NEW JOURNAL OF CHEMISTRY
·
2017
·Vol. 42
·期 3
·1771-1778
·
IF 3.269
Saisai Cheng,Xufeng Meng,Ningzhao Shang,Shutao Gao,Cheng Feng,Chun Wang,Zhi Wang
Well-dispersed Pd nanoparticles were anchored on g-C3N4 nanosheets, which were prepared by a liquid-phase exfoliation method. The hybrid material displayed excellent catalytic activity for the transfer hydrogenation of nitroarenes. The reactions can be conducted smoothly in water at room temperature with formic acid as hydrogen source. Aniline was produced in excellent yield (>99%; turnover frequency: 853), surpassing the majority of reported heterogeneous catalysts using formic acid or formates as hydrogen source. The increased activity of such a hybrid catalyst can be ascribed to the nitrogen-rich and amphipathic property of the carbon nitride support, the stable and uniform dispersed Pd nanoparticles and the Mott–Schottky effect between the g-C3N4 nanosheets and the metal nanoparticles. The heterogeneous Mott–Schottky catalyst can be reused for five cycles without any obvious loss of its catalytic activity.
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NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Meng Li,Diangen Zhou,Hualiang An,Shanshan Dong,Xinqiang Zhao,Yanji Wang
2-Ethylhexanal (2EH) is an important intermediate for the production of 2-ethyhexanoic acid (2-ETA), and studying the direct synthesis of 2EH through heterogeneous catalysis of n-butanal aldol condensation-selective hydrogenation reaction integration is of great significance for the industrial production of 2-ETA. Herein, a series of Pd/TiO2 catalysts were prepared and characterized by XRD, CO pulse adsorption, TEM, CO2/NH3-TPD and H2-TPR. Their catalytic performance for direct synthesis of 2EH from n-butanal was investigated in stainless steel autoclave first. The results showed that the Pd/TiO2 prepared by the excessive impregnation method, loaded with 0.5 wt.% of Pd, and reduced at 400 ℃ showed excellent catalytic performance: 95.4% conversion of n-butanal and up to 99.9% selectivity of 2EH. The particle size of Pd, the base strength and the amount of acid/base of the catalyst are the main factors affecting its catalytic performance. The smaller the particle size of Pd, the greater the base strength and the larger the amount of acid/base of the catalyst, the better its catalytic performance. Then the integrated reaction mechanism was established based on the results of characterization and FT-IR of online sampling. Furtherly, the continuity of the reaction process was achieved on fixed-bed reactor. Under the reaction conditions of a liquid hourly space velocity (LHSV) of 7.2 h-1, a reaction temperature of 190 °C and a H2 pressure of 3.2 MPa, the conversion of n-butanal and the selectivity of 2EH were 91.2% and 89.8%, respectively. During the continuous operation for 300 h under optimal conditions, the conversion of n-butanal decreased slightly first and then stabilized, while the selectivity of the target product 2EH remained basically unchanged.
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FUEL
·
2024
·
IF 6.7
Yang Sun,Fan Yang,Siyuan Sun,Yankun Sun,Hongchen Liu,Chunhui Yu,Junpu An,Xi Li,Yongfeng Li
The preparation of highly active and stable Pd-based catalysts for direct alcohol fuel cells (DAFC) is hampered by inefficient utilization of the active sites, susceptibility to CO poisoning, poor stability, and relatively slow reaction kinetics. Herein, the stability and anti-toxicity of the catalysts (Pd/ZnO/MDC) are tuned by loading Pd nanoparticles on the carbon-coated ZnO support, achieving efficient electrocatalysis for methanol and ethanol oxidation reaction (MOR and EOR). TEM result shows the ZnO is covered by the carbon layer formed outside of MOF-5 derived porous carbon, which can prevent it from dissolving under harsh conditions. The mass activities of the well-tuned catalyst Pd/ZnO/MDC (8 0 0) for MOR and EOR are 931.83 mA/mg and 1838.30 mA/mg, respectively. It is due to the improved electron transport efficiency between the Pd and ZnO, and the enhanced stability by carbon layer outside the ZnO. It is also found that the onset potential and the peak potential of Pd/ZnO/MDC (8 0 0) (−0.813 V, −0.228 V) in CO stripping experiment in MOR are more negative than Pd/MDC (8 0 0) (−0.261 V, −0.215 V). This result indicates that the existence of ZnO helps to provide surface hydroxyl group, which promotes the oxidation of the intermediates. This work indicates provides a feasible idea for DAFC catalyst design and construction.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zheng Li,Jiehao Xie,Zipin Peng,Zhuo Ma,Yihui Li,Xingkun Chen,Yuan Tan,Wenshao Yang,Yunjie Ding
