RSC Advances
·
2019
·Vol. 9
·期 57
·33302-33309
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IF 3.049
Yanhua Zhang,Hui Huang,Hao Fu,Meng Zhao,Zhihua Wu,Yang Dong,He Li,Yourong Duan,Ying Sun
As known to all, ovarian cancer ranks the most lethal of the gynecological malignancies. The antitumor drugs based on platinum are first-line chemotherapy drugs for ovarian cancer. However, their therapeutic efficiency is severely limited owing to dose-limiting toxicities of platinum. New theranostic strategies to overcome chemotherapy toxicity is highly desirable. Meanwhile, the real-time treating effect is not visible for doctors. Herein, we constructed PFH/siRNA/Fe3O4@Pt(IV) NPs-cRGD (NPs-cRGD) for precise theranostics against ovarian tumors with real-time imaging. The NPs-cRGD had a good storage stability and resisted the serum-induced aggregation, which was beneficial for drug delivery. Additionally, gel-retardation assay demonstrated that the NPs-cRGD exhibited great protection to siRNA to resist nuclease degradation. In vitro, the NPs-cRGD showed good dual-mode US/MRI imaging and the relative imaging research was also discussed. Moreover, the in vitro experiments indicated that the NPs-cRGD with US exhibited excellent antitumor therapeutic efficiency, resulting from the cRGD ligands and US exposure enhanced the cellular uptake efficiency. Thus, the dual-mode nanoparticles in this work may provide precious insight into the development of various multi-mode nanoplatforms delivering drugs or genes for precise theranostics against various cancer.
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高影响因子
LANGMUIR
·
2023
·
IF 3.9
Wen Chen,Zhiwei Huang,Jiangwei Ni,Qiqi Zhou,Xiaomin Wu,Huazhen Shen,Huawang Zhao,Guohua Jing
Volatile organic compounds such as benzene are hazardous air pollutants that require effective elimination. Noble metal-based catalysts exhibit high benzene combustion activity, but their prohibitive cost necessitates strategies to enhance utilization efficiency. This study investigates a Pt–Cu alloy catalyst for improved benzene combustion by preferentially exposing Pt active sites through Cu alloying. Aberration-corrected scanning transmission electron microscopy and X-ray spectroscopy characterize the nanoscale distribution and enrichment of Pt on the alloy surface. Kinetic measurements demonstrate substantially enhanced activity compared with Pt catalysts, attributed to increased Pt metallic site exposure rather than alteration of the reaction mechanism. In situ Fourier transform infrared (FTIR) spectroscopy reveals a higher abundance of terrace-like Pt sites in the alloy, beneficial for benzene adsorption. Partial pressure dependence analyses indicate competitive adsorption of benzene and O2, following Langmuir–Hinshelwood kinetics. These findings provide conceptual insights into tuning surface composition in bimetallic catalysts to optimize noble metal efficiency, with broad applicability for sustainable catalytic process advancement.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Xun Li,Heng He,Tian Tan,Zhihan Zou,Zhanyou Tian,Wanling Zhou,Yuwen Bao,Xiaohong Xia,Yun Gao
Low power consumption is a new emerged requirement for methane sensors long-term working in a gas supervisory control system. Great challenges remain in development of heat free methane sensors based on metal oxide semiconductors (MOS). In this work, Pt-doped SnO 2 (Pt-SnO 2 ) grow on well aligned ZnO nanorod-array to form an inter-staggered double-layer structure on AZO glass by a two-step hydrothermal method, with the annealing temperature being systematically studied. The optimized processing parameters are 1 at% Pt doping content and 700 °C annealing temperature, offering the best sensing response of 3.36 to 800 ppm CH 4 at room temperature. SnO 2 /ZnO without Pt doping shows linear I-V relationship, while the Pt-SnO 2 /ZnO shows a Schottky-like I-V curve with the Schottky barrier height decreases as increasing the CH 4 concentration. The activation energy (Δ E a ) for CH 4 dissociation decreases with increasing the annealing temperature, and the Δ E a of the optimized Pt-SnO 2 /ZnO sample is only one-third of that in the SnO 2 /ZnO. In addition to the piezoelectric polarization electric field in ZnO, the build up Schottky-like barrier and the reduced activation energy via Pt doping and annealing are demonstrated to be efficient for enhancing the methane sensing performance at low operation temperature.
