ACS Applied Materials & Interfaces
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2021
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IF 9.229
Xiao Chen,Xing-Bao Wang,Shuhua Han,Dong Wang,Chuang Li,Weixiang Guan,Wen-Ying Li,Changhai Liang
Interactions between metals and oxide supports are crucial in determining catalytic activity, selectivity, and stability. For reducible oxide supported noble metals, a strong metal–support interaction (SMSI) has been widely recognized. Herein we report the intermediate selectivity and stability over an irreducible SiO2 supported Pt catalyst in the hydrogenation of anthracene that are significantly boosted due to the SMSI-induced formation of intermetallic Pt silicide and Pt–SiO2 interface. The limitation in the strong interaction between Pt nanoparticles and irreducible SiO2 has been breached by combining the strong electrostatic adsorption method and following the high temperature reduction strategy. Due to the isolated Pt active sites by Si atoms, the activated H species produced over the Pt2Si/SiO2 catalyst with an initial catalytic activity of 2.49 μmol/(m2/g)/h as well as TOF of 0.95 s–1 preferentially transfer to the outer ring of anthracene to 87% yield of symmetric octahydroanthracene (sym-OHA) by subsequent hydrogenation. In addition, the Pt2Si/SiO2 catalyst presents an excellent stability after five cycles, which can be attributed to the fact that intermetallic Pt2Si nanoparticles are anchored firmly onto the surface of the SiO2 support. The discovery contributes to broaden the horizons on the SMSI effect in the irreducible oxide supported metal particle catalysts and provides guidance to design the metal–SiO2 interface and tune the surface chemical properties in diverse application conditions.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
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IF 14.224
Yunchong Liu,Xunxun Li,Dongyun Chen,Najun Li,Qingfeng Xu,Hua Li,Jinghui He,Jianmei Lu
An optimized oxygen activity of catalysts can facilitate oxidation of volatile organic compounds. This work shows the first construction of Ce–Co oxide thin–walled nanoboxes. Bulk–phase lattice oxygen is activated by metal–metal interactions. The subsequent uniform dispersion of low loaded Pt nanoparticles further enhances the surface–adsorbed oxygen content, and creates an oxygen–rich reaction interface. Competitive adsorption of water vapor was also inhibited, and complete catalytic oxidation of toluene was achieved at low temperature (T 90 =140 °C). A diffuse reflectance infrared Fourier–transform spectroscopy probe was used to investigate the adsorption–catalytic process and the possible synergistic catalytic mechanism (Langmuir–Hinshelwood and Mars–van Krevelen). This work provides a strategy for improving the catalyt Crystal structure ic oxidation performance of nanocatalysts for volatile organic compounds by increasing the catalytic oxygen activity.
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ANALYTICAL LETTERS
·
2026
·
IF 1.8
Hanwen Zhang,Yuhan Zhang,Yiqi Zhao,Ning Zhao,Qian Lu,Sheng Gao,Zhizhou Yang,Xian Zhang
Nanozymes have attracted extensive attention due to their tunable composition, low preparation cost and facile synthesis. In this study, oxidase -like Pt-doped poly (N-isopropylacrylamide) nanogels (Pt@PNIPAM NG) were prepared by in situ polymerization of N-isopropylacrylamide in the presence of Pt nanoparticles (Pt NPs). The catalytic mechanism was studied by selective scavengers for specific reactive oxygen species (ROS). Results revealed that Pt@PNIPAM NGs could catalyze molecular oxygen to produce singlet oxygen (1O2) and superoxide radicals (O2•-). Michaelis-Menten kinetics analysis revealed that Pt@PNIPAM NGs exhibit a significantly lower Km (0.121 mM) than pure PNIPAM NGs (7.617 mM). This enhanced substrate affinity indicates that incorporating Pt NPs into the nanogel matrix effectively boosts the overall oxidase-like catalytic performance. Pt@PNIPAM NG can catalyze the oxidation of colorless 3,3,5,5-tetramethylbenzidine (TMB) into blue oxidized TMB (oxTMB). Moreover, ascorbic acid (AA) can reduce oxTMB back to TMB, resulting in a color change and a corresponding decrease in absorbance. Additionally, Pt@PNIPAM NG can also catalyze the oxidation of AA to dehydroascorbic acid (DHA) by reactive oxygen species; o-phenylenediamine (OPD) subsequently reacts with DHA to form fluorescent quinoxaline derivatives. Based on these reactions, a dual-mode colorimetric and fluorometric detection platform for AA was constructed. The platform enabled rapid detection of AA within 10 min. The platform enabled rapid AA detection within 10 min with linear ranges of 1–85 and 1–120 μM and LODs of 0.76 and 0.062 μM for colorimetric and fluorometric modes, respectively. Finally, the dual-mode detection platform was validated using serum mimetic samples, yielding satisfactory analytical results.
