BIOORGANIC CHEMISTRY
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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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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Shuqian Xie,Lu Deng,Hui Huang,Jie Yuan,Jingkun Xu,Ruirui Yue
Herein, a ternary-nanocomposite Pd-polypyrrole/nitrogen-doped graphene (Pd-PPy/NGE) has been prepared facilely by the one-pot method. In simple terms, PPy was in-situ polymerized on the surface of NGE with PdCl 4 2- as the oxidant, and simultaneously Pd nanopaticles were loaded on the surface of PPy or embedded in PPy particles. The obtained Pd-PPy/NGE nanocomposite exhibits promising electrocatalytic properties toward the oxidation reaction of alcohols in alkaline medium. Especially, the optimized Pd-PPy/NGE (1:50) catalyst possesses mass activity of 2176.7, 1192.7 and 498.9 mA mg Pd -1 toward ethylene glycol , methanol and ethanol electrooxidation , respectively, which are 4.3, 6.7 and 2.9 times of those for commercial Pd/C catalyst. Moreover, the Pd-PPy/NGE (1:50) also shows higher anti-poisoning ability and operating stability than the Pd/C catalyst. The promising electrocatalytic performance of the Pd-PPy/NGE (1:50) for alcohols oxidation can be ascribed to the well dispersion of Pd nanoparticles , the porous and stable three dimentional structure of the composite, and the synergistic effect between different components. The structural randomness of the conducting polymer and the potential synergistic effect between the metal nanoparticles and various supports would provide broad development space for these composites as electrocatalysts in direct alcohol fuel cell .
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Zareen Zuhra,Shafqat Ali,Sajjad Ali,Hu Xu,Rongzhen Wu,Yuanyuan Tang
Designing materials for selective recovery of precious metals is a critical challenge in response to recent outbreaks of electronic wastes owing to economic and environmental concerns. We introduced high-performance hybrid materials (MCNTs) comprising of six-amino groups based on hexaaminobenzene metal-organic framework (HAB-MOF) and carbon nano-tube (CNT) sponge for selective recovery of Au(III) and Pd(II). Among all MOFs ever reported in the literature, the particular synthesized 30-MCNT (30 mg HAB-MOF on CNT sponge) exhibited the highest adsorption capacity ( q e ) of 1832 mg/g (45 °C, pH 3.0) for Au(III) and 1651 mg/g (45 °C, pH 1.0) for Pd(II), which can be regarded as a benchmark in the MOF family. The highly selective nature of 30-MCNT was examined in the presence of ten different metal ions and the results showed that the Au(III)/Pd(II) adsorption efficiency was decreased by only 5–10%. Moreover, the Au(III) and Pd(II) recovery was maintained ∼ 100% from the initial solution with metal concentration of 200 mg/L. The superior performance was mainly attributed to the role of abundant amino groups in the hybrid framework, developing several types of interactions with Au(III) and Pd(II) ions such as hydrogen bonding, electrostatic interactions, acid-base affinity and π-π inner sphere complexation. Furthermore, the remarkably high surface area and robust chemical and mechanical stability of CNT-sponge provided an exceptional support for impregnation of HAB-MOF to avail greater active sites and easier handpicked recycle. Density functional theory (DFT) simulation and X-ray photoelectron spectroscopy (XPS) studies were employed to explore the interaction mechanisms during the adsorption processes. Owing to facile and environment-friendly synthesis, excellent recovery and recycling, the material can be possibly considered for industrial application in precious metal recovery.