4-Chlorophenol (4-CP) is a pervasive environmental pollutant commonly found in wastewater and groundwater, posing great risks to both human health and the ecosystem. Catalytic hydrodechlorination (HDC) of 4-CP by utilizing hydrogen (H 2 ) as a reductant has emerged to be an efficient and sustainable way to treat pollutant water. This study focuses on the development of an efficient and stable Pd-based catalyst for the catalytic HDC of 4-CP. By incorporating an appropriate amount of Ni into Al 2 O 3 support, a NiAl 2 O 4 (NA) spinel was synthesized, enhancing the interaction between Pd and the support, leading to precise control over Pd species and oxygen vacancies. The tailored properties of the Pd/NA-1 catalyst result from meticulous adjustment of the Pd 2+ /Pd 0 ratio and oxygen vacancies, which promotes electron transfer from Pd to Ni within the NiAl 2 O 4 spinel. In comparison to the Pd/Al 2 O 3 catalyst, the Pd/NA-1 catalyst exhibits exceptional stability, with continuous operation for over 120 h without deactivation. Comprehensive characterization analyses indicate that the Pd/NA-1 catalyst effectively prevented the aggregation of Pd nanoparticles, maintaining the Pd 2+ /Pd 0 ratio at 1, which is crucial for its superior stability. This work provides valuable insights into the development of Pd-based catalysts for HDC reactions, highlighting the potential use of Pd/NA-1 catalysts in treating hazardous pollutants like 4-CP in waste systems.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Jianfeng Shan,Zheng Chen,Dengfeng Wang,Guangyu Zhang,Sheng Li,Chuan Sun,Dongchao Wang,Caixia Ju,Xuelan Zhang,Lei Li
Catalytic conversion of ethyl levulinate (EL) to γ-valerolactone (GVL) is a pivotal reaction in biomass conversion. Here, Pd/CoO x was studied and showed much higher EL hydrogenation reactivity than other Pd based catalysts. Further investigation revealed that EL conversion increased linearly with PdCo alloying degree elevating, indicating that PdCo alloy is ascribed to the superior reactivity of Pd/CoO x . Interestingly, Pd/CoO x with low Pd loading also exhibited excellent hydrogenation performance, and surface enrichment of Pd was identified as the main reason. Additionally, employing HZSM-5 as a co-catalyst not only accelerated ethyl 4-hydroxypentanoate lactonization, but also dramatically improved the stability of Pd/CoO x . As a result, a 99.1 % yield of GVL was achieved by the synergistic catalysis of HZSM-5 and Pd/CoO x containing 0.58 wt% Pd, which is comparable with the best catalyst ever reported in alkyl levulinate hydrogenation to GVL. Furthermore, the insights gained from this work have broad potential applications in biomass hydrogenation.
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MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 12
·1-10
·
IF 5.3
Li Chengcheng,Lu Jinhui,Xiang Chao,Zhang Enhui,Tian Xiaofang,Zhang Ling,Li Tingting,Li Chengyao
Three-metal-core-shell nanoparticles (Au@Pt@PdNPs) providing excellent peroxidase-like activity were applied in lateral flow immunoassay (LFIA), designated as Au@Pt@Pd-LFIA, for detecting the nucleocapsid protein (NP) of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2). An Au@Pt@Pd-LFIA was developed for quantitatively testing of SARS-CoV-2 NP with a range 0.12–31.25 ng/mL. The limit of detection (LOD) of Au@Pt@Pd-LFIA strip was 0.06 ng/mL, which was 16-fold or eightfold more sensitive than that of the gold lateral flow immunoassay (Au-LFIA) and the gold flower flow immunoassay (AF-LFIA) strips, respectively. For detection of clinical samples from nasal swabs using test strips, Au@Pt@Pd-LFIA had 84.09% sensitivity, 100% specificity, and 92.55% accuracy. In terms of detection time, the testing of Au@Pt@Pd-LFIA strip was 16 min similar to Au-LFIA (15 min) and AF-LFIA (10 min), but much shorter than ELISA (2 h). In conclusion, Au@Pt@Pd-LFIA is a sensitive, rapid, and simple test for quantitative detection of SARS-CoV-2 NP in nasal swab samples. Graphical Abstract
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JOURNAL OF NANOBIOTECHNOLOGY
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2024
·Vol. 22
·期 1
·1-18
·
IF 10.6
Zou Ting,Huang Yun,Zhou Zongtao,He Shuangyan,Liu Jia,Chen Yalan,Liu Hongdu,Luo Zhonghui,Liu Miaoxin,Wei Hua,Yu CuiYun
Clinical treatment of hepatocellular carcinoma (HCC) with 5-fluorouracil (5-FU), the primary anticancer agent, remains unsatisfactory due to the glutathione (GSH)-associated drug resistance and immunosuppressive microenvironment of HCC. To develop a facile yet robust strategy to overcome 5-FU resistance for enhanced immunotherapy treatment of HCC via all dimensional GSH exhaustion, we report in this study construction of a minimalist prodrug consisting of 5-FU linked to an indoleamine-(2,3)-dioxygenase (IDO) inhibitor (IND) via a disulfide bridge, FU-SS-IND that can further self-assemble into stabilized nanoparticles, FU-SS-IND NPs. Specifically, besides the disulfide linker-induced GSH exhaustion, IND inhibits GSH biosynthesis and enhances the effector function of T cells for turning a “cold” tumor to a “hot” one, which synergistically achieving a tumor inhibition rate (TIR) of 92.5% in a 5-FU resistant mice model. Most importantly, FU-SS-IND NPs could upregulate programmed death ligand 1 (PD-L1) expression on the surface of tumor cells, which enables facile combination with immune checkpoint blockade (ICB) for a ultimate prolonged survival lifetime of 5-FU-resistant tumors-bearing mice. Overall, the minimalist bioreducible nano-prodrug developed herein demonstrates great translatable potential for efficiently reversing drug resistance and enhancing immunotherapy of HCC.
