JOURNAL OF ORGANIC CHEMISTRY
·
2025
·
IF 3.6
Shuaikang Zhou,Siyi Qin,Xifang Zhang,Ying Song,Yuanfei Zhang
A Pd-catalyzed protocol that provides efficient access to acyclic 1,2-dioxygenated dienes has been established. The installation of the bifunctional carbonate electrofuge to the diene cores enabled such dienes to undergo a regioselective decarboxylative Diels–Alder cycloaddition/aromatization reaction, affording diverse synthetic challenging multisubstituted phenols with ease.
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DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2024
·
IF 10.7
Bin Zhang,Xulong Song,Zhiheng Wang,Binbin Xu,Wenkai Ye,Lilong Zhang,Han Lin,Tuo Ji,Xiaohua Lu,Jiahua Zhu
The construction of highly active hydrogen evolution electrocatalysts is necessary to improve the efficiency of water electrolysis devices. Pt-based precious metal catalysts have been reported to have high activity, but their high cost and scarcity limit their further application. Herein, we constructed a monolithic electrode containing both Pd nanoparticles (NPs) and Pd single atoms (SAs) anchored on carbonized wood (CW) via atomic layer deposition (ALD). The optimal electrode obtained by adjusting the number of ALD cycles exhibited a lower overpotential of 50.5 mV at 10 mA cm−2 and a smaller Tafel slope of 30.8 mV dec−1 in alkaline electrolyte. Moreover, the optimal CW-Pd20 electrocatalyst was found to possess fast HER kinetics and excellent stability. Theoretical calculations illustrate that Pd NPs facilitated the decomposition of water, while the Pd SAs promoted the adsorption of H, thus leading to excellent HER activity of CW-Pd20.
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DOI
高影响因子
CHEMISTRY OF MATERIALS
·
2019
·
IF 10.159
Hao Zhao,Jiabao Xu,Wenjing Huang,Yanbing Zhao,Xiangliang Yang
Although bivalent palladium [Pd(II)] compounds exhibit favorable antitumor efficacy against platinum-resistant cancers, the mechanism remains unclear. Moreover, some drawbacks, such as structural lability, rapid elimination in vivo, and poor intratumoral retention, heavily limit their application in systemic tumor chemotherapy. Here, thermosensitive Pd-PNS nanogels are rationally designed by cross-linking coordination of Pd(II) ions with poly(styrenesulfonate-b-N-isopropylacrylamide-b-styrenesulfonate) (PNS), achieving high drug-loading ability (ca. 80% of entrapment efficiency and 40% of drug-loading efficiency), sustained release, and long-term retention of highly water-soluble K2PdCl4 in intratumoral administration. Cytotoxicity on sensitive/resistant MCF-7 cells and cancer stem cell (CSC) spheroids indicates that Pd-PNS nanogels could inhibit the palladium efflux of P-glycoprotein and multidrug resistance-associated protein-1 and thus enhance the DNA damage and toxicity of platinum-resistant MCF-7/Pt cells and their CSCs. Based on their temperature-sensitive sol–gel transition, Pd-PNS nanogels show sustained release profiles and long-term retention in tumors, further enhancing in vivo antitumor efficacy on MCF-7/Pt tumor-bearing BALB/c nude mice. Owing to these advantages of prolonged retention, efflux inhibition, and efficient CSCs killing ability, Pd-PNS nanogels are promising to be developed as a new temperature-sensitive delivery nanoplatform for injectable regional chemotherapy on platinum-resistant cancers.
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DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2019
·Vol. 29
·期 12
·1806916
·
IF 15.621
Xiaowei Liu,Yanlin Feng,Guangchao Xu,Yang Chen,Ya Luo,Jinen Song,Yu Bao,Jiqiao Yang,Chune Yu,Yanna Li,Haoyu Ye,Bowen Ke,Bo Chen,Jianping Hu,Jie Xu,Huan Meng,Haiyuan Zhang,Hubing Shi
The combination of BRAF/MEK-targeted therapy with immune checkpoint blockade is regarded as a promising regimen for patients with metastatic melanoma due to their complementary advantages. However, MEK-inhibitor-induced T-cell toxicity impedes effective cooperation. In this experiment, a pH-responsive on-demand controlled release mesoporous silica nanoparticles (MSNPs) system is designed. Fluorescein-isothiocyanate-loaded MSNP can be specifically delivered into tumor cells rather than T-cells. MEK-inhibitor-loaded MSNP avoids proliferative and functional inhibitions of T-cells, while preserving growth suppression of tumor cells in vitro. In an in vivo model, MSNP encapsulation reverses the MEK-inhibitor-induced suppression of activated CD8 + T-cells, and enhances the secretion of INF-γ and IL-2. The combination of BRAF inhibitor plus MSNP-loaded MEK inhibitor and anti-PD-1 antibody synergistically inhibits tumor growth via promoting robust immune-related antitumor response. This work provides a novel and generalized framework for combining T-cell-impaired targeted therapy and immune checkpoint blockade by using a nanoparticle-based delivery system.
