INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Chao Wang,Hu Zang,Changjiang Liu,Jiahao Wang,Long Kuai,Baoyou Geng
The hydrogen evolution reaction (HER) involves two-step elementary reactions, providing an opportunity to establish dual-site synergistic catalysts. This work demonstrates carbon-supported Pt single atoms and clusters (Pt1+Cs-NPC) as an efficient catalyst for acidic HER, which exhibits an ultralow Tafel slope of 12.5 mV/dec and an overpotential of 24 mV at 10 mA/cm2 with an ultralow platinum content of 3.8 wt %. The Pt mass activity and turnover frequency (TOF) are 10.2 times and 5.4 times that of commercial Pt/C, respectively. The density functional theory (DFT) study shows that the Pt cluster regulates the electronic state structure of the adjacent Pt single atom, so that the ΔGH* at the Pt1 site approaches 0. Moreover, the DFT study confirms that Pt clusters and neighboring Pt single atoms can synergistically catalyze the Tafel step and reduce the energy barrier in forming the H–H bond. At the same time, the platinum cluster reduces the energy barrier of the nearby platinum single-atom site to the Heyrovsky step and accelerates the reaction with hydrated hydrogen ions. Studies have shown that platinum clusters and platinum single-atom composite loading structures exhibit excellent activity for the Volmer–Tafel or Volmer–Heyrovsky reaction paths of HER reactions. This work provides a clear understanding of the synergistic effect of Pt1+Cs-NPC, which provides guidance for developing efficient HER catalysts.
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PubMed
高影响因子
ChemNanoMat
·
2022
·Vol. 8
·期 10
·e202200268
·
IF 3.82
Mengmeng Liu,Jingjing Li,Pengfei Wang,Shuai Chen,Zhengping Dong,Fengwei Zhang
Graphical The encapsulation of Pt/TiO 2 -450H catalyst with SMSI into zeolite silicalite-1 (S-1) is reported. The resulting Pt/TiO 2 @S-1 catalyst dispalyed superior catalytic performance especially for halogenated nitroaromatics and without degradation in selectivity after 7 cycles. It is attributed to the high surface area, SMSI effect in confined space and the pore structure of S-1 with selective adsorption of substrates. The encapsulation of metal nanoparticles (NPs)-based active sites and homogeneous catalysts in nanoporous materials has been of highly research focus for tuning their catalytic activity, selectivity and stability. Although the catalysts with strong metal-support interaction (SMSI) hold the reversible encapsulation feature in a certain atmosphere, there is still a lack of systematic research on them in a real confined environment. Herein, we present a highly selective and stable Pt/TiO 2 @S-1 catalyst, which is prepared by in-situ growth of classical silicalite-1 on the external surface of Pt/TiO 2 -450H pre-catalyst with SMSI effect. Encouragingly, the encapsulated 20Pt/TiO 2 @S-1 catalyst demonstrates unprecedented catalytic performance for various nitroaromatics and without any degradation in selectivity after 7 cycles (>99%) for the hydrogenation of 1-chloro-4-nitrobenzene. Such situation is attributed to the high surface area, SMSI effect in confined space as well as the pore structure of silicalite-1 with selective adsorption of substrates.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Zhuo Wang,Meiting Wang,Luan Fang,Zihan Li,Ping Nie,Yuting Gao,Juan Jian,Limin Chang
Hydrogen produced through self-powered water-splitting can effectively meet the demand for miniaturized devices. However, the design of an efficient catalyst that integrates a zinc-air battery (ZAB) with a water-splitting cell is crucial for the development of such devices. In this study, we synthesized Pt/Ni 3 (PO 4 ) 2 on nickel foam (NF) via a two-step process. The resulting Pt/Ni 3 (PO 4 ) 2 /NF exhibited significantly enhanced trifunctional properties (hydrogen evolution reaction, HER; oxygen evolution reaction, OER; oxygen reduction reaction, ORR) compared to the Ni 3 (PO 4 ) 2 /NF precursor. Additionally, the ZAB assembled using Pt/Ni 3 (PO 4 ) 2 /NF as the air-cathode demonstrated superior rechargeable performance compared to the Ni 3 (PO 4 ) 2 /NF-based counterpart. Moreover, when Pt/Ni 3 (PO 4 ) 2 /NF was directly used as both the cathode/anode for the water-splitting device and the air-cathode for the ZAB, the self-powered hydrolysis device exhibited excellent hydrogen production performance. Upon investigating the influence of in-situ decorated Pt nanoparticles, we found that these Pt nanoparticles: 1) facilitate the morphological reconstruction of Ni 3 (PO 4 ) 2 , thus increasing the electrochemical surface area of the catalyst; 2) lower the hydrogen adsorption free energy of Pt/Ni 3 (PO 4 ) 2 , and the associated OER theorical potential; 3) shift the d-band center of Pt/Ni 3 (PO 4 ) 2 closer to the Fermi level, ultimately enhancing its intrinsic catalytic activity. This work is expected to provide a foundation for experimental, theoretical, and practical applications of other Ni 3 (PO 4 ) 2 -based multifunctional materials.
