CERAMICS INTERNATIONAL
·
2021
·
IF 4.527
Yi Wang,Jialiang Chen,Lan Wang,Hanqin Weng,Zhihao Wu,Limin Jiao,Yusa Muroya,Shinichi Yamashita,Sheng Cheng,Fuhai Li,Hongbing Chen,Wei Huang,Mingzhang Lin
The large-scale synthesis and the stabilization of noble metal nanocatalysts with ultrasmall sizes are crucial to their practical application. Herein, Pd, Au, and Pt nanoparticles (NPs) are in situ embedded on boron nitride nanosheets (BNNSs) via the reduction of precursor salts induced by 60 Co γ-irradiation, which is a mature technique widely used in industry. The reduction mechanism was elucidated by pulse radiolysis experiments. In comparison with other BN substrates like hexagonal BN ( h -BN), BNNSs had not only large surface area of 263 m 2 g −1 , but also abundant hydroxyl groups produced during the sonicated exfoliation, resulting in ultrasmall sizes, large loading amounts, and uniform distribution of the anchored NPs. The particle sizes of the loaded Pd, Au, and Pt NPs were measured to be 2.9, 3.1, and 3.0 nm, respectively. As a consequence, in the model reaction of 2-nitroaniline reduction, the Pd-, Au- and Pt-BNNSs composite nanocatalysts showed much higher catalytic activities than those composites loading the corresponding NPs on other BN substrates. Particularly, most of the 2-nitroaniline could be reduced within merely 40 s when using Pd-BNNSs as catalysts, performing a rate constant of 1.1 × 10 −1 s −1 . The number of hydroxyl groups on BNNSs support as well as the catalytic performance of the corresponding NPs-loaded BNNSs composites could be improved by extending the sonicated exfoliation time, because more NPs were loaded and the hydroxyl groups were also proved to play an important role in enhancing the catalytic activity. Moreover, Pd-BNNSs catalysts still displayed prominent activity even after five cycles owing to the high stability of BNNSs and their strong affinity for PdNPs. This work not only demonstrates BNNSs as ideal supports to load noble metal NPs for catalysis, but also reveals the feasibility to synthesize and in situ embed ultrasmall noble metal NPs on BNNSs via γ-irradiation.
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NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 3
·1686-1694
·
IF 3.591
Kezhong Wu,Pengyuan Fu,Bei Ruan,Mengmeng Wu,Mingxing Wu,Ruitao Wu
Replacing the expensive Pt catalyst of counter electrodes (CEs) with a low-cost Pt-free catalyst has been regarded as one of the crucial steps for cost effectiveness of dye-sensitized solar cells (DSSCs). Herein, MnWO4 as a binary mixed oxide (MnO–WO3) has been prepared with (NH4)10H2(W2O7)6·xH2O and Mn(NO3)2·4H2O via a facile hydrothermal method. DSSCs using MnWO4 CEs show power conversion efficiency (PCE) of 4.93%. To improve the catalytic activity of MnWO4 CEs further, three proportions of MnWO4@AC mixed oxide composite catalysts have been fabricated via simple physical mixing MnWO4 with activated carbon (AC) by ball-milling. Moreover, the DSSCs with the MnWO4@AC composites CEs generate high PCE of 6.50, 6.45 and 6.12%, respectively, from MnWO4 : AC mass ratios of 1 : 2, 1 : 1 and 2 : 1 for the regeneration of traditional iodide/triiodide (I3−/I−) redox couples, which were superior to the pristine MnWO4, Pt- and AC-based counterpart 4.93%, 4.54% and 2.10% CEs under the same test conditions and method. The favorable performances make MnWO4@AC composites act as a new resource of electro-catalytic Pt-free materials for high-performance CEs in the encapsulation of DSSCs.
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Nano Select
·
2021
·Vol. 2
·期 11
·2126-2134
·
IF 0
Junwei Liang,Yuxiang Liu,Rongzheng Liu,Sufan Zheng,Zhichun Si,Duan Weng,Feiyu Kang
Preparing stable highly dispersed Pt based electrocatalyst is promising to reduce material expense of H 2 product via electrocatalytic water splitting. However, it is still a great challenge to obtain stable single atomic Pt catalysts which can be applied in acidic electrolyte. In the present work, we synthesized Pt atomic clusters on carbon quantum dots (CQDs) grafting multiwall carbon nanotube (CNT) (Pt content: 1 wt.%) catalysts and then loading the catalysts on carbon cloth (Pt content: 0.01 mg▪cm –2 ) for activity test. The overpotential of 29 mV versus RHE was obtained over 1%Pt/CQDs/CNT catalysts at the current density of 10 mA▪cm –2 , and the Tafel slope of 22 mV decade –1 was obtained, too. Especially, the catalysts showed significant stability in hydrogen evolution reactions (HER) in acidic solution, of which the overpotential was still smaller than that of 20%Pt/C after 10,000 CV cycles. CQDs provided coordinating sites for dispersing Pt atomic clusters and improved the H + concentration in adjacent area around the Pt clusters. This method provides a general strategy to design the highly efficient electrocatalysts with ultra-low precious metals for H 2 evolution in acidic electrolyte.