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DOI
高影响因子
JOURNAL OF POLYMERS AND THE ENVIRONMENT
·
2023
·Vol. 31
·期 12
·5261-5271
·
IF 5.3
Li Yuqi,Zhang Hui,Lin Xiaoying,Gong Lingzhu,Shi Ronghui
Water pollution caused by dyeing wastewater discharge, organic chemical reagent leakage and frequent oil spill incidents has aroused widespread international concern. Various methods have been proposed to remove single pollutant from wastewater. However, it is still a challenging task to develop advanced materials that can simultaneously and effectively remove various pollutants from wastewater. In this study, we successfully fabricated a novel multifunctional Pd-decorated alginate/nanofibrillated cellulose (Pd@ALG/NFC) aerogel through a facile and green in-situ reduction, followed by solution-aerogel conversion strategy. The as-prepared Pd@ALG/NFC aerogel exhibited superior catalytic activity toward methylene blue (MB) with a high degradation efficiency above 99% and excellent underwater superoleophobicity with OCA > 150° for various oils. It enabled rapid degradation of MB and efficient separation of different kinds of organic pollutants and oils from water by gravity, with an efficiency exceeding 98.3% and a water flux above 120.5 L·m − 2 ·min − 1 . Moreover, the aerogel is compressible, shape stable and recyclable. These features make the hybrid aerogel a promising candidate for multi-pollutants wastewater treatment.
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Jingmin Duan,Zhongqing Xiang,Hongsong Zhang,Bing Zhang,Xu Xiang
Formic acid (FA) is widely regarded as a hydrogen storage material with great application potential, so finding a suitable and effective catalyst for FA dehydrogenation to generate pure hydrogen under mild conditions is critical for practical applications. Herein, we converted poplar catkin (PC) with microtube structure into N-doped carbon microsheets (NPC) through carbonization, ultrasonic crushing and modification processes , and further immobilized fine Pd and Co 2 P nanoparticles on NPC microsheets to form a novel ternary catalyst of Pd-Co 2 P/NPC . The Pd-Co 2 P/NPC catalysts have excellent catalytic performance for dehydrogenation of FA under mild conditions, with a high selectivity of 100%, high initial turnover frequency value (TOF) of 2980 h −1 at 50 °C and maintained 1530 h −1 even at 30 °C. The catalyst could be recycled consecutively up to seven times without remarkable change in the catalytic activity. The significantly improved performances of Pd-Co 2 P/NPC can be attributed to high dispersity of Pd-Co 2 P nanoparticles and synergetic effect between different components. These results suggest that the biomass-based NPC microsheets may be a promising low-cost supports for the manufacturing various highly efficient nanocatalyts.
