution, which are highly beneficial to promoting OER. The unique 3D integrated construction also can accelerate the electron and mass transfer and improve structural stability. Owing to the above merits, CH@NCHC NT-Pd/CF shows excellent OER electrocatalytic activity and stability in alkaline solution, delivering a current density of 100 mA cm–2 at a low overpotential of 207 mV and small voltage fluctuation in 12 h of electrolysis.
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