International Journal of Electrochemical Science
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2023
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IF 1.5
Xianming Fu,Zhenming Chen,Siyu Shen,Lilan Xu,Zhimin Luo
An amperometric nonenzymatic biosensor for sensitive and selective detection of glucose has been developed by using reduced graphene oxide/ultrasmall platinum nanowire nanocomposites (rGO-PtNW) as electrode material. rGO-PtNW displays good electrocatalytic activity towards the oxidation of glucose in alkaline solution. The fabricated biosensor shows good analytical performance including low detection limit (4.6 μmol/L), wide linear range (0.032-1.89 mmol/L), high sensitivity (56.11 μA·(mmol/L) -1 ·cm -2 ), and good anti-interfering ability towards species (uric acid and ascorbic acid) coexisting with glucose in human blood at the work potential of 0 V. It indicated that rGO-PtNW nanocomposite can serve as a promising candidate material for high-performance glucose nonenzymatic biosensors.
研究领域:
生物医学工程
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纳米技术
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分析化学
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电化学传感
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生物传感器
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高影响因子
CATALYSIS LETTERS
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2018
·Vol. 148
·期 8
·2418-2431
·
IF 2.911
Sun Rong,Huang Wan,Zhang Qian,Hong Jun-ming
Abstract This study developed nitrogen-doped graphene/Pt/TiO 2 (N-GN/Pt/TiO 2 ) as anode to effectively degrade aminophenol (APAP) in electrocatalytic process. Due to the different physicochemical properties of graphene with various N species loading, the efficiency of catalysts was novelty discussed. The morphology, N-doped content/species, and the graphene defects of the catalyst were analyzed by TEM, FTIR, XPS, EA, and Raman spectroscopy. The results show that the doping morphology of the N atoms gradually shifted from pyridinic N and pyrrolic N to graphitic N with increased hydrothermal time, in order to decrease the defect degrees and redox activity. However, the conductivity of material increased with the graphitic N generation. The best APAP degradation efficiency (100% with 20 mA, 1 g/L NaCl, and initial pH 3.0) can be achieved with 1.5-N-GN/Pt/TiO 2 (mainly pyridinic N and pyrrolic N doping). A detailed investigation was conducted to determine the oxidation intermediates of APAP using GC-MS analysis. Finally, a possible degradation pathway was proposed. Graphical Abstract
研究领域:
环境科学
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材料科学
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PROCEEDINGS OF THE COMBUSTION INSTITUTE
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2026
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IF 4.6
Lei Luo,Fanggang Zhang,Yuhang Sun,Jiayu Sun,Kai Hong Luo,Yu Cheng Liu,Ran Sui
Soluble catalysts that are readily blended with fuels render significant potentials in long-term storage and engine compatibility to improve ignition and combustion reliability under demanding conditions. However, the mechanistic role of such additives under droplet combustion scenarios that involve evaporation-reaction coupling remains unclear. In this study, single-droplet combustion experiments were conducted using RP-3 aviation kerosene doped with two different soluble catalysts, palladium acetylacetonate (Pd(acac) 2 ) and platinum acetylacetonate (Pt(acac) 2 ), over a range of ppm-level concentrations. Ignition delay time, burning rate and droplet lifetime were systematically quantified to elucidate the influence of catalysts on the fuel combustion behaviors. A stage-resolved analysis was conducted to differentiate ignition onset from quasi-steady burning. The results revealed that both catalysts improve ignition and combustion performance, yet exhibit distinct catalytic roles governed by their thermochemical properties and oxidation states. Earlier ignition is promoted by Pd(acac) 2 due to its low-temperature sublimation and the formation of catalytically active Pd and PdO. The former, however, also competes with the fuel for oxygen at the flame front, inducing an inhibiting effect on droplet burning. These effects together result in a non‑monotonic concentration dependence of the burning rate. In contrast, steadier burning is sustained by Pt(acac) 2 through its stable metallic state Pt. These findings clarify how catalyst decomposition characteristics and oxidation-state stability govern ignition onset and subsequent burning behavior. The present study provides mechanistic insights into fuel-catalyst interactions and guidance for developing fuel-soluble additives to enhance ignition reliability and combustion efficiency in advanced aero-engine systems. Novelty and significance statement This study advances the understanding of fuel-soluble noble-metal catalytic additives by revealing how their transient physicochemical evolution affects single-droplet combustion behaviors. By comparatively resolving the thermochemical evolution of two catalysts, this work demonstrates that decomposition pathways, oxidation-state stability, and catalytic activity collectively modulate stage-specific responses during droplet evaporation, ignition and burning. This stage-resolved perspective moves beyond treating soluble catalysts as static combustion enhancers and clarifies the intrinsic coupling between catalyst evolution and droplet combustion. These mechanistic insights establish transferable principles for the rational design of next-generation fuel-soluble catalytic additives and support an engine-compatible strategy for enhancing high-altitude ignition reliability and combustion efficiency without structural modifications to existing aero-engines. In addition, a U-Net-based deep learning framework is introduced for automatic droplet contour recognition, enabling accurate and efficient droplet combustion diagnostics.