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Nanoscale Research Letters
·
2013
·Vol. 8
·期 1
·1-8
·
IF 2.524
Jamal Ruxangul,Xu Feng,Shao Weiwei,Abdiryim Tursun
The solid-state method was applied for synthesizing polyaniline (PANI)/noble metal hybrid materials with the presence of HAuCl 4 ·4H 2 O or H 2 PtCl 6 ·6H 2 O in the reaction medium. The structure, morphology, and electrochemical activity of the composites were characterized by Fourier transform infrared (FTIR) spectra, UV-visible (vis) absorption spectra, energy dispersive spectrum (EDS), X-ray powder diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM), and cyclic voltammetry. The results from FTIR and UV-vis spectra showed that the oxidation degree and doping level of the PANI in composites can be influenced by HAuCl 4 ·4H 2 O and H 2 PtCl 6 ·6H 2 O. The EDS data demonstrated that the composites contain a certain amount of Au (or Pt) element. XRD analysis indicated the presence of crystalline-state Au particles in PANI matrix prepared from the presence of HAuCl 4 ·4H 2 O and revealed that the H 2 PtCl 6 ·6H 2 O cannot be converted into metal Pt. The TEM and SEM images implied that the Au particles did exist in the polymer matrix with the size of about 20 nm. The enzymeless H 2 O 2 sensor constructed with PANI/Au composite from the presence of HAuCl 4 ·4H 2 O showed a short response time (within 5 s) and displayed an excellent performance in wide linear range.
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高影响因子
Science China-Materials
·
2017
·Vol. 60
·期 11
·1121-1128
·
IF 3.956
Yang Hongchao,Wang Changhong,Hu Feng,Zhang Yejun,Lu Huan,Wang Qiangbin
The synthesis of atomic-scale metal catalysts is a promising but very challenging project. In this work, we successfully fabricated a hybrid catalyst of Ptc/Ni(OH) 2 with atomic-scale Pt clusters uniformly decorated on porous Ni(OH) 2 nanowires (NWs) via a facile room-temperature synthesis strategy. The as-obtained Pt c /Ni(OH) 2 catalyst exhibits highly efficient hydrogen evolution reaction (HER) performance under basic conditions. In 0.1 mol L −1 KOH, the Pt c /Ni(OH) 2 has an onset overpotential of ~0 mV vs. RHE, and a significantly low overpotential of 32 mV at a current density of 10 mA cm −2 , lower than that of the commercial 20% Pt/C (58 mV). The mass current density data illustrated that the Pt c /Ni(OH) 2 reached a high current density of 6.34 Amg
−1 Pt
at an overpotential of 50 mV, which was approximately 28 times higher than that of the commercial Pt/C (0.223 A mg
−1 Pt
) at the same overpotential, proving the high-efficiency electrocatalytic activity of the as-obtained Pt c /Ni(OH) 2 for HER under alkaline conditions.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2025
·Vol. 27
·期 30
·16030-16038
·
IF 2.9
Kyong–Mi Kim,Kyong–Sik Ju,Sung–Nam Pak
The ethanol oxidation reaction (EOR) was studied on carbon-supported Pt and Pt–Mo electrocatalysts prepared by the formic acid reduction method following heat-treatment. The catalysts were physically characterized by X-ray diffraction (XRD) and transmission electron microscopy (TEM). The electrocatalytic activity of the Pt/C and Pt–Mo/C electrocatalysts for the EOR was investigated by potentiostatic and potentiodynamic measurements with pinhole on-line differential electrochemical mass spectrometry (PODEMS). The results show that the Pt–Mo/C electrocatalyst compared with Pt/C has higher ethanol oxidation efficiency and, acetaldehyde and acetic acid are majority products during the EOR under the given conditions. The CO2 current efficiencies (CCEs) on the Pt/C and Pt–Mo/C catalysts are 6.9% and 8.8% after calibration of the mass to charge signal m/z = 44, respectively, which reveals that the co-metal molybdenum produces more CO2 for ethanol electrooxidation and promotes the performance of the Pt-based anode catalyst.
