JOURNAL OF MATERIALS SCIENCE
·
2022
·Vol. 58
·期 1
·170-185
·
IF 4.682
Zang Yu,Gao Shan,Jing Boyu,Sun Hong,Wang Jianjun,Liu Jiao,Miao Fengjuan,Xu Liang
Four kinds of conjugated microporous polymers (CMPs) with imine structures were synthesized by a Sonogashira coupling reaction followed by a postreaction between aldehydes and amines. Palladium nanoparticles (Pd NPs) were successfully supported on the CMPs to prepare Pd/CMP heterogeneous catalysts and were used to catalyze the Suzuki–Miyaura coupling reaction. The number of aromatic nuclei and nitrogen atoms in the CMPs highly affects Pd loading. In the Suzuki–Miyaura coupling reaction, the Pd/CMP with good Pd NPs dispersibility and appropriate Pd content (Pd/CMP-NA) exhibited the highest catalytic efficiency with 100% conversion and 95.4% yield which can be used for many substrates. The Pd/CMP-NA heterogeneous catalyst was easy to recover and still exhibited good catalytic efficiency after 5 cycles. To further understand the catalytic mechanism of Pd/CMP-NA on the Suzuki–Miyaura coupling reaction, we proposed a rational catalytic cycle. This paper provides an idea for the structural design of CMPs used for Suzuki–Miyaura catalytic reaction.
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International Journal of Minerals Metallurgy and Materials
·
2023
·Vol. 30
·期 5
·877-885
·
IF 4.8
Wang Junlian,Liu Lu,Xu Wen,Liu Hui,Xu Guodong,Huang Kun,Yu Fengshan,Huang Guoyong
Platinum group metals (PGMs), especially Pd, Pt, and Rh, have drawn great attention due to their unique features. Direct separation of Pd and Pt from highly acidic automobile catalyst leach liquors is disturbed by various factors. This work investigates the effect of various parameters including the acidity, extractant concentration, phase ratio A/O, and diluents on the Pd and Pt extraction and their stripping behaviors. The results show that the Pd and Pt are successfully separated from simulated leach liquor of spent automobile catalysts with monothio-Cyanex 272 and trioctylamine (TOA). Monothio-Cyanex 272 shows strong extractability and specific selectivity for Pd, and only one single stage is needed to recover more than 99.9% of Pd, leaving behind all the Pt, Rh, and base metals of Fe, Mg, Ce, Ni, Cu, and Co in the raffinate. The loaded Pd is efficiently stripped by acidic thiourea solutions. TOA shows strong extractability for Pt and Fe at acidity of 6 mol·L −1 HCl. More than 99.9% of Pt and all of the Fe are extracted into the organic phase after two stages of countercurrent extraction. Diluted HCl easily scrubs the loaded base metals (Fe, Cu, and Co). The loaded Pt is efficiently stripped by 1.0 mol·L −1 thiourea and 0.05–0.1 mol·L −1 NaOH solutions. Monothio-Cyanex 272 and TOA can realize the separation of Pd and Pt from highly acidic leach liquor of spent automobile catalysts.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Yaya Fang,Weiwei Lu,Peng Xu,Kaisheng Yao,Jun Zhang,Xuefeng Wei,Shuge Peng,Kunpeng Sun
In this work, we propose a plasmon-mediated method to activate oxygen for oxidizing benzyl alcohols to aldehydes. First, hollow Ag@Pd core–shell nanoparticles were prepared and characterized and afterward explored for selective oxidation of benzyl alcohols under visible light illumination. Then, electron paramagnetic resonance analysis and spectroscopic measurements suggested that the main active species responsible for the selective oxidation was 1O2, which was subsequently proved to be generated from the transformation of superoxide radicals •O2–. The light illumination and the presence of a Pd shell were the prerequisites for the successful generation of •O2– and 1O2. Furthermore, the wavelength-dependent performance of Ag@Pd verified the plasmon-mediated nature of these core–shell-type nanocatalysts. Finally, a plausible mechanism of plasmonic activation of oxygen and selective oxidation of benzyl alcohols on Ag@Pd was proposed. Our research opens a green and sustainable way to activate molecular O2 into 1O2 for selective oxidation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Kaiyang Xu,Yu Chen,Hua Yang,Yuyan Gan,Lizhi Wu,Li Tan,Yihu Dai,Yu Tang
Cyclohexanone is an important raw material for manufacturing nylon and other chemicals. The sustainable conversion of biomass derived molecules to cyclohexanone is desired but still challenging. Herein, a palladium single atom catalyst anchored in the micropores of zeolite (namely Pd 1 /ZSM-5) is designed and exhibits remarkable catalytic activity in transforming anisole to cyclohexanone in water medium (H 2 O), without using of organic solvent or halogen promoter. The selectivity to cyclohexanone is 91.2% and the turnover rate (TOR) is 400.8 h −1 at 453 K. The Pd sites, acid sites, and microporous confinement environment of zeolite cooperate to promote the partial hydrogenation to cyclohexanone, and inhibit further hydrogenation as the side reaction. H 2 O not only acts as the solvent, but also participates significantly in the partial hydrogenation. Moreover, as revealed by isotope labelled experiments (D 2 O and H 2 18 O), the water participated hydrogenolysis and the consequent partial hydrogenation mechanism is proposed.