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MICROCHIMICA ACTA
·
2025
·Vol. 192
·期 8
·1-17
·
IF 5.3
Liang Jintao,Li Canru,Zhou Yu,Fan Lingling,Liu Lin,Liang Jianlu,Tan Xiaohong,Zhou Zhide,Li Guiyin
Golgi protein 73 (GP73) is highly expressed in hepatocellular carcinoma (HCC) and considered a sensitive serum biomarker for HCC diagnosis. Herein, a label-free electrochemical aptasensor for ultrasensitive detection GP73 based on nitrogen-doped reduced graphene oxide-ferrocene-platinum@palladium nanoparticles (NRGO-Fc-Pt@Pd NPs) was constructed. The NRGO-Fc-Pt@Pd NPs offered excellent conductivity, biocompatibility, and large surface area, serving as both an electrode modifier and a redox probe due to Fc's good electroactivity. GP73 aptamer (GP73 Apt ) was covalently bound with the NRGO-Fc-Pt@Pd NPs to form the signal probe. When GP73 specifically bound to GP73 Apt to form GP73-GP73 Apt complex and fell off from the electrode, it leads to an increased Fc(Fe(II)/Fe(III)) peak current in differential pulse voltammetry (DPV) due to the enhancing of the sensing interface's electroactivity. Under optimized conditions, the label-free electrochemical aptasensor demonstrated a linear relationship with GP73 concentration in the range 1.0 ng/mL-300 ng/mL, with R 2 of 0.99594 and a limit of detection (LOD) of 0.3524 ng/mL. In addition, the aptasensor showed good specificity, reproducibility, and stability. Furthermore, the developed aptasensor was applied to detect the GP73 in actual serum samples with good recoveries (97.85%-107.48%) and relative standard deviations (RSDs) (0.37%–7.85%) via the spiked recovery method. All the results may provide a new approach for HCC clinical detection. Graphical
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Yuanjie Xu,Run Hou,Kunxiang Chi,Bo Liu,Zemin An,Lizhi Wu,Li Tan,Xupeng Zong,Yihu Dai,Zailai Xie,Yu Tang
Palladium-based catalysts have long been considered the benchmark for methane combustion; however, the authentic phase of catalytic active sites remains a subject of ongoing debate. Additionally, challenges like water-poisoning and long-term stability need to be addressed to advance catalyst performance. Herein, we investigate Pd on Co 3 O 4 nanorods as a highly effective catalyst for catalytic oxidation of methane, demonstrating long-term stability and water tolerance during a 100-h continuous operation at 350 °C. Comprehensive characterizations reveal the presence of an active Pd-oxygen vacancy (O v )-cobalt interface in Pd/Co 3 O 4 , which effectively adsorbs molecular O 2 . The absorbed oxygen species on this interface are activated and directly participate in methane combustion. Moreover, near-ambient pressure X-ray photoelectron spectroscopy demonstrates that Pd nanoparticles undergo a rapid phase transition and predominantly remain in the metallic state during the reaction. This behavior is attributed to the electronic metal-support interaction between Pd and Co 3 O 4 . Furthermore, in situ Fourier transformed infrared spectrum reveals that under reaction conditions, HCO 3 * species are formed initially and subsequently transformed into formate species, indicating that the formate pathway is the dominant mechanism for CH 4 oxidation.
