JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Shilong Zhong,Haixian Shi,Chengwei Xiao,Xirui Gu,Jing Wu,Shaolin Lu,Zhongke Yuan,Yuzhao Yang,Dingshan Yu,Xudong Chen
Constructing single-atom catalysts (SACs) using organic porous framework materials as supports presents a promising approach for developing highly efficient photocatalysts for hydrogen evolution. However, the fabrication of SACs that are both highly stable and active poses a significant challenge, particularly in the precise anchoring of metal single atoms. In this study, we utilized 1,3,6,8-tetra (p-methyl benzoate) pyrene as a ligand to synthesize pyrene-based hydrogen-bonded organic frameworks (denoted as PFC-1) through a self-assembly approach. Subsequently, a liquid-phase photoreduction process was employed to deposit noble metal platinum (Pt) onto PFC-1, resulting in the fabrication of SACs (PFC-1@Pt). Characterization results confirmed that Pt existed in a monatomic state, anchored through Pt C and Pt O coordination bonds with PFC-1. Serving as electron capture and separation centers, the Pt single atoms effectively suppressed electron-hole recombination, thereby prolonging carrier lifetimes. Consequently, the PFC-1@Pt SAC exhibited efficient hydrogen evolution performance with a rate of 2202.5 μmol g −1 h −1 and maintained photocatalytic activity for over 40 h. Our findings provide a systematic approach for developing efficient and stable SACs based on HOFs, expanding the potential applications of HOF materials in photocatalysis.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Wenchen Ren,Huanxi Wang,Qianlin Zhang,Mengchi Chen,Zhongrui Li,Huan Guo,Jing Bai,Xiaomin Dai,Santosh Kumar Verma,Yunhua Xu
In this paper, petal sheet layered Co-Al bimetallic hydroxides were prepared using the hydrothermal method using methanol as a solvent. Pt/Co-Al-O catalysts were produced after the impregnation method and H 2 reduction. This catalyst was applied to the dehydrogenation reaction process of methylcyclohexane to toluene. A fixed-bed reaction device carried out comparative tests of this series of catalysts, and the effect of Co addition on the performance of Pt/Co-Al-O catalysts was investigated in detail. Among them, the Pt/Co 3 -Al 1 -O catalyst showed the best performance with high toluene selectivity throughout the dehydrogenation process. The MCH conversion started to be greater than 90% at 330 °C, and the hydrogenolysis rate was 262.7 mmol/g Pt /min. The conversion gradually increased with the reaction temperature, and the conversion could reach 99.5% at 410 °C. The appropriate introduction of Co element can reduce the excessive strong acidic sites of Al 2 O 3 itself and retain a certain number of weak acidic sites, while the bimetallic hydroxide carrier improves the dispersibility of the active component, reduces its particle size, and forms a certain strong interaction between the carrier and Pt. The final conversion of the catalyst decreased by about 2% in the 100 h stability test at 380 °C, which indicated that the Pt/Co 3 –Al 1 –O catalyst had strong coking resistance and good stability. These results indicate that the Pt/Co–Al–O series catalysts have potential industrial applications in hydrogen energy utilization.
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Nature Communications
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2024
·Vol. 15
·期 1
·1-10
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IF 14.7
Fang Cao,Xu Chang,Zhang Wei,Zhou Meng,Tan Dong,Qian Lixia,Hu Daqiao,Jin Shan,Zhu Manzhou
Dual emission (DE) in nanoclusters (NCs) is considerably significant in the research and application of ratiometric sensing, bioimaging, and novel optoelectronic devices. Exploring the DE mechanism in open-shell NCs with doublet or quartet emissions remains challenging because synthesizing open-shell NCs is difficult due to their inherent instability. Here, we synthesize two dual-emissive M 1 Ag 13 (PFBT) 6 (TPP) 7 (M = Pt, Pd; PFBT = pentafluorobenzenethiol; TPP = triphenylphosphine) NCs with a 7-electron open-shell configuration to reveal the DE mechanism. Both NCs comprise a crown-like M 1 Ag 11 kernel with Pt or Pd in the center surrounded by five PPh 3 ligands and two Ag(SR) 3 (PPh 3 ) motifs. The combined experimental and theoretical studies revealed the origin of DE in Pt 1 Ag 13 and Pd 1 Ag 13 . Specifically, the high-energy visible emission and the low-energy near-infrared emission arise from two distinct quartet excited states: the core-shell charge transfer and core-based states, respectively. Moreover, PFBT ligands are found to play an important role in the existence of DE, as its low-lying π * levels result in energetically accessible core-shell transitions. This novel report on the dual-quartet phosphorescent emission in NCs with an open-shell electronic configuration advances insights into the origin of dual-emissive NCs and promotes their potential application in magnetoluminescence and novel optoelectronic devices.