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MOLECULES
·
2023
·Vol. 28
·期 19
·6879
·
IF 4.6
Tiantian Zhang,Jiacheng Xu,Yan Sun,Shiyu Fang,Zuliang Wu,Erhao Gao,Jiali Zhu,Wei Wang,Shuiliang Yao,Jing Li
Pt-based catalysts exhibit unique catalytic properties in many chemical reactions. In particular, metal–support interactions (MSI) greatly improve catalytic activity. However, the current MSI mechanism between platinum (Pt) and the support is not clear enough. In this paper, the interaction of 1 wt% Pt nanoparticles (NPs) onβ-MnO2in carbon monoxide (CO) oxidation was studied. The Pt onβ-MnO2inhibited CO oxidation below 210 °C but promoted it above 210 °C. A Pt/β-MnO2catalyst contains more Pt4+and less Pt2+. The results of operando DRIFTS-MS show that surface-terminal-type oxygen (M=O) plays an important role in CO oxidation. When the temperature was below 210 °C, Mn=O consumption on Pt/β-MnO2was less thanβ-MnO2due to Pt4+inhibition on CO oxidation. When the temperature was above 210 °C, Pt4+was reduced to Pt2+, and Mn=O consumption due to CO oxidation was greater thanβ-MnO2. The interaction of Pt andβ-MnO2is proposed.Keywords:metal–support interaction;CO oxidation;terminal-type oxygen;bridge-type oxygen;Pt;MnO2
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INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Hongjing Wang,Yuqin Liang,Songliang Liu,Hongjie Yu,Kai Deng,You Xu,Xiaonian Li,Ziqiang Wang,Liang Wang
The research on high-efficiency two-dimensional (2D) catalytic materials for the small-molecule oxidation-assisted hydrogen evolution reaction (HER) is prospective for efficient hydrogen production. Herein, we report heterostructured Pt/Rh metallene with Pt nanoparticles (NPs) uniformly anchored on Rh metallene for the HER and ethylene glycol oxidation reaction (EGOR). The ultrathin sheet structure of the Pt/Rh metallene offers high surface areas and sufficient active sites. More importantly, the Pt/Rh heterostructure can optimize catalytic active centers and adjust electronic structure. Thus, Pt/Rh metallene exhibits superior electrocatalytic HER activity with a low overpotential of 28 mV in 1 M KOH at 10 mA cm–2 and EGOR activity with a specific activity of 8.39 mA cm–2 in 1 M KOH with 3 M EG, along with outstanding CO tolerance. In a two-electrode system, Pt/Rh metallene requires a low potential of 0.51 V for stable and efficient hydrogen production at 10 mA cm–2 in 1 M KOH + 3 M EG, with the simultaneous production of high-value-added products. The job proposes an attractive strategy for the synthesis of 0D/2D metallene toward simultaneous energy-saving hydrogen production and chemical update.
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CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Yi-Fan Xue,Jie Feng,Jin-Yao Ma,Wen-Ying Li
C–N bond breaking is a difficult but crucial step in the quinoline removal of coal-based liquids. Noble metal catalysts have higher C–N bond breaking activity, but their surface bond breaking mechanism is unclear. Atomic layer deposition creates more metal-oxide sites and generates different active species, which facilitates the mechanism study. For this reason, we used atomic layer deposition to deposit TiO 2 on the catalyst surface and suggested a more complete C–N bond breaking mechanism in this study. The particle size and pore structure of the catalyst did not change significantly after the deposition, and the hydrogen adsorption was reduced when there were too many layers deposited and the surface Pt sites were occupied to a high degree. TiO 2 is extremely susceptible to reduction to Ti 3+ under hydrogen, and can change the nature of the electron density of Pt through oxygen vacancies, creating Ti 3+ -Pt δ− sites that are prone to protonation reactions. That means, the occurrence of these protonation reactions not only easily breaks the C–N bond, but also accelerates the rate of C–N bond cleavage due to the increased H coverage on the surface of the xcTi-PtAl catalysts. And the Ti 3+ -Pt δ− sites in catalyst had a stronger adsorption effect on the nitrogen-containing compounds, which in turn lowered the energy barriers of bond cleavage. It is concluded that protonation is a necessary step before the C–N bond can be broken. The subsequent steps were showed by the DFT calculations that the nitrogen-containing compounds adsorbed on the Ti 3+ -Pt δ− sites undergo β-H fracture after the protonation reaction, with the elimination reaction cleaving the C–N bond. The xcTi-PtAl catalysts by atomic layer deposition of Ti not only improve the C–N bond breaking performance, but also improve bond breaking stability by a factor of four compared to the Pt/Al 2 O 3 catalysts.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 26
