CHEMISTRY-A EUROPEAN JOURNAL
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2015
·Vol. 21
·期 43
·15439-15445
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IF 5.731
Yuan-Yuan Jiang,Hong-Bin Dai,Yu-Jie Zhong,De-Min Chen,Ping Wang
Graphical Highly active and robust : Ni–Pt alloy nanocatalysts supported on mesoporous ceria, prepared by a one-pot evaporation-induced self-assembly method, selectively promote decomposition of hydrazine monohydrate at a high rate to generate hydrogen with high selectivity (see figure). Moreover, the catalysts exhibit high cycle stability. The development of active, selective, and robust catalysts is a key issue in promoting the practical application of hydrazine monohydrate (N 2 H 4 ⋅ H 2 O) as a viable hydrogen carrier. Herein, the synthesis of a supported Ni–Pt bimetallic nanocatalyst on mesoporous ceria by a one-pot evaporation-induced self-assembly method is reported. The catalyst exhibits exceptionally high catalytic activity, 100 % selectivity, and satisfactory stability in promoting H 2 generation from an alkaline solution of N 2 H 4 ⋅ H 2 O at moderate temperatures. For example, the Ni 60 Pt 40 /CeO 2 catalyst enabled complete decomposition of N 2 H 4 ⋅ H 2 O to generate H 2 at a rate of 293 h −1 at 30 °C in the presence of 2 M NaOH, which compares favorably with the reported N 2 H 4 ⋅ H 2 O decomposition catalysts. Phase/structural analysis by XRD, TEM, and Auger electron spectroscopy was conducted to gain insight into the excellent catalytic performance of the Ni–Pt/CeO 2 catalyst.
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JOURNAL OF EXPERIMENTAL & CLINICAL CANCER RESEARCH
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2025
·Vol. 44
·期 1
·1-25
·
IF 12.8
Wang Pengyu,Guo Weihua,Liu Shuyue,Li Shouyi,Li Jiaqi,Ding Bowen,Yin Fengyi,Yang Yang,Li Xingjiang,Cao Pei,Ma Chaozhe,Zhang Wanying,Song Yidan,Geng Yating,Liu Lantao,Hu Jing,Hao Jihui,Feng Yukuan
Background Copper accumulation triggers mitochondrial-driven cell death, known as cuproptosis, offering a promising mechanism for targeted cancer therapy. Recent studies have highlighted the critical role of intratumoral copper levels in regulating the expression of programmed cell death ligand-1 (PD-L1), suggesting that copper-induced cuproptosis not only enhances cancer cell death but may also amplify the effects of anti-PD-L1 antibodies (αPD-L1). However, in tumors where monotherapy with αPD-L1 shows limited efficacy, particularly in pancreatic ductal adenocarcinoma (PDAC), the role of copper-induced cuproptosis in enhancing αPD-L1 treatment efficacy and its underlying mechanisms remain unclear. Meanwhile, inadequate tumor drug accumulation and glycolysis significantly restrict the efficacy of cuproptosis. To address these challenges, we have synthesized a novel nanozyme, Pt@PCN-Cu, designed to stabilize intracellular copper accumulation and effectively induce cuproptosis. Additionally, we aim to determine whether this strong induction of cuproptosis can synergize with αPD-L1 to enhance cancer therapy, ultimately paving the way for novel strategies to improve PDAC treatment. Methods Pt@PCN-Cu was synthesized via a one-pot method, and its therapeutic potential was assessed in combination with αPD-L1 for the treatment of PDAC. Initially, the material’s properties were characterized, and its efficient cellular uptake was confirmed. Anti-tumor efficacy was evaluated by inducing cuproptosis in PDAC cell lines and xenograft models. RNA sequencing (RNA-seq) was utilized to identify key regulators involved in the modulation of PD-L1 expression by cuproptosis. Lastly, the therapeutic efficacy of Pt@PCN-Cu combined with αPD-L1 was evaluated in vivo, focusing on tumor growth inhibition and immune modulation within the tumor microenvironment (TME). Results Pt@PCN-Cu demonstrates excellent physicochemical properties and remarkable cascade catalytic activity, providing a solid foundation for further in vitro and in vivo studies. In vitro, Pt@PCN-Cu efficiently transports copper and induces cuproptosis primarily through mitochondrial dysfunction. Mechanistic studies show that Pt@PCN-Cu triggers the dissociation of hexokinase 2 (HK2) from mitochondria, leading to a reduction in HK2 activity. This decline in HK2 activity impairs glycolysis, a metabolic pathway essential for tumor energy metabolism, which in turn results in elevated PD-L1 levels. In vivo, Pt@PCN-Cu demonstrates excellent safety and accumulates at the tumor site in a subcutaneous PDAC mouse model, inducing cuproptosis. Moreover, the combination of Pt@PCN-Cu with αPD-L1 further enhanced its therapeutic efficacy and effectively reprogrammed the immunosuppressive TME. Conclusion This study presents strong evidence confirming the safety and therapeutic potential of Pt@PCN-Cu in PDAC treatment. Importantly, Pt@PCN-Cu not only induces cuproptosis but also significantly enhances antitumor efficacy in combination with αPD-L1 by regulating PD-L1 expression through HK2 modulation. These findings underscore a more effective and innovative approach for treating PDAC.
