Chemistry-An Asian Journal
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2022
·Vol. 18
·期 1
·e202200947
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IF 4.839
Zheng Zeng,Ma Juan Guan,Hongyu Chen,Xiang Xu,Ma Jianwu Zou,Ma Chongjie Zhang,Yankun Du,Liqing Li
Graphical As shown in the following figure, for PtFe 3 −C, toluene was directly adsorbed on the surface oxygen position and finally converted into H 2 O and CO 2 . For PtFe 3 −CeO 2 , two reaction channels containing both lattice oxygen (blue ball) from CeO 2 and surface oxygen (pink ball) and result in a better toluene catalytic performance than PtFe 3 −C. Elimination of VOCs by catalytic oxidation is an important technology. Here, a general synergistic capture-bonding superassembly strategy was proposed to obtain the nanoscale dispersed 5.8% PtFe 3 −CeO 2 catalyst, which showed a high toluene oxidation activity (T 100 =226 °C), excellent catalytic stability (125 h, >99.5%) and a good water resistance ability (70 h, >99.5%). Through the detailed XPS analysis, oxygen cycle experiment, hydrogen reduction experiment, and in-situ DRIFT experiment, we could deduce that PtFe 3 −CeO 2 had two reaction pathways. The surface adsorbed oxygen resulting from PtFe 3 nanoparticles played a dominant role, due to the fast cycling between the surface adsorbed oxygen and oxygen vacancy. In contrast, the lattice oxygen resulting from CeO 2 nanorods played an important role due to the relationship between the toluene oxidation activity and the metal-oxygen bonding energy. Furthermore, DFT simulation verified Pt sites were the dominant reaction active sites during this reaction.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED ENERGY
·
2023
·
IF 11.2
Xiangyu Yan,Buchu Lu,Hao Dong,Qibin Liu
Combining solar light and heat in dry reforming of methane (DRM) is a promising technology for reducing CO 2 to a valuable syngas and increasing the utilization of solar light in the solar-to-fuel process. The reaction temperature is still high and the mechanism remains unclear in DRM. Clarifying the synergistic mechanism of solar light and heat is pivotal for industrial applications. To this end, a nanoscale Ni/CeO 2 catalyst is prepared, and the synergistic effect of solar light and heat in DRM is experimentally investigated. The experimental results show that photo-thermochemistry leads to a 39.74% increase in relative conversion rate of CH 4 compared to thermochemistry, while the reaction temperature is reduced by 45 °C. The syngas production rate and the selectivity of DRM are improved by solar light. The in-situ infrared study indicates that solar light enhances the dissociation process of CH 4 and the production of HCOO ⁎ on the surface of the Ni/CeO 2 catalyst. The light response in the catalyst and microscopic enhancement of intermediate products are responsible for the increased DRM performance under photo-thermochemical conditions. These findings contribute to the understanding of the synergistic effects of solar light and heat, and guide the conversion of CO 2 into fuel with the aid of solar energy.
研究领域:
化学工程
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可再生能源
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Dong Liu,Feiyang Hu,Yue Yan,Runping Ye,Xiaohan Chen,Bingying Han,Zhang-Hui Lu,Li Zhou,Gang Feng,Rongbin Zhang
CO oxidation is the primary approach for eliminating CO from incomplete combustion, and the catalytic performance is dependent on the structure of catalysts. Herein, to explore the structure promotion in the CO oxidation reaction, polymethyl methacrylate was synthesized as the hard template to fabricate the three-dimensional ordered microporous (3DOM) Au/CeO 2 and compared the catalytic performance with the Au/CeO 2 rod catalyst. The 3DOM Au/CeO 2 catalyst could realize complete CO oxidation at 90 °C while 110 °C for Au/CeO 2 rod catalyst. The 3DOM Au/CeO 2 catalyst also showed outstanding stability for 60 h reaction. The achieved high performance could be attributed to the pore structures and the better metal-support interaction that facilitates abundant oxygen vacancies . Additionally, the Au distribution and oxygen vacancies promoted by the macropores structures were discovered using a series of characterizations. This work highlights the promotion of oxygen vacancies and metal-support interaction by 3DOM structure in CO oxidation reaction.