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Journal of Pharmaceutical Analysis
·
2022
·
IF 14.026
Yinfei Chen,Shiyu Zhu,Jiayu Fu,Jianguo Lin,Yan Sun,Gaochao Lv,Minhao Xie,Tao Xu,Ling Qiu
Despite advances in immunotherapy for the treatment of cancers, not all patients can benefit from programmed cell death ligand 1 (PD-L1) immune checkpoint blockade therapy. Anti-PD-L1 therapeutic effects reportedly correlate with the PD-L1 expression level; hence, accurate detection of PD-L1 expression can guide immunotherapy to achieve better therapeutic effects. Therefore, based on the high affinity antibody Nb109, a new site-specifically radiolabeled tracer, 68 Ga-NODA-cysteine, aspartic acid, and valine (CDV)-Nb109, was designed and synthesized to accurately monitor PD-L1 expression. The tracer 68 Ga-NODA-CDV-Nb109 was obtained using a site-specific conjugation strategy with a radiochemical yield of about 95% and radiochemical purity of 97%. It showed high affinity for PD-L1 with a dissociation constant of 12.34 ± 1.65 nM. Both the cell uptake assay and positron emission tomography (PET) imaging revealed higher tracer uptake in PD-L1-positive A375-hPD-L1 and U87 tumor cells than in PD-L1-negative A375 tumor cells. Meanwhile, dynamic PET imaging of a NCI-H1299 xenograft indicated that doxorubicin could upregulate PD-L1 expression, allowing timely interventional immunotherapy. In conclusion, this tracer could sensitively and dynamically monitor changes in PD-L1 expression levels in different cancers and help screen patients who can benefit from anti-PD-L1 immunotherapy.
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PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Haichuan Zhang,Zede Yi,Shiyu Fu,Changzhi Li,Lucian A. Lucia,Qiying Liu
A rational design of the intrinsic lattice structure of catalysts is vitally important to address catalytic performance. Herein is reported a top-down synthesis for the fabrication of a bifunctional metallic catalyst. First, palladium nanocubes with (100) lattices planes were synthesized through a shape-control strategy; next, the as-synthesized Pd/Co-ZIF was used as a template for in - situ phase reconstruction by a spontaneous phase transformation process in the presence of H 4 SiW under solvothermal conditions. Ultimately, formation of 3D hierarchical flower-like bimetallic nitride nanosheets (SiW 12 @Pd/Co-ZIF-NS) were generated because of this process. The SiW 12 @Pd/Co-ZIF-NS catalyst not only displays excellent catalytic transfer hydrogenolysis for C-O bond cleavage of lignin dimeric substrates, but also maintains superior recycling durability due to an encapsulation phenomenon preventing aggregation. Finally, the resulting nanocomposites exhibit superior activity and good size selectivity toward catalytic transfer hydrogenolysis of the actual lignin substrates to produce a significant amount of low-molecular-weight aromatic compounds .