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RSC Advances
·
2015
·Vol. 5
·期 91
·74899-74906
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IF 3.84
Weihua Wang,Mingda Zhu,Xiaolin Lu,Yanfang Gao,Lijun Li,Zhenzhu Cao,Caihong Li,Jinrong Liu,Haitao Zheng
Oxygen storage capacity is influenced by the morphology and crystal-plane(s) of CeO2, which can thus affect the ability of this material to oxidise carbon monoxide. To investigate the effect of different morphologies/crystal-planes of CeO2 on the electrocatalytic performance of DMFCs (Direct Methanol Fuel Cell), three different types of CeO2 nanocrystals with different crystal-planes were synthesised and later assembled into Pt–xCeO2/Graphene composites with graphene and Pt nanoparticles as the electrocatalyst for DMFCs. According to the HRTEM images, the original morphology and crystal-plane structures of CeO2 are essentially maintained in the three types of Pt–xCeO2/Graphene composite catalysts investigated in this work. The catalytic performance of the Pt–xCeO2/Graphene composites for methanol electrocatalytic oxidation was investigated by a series of electrochemical measurements. Compared with the other catalysts, Pt–rCeO2/Graphene demonstrates superior catalytic activity (onset potential: 0.15 V) and the strongest resistance to poisoning by carbonaceous species (If/Ib: 2.11). The results of H2-TPR shows that rCeO2 with the {110} facet has the best surface reducibility among the xCeO2 with different facets being investigated, which provides a rationale for the superior performance of the Pt–rCeO2/Graphene catalyst. This study indicates that metallic oxides with a suitable crystal plane and shape can effectively enhance the electrocatalytic performance of Pt-based catalysts for methanol electrooxidation.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
·
IF 8.3
Weijing Cao,Xu Chen,Fulong Liu,Xiaoli Gu,Yan Qing,Zupeng Chen
Lignocellulose biomass, a plentiful and renewable resource found in abundance on Earth, holds significant promise in reforming into H 2 and value-added biochemicals like lactic acid through photocatalytic technology. However, the efficient photorefinery encounters challenges, including the recombination of photo-induced carriers, poor H 2 evolution, and slow biomass oxidation. Here, we report a bimetallic catalyst supported on layered carbon nitride (PtRh/CN) for lignocellulose photoreforming. This catalyst combines the synergistic effects of Pt and Rh, enhancing both the absorption of visible light and the separation and migration of photogenerated charge carriers. The optimal catalyst achieves a high hydrogen production rate of 6.1 mmol g −1 h −1 and a lactic acid yield of 92.9 %. Mechanistic studies using specific scavengers demonstrate that e − , h + , 1 O 2 , ⋅O 2 − , and ⋅OH species all facilitate the simultaneous production of hydrogen and lactic acid. This study not only advances the efficient utilization of lignocellulose biomass but also provides a novel framework for designing highly efficient photocatalysts for photoreforming biomass into hydrogen and biochemicals.