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Catalysts
·
2023
·Vol. 13
·期 11
·1428
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IF 3.9
Ze Xiao,Xi Lin,Wenhua Feng,Binyi Chen,Qingwei Meng,Tiejun Wang
Hydrogen from biomass, as a promising alternative fuel, is becoming considerably attractive due to its high energy density and clean emissions. The aqueous phase reforming (APR) of biomass-derived oxygenated hydrocarbons and water is a renewable and efficient pathway for hydrogen production and shows great potential. However, the key to the application of this technique is to develop catalysts with high hydrogen productivity. In this work, we first synthesized polyaniline–platinum (PANI-Pt) organo-metallic hybrid precursors and then obtained a high-loaded (~32 wt.% Pt) and highly dispersed (~3 nm Pt particles) Pt@NC−400 catalyst after pyrolysis at 400 °C, and the nanoparticles were embedded in a nitrogen-doped carbon (NC) support. The Pt@NC−400 catalyst showed an almost three times higher hydrogen production rate (1013.4 μmolH2/gcat./s) than the commercial 20% Pt/C catalyst (357.3 μmolH2/gcat./s) for catalyzing methanol–water reforming at 210 °C. The hydrogen production rate of 1,2-propanediol APR even reached 1766.5 μmolH2/gcat./s over the Pt@NC−400 catalyst at 210 °C. In addition, Pt@NC−400 also exhibited better hydrothermal stability than 20% Pt/C. A series of characterizations, including ICP, XRD, TEM, SEM, XPS, N2physisorption, and CO chemisorption, were conducted to explore the physiochemical properties of these catalysts and found that Pt@NC−400, although with higher loading than 20% Pt/C (~23 wt.% Pt, ~4.5 nm Pt particle), possessed a smaller particle size, a more uniform particle distribution, a better pore structure, and more Pt metal active sites. This study provides a strategy for preparing high-loaded and highly dispersed nanoparticle catalysts with high hydrogen productivity and sheds light on the design of stable and efficient APR catalysts.Keywords:oxygenated hydrocarbons;Pt@NC catalysts;aqueous phase reforming;hydrogen production
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
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IF 9.9
He Xiao,Meng Bai,Man Zhao,Zimei Fu,Wenxiang Wang,Peipei Zhao,Jiamin Ma,Li Zhang,Junming Zhang,Yingluo He,Jian Zhang,Jianfeng Jia
To easily load Pt on smoothy graphene synthesized by cathodic exfoliation method and achieve adjacent plane distribution of Pt, carbon dots (CDs) are used to construct anchoring points to load highly dispersed Pt species due to strong interaction between CDs and Pt species. The composite of Pt-CDs/graphene is synthesized via a continuous process of cathodic exfoliation-hydrothermal-impregnation-reduction. Characterization results indicate the distribution configuration of Pt varies from coated structure of CDs@Pt to dispersed configuration of CDs&Pt or Pt&CDs, then to wrapping configuration of Pt@CDs with increased amount of CDs. It’s found that suitable introduction of CDs promotes the adjacent plane distribution of Pt species. The obtained best Pt-4CDs/G shows the low overpotential of 36 mV (10 mA⋅cm −2 ) and high mass activity of 3747.8 mA mg −1 at −40 mV towards electrocatalytic hydrogen evolution reaction (HER), 9.2 times more active than that of Pt/C (406.2 mA mg −1 ). The superior HER performance of Pt-4CDs/G is attributed to its relatively adjacent plane distribution of Pt, which supports high electrochemically active surface area and more adjacent Pt sites for H* adsorption. Benefitting from that, the HER process for Pt-4CDs/G favorably follows the Tafel pathway, resulting in low hydrogen adsorption free energy and excellent HER activity.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2017
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IF 3.012
Qinglin Sheng,Duo Liu,Jianbin Zheng
In this paper, a sensitive novel non-enzymatic nitrite electrochemical sensor based on Pt nanoparticles loaded Ni(OH) 2 /Multi-Walled Carbon Nanotubes nanocomposites (Pt/Ni(OH) 2 /MWCNTs) was described. The composition and morphology of the Pt/Ni(OH) 2 /MWCNTs were characterized by transmission electron microscope and investigated energy dispersive X-ray spectra respectively. Results showed that the Pt nanoparticles could be anchored on the surface of the Ni(OH) 2 /MWCNTs uniformly through a simple reduction process. The electrochemical investigation of the sensor revealed that the Pt/Ni(OH) 2 /MWCNTs exhibited remarkable electrocatalytic performance toward nitrite oxidation , with a sensitivity of 145 μA mM − 1 cm − 2 and a low detection limit of 0.13 mM. Moreover, the obtained Pt/Ni(OH) 2 /MWCNTs modified GCE with excellent reproducibility and selectivity also allows for practical application. It is expected that the combination of noble metal with Ni(OH) 2 /MWCNTs could be expanded to enhance the catalytic performances of nanocomposites and used for the construction of high-sensitive electrochemical sensors.