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DOI
高影响因子
JOURNAL OF APPLIED ELECTROCHEMISTRY
·
2024
·Vol. 54
·期 8
·1833-1843
·
IF 2.4
Guo Qi,Yin Jiaqi,Zhang Yuhao,Wang Yue,Zhai Hongguo,Yan Luting,Tian Meijia,Guo Yemin,Sun Xia,Zhang Yanyan
Pb(II) can accumulate in the body and gradually cause irreversible harm. In this work, a dual-mode colorimetric biosensor based on an aptamer was developed as an effective method for sensitive sensing of Pb(II). The aptamers were immobilized on silver nanoparticles (Ag NPs) by Ag–S bonding to increase the active sites on the electrode surface. Gold–palladium bimetallic nanoparticles (Au@Pd NPs) can not only serve as signal indicators but also play a role as nanozymes. On the one hand, Au@Pd NPs were modified on the aptamer to improve the conductivity of the sensor for the detection of Pb(II) by the electrochemical method of differential pulse voltammetry (DPV). On the other hand, Au@Pd NPs were porous nanomaterials with numerous active sites on their surface that can catalyze the decomposition of hydrogen peroxide (H 2 O 2 ) in solution to generate O 2 , so that 3,3′,5,5′-tetramethylbenzidine (TMB) was oxidized to blue oxTMB, enabling the visual prediction of Pb(II). At the same time, with the property that 8–17 deoxyribozyme and metal ions can co-catalyze, it promoted the binding of Au@Pd NPs functionalized aptamer to the electrode in the presence of Pb(II) and enhanced the electrochemical signal. Under optimal conditions, the detection range of Pb(II) was 1—1000 nmol L −1 , and the limit of detection (LOD) was 0.4 nmol L −1 . The biosensor has been successfully applied to the detection of edible mushroom samples. Graphical abstract
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DOI
高影响因子
HYDROMETALLURGY
·
2022
·
IF 4.217
Dechao Xiao,Haitao Zhou,Kaihui Cui,Kun Huang
This study proposes a new thin-layer oil membrane (TOM) extraction strategy for enhanced mutual separation of Pd(II) and Pt(IV) chlorocomplex anions in concentrated aqueous hydrochloric acid solutions using di- n -butyl sulfoxide (DBSO) as an extractant. It was discovered that Pd(II) could be preferentially extracted even in concentrated hydrochloric acid solutions. The separation coefficient between Pd(II) and Pt(IV) considerably increased than that between them during conventional extraction using a separating funnel. A new extractor was designed to perform TOM extraction by spreading a thin layer of organic extractant liquid membrane on the surface of aqueous feed solutions under laminar flow . A simplified TOM extraction model and controlled experiments were used to investigate the effect of H + and Cl − ion concentrations on the mutual separation between Pd(II) and Pt(IV). Molecular dynamics (MD) simulations were used to understand the microscopic separation mechanisms at the molecular level. Experimental results revealed that the competitive distribution of H + and Cl − ions in the boundary layer along the normal vertical direction of the organic-aqueous interface are crucial in enhancing the separation between Pd(II) and Pt(IV). The competitive adsorption and enrichment of Cl − ions at the interface prevent DBSO molecules from being protonated by H + ions, which is beneficial for the substituted coordination of DBSO molecules with PdCl 4 2− . However, the ionic association of protonated DBSO molecules with PtCl 6 2− remains dominant at the interface. As a result, even in concentrated hydrochloric acid solutions, the difference in mass transfer between PdCl 4 2− and PtCl 6 2− toward the interface was intensified.
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DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Wanqiu Zhu,Yakun Guo,Bangjun Ma,Xiaojiao Yang,Yingjun Li,Peilong Li,Yuanlin Zhou,Maobing Shuai
In this work, nanopalladium catalysts supported on the surface of reduced graphene oxide ( r GO/Pd) with different palladium loadings have been prepared by one-step reduction in aqueous phase . They were mixed with 1,4-bis(phenylethynyl)benzene (DEB) to form r GO/Pd-DEB composites according to a mass ratio of 1:3. It was shown that nanopalladium particles with particle size of about 2–6 nm were disperse uniformly on the surface of r GO when the Pd loadings were in the range of 3.97–10.60 wt%. The maximum hydrogen uptake capacity of r GO/Pd-DEB composites at 25 °C determined according to PCT method was about 182.5 ml/g after reacted with hydrogen for about 20 h, which was some lower than that of the common Pd/C-DEB pallet getter (216 ml/g) but significantly higher than alkynyl modified polyvinyl alcohol supported palladium hydrogen absorbing materials (0.32 ml/g), indicating that r GO/Pd could be used in solid phase catalytic hydrogenation due to the high dispersion of palladium nanoparticles and the physical proximity of r GO/Pd catalyst with DEB organic molecules. This provides a good potential technical way for perparing the moldable carbon aerogel hydrogen absorption materials.
