CARBON
·
2024
·
IF 10.5
Yongqing Shen,Peizhi Liu,Yangrui Li,Jianghong Wu,Yanhui Song,Junjie Guo
The structural stability of supported metal nanoparticles determines the activity and longevity of heterogeneous catalysts. Unfortunately, the chemical/thermal working environment inevitably accelerates metal sintering to larger crystallites that leads to the degradation of catalytic performance. Here, we demonstrate that the distribution of defects in carbon support as an inherent parameter plays a crucial role in catalyst sintering. Based on in-situ transmission electron microscopy studies, the strong metal-support interaction between platinum (Pt) nanoparticles and defect-rich graphene nanoflakes largely suppresses metal sintering up to 700 °C. Particularly, the optimal carbon support can be achieved in the annealing process, in which the mass transfer and charge transport can be enhanced by accurately manipulating the distribution of defects in carbon matrix and graphitization degree. It is worth noting that the screened Pt/GNs-300 exhibits impressive oxygen reduction reaction performance with high half-wave potential (0.91 V), mass activity (108.1 A g –1 Pt ) and excellent stability. By its ascendancy in ORR, the Pt/GNs-300 exhibits a high open-circuit voltage of 1.41 V and a maximum power density of 198.6 mW cm −2 in Zn-air battery, implying its brilliant practicability. This work paves a pathway for achieving sinter-resistant metal-loaded catalysts in energy electrocatalysis.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Yuzhe Liu,Weijie Qin,Jinguang Liu,Daming Gu,Xulei Sui,Zhenbo Wang
Highly loaded Pt catalysts often suffer from poor oxygen reduction performance due to challenges in controlling the dispersion and particle size of Pt particles, with carbon carriers playing a crucial role in this aspect. Herein, N-doped carbon carriers were prepared through a solvothermal reaction, combined with continuous microwave-assisted technology to effectively manage the particle size and dispersion of Pt nanoparticles. The resulting highly loaded Pt catalysts demonstrated excellent activity and durability. The nitrogen-doped carbon not only reduced the size and concentration of Pt particles but also regulated the electronic structure of Pt, thereby enhancing the interaction between Pt and the carriers. The catalysts exhibited an electrochemical active area of 114 m 2 g −1 Pt and a half-wave potential of 0.907 V. Following 30,000 accelerated durability tests, the mass activity decay rate was approximately 20%, surpassing that of commercial Pt/C catalysts. A peak power density of 1.22 W cm −2 was achieved in MEA under H 2 -Air conditions. Furthermore, the catalysts developed using nitrogen-doped modified carbon materials demonstrated the ability for large-scale production, holding promising potential for practical applications in proton exchange membrane fuel cells.
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CHEMISTRY OF MATERIALS
·
2024
·
IF 7.2
Xiao-Mei Yu,Yihu Ke,Xue Wang,Hai Liu,Hong Yuan
The specific structure of the support and the interactions between the catalyst components can lead to electron transfer, which in turn could affect the catalytic performance in heterogeneous catalytic reactions. In this paper, we have successfully prepared MnxOyCz composite materials from the calcination of the Mn-organic framework. Then bimetallic Au–Pt nanoparticles (NPs) were supported onto MnxOyCz via the colloidal-deposition method. These catalysts were tested in the selective oxidation of glycerol to glyceric acid under basic conditions. The results demonstrated that the catalytic activity of the bimetallic Au–Pt/MnxOyCz catalyst is considerably superior to those of the monometallic (Au and Pt) supported catalysts. Under the optimized conditions, 100% of glycerol can convert with 57.3% selectivity of glyceric acid. Multicharacterizations showed that the strong interaction between Au and Pt in the Au–Pt/MnxOyCz catalyst can enhance the dispersion of Au–Pt alloy NPs, promoting the electronic coupling effect on the metal surface. At the same time, the rich oxygen vacancies in this catalyst can facilitate the activation of oxygen, which causes the Au–Pt/MnxOyCz catalyst to show better catalytic activity. Specifically, the interaction between Au and Pt not only decreases the particle size of the Au–Pt alloy NPs but also promotes the reduction of Mn-based oxides and the mobility of oxygen. The absence of Au leads to a decrease in Pt 4f7/2 binding energy, resulting in an enrichment of electrons at the Pt active site and enhancing the oxidation ability of the primary hydroxyl group. In addition, the Au–Pt/MnxOyCz catalyst showed excellent stability without substantial loss of activity after being recycled five times. The insights and methodology may provide some new guidance for the reasonable design of bimetallic catalysts for the catalytic oxidation of biopolyols under mild conditions.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Xilong Wang,Yadong Li,Hongwei Zhu,Han-Pu Liang
