ChemistryOpen
·
2022
·Vol. 11
·期 4
·e202100301
·
IF 2.63
Yin-Qing Yao,Kai-Chun Zhao,Yi-Ying Zhuang,Xiao-Chao Chen,Yong Lu,Ye Liu
Graphical The one-pot synthesis of 2,5-furandicarboxylic acid from 2-furoic acid was achieved for the first time using a Pd-catalyzed bromination-hydroxycarbonylation tandem reaction in HOAc-NaOAc buffer. The synthesis process provides major improvements compared to previously reported methods, namely using biomass-based 2-furoic acid as low-cost raw material, one-pot synthesis without isolation of intermediate product, and no need for an acidification procedure. The one-pot synthesis of 2,5-furandicarboxylic acid from 2-furoic acid with a yield of 57 % was achieved for the first time using a Pd-catalyzed bromination-hydroxycarbonylation tandem reaction in HOAc-NaOAc buffer. This synthetic protocol shows major improvements compared to previously reported methods, such as using biomass-based 2-furoic acid as low-cost raw material, one-pot synthesis without isolation of intermediate products, and no need for an acidification procedure. Experiments indicate that the involved Xantphos-modified Pd-catalyst and the buffer solution play significant promoting roles for each individual reaction whereas Br 2 (as the brominating reagent) had a negative effect on the second hydroxycarbonylation step, while CO was deleterious for the first bromination step. Hence, in this practical one-pot synthesis, Br 2 should be consumed in the first bromination step as fully as possible, and CO is introduced after the first bromination step has been completed.
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PubMed
高影响因子
Small
·
2021
·Vol. 17
·期 52
·2105643
·
IF 13.281
Bo Liu,Linjuan Zhang,Yuanyuan Luo,Lei Gao,Guotao Duan
The supported metal catalysts on scaffolds usually reveal multiple active sites, resulting in the occurrence of side reaction and being detrimental to the achievement of highly consistent catalysis. Single atom catalysts (SACs), possessed with highly consistent single active sites, have great potentials for overcoming such issues. Herein, the authors used SACs to modulate kinetic process of gas sensitive reaction. The supported Pd SACs, established by a metal organic frameworks-templated approach, promoted greatly the detection capacity to hydrogen sulfide (H 2 S) gas with a very high sensitivity and selectivity. Density functional theory calculations show that the supported Pd SACs not only increased the number of electrons transferring from H 2 S molecules to Pd SACs, but strengthened surface affinity to H 2 S. Moreover, the H S bonds of H 2 S molecules absorbed on Pd atomic sites are more likely to be dehydrogenated directly into sulfur species. Significantly, quasi in situ XPS analysis confirmed the presence of sulfur species during H 2 S detection process, which may be a major cause for such detection signal. Based on these results, a suitable sensing principle for H 2 S gas driven by Pd SACs was put forward. This work will enrich catalytic electronics in chemiresistive gas sensing.
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PubMed
高影响因子
Journal of Materials Chemistry A
·
2013
·Vol. 2
·期 5
·1515-1523
·
IF 0
Kun Zhang,Hangrong Chen,Xiaoxia Zhou,Yun Gong,Guobin Zhang,Xia Wang,Yu Chen,Jianlin Shi
A useful and interesting unconventional phenomenon of Pd nanoparticle formation, i.e., significantly inhibited particle growth at elevated temperatures, has been observed for the first time by growing Pd nanoparticles on a type of nonreactor, amino group-functionalized hollow mesoporous silica nanoparticles (amino-HMSNs). Such an unconventional effect is evidenced to be a competitive result between temperature-dependent coordination and reduction action of amino groups on the shell of HMSNs based on a series of experiments of probing the coordination and reduction capability of the amino groups to a Pd precursor K2PdCl6. A possible mechanism has been proposed to demonstrate and clarify the unconventional growth of Pd nanoparticles on the shell of amino-HMSNs. The as-synthesized Pd nanoparticles on the amino-HMSNs, therefore, show a tunable temperature-dependent small size range (<10 nm) and high dispersity, and can be used as efficient Heck reaction catalysts. Such a finding of unconventional particle growth effect may offer a novel protocol for particle size modulation during materials design and fabrication.