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Small
·
2023
·Vol. 19
·期 20
·2207569
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IF 13.3
Yakun Tian,Ming Wen,Aijian Huang,Qingsheng Wu,Zhiguo Wang,Quanjing Zhu,Tao Zhou,Yongqing Fu
High stability and efficiency of electrocatalysts are crucial for hydrogen evolution reaction (HER) toward water splitting in an alkaline media. Herein, a novel nano-Pt/Nb-doped Co(OH) 2 (Pt/Nb Co(OH) 2 ) nanosheet is designed and synthesized using water-bath treatment and solvothermal reduction approaches. With nano-Pt uniformly anchored onto Nb Co(OH) 2 nanosheet, the synthesized Pt/Nb Co(OH) 2 shows outstanding electrocatalytic performances for alkaline HER, achieving a high stability for at least 33 h, a high mass activity of 0.65 mA µg −1 Pt, and a good catalytic activity with a low overpotential of 112 mV at 10 mA cm −2 . Both experimental and theoretical results prove that Nb-doping significantly optimizes the hydrogen adsorption free energy to accelerate the Heyrovsky step for HER, and boosts the adsorption of H 2 O, which further enhances the water activation. This study provides a new design methodology for the Nb-doped electrocatalysts in an alkaline HER field by facile and green way.
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高影响因子
Catalysts
·
2023
·Vol. 13
·期 3
·626
·
IF 3.9
Dengmao Wu,Xianyan Lv,Xiurong Ren,Changming Hou,Qianwei Ma,Junxuan Yao,Jiangliang Hu
The catalytic oxidation of VOCs is widely acknowledged as the most available technology to reduce air pollution. Among the catalysts for VOCs, 1 wt%-Pt/TiO2catalysts using metal as a doping element have shown amazing potential in many fields. However, achieving high catalytic performance at relatively low temperatures based on the activation of molecules is still a formidable challenge owing to the catalytic activity being highly dependent on temperature. Here, the role of the rare earth metal Ce in the catalytic oxidation of ethane was studied by preparing Pt/CexTi1−xO2(x = 0, 0.002, 0.005, 0.01, 0.02, and 0.05) catalysts. When the Ce/(Ce+Ti) molar ratio was 0.01, Pt/Ce0.01Ti0.99O2achieved 90% ethane conversion at 436 °C. This reaction temperature is 15% lower than that for Pt/TiO2. The characterization results show that the doping of Ce caused lattice expansion of TiO2and its distortion brought about by oxygen vacancies. Additionally, the appropriate amount of Ce-doping can alter the interaction between the active component Pt and the carrier TiO2, thereby improving the activity and concentration of the active surface lattice oxygen species of the catalyst. These results provide a foundation for the design of the catalytic oxidation of VOCs under mild operating conditions.Keywords:VOCs;Pt-based catalyst;catalyst carrier;catalysis;oxidation;Ce-doping
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Materials Today Nano
·
2023
·
IF 10.3
L.K. Pan,J.C. Qi,H. Mei,L. Yao,H.X. Liu,S.X. Zhou,G.Q. Zhu,J.J. Wang,L.F. Cheng,L.T. Zhang
Developing efficient and highly selective photocatalytic CO 2 reduction catalysts remains one of the most significant challenges in achieving carbon neutrality . Herein, the efficient conversion of CO 2 to CH 4 with selectivity close to 100% was achieved by loading uniformly dispersed Pt nanoparticles on the surface of Sr 2 Nb 2 O 7 nanosheets ; the optimal CH 4 yield was as high as 15.65 μmol/g/h. Various characterizations demonstrate that Pt nanoparticles have a significant photothermal effect that can increase the catalyst surface temperature, and improve the performance and electron transport rate of the catalyst. Additionally, Pt nanoparticles and Sr 2 Nb 2 O 7 nanosheets form heterojunctions , which facilitate the separation of photogenerated carriers and aggregation of photogenerated electrons on the Pt nanoparticles. Pt nanoparticles become new reactive sites that have a strong adsorption impact on the key intermediate ∗CO and reduce the reaction energy barrier of ∗CHO generation. The results revealed that the synergy between electron accumulation, strong adsorption of ∗CO, and reduction of the reaction potential of ∗CHO are the reasons for the efficient and selective conversion of CO 2 to CH 4 . This work provides novel insights into the role of metal-based cocatalysts in selective CO 2 photoconversion and new ideas for designing efficient CO 2 conversion systems.