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Xiaolan Li,Yangqi Huang,Zhenyu Chen,Shuqi Hu,Jinliang Zhu,Panagiotis Tsiakaras,Pei Kang Shen
A series of tri-functional nanoflower (NF) catalysts with numerous nanodendrites (Pt 3 NiRh, Pt 3 NiRu, Pt 3 NiPd, Pt 3 Ni, and Pt 2 Ni 2 Rh NFs) were synthesized by introducing Rh, Ru, and Pd into Pt-Ni nanoflowers, aiming at accelerating the sluggish kinetics of oxygen reduction reaction (ORR), methanol oxidation reaction (MOR), and hydrogen evolution reaction (HER). The as-prepared catalysts displayed superior anti-poisoning ability and excellent activity due to uniform morphology and good dispersibility. Their electrochemical characterization revealed that the Pt 3 NiRh NFs showed the highest mass activity (2.17 A m g P G M - 1 ) and specific activity (3.13 mA cm -2 ) toward ORR, close to 9.9 and 4.6 times higher than the values measured on Pt/C (46.7 %). As for MOR, mass and specific activities of Pt 3 NiRh NFs were 1.88 A m g P G M - 1 and 2.62 mA cm -2 , far exceeding the values on commercial Pt/C. Moreover, HER activity of Pt 3 NiRh NFs outperformed commercial Pt/C. This work is valuable to develop promising multi-functional catalysts with enhanced activity and anti-poisoning ability.
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Polymers
·
2022
·Vol. 14
·期 21
·4647
·
IF 4.967
Hao-Kun Cai,Zhong-Yi Jiang,Siyuan Xu,Ying Xu,Ping Lu,Jian Dong
Hydrogen gas production can be produced from dimethylamine borane by the catalytic effect of metal nanoparticles. Past research efforts were heavily focused on dehydrogenation in organic solvents. In this study, hydrolysis of the borane in aqueous solutions was investigated, which bears two significant advantages: that two-thirds of the hydrogen generated originate from water and that the hydrogen storage materials are non-flammable. Polymer hydrogels serve as good carriers for metal particles as catalysts in aqueous solutions. Kinetic analysis of hydrogen production was performed for Ni/Pd bimetallic nanoclusters dispersed in a polymer hydrogel with a 3-D network structure. The reaction catalyzed by the bimetallic nanoclusters has an activation energy of only 34.95 kJ/mol, considerably lower than that by Ni or other metal catalysts reported. A significant synergistic effect was observed in the Ni/Pd bimetallic catalysts (Ni–Pd = 20/1) with a higher activity than Pd or Ni alone. This proves the alloy nature of the nanoparticles in the borane hydrolysis and the activation of water and borane by both metals to break the O–H and B–H bonds. The hydrogel with the Ni/Pd metal can be recycled with a much longer lifetime than all the previously prepared catalysts. The aqueous borane solutions with a polymer hydrogel can become a more sustainable hydrogen supplier for long-term use.Keywords:hydrogen production;hydrolysis;dimethylamine borane;polymer hydrogel;Ni/Pd alloy nanoparticles;mechanism
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yabing Gan,Guoxing Yin,Zhaomin Xu,Huyang Zhou,Ting Yu,Haitao Li,Peng Yin
Gold (Au) and palladium (Pd) species have been widely used in synthetic chemistry, biology, and environmental sciences, raising hard-to-ignore health and environment risks due to their potential toxicity. Herein, a novel dual-functional fluorescent probe was rationally designed and developed for simultaneous quantification and visualization of Au 3+ and Pd species in the environmental and biological systems. Significant fluorescence enhancement at 484 and 606 nm and color changes were observed upon addition of Au 3+ and Pd 0 with high sensitivity. The detection limit for Au 3+ and Pd 0 was as low as 68 nM and 7 nM, respectively. Combined with smartphone chromaticity and dual-channel fluorescence imaging analysis, this probe was successfully applied to the quantification and visualization of Au 3+ and Pd species in real water samples. Thus, simultaneous naked-eye visualization and quantification of Au 3+ and Pd 0 in real water samples was achieved using this probe. The probe was also successfully applied to fluorescence imaging of Au 3+ and Pd 0 in HeLa cells and zebrafish, promoting the monitor and understanding about gold and palladium species in environmental and biological systems.