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Journal of Materials Chemistry A
·
2015
·Vol. 3
·期 46
·23607-23620
·
IF 7.443
Zhifeng Jiang,Deli Jiang,Wei Wei,Zaoxue Yan,Jimin Xie
In this work, we fabricated size-tunable metal (Pd, Ag) nanoparticles grafted on bionic dendritic α-Fe2O3 (M@Fe2O3) through an in situ growth method by using carbon nanodots as a reducing agent followed by a hydrothermal reaction. The size of the supported noble metal nanoparticles can be directly controlled on the surface of dendritic α-Fe2O3 by adjusting the added amount of noble metal salts. The catalytic performances of the resulting M@Fe2O3 hybrid composites were firstly evaluated by reduction of p-nitrophenol. The results indicated that the size of the noble metal nanoparticles had a crucial influence on the catalytic behaviors of the M@Fe2O3. In addition, the dendritic M@Fe2O3 also showed improved photocatalytic efficiencies for visible-light-driven MB degradation due to synergic effects between dendritic α-Fe2O3 and noble metal nanoparticles, including optical properties, unique structure, good dispersion, good charge separation and the SPR effect. The M@Fe2O3 composites have good reproducibility and are highly stable for p-nitrophenol reduction/degradation of MB. Our strategy can be extended to a general strategy for the formation of other novel composites consisting of a 3D hierarchical metal oxide and noble metal nanoparticles with tailorable size (e.g., Pt@TiO2, Pd@MnO2, Au@ZnO and Ag@Cu2O) for broad applications in water treatment.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2015
·Vol. 39
·期 6
·4519-4525
·
IF 3.086
Yansheng Liu,Xinlin Li,Xuanduong Le,Wei Zhang,Hao Gu,Ruiwen Xue,Jiantai Ma
MCM-48 mesoporous microspheres (M48N) with a pore size of 3.77 nm, an ultra-high surface area of 1250.77 m2 g−1 and a super-large pore volume of 1.52 cm3 g−1 were synthesized. The M48N microspheres were then modified with Pd, Pt and Ru nanoparticles using an incipient wetness impregnation technique. The modified M48N microspheres were investigated to determine their catalytic effect in the aqueous phase hydro-dechlorination (HDC) of 4-chlorophenol. The Pd–M48N, Pt–M48N and Ru–M48N catalysts were characterized by transmission electron microscopy, X-ray diffraction, nitrogen adsorption–desorption and X-ray photoelectron spectroscopy. The HDC experiments were performed using the fairly mild conditions of room temperature and an atmospheric pressure of H2. Pd–M48N showed a higher catalytic performance than Pt–M48N and Ru–M48N and various other Pd-based catalysts. The high catalytic performance of Pd–M48N resulted from the ultra-high surface area, super-large pore volume and unique pore structure of the M48N, which improved the mass transfer and increased the rate of adsorption–desorption of the compounds. This method has potential applications in the treatment of industrial wastewaters contaminated with chlorinated organic compounds.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2018
·
IF 6.434
Jiafeng Ding,Gaoyuan Long,Yang Luo,Runze Sun,Mengxia Chen,Yajun Li,Yanfang Zhou,Xinhua Xu,Weirong Zhao
Polychlorinated dibenzo- p -dioxins (PCDDs), as a group of notorious anthropogenic environmental toxicants, are arguably ubiquitous in nature. In this study, we investigated the photocatalytic reductive dechlorination of 2-chlorodibenzo- p -dioxin (2-CDD) over Pd/g-C 3 N 4 catalysts under UV–vis irradiation. The g-C 3 N 4 and a series of Pd/g-C 3 N 4 catalysts were prepared by thermal polymerization and mechanical mixing-illumination method and characterized by XRD, TEM, BET, SEM and UV–vis DRS analyses. Among all the samples, the Pd/g-C 3 N 4 (5 wt%) yielded the optimal dechlorination activity with a total 2-CDD conversion of 54% within 4 h, and 76% of those converted 2-CDD were evolved to dibenzo- p -dioxin (DD). The kinetics of dechlorination could be described as pseudo-first-order decay model (R 2 > 0.84). Corresponding rate constants (k) increased from 0.052 to 0.17 h −1 with Pd contents up to 5 wt% and decreased to 0.13 h −1 with a 10 wt% of Pd. The enhanced activities originated from the surface plasmonic resonance (SPR) effect of Pd nanoparticles and the formation of Schottky barrier between Pd and g-C 3 N 4 , which extend the spectrum responsive range and suppress the charge recombination of g-C 3 N 4 . This is the first report on the photocatalytic reductive removal of PCDDs and may provide a new approach for PCDDs pollution control.