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PubMed
高影响因子
ACS Applied Nano Materials
·
2025
·
IF 5.5
Xudong Zhao,Shuibo Wang,Hua Li,Yushi Wei,Yiming Li,Haocheng Li,Hongbo Yu,Kaijie Li,Haotian Li,Hongfeng Yin
Preventing nanoparticle migration and agglomeration on the surface of supported heterogeneous catalysts, especially at tailored bimetallic sites, poses a significant challenge. The reverse water–gas shift (RWGS) reaction is considered a promising route for converting CO2 into CO, an essential feedstock for industrial chemical production. Herein, a core–shell nanostructure anchoring on the surface was developed, which consists of a PtFe bicomponent core (∼2.6 nm) and a nitrogen-doped carbon nanoshell (∼1.3 nm). This structural design enhances the CO2 adsorption saturation, weakens the CO adsorption strength, and promotes hydrogen spillover. This PtFe core–shell material (Pt/Fe = 1:1) demonstrates an elevated reaction rate of 12.58 molCO2 gPt–1 h–1, with nearly 100% CO selectivity at 450 °C and atmosphere pressure. The activity is 5.1-fold higher than that of the Pt nanoparticle, attributed to the tuned geometric and electronic properties. The nitrogen-doped carbon nanoshell preserves the core–shell morphology at a high temperature. Moreover, the in situ experiments reveal the H-assisted dissociation/activation of the CO2 pathway for RWGS. The integration of the bimetallic synergy and core–shell structure is a potent strategy for thermal catalytic processes.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Jingxu Liu,Yanning Ren,Yi Zhao,Haoyun Zhou,Xiaohui Liu,Yong Guo,Yanqin Wang
The hydrotreatment of fats and oils for biofuel synthesis significantly contributes to carbon emission mitigation. Conventionally, this process necessitates a bifurcated pathway encompassing hydrodeoxygenation (HDO)/decarboxylation (DCO) and subsequent isomerization reactions. In this research, we synthesized a niobium-doped bifunctional catalyst, denoted as Pt/AlSiO-Nb, capable of concurrently executing HDO and isomerization of palm oil. Our examination of the palm oil hydrotreatment network, with palm acid and tripalmitin as representative model compounds, revealed that the oil undergoes hydrolysis to form fatty acids and then undergoes deoxygenation to n-alkanes via HDO or DCO routes, succeeded by n-alkane isomerization, where cracking reactions also transpire. Comprehensive characterizations of the catalyst delineated that niobium incorporation markedly augments the support–platinum interaction and proliferates the catalyst’s medium and weak acid sites, culminating in enhanced HDO and isomerization performance. These insights herald a novel methodology for biofuel generation from fats and oils, offering a streamlined approach to their catalytic transformation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2017
·
IF 4.233
Yan Gao,Yiwei Zhang,Yuming Zhou,Chao Zhang,Hongxing Zhang,Shuo Zhao,Jiasheng Fang,Mengqiu Huang,Xiaoli Sheng
In this work, we report a feasible approach to synthesize a ternary nanocomposites , Pt/lanthanum doped mesoporous zirconium oxide (Pt/La 2 O 3 -ZrO 2 ), via an effective two-step method. Ordered mesoporous La 2 O 3 -ZrO 2 composites were firstly fabricated with mesoporous silica KIT-6 as a hard template. Subsequently, uniform Pt nanoparticles encapsulated by 4 hydroxyl-terminated poly (amidoamine) (G4-OH PAMAM) dendrimers were deposited on the La 2 O 3 -ZrO 2 composites. The as-prepared samples were characterized by transmission electron microscope (TEM), N 2 adsorption–desorption isotherm analysis, energy dispersion X-ray analysis (EDX), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and temperature programmed reduction (H 2 -TPR). The average size of PtDENs was found to be 1.48 nm in diameter. Furthermore, the introduction of La could improve the structure of the supports which was confirmed by XRD and H 2 -TPR analysis. The reduction of p-nitrophenol to p-aminophenol by NaBH 4 was utilized to evaluate the catalytic performances of catalysts. Results indicated that the Pt/La 2 O 3 -ZrO 2 catalyst calcined in nitrogen at 550 °C exhibited the highest catalytic performance and still kept the high catalytic activity even after six cycles. This phenomenon suggests that synergistic effect among Pt-Zr-La could enhance the catalytic efficiency. Finally, reaction mechanism was proposed for the reduction of p-nitrophenol.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Guanwei Zhao,Wei Ma,Hongyu Pang,Ligang Zhang,Yuzheng Wang,Xiaoxue Ren,Kuo Liu,Hongling Yang,Yongchun Liu
