Molecular Catalysis
·
2025
·
IF 4.9
Esimoneze Emmanuel Chinedu,Dilong Qiang,Xueqian Wu,Wei Liu,Haizhou Cao,Zhaolian Ye,Zhen Li,Songjian Zhao
The Pt-based catalyst for purifying chlorinated volatile organic compounds (Cl-VOCs) has the advantages of high catalytic efficiency and low ignition temperature, but the problem of poor resistance to chlorine and water poisoning has not been effectively solved. A series of 0.5 Pt-Ti catalysts were prepared for chlorobenzene (CB) catalytic oxidation by adjusting the interfacial stability and dispersibility of the TiO 2 and Pt through the organic acid strategy in this study. The introduction of tartaric acid (TA) effectively enhanced the surface reduction performance of 0.5Pt-Ti-TA and the proportion of Pt 4+ on the surface. In addition, TA can strongly coordinate with Ti center to form stable titanium-containing complexes, improve the dispersion of Pt, prevent particles from agglomerating, and make the distribution of active sites more uniform. The designed 0.5Pt-Ti-TA exhibits excellent chlorine and water resistance at 300℃ (5 %H 2 O, 500 ppm CB), and has a higher potential of application.
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ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Yang Zeng,Lan Jiang,Xiaoxin Zhang,Songhai Xie,Yan Pei,Gongbing Zhou,Weiming Hua,Minghua Qiao,Zhen-Hua Li,Baoning Zong
Catalytic hydrogenolysis of biomass-derived glycerol to 1,3-propanediol (1,3-PDO) represents an important process for the sustainable production of value-added chemicals. However, there is a dearth of understanding of the effect of the polymorph of the support on this reaction. Herein, two Pt–WOx/TiO2 catalysts supported on rutile TiO2 (r-TiO2) and anatase TiO2 (a-TiO2) polymorphs were prepared to investigate the crystal phase effect of TiO2 on the structural property and catalytic performance in glycerol hydrogenolysis. The TiO2 polymorph was identified to impose profound effects on the size of the Pt nanoparticles (NPs) and the dispersion and location of the WOx species, which originated from the discrepancies in the crystal structures between the PtO2 and the TiO2 polymorphs and the discrepancies in the interactions of WOx with different TiO2 polymorphs. In glycerol hydrogenolysis, the Pt–WOx/r-TiO2 catalyst gave a 1,3-PDO selectivity of 51.2% at a glycerol conversion to liquid products of 74.5%, yielding 38.1% of 1,3-PDO. In contrast, the Pt–WOx/a-TiO2 catalyst showed much inferior glycerol conversion and 1,3-PDO selectivity, yielding only 1.0% of 1,3-PDO under identical reaction conditions. The superior catalytic performance of the Pt–WOx/r-TiO2 catalyst is attributed to the r-TiO2 polymorph that facilitates a faster hydrogen spillover than the a-TiO2 polymorph from the Pt NPs to the reaction intermediate on the WOx species, which is substantiated by an even higher 1,3-PDO yield of 44.8% over the physically mixed Pt/r-TiO2 + WOx/r-TiO2 catalyst. This work demonstrates the critical role of the polymorph of the TiO2 support in the design of efficacious Pt–WOx-based catalysts for glycerol hydrogenolysis to 1,3-PDO.
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Nanoscale
·
2021
·Vol. 13
·期 43
·18273-18280
·
IF 7.79
Zhuofan Gan,Chengyong Shu,Chengwei Deng,Wei Du,Bo Huang,Wei Tang
Electrochemical water splitting is a promising method to generate pollution-free and sustainable hydrogen energy. However, the specific activity and durability of noble metal catalysts is the main hindrance to the hydrogen evolution reaction. Based on the continuous pore regulation of hollow porous carbon spheres (N-HPCSs) by hexadecyl trimethyl ammonium bromide, the 6.21 wt% Pt/N-HPCSs exhibited good dispersibility, according to a low overpotential of 45 mV (10 mA cm−2/1 M KOH). Its mass activity was 4 times that of the commercial 20 wt% Pt/C at −0.07 V (vs. RHE) potential. We analyse that the excellent activity is due to the interaction between Pt nanoparticles and N-HPCSs so that the electron density around the Pt atoms increases, which is beneficial for H2O to obtain electrons and transform into Had. Meanwhile the sea urchin-like structure of N-HPCSs facilitates the desorption of H2. Furthermore, the overpotential showed no obvious decrease in the long-term durability test, which should be attributed to the confinement of Pt nanoparticles by the well-defined pores in N-HPCSs to avoid the aggregation of Pt nanoparticles during long-term testing.
