Nanoscale
·
2025
·
IF 5.1
Bo Li,Lipan Luo,Yujia Liu,Xiaohan Zhou,Yuyu Zhang,Lishuai Song,Nan Liu,Qing Tang,Zequan Li
Pt/TiO2 photocatalysts were synthesized using incipient wetness impregnation followed by oxidative and/or reductive thermal treatments. The loading dimensions of Pt elements on the TiO2 surface (PtP, PtSA, and PtC) were controlled by varying the impregnated solution. Experimental results demonstrate that PtC with intermediate size exhibits the highest photolysis rate under 300W xenon lamp irradiation, achieving a hydrogen yield of 11.42 mmol g^-1 h^-1 and an apparent quantum yield of 40.65%. Similarly, Ru/TiO2 and Ir/TiO2 photocatalysts prepared under the same conditions exhibited the same pattern. Photoelectrochemical tests reveal that PtC/TiO2 has the narrowest band gap, the highest interfacial charge transfer capacity, and the greatest carrier separation efficiency. DFT calculations indicate that PtC/TiO2 has the most suitable d-band center, resulting in a close-to-zero ΔGH* value of 0.05 eV. This optimal value significantly balances the adsorption and desorption of hydrogen intermediates (H*) during the photocatalytic hydrogen evolution (PHE) reaction. This study provides new insights into the preparation of precious metal-loaded photocatalysts.
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PubMed
高影响因子
ACS Applied Nano Materials
·
2021
·
IF 5.097
Ruya Guo,Li Xue,Gaozhe Cai,Wuzhen Qi,Yuanjie Liu,Jianhan Lin
Early screening of Salmonella is of utmost importance to minimize the incidence of related foodborne diseases. Here, we reported an immunosensor to fast detect Salmonella using Fe-MIL-88NH2 metal–organic framework (Fe-MOF) nanocubes to load platinum nanoparticles (PtNPs) for signal amplification and smartphone thermal imaging to monitor the temperature change. The Fe-MOF nanocubes decorated with PtNPs (Fe-MOF/PtNPs) were prepared as peroxidase mimics to catalyze hydrogen peroxide (H2O2) to produce O2. The immune magnetic nanoparticles (MNPs), the target bacteria, and the immune Fe-MOF/PtNPs were first mixed by the three-dimensional (3D) chaotic micromixer and conjugated in the microfluidic chip to form MNP–bacteria–Fe-MOF/PtNPs sandwich complexes. After magnetic separation and washing, H2O2 was injected and decomposed by Fe-MOF/PtNPs on the sandwich complexes to generate O2 in a sealed chamber. The increase in the pressure pushed the preloaded water to react with calcium oxide powder, resulting in the generation of heat, which was measured using the smartphone-based thermal sensor to determine the bacteria. The microfluidic immunosensor could detect Salmonella as low as 93 CFU/mL within 1 h.
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Journal of Materials Chemistry A
·
2025
·Vol. 13
·期 41
·35690-35700
·
IF 9.5
Quanming Ren,Xiaoya Zhao,Liping Zhou,Linghe Song,Juntai Tian,Jisheng Nie,Peng Liu,Daiqi Ye,Zhi Wang
Metal–support interaction (MSI) plays an essential role in affecting the catalytic activity of supported catalysts by establishing a unique interface between metal and the support. However, moderate modulation of MSI remains a major challenge, as both too weak and extremely strong MSI can lead to catalysts exhibiting inferior catalytic activity. Herein, a series of Pt catalysts supported on ceria with various levels of sodium modification were prepared via a facile impregnation method. A comprehensive investigation based on experimental studies and Density Functional Theory (DFT) calculations substantiates that the addition of sodium, as an effective motivator, triggers more significant electron transfer from Pt clusters to the CeO2 support accompanied by the formation of an interfacial sites (Ptδ+–OV–Ce3+), indirectly involved in reactions to decrease the activation energy of lattice oxygen in Pt–O–Ce, and Pt/1.1Na–CeO2 with moderate MSI is conducive to the oxygen species on the CeO2 adjacent to the Ptδ+ (e.g. Ptδ+–OV–Ce3+) configuration at the interface to take part in toluene oxidation. And the perimeter Pt0–OV–Ce3+ sites, as the active site, were formed by the Pt nanoparticles on the CeO2 for toluene adsorption. Pt/1.1Na–CeO2 (1.57 nm) with small particle size possesses a much larger number of perimeter Pt0–OV–Ce3+ sites than Pt/CeO2. Therefore, the catalytic activity and stability of Pt/1.1Na–CeO2 were remarkably enhanced in toluene oxidation compared to those of Pt/CeO2. This work emphasizes that alkali can be employed as a motivator to regulate MSI, providing a facile and powerful approach to design efficient catalysts for VOC oxidation.