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Acta Biomaterialia
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2025
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IF 9.6
Sheng Xu,Ziwei Hu,Weihao Zheng,Chaozhen Qin,Xiaoyu Bai,Qinghua Yang,Tao Zeng,Dandan Mo,Bo Zhou,Chun Lu,Xiaomin Chen,Biying Tan,Jinmin Zhao,Li Zheng
Osteosarcoma (OS), a highly malignant primary tumor, poses significant threats. Chemotherapy remains the main treatment approach but is limited by low drug bioavailability, poor permeability, and notable side effects. Herein, a near-infrared light (NIR)-driven and GSH-responsive poly(ethylene glycol)-SS-polystyrene-doxorubicin and platinum nanoparticles (PSPDP) nanomotor, wherein disulfide bonds served as GSH sponsors and platinum nanoparticles as producers of reactive oxygen species (ROS) to induce cell apoptosis, combined with NIR-driven propulsion to enhance the inhibitory effect of encapsulated doxorubicin (DOX). The results demonstrated that the PSPDP nanomotor can be effectively driven due to its good photothermal properties, with its movement speed increased 2.10 times under NIR laser exposure. Additionally, the efficiency of DOX release increased with the increase in GSH concentration, demonstrating favorable GSH responsiveness. Pt-NPs also exhibited good photothermal properties, enabling self-thermophoresis to drive. Minimal cytotoxic effects of PSPDP were observed on a series of cell lines compared with DOX solution and Pt-NPs. Notably, the Pt-NPs generated a significant amount of ROS, synergistically enhancing the therapeutic effect of DOX, as evidenced by a 5.53-fold increase in OS cell growth inhibition and evident osteosarcoma growth inhibition in the nude mice model. Thus, the NIR-driven, localized, and low-toxic nanomotor may offer a promising therapeutic strategy for OS intervention. Statement of significance Enhancing drug penetration efficiency and developing delivery systems that respond to the tumor microenvironment to release drugs are effective strategies for treating osteosarcoma (OS). Here, a near-infrared (NIR) light-driven and glutathione (GSH)-responsive nanomotor, integrating poly(ethylene glycol)-SS-polystyrene-doxorubicin and platinum nanoparticles (PSPDP), was produced and used for OS treatment. This PSPDP nanomotor exhibits significant advancements in photothermal activation and self-thermophoresis, enabling a 2.10-fold increase in movement speed under NIR exposure. Such enhanced motility improves the localized delivery and controlled release of doxorubicin, thus increasing drug bioavailability and minimizing systemic toxicity. Additionally, the nanomotor's ability to generate reactive oxygen species significantly amplifies its therapeutic impact, evidenced by a remarkable 5.53-fold increase in tumor growth inhibition. These features make the PSPDP nanomotor a promising candidate for effective and targeted OS treatment strategies.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
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2025
·Vol. 172
·期 3
·034516
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IF 3.3
Fadong Miao,Yuanyi Xiang,Wenbin Tang,Rongzhong Yang,Yi Zhou,Qinghong Huang,Nengfei Yu,Yuping Wu
Designing efficient and stable oxygen evolution reaction (OER) catalysts is crucial for advancing water electrolysis technologies toward sustainable hydrogen production. Ruthenium pyrochlore oxide (A2Ru2O7−δ) has attracted much attention due to its high OER catalytic activity and low cost. However, their catalytic activity and stability require further improvement to achieve commercial viability. In this study, a series of Pt-deposited Yttrium ruthenate (Y2Ru2O7−δ, YRO) bifunctional catalysts Pt(x%)-Y2Ru2O7 were prepared by hydrothermal and heat treatment methods. In an acidic environment, the OER activity and stability were significantly improved compared with YRO, and hydrogen evolution reaction (HER) performance gradually improved. Among them, Pt(25%)-YRO showed excellent OER (η10 = 260 mV, 43.1 mV dec−1) and HER (η10 = 120 mV, 51.2 mV dec−1) performance. In addition, Pt(25%)-YRO demonstrated excellent catalytic stability, with both the OER and the overall water splitting reaction maintaining stable operation at 10 mA cm−2 for over 50 h. This provides a new approach for developing high-activity, high-stability, dual-function water electrolytic catalysts for use in harsh acidic environments.
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SENSORS AND ACTUATORS B-CHEMICAL
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2024
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IF 8
Changlin Xiao,Zhuang Zhuang Ma,Xiaotong Gao,Peijin Zou,Lichao Jia
LaFeO 3 has been widely investigated as formaldehyde sensing material due to its enhanced performance. However, several disadvantages including the response/recovery speed, selectivity, and detection limit mortally restrict its practical applications. Along these lines, herein, platinum (Pt) functionalized LaFeO 3 porous structures were synthesized to optimize the sensing properties. The sensing test revealed that the best response value of Pt functionalized LaFeO 3 was around 2.5 times over that of the pristine material at the operating temperature of 125 o C. Meanwhile, the sensor also possessed the merits of shorter response/recovery time, better selectivity, and lower detection limits. From our analysis, it was demonstrated that the abundant pore structure and the increased adsorbed oxygen level are responsible for the excellent formaldehyde monitoring properties. Our work paves the way for the development of novel Pt functionalized LaFeO 3 porous structures, which can serve as a potential candidate for formaldehyde detection in many practical applications.