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JOURNAL OF CATALYSIS
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2023
·
IF 7.3
Mengya Guo,Feng Wang,Mingwei Zhang,Li Wang,Xiangwen Zhang,Guozhu Li
Encapsulation of clean metal nanoparticles (NPs) into interior of metal–organic framework (MOF) is of great importance to remarkably improve the stability and tune the catalytic performance of metal NPs. Herein, highly dispersed Pt NPs are encapsulated in UiO-66 with different functional groups on linker (UiO-66-X, X = F, H, NH 2 , OH) through enhanced electron attraction of metal precursor by MOF node and proper reduction by H 2 /Ar gas. Compared with traditional impregnation method, the encapsulation method gives well-defined Pt NPs and controllable microenvironment. Detailed characterizations reveal that functional group of the linker can effectively tune the microenvironment and electronic properties of guest Pt NPs. In situ FTIR was utilized to investigate the adsorption capability and strength of reactants on the catalysts. The electron-deficient Pt species and appropriate surface hydrophobicity match well with the reactants, which is responsible for enhanced catalytic hydrogenation activity of C C and nitro groups. The surface hydrophobicity plays a major role in promoting alkyne hydrogenation. This work is devoted to rationalize the relationship between hydrogenation performance and catalyst property of UiO-66 encapsulated Pt NPs, in terms of energy adaptability in electronic state and structure adaptability in surface chemistry. Rational design strategy of Pt-confined-in-MOF composites through molecular level regulation is provided for hydrogenation.
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FUEL PROCESSING TECHNOLOGY
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2022
·
IF 8.129
Hao Qin,Nengjie Feng,Quan Lv,Hui Wan,Guofeng Guan
Single atomic catalysts (SAC) isolated in zeolite have been reported for hydroisomerization of n-alkanes. However, it is widely found that metal species located outside zeolite crystals have beneficial effects on catalytic performance, rather than inside zeolite. Herein, we introduce cerium oxide as a binder to anchor Pt single atoms on the catalyst surface . Pt species were atomically dispersed on catalyst surface certified by AC HAADF-STEM and XAS. Pt 1 @CeO x /SAPO-11 not only shows significant activity but also effectively inhibits the selectivity of cracking or hydrogenolysis . The turnover frequency value of 0.05%Pt 1 @CeO x/ SAPO-11 reaches 9511 h −1 , 13 times higher than reported catalyst prepared with the space-confined strategy. Reaction mechanisms have been proposed to explain the different effects of platinum status and location on the reaction. Platinum single atoms located outside the catalyst crystal are speculated more favourable to this reaction. Conceptually, catalytic efficiency of this reaction can be improved by dispersing the active sites to reduce the local concentration of the product of a reversible step in an intermediate reaction. An appropriate loading of 0.05 wt% is needed to achieve the high efficiency of the metal and acid sites simultaneously.
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高影响因子
CHEMPHYSCHEM
·
2022
·Vol. 24
·期 7
·e202200505
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IF 3.52
Xujun Ma,Donghui Wang,Jianan Wu,Bin Zhao,Feng Chen
Graphical Fe 3+ doping was utilized to promote the formation of oxygen vacancies and improve the interaction between TiO 2 and atomic Pt. Single Pt atoms anchored on the oxygen vacancy sites of Fe−TiO 2 effectively modify the local energy band structure of TiO 2 , and thus significantly boost the catalytic performance of either the intrinsic or the sensitized photocatalytic process for Pt/Fe−TiO 2 . Single atomic site catalysts display the maximal atom-utilization efficiency, unique structural properties, and remarkable enhancements on catalytic activity. Herein, single Pt atoms loaded Fe−TiO 2 catalysts were prepared. Fe 3+ doping leads to the formation of oxygen vacancies and improve the interaction between TiO 2 and Pt. Single Pt atoms are thus anchored and effectively modify the local energy band structure of TiO 2 . The optimized local band structures improve the intrinsic photoexcitation of Pt/Fe−TiO 2 , promote the separation of photogenerated carriers, and extend the lifetime of photogenerated carriers. Meanwhile, the electrons transfer from the excited dyes to the conduction band edge of Pt/Fe−TiO 2 is also facilitated due to the shift-down of the conduction band edge. Therefore, with the increase of the Pt content (till up to 0.6 wt%), the photocatalytic performance of Pt/ Fe−TiO 2 with the confined single Pt atoms is significantly boosted in either the intrinsic or the sensitized photocatalytic process.