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高影响因子
MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Xuan-Yu Yang,He-Jie Wang,Hao-Nan Chen,Li-Juan Yue,Fei-Long Gong,Ke-Feng Xie,Shi-Zhong Wei,Yong-Hui Zhang
Electronic modulation of Pt sites is of great significance in catalytic reaction involved chemical engineering process. Alkali metal doping is a promising strategy to modify the d orbit of Pt, which can effectively affect the reaction between material and adsorbates, however, the relationship is still unclear. Here, we have rationally designed Pt-modified Na-doped WO 3 nanorods, and the electronic modulation of Pt can be finely modified by Na doping. The Pt-Na/WO 3 -Ar nanorods exhibit excellent H₂S sensing performance, with high response (R a /R g = 701 @ 1 ppm), low operating temperature (110 °C), and detection limit as low as 2.42 ppb. Experimental and theoretical results indicate that the introducing of Na effectively enhances the interaction between Pt nanoparticles (NPs) and WO 3 . Additionally, Na doping successfully modulate the d-band center of Pt, optimizing the adsorption and desorption processes during sensing. The synergistic effects of these components enable the Pt-Na/WO 3 -Ar sensor to exhibit outstanding H₂S sensing performance. Notably, the fabricated sensors are further used to monitor the hydrogen sulfide (H 2 S) of halitosis biomarkers, which holds significant application potential in environmental protection and medical diagnostics.
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Journal of Biomedical Nanotechnology
·
2022
·Vol. 18
·期 9
·2264-2277
·
IF 3.641
Du Lidong,Zhang Ruoyu,Zhao Lei,Tang Shaojian,Hou Zhaohua,Xue Peng
Aim: To assess the anticancer activity of nanoparticles synthesized via a green method using American ginseng (AG). Methods: Stem-leaf saponins from AG (SAG) and heat-transformed stem-leaf saponins from AG (TSAG) were used to synthesize different SAG nanoparticles (SAG-NPs)
and TSAG nanoparticles (TSAG-NPs). The NPs were characterized, and their anticancer activity was assessed in vitro. Results: The NPs, which differed in size (16.69 nm∼253.8 nm), were spherical or polyhedral with a low PDI and good stability. The TSAG-NPs inhibited cancer
cells by inhibiting proliferation, promoting cancer cell apoptosis and directly leading cancer cells to necrosis. The small cell lung cancer cell line (SCLC) NCI-H446 was the most sensitive to the TSAG-AgNPs, with an IC50 value of 20.71±2.38 μg/mL, and the TSAG-AgNPs
inhibited invasiveness and reduced the risk of metastasis. Conclusion: TSAG-AgNPs, selected from many SAG-NPs and TSAG-NPs, are sensitive to SCLC and provide a new approach to the currently limited treatment.
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Nature Communications
·
2025
·Vol. 17
·期 1
·90
·
IF 15.7
Tuo Yongxiao,Qu Jingying,Sun Huailu,Lu Qing,Wang Bin,Gai Hongwei,Yin Defu,Feng Xiang,Chen De
Catalyst design is often reaction-specific due to the lack of universal descriptors linking molecular structures to optimal active-site configurations. Here, we uncover a reactant-dependent volcano relationship in Pt-catalyzed dehydrogenation, governed by the Pt-Pt coordination number (CN Pt-Pt ). Using a tunable Pt/MgAl 2 O 4 system, we identify optimal CN Pt-Pt values of ~2.5, ~4.7, and ~7.0 for cyclohexane, methylcyclohexane, and decalin, respectively. This activity trend is explained by an orbital hybridization-guided mechanism, where optimal activity emerges from a balance between C-H bond activation and product desorption, mediated by the interactions between Pt d-orbitals and the π* orbitals of dehydrogenated intermediates. We introduce the LUMO energy of aromatic products as a universal electronic descriptor that serves as a proxy for π* orbital energy. LUMO energy shows strong linear correlations with the d-band center of Pt at the optimal CN Pt-Pt , enabling rational tuning of electronic interactions across diverse reactants. The optimized Pt/MgAl 2 O 4 catalyst delivers 2-3 times higher activity with >100 h stability under industrial conditions at only 300 o C, offering a robust strategy for hydrogen release and active-site engineering in dehydrogenation catalysis.