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Reaction Kinetics Mechanisms and Catalysis
·
2021
·Vol. 134
·期 2
·777-792
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IF 2.081
Liu Yingxin,Zhang Kaiyue,Zhang Liang,Wang Yun,Wei Zuojun
The selective reductive amination of levulinic acid (LA) into pyrrolidone derivatives is regarded as one of the most promising reactions in the fields of biomass conversion into high value-added chemicals. Herein, we report a one-pot synthesis of N -substituted-5-methyl-2-pyrrolidones by reductive amination of LA/ester with nitriles over several commercial catalysts. Among the catalysts texted, Pd/C was found to be the most efficient for the reductive amination of LA/ester with various nitriles to give high yields of pyrrolidones (up to 92%) under mild reaction conditions (80 °C, 1.6 MPa H 2 , tetrahydrofuran solvent). And the catalyst showed good reusability.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Yalin Yu,Zhihao Dong,Ling Tan,Nannan He,Rong Tang,Fang Jiang,Huan Chen
Diminishing the size of metal nanostructures can significantly improve the performance of catalysts. However, the self-aggregation of small particles is still an insurmountable obstacle, resulting in the unfavorable stability and recyclability. Herein, we designed and fabricated the Pd-CeO 2-x -NC catalyst though an accurate deposition strategy to downsize the Pd particle to sub-nanometer level and enhance its running stability. The CeO 2-x nanoclusters were firstly dispersed on the nitrogen-doped carbon nanosheets. Further, the active Pd sub-nanoclusters were accurately scattered on the surface of CeO 2-x ascribing to the strong metal-support interaction (SMSI) between Pd and CeO 2-x , which was beneficial to promote the catalytic activity. Subsequently, the high oxidation state Pd n + species were formed due to the electron transfer from Pd to CeO 2-x caused by the SMSI effect. Strikingly, the HER performance of Pd-CeO 2-x -NC was surprisingly correlated with the ratio of Pd n + , suggesting Pd n + acted as the dominant active species. Besides, the SMSI effect stabilized the valence state of active Pd n + species and prevented the sub-nanometer Pd clusters from aggregation, which played a vital role for the enhanced stability of the hybrid catalyst. This synthetic process described here is contributed to prepare various nanostructured catalysts with satisfactory stability through the direct targeting strategy.
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高影响因子
CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2021
·Vol. 37
·期 6
·1296-1300
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IF 1.307
Rong Xin,Lu Xiuli,Lu Tongbu
T he fabrication of highly active and easily recyclable Pd-based catalyst is meaningful for their practical application. Herein, a Pd-based dip-catalyst(Pd@Pyr-GDY) is fabricated on graphdiyne(Pyr-GDY) grown on copper foam, and applied in the reduction of nitroarenes. Specially, the as-formed Pd@Pyr-GDY shows good catalytic performance toward the reduction of 4-nitrophenol(4-NP) to 4-aminophenol(4-AP) by NaBH 4 with a rate constant k value of 3.84 min −1 , which is 12-fold higher than that of the commercial Pd/C. More importantly, Pd@Pyr-GDY could be easily and rapidly recovery from the reaction medium and no distinct inactivation was found after six cycles of the reaction. This work presents an easy way to design an efficient and easily recyclable Pd-based catalyst for practical use.
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高影响因子
JOURNAL OF POROUS MATERIALS
·
2021
·Vol. 28
·期 6
·1737-1747
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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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Green Energy & Environment
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2021
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IF 8.207
Jiaqin He,Dongyun Chen,Najun Li,Qingfeng Xu,Hua Li,Jinghui He,Jianmei Lu
Improving catalytic performance is a yet still challenge in thermal catalytic oxidation. Herein, uniform mesoporous MnO 2 nanosphere-supported bimetallic Pt–Pd nanoparticles were successfully fabricated via a SiO 2 template strategy for the total catalytic degradation of volatile organic compounds at low temperature. The introduction of mesopores into the MnO 2 support induces a large specific surface area and pore size, thus providing numerous accessible active sites and enhanced diffusion properties. Moreover, the addition of a secondary noble metal can adjust the O ads /O latt molar ratios, resulting in high catalytic activity. Among them, the catalyst having a Pt/Pd molar ratio of 7:3 exhibits optimized catalytic activity at a weight hourly space velocity of 36,000 mL g −1 h −1 , reaching 100% toluene oxidation at 175 °C with a lower activation energy (57.0 kJ mol −1 ) than the corresponding monometallic Pt or non-Pt-based catalysts (93.8 kJ mol −1 and 214.2 kJ mol −1 ). Our findings demonstrate that the uniform mesoporous MnO 2 nanosphere-supported bimetallic Pt–Pd nanoparticles catalyst is an effective candidate for application in elimination of toluene.