Facile synthesis of highly-dispersed Pt-based electrocatalysts on porous carbon supports with strong durability is extremely desirable for oxygen reduction reaction but remains challenging. The influence of pores in carbon supports on the stability and activity of catalysts is ambiguous and needs to be elucidated. Targeting this aim, herein, we prepared a series of carbon nanofibers with tunable pore diameter and specific surface area using the resorcinol-formaldehyde (RF) resins as a model system. Homogeneous composite precursors composed of RF resins and silica colloids were synthesized by the surfactant-assisted simultaneous polycondensation of RF resins and tetraethylorthosilicate (TEOS). The diameter of the pores induced by removal of silica could be controllable tailored through thermal treatment of the composite under various target temperatures. Pt 3 Co alloy nanoparticles loaded on the as-synthesized porous carbon nanofibers were prepared by an optimized wet-impregnation method. The experimental results indicated that the carbon nanofibers with pore size distribution focused on ∼1.27 nm and ∼2.34 nm provided the best stability without limiting current density decay, and negative shift of half-wave potential (E 1/2 ) and mass activity (MA) loss of Pt after 20000 potential cycles are relatively mild. Conversely, negative shift of 21 mV, 15 mV and 22 mV in E 1/2 and mass activity loss of 51.8%, 30.2% and 33.0% were observed for the Pt 3 Co nanoparticles supported on MC-60, MC-100 and MC-140 matrices which have pore size distribution focused on ∼2.73 nm, ∼2.73 nm as well as ∼4.66 nm, and ∼4.66 nm, respectively. This work demonstrates the importance of micropores and small mesopores for activity and long-term stability enhancement of carbon supported Pt-based electrocatalysts .
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BIOSENSORS & BIOELECTRONICS
·
2017
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IF 7.78
Jingyi Luo,Danfeng Jiang,Tao Liu,Jingmeng Peng,Zhenyu Chu,Wanqin Jin
In this work, a novel sandwich-type aptasensor was designed for the ultrasensitive recognition of trace mercury ions in water. Numerous oriented platinum nanotube arrays (PtNAs) were in-situ crystallized on a flexible electrode as a sensing interface, while thionine labelled Fe 3 O 4 /rGO nanocomposites as signal amplifiers. Both PtNAs/CF and nanocomposites were synthesized by easy hydrothermal processes. With their large surface area, it was favorable for electrochemical performance and immobilization of capture DNAs (cDNA) and report DNAs (rDNA). Upon the existence of Hg 2+ , partial linker DNAs were tightly bound with cDNAs through thymine-Hg 2+ -thymine pairing (T-Hg 2+ -T). Then rDNAs attached Fe 3 O 4 /rGO nanoprobes were fixed on the electrode through the match of remaining linker DNAs and rDNAs. Under the optimal conditions, the Hg 2+ aptasensor showed a synergistic amplification performance with a wide linear range from 0.1nM to 100 nM, as well as a low detection limit of 30 pM. Moreover, the as-prepared aptasensor also exhibited reliable performance for assay in real lake water samples.
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高影响因子
ANALYTICAL SCIENCES
·
2024
·Vol. 40
·期 8
·1437-1448
·
IF 1.8
Feng Chengqi,Chen Zhiyuan,Yin Haoyong,Gong Jianying,Wang Hui,Wu Shengji,Wang Ling
Designing portable electrochemical sensors combined with highly efficient glucose oxidation electrodes offers a significant opportunity for convenient glucose detection. In this report, we present the design and preparation of platinum deposited Ni/NiFe 2 O 4 /Carbon composite (Pt/Ni/NiFe 2 O 4 /C) derived from Ni/Fe metal–organic frameworks (MOFs) followed by Pt deposition. Energy-dispersive X-ray spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and electron microscopy (EM) were utilized to analyze the crystal structure, morphology, and chemical composition of the resulting materials. The glucose sensing capabilities of the optimal Pt/Ni/NiFe 2 O 4 /C-3 were assessed using amperometry methods on a smartphone-based portable device. Acting as a nonenzymatic glucose sensor, the Pt/Ni/NiFe 2 O 4 /C-3 electrode demonstrated notable sensitivity and a low limit of detection for glucose. The portable sensor exhibits high sensitivities of 131.88 μM mM cm −2 at low glucose concentration (3–500 μM) and 29.52 μA mM cm −2 at high glucose concentration (700–4000 μM), achieving a low detection limit of 1.1 μM (S/N = 3). The sensor also demonstrates enhanced selectivity and stability for detecting glucose. Furthermore, the portable sensor exhibits a clear step-ampere response in the detection of serum samples with satisfactory recovery ranging from 99.30 to 101.32%. This suggests the significant potential of portable glucose sensing applications. Graphical abstract