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Catalysts
·
2025
·Vol. 15
·期 11
·
IF 4
Juan Du,Wanting Qiu,Sunbal Ayaz,Jian Long,Wenze Guo,Ling Zhao,Zhenhao Xi
2,5-furandicarboxylic acid (FDCA), a high-value biomass-derived monomer, serves as a crucial building block for sustainable polymers including polyesters, polyamides, and polyurethanes. This study systematically investigated the catalytic oxidation of 5-hydroxymethylfurfural (HMF) to FDCA over Pt/Al2O3and Pt–Bi/Al2O3catalysts. The 5Pt/Al2O3catalyst yielded 60.6% FDCA after 12 h under optimized conditions (80 °C, 0.1 MPa O2, 1 equiv. Na2CO3). Remarkably, Bi-modified 5Pt–1Bi/Al2O3catalyst dramatically enhanced catalytic performance, achieving 94.1% FDCA yield within 6 h under optimized conditions (80 °C, 1.5 MPa O2, 2 equiv. Na2CO3). Comprehensive characterization revealed that the exceptional activity originates from Bi–O–Pt interactions that modulate the electronic structure and oxidation state of Pt active sites, which facilitates the oxidation of intermediate 5-formyl-2-furancarboxylic acid (FFCA) to FDCA, the rate-limiting step of HMF oxidation. This work demonstrates an efficient Bi-promoted Pt catalytic system for FDCA production with significant potential for industrial application.
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Catalysts
·
2025
·Vol. 15
·期 3
·220
·
IF 4
Jiani Chen,Yanxuan Wang,Jianghua Huang,Shuting Ma,Yiyang Zhang,Fukun Bi,Xiaodong Zhang
Nowadays, volatile organic compounds (VOCs) increasingly jeopardize ecosystem sustainability and human well-being. In this study, UiO-66 and its different electron beam (EB) irradiation doses (100, 300, 500 kGy) modified materials supported Pt catalysts, Pt/UiO-66 and Pt/UiO-66-X (X = 100, 300, and 500, representing the irradiation doses), were synthesized, and a series of characterizations were conducted on the samples. On this basis, the effectiveness of these catalysts was evaluated through the degradation of ethyl acetate. The study findings indicated that the sample irradiated at 100 kGy demonstrated superior catalytic performance. Thereafter, extensive tests with regard to water resistance, stability, and cycle performance indicated that the Pt/UiO-66-100 catalyst was characterized by satisfactory reusability and catalytic stability, even when faced with high heat and humidity. Further work with in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and thermal desorption–gas chromatography–mass spectrometry (TD-GC–MS) uncovered the process of degradation of ethyl acetate. This research provides a guideline for the design of high-performance VOC degradation catalysts through EB modification.
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Nano Research
·
2024
·Vol. 17
·期 7
·5835-5844
·
IF 9.5
Liu Yu,Shi Yawen,Wang Hua,Zhang Shengbo
Photocatalytic hydrogen generation from hydrogen storage media is an effective and promising approach for the green hydrogen industry as well as for achieving carbon neutrality goals. However, the lower photocatalytic efficiency due to the limited light trapping capacity, low electron transfer rate, and severe aggregation of nanoparticles caused by high surface energy seriously restricts their practical application. Herein, we constructed a series of donor–acceptor (D–A) type covalent organic frameworks to confine ultrafine bimetallic Pt-based nanoclusters for photocatalytic hydrogen generation from ammonia borane (AB) hydrolysis. Under visible light irradiation at 20 °C, PtCo 2 @covalent organic framework (COF) showed the highest photocatalytic activity with a turnover frequency (TOF) of 486 min −1 . Experiments and density functional theory (DFT) calculations reveal that the high catalytic activity is mainly attributed to the strong electronic interactions between D–A type COF and ultrafine PtCo 2 nanoclusters. Specifically, the D–A type COF can significantly enhance the light-trapping ability by fine-tuning the electron-acceptor type in the framework, and accelerate the photogenerated electron transfer from D–A type COF to PtCo 2 nanocluster, which promotes the adsorption and activation of H 2 O and AB molecules and accelerates hydrogen release. Furthermore, PtCo 2 @COF also exhibited ultra-high durability due to the significantly enhanced resistance to nanocluster aggregation caused by the nanopore confinement effect of D–A type COF. We believe that this work will provide a theoretical guide for the rational design of efficient D–A COF-based catalysts for photocatalysis.
