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
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
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Jiasheng Wang,Ying Zhang,Xiaonan Xu,Ming Bao
Halogenated arylamines are important intermediates for the synthesis of dyes, pesticides, herbicides, and other chemicals. One important way to prepare halogenated arylamines is catalytic hydrogenation of halogenated nitroarenes. Ni-based catalysts have been used in the hydrogenation of halogenated nitroarenes but suffer from low activity and dehalogenation side reaction. In this paper, Ni–CeO2/SiO2 heterojunction catalyst with a “raisin-bun” structure was prepared by reverse microemulsion. A built-in electric field and more oxygen vacancies were formed due to electron transfer from Ni to CeO2 as a result of their work function difference. The built-in electric field leads to the heterolytic cleavage of H2, thereby improving the hydrogenation activity. Oxygen vacancies preferentially adsorb and activate nitro groups, inhibiting the dehalogenation side reaction. Through the cooperation of built-in electric field and oxygen vacancy, synchronous enhancement of the activity and selectivity is obtained successfully. This finding provides a new view for the design of non-noble metal-based catalysts with high activity and selectivity.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
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
Journal of Energy Chemistry
·
2020
·
IF 7.216
Shuangxi Lin,Ziwen Hao,Jindong Shen,Xiao Chang,Shouying Huang,Maoshuai Li,Xinbin Ma
The metal-support interaction is of critical importance to enhance the catalytic activity and selectivity. However, it is still challenging to construct an appropriate interaction starting from the catalyst fabrication and/or activation. We herein established low-temperature treatment of Ni 2+ ions impregnated on ceria in reductive atmosphere and reduction–oxidation cycles as effective approachs to regulate the metal-support interaction and raise the catalytic performance in the CO 2 methanation. The proposed construction approach yielded Ni/CeO 2 that displayed highly dispersed Ni nanoparticles in contact with CeO 2 (111) and (100) facet, higher density of surface oxygen vacancies and larger amounts of weak basic sites relative to the reference samples, which increased the capacity for H 2 and CO 2 adsorption/activation. The interaction resulted in appreciably (2–3 fold) higher activity in the CO 2 methanation with maintaining almost full selectivity to CH 4 and high stability. Coverage of Ni surface by CeO 2− x thin layer as a typical structure of strong metal-support interaction resulting from high-temperature reduction, can be alleviated via reduction–oxidation cycles. We also demonstrate the activation treatment-determined metal-support interaction effect can generally extend to (TiO 2 and ZrO 2 ) supported Ni catalysts.
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
·
2024
·
IF 8.1
Yunzhu Wang,Yang Chen,Songshan Zhu,Di Song,Tianhao Ai,Sufang He,Yongming Luo
Steam reforming of glycerol (GSR) to produce hydrogen has been considered a sustainable and low-cost route for hydrogen production. The selection of a suitable catalyst support is crucial for achieving efficient hydrogen production at lower temperatures. CeO 2 has been widely used in heterogeneous catalysis and exhibits excellent low-temperature catalytic performance. However, different calcination mode may influence catalyst performance. In this study, the Ni/CeO 2 catalyst prepared by rapid calcination mode (Ni/CeO 2 -RC), was used for hydrogen production from GSR, and the Ni/CeO 2 catalyst with the conventional programmed-heating calcination method (Ni/CeO 2 -PC) was applied for comparison. The effect of different calcination modes on the physico-chemical properties of the catalysts was investigated through multiple characterizations such as N 2 adsorption-desorption, X-ray diffraction, hydrogen temperature programmed reduction, transmission electron microscopy, X-ray photoelectron spectroscopy, H 2 chemisorption, CO-oxygen storage capacity and conversion, temperature programmed oxidation, and Raman spectroscopy. The rapid calcination mode promoted stronger metal-support interactions in Ni/CeO 2 -RC, inducing the formation of nickel species highly susceptible to reduction due to the electronic effect. Additionally, rapid calcination facilitated the increased incorporation of nickel particles into the cerium dioxide lattice, leading to lattice distortions, thereby contributing to the formation of more oxygen vacancies. The abundant oxygen vacancies promoted the activation of water, thus realizing the high H 2 selectivity of Ni/CeO 2 -RC. Moreover, the strong oxygen storage-release ability of Ni/CeO 2 -RC facilitated the oxidative effect of carbon deposition and the strong Ni–CeO 2 interaction effectively inhibit sintering of nickel nanoparticles on Ni/CeO 2 -RC. Therefore, Ni/CeO 2 -RC exhibited outstanding catalytic stability, remaining active for 35 h without deactivation, whereas Ni/CeO 2 -PC rapidly deactivated after 25 h of reaction.