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JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY
·
2019
·Vol. 19
·期 2
·877-881
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IF 1.093
Huynh Tai Thien,Pham Hau Quoc,Nguyen At Van,Nguyen Son Truong,Bach Long Giang,Ho Van Thi Thanh
In this work, mesoporous Ti0.7W0.3O2 materials with high conductivity and surface area as promising catalyst support for Pt in Proton-Exchange Membrane Fuel Cells (PEMFCs) were synthesized via a single-step solvothermal process at low-temperature without
using any surfactants or stabilizers. The characterizations of material are measured via XRD, TEM, SEM-EDS, and BET as well as electronic conductivity measurement. As a result, Ti0.7W0.3O2 formed a homogenous solid solution with mesoporous anatase-TiO2
structure and uniformly spherical nanoparticles morphology of about ~10 nm diameter, together with a high electrical conductivity of 0.022 S/cm compared to that of undoped-TiO2 (1.37×10−7 S/cm), which implied that tungsten (VI) ions was successfully doped
into anatase-TiO2 lattices. The N2 adsorption/desorption isotherms indicated that Ti0.7W0.3O2 is being mesoporous structure with high surface area up to ~202 m2/g, which is nearly similar to that of the commercial Vulcan XC72
(~232 m2/g). The Pt nanoparticles was easily anchored onto Ti0.7W0.3O2 surface by the chemical reduction process using NaBH4 as a reducing agent. The spherical Pt nanoparticles of ~9 nm in diameter were deposited uniformly on the mesoporous support.
These results suggested that mesoporous Ti0.7W0.3O2 materials synthesized are promising catalyst supports to replace carbon-based supports for Proton-exchange membrane fuel cells.
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JOURNAL OF POROUS MATERIALS
·
2021
·Vol. 29
·期 1
·49-61
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IF 2.496
Liu Wei,Zhang Guoliang,Hao Songyuan,Yuan Hong,He Weidong
Waste cooking oils (WCOs) are a cheap and rich source of carbon and hydrogen, and they exhibit great potential for the preparation of hydrogen gas and carbon nanomaterials. Here, we prepared three Pt–Ni/SBA-15 catalysts with Pt contents ranging from 0 to 2% to examine their activity in the catalytic cracking of WCO towards the production of hydrogen and carbon nanotubes (CNTs). A mixture of soybean oil, oleic acid and animal fat was used as a model compound of WCO, and the catalysts were characterised by inductively coupled plasma–optical emission spectrometry, scanning and transmission electron microscopy, X-ray diffraction, N 2 adsorption–desorption isotherms, temperature programmed reduction, thermogravimetric analysis and Raman spectroscopy. The effect of Pt loading and cracking temperature on the hydrogen production and the quality of CNTs was also evaluated. Among the prepared catalysts, 2%Pt–30%Ni/SBA-15 showed excellent catalytic activity at 750 °C, affording a maximum hydrogen content of 66.2 vol%, while CNTs with diameters of 20–100 nm and high crystallinity, oxidation stability, graphitisation and purity were also prepared.
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ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Chen Tai,Huarong Liu,Yuan Hu
Hydrogen is a very promising green energy alternative to fossil fuel owing to both environmental friendliness and high-energy nature; however, improving the hydrogen production efficiency of photocatalysts under visible light has remained a challenge. Herein, CdS/Pt/MIL-125 nanocomposite has been fabricated using γ-ray irradiation, where Pt and CdS nanoparticles with clean surfaces are well dispersed inside and on the surface of MIL-125, respectively, which greatly promotes effective space separation of photogenerated carriers and thus improves the visible-light catalytic activity. The hydrogen generation rate of CdS/Pt/MIL-125 nanocomposite is found up to 6783.5 μmol/(g·h) under visible-light illumination, which is 7.3 times that of CdS/MIL-125 without Pt as electron trap reservoirs and 4.4 times that of Pt/CdS/MIL-125 without effective spatial separation between CdS and Pt. The reason is attributed to the synergy of ternary CdS/Pt/MIL-125 with a unique ordered mesoporous structure that may widen the absorption range of the light, improve the efficiency of light harvesting, facilitate mass transfer, prevent the aggregation of CdS and Pt nanoparticles, suppress the electron–hole (e–h) pair recombination, and provide more active sites. Moreover, the loading amount of Pt or CdS nanoparticles also affects the activity of CdS/Pt/MIL-125 nanocomposite for visible-light catalytic H2 evolution. In view of the extensive use of γ-ray irradiation in industry, this research presents a rational route to the fabrication of novel hybrid photocatalysts for improved visible-light catalytic hydrogen evolution.