·期 4
·3263-3273
·
IF 3.3
Ziwei Zhai,Bofeng Zhang,Yutong Wang,Guozhu Liu
Based on the disturbance of electronic density, nitrogen-doped nanocarbons show promising properties to anchor metal clusters. However, precisely regulating the coordination mode between N species and the active site remains challenging. Herein, we rationally designed three N types (graphitic N, pyridinic N and pyrrolic N) in nanocarbons to anchor Pt clusters for the benchmark propane dehydrogenation. The specific activity of the pyridinic-N-doped catalyst was 147.54 molC3H6 molPt−1 h−1 at 550 °C, which was 1.3 times higher than those of graphitic- and pyrrolic-N-doped catalysts. Unlike the regular tetrahedron Pt cluster in the graphitic-N catalyst or the distorted three-layered Pt cluster in the pyrrolic-N catalyst, the Pt cluster in the pyridinic-N catalyst was an inverted tetrahedron, which increased the contact degree without geometric repulsion towards C–H bond scission. The geometric parameters of detached H and C atoms in the methylene group for the pyridinic N catalyst was decreased to strengthen the C–H bond scission. After CH3CHCH3* adsorption, the Bader charge of the Pt active site also became highly positive, which tailored the d-band center closer to the Fermi level and provided more vacant orbitals for C–H bond breakage. Therefore, pyridinic N in nanocarbons is promising to anchor small-sized Pt for alkane dehydrogenation in terms of geometric and electronic effects.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Ziyu Wang,Xuekun Jin,Fengjuan Chen,Xuanyu Kuang,Junyong Min,Haiming Duan,Junhua Li,Jianjun Chen
In proton exchange membrane fuel cells (PEMFC S ), a Pt-based catalyst has been plagued by activity and durability, making it difficult to implement in large-scale commercial applications. In this paper, a composite material formed by titanium dioxide and carbon black containing oxygen vacancies (TiO 2 (O V )-C) was used as a functional support to successfully load Pt nanoparticles (NP S ). The introduction of oxygen vacancies induces the formation of a connection between Pt and TiO 2 , which not only strengthens the fixation of Pt by the composite support but also optimizes the local charge density of Pt. Compared with Pt/C (0.842 V) and Pt/TiO 2 -C (0.841 V), the half-wave potential (E 1/2 ) of Pt/TiO 2 (O V )-C (0.862 V) is increased by 20 mV and 21 mV, respectively. After a long-term durability test, the E 1/2 of Pt/TiO 2 (O V )-C is only attenuated by 5 mV. In addition, the mass activity (MA) and specific activity (SA) decreased from 183.4 mA mg −1 and 0.565 mA cm −2 to 144.4 mA mg −1 and 0.483 mA cm −2 at 0.85 V, only decreasing by 21% and 17 %, showing good stability. X-ray photoelectron spectroscopies (XPS) and density functional theory (DFT) calculations show that the interaction between Pt and TiO 2 reduces the d-band center of Pt, thereby improving the desorption of intermediates *OH, which in turn promotes the activity of alkaline ORR . This study not only shows that O V plays a key role in the process of inducing interaction, but also deeply studies the influence of this interaction on the active site Pt, which provides more choices for the design of excellent multiphase catalysts.
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Nanoscale
·
2023
·Vol. 15
·期 30
·12558-12566
·
IF 6.7
Shurui Yuan,Ling Yang,Xiankun Lin,Qiang He
Chemically powered colloidal motors propelled by the self-phoretic effect have attracted widespread attention. However, the low motion efficiency and ion tolerance hinder their application in complex media. Herein, we report a scalable and simple method to synthesize 2.6 nm Platinum nanoparticles (Pt NPs) in the nanoporous wall of carbonaceous flasklike colloidal motors in a ligand-free manner. The obtained Pt NPs-modified flasklike colloidal motors (Pt-FCMs) are propelled by the catalytic decomposition of H2O2 fuels. They exhibit ultrafast mobility with an instantaneous velocity of 134 μm s−1 at 5% H2O2, which is equivalent to 180 bodylengths per second. Particularly, these Pt-FCMs have an enhanced ion tolerance, due to the higher catalytic activity of small-sized Pt NPs in the carbonaceous wall. Furthermore, the direction of motion could be reversed by adding cationic surfactant cetyltrimethylammonium bromide. Such ultrasmall Pt NPs funtionalized flasklike colloidal motors exhibit a great potential utilization in the field of biomedicines and environmental technology.