研究领域:
催化化学
·
能源材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2020
·
IF 5.006
Feng Lin,Yulong Ma,Yonggang Sun,Xiuqin Men,Yingbo Zhu,Tingting Gao,Kanghe Zhao
Strategies for catalytic lignin depolymerization to yield ethylbenzene chemicals are green, sustainable and environmentally friendly methods. In this study, a series of Ni-CeO 2 /H-ZSM-5 catalysts were prepared via the precipitation method, which catalytically degraded the β-O-4 chemical bonding structure to yield ethylbenzene chemicals. The 2-(2-methoxy-phenoxy)-1-phenylethanol substance (β-O-4) was selected as a typical lignin model compound for the investigation of the intrinsic depolymerization mechanism and the catalytic performance. The results demonstrated that the introduced CeO 2 active phase can effectively promote the catalytic conversion of the β-O-4 chemical bonding structure to ethylbenzene chemicals. Physicochemical data demonstrate that the reaction pathways and hydrogenation selectivity were effectively regulated and controlled by the tuning of the dehydration and hydrogenolysis processes via the introduction of CeO 2 , which realized the selective adjustment of the redox properties and the surface valence states of active species in the catalytic process due to its excellent oxygen transfer performance.
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
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
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhuwei Yang,Linsen Li,Xiao Yang,Hui Xiong,Riguang Zhang,Zhao Jiang
In this study, a series of Ni-CeO 2 /TS-1 (Titanium Silicalite-1) catalysts were synthesized for dry reforming of methane (DRM). Among them, 5Ni-10CeO 2 /TS-1 exhibited the highest catalytic performance with 89 % CH 4 and 93 % CO 2 conversions, 4.81 mol CH4 ·g Ni -1 ·h −1 and 4.99 mol CO2 ·g Ni -1 ·h −1 specific activities, 95.5 % H 2 /CO ratio after 50 h, accompanied by the good stability with 2.9 % CH 4 and 2.3 % CO 2 activity loss within 100 h. Combined with various characterizations, the structure–function relationship was also investigated. For the physical and morphological analysis, it was indicated that the appropriate CeO 2 content could effectively diminish, disperse the Ni nanoparticles, and maintain MFI backbone structure. For the electronic structure, the introduced CeO 2 could improve the amount and strength of the surface Ni-O-X (Ti or Ce) species by changing the interaction among Ni nanoparticles, TS-1 and CeO 2 . It led to more Ni nanoparticles in stronger electron-deficient state, as well as more medium-strength basic sites, favoring for the activation of CH 4 and CO 2 . However, Ni nanoparticles would be covered when excessive CeO 2 was introduced, preventing the exposure of the active sites. Therefore, only the suitable CeO 2 in the catalysts could significantly improve catalytic performance for DRM with long-term stability. Furthermore, the good anti-sintering and anti-coking properties of 5Ni-10CeO 2 /TS-1 were mainly dependent on the optimal amount of surface Ni-O-X species with high strength. In-situ DRIFTS (diffuse reflectance infrared spectroscopy) analysis demonstrated that the introduced CeO 2 could help catalyst favor for activating CH 4 and CO 2 molecules, and inhibiting the CH 4 overcracking and carbon accumulation, confirmed by the long-term measurement and structure analysis of spent catalysts.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hongwang Liu,Yining Zhang,Sibao Liu,Sha Li,Guozhu Liu
Ammonia is a promising hydrogen storage material due to its ease of storage and decomposition to CO x -free hydrogen. Herein, we report colloidal solution combustion synthesis (CSCS) to construct Ni-CeO 2 nanocomposite catalysts for efficient ammonia decomposition to generate hydrogen. Unlike conventional supported Ni/CeO 2 catalyst, the prepared Ni-CeO 2 nanocomposite catalyst exhibited nickel embedded in CeO 2 matrix with enhanced metal-support interaction. The physicochemical properties and metal-support interaction of the catalysts can be tuned by adjusting the amount of silica sol template. The resulted Ni-CeO 2 nanocomposite catalysts exhibited outstanding catalytic performance in terms of activity and stability. The hydrogen production rate reached 32.9 mmol g cat −1 min −1 at 500 °C, which is superior to other state-of-the-art Ni-based catalysts and even comparable or better than some reported Ru-based catalysts. The systematic characterizations demonstrated that the unique Ni-CeO 2 nanocomposite structure with enhanced metal-support interaction, not only provided a rich Ni-CeO 2 interface to stabilize small-sized Ni nanoparticles, but also had a high concentration of oxygen vacancy to strengthen electronic metal-support interaction, making nickel surface electron-rich. The integrated studies of kinetics, temperature-programmed surface reaction, and DFT calculations corroborated that this enhanced metal-support interaction including geometric and electronic effects, favored the enrichment of NH 3 on the catalyst surface and facilitated rate-determining N≡N bond formation step, thereby boosting the reaction rate. This study highlights the importance of designing new structural catalysts with enhanced metal-support interaction for boosting hydrogen production from ammonia decomposition.