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Rundong Ma,Han Tian,Xu Yu,Xiangzhi Cui,Xinmei Hou,Shengli An
Hydrogen oxidation reaction (HOR) as the anode reaction in proton exchange membrane fuel cell, usually suffers from the high loading of platinum (Pt) and subsequent CO poisoning especially by using industrial crude hydrogen as fuel. In this work, we propose a directional electron transfer route from Pt to MoO 2- x in the macroporous structure to significantly enhance the HOR activity as well as the CO tolerance, which is constructed by interface engineering and defect strategy to anchor highly dispersed Pt nanoparticles onto the three-dimensional MoO 2- x -C framework. The optimized 2Pt-MoO 2- x -C with 1.02 wt% Pt demonstrates higher HOR peak current density (3.57 mA cm −2 ) and nearly 25 times higher mass activity than 20 wt% Pt/C. The excellent HOR performance is attributed to the synergistic effect between Pt and MoO 2- x species, in which the charge transfer from Pt to MoO 2- x improves H 2 adsorption ability of Pt and accelerates the activation of H 2 due to the reduced hydrogen binding energy of MoO 2- x caused by Pt-O construction, leading to the release of H* thereby the enhancement of HOR activity. The construction of three-dimensional macroporous structure enhances the HOR dynamics by promoting the conductivity, mass transfer and the exposure of active sites. Moreover, the formed Mo-OH in Pt-MoO 2- x -C can effectively react with CO species to remove the CO poisoning of Pt, endowing the excellent CO tolerance.
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CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Zijiang Zhao,Songtao Huang,Guanglu Dong,Yi Chen,Mingxuan Wang,Molin Xia,Xin Song,Xiaonian Li,Zhongzhe Wei,Jianguo Wang
The hydrogenation of vanillin stands as a pivotal platform reaction within biomass conversion processes, presenting a significant challenge in achieving controlled synthesis of different products. Here, we proffer different methodology for elaborately designing the electronic structure of Pt via regulating the strong metal-support interactions (SMSI) between Pt and Mo 2 TiC 2 , thereby facilitating the targeted synthesis of vanillyl alcohol (VA) and 2-methoxy-4-methylphenol (MMP) from vanillin. Appropriate H 2 reduction can enhance the SMSI between Pt and Mo 2 TiC 2 , promoting the electron transfer from Mo 2 TiC 2 to Pt, resulting in 200-Pt/Mo 2 TiC 2 with 68.1 of Pt 2+ . However, the SR-Pt/Mo 2 TiC 2 obtained through the galvanic replacement strategy possesses 64.7 % of Pt 4+ , which is attributed to the weaker spontaneous SMSI between Pt and Mo 2 TiC 2 . XPS adsorption experiments highlight the pivotal role of Pt 2+ in facilitating the desorption of VA, resulting in the 200-Pt/Mo 2 TiC 2 catalyst demonstrating exceptional selectivity towards VA (96 %). Meanwhile, SR-Pt/Mo 2 TiC 2 showcases a predilection for the direct hydrogenation and deoxygenation of vanillin into MMP. This research not only marks the application of the MXene system to biomass conversion but also illuminates the relationship between the electronic structure of Pt and its selectivity towards VA and MMP.
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JOURNAL OF NANOBIOTECHNOLOGY
·
2025
·Vol. 23
·期 1
·1-20
·
IF 12.6
Fang Man,Cao Lei,Zhang Zhao,Yu Zhen,Shen Yue,Chen Jieqi,Chen Juan,Li Yue-Qin,Liu Zhaoqian,Meng Yingcai,Xiao Haihua,Qu Qiang,Yin Ji-Ye,Li Xiang-Ping
Non-small cell lung cancer (NSCLC) represents the most prevalent form of lung cancer, exerting a substantial impact on global health. Cisplatin-based chemotherapy is the standard treatment for NSCLC, but resistance and severe side effects present significant clinical challenges. Recently, novel tetravalent platinum compounds have attracted significant interest. While numerous studies concentrate on their functional modifications and targeted delivery, tumor-induced platinum resistance is frequently overlooked. Previous tetravalent platinum compound demonstrated antitumor activity, yet proved ineffective against cells exhibiting resistance to cisplatin. In order to enhance the efficacy and potential applications of tetravalent platinum in NSCLC, a glutathione (GSH)-responsive albumin nanoquadrivalent platinum (HSA@Pt) have been constructed. In light of previous research into drug conjugation, this study was to develop a combined chemo-immunotherapy approach. The HSA@Pt demonstrated high efficacy and low toxicity, with targeted tumor accumulation. Furthermore, Ammonium Tetrathiomolybdate (TM) has been demonstrated to exert a synergistic inhibitory effect on ATPase Copper Transporting Beta (ATP7B) and Programmed Death Ligand 1 (PD-L1), impede platinum efflux, induce cellular stress, and activate antitumor immunity. The findings suggest HSA@Pt’s potential for clinical use and a novel chemo-immunotherapy strategy for NSCLC, enhancing the utility of established drugs through synergistic sensitization.