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
SOLID STATE SCIENCES
·
2019
·
IF 2.155
Wei Li,Pengcheng Liu,Ruyue Niu,Jinping Li,Shuang Wang
Three CeO 2 supports with different concentration of surface oxygen vacancies were prepared by using C 12 H 29 NO (TPAOH), C 2 H 8 N 2 (EDA) and NaOH as precipitant under hydrothermal conditions, respectively. Catalytic experiments showed that the Ru/CeO 2 -TPAOH catalyst has superior catalytic activity (22000 μmol g −1 h −1 ) than Ru/CeO 2 -EDA (19000 μmol g −1 h −1 ) and Ru/CeO 2 –NaOH (16500 μmol g −1 h −1 ) at 450 °C, 3 MPa. In addition, the introduction of Cs and Ba promoters improve the catalytic activity of the Ru/CeO 2 -TPAOH. However, the introduction of K promoter inhibits the catalytic activity of the Ru/CeO 2 -TPAOH. The 4% Cs promoter can effectively increase the catalytic activity of the Ru/CeO 2 -TPAOH (32000 μmol g −1 h −1 ). BET and TEM indicated that 5.5 nm average pore size of CeO 2 -TPAOH support contributes to the dispersion of active metal Ru. XPS and CO 2 -TPD proved that the Ru/CeO 2 -TPAOH catalyst has higher Ce 3+ concentration, more oxygen vacancies, and higher basic site density, which are important factors for improving ammonia synthesis activity.
研究领域:
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF CATALYSIS
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2021
·
IF 7.92
Pingping Xie,Xin Yong,Yongdan Li,Shetian Liu,Cuijuan Zhang
The 5%BaCoO 3 -CeO 2 catalysts show excellent catalytic performance for NO direct decomposition; however, the reasons for the high activity remain to be explored. Here, the catalyst was prepared by different methods (citric acid–nitrate one-pot method, impregnation method and mechanical mixing method), aiming to reveal the factors determining the catalytic activity. The results show that the one-pot derived materials display superior activity and oxygen resistance, which is stemmed from the smaller grains and uniform distribution of components, higher surface area, larger interface, better redox activity, faster oxygen desorption kinetics and better NO sorption capability. The catalytic mechanism was discussed based on the diffuse reflectance infrared Fourier transform spectroscopy and kinetic study . This work demonstrates that the one-pot method is promising to synthesize high performance heterogeneous catalysts and the derived 5%BaCoO 3 -CeO 2 is a competitive candidate for NO direct decomposition.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 9
·3241-3250
·
IF 6.119
Ming Jiang,Xiaopeng Chen,Linlin Wang,Jiezhen Liang,Xiaojie Wei
Selective hydrogenolysis of aryl ethers to produce aromatic compounds is a key strategy for lignin valorization. The use of non-noble-metal catalysts to realize the cleavage of C–O ether bonds under mild conditions has been of considerable research interest recently. We herein report the synthesis of a nitrogen-doped porous-carbon-skeleton-supported Ni–CeO2 catalyst (Ni–CeO2/CN). The synergistic effect between Ni and CeO2 species led to the Ni–CeO2/CN catalyst having a high activity and selectivity for the cleavage of C–O ether bonds at a low reaction temperature. In particular, the Ni–CeO2/CN catalyst showed excellent effectiveness in the hydrogenolysis of benzyl phenyl ether (α-O-4 bonds), and the full conversion was achieved after 2 h at a temperature of 60 °C, with phenol and toluene as the sole reaction products. In addition, the conversion of more robust β-O-4 ether bonds in 2-phenoxy-1-phenylethanol reached up to 100% with the yield of ethylbenzene and phenol at 150 °C for 2.5 h being 60.2% and 68.3%, respectively. The reusability-experiment results indicate that Ni–CeO2/CN maintained a high catalytic activity in five reaction runs, making this a promising route for C–O ether bond cleavage under mild conditions.