研究领域:
催化
·
材料科学
·
化学工程
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Haiming Gu,Xuxing Shen,Minyu Yu,Miaomiao Niu,Shanhui Zhao,Siwen Zhang,Xiaolong Bi,Yadong Yu,Mofei Zhong,Lianggan Guan
Sorbent looping dry reforming of methane (SLDRM) represents a promising approach for CO 2 emission reduction and resource utilization, with its advancement hinging on the development of dual functional materials (DFMs) capable of simultaneous CO 2 capture and catalytic methane conversion. In this study, CaO-Ni based DFMs supported on various materials were synthesized via sol–gel method and characterized using SEM, XRD and TGA. Isothermal SLDRM experiments were performed in a fixed bed to evaluate the performance of these materials. Initial screening of support materials revealed that CH 4 conversion activity followed the order: CeO 2 >Al 2 O 3 >La 2 O 3 >MgO ≈ Y 2 O 3 , with CeO 2 emerging as the optimal support due to its superior performance. The synergistic effect of the Ni catalyst and CH 4 atmosphere significantly enhanced low-temperature decarbonization of the sorbent, mitigating sintering and enhancing cyclic CO 2 capture capacity. In-situ CO 2 conversion during CH 4 reforming disrupted the decarbonization reaction equilibrium, enabling efficient isothermal CO 2 capture and decarbonation. Ni decoration significantly enhanced CH 4 conversion, increasing from nearly 0% without Ni to 87% at 10% Ni loading, while higher loadings provided only marginal improvements. Although an increase in reaction temperature enhanced CH 4 conversion, it also increased CO 2 partial pressure, promoting the reverse water gas shift reaction and resulting in a H 2 /CO ratio below 1 when the temperature exceeded 650°C. Stability tests over 10 consecutive SLDRM cycles demonstrated good stability of CaO-10Ni/CeO 2 , maintaining a CH 4 conversion efficiency of 87% and a stable H 2 /CO ratio of approximately 1 at 650°C. Carbon deposition during the CH 4 step was effectively removed during carbonation, as confirmed by Raman spectroscopy, while SEM and XRD analyses revealed preserved surface morphology and phase composition. These findings highlight the excellent reactivity and stability of CaO-10Ni/CeO 2 , positioning it as a highly promising candidate for advancing CO 2 emission reduction and resource utilization strategies.
研究领域:
化学工程
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Yingying Jin,Kaihao Fan,Miao Feng,Yaoguang Wang,Hongfeng Chen,Xuesong Liu
This study investigates synergistic effects in Ni/CeO 2 catalysts for ammonia decomposition, comparing impregnation and mechanical mixing preparation methods. The impregnated catalyst achieved >90 % NH 3 conversion above 500 °C, outperforming Ni/SiO 2 and mixed counterparts. Strong interactions at the Ni-CeO 2 interface facilitated the formation of Ni-O-Ce bonds, lattice distortion, and oxygen vacancies (O v )/Ce 3+ species, enhancing Ni dispersion (34.7 nm vs. 73.1 nm) and electron transfer. Optimal NH 3 pretreatment (550 °C, 1.5 h) generated metallic Ni 0 as the primary active species, with higher Ni 0 content (XPS) and reducibility (H 2 -TPR). The novelty lies in establishing how NH 3 pretreatment dynamically assembles contiguous Ce 3+ -O v -Ni 0 triads. These sites facilitate rate-limiting N 2 desorption through localized electron donation from O v and Ce 3+ to Ni 0 , which weakens N-N bonds (NH 3 -TPD). Impregnation-derived synergy: (i) enhances Ni dispersion/reduction, (ii) promotes O v formation, and (iii) enables NH 3 -pretreatment-induced assembly of contiguous Ce 3+ -O v -Ni 0 triads that create electron-rich sites, lowering the activation barrier. This work provides a foundation for designing cost-effective catalysts via atomic-scale control of metal-support interactions.
研究领域:
催化
·
材料科学
·
化学工程
·
表面科学
·
环境科学
✓ 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）