ChemSusChem
·
2024
·
IF 7.5
Yanan Wei,Jianming Pan,Xu Yan,Yanli Mao,Yunlei Zhang
Graphical The AuPd/CeO 2 catalyst was employed for the oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA), showing that high oxygen vacancy of CeO 2 and electron-rich state of interfacial Au−Pd−CeO 2 can strengthen the adsorption and activation of HMF and molecular oxygen, greatly promoting the elimination of β -hydride for the conversion of HMF to FDCA. The design of high activity catalyst for the efficiently conversion of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) gains great interest. The rationally tailoring of electronic structure directly affects the interaction between catalysts and organic substrates, especially molecular oxygen as the oxidant. This work, the bimetallic catalysts AuPd/CeO 2 were prepared by the combining method of chemical reduction and photo-deposition, effectively concerting charge between Au and Pd and forming the electron-rich state of Au. The increasing of oxygen vacancy concentration of CeO 2 by acidic treatment can facilitate the adsorption of HMF for catalysts and enhance the yield of FDCA (99.0 %). Moreover, a series of experiment results combining with density functional theory calculation illustrated that the oxidation performance of catalyst in HMF conversion was strongly related to the electronic state of interfacial Au−Pd−CeO 2 . Furthermore, the electron-rich state sites strengthen the adsorption and activation of molecular oxygen, greatly promoting the elimination of β -hydride for the selective oxidation of 5-hydroxymethyl-2-furancarboxylic acid (HMFCA) to FDCA, accompanied with an outgoing FDCA formation rate of 13.21 mmol ⋅ g −1 ⋅ min −1 at 80 °C. The perception exhibited in this research could be benefit to understanding the effects of electronic state for interfacial sites and designing excellent catalysts for the oxidation of HMF.
研究领域:
催化化学
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材料科学
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理论计算化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2018
·
IF 6.434
Guangjun Zhai,Jinguo Wang,Zimei Chen,Shuaifeng Yang,Yong Men
Three-dimensionally ordered macroporous (3DOM) Co 3 O 4 -CeO 2 catalysts with controllable Co/Ce molar ratios synthesized by colloidal crystal template method were developed to catalyze the NO x -assisted soot oxidation for the first time, and the obtained 3DOM Co 3 O 4 -CeO 2 catalysts exhibited highly enhanced soot oxidation activity. Detailed characterizations of 3DOM Co 3 O 4 -CeO 2 catalysts revealed that the highly enhanced soot oxidation activity was originated from the synergistic promoting effect by combining the macroporous effect resulted from the unique 3DOM framework, the chemical nature associated with more Co 3+ reactive sites, the surface enrichment of Ce species and the improved redox properties. Meanwhile, the high NO x storage and oxidation capacity resulted from the integrated respective merits of Co 3 O 4 and CeO 2 also accounted for the enhanced soot oxidation activity via NO x -assisted mechanism. Furthermore, the 3DOM Co 3 O 4 -CeO 2 catalysts demonstrated strong stability because of the surface enrichment of Ce species improving the thermal stability and the robust 3DOM framework inhibiting the structural collapse, showing their potential applications under practical conditions.
研究领域:
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
WATER ENVIRONMENT RESEARCH
·
2021
·Vol. 93
·期 12
·2903-2913
·
IF 1.946
Pan Xiong,Siqi Fan,Jinshan Song,Qizhou Dai
In this study, a magnetic nanocatalyst (Fe 3 O 4 @SiO 2 @CeO 2 ) was prepared and applied in the catalytic ozonation of methyldopa (MD). The effects of operational parameters on catalytic ozonation performance were investigated, including ozone dosage, catalyst dosage, initial MD concentration, and pH. The removal of MD was 45.2% in ozonation, whereas the efficiency was achieved to 83.0% with the addition of Fe 3 O 4 @SiO 2 @CeO 2 . The results showed that Fe 3 O 4 @SiO 2 @CeO 2 could significantly improve the catalytic ozonation performance. And the enhanced mechanism study showed that it was attributed to promotion of ozone decomposition to generate hydroxyl radical. The reaction model was explored, and the reaction rates were calculated for the MD degradation in catalytic ozonation. A higher degradation efficiency of MD in catalytic ozonation was attributed to the enhanced surface effect of the catalysts, which was confirmed by using TBA, PO 4 3− , and p -BQ as scavengers of hydroxyl radical, surface reaction, and superoxide radical. The hydroxyl radical and superoxide radical played an important role in the degradation of MD. The mechanism of catalytic ozonation by Fe 3 O 4 @SiO 2 @CeO 2 was discussed via X-ray photoelectron spectroscopy (XPS) spectra and experimental data. Practitioner Points Fe 3 O 4 @SiO 2 @CeO 2 could promote the decomposition of ozone to produce hydroxyl radicals. High degradation efficiency of methyldopa with Fe 3 O 4 @SiO 2 @CeO 2 was achieved. A mechanism of catalytic ozonation with Fe 3 O 4 @SiO 2 @CeO 2 was proposed.