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DOI
PubMed
高影响因子
Catalysts
·
2025
·Vol. 15
·期 11
·1005
·
IF 4
Kuo Zhou,Jialin Xu,Shengrong Guo,Hongjun Wu
The catalytic synthesis of 1,2-pentanediol from biomass-derived feedstocks is of remarkable significance for addressing current environmental challenges and energy crises. In this paper, a series of Pt-based catalysts were prepared and evaluated in the hydrogenolysis of furfuryl alcohol. The 5Pt0.5Y/MgO provided a 1,2-pentanediol yield of 68.9% and a tetrahydrofurfuryl alcohol yield of 19.8% with 98.1% conversion of furfuryl alcohol, at 200 °C and 2 MPa H2for 10 h. The promotional effect of yttrium on the catalytic performance was investigated through catalytic reaction and comprehensive characterization. It was found that the reducibility of Pt species was suppressed by the introduction of Y species, resulting in reduced activity compared to the 5Pt/MgO catalyst. However, the addition of Y notably shifted the reaction pathway towards 1,2-pentanediol formation at the expense of tetrahydrofurfuryl alcohol selectivity. This increase in 1,2-pentanediol selectivity was attributed to a higher concentration of medium-strength basic sites on the Y-modified Pt catalyst. Furthermore, the strong interaction between Y2O3, Pt particles, and the MgO support led to high Pt dispersion and stability on the MgO surface, consequently yielding satisfactory recyclability.
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CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Fan Li,Lianlian Song,Quanxing Zhang,Caoying Kang,Wenhan Li,Chuanqin Ding,Mengyuan Liu,Feng Du,Lin He,Kunming Zhang,Wenjuan Yan,Xin Jin,Chaohe Yang
Aqueous oxidation of 1,5-pentanediol (1,5-PDO), a furfural-based intermediate, presents a sustainable pathway to synthesize glutaric acid (GA) for polyester industry. Kinetic analysis and mechanistic modeling for this reaction is indispensable for catalyst optimization and process scale-up. In this work, power law and modified Langmuir-Hinshelwood kinetic study confirmed a unique 2nd order kinetics on aqueous oxidation of 1,5-PDO over Pt-based catalysts. Notably, bimetallic PtAu/TiO 2 catalysts exhibited superior selectivity toward target carboxylic acids (5-hydroxyvaleric acid and GA) by facilitating oxidation of –CHO group in the key intermediate 5-hydroxypentanal compared to monometallic Pt/TiO 2 catalyst. Furthermore, a preliminary technoeconomic comparison with the fossil-based synthetic route was evaluated to highlight the advantage of bio-GA studied in this work. The outcome of kinetic modeling would provide useful information for optimizing cost-effective catalysts and process design in producing bio-derived dicarboxylic acids.
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Surfaces and Interfaces
·
2025
·
IF 6.3
Fan Yang,Jingrui Duan,Yan Chen,Huiying Meng,Wanying Zhang,Ruiting Li,Wen Luo,Yang Wu,Yong Wang,Peng Zhang,Yifan Zhang
In this study, a bimetallic Pt-Ni alloy catalyst, designated PN 0.5 /VCN 1 , was synthesized with the objective of enhancing the photocatalytic hydrogen evolution performance. Photoelectrochemical characterizations confirm that PN 0.5 /VCN 1 significantly improves light absorption, charge transfer efficiency, and proton adsorption/activation capability, leading to enhanced photocatalytic performance. The results demonstrate that under optimized conditions (300 W Xe lamp, lactic acid as the hole scavenger) PN 0.5 /VCN 1 achieves a hydrogen evolution rate of 8.77 mmol·g -1 ·h -1 (4079 times higher than pure CN) with remarkable stability. And stability tests over four cycles (20 h total) indicate no significant activity loss. This enhancement is attributed to the localized surface plasmon resonance (LSPR) effect of the alloy, interfacial electron redistribution, and synergistic metal-defect interactions. The modification strategy proposed in this study offers a rational and cost-effective approach for efficient photogenerated charge separation and accelerated proton reduction kinetics, providing a competitive advantage in the market. This work provides a foundation for designing high-performance photocatalytic systems.