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高影响因子
Catalysis Science & Technology
·
2020
·Vol. 10
·期 5
·1467-1476
·
IF 5.721
Zhuo-Qian Li,Xinxin Fu,Caiyan Gao,Jinyu Huang,Baojun Li,Yongpeng Yang,Jie Gao,Yonglong Shen,Zhikun Peng,Jing-He Yang,Zhongyi Liu
The one-step hydroalkylation of benzene to cyclohexylbenzene (CHB) needs to occur on bifunctional metal/zeolite catalysts, and introducing more acid sites to match the metal sites plays a key role in improving the matching of acid/metal sites toward the requirements of benzene hydroalkylation. Herein, we designed and constructed a Si–Al framework coating with extra acid sites outside the surface of the Pd/HBeta catalyst and obtained a zeolite-encaged Pd NP structure (Pd@HBeta). Notably, the Pd@HBeta catalysts achieved excellent catalytic performance with 44.0% CHB selectivity at about 85.0% benzene conversion, which is much higher than that of the Pd/HBeta catalyst with a CHB selectivity of 25.1% at the same benzene conversion. The remarkable increment of CHB selectivity of Pd@HBeta is mainly attributed to the extra acid sites provided by the coated Si–Al framework as well as the increase of the B/L ratio. Moreover, the adsorption capacity of benzene and cyclohexene is greatly improved after introducing extra acid sites by coating the Si–Al framework, which is beneficial for both hydrogenation and alkylation. Further DFT calculations reveal that C6H10 can easily desorb from Pd NPs and migrate to the acidic channel of HBeta in the Pd@HBeta catalyst than that in Pd/HBeta. Our work presents an elegant example of catalytic hydroalkylation selectivity regulation by coating an extra Si–Al framework to enhance the matching of acid/metal balance.
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高影响因子
Journal of Physical Chemistry C
·
2011
·
IF 4.524
Maiyong Zhu,Guowang Diao
An efficient magnetic carbon nanocomposite supported Pd nanoparticle catalyst has been prepared by a three-step process in this report. The morphology, inner structure, and magnetic properties of all products were studied with transmission electron microscopy, X-ray powder diffraction, Fourier translation infrared spectroscopy, X-ray photoelectron spectroscopy, and vibrating sample magnetometer. The Suzuki and Heck coupling reactions were used to demonstrate the catalytic efficiency of the as-prepared Pd/Fe3O4@C (Pd/MFC) nanocomposite catalyst. The results showed that the catalyst is completely recoverable with the simple application of an external magnetic field and the catalytic efficiency shows no obvious loss for Suzuki and Heck coupling reactions even after five repeated cycles.
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高影响因子
Materials Today Bio
·
2025
·
IF 10.2
Yeyang Sun,Xietao Ye,Lin Yang,Shuo Dong,Chen Chen,Yani Wang,Jianan Qiao,Congyan Liu,Yuping Liu,Yan Chen
Programmed cell death protein 1 (PD-1) inhibitors are integral to contemporary cancer immunotherapy. However, their objective response rate in microsatellite-stable colorectal cancer (MSS CRC) remains below 5 %. This limited efficacy is primarily due to insufficient tumor-infiltrating lymphocytes (TILs), a consequence of the combined effects of low tumor immunogenicity and impaired dendritic cell (DC)-mediated antigen presentation. The combination of ursolic acid (Ua) and ginsenoside Rg3 (Rg3) enhances TIL infiltration by inducing immunogenic cell death (ICD) in tumor cells and promoting DC maturation. Due to their poor oral bioavailability, an oral ZIF nanoplatform was engineered with a chitosan oligosaccharide (Cos) and inulin (In) bilayer coating [(In/Cos)@Ua-Rg3-ZIF] for targeted delivery of Ua and Rg3 to the CRC microenvironment. Efficient dual-drug co-loading was achieved with a loading efficiency of 24.07 wt%. After oral administration, the (In/Cos) coating protects the formulation from degradation in the upper gastrointestinal tract, while specific enzymatic cleavage by colonic microbiota releases Ua-Rg3-ZIF into tumor tissues. The ZIF platform responds to elevated adenosine triphosphate (ATP) in the tumor microenvironment, enabling controlled release of Ua and Rg3 to enhance cytotoxic T lymphocyte (CTL) levels. In vivo studies demonstrate that combining (In/Cos)@Ua-Rg3-ZIF with α-PD-1 results in an 80.86 % tumor inhibition rate, significantly outperforming monotherapies. This strategy presents an innovative oral delivery system capable of resisting gastrointestinal degradation and facilitating microbiota-responsive drug release, effectively enhancing antitumor immunity and improving the therapeutic outcome of immunotherapy in MSS CRC.
