CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Zeyu Jiang,Shengying Zhao,Yuhao Yang,Minghui Tan,Guohui Yang,Yisheng Tan
As one of the most important green chemicals, dimethyl carbonate (DMC) has wide application prospects in electrochemistry, fuel additive, solvent and building block in organic synthesis. The effective utilization of CO 2 to synthesize DMC has been proved to be highly advantageous. In this study, a series of Ce-BTC MOF-derived nanorod CeO 2 catalysts for the direct synthesis of DMC from CO 2 and methanol were prepared via complexation reaction at room temperature and then thermal decomposition under different atmospheres. The calcination atmosphere had great influence on the structure and catalytic properties of obtained CeO 2 catalysts. The CeO 2 derived from calcination of Ce-BTC at 500 °C under H 2 atmosphere exhibited higher specific surface area, oxygen vacancy concentration and CO 2 adsorption capacity. And thus, its DMC yield was up to 6.332 mmol/g CeO2 within 4 h, much higher than that of commercial nano CeO 2 and other as-prepared catalysts in absence of dehydrating agents.
研究领域:
化学工程
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Energies
·
2024
·Vol. 17
·期 24
·6314
·
IF 3
Zhiyin Zhang,Huimin Hu,Jie Yang,Zhengguang He,Kai Yan,Tianyu Liu,Chang Wen
The photo-thermochemical cycle (PTC) for water splitting offers a sustainable method for hydrogen production by efficiently utilizing solar energy. This study explored the use of CeO2as a catalyst in the PTC system to enhance hydrogen yield. A nanostructured CeO2catalyst was synthesized via the sol-gel method, achieving an H2yield of 8.35 μmol g−1h−1. Stability tests over five cycles showed consistent yields between 7.22 and 8.35 μmol g−1h−1. Analysis revealed that oxygen vacancies (VOs) increased after the photoreaction and depleted during the thermal reaction, which aligns with the expected PTC mechanism for hydrogen production. Single-factor experiments highlighted that photoreaction duration mainly influenced VOs generation, while thermal duration and temperature impacted VOs consumption and intermediate reaction rates. A response surface methodology (RSM) model predicted optimal conditions for maximum H2yield (8.85 μmol g−1h−1) with a photoreaction duration of 46.6 min, thermal duration of 45.4 min, and thermal temperature of 547.2 °C.
研究领域:
材料科学
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能源科学
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催化化学
✓ 已验证
DOI
高影响因子
RENEWABLE ENERGY
·
2024
·
IF 9
Daxin Jiang,Min Lin,Yuhao Yan,Lulu Zhan,Rui Li,Yulong Wu
Catalytic hydrodeoxygenation (HDO) is an effective way to produce high–value products from lignin-derived phenolic compounds. In this work, three different morphologies of Ni/CeO 2 catalysts (amorphous, cubic, and rod-shaped) have been prepared through the conventional wet impregnation method. They can be used for the HDO of guaiacol to prepare cyclohexanol, an important chemical raw material. The influence of different morphologies of CeO 2 on catalytic activity was explored. The research results indicate that Ni/CeO 2 –r catalysts with rod-shaped structures exhibit excellent catalytic properties. As a result, a 100 % conversion rate and 96.9 % cyclohexanol yield were achieved on the Ni/CeO 2 –r catalyst at 240 °C. The catalytic performance of the three catalysts follows this order: Ni/CeO 2 –r (rod-shaped) > Ni/CeO 2 –c (cubic) > Ni/CeO 2 –p (amorphous). The results of Raman and XPS indicate significant differences in the surface oxygen vacancy in catalysts with different morphologies. The Ni/CeO 2 –r catalyst has the highest oxygen vacancy concentration and defect. In addition, Ni/CeO 2 –r also has the largest specific surface area (S BET ) and the highest nickel dispersion, and forms more Ni 0 because of the strong interaction of Ni species and CeO 2 support. Therefore, Ni/CeO 2 –r exhibits the most excellent catalytic performance for the hydrogenation of guaiacol than the other two catalysts. Moreover, the cycling activity test was also investigated over the Ni/CeO 2 –r catalyst. After five cycles, the conversion rate of guaiacol and the yield of cyclohexanol hardly decrease. This work provides vital ideas for the development of higher-activity, higher-stability, and low-cost catalysts for the conversion of lignin-derived phenolic compounds in the future.