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高影响因子
Science China-Chemistry
·
2025
·
IF 9.7
Chen Tao,Lv Liang,Yu Jing,Du Junfeng,Ma Zihan,Guan Chaohui,Wei Hang,Chu Haibin
The electrocatalytic oxidation of glycerol to produce high-value-added chemicals ( e.g. , glycerate, GLA) constitutes a crucial process for harnessing the potential of glycerol. However, the high electrocatalytic activity is typically accompanied by catalyst deactivation by strong adsorption of the intermediates or products. Here, the Pt/RENC catalyst was prepared with small Pt nanoparticles supported on rare earth single-atom nitrogen-carbon (RENC, RE = La, Ce, Pr, Y) material. Aberration-corrected scanning transmission electron microscopy and X-ray absorption spectra confirm that the highly dispersed Ce sites are well maintained after the in situ formation of the Pt nanoparticles. The kinetic experiments, in situ IR and valence band characterizations, reveal that the synergy of a single atom of Ce-N x sites and Pt nanoparticles leads to the alleviation of the strong adsorption of GLA, and the enhancement of the H 2 O dissociation into active OH*, resulting in the fast conversion of glycerol. The rare earth single-atom sites also improve the anchoring of Pt nanoparticles. Remarkably, even in a high glycerol concentration of 0.6 M, the Pt/CeNC catalyst achieves a fast GLA production rate of 233 mmol h −1 g Pt −1 and GLA yield of 51.7% with superior cycling stability, tripling the performance of the counterpart Pt/NC catalyst (75 mmol h −1 g Pt −1 and 15.0%).
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高影响因子
International Journal of Electrochemical Science
·
2023
·
IF 1.5
Fang Lu,Chunyong Zhang,Jiehong Cheng,Cheng Zhu,Haojing Zhang,Xian Cheng
A direct methanol fuel cell (DMFC) electrode based on the carbon fiber cloth (CFC) modified with wrap-like graphene oxide (GO) decorated with platinum nanoparticles was prepared by multicycle CV method. Also, the Pt/CFC composite and GO/CFC composite were prepared by multicycle CV and potentiostatic method, respectively. The four electrodes (GO-Pt/CFC, Pt/CFC, GO/CFC and CFC) were tested in a fuel cell for electro-oxidation of methanol and were analyzed by scanning electron microscopy (SEM) and X-Ray powder diffraction (XRD). The SEM image indicated that the surface of CFC was covered by a wrap-like graphene oxide (GO) film completely, which increased the contact area with methanol solution and provided more load points. And the Pt nanoparticles supported GO/CFC electrode possessed the ball-like morphology. The electrochemical measurements showed that the electrocatalytic peak current density of methanol oxidation of GO-Pt/CFC electrode (218 mA/cm 2 ) was about 27% higher than Pt/CFC electrode (172 mA/cm 2 ) and the steady-state current density of GO-Pt/CFC electrode was 57.6%, 114.5% and 497.9% higher than that of Pt/CFC, GO/CFC and CFC electrodes, respectively. And this date revealed that the ball-like morphology of Pt nanoparticles and a wrap-like GO film coated on CFC surface were favorable to improve the electrocatalytic oxidation activity of methanol.