研究领域:
环境科学
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化学工程
·
药学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Jie Fan,Yuhang Sun,Mingli Fu,Jiaqi Li,Daiqi Ye
Metal support interactions modulation is one of the effective strategies to enhance the catalytic performance. Herein, we reported that modulating metal support interactions by switching the strength (CO, H 2 , NH 3 ) and temperature (200, 300, 400 °C) of reducing gases is a facile way to improve the catalytic performance of Pt/CeO 2 for toluene oxidation . The distinct reduction treatments will stepwise enhance the reducibility, ratio of Pt 0 and oxygen vacancy concentration, which dominated the activity. The metal support interactions modulation can significantly affect toluene deep oxidation (from benzoate to formate or monodentate carbonate) via enhancing the mobility of surface/lattice oxygen and activation ability towards O 2 molecules, since the main activation sites for O 2 molecules expand from Pt 0 sites to oxygen vacancies and Pt 0 sites with temperature increasing.
研究领域:
催化化学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2017
·
IF 9.446
Hui He,Xueting Lin,Shujun Li,Zeng Wu,Jingheng Gao,Junliang Wu,William Wen,Daiqi Ye,Mingli Fu
Surface species and oxygen vacancies were studied in MnO x (0.4)-CeO 2 toward repeated soot oxidation. MnO x (0.4)-CeO 2 catalysts prepared by the citric acid complex method were repeatedly used in a 10% O 2 /Ar gas flow and showed favorable activity and satisfactory durability toward soot oxidation. X-ray diffraction (XRD), N 2 adsorption/desorption, Electron paramagnetic resonance (EPR), X-ray photoelectron spectroscopy (XPS) and in situ visible/UV Raman characterization methods were utilized to investigate the structural features of fresh and reused catalysts. The irreversible conversion of high valence manganese species as well as the reduction of Frenkel-type oxygen vacancies and lattice oxygen could be clearly observed in the reused samples, which were associated with the slight deactivation. Spectators and participators were two existing forms of Frenkel-type oxygen vacancies. It was noteworthy that the participators almost fully regenerated after each reaction cycle, which ensured the ability to activate O latt in repeated soot oxidation process. Therefore, the catalysts maintained favorable activity and satisfactory durability, which was mainly because the relatively stable level of participators.
研究领域:
催化化学
·
环境催化
·
材料化学
·
表面科学
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能源化学
✓ 已验证
DOI
高影响因子
JOURNAL OF RARE EARTHS
·
2025
·
IF 7.2
Chao Peng,Guoqing Yang,Hanqing Ge,Zhongwen Liu
The oxidative dehydrogenation of propane with carbon dioxide (CO 2 -ODP) has received significant attention as an environmentally benign route for the propene production. However, the development of high-performance catalysts remains a critical challenge hindering its industrial implementation. In this work, CeO 2 samples with distinct morphologies resembling flowers (F-CeO 2 ), rods (R-CeO 2 ), spindles (SP-CeO 2 ), and sheets (SH-CeO 2 ) were successfully synthesized by simply changing the hydrothermal conditions, and the shape-dependent impact of oxygen-defect contents over CeO 2 on the structural and electronic properties of the impregnated PtSn/CeO 2 catalysts was studied for CO 2 -ODP. Characterizations reveal a positive correlation between the Pt electron density and oxygen-defect contents in an increasing order of PtSn/F-CeO 2 < PtSn/R-CeO 2 < PtSn/SP-CeO 2 < PtSn/SH-CeO 2 . In the case of the catalytic results, the same changing pattern is observed for the initial C 3 H 8 conversion and C 3 H 6 selectivity. Moreover, the highest initial propene space-time yield of 0.71 achieving over the PtSn/SH-CeO 2 catalyst is still retained at 0.35 after a time on stream of 200 min. This performance surpasses those of most reported CO 2 -ODP catalysts. The morphology-dependent catalytic phenomena are attributed mainly to the varied activation energies of CO 2 -ODP, which are determined by the oxygen defect-induced electronic and structural interplay between Pt, Sn, and CeO 2 . These findings provide valuable insights for the rational design and optimization of Pt-based catalysts for CO 2 -ODP, particularly in the selection of oxide supports.