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CRYSTENGCOMM
·
2023
·Vol. 25
·期 25
·3655-3661
·
IF 3.1
Ningkang Qian,Degong Ding,Liang Ji,Junjie Li,Hui Zhang,Deren Yang
Lattice engineering is a powerful strategy not only to optimize electrocatalytic performances, but also to deepen the understanding of electrocatalytic mechanisms. Lattice engineering can be effectively achieved in core–shell nanocrystals owing to the lattice mismatch of heterostructures. Herein, we constructed three kinds of icosahedra consisting of Au73Pd27@Pt, Au66Pd34@Pt and Pd@Pt core–(interlayer)–shell by a seed-mediated method. The introduction of an ultrathin Pd interlayer in the Au66Pd34@Pt icosahedra enables us to separately identify the strain effect and ligand effect. The specific activities towards the EOR of these icosahedra are in the sequence Au73Pd27@Pt > Au66Pd34@Pt > Pd@Pt, indicating that both the ligand effect and strain effect caused by Au can enhance the activity of Pt towards the EOR. The in situ FTIR studies confirm that the EOR processes on these icosahedra are all dominated by the C2 pathway, and hence we ascribe the enhancements of EOR activities to the faster kinetics of the C2 pathway by producing acetate or acetaldehyde.
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JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Mengya Guo,Feng Wang,Mingwei Zhang,Li Wang,Xiangwen Zhang,Guozhu Li
Encapsulation of clean metal nanoparticles (NPs) into interior of metal–organic framework (MOF) is of great importance to remarkably improve the stability and tune the catalytic performance of metal NPs. Herein, highly dispersed Pt NPs are encapsulated in UiO-66 with different functional groups on linker (UiO-66-X, X = F, H, NH 2 , OH) through enhanced electron attraction of metal precursor by MOF node and proper reduction by H 2 /Ar gas. Compared with traditional impregnation method, the encapsulation method gives well-defined Pt NPs and controllable microenvironment. Detailed characterizations reveal that functional group of the linker can effectively tune the microenvironment and electronic properties of guest Pt NPs. In situ FTIR was utilized to investigate the adsorption capability and strength of reactants on the catalysts. The electron-deficient Pt species and appropriate surface hydrophobicity match well with the reactants, which is responsible for enhanced catalytic hydrogenation activity of C C and nitro groups. The surface hydrophobicity plays a major role in promoting alkyne hydrogenation. This work is devoted to rationalize the relationship between hydrogenation performance and catalyst property of UiO-66 encapsulated Pt NPs, in terms of energy adaptability in electronic state and structure adaptability in surface chemistry. Rational design strategy of Pt-confined-in-MOF composites through molecular level regulation is provided for hydrogenation.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 35
·84609-84619
·
IF 5.8
Wu Zhaojiang,Lin Zheng,Wang Shengye,Yang Bo,Xiao Ke
The recovery of platinum from industrial waste is of critical importance. Usually, the recovery method is to dissolve the solid waste with acid to form a solution where platinum mainly exists in the form of Pt(IV). Therefore, it is urgent to efficiently and selectively adsorb Pt(IV) ions from acid leachates. In this study, a highly efficient adsorbent was developed by grafting of carboxyl and amine groups onto melamine sponge with alginate-Ca and polyethylenimine-glutaraldehyde (ML/ACPG). Combination of SEM, FTIR and XPS showed that the ML/ACPG sponge had a tree structure and the amino, carboxyl and hydroxyl groups were successfully introduced. Maximum adsorption capacity of ML/ACPG sponge reached up to 101.1 mg/L at pH of 1 (optimum initial pH value). The Pt(IV) ions were readily desorbed (within 60–80 min) using 0.1 M HCl + 0.025 M thiourea solution. Desorption efficiency remained higher than 83.3% while adsorption capacity decreased by less than 6.0% after 5 cycles operation. The ML/ACPG sponge was stable in 3 M of HNO 3 , NaCl after shaking for 72 h at 300 rpm with mass loss less than 2.5%. The mechanism of Pt(IV) adsorption onto ML/ACPG sponge mainly involved coordination by electrostatic attraction and carboxyl groups by protonated amine groups. The above results confirmed that the ML/ACPG sponge has a good practical application potential for Pt(IV) recovery from acid leachates.
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