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JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Bin Zhu,Xin He,Lingze Liu,Jinglin Liu,Xiaomin Zhang,Ben W.-L. Jang
Perovskite is one of the most promising materials for catalytic oxidation of volatile organic compounds (VOCs) because of its special tunable structure and properties as well as high stability. However, it commonly suffers from relatively low catalytic activity due to the low specific surface area and limited numbers of active sites caused by high synthesis temperature required. To improve the reactivity of the perovskite catalyst, a promising strategy is to construct highly dispersed noble metal sites on surfaces perovskite. However, generating highly active metallic sites while exhibiting good thermal stability remains a formidable challenge. Here, it’s demonstrated that the construction of highly efficient and robust platinum (Pt) sites on La 0.8 Sr 0.2 MnO 3-δ (Pt/LSMO) for toluene oxidation resulted in an almost three-fold increase in toluene conversion with a good stability. The key to the construction of these Pt sites is treating the oxidized Pt species on LSMO with hydrogen (H 2 ) plasma at low temperatures, which leads to the formation of high metallic Pt (Pt 0 ), ultrasmall Pt nanoparticles (∼1.3 nm), and high concentration of oxygen vacancy (O v ). These features facilitate the generation of a large number of highly active and stable Pt 0 -Mn 3+ -O v sites on Pt/LSMO, which contribute to the activation of toluene and oxygen species and, therefore, the catalytic reaction. This investigation demonstrates a promising approach of using the cold plasma technique to design and construct high-performing noble-based perovskite catalysts for toluene oxidation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Lin Huang,Maoqing Chen,Ying Yang,Qingshou Zheng,Li Gu,Ruobing Cheng,Xuebo Cao
Electro-reforming of organics such as alcohols into commodity chemicals and H 2 powered by renewables is intriguing and prevailing with the remarkable renaissance of electrochemical technology. Integrating Pt/Pd with an auxiliary metal, metal oxide, and metal hydroxide are feasible strategies to design the desirable catalysts toward alcohols electro-oxidation reactions. These catalysts however have high affinity toward carbonyl intermediates that occupy and poison the active sites. Thus, the target products suffer from poor selectivity. To address these issues, a facile binary Pt–Ag alloy nanowires (NWs) catalytic system was reported for efficient electro-oxidative reforming of ethylene glycol (EG), yielding glycolate with a selectivity of 91.5 %, an EG conversion of 96.4 %, and Faradaic efficiency (FE) of 87.4 %. Experimental and theoretical investigations revealed that Ag-induced electronic structure perturbations in Pt 0.66 Ag catalyst boosted the kinetics and robustness as a conventional promoter toward EG electro-oxidation reaction (EGOR). Moreover, the one-electron oxidation of water/hydroxide ion to generate abundant hydroxyl adspecies (OH ad ) on Ag served as another crucial promoter for efficient dehydrogenation, glycolate formation, and carbonyl intermediates release via a highly efficient, noncompetitive Langmuir–Hinshelwood (L–H) mechanism, but not the competitive L–H mechanism or the Eley–Rideal (E–R) mechanism. These findings provide new insights into the selective alcohol electro-oxidation reaction, and facilitate the generation of commodity chemicals via partial electro-oxidation reactions.
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JOURNAL OF MATERIALS CHEMISTRY
·
2012
·Vol. 22
·期 18
·9117-9122
·
IF 5.968
Sha Chen,Hongye Zhang,Lingyan Wu,Yanfei Zhao,Changliang Huang,Maofa Ge,Zhimin Liu
Based on the galvanic replacement reaction between Cu nanoparticles and noble metal ions, a simple and efficient strategy was developed for the preparation of supported Cu–M (M = Pt, Pd, Ru, Rh) bimetallic nanoparticles under intense ultrasonication irradiation at ambient environment. A series of Cu–M/TiO2 bimetal catalysts with controllable composition, metal particle size less than 2 nm and narrow size distribution were obtained, and characterized by transmission electron microscopy (TEM), high resolution transmission electron microscope (HRTEM) with scanning TEM (STEM) mode, energy-dispersive X-ray spectrometers (EDS), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and ICP-AES analysis. It was demonstrated that most of the metal particles were present in the form of bimetallic state. The mechanism of this strategy was discussed. The resultant Cu–Pd/TiO2 was used to reduce nitrate at room temperature, and it exhibited extremely high activity.
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