Environmental Science-Nano
·
2020
·Vol. 7
·期 5
·1566-1581
·
IF 7.683
Zimo Lou,Zheni Wang,Jiasheng Zhou,Chuchen Zhou,Jiang Xu,Xinhua Xu
Electrocatalytic hydrodechlorination (ECH) has been proposed as a potential technology for the effective degradation of organochlorine contaminants. In this study, a nanoscale Pd/TiC catalyst with low resistance was dip-coated onto Ti, aiming to fabricate a stable Pd/TiC/Ti electrode with enhanced ECH reactivity for efficient dechlorination. Electrochemical techniques indicated that the Pd/TiC/Ti electrode had a larger electrochemically active surface area and more rapid interfacial charge transfer than the conventional Pd/C/Ti electrode. In a batch experiment, the dechlorination rate for ECH of 2,4-dichlorobenzoic acid (2,4-DCBA, a model pollutant) by Pd/TiC/Ti was 1.3–14.5 times higher than those by Pd/C/Ti, Pd/MWCNTs/Ti, and Pd/MoS2/Ti, respectively. Scavenger experiments, ESR spin-trapping spectroscopy, and cyclic voltammetry clarified the intensified atomic H* generation by Pd/TiC/Ti. DFT calculations revealed that Pd/TiC/Ti had stronger binding ability with atomic H* (Eads: −2.89 eV vs. −2.44 eV) and 2,4-DCBA (Eads: −3.62 eV vs. −2.15 eV), respectively, when compared with Pd/C/Ti. As a result, enhanced generation of atomic H*, together with strengthened adsorption of atomic H* and 2,4-DCBA, would contribute to a faster ECH reaction. The Pd/TiC/Ti electrode retained its reactivity after 10 successive batch experiments (80 h), and showed high tolerance to the constituents in actual water matrices including lake water and river water. This study proposed a promising ECH electrode for the treatment of chlorinated organics in water matrices.
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DOI
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 92
·89157-89166
·
IF 3.289
Zhen Liu,Baoyang Lu,Yansha Gao,Taotao Yang,Ruirui Yue,Jingkun Xu,Lei Gao
In this study, bimetallic Pd–Au/PEDOT/graphene (Pd–Au/PEDOT/rGO) nanocomposites were facilely prepared in an aqueous medium by a one-pot method. In addition to the Pd–Au/PEDOT nanoparticles, dendritic bimetallic Pd–Au nanoclusters were also obtained in the composites, which were verified by transmission electron microscopy and element analysis mapping characterization. The morphology of the nanocomposites was greatly influenced by the molar ratio of the added metal salt precursors. X-ray photoelectron spectroscopy and X-ray diffraction analyses indicated the presence of synergism and electron exchange between the Pd–Au bimetallic nanostructures, which play an important role in the enhancement of the electrocatalytic activity of the composite toward the oxidation of caffeic acid (CA). Under optimized conditions, the Pd–Au/PEDOT/rGO modified glassy carbon electrode showed a wide linear range of 0.001–55 μM and a low detection limit of 0.37 nM (S/N = 3) for CA detection. These results provide valuable insight on the development of novel modified electrodes based on bimetallic graphene nanocomposites for high performance electrochemical sensors.
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高影响因子
Catalysis Science & Technology
·
2022
·Vol. 12
·期 8
·2519-2530
·
IF 6.177
Lixue Qi,Jiajun Dai,Yichen Liao,Jian Tian,Daohua Sun
The low olefin selectivity of Pd-based catalysts is a long-term challenge for the selective hydrogenation of 1,3-butadiene. Hybrid Pd/metal–organic framework (MOF) catalysts may help tackle this problem as they can stabilize Pd nanoparticles and regulate their electronic property. Herein, both surface-supported Pd/ZIF-67 and encapsulated Pd@ZIF-67 catalysts were prepared to explore the synergy between Pd and ZIF-67 and the structure–performance relationship of the catalysts. SEM and TEM reveal the different spatial positions of Pd on the two catalysts. Interestingly, encapsulated Pd@ZIF-67 shows excellent catalytic performance in the 40 h test, with a conversion of 100% and a butene selectivity of 98%, outperforming the surface-supported Pd/ZIF-67 catalyst. XPS, CO-IR and DFT calculations indicate that the encapsulated structure promotes the synergistic interaction between the ZIF-67 and Pd sites. Furthermore, in situ DRIFTS of 1-butene reveals that the enhanced synergistic interaction weakens the adsorption of 1-butene on the catalyst surface while inhibiting its isomerization and further hydrogenation. The presented strategy together with the mechanistic results clarify the relationship between the structure and the synergistic interaction and provide a promising approach for the application of synergistic interactions in hydrogenation catalysts.