研究领域:
催化化学
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材料科学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2025
·
IF 5.5
Sajid Ali,Xingwen Cha,Jinxin He,Muhammad Ubaid Ali,Muhammad Junaid Aslam,Songbo Chen,Kok Bing Tan,Guowu Zhan
Tunable electronic properties of supported Cu/CeO2 catalysts are critical for improving the active site activity in catalysis. In this contribution, we propose a surface engineering protocol that utilizes unique ascorbic acid (AA) properties to generate surface defects and modify the electronic properties of Cu–Ce catalysts. This approach relies on forming abundant (Ce3+-Ov) defective sites on the CeO2 surface synthesized with a Ce-benzene-tricarboxylate metal–organic framework (MOF) as a precursor through AA adsorption. Subsequently, Cu sites can be effectively anchored onto the generated Ce3+-Ov, exhibiting excellent electronic transfer between (Ce3+-Ov/Ce4+ ↔ Cu2+/Cu+) CuCe, resulting in highly active Cu+ with well-balanced Ce3+-Ov defects. A high fraction of Cu+ with Ce3+-Ov was dedicated to the presence of AA. The resultant Cu/AA-MOF-CeO2 catalyst demonstrated outstanding performance toward CO oxidation (90–95 °C), being far superior to that of the conventionally prepared Cu/MOF-CeO2 catalyst (110–115 °C). In-depth characterizations confirmed that the remarkable performance was considerably related to the enhanced Cu–Ce interaction, enriched Cu+ active sites, and balanced Ce3+-Ov defects. This work highlights the potential of the Cu/AA-MOF-CeO2 catalyst as a sustainable solution for low-temperature catalytic CO oxidation reaction.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Shengnan Guan,Qifu Huang,Jianru Ma,Wenzhi Li,Ajibola T. Ogunbiyi,Zean Zhou,Kun Chen,Qi Zhang
The catalytic performance of MnO2(x)–CeO2 (x = Mn/Ce molar ratio) and the synergistic effect have been investigated in formaldehyde removal. The results showed that formaldehyde achieved 100% conversion at 60 °C for MnO2(1.5)–CeO2, with the gas hourly space velocity = 120 000 mL h–1 gcat–1. It was lower than the formaldehyde removal temperature of MnO2 (130 °C) and CeO2 (170 °C). The apparent activation energy for HCHO oxidation with MnO2(1.5)–CeO2 was 34.2 kJ mol–1. The partial mutual replacement of Mnx+ and Cex+ decreases the crystallite size due to the MnO2/CeO2 interaction. The X-ray photoelectron spectroscopy and the Raman analyses show that the Mn3+/Mn and Oads/Olatt ratios and the relative concentrations of oxygen vacancies for MnO2(1)–CeO2 and MnO2(1.5)–CeO2 were higher than those of the rest of the catalysts. Thus, the lattice oxygen (Olatt) from CeO2 readily transfers to the oxygen vacancy, achieving Olatt activation to surface-adsorbed oxygen (Oads).
研究领域:
催化化学
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环境科学
✓ 已验证
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Shafqat Ullah,Yongqi Pan,Qiangqiang Xue,Tianyi Huang,Yizhi Hu,Runping Ye,Yujun Wang,Guangsheng Luo
CO 2 methanation has emerged as a key strategy for its potential uses and ability to alleviate climate change by reducing CO 2 emissions. Herein, we present a controllable and continuous improved coprecipitation catalyst preparation method employing a T-junction microreactor to investigate La doped Ni-CeO 2 catalysts. A series of catalysts was systematically synthesized, with Ni/CeLa (5:5) emerging as the most promising candidate, exhibiting 76 % CO 2 conversion at 250 °C and 60.5 mmol/g cat .h space–time yield of methane. Different structural characterization techniques, including in-situ Raman, Quasi in-situ XPS, in-situ DRIFTS, and DFT calculations were employed to unravel the structure activity mechanisms contributing to the enhanced catalytic performance. The findings indicate that the introduction of La as a dopant reduces particle size, promotes Ni dispersion, and increases interfacial sites. These enriched interfacial sites contribute a pivotal role in facilitating the adsorption and hydrogenation of bicarbonate species, ultimately leading to improved methanation performance. This study not only highlights the efficiency of the La doped Ni-CeO 2 catalyst, but it also gives valuable insights for chemical strategy to improve structure activity relationships and mechanism studies for efficient CO 2 methanation performance.