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高影响因子
FUEL
·
2025
·
IF 7.5
Chen-Xu Chen,Jing-Pei Cao,Nai-Yu Yao,Wen Tang,Wei Jiang,Chuang Zhang,Xiao-Yan Zhao,Xiao-Yu Qiao,Tungalagtamir Bold
Improving the catalytic efficiency and catalyst life of Pt/Al 2 O 3 catalyst for methylcyclohexane dehydrogenation is of great significance for the study of organic liquid hydrogen storage. In this work, the promotion effects of Ga and Ce on the substantial improvement of catalytic stability and activity over the Pt / Al 2 O 3 during the methylcyclohexane dehydrogenation were investigated. The catalyst with optimizing Ga and Ce loading (1.5 wt%) exhibits ∼99.76 % selectivity and H 2 evolution rate of 2102 mol/g Pt /min at 300 °C. In 100 h long-time reaction, the conversion of methylcyclohexane remains around 75 % with no significant decrease. The characterization results show that introducing proper amount of Ga and Ce helps Ga 3+ cations incorporate into the lattice structure of CeO 2 that increase concentration of oxygen vacancies and CeO 2 reducibility in the catalyst, which boost the capability of methylcyclohexane dehydrogenation and tolerance for coke formation. Thus, the excellent stability and activity are achieved over the GaCe-modified catalyst. This study may share new light on the rational construction of highly efficient Pt-based catalysts for methylcyclohexane dehydrogenation.
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MICROCHIMICA ACTA
·
2018
·Vol. 185
·期 9
·1-10
·
IF 5.705
Sun Ying,Wang Ruixue,Liu Xuan,Shan Guiye,Chen Yanwei,Tong Ti,Liu Yichun
Platinum nanoparticles (PtNPs) were uniformly grown on the surface of gold nanorods (AuNRs) by a laser irradiation procedure. Transmission electron microscopy confirmed that the PtNPs are uniformly grown on the surface of the AuNRs. The formation of PtNPs on the AuNRs leads to a red-shift of the absorption maximum from 734 nm to 766 nm. In addition, the efficiency of surface enhanced Raman scattering (SERS) is increased, but the photothermal conversion efficiency is decreased compared to pure AuNRs. The result indicates that electron transfer occurs between gold and platinum. The peroxidase mimicking effect of PtNPs, AuNRs and Au/Pt NRs by catalyzing the oxidation of colorless 3,3’,5,5’-tetramethylbenzidine (TMB) to blue oxidized 3,3’,5,5’-tetramethylbenzidine (oxTMB; a quinone) in the presence of H 2 O 2 . The catalytic activity of Au/Pt NRs is higher than that of sole AuNRs or PtNPs by factors of 4.2 and 2.1, respectively. Thus, Au/Pt NRs have been used for the detection of peroxide and the limit of detection is 0.04 μM. This work provides an approach to integrate the peroxidase mimicking effect with SERS enhancement for potential application in detection.
A schematic diagram for the laser-induced growth of Au/Pt NRs and the colorimetric determination of hydrogen peroxide concentration with their peroxidase mimicking properties. The limit of detection is 0.04 μM based on the use of Au/Pt NRs as a catalyst.