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高影响因子
RARE METALS
·
2020
·Vol. 39
·期 12
·1473-1482
·
IF 2.161
Feng Shao-Ping,Huang Kun
Abstract Separation of palladium (Pd) and platinum (Pt) by solvent extraction is difficult because of their extremely similar physicochemical properties. Development of new extractants with a high extraction efficiency and excellent separation selectivity is the primary focus for enhancing the separation of Pd and Pt by solvent extraction. In this study, a new extractant, 2-((2-methoxyethyl)thio)-1H-benzimidazole (MOBI), which contains N, S, and O atoms, was synthesized and used to separate Pd(II) and Pt(IV) from a hydrochloric acid aqueous solution. The experimental results revealed that Pd(II) and Pt(IV) were effectively separated under the optimal conditions: MOBI concentration of 0.005 mol·L −1 , HCl concentration of 0.2 mol·L −1 , organic/aqueous (O/A) phase ratio of 1.0, and contact time of 15 min. The separation coefficient between Pd(II) and Pt(IV) was 1246.40, which indicates that MOBI has a higher selectivity for Pd(II) than Pt(IV). In addition, the mechanism of coordination between Pd(II) and MOBI was demonstrated through the slope method, Fourier transform infrared spectroscopy (FTIR), hydrogen-1 nuclear magnetic resonance spectroscopy ( 1 H NMR), and carbon-13 nuclear magnetic resonance spectroscopy ( 13 C NMR). The results revealed that MOBI could coordinate with Pd(II) via the N atom in the benzimidazole ring of MOBI molecules to form [Pd(MOBI) 2 Cl 2 ] (O) . Graphic abstract
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高影响因子
APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Zonggao Hu,Guoli Zhou,Li Xu,Jinghe Yang,Bing Zhang,Xu Xiang
The heterogeneous catalysts based on ternary Pd/CeO 2 -nitrogen-doped graphene (NG) were prepared and utilized for solvent-free aerobic oxidation of benzyl alcohol to benzaldehyde in the presence of green oxidant O 2 . Characterization results revealed that CeO 2 dramatically enhanced the dispersion of Pd nanoparticles, reduced their particle size and inhibited the Pd oxidation formation. With high lattice oxygen storage capability of CeO 2 , excellent electrical conductivity of NG and high catalytic activity of Pd, the ternary catalyst was designed by combining the complementary superiorities of these three components. The ternary composite Pd/5CeO 2 -NG exhibited significantly higher catalytic activity with turnover frequency (TOF) of 30.74 s −1 for solvent-free aerobic oxidation of benzyl alcohol compared with the corresponding binary composites including 5CeO 2 -NG, Pd/NG and Pd/CeO 2 , verifying the synergistic effect among Pd, CeO 2 and NG. The ternary composite was stable and could be recycled up to 6 times without remarkable loss in the activity and selectivity towards benzaldehyde. Owing to its excellent activity, high selectivity, and exceptional stability and recyclability, the Pd/CeO 2 -NG composite has great application potential in the fields of organic synthesis, electrochemical biosensors and fuel cells.