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Molecular Catalysis
·
2023
·
IF 4.6
Haoyu Liu,Yanran Cui,Minglu Zhu,Yugang Fu,Yue Sun,Zhen Meng,Bo Peng,Lei Nie
Advanced engine technologies and environmental restrictions require new-generation automotive catalysts to be low-temperature (LT) active and high-temperature (HT) stable simultaneously. Here, incorporation of Ag over high temperature (800 °C) treated Pt/CeO 2 was applied to address the challenge. Strong Pt-O-Ce bonds in Pt/CeO 2 helped improve thermal stability dramatically. Detailed reaction kinetics analysis indicated Eley-Rideal (ER) mechanism for Ag/CeO 2 catalysts and Mars-van Krevelen (Mvk) mechanism for both Pt/CeO 2 and Ag/Pt/CeO 2 catalyst. After calcined at 800 °C, CO adsorbed on ionic Pt site could be readily oxidized by neighbouring oxygen species at a temperature as low as 132 °C over Ag/Pt/CeO 2 , about 60 °C lower than Pt/CeO 2 and Ag/CeO 2 . Raman spectroscopy and XPS results suggested that incorporation of Ag created more oxygen defects over Pt/CeO 2 and oxygen species on Ag nanoparticles might be more active than bare Pt/CeO 2 which would enhance the low-temperature activity for Ag/Pt/CeO 2 . It might be an effective and cost-efficient approach to develop new catalysts for vehicle emission oxidation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
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IF 22.1
Tiantian Wang,Dan Zhang,Jiawei Fei,Wenhao Yu,Jiawei Zhu,Yanyun Zhang,Yue Shi,Minge Tian,Jianping Lai,Lei Wang
The construction of interactions and synergies between sub-nanometric clusters and supports provides unexpected opportunity to realize high performance and low-cost composite catalysis. However, hierarchical micro/nano-porous structured catalysts closely related to mass transport have been neglected as support, which may play a leading role in industrial practical applications. Herein, we report sub-nanometric Pt clusters supported Co aerogel (Pt x /Co, X is the wt% of Pt) with hierarchical micro/nano-porous structure, and after optimization of the loading, Pt 0.25 /Co shows excellent HER performance. Additionally, Pt 0.25 /Co demonstrates the industrially needed current density of 1.0 A cm −2 at 1.8 V in PEM electrolyser, achieving stability in excess of 200 h. Theoretical calculations show that the advantages of the hierarchical micro/nano-porous structure accelerate the mass transport at the three-phase interface, and the strong interaction between sub-nanometric Pt clusters and Co aerogel not only optimizes the electronic structure of Pt 0.25 /Co, but also inhibits the dissolution of sub-nanometric Pt clusters.
