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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BIOSENSORS & BIOELECTRONICS
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2015
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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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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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Nanoscale
·
2022
·Vol. 14
·期 20
·7596-7606
·
IF 8.307
Yiming Jiang,Jiawei Zhu,Li Li,Yahui Gao,Juncai Leng,Jiai Yan,Shuoming Liu,Feng Zhang,Han Liu,Chenlu Zhu,Lichun Guo,Haijiao Xie,Wei Zhao
Although the application of nanoscale artificial enzymes in various industries is an attractive way to circumvent the intrinsic drawbacks of natural enzymes, their catalytic constant (Kcat) as a critical reaction parameter is far from satisfactory. Presented here is the rational design and fabrication of a unique peroxidase mimic catalyst based upon Pd@PtxRu4−x (1 ≤ x ≤ 3) prepared by coating PtRu alloy as conformal, ultrathin shells on Pd nanocrystals. Benefiting from an optimal Pt/Ru ratio and well-defined {100} facets, together with confining the Pt–Ru alloy to a shell of averagely 3.3-atomic-layer thick (i.e. Pd@Pt–Ru3.3L), the nanocrystals exhibit the highest catalytic activity and kinetics (1.2 × 106 s−1), resulting in a significant increase of catalytic activity compared with the classical PtRu nanozyme (3.6 × 103 s−1) and horseradish peroxidase (4.0 × 103 s−1), respectively. The following density functional theory calculations demonstrate that the origin of the superior catalytic performance could be attributed to the modulation of the adsorption behavior of the key reaction intermediates on the surface. As a proof of concept, its peroxidase mimicking ability is adopted for sensing glucose and glutathione molecules in human serum, with a long linear range and high selectivity. This work opens new horizons for the future development of advanced catalysts based upon alloy nanocrystals for various applications.
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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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ANALYTICA CHIMICA ACTA
·
2025
·
IF 6
Tongfang Chen,Jingjie Liang,Weiqing Liu,Xiaorong Luo,Fengxia Zhou,Yingchun Zhou,Shan Xing
Background Colorectal cancer (CRC) requires accurate diagnostic approaches for effective clinical management. Serum biomarkers PD-L1, SORL1, and GDF-15 offer valuable diagnostic information, but their simultaneous detection is hindered by the limited sensitivity and multiplexing capacity of conventional immunoassays. This work addresses the critical need for a highly sensitive multiplexed platform for precise CRC diagnosis. Results We constructed a multicolor QDs-K@FLISA platform employing K24 polylysine-conjugated CdTe quantum dots with distinct emissions (543/587/647 nm). The K-peptide enabled multi-QD loading, significantly amplifying fluorescence signals and facilitating ultrasensitive triplex detection. The assay achieved exceptional sensitivity with detection limits of 0.996 pg/mL (PD-L1), 1.101 pg/mL (SORL1), and 1.035 pg/mL (GDF-15), along with wide linear ranges (7.8-500 pg/mL for PD-L1/SORL1; 6-1600 pg/mL for GDF-15). High reproducibility was demonstrated (RSD < 2.3%). Clinical validation using 120 serum samples revealed strong correlation with reference methods (R 2 > 0.99) and effective discrimination between CRC patients and healthy controls. Significance and Novelty This work establishes a novel peptide-mediated multi-QD loading strategy that enables ultrasensitive multiplexed detection of CRC biomarkers. The platform presents significant potential for clinical applications in CRC diagnosis and biomarker profiling.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Zirui Qin,Jiehao Xie,Xiaofang Wen,Hongcan Lou,Zipin Peng,Xingkun Chen,Yuan Tan,Jisong Zhang
Chlorinated phenols are priority pollutants that require efficient low-temperature removal technologies. Here, we synthesize a series of spinel-type MAl 2 O 4 (M = Co, Mg, Zn, Cu) supports and deposit 1 wt% Pd via incipient-wetness impregnation to evaluate their hydrodechlorination (HDC) performance toward 4-chlorophenol under ambient aqueous conditions (30 °C, 0.2 MPa H 2 ). Catalytic screening shows that the identity of the divalent A-site cation strongly modulates activity: Pd/Co-Al achieves 91.8 % conversion with > 98.3 % selectivity to phenol, outperforming Pd/Ni-Al (84.7 %) and the remaining analogues. Pd/Cu-Al exhibits almost no conversion (<5.0 %), while Pd/Mg-Al and Pd/Zn-Al give moderate conversions (ca.55.4–58.7 %). Detailed characterization by XRD, N 2 -physisorption, H 2 -TPR, XPS and STEM reveals that the superior performance of Pd/Co-Al is rooted in (i) strong metal–support interactions that stabilize a balanced Pd 2+ /Pd 0 surface ensemble, (ii) coherent lattice matching at Pd(1 1 1)/CoAl 2 O 4 (311) interfaces that suppress particle growth, and (iii) high spinel thermostability that mitigates leaching and coking. A 30 h continuous-flow test confirms stable operation without activity loss. This work elucidates how subtle variations in spinel composition dictate Pd electronic structure and interfacial geometry, providing design principles for next-generation HDC catalysts.
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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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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Kai-Qiang Jing,Yu-Qing Fu,Zhe-Ning Chen,Teng Zhang,Jing Sun,Zhong-Ning Xu,Guo-Cong Guo
Strong metal–support interaction is crucial to the stability of catalysts in heterogeneous catalysis. However, reports on boosting interfacial electron transfer between metal and support via defect induction for enhanced metal–support interaction are limited. In this work, ultrathin reducible ZnTi-layered double hydroxide (LDH) nanosheets with rich oxygen defects were synthesized to stabilize Pd clusters, and the rich oxygen defects promoted Pd cluster bonding with Zn and Ti atoms in supports, thereby forming a metal–metal bond. Electron spin resonance (ESR), X-ray absorption fine spectra (XAFS), and density functional theory (DFT) calculations demonstrate remarkable interfacial electron transfer (0.62 e). The Pd/ZnTi-LDH catalyst shows superior catalytic stability for CO direct esterification to dimethyl oxalate. By contrast, the nonreducible Pd/ZnAl-LDH catalyst with a few oxygen defects shows minimal interfacial electron transfer (0.08 e), which leads to relatively poor catalytic stability. This work provides a deep insight into promoting the stability of catalysts by boosting interfacial electron transfer via defect induction.
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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 ORGANIC CHEMISTRY
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2025
·
IF 3.6
Jingru Zou,Lingmeng Xie,Wen Qin,Xingang Xie,Xing Huo
The Groebke–Blackburn–Bienaymé (GBB) reaction provides efficient access to imidazole-fused heterocycles, yet it is inevitably endowed with an isocyanide-derived secondary amino group in products. Herein, we report a Pd(II)-catalyzed sp2 C–H carbonylative amidation strategy using Co2(CO)8 as a safe CO surrogate. Leveraging the native aryl amino group as a directing motif, this protocol enables direct conversion of GBB adducts into pharmaceutically relevant imidazo[1,2-a]pyridine-fused δ-lactams with up to 86% yield. The method demonstrates exceptional functional group tolerance and eliminates prefunctionalization requirements, offering a streamlined approach to access complex nitrogen-rich architectures.
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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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