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高影响因子
Nanoscale Research Letters
·
2019
·Vol. 14
·期 1
·1-9
·
IF 3.159
Li Xiaoliang,Feng Jiangjiang,Sun Jia,Wang Zhe,Zhao Wei
TiO 2 (P25)-supported Au-Pd bimetal nanoparticles displayed excellent performance in the solvent-free benzyl alcohol catalytic oxidation. However, little research attention has been paid to investigate the effects of TiO 2 form on the catalytic activity of Au-Pd/TiO 2 . In the present research, rutile, brookite, and anatase TiO 2 were successfully synthesized and subsequently applied as the carrier to load Au-Pd nanoparticles by the deposition-precipitation method. The experimental results indicated that the benzyl alcohol conversion employing the rutile TiO 2 -supported Au-Pd catalyst is higher than the conversion of anatase and brookite TiO 2 -loaded Au-Pd catalysts. However, the Au-Pd/TiO 2 -rutile displayed the lowest and highest selectivity toward benzaldehyde and toluene, respectively. ICP-AES, XRD, XPS, and TEM were conducted to characterize these catalysts. The corresponding experimental results revealed that the excellent performance of Au-Pd/TiO 2 -rutile catalyst was attributed to both the smaller Au-Pd nanoparticle size distribution and the higher concentrations of O α and Pd 2+ species on the catalyst surface. In the recycle experiments, the Au-Pd/TiO 2 -rutile catalyst displayed lower reaction stability compared with the Au-Pd/TiO 2 -anatase and Au-Pd/TiO 2 -brookite, which might be due to the coverage of larger amount of aldehyde products on the surface.
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高影响因子
JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Fengxia Tong,Jing Wang,Min Lv,Xiaolei Bao,Wen Xie,Xizhuang Liang,Zhaoke Zheng
Hybrid plasmonic nanostructures exhibit strong interactions with incident light, providing new opportunities for activating the C–H bond in formic acid (HCOOH) for H 2 production. However, it remains a challenge to effectively exciting and extracting plasmonic energy into reactants. Herein, we report a facile strategy to boosting energy transfer by amplifying local electromagnetic field and elucidate plasmon-induced bond activation mechanism at single-particle level. Snowflake-like Pd-Au superstructures (Pd-Au SSs) were chemically synthesized through the selective growth of ordered perpendicular Pd nanoarrays on Au nanostars. Pd-Au SSs possess self-constructed hotspots and high surface-to-volume ratio, enabling efficient energy transfer. The obtained structures exhibited a turnover frequency (TOF) of 15,943 h −1 for H 2 production under plasmon excitation. Furthermore, in situ single-particle analysis showed that the photoluminescence (PL) density of individual Pd-Au SSs was reduced when immersed in HCOOH, which potentially implies that dehydrogenation process might involve indirect energy transfer through charge carriers and direct energy transfer by metal-adsorbate electronic states. Theoretical and experimental analyses revealed that the enhanced local electromagnetic field, which allows high rates of direct resonant transfer of charge from plasmonic nanostructures to the adsorbed molecules, makes significant contributions to C–H bond activation and H 2 production. This work not only provide valuable insights into plasmon-enhanced catalytic processes at single-particle level, but also establish a universal framework for designing novel high-performance multicomponent plasmonic nanostructures with precise geometries.
