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
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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ACS Sustainable Chemistry & Engineering
·
2017
·
IF 5.951
Yafu Tang,Yuechao Yang,Dongdong Cheng,Bin Gao,Yongshan Wan,Yuncong C. Li
Soil, air, and water pollution caused by lignite is considered a serious environmental problem. Activation methods thus have been developed to extract humic acid from lignite to support the agricultural production as the soil amendment or fertilizer synergist. The traditional activation methods of humic acid from lignite, however, are not environmentally friendly. As the first study, this work developed a novel solid-phase activation method with a Pd/CeO2 nanocatalyst for lignite-derived humic acid. This study analyzed the morphology and structures of the as-synthesized Pd/CeO2 nanocatalyst with various characterization tools. The mechanisms of the Pd/CeO2 nanocatalyst for lignite activation were determined. The Pd/CeO2 catalyst effectively promoted the production of water-soluble humic acids from lignite via KOH solid-phase activation at room temperature. It increased the amount of small molecular active groups and the corresponding small molecules of humic acid. The existence of a strong synergistic effect at the interface sites between Pd/CeO2 nanoparticles and lignite was one of the key factors for the outstanding catalytic performance. In conclusion, this study has great application perspectives for reducing lignite pollution and increasing humic acid utilization by crops, which can improve the sustainability of the environment and agricultural systems.
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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
JOURNAL OF ALLOYS AND COMPOUNDS
·
2020
·
IF 4.65
Yingfang Zhu,Sihao Wang,Qingyu Luo,Haifu Huang,Shaolong Tang,Youwei Du
Developing electrocatalysts with high-Pt-utilization efficiency and appropriate surface oxygen affinity through a facile and scalable route is urgently needed for proton exchange membrane fuel cells. Here, SPD-annealing strategy is demonstrated to prepare ordered low-Pt-loading Pd–Pt–Fe nanoalloys with an average particle size of less than 5 nm and excellent electrocatalytic performance. Furthermore, the ORR performances of Pd–Pt–Fe/C nanoalloy catalysts are rationally modified by means of both precise composition control and structural transformation. With an optimal component proportion, the prepared Pd 0 . 75 Pt 0 . 25 Fe/C catalyst exhibits the most excellent intrinsic activity due to the synergistic interaction of lattice strain and ligand effect. Benefiting from the compressive strain effect induced by the relatively tight arrangement of the ordered structure, the adsorption energy of the intermediate oxygen-containing species is effectively weakened, enabling the Pd 0 . 75 Pt 0 . 25 Fe/C to obtain enhanced ORR catalytic performance in acidic condition. Notably, compared with the disordered Pd 0 . 75 Pt 0 . 25 Fe/C, the ordered Pd 0 . 75 Pt 0 . 25 Fe/C shows an extremely superior stability of 98.5% mass activity retention after 10 000 cycles. This work could provide a facile and versatile approach to constructing the ordered low-platinum electrocatalysts with enhanced ORR properties.
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JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Tian-Hong Jing,Kai-Chun Zhao,Guang-Hui Shi,Yi-Ying Zhuang,Xiao-Chao Chen,Xiao-Li Zhao,Yong Lu,Ye Liu
A series of bis-P,O-hybrid ligands ( L1–L4 ) were synthesized and characterized. The crystal structures demonstrated that the ligand of L2 , 1,4-bis((2-(diphenylphosphaneyl)phenoxy)methyl)benzene, not only acted as a typical trans -positioned diphosphine as observed in the complexes Pd( L2 )(OAc) 2 and Pd( L2 )Cl 2 , but also potentially as a P,P,O-tripodal pincer. As a result, under mild conditions (80 °C, 0.5–3.0 MPa), L2 enabled Pd(OAc) 2 to exhibit remarkable performance in terms of high activity and excellent regioselectivity ( l / b > 97/3) in the alkoxycarbonylation of vinyl arenes with the isolated yields of 57–91 %.
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高影响因子
Catalysts
·
2019
·Vol. 9
·期 12
·1061
·
IF 3.444
Zhenhua Dong,Pengwei Gao,Yongmei Xiao,Jing Chen,Wentao Wang
We reveal the Suzuki–Miyaura reaction catalyzed by a Pd–Co nanocatalyst supported by Mg–Fe–CHT (calcined hydrotalcites). A variety of boronic acids and aryl halides were transformed into functionalized biphenyls in excellent yields using water as a solvent. The reaction could proceed under mild conditions with a simple operation and high turnover numbers. The excellent catalytic activities are reasonably attributed to the Co-doping, which forms a Pd–Co alloy on the surface of CHT.Keywords:Suzuki–Miyaura reaction;water solvent;nanocatalyst;palladium;cobalt
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高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2022
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IF 4.598
Yuting Zhong,Zhirui Wu,Xiaoguang Liu,Ling Li
The combination of multi-metallic alloys and support materials is a promising approach for the design of electrocatalysts. In this study, Pd-M (M = Fe, Sb, Pb, Sn, Ag) bimetallic alloys embedded composites of 2D Ca-based metal–organic framework (Ca-MOF) nanosheets and reduced graphene oxide (rGO) were fabricated by a facile hydrothermal and impregnation reduction method, then applied as ethylene glycol oxidation reaction (EGOR) electrocatalysts. Remarkably, the forward peak current density of the best catalytic performer PdAg@rGO/Ca-MOF is as high as 258.30 mA cm −2 , which is 9.55 times greater than that of Pd/C. It also exhibits the biggest electrochemical active surface area of 3022.51 m 2 g −1 . After 3600 s chronoamperometry test, the retained current density of PdAg@rGO/Ca-MOF is about 87.94 % of the initial current density. These results imply that bimetallic Pd-M@rGO/Ca-MOF have superior electrocatalytic activity and anti-CO poisoning capacity compared to monometallic and Pd/C for EGOR, especially PdAg@rGO/Ca-MOF. The enhanced EGOR performance is due to the combined effect of Pd-M alloys and folded thin layer wrapped nanosheet rGO/Ca-MOF composites.