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Molecular Catalysis
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2024
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IF 3.9
Mingzhen Huang,Jinxin He,Kaiji Xu,Dongren Cai,Guowu Zhan
The supported Pt/CeO 2 catalysts are widely used for the catalytic oxidation of CO at ambient conditions. Herein, we reported a new strategy for modifying the interaction between Pt and CeO 2 support via pulsed steam treatment, which significantly optimized the catalytic performance of Pt/CeO 2 for CO oxidation. Specifically, the hollow CeO 2 nanospheres were prepared by using carbon spheres as sacrificial templates and then subjected to pulsed steam treatment at 150 °C for different times to obtain the CeO 2 -xH support (x means the time of pulsed steam treatment, min). It was found that the complete oxidation of CO can be achieved at 90 °C over the Pt/CeO 2 –50H sample, which was much lower than that (130 °C) on Pt/CeO 2 without pulsed steam treatment. The XPS and in-situ DRIFTS characterizations were conducted to reveal the high performance of the Pt/CeO 2 –50H catalyst for CO oxidation. It was found that the valence state of Pt significantly controlled by pulsed steam treatment was critical to the catalytic activity, whereby the presence of two types of active sites (Pt 0 -CO and Pt δ+ -CO) over Pt/CeO 2 –50H greatly promoted the combination of adsorbed CO and O 2 to generate CO 2 . Accordingly, this study provides a facile method to regulate the Pt valence state by pulsed steam treatment for CeO 2 support, which is critical to the CO oxidation activity.
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Nature Communications
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2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Shi Fenglei,Tieu Peter,Hu Hao,Peng Jiaheng,Zhang Wencong,Li Fan,Tao Peng,Song Chengyi,Shang Wen,Deng Tao,Gao Wenpei,Pan Xiaoqing,Wu Jianbo
Corrosion of electrocatalysts during electrochemical operations, such as low potential - high potential cyclic swapping, can cause significant performance degradation. However, the electrochemical corrosion dynamics, including structural changes, especially site and composition specific ones, and their correlation with electrochemical processes are hidden due to the insufficient spatial-temporal resolution characterization methods. Using electrochemical liquid cell transmission electron microscopy, we visualize the electrochemical corrosion of Pd@Pt core-shell octahedral nanoparticles towards a Pt nanoframe. The potential-dependent surface reconstruction during multiple continuous in-situ cyclic voltammetry with clear redox peaks is captured, revealing an etching and deposition process of Pd that results in internal Pd atoms being relocated to external surface, followed by subsequent preferential corrosion of Pt (111) terraces rather than the edges or corners, simultaneously capturing the structure evolution also allows to attribute the site-specific Pt and Pd atomic dynamics to individual oxidation and reduction events. This work provides profound insights into the surface reconstruction of nanoparticles during complex electrochemical processes.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Lin-Ya Xu,Qian Zhou,Cai-Hao Wen,Hua-Hui Xu,Xi Zhao,Fu-Dong Liu,Meng-Fei Luo,Jian Chen
Understanding of the mechanism of saturated alkanes catalytic combustion is crucial for the petrochemical industrial exhaust elimination. Noble metals are commonly proposed to be the active sites for C–H bond activation of saturated alkanes, whereas the critical role of support is largely underestimated. Herein, we reveals a novel pathway for propane activation and combustion on acidic support of Pt catalyst, driven by oxygen spillover, which differs significantly from previously reported reaction mechanisms. Specifically, the Pt/AlSO x -I catalyst was prepared by pyrolyzing the Al 2 (SO 4 ) 3 sol–gel to obtain the acidic micro-mesoporous AlSO x support, followed by loading the Pt active sites using wetness impregnation. In comparison to Pt catalysts supported by Al 2 O 3 nanoparticles (10 nm) or commercially available common γ-Al 2 O 3 , the Pt/AlSO x -I catalyst demonstrates superior catalytic activity for propane combustion. It is found that gaseous oxygen species activated on Pt active sites spillovers to acidic support of Pt/AlSO x -I and then drives propane to activation and further oxidation on acidic support, thereby remarkably decreasing the apparent activation energies (Ea) from 112.4 to 72.0 kJ·mol −1 . Kinetic results suggest that the negative effect of oxygen competitive adsorption is weakened because propane can be activated on the acidic AlSO x support. Additionally, high proportion of metallic Pt species benefits to gaseous oxygen activation as observed on Pt/AlSO x -R, leading to the further increased catalytic activity with highest specific mass reaction rate of 170.2 μmol g Pt −1 s −1 and TOF Pt of 0.289 s −1 at 220 °C. Our primary results provide novel insights into revealing the reaction mechanism of saturated alkanes combustion on dual active sites.