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DOI
PubMed
高影响因子
BIOSENSORS & BIOELECTRONICS
·
2015
·
IF 6.409
Yulan Wang,Hongmin Ma,Xiaodong Wang,Xuehui Pang,Dan Wu,Bin Du,Qin Wei
An ultrasensitive sandwich-type electrochemical immunosensor based on a novel signal amplification strategy was developed for the quantitative determination of human immunoglobulin G (IgG). Pd nanocubes functionalized magnetic graphene sheet (Pd–Fe 3 O 4 -GS) was employed as the matrix to immobilize the primary antibodies (Ab 1 ). Owing to the synergetic effect between Pd nanocubes and magnetic graphene sheet (Fe 3 O 4 -GS), Pd–Fe 3 O 4 -GS can provide an obviously increasing electrochemical signal by electrochemical catalysis towards hydrogen peroxide (H 2 O 2 ). Silicon dioxide (SiO 2 ) was functionalized as the label to conjugate with the secondary antibodies (Ab 2 ). Due to the larger steric hindrance of the obtained conjugate (SiO 2 @Ab 2 ), the sensitive decrease of the electrochemical signal can be achieved after the specific recognition between antibodies and antigens. In this sense, this proposed immunosensor can achieve a high sensitivity, especially in the presence of low concentrations of IgG. Under optimum conditions, the proposed immunosensor offered an ultrasensitive and specific determination of IgG down to 3.2 fg/mL. This immunoassay method would open up a new promising platform to detect various tumor markers at ultralow levels for early diagnoses of different cancers.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Jaehyeong Park,Sungjun Bae
In this study, a magnetically recyclable Pd catalyst was developed by using the novel support of iron-rich coal fly ash/silica (IRFA@SiO 2 ) for highly efficient reduction of p -nitrophenol ( p -NP). IRFA microspheres were coated with amorphous SiO 2 synthesized from non-magnetic coal fly ash (NMFA) and then loaded with Pd by impregnation method for the synthesis of Pd/IRFA@SiO 2 . Various surface analyses demonstrated that amorphous SiO 2 was well deposited on the surface of IRFA, providing a unique three-dimensionally structured SiO 2 layer to suppress aggregation of IRFA and enhance dispersion of Pd nanoparticles. Pd/IRFA@SiO 2 exhibited a significantly enhanced p -NP reduction than those of Pd/IRFA, Pd/Al 2 O 3 , and Pd/SiO 2 . Compared to other Pd- and metal-loaded catalysts, Pd/IRFA@SiO 2 showed ˜4000× enhancements in k obs-p-NP /C M (L min −1 g M −1 , M = precious metals) values and ˜3800× increases in price-normalized k obs-p-NP values, indicating that Pd/IRFA@SiO 2 is a highly efficient and cost-effective alternative catalyst. The catalyst was successfully recycled five times without significant leaching of Pd, Si, and heavy metals because of the magnetic property of Pd/IRFA@SiO 2 . The experimental results suggest the applicability of the surface-modified IRFA support for the development of novel magnetically recoverable catalysts without severe toxicity problems.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Ying Duan,Pan Guo,Dong Sui,Dongsheng Deng,Tianliang Lu,Yanliang Yang
The development of a cost-effective catalyst for hydrogen evolution from ammonia borane is of importance for the application of AB as a hydrogen storage material. In this manuscript, a series of noble metal catalysts M@CuOx/C (M = Ru, Rh, Pd, and Pt) are prepared by the galvanic reduction method. The catalysts are characterized by XRD , TEM , EDS mappings and lines scanning, XPS , HAADF-STEM, and ICP-OES. The noble metal is highly dispersed on the surface of Cu nanoparticles . The morphology of Cu nanoparticles changed according to different metals after the introduction of noble metal and there has an interaction between the noble metal and Cu. The M@CuOx/C is used for the hydrolysis of AB. For the same metal catalyst, the activity of M@CuOx/C is increased by about 3–7 times than the corresponding M/C at 298 K. The Rh shows the highest TOF and lowest activation energy among the four noble metals.
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