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Nanomaterials
·
2023
·Vol. 13
·期 19
·2633
·
IF 5.3
Qian Zhang,Minying Wu,Yuanyuan Fang,Chao Deng,Hsin-Hui Shen,Yi Tang,Yajun Wang
In this study, Pt nanoparticles-loaded nitrogen-doped mesoporous carbon nanotube (Pt/NMCT) was successfully synthesized through a polydopamine-mediated “one-pot” co-deposition strategy. The Pt source was introduced during the co-deposition of polydopamine and silica on the surface of SiO2nanowire (SiO2NW), and Pt atoms were fixed in the skeleton by the chelation of polydopamine. Thus, in the subsequent calcination process in nitrogen atmosphere, the growth and agglomeration of Pt nanoparticles were effectively restricted, achieving the in situ loading of uniformly dispersed, ultra-small (~2 nm) Pt nanoparticles. The method is mild, convenient, and does not require additional surfactants, reducing agents, or stabilizers. At the same time, the use of the dual silica templates (SiO2NW and the co-deposited silica nanoclusters) brought about a hierarchical pore structure with a high specific surface area (620 m2g−1) and a large pore volume (1.46 cm3g−1). The loading process of Pt was studied by analyzing the electron microscope and X-ray photoelectron spectroscopy of the intermediate products. The catalytic performance of Pt/NMCT was investigated in the reduction of 4-nitrophenol. The Pt/NMCT with a hierarchical pore structure had an apparent reaction rate constant of 0.184 min−1, significantly higher than that of the sample, without the removal of the silica templates to generate the hierarchical porosity (0.017 min−1). This work provides an outstanding contribution to the design of supported noble metal catalysts and also highlights the importance of the hierarchical pore structure for catalytic activity.Keywords:platinum;nitrogen doping;mesoporous carbon nanotubes;catalysis
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Journal of Energy Chemistry
·
2023
·
IF 13.1
Feng Zhou,Xiaofeng Ke,Yihuang Chen,Mei Zhao,Yun Yang,Youqing Dong,Chao Zou,Xi'an Chen,Huile Jin,Lijie Zhang,Shun Wang
The scarcity, high cost and susceptibility to CO of Platinum severely restrict its application in alkaline hydrogen oxidation reaction (HOR). Hybridizing Pt with other transition metals provides an effective strategy to modulate its catalytic HOR performance, but at the cost of mass activity due to the coverage of modifiers on Pt surface. Herein, we constructed dual junctions’ Pt/nitrogen-doped carbon (Pt/NC) and δ-MoC/NC to modify electronic structure of Pt via interfacial electron transfer to acquire Pt-MoC@NC catalyst with electron-deficient Pt nanoparticles, simultaneously endowing it with high mass activity and durability of alkaline HOR. Moreover, the unique structure of Pt-MoC@NC endows Pt with a high CO-tolerance at 1,000 ppm CO/H 2 , a quality that commercial Pt-C catalyst lacks. The theoretical calculations not only confirm the diffusion of electrons from Pt/NC to MoC/NC could occur, but also demonstrate the negative shift of Pt d -band center for the optimized binding energies of *H, *OH and CO.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Wei Li,Liang Xian,Yamin Zhao,Chufeng Sun
Ultrafine Pt nanoparticles (Pt UPs) were prepared using a stepwise modulation approach, ensuring consistent reaction kinetics throughout each step to achieve uniform size and high dispersion of Pt UPs. The morphology of the Pt nanoparticle was precisely controlled by managing the reaction conditions at each step, thereby enhancing the catalytic activity of the Pt metals. In order to form photoinduced hydrolysis products with different dispersions and particle sizes, two steps were conducted. First, homogeneously dispersed photoinduced hydrolysis products were adsorbed on nitrogen-doped multiwalled carbon nanotubes using ice photochemistry under stabilizer-free conditions. Second, these products were photoinduced by using different wavelengths of light. Subsequent in situ reduction with various reducing agents influenced the composition, particle size, and dispersion degree of the Pt UPs. Furthermore, the subtle charge transfer between the supporter and Pt was adjusted by employing low- and high-temperature nitrogen doping methods, resulting in Pt UPs with electron-deficient and electron-rich charge structures on the surface. This study offers insights into the precise modulation of the Pt nanoscale morphology and reveals the subtle adjustments in charge transfer between the supporter and the metal through nitrogen doping. Additionally, the origin of the catalytic activity of Pt in various reactions was explored.
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ENERGY & FUELS
·
2023
·
IF 5.3
Jun Tang,Jinzhao Huang,Sixuan Zhang,Zehui Liu,Xiaolong Deng
Metal-phase MoS2 (1T-MoS2) is considered a promising candidate as a catalyst for the hydrogen evolution reaction (HER). However, the instability of 1T-MoS2 limits its electrocatalytic activity. Herein, we first synthesized 1T-MoS2 with excellent HER catalytic performance by a simple one-pot hydrothermal strategy of introducing the d-electron-rich transition metal atom Ni into MoS2. A bimetallic monatomic catalyst (Pt@1T-MoS2–Ni) was also prepared by modifying 1T-MoS2–Ni with Pt single atoms (Pt SAs). Experiments show that the electron transfer caused by Ni doping leads to the 1T phase transition, and the modification of Pt SAs further improves the electrical conductivity. These two factors synergistically modulate the electronic composition of MoS2 and increase the number of reactive sites. In consequence, the Pt@1T-MoS2–Ni catalyst exhibits significantly enhanced HER activity, achieving an overpotential as low as 76 mV at 10 mA/cm2 with the corresponding Tafel slope of only 46 mV/dec. Moreover, the current attenuation is negligible within 12 h, surpassing the performance of MoS2. This study offers ideas for improving the efficiency and stability of 1T-MoS2 catalyst designs.
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