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Nanomaterials
·
2022
·Vol. 12
·期 21
·3771
·
IF 5.719
Shizhuo Wang,Jikang Jiang,Minyan Gu,Yuanbo Song,Jiang Zhao,Zheng Shen,Xuefei Zhou,Yalei Zhang
To substitute fossil resources, it is necessary to investigate the conversion of biomass into 1,2-propanediol (1,2-PDO) as a high-value-added chemical. The Pt/deAl-Beta@Mg(OH)2catalytic system is designed to obtain a higher 1,2-PDO production yield. The optimal yield of 1,2-PDO is 34.1%. The unique shell-core structure of the catalyst demonstrates stability, with a catalytic yield of over 30% after three times of use. The primary process path from glucose to 1,2-PDO, glucose-hexitol-1,2-PDO, is speculated by the experiments of intermediate product selectivity. The alkaline catalytic mechanism of the reaction process is elucidated by studying catalyst characterization and analyzing different time courses of products. The introduction of Mg(OH)2improves the target yield by promoting the isomerization from glucose to fructose and retro-aldol condensation (RAC) conversion, with pseudo-yield increases of 76.1% and 42.1%, respectively. By studying the processes of producing lactic acid and 1,2-PDO from glucose, the glucose hydrogenolysis flow chart is improved, which is of great significance for accurately controlling 1,2-PDO production in industrial applications. The metal, acid, and alkali synergistic catalytic system constructed in this paper can provide a theoretical basis and route reference for applying biomass conversion technology in practice.Keywords:1,2-propanediol;alkaline modification;core–shell catalyst
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ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Guohua Zhu,Kui Wu,Liang Tan,Weiyan Wang,Yanping Huang,Diyu Liu,Yunquan Yang
Magnetic colloidal sol was first prepared and added in the mixed solution of Ni(NO3)2 and Al(NO3)3. After the constant-pH coprecipitation and calcination, magnetic NiO–Al2O3@Fe3O4 mixed oxides were formed and used as supports for Pt-based catalysts. The activities of these magnetic Pt/NiO–Al2O3@Fe3O4 catalysts were tested in the hydrodeoxygenation (HDO) of phenols such as 4-ethylphenol, 4-methylphenol, and guaiacol. These exhibited high HDO activity, and aromatic hydrocarbons were produced through a coupling process of hydrodeoxygenation and dehydrogenation. The addition of Fe enhanced both the conversion and aromatic hydrocarbons selectivity, which was attributed to the electron transfer between metallic Pt and Fe. For example, after the liquid phase HDO of 4-ethylphenol at 300 °C and 2.0 MPa for 1.5 h, 97.9% conversion and 18.3% toluene selectivity were obtained. When the reaction time was prolonged to 8 h, ethylbenzene selectivity increased to 88.0%. Moreover, these Pt/NiO–Al2O3@Fe3O4 catalysts were easily recycled from the liquid reaction mixture by employing an external magnet, but the dehydrogenation stability needs to be further improved.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Xunfu Zhou,Shiying Song,Xiaoxing Yu,Zhongda Wu,Zhanhao Xiao,Zuofang Yao,Xiaoqin Zhou,Jin Luo,Xuliang Fan,Xiaosong Zhou
Polymer carbon nitride (g-C 3 N 4 ) demonstrates a thermodynamically favorable profile for photocatalytic overall water splitting. Nonetheless, the practical catalytic performance is limited by slow reaction kinetics, mainly because of the inadequate quantity of surface redox-active sites. It is evident that pristine g-C 3 N 4 shows minimal activity in the photocatalytic process of overall water splitting. Herein, we developed a strategy for achieving pure water splitting using photoexcited g-C 3 N 4 with MnOOH and Pt serving as redox cocatalysts. The innovation of this work is based on the deposition of Mn 2 N 0.86 /Mn 4 N onto g-C 3 N 4 as a precursor material. This precursor undergoes in-situ hydrolysis to form Mn(OH) 2 and in-situ photo-oxidation to generate MnOOH, which acts as an oxygen evolution cocatalyst by capturing photogenerated holes and facilitating the oxygen evolution reaction. Concurrently, H 2 PtCl 6 is employed as a precursor and undergoes in-situ photo-reduction to form Pt nanoparticles, which serve as a hydrogen evolution cocatalyst by capturing electrons and promoting the hydrogen evolution reaction. With the synergistic effect of these dual cocatalysts, efficient photocatalytic water splitting was achieved, yielding hydrogen (11.64 μmol h −1 ) and oxygen (5.47 μmol h −1 ) in a nearly 2:1 stoichiometric ratio under light irradiation.
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Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 27
·13694-13701
·
IF 11.301
Wei Wang,Xiaoling Hong,Qilu Yao,Zhang-Hui Lu
In this work, mesoporous N-doped carbon (MNC) materials have been successfully prepared by a nanocasting route using SBA-15 as the template and ethylenediamine (EDA) and carbon tetrachloride (CTC) as carbon nitride precursors. The specific surface area and pore size of the MNC, as well as the C/N content are strongly dependent on the pyrolysis temperature. The as-obtained MNC-supported NiPt nanoparticles (NPs) were used as efficient catalysts toward complete dehydrogenation of hydrazine borane (HB) in alkaline solution at room temperature. Among all the catalysts investigated, the Ni60Pt40/MNC-800 nanocomposites (NCs) show the highest catalytic activity and 100% hydrogen selectivity. The total turnover frequency (TOF) of Ni60Pt40/MNC-800 NCs reached 1111 h−1 at room temperature, the highest activity among all catalysts reported to date. The superior catalytic properties were possibly a result of the electronic interaction between Ni and Pt, the synergistic effects of the NiPt NPs and MNC support, the ordered pore structure for free mass transfer and the small-sized metal NPs.