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Muchen Lu,Jie Sun,Boyang Cui,Jian Zhang,Junlian Ren,Ruoyi Li
In this study, Pd/Ru/MXene/ nickel foam (NF) electrodes were prepared by the impregnation method and galvanostatic electrodeposition technique to investigate their electrocatalytic degradation of tetracycline (TC). Subsequently, the electron transfer mechanism during this degradation process was studied. Under the optimal conditions, the degradation efficiency of the Pd/Ru/MXene/NF composite electrode for TC reached 92.02 % at 60 min. Bursting experiments as well as H 2 O 2 generation experiments showed that OH, H* and ClO − together realized the degradation of TC. The composite electrode could effectively reduce the biotoxicity of the intermediate products of the TC degradation process. In order to reduce the aggregation of Pd and Ru nanoparticles, a scaffold structure and the introduction of a MXene intermediate layer were used to solve the problem. Electrocatalytic degradation of antibiotic molecules was facilitated by tuning the interface of the catalytic electrode to expose active sites and modulating the electronic state of the catalyst to enhance intrinsic activity.
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DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2019
·Vol. 33
·期 11
·e5198
·
IF 3.259
Yu Ru,Yanli Huang,Yuanyuan Wang,Liyi Dai
Well distributed Pd-Cu bimetallic alloy nanoparticles supported on amine-terminated ionic liquid functional three-dimensional graphene (3D IL-rGO/Pd-Cu) as an efficient catalyst for Suzuki cross-coupling reaction has been prepared via a facile synthetic method. The introduction of IL-NH 2 cations on the surface of graphene sheets can effectively avoid the re-deposition of graphene sheets, allowing the catalyst to be reused up to 10 cycles. The addition of Cu not only saves cost but also ensures high catalytic efficiency. It is worthy to note that the catalyst 3D IL-rGO/Pd 2.5 Cu 2.5 can efficiently catalyze the Suzuki cross-coupling reaction with the yield up to 100% in 0.25 h, almost one-fold higher than that by the pristine IL-rGO/Pd 2.5 catalyst (52%). The Powder X-Ray Diffraction (XRD), combining energy dispersive X-ray spectroscopy (EDS) mapping results confirm the existence and distribution of Pd and Cu in the bimetallic nanoparticles. The transmission electron microscopy (TEM) reveals the nanoparticle size with an average diameter of 3.0 ± 0.5 nm. X-ray photoelectron spectroscopy (XPS) analysis proved the presence of electron transfer from Cu to Pd upon alloying. Such alloying-induced electronic modification of Pd-Cu alloy and 3D ionic liquid functional graphene with large specific surface area both accounted for the catalytic enhancement.
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Yongli Yang,Qingxiu Shi,Chao Wu,Yujun Si
Pd nanoparticles were encapsulated within the Fe, N-doped carbon nanotubes. • The catalyst provides metallic Pd and Fe-N x as dual active sites to ORR. • Thinner, mesoporous and defective carbon walls of the nanotubes were constructed. • The catalyst shows outstanding ORR properties and practical performance. The cost, activity and durability of Pd-based catalyst can be balanced by supporting Pd on carbon materials. Herein, we report an oxygen reduction reaction (ORR) catalyst fabricated by encapsulating Pd nanoparticles within Fe, N doped carbon nanotubes, in which metallic Pd and Fe-N x serve as dual active sites. The porosity of carbon nanotube walls was tailored through a sequential process involving pyrolysis, acid leaching, and a second pyrolysis step. The resulting catalyst, Pd@FeNC7A8, exhibits smaller nanotubes with thinner carbon walls, more mesopores and greater defectivity, collectively enhancing the accessibility of the encapsulated Pd nanoparticles. Consequently, the Pd@FeNC7A8 exhibits reduced diffusion/mass-transport resistance with 33 Ω·s −1/2 of Warburg coefficient, compared with 43 Ω·s −1/2 of the control catalyst, Pd@FeNC48A, with compact carbon structure. Pd@FeNC7A8 catalyst delivers 0.904 V of half wave potential, 5.209 mA cm −2 of limited current density, and 48 mF cm −2 of electrochemical active surface area, outperforming Pd@FeNC48A in ORR performance. It also exhibits superior methanol resistance and durability compared with Pt/C. Moreover, the Pd@FeNC7A8-based the Zn-air battery demonstrates a higher discharge voltage, greater power density and specific capacity compared to its Pt/C-based counterpart, highlighting the potential of this catalyst in practical applications. Download: Download high-res image (144KB) Download: Download full-size image
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高影响因子
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