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ACS Sensors
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2024
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IF 8.2
Chengming Sui,Mingxue Zhang,Yueyue Li,Yilin Wang,Yuanzhen Liu,Ziqi Liu,Jihao Bai,Fengmin Liu,Geyu Lu
Bimetallic nanocrystals (NCs) have obtained significant attention due to their unique advantages of the intrinsic properties of individual metals and synergistic enhancements resulting from the electronic coupling between two constituent metals. In this work, Pd@Pt core–shell NCs were prepared through a facile one-pot solution-phase method, which had excellent dispersion and uniform size. Concurrently, ZnO nanosheets were prepared via a hydrothermal method. To explore their potential in nitrogen dioxide (NO2) gas sensing applications, sensitive materials based on ZnO nanosheets with varying mass percentages of Pd@Pt NCs were generated through an impregnation process. The sensor based on 0.3 wt % Pd@Pt-ZnO exhibited remarkable performance, demonstrating a substantial response (Rg/Ra = 60.3) to 50 ppb of NO2 at a low operating temperature of 80 °C. Notably, this sensor reached an outstanding low detection limit of 300 ppt. The enhancement in gas sensing capabilities can be attributed to the sensitization and synergistic effects imparted by the exceptional catalytic activity of Pd@Pt NCs, which significantly promoted the reaction. This research introduces a novel approach for the utilization of core–shell structured bimetallic nanocrystals as modifiers in metal-oxide-semiconductor (MOS) materials for NO2 detection.
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Small
·
2025
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IF 12.1
Xiaoyan Zheng,Xiaoxiao Wu,Rui Wan,Yuguang Wang,Bin Chen,Guowen Meng
Pt single-atoms catalysts have been widely confirmed as ideal electrocatalysts for high-efficiency hydrogen evolution reaction (HER), but their activity and durability at high current density remain great challenges, especially in alkaline media. Herein, a unique Ohmic contact heterostructure is fabricated by integrating Ni and NiO to immobilize Pt single-atoms (Ni-NiO-Pt) via Pt-O 4 coordination for boosting the alkaline HER. Owing to transient high temperature and pressure in the laser ablation process, Ohmic contact heterojunctions are constructed at the interfaces between metal Ni core and nanoporous semiconducting NiO shell with adequate oxygen vacancies. The large work function difference triggers the electron transfer from Ni to Pt-decorated NiO, which dramatically eliminates the electron conduction impedance and regulates the charge redistribution. Density functional theory calculation unveils that the multiple regulations of energy barrier and charge redistribution on Ohmic contact endow Ni-NiO-Pt with outstanding electrical conductivity and favorable hydrogen binding energy. Consequently, Ni-NiO-Pt displays superior alkaline HER performances with an overpotential of 23.54 mV at 10 mA cm −2 and protruding durability for 75 h at 500 mA cm −2 , drastically outperforming commercial Pt/C and most reported HER electrocatalysts. The immobilization of Pt single-atoms on Ohmic contact opens up an avenue toward the rational design of high-efficiency electrocatalysts.
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CERAMICS INTERNATIONAL
·
2024
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IF 5.1
Xuechen Liu,Mingwen Wang,Shuai Yang,Xuexin Li,Kailai Lu,Yang Li,Juru Zhang,Jie Wu,Linghang Wang,Jinglei Li,Fei Li
Piezocatalysis presents an innovative catalytic technique that utilizes the piezoelectric properties of catalysts to convert mechanical energy into electrical energy, thereby driving chemical processes. While various methods for driving piezocatalytic reactions have been developed, there is a notable absence of comprehensive research on piezocatalytic performance across multiple methods. In this context, this study explores the potential of (1- x )Pb(Ni 1/3 Nb 2/3 )O 3 - x PbTiO 3 (PNN-PT) based catalysts as efficient piezocatalysts using both ultrasonic vibration and ball milling . The optimal reaction rate constants of the PNN-PT piezocatalyst under ultrasonic vibration and ball milling are found to be 0.0775 min −1 and 0.0265 min −1 , respectively. Notably, PNN-PT-based catalysts exhibit outstanding catalytic activity up to ultra-high substrate concentrations (65 mg/L), suggesting possible industrial applications. The exploration of the reaction mechanism indicates that •OH is the main reactive radical, the catalytic reaction activity demonstrates a direct relationship with •OH quenching, and the high •OH generation rate of PNN-PT further illustrated their suitability as environmental purification catalysts.
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