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高影响因子
JOURNAL OF CATALYSIS
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2021
·
IF 7.92
Jianguo Liu,Shanshan Lin,Jiangming Sun,Longlong Ma
Transition metal-catalyzed semi-hydrogenation of alkynes has become one of the most popular methods for alkene synthesis. Specifically, the noble metal Pd, Rh, and Ru-based heterogeneous catalysts have been widely studied and utilized in both academia and industry. But the supported noble metal catalysts are generally suffering from leaching or aggregation during harsh reaction conditions, which resulting low catalytic reactivity and stability. Herein, we reported the facile synthesis of nitrogen doped graphene encapsulated Pd catalyst and its application in the chemo-selective semi-hydrogenation of alkynes. The graphene layer served as “bulletproof” over the active Pd Nano metal species, which was confirmed by X-ray and TEM analysis, enhanced the catalytic stability during the reaction conditions. The optimized prepared Pd@N/C catalyst showed excellent efficiency in semi-hydrogenation of phenylacetylene and other types of alkynes with un-functionalized or functionalized substituents, including the hydrogenation sensitive functional groups (NO 2 , ester, and halogen).
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Qianqian Li,Hairong Yue,Changjun Liu,Kui Ma,Shan Zhong,Bin Liang,Siyang Tang
Transformation from photocatalytic oxidative dehydrogenation of ethane (PODHE) to photocatalytic dehydrogenation of ethane (PDHE) is an attractive process. A series of Pd/TiO 2 photocatalysts with different Pd loading amount were synthesized by photochemical deposition. And the Pd particle sizes varied from 1 nm to 4 nm. PDHE happened instead of POHDE over Pd particles smaller than 3 nm. The best PDHE performance (H 2 , 799.4; C 2 H 4 , 614.9, in micromoles per gram of catalyst) was obtained over 0.5 wt.% Pd/TiO 2 catalyst. And it was 3 times of it of PODHE over 1 wt.% Pd/TiO 2 . Reducing the Pd particle size of Pd/TiO 2 would increase Pd 0 /Pd 2+ and lower the valence band and conductive band of Pd/TiO 2 , which affect the catalytic behaviors. Detailed formation of products was investigated in this work.
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RSC Advances
·
2016
·Vol. 6
·期 106
·104398-104406
·
IF 3.289
Cong Zhang,Jingbo Qi,Jing Xing,Si-Fu Tang,Liang Song,Yuanyuan Sun,Chuanhui Zhang,Hongchuan Xin,Xuebing Li
Aqueous phase catalytic upgrading of lignin monomers to hydrocarbons via hydrodeoxygenation (HDO) has been explored using a combination of Pd/C and HZSM-5 catalysts under 2 MPa of H2 (ambient temperature). Model monomers with varying numbers of methoxy groups, including phenol, anisole, guaiacol and 2,6-dimethoxy-phenol, were chosen as lignin model compounds. Mechanistic studies revealed cascade and parallel reaction pathways via hydrogenation and dehydration (hydrolysis) processes, which were catalyzed by Pd/C and HZSM-5, respectively. Hydrogenation was preferred at lower temperature, whereas higher temperature was favorable for the removal of oxygen-containing functional groups. The effect of methoxy groups on the HDO of these monomers was also investigated systematically. Basically, the conversion of multi-substituted monomers was tougher than that of mono-substituted ones, due to steric constraint and the inhibition of the electron-donating hydroxyl group. The selectivities to cyclohexane from phenol and anisole were improved significantly by increasing the temperature to 413 K. However, cyclohexanone was preferably produced over cyclohexane when using model compounds with multi-substituents (guaiacol and 2,6-dimethoxy-phenol), even at temperatures above 513 K. Comparative experiments were also conducted on the HDO of 1,2-cyclohexanediol with or without the presence of phenol, which clearly suggested that the further HDO of guaiacol and 2,6-dimethoxy-phenol was inhibited, probably due to the strong interactions between cyclohexanediol molecules and Brønsted acid sites.
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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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高影响因子
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