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产品关联
DOI
高影响因子
BIOMATERIALS
·
2025
·
IF 12.9
Rui Hu,Xin Jiang,Lijie Zhu,Rui Meng,Rongbo Yang,Wenjie Sun,Zhenzhou Zhao,Yuehua Lyu,Ruoyuan Huang,Fei Xue,Mengke Shi,Zaigang Zhou,Jianliang Shen,Congying Xie
Currently, certain lung cancer patients exhibit resistance to radiotherapy due to reduced DNA damage under hypoxic conditions and the cytoprotective and immune-resistance effect caused by increased programmed death ligand-1 (PD-L1) and Cyclooxygenase 2 (COX-2) expression after radiotherapy. At present, existing nanoparticles or drugs could hardly effectively, and easily address these obstacles faced by highly effective radiotherapy simultaneously, especially the simultaneous depression of PD-L1 and COX-2. In this study, it is newly proved that some typical nitric oxide (NO) gas donors could co-inhibit PD-L1 and COX-2 expression, revealing the possible not fully proven role of NO in reversing tumor immunotherapy resistance. Then, to realize selective NO generation in tumors, a simple tumor glutathione (GSH) responsive NO gas nanogenerator named SAB-NO nanoparticles was designed and prepared, which was composed of the NO donor Isoamyl Nitrite conjugated with serum albumin (SAB). By doing this, SAB-NO nanoparticles more effectively sensitized radiotherapy through breaking the cytoprotective effects faced by radiotherapy in vitro by generating more DNA damage through reversing tumor hypoxia and impairing the DNA damage repair process through decreasing PD-L1 expression. Then, the combination therapy of SAB-NO nanoparticles and radiotherapy effectively transformed cold tumors into hot ones through avoiding some potential immune-resistance effects induced by radiotherapy treatment alone through PD-L1 and COX-2 co-inhibition. In conclusion, the combined treatment of radiotherapy and SAB-NO nanoparticles finally almost completely suppressed the growth of lung tumors, revealing the novel role of NO donors in sensitizing tumor immunotherapy by avoiding the potential cytoprotective and immune-resistance effects.
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PubMed
高影响因子
CERAMICS INTERNATIONAL
·
2021
·
IF 4.527
Yi Wang,Jialiang Chen,Lan Wang,Hanqin Weng,Zhihao Wu,Limin Jiao,Yusa Muroya,Shinichi Yamashita,Sheng Cheng,Fuhai Li,Hongbing Chen,Wei Huang,Mingzhang Lin
The large-scale synthesis and the stabilization of noble metal nanocatalysts with ultrasmall sizes are crucial to their practical application. Herein, Pd, Au, and Pt nanoparticles (NPs) are in situ embedded on boron nitride nanosheets (BNNSs) via the reduction of precursor salts induced by 60 Co γ-irradiation, which is a mature technique widely used in industry. The reduction mechanism was elucidated by pulse radiolysis experiments. In comparison with other BN substrates like hexagonal BN ( h -BN), BNNSs had not only large surface area of 263 m 2 g −1 , but also abundant hydroxyl groups produced during the sonicated exfoliation, resulting in ultrasmall sizes, large loading amounts, and uniform distribution of the anchored NPs. The particle sizes of the loaded Pd, Au, and Pt NPs were measured to be 2.9, 3.1, and 3.0 nm, respectively. As a consequence, in the model reaction of 2-nitroaniline reduction, the Pd-, Au- and Pt-BNNSs composite nanocatalysts showed much higher catalytic activities than those composites loading the corresponding NPs on other BN substrates. Particularly, most of the 2-nitroaniline could be reduced within merely 40 s when using Pd-BNNSs as catalysts, performing a rate constant of 1.1 × 10 −1 s −1 . The number of hydroxyl groups on BNNSs support as well as the catalytic performance of the corresponding NPs-loaded BNNSs composites could be improved by extending the sonicated exfoliation time, because more NPs were loaded and the hydroxyl groups were also proved to play an important role in enhancing the catalytic activity. Moreover, Pd-BNNSs catalysts still displayed prominent activity even after five cycles owing to the high stability of BNNSs and their strong affinity for PdNPs. This work not only demonstrates BNNSs as ideal supports to load noble metal NPs for catalysis, but also reveals the feasibility to synthesize and in situ embed ultrasmall noble metal NPs on BNNSs via γ-irradiation.