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ACS Catalysis
·
2017
·
IF 10.614
Fanpeng Kong,Chunyu Du,Jinyu Ye,Guangyu Chen,Lei Du,Geping Yin
Heterogeneous nanostructures hold substantial promise in many fields including energy conversion and catalysis, and their functionality is largely determined by the interactive surface features of respective architectural components. Herein, we report the facile preparation of a Pt–Au heterogeneous nanostructure, which as a model exhibits not only the enhanced electrocatalysis for oxygen reduction reaction (ORR) and ethanol oxidation reaction (EOR), but also an unprecedented activity for formic acid oxidation (FAO). Further, selective under-potential deposition coupled with CO adsorption is employed to probe the electrocatalytic mechanism of the Pt–Au heterogeneous nanostructure. The electronic effect is clarified for the ORR and EOR mechanisms on the Pt–Au nanostructure. A synergetic mechanism in that Pt ruptures the C–H bond of HCOOH and Au converts the resulted −COOH into CO2 is revealed for FAO. This strategy provides a versatile and powerful tool for the selective surface engineering and in-depth analysis of the functionalizing mechanism of heterogeneous nanostructures.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Dihua Huang,Yiming Zhu,Binglong Mao,Jun Zhang,Quanxing Liu,Xiang Li,Kexing Song
Felicitously incorporating noble metals with some transition metals to fabricate composite nanoagents with diverse shape and microarchitecture is a more promising solution for obtaining highly effective and cost-cutting catalyst. Herein, we report a facile and flexible synthesizing tactics, or Galvani substitution modulated self-assembly protocol, to fabricate Cu nanowire (core)-Pt nanoparticle (shell) unique microarchitecture (Cu-NWs@Pt) with porously hiberarchy. The comprehensive characterizations reveal that as-fabricated bimetallic nanowires with average aspect ratio of ca. 80 and apparent diameter of ca 60 nm, hold the razor-thin Cu–Pt alloy sublayer in the metallic contact interface, with the prebuilt Cu nanowires cladded by orderly oriented Pt nanograins to form loose, porous and stratiform structure. The thickness and microarchitecture of the Pt shell could be duly regulated by adjusting dosage of the metal precursors and substituting time. The verified formation of electronic synergic effect in the bimetallic nanoagents avails the adsorption of H to form metal-H species, leading to enhance the catalytic activity . Their catalytic ability overall increases with rising of Pt/Cu molar ratios , of which the Cu 0.6 Pt 0.4 even exceeds Pt-NPs, with a turnover frequency of 77.26·min −1 and apparent activation energy of 30.25 kJ·mol −1 , and maintaining 89% of the incipient catalytic ability after 5 recycling runs.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2018
·
IF 3.235
Lei Gao,Ruirui Yue,Jingkun Xu,Zhen Liu,Jingdang Chai
In this paper, Pt-PEDOT/reduced graphene oxide (Pt-PEDOT/rGO) nanocomposites were facilely prepared by a simple and cost-effective one-pot method. The obtained nanocomposites were characterized and confirmed by scanning electron microscopy, transmission electron microscopy, energy dispersive X-ray spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy and Raman spectra . As expected, the Pt-PEDOT/rGO nanocomposites modified glassy carbon electrode (Pt-PEDOT/rGO/GCE) exhibited higher charge transfer efficiency and electrocatalytic activity to the oxidation of caffeic acid (CA) in comparison with the bare GCE, rGO and Pt-PEDOT modified electrodes (rGO/GCE and Pt-PEDOT/GCE). Furthermore, the Pt-PEDOT/rGO/GCE showed a wide linear range of 5.0 × 10 −9 to 5.0 × 10 −5 M with a low detection limit of 2.0 × 10 −9 M (S/N = 3) for the determination of CA. More experiments indicated that the Pt-PEDOT/rGO/GCE performed superior reproducibility, selectivity and long-term stability. Finally, the modified electrode was also applied to detect CA in green tea and black tea samples with promising recovery and application prospect.
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Tianhao Li,Jing Yang,Yaozong Tan,Yaning Yue,Zongyu Sun,Mengxi Han,Pai Peng,Qiang Chen
Zeolite-encapsulated metal nanoparticle systems have exhibited interesting catalytic performances via the hydrogen spillover process, yet how to further utilize the function of zeolite supports to promote catalytic properties in such a process is still challenging and has rarely been investigated. Herein, to address this issue, the strategy to strengthen the adsorption energy of reactant onto the zeolite surface via a simple ion exchange method has been implemented. Ion-exchanged linde type A (LTA) zeolite-encapsulated platinum nanoclusters (Pt@NaA, Pt@HA, Pt@KA, and Pt@CaA) were prepared to study the influence of ion exchange on the catalytic performance in the model reaction of hydrogenation of acetophenone to 1-phenylethanol. The reaction results showed that the Pt@CaA catalyst exhibited the best catalytic activity in the series of encapsulated catalysts, and the selectivity of 1-phenylethanol approached 100%. As revealed by density functional theory (DFT) calculations and acetophenone temperature-programmed desorption (acetophenone-TPD) experiments, in comparison with introduced cations of Na+, H+, and K+, ion-exchanged Ca2+ on the zeolite maximumly enhanced the adsorption of carbonyl groups in acetophenone, playing a critical role in achieving the highest activity and excellent catalytic selectivity among the Pt@A catalysts.
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