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Jiao Chen,Hongye Qin,Yaping Pan,Jinli Wu,Jianan Liu,Wanying Lin,Jun Jiang,Enzuo Liu,Junwei Sha,Fang He,Liying Ma,Naiqin Zhao
It is necessary and challenging to develop platinum-based electrocatalysts with low Pt content and high performance for industrial development in a suitable strategy. Herein, ultralow Pt (0.35 wt%) loading Ni(OH) 2 nanosheets (named as 2-Pt/Ni(OH) 2 ) with cataphracted structure is synthesized on nickel foam by one-step hydrothermal process. It only needs an overpotential of 34 mV to achieve a current density of 10 mA cm -2 without any significant decrease for 40 hours. This excellent performance of hydrogen evolution reaction (HER) is attributed to the fact that the cataphracted structure not only has a larger active area and more active sites, but also effectively limits the size of Pt nanoparticles to 2~3 nm, which results in a higher active quality. In addition, the relatively simple and easily operational one-step method can reduce the Pt content to 0.35 wt% significantly. This facile strategy opens up new approaches in the rational design and synthesis of low loading Pt electrocatalysts with eminent electrocatalytic activity for industrial production.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Yaru Wang,Jianjun Zhao,Xianqiang Xiong,Shengwei Liu,Yiming Xu
Anatase TiO 2 is the most studied environmental photocatalyst, but its efficiency is still not high enough to enable application. Herein we report a positive effect of Ni 2+ ions on the photocatalytic reaction in neutral aqueous solution. On addition of 1 mM Ni(ClO 4 ) 2 , the rates of phenol oxidation on TiO 2 and 0.5 wt.% Pt/TiO 2 increased by factors of 2.1 and 8.0, respectively. Meanwhile, the formation of organic intermediate was reduced, and the removal of total organic content was enhanced. Interestingly, Ni 2+ concentration did not change with irradiation time. Moreover, a maximum rate of phenol degradation was observed with Ni 2+ ions, occupying half the surface of TiO 2 or Pt/TiO 2 , where Ni(OH) + was more active than Ni(OH) 2 . X-ray photoelectron spectroscopy identified a Ni 3+ species produced in absence of phenol. A (photo)electrochemical study revealed that Ni 2+ oxidation was favored over H 2 O oxidation, whereas Ni 2+ and Pt inhibited and facilitated O 2 reduction, respectively. It is proposed that the adsorbed Ni(OH) + on TiO 2 is oxidized to Ni 3+ by the photogenerated holes of TiO 2 , followed by regeneration through phenol oxidation. The Ni 2+ -catalyzed organic oxidation then promotes the Pt-catalyzed O 2 reduction, and vice visa, resulting into the greatly improved efficiency of charge separation. This work highlights the possibility of Ni 2+ ions as the hole mediator of organic oxidation over a semiconductor.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2020
·Vol. 167
·期 14
·146509
·
IF 3.721
Yijun Liu,Suyu He,Fengping Zhan,Feng Gao,Wei Sun,Qingxiang Wang
Developing robust and low-cost electrocatalysts for efficient hydrogen evolution reaction (HER) through facile methods is of great significance to the energy and environment sustainability. Herein, a simple one-pot solvothermal method has been developed to synthesize a hybrid material of nickel@nickel carbide (Ni@Ni3C) nanochain embedded in a network of single-walled carbon nanotubes (SWCNTs). The electrochemical experiments indicate that the composite of Ni@Ni3C-SWCNTs has the HER electrocatalytic performance comparable to that of Pt/C in an acidic medium (0.5 M H2SO4). The overpotential to reach a current density of 10 mA cm−2 in 0.5 M H2SO4 is only −74 mV with a Tafel slope of 46.9 mV dec−1. Compared to Ni@Ni3C in the absence of SWCNTs, the enhanced HER performance of Ni@Ni3C-SWCNTs can be attributed to the increased intrinsic activity, improved electronic conductivity, and the electron coupling effect between Ni@Ni3C and SWCNTs. The Ni@Ni3C-SWCNTs composites also show high stability at the overpotential of −0.2 V for 24 h. This work provides guidance for the synthesis of high-performance non-precious metal electrocatalysts for HER.
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