研究领域:
催化化学
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材料科学
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环境科学
✓ 已验证
DOI
高影响因子
Molecular Catalysis
·
2021
·
IF 5.062
Rui Tang,Niamat Ullah,Yajun Hui,Xin Li,Zhenhua Li
Carbon dioxide hydrogenation for value-added chemicals has been regarded as a promising way for CO 2 utilization. This paper describes the preparation of Ni/CeO 2 catalysts derived from Ce-MOF precursor by impregnation or one-pot method and their application in carbon dioxide methanation. Various techniques were employed to characterize the prepared catalysts, including N 2 adsorption–desorption, X-ray diffraction (XRD), Raman spectroscopy, field emission scanning electron microscopy (SEM), H 2 -temperature programmed reduction (H 2 -TPR), H 2 -temperature programmed desorption (H 2 -TPD) and CO 2 -temperature programmed desorption (CO 2 -TPD). The results showed that compared with commercial CeO 2 and CeO 2 prepared by precipitation, CeO 2 derived from Ce-MOF exhibited more oxygen vacancies and lower temperature reducibility, making it more beneficial for the adsorption and activation of CO 2 . Consequently, nickel supported on rod-shaped CeO 2 derived from Ce-MOF exhibited higher CO 2 conversion and methane selectivity at low temperatures. Furthermore, the Ni/CeO 2 −M-1 catalysts prepared by one-pot method showed superior activity since nickel could be partially incorporated into ceria lattice, leading to the formation of Ce 1-x Ni x O 2-y solid solutions and oxygen vacancies. The effect of nickel loading on the properties of the catalysts by one-pot method was also investigated, and the optimum Ni loading was 15 wt.% owing to the maximum number of oxygen vacancies being reached.
研究领域:
催化化学
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Weiyuan Yao,Xiaoqiang Wang,Yue Liu,Zhongbiao Wu
In this paper, Ce O P material (mainly consisted of CePO 4 ) and TiO 2 supported CeO 2 catalysts were prepared by wet impregnation route for the selective catalytic reduction (SCR) of NO with NH 3 . The SCR activity results had revealed that CeO 2 /Ce O P-0.4 catalyst yielded over than 90% NO conversion within the temperature range of 200–300 °C, whereas the deNO x efficiency of CeO 2 /TiO 2 -0.4 catalyst was less than 30% at 200 °C. After a series of characterization tests, it was found that CeO 2 /Ce O P catalysts were of better dispersion of active phase than CeO 2 /TiO 2 owing to the strong interactions between CeO 2 and surficial Ce O species on Ce O P material. Thus, more active oxygen species could participate in the SCR reaction at low temperature. Furthermore, compared to CeO 2 /TiO 2 sample, the surface acidity was greatly enhanced for CeO 2 /Ce O P catalysts by the introduction of the acidic support, benefiting the adsorption of NH 3 . Both of which were attributed to the main reasons of the promoted SCR performance over CeO 2 /Ce O P catalysts. Moreover, the NO x ad-species on CeO 2 /TiO 2 sample were very stable and could hardly react with adsorbed NH 3 , impeding L-H reaction pathway at low temperature.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
ChemCatChem
·
2024
·
IF 3.8
Pengchao Ren,Zhenzhou Zhang,Tingting Hu,Zhihui Fan,Shanshan Dang,Sifan Cheng,Weifeng Tu,Yi-Fan Han
Graphical The apparent rate coefficients for CH 3 OH synthesis from CO hydrogenation are a single-valued function of the CO 2 -to-CO ratio in the contacting gas phase, because this ratio determines the extent of surface oxidation of Ce 2 O 3 to CeO 2 , the relative abundance of surface Ce 3+ , and in turn the density of Cu 0 -Ce 3+ sites pair on the working Cu/CeO 2 catalyst. This study investigated the dynamic structure of a working Cu/CeO 2 catalyst and its catalytic consequences for CH 3 OH synthesis via CO hydrogenation by kinetics, high-precise chemical titration, and a series of in situ X-ray spectroscopies. We have revealed that the apparent rate coefficients for CH 3 OH synthesis from CO hydrogenation are a single-valued function of the CO 2 -to-CO ratio in the contacting gas phase. This ratio determines the extent of surface oxidation of Ce 2 O 3 to CeO 2 , the relative abundance of surface Ce 3+ and Ce 4+ sites, and in turn, the density of Cu 0 -Ce 3+ sites pair on the working Cu/CeO 2 catalyst, although the chemical state of Cu and elemental distribution of both Cu and Ce were insensitive to the ratio. The reactivity of CH 3 OH formation and the Cu 0 -Ce 3+ sites decrease monotonously with an increase in the CO 2 -to-CO ratio. The direct connection of the reactivity and the oxidant-to-reductant ratio appears to be general for heterogeneous catalysis, for which the oxidant oxidizes metal atoms. In contrast, the reductant scavenges surface oxygen atoms, thus dictating the density of surface sites and their thermodynamic activities.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 102
·99842-99850
·
IF 3.289
Kun Zhang,Xu Zhang,Tianwei Tan
In this study, the conversion from Botryococcus braunii liquid to bio-jet fuel via a Ru/CeO2 catalyst was conducted. At first, novel Ru/CeO2 catalysts were prepared in order to increase the catalytic activity. “Ru/CeO2-alcohol thermal” showed the highest activity: the squalane conversion exceeded 90%, an increase of about 22% in comparison with “Ru/CeO2-impregnation”. When the B. braunii liquid was used as the raw material, no obvious catalytic activity was noticed. Therefore, the influence of impurities in the B. braunii liquid on the Ru/CeO2 reaction were preliminarily analysed, confirming that the pigments (such as β-carotenoid) and the oxygen compounds (such as fatty acids) were the main factors influencing the Ru/CeO2 reaction. Based on these results, the reaction process was optimized: prolonging the reaction time and pretreating the B. braunii liquid with H2. Finally, the production of bio-jet fuel over Ru/CeO2 was successfully achieved.