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高影响因子
SYNTHETIC METALS
·
2022
·
IF 4
Zhi Teng,Zhengyan Zhang,Xingwei Li
The supports are of vital importance for supported catalysts. In this work, an excellent anode catalyst support for methanol oxidation reaction is prepared by using polyaniline (PANI) surface modified carbon black (CB), and Pt catalysts are supported on the surface of carbon black modified by polyaniline (Pt/PANI-CB). The characterizations of structure and morphology show that Pt nanoparticles with an average diameter of 2.89 nm are uniformly dispersed on the surface of carbon black modified by polyaniline. Compared with Pt supported on the surface of carbon black (Pt/CB) and commercial Pt/C catalysts, the optimal Pt/PANI-CB has higher electrocatalytic activity, and better stability for methanol oxidation reaction. In 0.5 M H 2 SO 4 solution containing 0.5 M CH 3 OH, the area specific activity of Pt/PANI-CB is 1.81 mA cm −2 Pt, and those of Pt/CB and Pt/C is 1.29 and 0.68 mA cm −2 Pt. After 1000 cycles of cyclic voltammetry , the area specific activity retention of Pt/PANI-CB is 74.0%, while those of Pt/CB and Pt/C are 60.4% and 38.2%. Obviously, as a catalyst support, carbon black modified by polyaniline has broad application prospects.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 26
·期 4
·3263-3273
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IF 3.3
Ziwei Zhai,Bofeng Zhang,Yutong Wang,Guozhu Liu
Based on the disturbance of electronic density, nitrogen-doped nanocarbons show promising properties to anchor metal clusters. However, precisely regulating the coordination mode between N species and the active site remains challenging. Herein, we rationally designed three N types (graphitic N, pyridinic N and pyrrolic N) in nanocarbons to anchor Pt clusters for the benchmark propane dehydrogenation. The specific activity of the pyridinic-N-doped catalyst was 147.54 molC3H6 molPt−1 h−1 at 550 °C, which was 1.3 times higher than those of graphitic- and pyrrolic-N-doped catalysts. Unlike the regular tetrahedron Pt cluster in the graphitic-N catalyst or the distorted three-layered Pt cluster in the pyrrolic-N catalyst, the Pt cluster in the pyridinic-N catalyst was an inverted tetrahedron, which increased the contact degree without geometric repulsion towards C–H bond scission. The geometric parameters of detached H and C atoms in the methylene group for the pyridinic N catalyst was decreased to strengthen the C–H bond scission. After CH3CHCH3* adsorption, the Bader charge of the Pt active site also became highly positive, which tailored the d-band center closer to the Fermi level and provided more vacant orbitals for C–H bond breakage. Therefore, pyridinic N in nanocarbons is promising to anchor small-sized Pt for alkane dehydrogenation in terms of geometric and electronic effects.
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CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Yi-Fan Xue,Jie Feng,Jin-Yao Ma,Wen-Ying Li
C–N bond breaking is a difficult but crucial step in the quinoline removal of coal-based liquids. Noble metal catalysts have higher C–N bond breaking activity, but their surface bond breaking mechanism is unclear. Atomic layer deposition creates more metal-oxide sites and generates different active species, which facilitates the mechanism study. For this reason, we used atomic layer deposition to deposit TiO 2 on the catalyst surface and suggested a more complete C–N bond breaking mechanism in this study. The particle size and pore structure of the catalyst did not change significantly after the deposition, and the hydrogen adsorption was reduced when there were too many layers deposited and the surface Pt sites were occupied to a high degree. TiO 2 is extremely susceptible to reduction to Ti 3+ under hydrogen, and can change the nature of the electron density of Pt through oxygen vacancies, creating Ti 3+ -Pt δ− sites that are prone to protonation reactions. That means, the occurrence of these protonation reactions not only easily breaks the C–N bond, but also accelerates the rate of C–N bond cleavage due to the increased H coverage on the surface of the xcTi-PtAl catalysts. And the Ti 3+ -Pt δ− sites in catalyst had a stronger adsorption effect on the nitrogen-containing compounds, which in turn lowered the energy barriers of bond cleavage. It is concluded that protonation is a necessary step before the C–N bond can be broken. The subsequent steps were showed by the DFT calculations that the nitrogen-containing compounds adsorbed on the Ti 3+ -Pt δ− sites undergo β-H fracture after the protonation reaction, with the elimination reaction cleaving the C–N bond. The xcTi-PtAl catalysts by atomic layer deposition of Ti not only improve the C–N bond breaking performance, but also improve bond breaking stability by a factor of four compared to the Pt/Al 2 O 3 catalysts.
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