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SOLID STATE PHENOMENA
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2018
·
IF 0
Hau Quoc Pham,Tai Thien Huynh,At Van Nguyen,Anh Tram Ngoc Mai,Vi Thuy Thi Phan,Long Giang Bach,Trinh Duy Nguyen,Van Thi Thanh Ho
The tungsten-modified titanium dioxide, which prepared through the one-pot solvothermal process, exhibited the large specific surface area (~ 202 m2/g) and greater electrical conductivity (~ 0.022 S/cm). Furthermore, for the comparison purpose to find appropriate approach for the synthesis 20 wt. % Pt NPs/Ti0.7W0.3O2 catalyst, the modified chemical reduction utilizing NaBH4 and the rapid microwave-assisted polyol using ethylene glycol were employed without any surfactants or stabilizers. The characterization of Pt-based electrocatalyst was investigated through XRD, SEM-EDX, TEM measurements. As result, the platinum nanocatalyst formation with the face-centered cubic structure (fcc) and the amount loading on Ti0.7W0.3O2 support approximately 20 wt. % of two synthesized methods. However, the diameter size and distribution of Pt nanoforms have clearly classified in two reduction route. For example, the Pt nanocatalyst, which was created by the rapid microwave-assisted polyol at 160 °C for 2 min, exhibited the good distribution on support with ~3 nm diameter. This could be ascribed to the fast and uniform heating of microwave-assisted and moderate reducing possibility of ethylene glycol. These results indicate that the rapid microwave-assisted polyol was an appropriate approach not only for synthesizing 20 wt. % Pt NPs/Ti0.7W0.3O2 catalyst but also for preparing Pt-based electrocatalysts.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 30
·16427-16435
·
IF 12.732
Xue Zhao,Mai Zheng,Zhenyang Zhang,Yufeng Wang,Yingtang Zhou,Xiaohai Zhou,Haibo Zhang
Electrochemical hydrogen evolution reaction (HER) is a green and convenient way to produce hydrogen with high calorific value and zero environmental pollution, but the precious metal Pt, which catalyzes its efficient operation, faces the dilemma of resource scarcity. Before finding an HER catalyst to replace platinum-based materials, morphology control engineering can achieve high-efficiency hydrogen production with a lower platinum input. Here, we used a supramolecular assembly (host: cucurbituril[7]; guest: closo-[B12H12]2−) with weak reducibility as a carrier to convert Pt4+ into ultrafine and highly dispersed Pt nanoparticles (BOPs@Pt) in situ, and the supported Pt-based catalyst (BC3N@Pt) obtained after pyrolysis had the ability to very efficiently catalyze HER. BC3N@Pt exhibited excellent performance in catalyzing HER in the full pH range. Among them, the overpotentials to achieve a current density of 10 mA cm−2 in the media of pH = 14, pH = 7 and pH = 1 were only 26.1 mV, 38.5 mV and 23.1 mV, respectively, and the corresponding Tafel slopes were as low as 41.59 mV dec−1, 59.05 mV dec−1, and 61.07 mV dec−1, respectively. In terms of mass activity, the rate of HER driven by BC3N@Pt was at least three times than that achieved with the commercial 20 wt% Pt/C. The density functional theory (DFT) calculations verified that B doped on CN changes the local electronic distribution, facilitates water dissociation and hydrogen adsorption, and hence enhances the HER activity. The annealing treatment converts the organic polymer into an inorganic BC3N matrix, which not only accelerates the electron transfer rate in HER, but also ensures the stability of BCN@Pt when catalyzing HER in the entire pH range.