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高影响因子
BIOSENSORS & BIOELECTRONICS
·
2019
·
IF 9.518
Malik Saddam Khan,Hafsa Ameer,Asghar Ali,Romana Manzoor,Lei Yang,Ruiqing Feng,Na Jiang,Qin Wei
Herein, a highly efficient electrochemiluminescence resonance energy transfer (ECL-RET) immunosensor was established for ultrasensitive insulin detection. Silver/silver orthophosphate/graphene oxide composites (Ag/Ag 3 PO 4 /GO) were prepared as sensing platform for capture-antibody (Ab 1 ) incubation. Ag 3 PO 4 is a novel ECL donor whose emission could be remarkably enhanced by the synergetic assistance of GO with Ag NPs. Notably, GO presented excellent electrical conductivity and ultrahigh specific surface area to improve the loading capacity Ab 1 and Ag 3 PO 4 , and Ag NPs with fine biocompatibility and catalytic property could immobilize Ab 1 via Ag–N bond and further hasten the electron transfer to catalyze the generation of SO 4 •− radicals for boosting the ECL emission of donor. To establish a new ECL-RET system, Pd@Au core-shell nanoflower was prepared as a suitable ECL acceptor which could immobilize the detection-antibody (Ab 2 ). Due to the fine spectral overlap , Pd@Au nanoflower could significantly quench the ECL emission of Ag 3 PO 4 , causing distinct decreases in ECL intensity. The proposed ECL-RET immunosensor exhibited sensitive response to insulin in a linear range of 0.0001–80 ng/mL with a low detection limit of 0.02 pg/mL ( S/N = 3), it not only provides a reliable tool for insulin detection in diagnostics of diabetes, but also lights up a new avenue for designing effective ECL-RET pairs in bioanalysis .
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高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Xiaoliang Li,Jiangjiang Feng,Michal Perdjon,Rena Oh,Wei Zhao,Xiaoyang Huang,Shusen Liu
Au-Pd bimetallic nanoparticles immobilized on series of CeO 2 supports with different morphologies, e.g. , rod, cube, and polyhedrons were prepared through the deposition-precipitation method with a consequent investigation on their catalytic performances for benzyl alcohol oxidation in the absence of solvent. The experimental results exhibited that the morphology of CeO 2 has a markedly impact on the catalytic performance of Au-Pd/CeO 2 . In which Au-Pd supported on CeO 2 rod could achieve higher benzyl alcohol conversion than that supported on CeO 2 polyhedrons and CeO 2 cube, however, CeO 2 cube supported Au-Pd showed the highest selectivity towards the production of benzaldehyde. ICP-AES, XRD, Raman, N 2 -BET, TEM, HAADF-STEM, and XPS were conducted to characterize the catalysts. The results revealed that the excellent behavior of Au-Pd/CeO 2 -rod in benzyl alcohol oxidation was closely related with the smaller size of CeO 2 particle, the higher concentration of oxygen defects in support and the higher number of Ce 3+ and Pd 2+ species on the catalyst surface. The present study on the morphologies of CeO 2 support in solvent-free benzyl alcohol oxidation would offer a notable approach for the future catalyst design.
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高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Ting Liu,Yinghui Sun,Bo Jiang,Wei Guo,Wei Qin,Yiming Xie,Bo Zhao,Liang Zhao,Zhiqiang Liang,Lin Jiang
The large amount of 4-nitrophenol (4-NP) wastewater produced by the chemical industry has received increased concern over the growing risk of environmental pollution. The ability to catalyze the reduction of highly concentrated 4-NP wastewater is highly desirable for the practical treatment of industrial wastewater, yet it remains a significant challenge. Herein, we report Pd nanoparticle-decorated 3D-printed hierarchically porous TiO2 scaffolds (Pd/TiO2 scaffolds) for the efficient reduction of highly concentrated 4-NP wastewater (2 g·L–1, ∼14.38 mM). The millimeter-sized interconnected channels in the scaffolds are conducive to rapid mass and ion transportation; meanwhile, the abundant micrometer- and nanometer-sized pores on the surface of the scaffolds offer adequate anchoring sites for Pd nanoparticles. The turnover frequency of the hierarchically porous Pd/TiO2 scaffold (16 layers) is up to 2.69 min–1, which is 1063 times higher than that of the Pd/TiO2-bulk material with the same size (0.00253 min–1). Importantly, no obvious deactivation of the catalytic activity is observed even after 20 cycles of catalytic reduction of 4-NP, showing excellent catalytic stability and reusability. Our strategy of loading the nanostructured catalyst on 3D-printable hierarchically porous structures put forward a flexible and versatile approach for boosting the catalytic performance of the catalysts, including catalytic activity, stability, and reusability, which can help promote their practical application in industry.
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高影响因子
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