研究领域:
催化化学
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材料科学
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化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xing Yi,Yan Wang,Zongpeng Zou,Yuan He,Li Lv,Wenxiang Tang,Tao Zhang,Shengwei Tang
The microreactor coupled mini-channel microdroplets extraction and separation technology (MES) was developed by adding polyvinyl alcohol (PVA) into microdroplets, realizing the controllable synthesis of a series of mono-component and multi-component metal oxide nano particles (MONPs). A double-layer surfactant structure composed of Span20 (oil phase surfactant) and PVA (water phase surfactant) was designed as a barrier to intercept and collect the precipitated salt at the microdroplet interface, the addition of PVA reduces the loss of salt components during the extraction process from 41.7 wt% to 1.1 wt%. The size control of mono-component MONPs (CuO, Co 3 O 4 , and NiO) was achieved using MES method. Furthermore, in the application direction of preparing multi-component MONPs, the advantages of MES in preparing multi-component catalysts (Ni/CeO 2 ) were verified. TEM, XRD, H 2 -TPR, CO 2 -TPD, XPS, BET et al. characterizations have shown that Ni entered the lattice of CeO 2 during precipitation to form a Ni-O-Ce solid solution and was therefore highly dispersed in CeO 2 . Ni/CeO 2 -MES showed high CO 2 conversion and CO selectivity in reverse water gas shift (RWGS) testing compared to Ni/CeO 2 catalysts prepared by impregnation method which has excellent thermal stability and can maintain over 99 % CO selectivity even after 50 h of reaction at 600 °C. The MES method was proved to be an efficient synthesis technology for MONPs and can be extended to a variety of metal oxides catalysts.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2022
·
IF 12.92
Anxiang Guan,Yueli Quan,Yangshen Chen,Zhengzheng Liu,Junbo Zhang,Miao Kan,Quan Zhang,Haoliang Huang,Linping Qian,Linjuan Zhang,Gengfeng Zheng
The electrocarboxylation reaction is an attractive means to convert CO 2 into valuable chemicals under ambient conditions, while it still suffers from low efficiency due to the high stability of CO 2 . In this work, we report a double activation strategy for simultaneously activating CO 2 and acetophenone by silver-doped CeO 2 (Ag-CeO 2 ) nanowires, featuring as an effective electrocatalyst for electrocarboxylation of acetophenone with CO 2 . Compared to the Ag foil, Ag nanoparticles and CeO 2 nanowires, the Ag-CeO 2 nanowire catalyst allowed to reduce the onset potential difference between CO 2 and acetophenone activation, thus enabling efficient electrocarboxylation to form 2-phenyllactic acid. The Faradaic efficiency for producing 2-phenyllactic acid reached 91% at −1.8 V versus Ag/AgI. This double activation strategy of activating both CO 2 and organic substrate molecules can benefit the catalyst design to improve activities and selectivities in upgrading CO 2 fixation for higher-value electrocarboxylation.