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Solar RRL
·
2021
·Vol. 5
·期 4
·2000813
·
IF 8.582
Di Li,Changjian Zhou,Zhongkai Xie,Donghai Chen,Yimeng Zhou,Xiangli Shi,Deli Jiang,Min Chen,Weidong Shi
Due to the low charge separation efficiency and high stability of the CO 2 molecule, photoreduction of CO 2 into a single multielectron product such as CH 4 with a simultaneous high conversion rate and selectivity is challenging. Therefore, it is highly desirable to accelerate charge separation and transfer and provide an electron-enriched catalyst surface for the deep reduction of CO 2 . Herein, a Pd/Cu 2 O/TiO 2 ternary hybrid photocatalyst consisting of Pd nanoparticles (NPs) and Cu 2 O NPs-decorated TiO 2 nanosheets is rationally designed, and highly selective photocatalytic photoreduction of CO 2 into CH 4 is achieved. The Pd/Cu 2 O/TiO 2 photocatalyst shows a high CH 4 production rate of 42.8 μmol g −1 h −1 with an extremely high selectivity of 99.5%. This CH 4 production rate is 61.1, 5.4, and 2.8 times higher than the bare TiO 2 , Cu 2 O/TiO 2 , and Pd/TiO 2 , respectively. In this Pd/Cu 2 O/TiO 2 hybrid, a consecutive multistep charge transfer is steered between the Cu 2 O/TiO 2 heterojunction and Pd, ensures accelerated charge separation and transfer, and leads to the formation of a spatially separated electron-enriched surface (Pd) and hole-enriched surface (Cu 2 O). This spatially oriented charge transfer and the charge-enriched catalyst surface synergistically contribute to the simultaneous high conversion rate and selectivity of CH 4 .
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高影响因子
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 CONTROLLED RELEASE
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2021
·
IF 9.776
Minglu Zhou,Chaohui Luo,Zhou Zhou,Lian Li,Yuan Huang
Triple negative breast cancer (TNBC) with highly metastatic features generally does not respond to anti–programmed cell death 1 ligand 1 (PD-L1) therapy due to multiple immunosuppressive mechanisms to exclude and disable T cells . Here, we develop a polymer-based combinatory approach consisting of both immunogenic cell death (ICD)-inducing and CXCR4-inhibiting function to prime tumor microenvironment and improve anti-PD-L1 therapy in TNBC. Our findings revealed that the combination therapy was able to spur the T cell response in primary tumors by increasing the tumor immunogenicity to recruit T cells, removing the physiological barriers of intratumoral fibrosis and collagen to increase T cell infiltration , and reducing the immunosuppressive cells to revive T cells. Meanwhile, such approach efficiently inhibited the formation of pre-metastatic niche in abscopal lung. Because of the significant promotion of anti-tumor and anti-metastasis immunity, the non-responding TNBC gained robust responsiveness to anti-PD-L1 therapy which resulted in complete eradication of orthotopic tumors, inhibition of pulmonary metastasis , and durable memory effects against tumor recurrence . Our work provided a generalizable approach of simultaneous ICD induction and CXCR4 blockade to apply anti-PD-L1 therapy in TNBC.
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高影响因子
JOURNAL OF WOOD CHEMISTRY AND TECHNOLOGY
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2021
·
IF 2.63
Dong Chen,Rongrong Miao,Liang He,Qingqing Guan
Ethyne is often an unwanted impurity in ethene streams used in plastics industry. Supported Pd catalysts offer high ethyne conversion, but poor ethene selectivity due to over-hydrogenation which leads to the formation of carbonaceous deposits. In this paper, acrylamide was grafted by free radical polymerization onto bagasse pith hemicellulose (to form HEMI-g-AAMs), which was then used as a porous bio-based carrier of Pd nanoparticles. The obtained Pd/HEMI-g-AAMs catalyst showed an ethyne conversion and ethene selectivity of 100% and 94.70%, respectively, at 100 °C and a space velocity of 70,000 h−1. The nitrogen-rich bio-based support regulated the physicochemical properties and catalytic activity of the supported Pd nanoparticles. Results guide the development of new and improved Pd-based catalysts for the partial catalytic hydrogenation of ethyne to ethene.
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