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Small
·
2025
·
IF 12.1
Chenggong Zhu,Qunfang Huang,Ruijie Fu,Zhen Xun,Qishui Ou,Yunlei Xianyu,Can Liu
Hepatitis B virus (HBV) infection remains a significant global public health issue, and rapid detection of HBV DNA is crucial for disease prevention and control. However, traditional methods for HBV DNA detection are limited by their reliance on precise instruments and single readout, which can hardly meet the requirements of on-site detection. In this study, the Mg 2+ -enhanced trans-cleavage activity of clustered regularly interspaced short palindromic repeats/associated protein 12a (CRISPR/Cas12a) is reported and coupled with loop-mediated isothermal amplification (LAMP) and Au@Pt nanoparticles as a signaling reporter for on-site detection of HBV DNA. This triple-modal biosensing strategy enables multiple signal readouts including UV–vis spectrum, RGB value, and temperature with high sensitivity and accuracy. The linear detection ranges using UV–vis spectroscopy, RGB color recognition, and photothermal modes are from 50 to 10,000 copies µL −1 , with the limitation of detection of 24.07, 39.65, and 23.33 copies µL −1 , respectively. This biosensing strategy is further employed for the qualitative detection of HBV DNA in 48 serum samples, achieving sensitivities of 100%, 100%, and 95.24% for triple modes. This work offers a promising tool of next-generation LAMP-CRISPR/Cas12a for the rapid and portable detection of nucleic acids.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Yuxuan Xie,Xinyu Yang,Zhao Li,Ziruo Zeng,Shuangyou Bao,Xin Sun,Yixing Ma,Kunlin Li,Chi Wang,Fei Wang,Ping Ning,Kai Li
High-electron-density Pt 0 nanoparticles (NPs) with excellent hydrogen activation and spillover capacity offer unique advantages in volatile organic sulfur selective hydrogenation reactions. Taking advantage of the more preferential and effective anchoring of Mo atoms at the γ-Al 2 O 3 terminal hydroxyl (OH) groups and its electron modification role, competitive anchoring is induced by a simple co-impregnation synthesis method to promote the agglomeration of low-loading Pt atoms into high concentrations of electron-rich and enlarged Pt NPs, which resulted in a substantial increase in the active centers for hydrogen dissociation. The Mo doping amount with the best Pt aggregation efficiency is 3 wt.%, and the hydrogen spillover efficiency of 1Pt3Mocom/Al catalyst is significantly higher than that of 1Pt/Al catalyst, which efficiently convert carbon disulfide (CS 2 ) (95%–100%) while maintaining a methanethiol (CH 3 SH) selectivity of 85% at 250 °C or a methane (CH 4 ) selectivity of 92% at 310 °C in the 24 h long-term test. In situ DRIFTS revealed that the improved catalyst performance is due to the elevated capacity to generate the intermediates HCSS * , CH 2 S * , and CH 3 S * . The 1Pt3Mocom/Al catalyst synthesized by competitive anchoring strategy greatly reduces the Pt consumption and is instructive for the exploitation of low-cost Pt NPs active centers.
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Petroleum Science
·
2025
·
IF 6.1
Chuan-Hao Zhang,Qi Dong,Fei Wang,Ning-Yue Lu,Feng Yu,Bin-Bin Fan,Rui-Feng Li
Deep hydrogenation of polycyclic aromatic hydrocarbons (PAHs) into jet fuel is an important strategy for the upgrading of light cycle oil (LCO). Zeolite-supported metal catalysts have exhibited good catalytic performance for hydrogenation of PAHs under relatively mild conditions. However, the impacts of acidity variations in zeolite supports, arising from the differences in framework Al (Al F ) distribution on the catalytic behavior of zeolite-supported metal catalysts in the deep hydrogenation of PAHs remains unclear. Herein, two series of mesoporous ZSM-5 samples, that is ZSM-5-E- x and ZSM-5-F- x , with the differences in Al F distribution but similar Si/Al ratios, were prepared in the crystallization system with or without NaOH. The results of NH 3 -TPD, Pyridine-IR, N 2 adsorption-desorption and SEM reveal that two series of HZSM-5 samples have similar acid density and acid strength, textural properties, morphology and particle size. However, the results of XPS, 27 Al MAS NMR, 2,6-Ditert-butylpyridine-IR, catalytic cracking of 1,3,5-triisopropylbenzene and the controlled reactions as well as DFT calculation indicate that the higher enrichment degree of Al F on the external surface and the suitable arrangement mode of Al F in ten-membered ring (10-MR) of HZSM-5-F- x compared to HZSM-5-E- x in case of the similar Si/Al ratios, result in Pt/HZSM-5-F- x exhibiting remarkably-improved deep hydrogenation performance of phenanthrene (PHE) compared to Pt/HZSM-5-E- x . Particularly, the selectivity to perhydrophenanthrene (PHP) over Pt/HZSM-5-F-50 can reach above 99.0% at a conversion of PHE (>99.0%). Furthermore, Pt/HZSM-5-F-50 exhibits well reusability. This work helps to clarify the impact of Al F distribution in ZSM-5 on catalytic hydrogenation performance for PAHs, providing valuable guidance for design and development of efficient catalysts for the hydrogenation of PAHs.
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