研究领域:
化学
·
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
ACS Catalysis
·
2020
·
IF 12.35
Qingsong Zhang,Jiahao Bu,Jiandian Wang,Changyong Sun,Dongyang Zhao,Guangzhe Sheng,Xiaowei Xie,Ming Sun,Lin Yu
Pt/CeO2 catalysts with different support shapes and prereduction temperatures were prepared and tested in the liquid-phase hydrogenation of nitrobenzene. Detailed characterizations reveal that the support shape effect of Pt/CeO2 catalysts on nitrobenzene hydrogenation originates from the exposed crystal planes on CeO2 with different reducibilities. A high-energy surface is readily reduced to generate more Ce3+ surface sites and oxygen vacancies, not only favoring the dispersion and stabilization of Pt species due to stronger metal–support interaction but also providing more adsorption sites for reactants and intermediates. Reduction treatment at high temperatures has been proved to be an effective way to improve the performance of Pt/CeO2 catalysts by providing additional Ce3+ surface sites and high H-spillover capability. The additional Ce3+ far away from Pt, derived from a high-temperature reduction, can adsorb the N-phenylhydroxylamine intermediate more effectively due to its stronger electron-donating ability and in turn promote aniline formation. It is also found that Na ions with suitable content facilitate the generation and stabilization of surface Ce3+ by charge transfer and help Pt particles to maintain a smaller size. Consequently, a 0.25 wt % Pt catalyst, supported on Na-containing CeO2 nanorods and reduced at 600 °C, displays a high level of aniline productivity of 40.8 molAN/gPt/h and excellent stability in nitrobenzene hydrogenation at room temperature. A pathway of nitrobenzene hydrogenation catalyzed by Pt/CeO2 is also proposed.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Tuya Naren,Guojuan Jing,Lei Xue,Qi Wang,Yuansong Zhao,Caixia Li,Suhong Lu,Jinfang Wu,Shanghong Zeng
The development of superior catalysts for preferential oxidation of CO has always maintained challenging in heterogeneous catalysis . Herein it is found that the Pt 0.05 /CuO–CeO 2 catalyst exhibited high activity and selectivity for preferential oxidation of CO at working temperature of proton-exchange membrane fuel cells (~80 °C). The studies indicate that the presence of platinum and cerium promote the generation of oxygen vacancy and the dissociation of O 2 molecules. Meanwhile, the introduction of platinum facilitates the reduction of copper and cerium species as well as enhances the quantity of lattice oxygen. The timely update of lattice oxygen promotes CO oxidation with the help of oxygen vacancy. The finding may provide new ideas for developing the excellent ternary catalyst for preferential oxidation of CO at the proton-exchange membrane fuel cells working temperature.
研究领域:
催化
·
材料科学
·
燃料电池技术
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Hao Liu,Shan Yang,Jinxing Mi,Chuanzhi Sun,Jianjun Chen,Junhua Li
N2O and CO coexist in various industrial and mobile sources. The synergistic reaction of N2O and CO to generate N2 and CO2 has garnered significant research interest, but it remains extremely challenging. Herein, we constructed an atomically dispersed Rh-supported CeO2 catalyst with asymmetric Rh–O–Ce sites through gradient Rh 4d–O 2p–Ce 4f orbital coupling. This design effectively regulates the 4f electron states of Ce and promotes the electron filling of the O 3π* antibonding orbital to facilitate N–O bond cleavage. Near-ambient-pressure X-ray photoelectron spectroscopy (NAP-XPS) reveals that CO reacts with the surface-adsorbed O* generated by N2O decomposition through self-tandem catalysis, accelerating the rate-limiting step in N2O decomposition and activating the synergistic reaction of N2O and CO at temperatures as low as 115 °C. This work can guide the development of high-performance catalysts using the strategy of high-order orbital hybridization combined with the tandem concept to achieve versatile catalytic applications.
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RENEWABLE ENERGY
·
2021
·
IF 8.001
Shanshan Shao,Chengyue Liu,Xianliang Xiang,Xiaohua Li,Huiyan Zhang,Rui Xiao,Yixi Cai
Catalytic conversion of pyrolysis vapor from biomass was performed over CeO 2 catalysts to produce ketones. Thermogravimetric-gas chromatography/mass spectrometry (TG-GC/MS) and TG-MS were applied to understand the distribution of pyrolysis vapors from various biomass including rape straw, poplar, cypress and bagasse. The favorable biomass feedstock with high yield of ketones and other useful components were screened out for directional ketonization. The results showed that the temperature range of biomass pyrolysis was generally below 400 °C, and bagasse was a reasonable raw material for ketonization with the highest yield of ketones of 33.68% at 380 °C, since it contained the most cellulose and hemicellulose in biomass of the same quality. The activity of acetone increased at higher temperature, and secondary reaction occurred, resulting in a reduction in the overall yield of ketones. The total yield of ketones from bagasse treated for 9 h was boosted by 16.18% higher than that from nonseawater-treated biomass. By the introduction of metal ions effectively, the component of the pyrolysis vapor changed, making it easier for large molecular substances to be converted to small ones during pyrolysis. Through this research, the effective utilization of biomass could be realized.
研究领域:
能源与环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）