研究领域:
催化化学
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生物质转化
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材料科学
✓ 已验证
DOI
高影响因子
CATALYSIS TODAY
·
2024
·
IF 5.2
Lan Zhang,Xiaomin Hu,Ning Wang,Biaohua Chen
The escalating emission of CO 2 has caused a significant environmental impact. Hydrogenation of CO 2 to methanol stands as the primary objective in the liquid sunlight vision, aiming to mitigate CO 2 emissions. CuZn-based transition metal catalysts, known for their cost-effectiveness, demonstrate commendable catalytic performance at moderate temperatures and pressures, showcasing considerable potential in industrial applications. Consequently, a series of catalysts, composed of CuZn-based species supported on CeO 2 with strategically introduced appropriate oxygen vacancies, were meticulously prepared. It worth to noting that the size of Cu was precisely tuned, along with the enhanced ability to the adsorption and activation of CO 2 and H 2 . As a result, the optimal CuZn/CeO 2 catalyst exhibits high methanol formation rate, recording at 433.4 g MeOH kg cat −1 h −1 with selectivity of 68.5% at 260 °C and 3 MPa. Simultaneously, the reaction path and the evolution of intermediates in CO 2 hydrogenation was thoroughly delineated.
研究领域:
催化化学
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环境科学
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能源化学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
·
IF 20.2
Chunmin Zhang,Chunli Wang,Qingyun Shi,Xiaoli Wang,Shaolei Zhao,Long Liang,Qingshuang Wang,Limin Wang,Yong Cheng
The high hydrogen release temperature and thermodynamic stability of the coordination hydride LiAlH 4 render it unsuitable for direct application. This work intends to improve the hydrogen release properties via compositing LiAlH 4 and AlH 3 with similar initial hydrogen release temperatures and introduce efficient additive Ni/CeO 2 composite. The thermal stability of the composite system LiAlH 4 -AlH 3 is enormously reduced compared to that of LiAlH 4 . In addition, the preferential release of hydrogen from LiAlH 4 in the composite system provides additional heat for the subsequent release of hydrogen from AlH 3 , accelerating the hydrogen release process. As a result, LiAlH 4 -AlH 3 -Ni/CeO 2 composite performs enhanced hydrogen release performance with a hydrogen release capacity of 8.27 wt% hydrogen within 300 ℃ and a dehydrogenation onset temperature as low as 72.9 ℃. The enthalpy change of the first step hydrogen release reaction decreases from −11.99 kJ mol −1 (LiAlH 4 ) to −2.02 kJ mol −1 (LiAlH 4 -AlH 3 ). Theoretical calculations indicate that both atomic dehybridisation and electron redistribution expedite the breaking of the Al-H bond and the consequent release of hydrogen.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
AICHE JOURNAL
·
2024
·
IF 3.5
Yan Shao,Bohong Wu,Boya Qiu,Rongsheng Cai,Cui Quan,Ningbo Gao,Feng Zeng,Xiaolei Fan,Huanhao Chen
Synergistic Pd–In 2 O 3 catalysts are promising candidates for producing methanol via CO 2 hydrogenation, and the metal phases in them can be tuned by thermal reduction treatment affecting the catalytic activity significantly. This work presents a comprehensive investigation to gain an insight into the effect of thermal reduction temperature on the variation and interaction of Pd and In 2 O 3 phases supported on CeO 2 (viz., PdIn/CeO 2 ) and their correlations with CO 2 hydrogenation toward methanol synthesis. The findings show that Pd/In-rich PdIn alloys and In 2 O 3 with relatively strong interaction are key phases (by reducing the PdIn/CeO 2 at 300°C) for promoting methanol formation, leading to a high selectivity to methanol at 78.9% and space–time yield (STY) of 3.6 g CH3OH g PdIn −1 h −1 . A further increase in reduction temperature (from 300 to 500°C) promoted the formation of homogenized PdIn intermetallic alloys with significantly poor ability for H 2 dissociation and CO 2 activation, and hence poor methanol yield.