Low-temperature catalytic oxidation is a prevalent technology for toluene removal due to its reduced energy demand. In this study, N,N-dimethylformamide (DMF) was used to control the particle size of active metals. The activity tests revealed that Pt nanoparticles with a particle size of 5–15 nm exhibited higher activity for toluene oxidation and maintained good hydrothermal stability on the SBA-15 support. The results suggest that despite the increase of Pt particle size by using DMF, the proportion of Pt 0 and the oxygen activation ability were both increased. The reaction pathway of the toluene oxidation over Pt/SBA-15 was examined in depth by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), proton transfer reaction time-of-flight mass spectrometry (PTR-TOF-MS) and cluster analysis, revealing that the benzyl alcohol, benzaldehyde, and benzoic acid species were primary intermediate products. The benzaldehyde on the larger Pt nanoparticles is conducive to decomposing and generating CO 2 for complete mineralization, promoting the activity of toluene oxidation. This work highlights the significance of DMF-induced size effects in the development of low-temperature oxidation catalysts and understanding of reaction mechanism, guiding the design of new efficient toluene oxidation catalysts.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Anqi Zhao,Wei Zhou,Xin Wang,Zhongjie Song,Nannan Zhang,Huan Zhang,Xinyu Gu,Jiawei Qiang,Zhengying Wu,Yong Wang,Yukou Du
Strong electronic interactions at the heterojunction interfaces of heterostructured catalysts can effectively regulate the electronic structure, optimize the adsorption of reactants and intermediates, and enhance the electrooxidation of alcohols. Due to this unique structural advantage, heterostructured catalysts are widely utilized as anode catalysts for alcohol fuel cells. However, the controlled synthesis of ternary metal heterostructures remains a significant challenge. In this study, we successfully synthesized Pt-PdPtFe ternary metal hetero-nanosheets (HNSs) using a seed-mediated method. The synergistic effects of the three metals, along with the strain effect at the heterojunction interface, contribute to the enhanced alcohol oxidation performance of Pt-PdPtFe HNSs compared to commercial Pd/C and numerous previously reported advanced catalysts. The mass activities for ethylene glycol oxidation reaction (EGOR) and glycerol oxidation reaction (GOR) are 9.77 A mg Pd+Pt −1 and 6.04 A mg Pd+Pt −1 , respectively. Furthermore, CO stripping tests and durability tests indicate that Pt-PdPtFe HNSs exhibit excellent anti-poisoning ability and cyclic stability. This research presents a viable strategy for the controlled synthesis of ternary metal heterostructures, while also offering valuable insights into the rational design of high-performance electrocatalysts.
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高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2025
·
IF 3.7
Yi-Fan Xue,Fei Zhao,Jie Feng,Wen-Ying Li
In hydrofining processes, the competitive interactions among sulfur-containing compounds, aromatic hydrocarbons, and nitrogen-containing intermediates fundamentally govern catalytic performance. Nevertheless, the complex kinetic relationships within hydrodenitrogenation (HDN) systems have remained unclear and insufficiently investigated. This research comprehensively and systematically examined the competitive reaction kinetics of naphthalene (an aromatic model) and dibenzothiophene (a sulfur-based model) during the HDN of 1,2,3,4 - tetrahydroquinoline over Pt-based catalysts. Through systematic analysis of conversion rates and product distributions across various reaction conditions, it demonstrated that both dibenzothiophene and naphthalene exert distinct inhibitory effects on HDN through mechanistically differentiated pathways. Quantitative evaluation revealed a pronounced temperature dependence in mitigating these inhibitory effects, whereas pressure variations exhibited negligible influence. These findings collectively demonstrate that surface adsorption competition, rather than hydrogen availability, dictates the reaction kinetics. Rigorous kinetic calculations and rate constant fittings identified the hydrogenation of 1,2,3,4-tetrahydroquinoline to decahydroquinoline as the rate-limiting step susceptible to competitive inhibition. This phenomenon predominantly arises from the tripartite competitive adsorption among naphthalene, dibenzothiophene, and 1,2,3,4-tetrahydroquinoline at catalytic active sites, as corroborated by theoretical adsorption energy calculations. Notably, the two inhibitors manifest divergent interaction mechanisms: H + ions generated during H 2 S formation in dibenzothiophene desulfurization facilitate C–N bond cleavage, whereas naphthalene directly suppresses this critical step. Furthermore, atomic-layer-deposited TiO 2 on Pt/Al 2 O 3 engineered the catalyst surface through three synergistic effects: enhanced nitrogen adsorption capacity, optimized hydrogen spillover pathways, and generation of additional C–N bond cleavage sites. This multi-effect strategy effectively reduces the negative impacts of competitive adsorption, emphasizing the crucial role of competitive reaction kinetics in designing sulfur/aromatic-resistant HDN catalysts.
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