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CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Yijun Xue,Wei Sun,Qian Wang,Limei Cao,Ji Yang
MOFs (metal-organic frameworks) are stable materials with both organic and inorganic pores, and possess high surface area fascinating structures. Owing to the unique octahedral of aluminum center and strong Al–O bonds, Al-based MOFs show excellent thermal stability. In this paper, MIL-96(Al) is proved to be effective at dispersing Pt particles evenly and sparsely as it is employed as catalyst support. MIL-96(Al) is synthesized via a water based route and different contents of Pt particles are directly deposited on the surface of MIL-96 in one step by hydrothermal method to prepare Pt X MIL-96 (x represents Pt content) catalysts. The catalyst are sprayed evenly on carbon paper, with Pt content of 0.03%, 0.11%, 0.27% and 0.41%, respectively, and are applied in a gas diffusion reactor with snakelike flow field for low temperature H 2 -SCR. For Pt 5 MIL-96/CP, the NO removal efficiency can reach up to 100% at 60 °C. Electron transfer between Pt and MIL-96 is observed via X-ray photoelectron spectron (XPS). It reveals that the deposited Pt is in metallic state. Meanwhile, the electronic structure of MIL-96 is kept intact in the process of Pt depositing. The excellent performance of Pt 5 MIL-96/CP catalyst strongly suggests its potential application.
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Molecular Catalysis
·
2024
·
IF 3.9
Meng Xu,Xiaoling Liu,Zhuo Xiong,Yue Wu,Zhen Meng,Yu Zhou,Jun Wang
Furfural is an abundant biomass-derived building block that can be converted into furan-based N-containing compounds through direct reductive amination by using dihydrogen (H 2 ). Nonetheless, the synthesis of furan-based tertiary amines is highly limited via this route. Herein, we reported the straightforward synthesis of MFI zeolite encapsulated Pt nanoparticles and finely modulated the surface electronic state by facilely controlling the reduction process. The constructed catalyst Pt@Z5 effectively catalyzed the amination of furfural with diethylamine for the synthesis of N-ethyl-N-(furan-2-ylmethyl)ethanamine, affording the high yield (>95 %), large turnover number (TON) of 2058, turnover frequency (TOF) of 1029 h −1 , and stable recyclability. Systematic investigations comprising in-situ Fourier transform infrared spectroscopy (FTIR) spectra and kinetic isotope effect (KIE) unraveled that the mild reduction condition allowed the catalyst with a superior affinity towards H atom and beneficial furfural adsorption behavior, accelerating the H 2 activation in the rate-determining step for the conversion of furfural into furan-based amine.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Shan Hu,Panzhe Qiao,Xinming Liang,Guiming Ba,Xiaolong Zu,Huilin Hu,Jinhua Ye,Defa Wang
Photoreduction of CO 2 and H 2 O into fuels and value-added chemicals is a promising green technology for solar-to-chemical conversion. However, improving the conversion efficiency with regulated product selectivity is a big challenge due to the sluggish dynamic transfer and insufficient active sites. Herein, we report on Pt single atoms anchored porous C 3 N 4 nanosheet photocatalyst (Pt 1 @CN) with Pt–N 4 coordination for stable and efficient CO 2 photoreduction using H 2 O as reductant. The Pt 1 @CN exhibits an evolution rate of 84.8 μmol g −1 h −1 with nearly 100% CO selectivity, outperforming most previous C 3 N 4 -based single-atom photocatalysts. Experimental and DFT calculation results reveal that the Pt–N 4 coordinated active sites promote the photogenerated electron transfer, CO 2 adsorption/activation, *COOH generation, and *CO desorption, thus accounting for the significantly improved CO 2 photoreduction activity with ∼100% CO selectivity. This study provides a deep insight into the significant roles of single-atom active sites in enhancing the CO 2 photoreduction activity and regulating the product selectivity.
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