研究领域:
催化化学
·
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
ChemCatChem
·
2024
·
IF 3.8
Siyang Yan,Ruilin Feng,Jiaxu Liu,Chenxi Bai,Yanlong Qi
Graphical The dehydration of 2,4-pentanediol to unsaturated alcohol was performed over ceria-based catalysts with high selectivity. A stereocatalytic effect of CeO 2 catalyst was observed for the production of trans -3-penten-2-ol, with negligible content of cis -3-penten-2-ol. The transformation of biobased alkanediols over heterogeneous catalysts is a major object. Here, a series of catalysts were prepared for 2,4-pentanediol dehydration to 3-penten-2-ol. Ceria-based catalysts had a unique property of showing high efficiency. More importantly, a stereocatalytic effect was observed for CeO 2 , yielding trans -3-penten-2-ol with a high selectivity. Raman, XPS, TPD, and TPR were carried out to clarify the catalyst structure, and the relationship between the catalyst structure and catalytic performance were studied. The amount of Lewis acid sites can hardly be correlated with the total concentrations of the oxygen vacancies. It was suggested that the geometry structure of the active sites played a crucial role in trans -3-penten-2-ol production. The oxygen vacancies originating from CeO 2 consisted of active sites with a geometrical structure, which were different from those created by Pr doping CeO 2 . In addition, the Pr doping enhanced the oxygen migration, which resulted in side reactions, consequently, giving a lower selectivity to trans -3-penten-2-ol.
研究领域:
催化化学
·
材料科学
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Liang Zhu,Yang Liu,Yanhui Gao,Ningxujin Ding,Danyu Wang,Liuliu Long,Beibei Wang,Junyu Lang,Evgeny I. Vovk,Yong Yang
The hydrogen dissociation and spillover mechanism on oxide-supported Cu catalysts play a pivotal role in the hydrogenation of carbon dioxide to methanol. This study investigates the hydrogen spillover mechanism on Cu/CeO2 catalysts using in situ spectral characterization under high-pressure reaction conditions and density functional theory (DFT) simulations. The research confirms that the Cu sites serve as the initial dissociation points for the hydrogen molecules. The chemically adsorbed hydrogen (H*) then spills over onto the CeO2 support and interacts with the lattice oxygen to form special hydroxyl groups, while simultaneously reducing the surrounding Ce4+ to form Ce3+. Interestingly, the temperature-programmed desorption (TPD) results found that heating the hydroxyl-containing surface mainly reverses H2 dissociation by desorbing H2 instead of forming H2O, while no significant vacancy formation was detected. The DFT calculation identified a subsurface pathway favoring hydrogen migration, which explained the dominating H2 in the TPD products. A chemical loop study after CO2/H2 cofeeding on the catalyst reveals that hydrogen spillover facilitates the highly reduced surface serving as the active centers, enabling a secondary methanol synthesis in a vacuum. This study provides a model of the formation and desorption pathways of hydrogen species on Cu/CeO2 catalysts and illustrates the key role of the hydrogen spillover mechanism in promoting the CO2 hydrogenation to methanol reaction through important experimental analysis.
研究领域:
催化化学
·
材料科学
·
理论计算化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Zhen-Yu Zhang,Tao Xie
Solar-driven photo-thermal dry reforming of methane (DRM) is an environmentally friendly production route for high-value-added chemicals. However, the lack of thorough understanding of the mechanism for photo-thermal reaction has limited its further development. Here, we systematically investigated the mechanism of photo-thermal DRM reaction with the representative of Ru/CeO 2 catalyst. Through in situ DRIFTs and transient experiments, comprehensive investigation into the reaction steps and their reactive sites in the process of DRM reaction were conducted. Besides, the excitation and migration direction of photo-electron was determined by ISI-XPS experiments, and the change of surface defect structure induced by light was characterized by ISI-EPR experiments. Based on the above results, the photo-enhancement effect on each micro-reaction step was determined. This study provides a theoretical basis for the industrialization of photo-thermal DRM reaction and its development of catalysts.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）