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ACS Sensors
·
2025
·
IF 9.1
Zhenguo Zhang,Xue Li,Shuo Zhang,Mingshuang Zheng,Fangping Yuan,Shushen Li,Bei Yuan,Lisheng Liu,Xin Du
Although immunotherapy has become an established approach in cancer treatment, not all patients exhibit a positive response. Current research on PD-1 primarily focuses on immune cells using conventional methods, yet PD-1 expression on tumor cells is also widespread and plays an increasingly critical role in assessing immunotherapy efficacy. To address this, we developed an electrochemical biosensor capable of specifically detecting PD-1 at both the protein and tumor cellular levels in situ, eliminating the need for sample fixation and thereby streamlining the analytical process. Additionally, our probe enables simultaneous localization analysis of PD-1 through fluorescence signaling. The biosensor integrates a bifunctional probe composed of a nanometal–organic framework (MOF, ZIF-8) conjugated with quantum dots (QDs) and an electrode modified with a carbon nanotube (CNT)–gold nanoparticle (AuNP) nanocomposite. The morphology and performance of the nanocomposite were thoroughly characterized, and the resulting PD-1 biosensor demonstrates high specificity, reproducibility, and sensitivity. To facilitate clinical translation, we successfully applied the biosensor to detect differential PD-1 expression across various tumor cell lines and cancer tissues. This study establishes that our dual-mode electrochemical and fluorescent sensing platform provides a powerful tool for in situ PD-1 detection on tumor cells, offering valuable insights for evaluating tumor immunotherapy responses.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Huan Su,Chao Shan,Xiaolin Zhang,Bingcai Pan
Chemical oxidation is essential in treating P(I)/P(III)-bearing wastewater, while conventional oxidation processes suffer from low selectivity and high cost induced by oxidant reagents. Herein, a low-cost catalyst PdNi 10 was developed to rival the noble metal Pd, which had been known as the only catalyst enabling chemical-free oxidation of P(I)/P(III) into P(V) by ambient O 2 . The PdNi 10 fabricated via optimized method even outperformed Pd in catalytic activity at identical dosage (0.10 g L −1 ), achieving efficient conversion of 1.00 mM of P(I) into P(V) (>94% in 30 min) with wide applicable pH range from 3.0 to 9.0. The aerobic oxidation of P(I) and P(III) over PdNi 10 was confirmed via scavenging experiments to be both dominated by non-radical pathways with apparent activation energies of 44.5 and 21.3 kJ mol −1 , respectively. Interestingly, the individual roles of Ni components of PdNi 10 in the catalytic oxidation were found negligible. The H 2 O-methanol binary solvent experiment suggested that H 2 O mediated the catalytic reaction and the interfacial OH groups as a result of H 2 O dissociation served as the main reactive oxidant species for P(I)/P(III) oxidation. Furthermore, synergistic mechanism was proposed for the Ni and Pd sites with favorable roles in the essential reaction steps of dehydrogenation and hydroxylation, respectively. This study is believed to advance the treatment strategy of P(I)/P(III)-rich wastewater and to shed new light on the development of low-cost catalysts enabling chemical-free aerobic oxidation processes under facile condition.
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Arthritis & Rheumatology
·
2025
·
IF 10.9
Jin-Fen Ma,Ting Xu,Hao-Xian Zhu,Xiao-Min Chen,Liang Li,Zhi-Bin Zhao,Liwei Lu,Yang Li,Zhe-Xiong Lian,Cai-Yue Gao
Objective Activated T cells play a pivotal pathogenic role in the progression of Sjögren disease (SjD); however, there are currently no targeted therapies specifically designed to address them. This study aims to identify pathogenic CD8 + T cells in SjD and develop targeted therapeutic strategies. Methods Il12b-/-Il2ra-/- mice, a murine model for overlapping primary biliary cholangitis and SjD, were employed in this study. Pathogenic CD8 + T cells were identified through single-cell RNA sequencing and flow cytometry analyses of samples from both patients with SjD and relevant murine models. Shared T cell receptor analysis was conducted to trace the potential precursors of pathogenic CD8 + T cells. The efficacy of PD-1-targeted chimeric antigen receptor (CAR)–T cell therapy was evaluated through the assessment of salivary gland secretory function, immunologic profiles, and histopathological changes in the murine model. Results We identified PD-1 as a comprehensive marker of clonally expanded and activated pathogenic CD8 + T cells in the salivary glands and peripheral tissues. Flow cytometry further confirmed the activation phenotype and cytotoxicity of PD-1 + CD8 + T cells in the salivary glands of patients with SjD. Notably, the number of PD-1 + CD8 + T cells in the labial glands positively correlated with disease activity in patients with SjD. These findings highlight the therapeutic potential of depleting PD-1 + CD8 + T cells in SjD. Furthermore, PD-1-targeted CAR-T cell therapy significantly alleviated SjD symptoms in a murine model. Conclusion We identified the pathogenic role of PD-1 + CD8 + T cells in both patients with SjD and a murine model and demonstrated the efficacy of PD-1-targeted CAR-T cell therapy in SjD model mice. Our findings suggest a promising avenue for developing clinical therapeutic strategies for patients with SjD.
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