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Advanced Science
·
2022
·Vol. 9
·期 27
·2202744
·
IF 17.521
Songtao Dong,Yuan Zhang,Xiangnan Guo,Chuang Zhang,Zhaomeng Wang,Jiang Yu,Yubo Liu,Chang Li,Yuting Hu,Bingjun Sun,Mengchi Sun,Haotian Zhang,Defang Ouyang,Zhonggui He,Yongjun Wang
Spatiotemporal delivery of nanoparticles (NPs) at the “cellular level” is critical for nanomedicine, which is expected to deliver as much cytotoxic drug into cancer cells as possible when NPs accumulate in tumors. However, macrophages and cancer-associated fibroblasts (CAFs) that are present within tumors limit the efficiency of spatiotemporal delivery. To overcome this limitation, glutathion pulse therapy is designed to promote reduction-sensitive Larotaxel (LTX) prodrug NPs to escape the phagocytosis of macrophages and penetrate through the stromal barrier established by CAFs in the murine triple negative breast cancer model. This therapy improves the penetration of NPs in tumor tissues as well as the accumulation of LTX in cancer cells, and remodels the immunosuppressive microenvironment to synergize PD-1 blockade therapy. More importantly, a method is established that can directly observe the biodistribution of NPs between different cells in vivo to accurately quantify the target drugs accumulated in these cells, thereby advancing the spatiotemporal delivery research of NPs at the “cellular level.”
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高影响因子
FUEL
·
2022
·
IF 8.035
Baicheng Feng,Zichen Zhang,Jiaqiang Wang,Donglin Yang,Qun Li,Yaping Liu,Hengjun Gai,Tingting Huang,Hongbing Song
The catalytic hydrogenation of carbon dioxide (CO 2 ) into formic acid is among the most important reactions to alleviate global warming and realize the carbon cycle. How to achieve rapid activation of CO 2 remains a challenge. In this work, we designed two novel hydrophobic poly(ionic liquid)s (PILs) with a good affinity for CO 2 . Since the abundant N atoms in the PILs can anchor palladium (Pd) nanoparticles, the designed catalyst can rapidly activate CO 2 and H 2 simultaneously, thus efficiently catalyzing the hydrogenation of CO 2 to formic acid under mild conditions. Due to the synergy from the bis(trifluoromethanesulfonyl)amide anion ([Tf 2 N − ]) with strong hydrophobicity and CO 2 affinity and trimethylamine (NEt 3 ) as a low dissociation energy alkaline additive, the resultant Pd/PIL-bip-Tf 2 N exhibited the best catalytic performance on the hydrogenation of CO 2 to formic acid. The TOF value reached 1,190 h −1 in the aqueous solution of NEt 3 at 100 °C, 1 h, and a total pressure of 4 MPa. The activation energy and dissociation energy during the catalytic process were calculated by DFT, indicating that the synergistic effect of NEt 3 is better than that of other alkaline additives. In addition, the catalytic activity of the catalyst remained stable after several cycling experiments. Based on the obtained results, we proposed a possible reaction pathway. Therefore, PILs have great potential as catalyst carrier material for CO 2 hydrogenation.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Xiaoying Qi,Xiang Gong,Na Ye,Zhao Jiang,Tao Fang
Direct methanol and formic acid fuel cells attracted extensive attention with high specific energy and low operating temperature. The efficient electrocatalyst was one of the important factors to limit their commercial applications. Here, the nitrides-modified Pd/C catalysts (Pd–NbN/C, Pd–Mo 2 N/C, Pd-VN/C and Pd-BN/C) were prepared using sodium citrate as a reducing agent in ethylene glycol solution. The mass activities followed the trend of Pd–NbN/C > Pd–Mo 2 N/C > Pd-VN/C > Pd-BN/C > Pd/C, where Pd–NbN/C exhibited the highest mass activity (4052.19 A g Pd −1 ) for MOR, 19.2 times that of the commercial Pd/C (210.53 A g Pd −1 ). Electrochemical measurements (LSV, Tafel, EIS, CA) indicated that the addition of nitrides increased the charge-transfer kinetics, reaction rate and CO tolerance of catalysts for MOR in alkaline media . The rate-determining step was CO ads oxidation process . Combined the structural analysis (HRTEM, XRD , XPS , ICP) with electrochemical results, the enhanced catalytic performance was ascribed to that higher ECSAs and the charge transfer between Pd and nitrides, leading to the negative shift of the d-band center towards the Fermi level . The linear correlations were found for the d-band center VS the mass activities and the onset potential of CO oxidation VS the d-band center, indicating that the activity and anti-CO poisoning ability could be enhanced by controlling the d-band structure of catalysts for MOR. Furthermore, the higher mass activity for FAOR in acidic media suggested that nitrides-modified Pd/C may be the promising bi-functional materials.
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