研究领域:
生物技术
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催化化学
·
可再生能源
✓ 已验证
DOI
高影响因子
CATALYSIS LETTERS
·
2025
·Vol. 155
·期 6
·1-17
·
IF 2.4
Sun Ran,Hou Kunge,Jin Xingpeng,Yang Lihui,Song Lijie,Ouyang Chuang,Hou Jianyuan,Yuan Yuan,Liu Xingang,Zhang Renxi
The development of new technologies for removal of NO and chlorobenzene in complex flue gas situations at low temperature is a complex and demanding task. Here, the synergistic removal of NO and chlorobenzene was achieved through catalysis assisted dielectric barrier discharge (DBD) mechanism under different conditions. The experimental results suggested that the increase of specific energy density (SED) and the loading of CeO 2 strengthened the treatment of NO and chlorobenzene. A higher degradation efficiency of NO and a lower production rate of NO 2 were achieved after the introduction of chlorobenzene. The removal of chlorobenzene could also be benefited from this process, and the introduction of NO promoted CO 2 selectivity of chlorobenzene. The XPS and H 2 -TPR analyses confirmed that the reaction between chlorobenzene and NO occurred by the assistance of Ce 3+ /Ce 4+ redox cycle as well as the consumption and regeneration of chemically adsorbed oxygen. During the reaction, the oxygen vacancies (OVs) caused by plasma etching promote the redox cycle and alleviate the catalyst poisoning caused by chloride ions (Cl − ). Furthermore, a comprehensive analysis of the resulting byproducts revealed phenol as the most significant intermediate in chlorobenzene degradation, while acetaldehyde emerged as the major product resulting from ring-opening processes of chlorobenzene. Utilizing chlorobenzene from flue gas subtly, this method presents a more sustainable alternative for NO reduction, showing promise for addressing industrial emission challenges. Graphical
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Bin Fu,Yuqiong Zhao,Shipeng Zhang,Ying Wang,Jun Liu,Guojie Zhang
Nickel-based catalysts frequently encounter significant challenges in achieving both high CO 2 conversion and superior CO selectivity during reverse water gas shift (RWGS) reactions. To address this issue, we developed a facile strategy to prepare highly dispersed Ni/CeO 2 catalysts by forming Ce 1−x Ni x O 2−y solid solutions. Under conditions of 300–600 °C, 0.1 MPa, and a gas hourly space velocity (GHSV) of 40,000 mL g cat −1 h −1 , the 5Ni/CeO 2 -A catalyst exhibited outstanding selectivity, approaching 100 %. The RWGS reaction rate reached 1332 μmol CO g Ni −1 s −1 and maintained stable for 50 h almost without deactivation. The formation of Ce 1−x Ni x O 2−y solid solution uniformly disperses numerous Ni species in the CeO 2 lattice, effectively inhibiting Ni aggregation. This highly dispersed Ni weakens CO adsorption and facilitates its direct desorption without excessive hydrogenation. Moreover, the catalyst remains well-dispersed state even after reduction. The formed Ce 1−x Ni x O 2−y solid solution generates abundant oxygen vacancies on the catalyst surface, enhancing H 2 dissociation. The catalyst’s pore size distribution is also modified, creating stacked pores that favor reactant diffusion and expose more active centers. In-situ DRIFTS experiments demonstrate that Ce-OH plays a pivotal role in CO 2 adsorption on the 5Ni/CeO 2 -A catalyst, while the stabilization of bicarbonate and formate intermediates by the highly dispersed Ni further promotes catalytic performance. This study introduces a novel preparation method and provides valuable insights for designing Ni-based catalysts with exceptional CO selectivity.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
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