ENERGY
·
2024
·
IF 9
Tao Tan,Yushu Chen,Yongyue Wang,Zuhao Li,Zhige Zhang,Jun Xie,Yong Chen
The use of green biogas as a raw material for producing methanol-friendly syngas (H 2 /CO ≈ 2) for one-step methanol synthesis has gained significant attention. However, developing efficient catalysts with high activity and stability remains challenging, as they often face issues with stability and carbon deposition. This study presents a Ni/CeO 2 /HT catalyst designed for high activity and long-term stability by leveraging the Ce redox cycle and strong interactions between Ni-CeO 2 and hydrotalcite (HT). The catalyst benefits from abundant oxygen vacancies generated by the Ce 3+ - Ce 4+ pathway, enhancing its ability to activate CO 2 and H 2 O and providing excellent coke resistance. Comprehensive analyses of CO 2 /H 2 O adsorption and carbon elimination mechanisms were conducted using techniques such as in situ H 2 -TPR, CO 2 /H 2 O-TPSR, in situ CH 4 -TPSR, CO 2 /H 2 O-TPO, and FTIR. The Ni/CeO 2 /HT catalyst outperformed others in CO 2 /H 2 O adsorption and CH 4 activation capacity, promoting the generation of active oxygen species and effectively removing coke precursors, thereby improving resistance to Ni sintering and carbon deposition. At 750 °C and a weight hourly space velocity (WHSV) of 32,400 mLg Cat −1 h −1 , it achieved CH 4 and CO 2 conversions of 93 % and 66 %, respectively, with long-term stability exceeding 200 h.
研究领域:
催化化学
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可再生能源
·
材料科学
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产品关联
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2024
·Vol. 30
·期 68
·e202402516
·
IF 3.9
Chaoyang Yang,Junlei Zhang,Weiping Liu,Yao Cheng,Xueyi Yang,Wanglei Wang
Graphical This study investigated the impact of H 2 /CO 2 partial pressure ratios on CO 2 methanation using Ni/CeO 2 . Results show elevated H 2 /CO 2 ratios enhance CO 2 conversion and CH 4 selectivity, achieving complete methanation at 250 °C and 100 % selectivity at 400 °C. In-situ DRIFTS analysis indicates formate pathway dominance at higher ratios, key for CH 4 production and CO 2 mitigation strategies. On the way to carbon neutrality, directly catalyzing atmospheric CO 2 into high-value chemicals might be an effective approach to mitigate the negative impacts of rising airborne CO 2 concentrations. Here, we pioneer the investigation of the influence of the H 2 /CO 2 partial pressure ratio (PPR) on air-level CO 2 methanation. Using Ni/CeO 2 as a case catalyst, increasing H 2 /CO 2 PPR significantly improves low-temperature CO 2 conversion and high-temperature CH 4 selectivity, i. e., from 10 of H 2 /CO 2 PPR on, CO 2 is completely methanized at 250 °C, and nearly 100 % CH 4 selectivity is achieved at 400 °C. 100-hour stability tests demonstrate the practical application potential of Ni/CeO 2 at 250 °C and 400 °C. In-situ DRIFTS reveal that reinforced formate pathway by increasing H 2 /CO 2 PPR is responsible for the high CH 4 yield. In contrast, even though the CO pathway dominated CO 2 conversion on Ni is enhanced by rising H 2 /CO 2 PPR, but at a high reaction temperature, the promoted CO desorption still leads to lower CH 4 selectivity. This work offers deep insights into the direct air-level CO 2 resourceization, contributing to the achievement of airborne CO 2 reductions.
研究领域:
化学工程
·
环境科学
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产品关联
DOI
PubMed
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
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材料科学
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DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2024
·
IF 3.7
Yutong Pan,Pengju Gao,Shixiong Tang,Xiaoyu Han,Ziwen Hao,Jiyi Chen,Zhenmei Zhang,Heng Zhang,Xiaohui Zi,Maoshuai Li,Shiwei Wang,Yue Wang,Xinbin Ma
This work synthesized a series of Ni/CeO 2 /Al 2 O 3 catalysts with varying CeO 2 doping amounts to enhance low-temperature CO 2 methanation. The introduction of CeO 2 weakens the interaction between Ni and Al 2 O 3 , leading to the formation of Ni-CeO 2 active sites. This results in a high dispersion of Ni and CeO 2 , improved catalyst reducibility, increased number of active sites, and enhanced the CO 2 methanation. This work further investigated the impact of WHSV and catalyst stacking configuration to enhance the reaction. When the catalyst is stacked into three segments with a temperature gradient of 330 °C, 300 °C, and 250 °C under WHSV=9000 ml·h –1 ·(g cat) –1 , the CO 2 conversion significantly increases to 95%, which is remarkably close to the thermodynamic equilibrium (96%).
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2025
·
IF 6.2
Tong Zhang,Haiyong Wang,Chenguang Wang,Qiying Liu
Acetol is the important platform molecule, which showed diversified applications in organic synthesis, pharmaceutic, food and polymer industrials. The production of acetol from selective fructose hydrogenolysis is of scientific and practical interests. However, by catalysis, precisely controlling the target C-C and C-O bonds splitting is an open challenge, resulting in the low target product yields. Herein, by regulating the metal-support-interactions, which enhanced electron transfer capacity and improved acetol production from fructose hydrogenolysis through controlling the important intermediate species, obtaining the highest 53.6 % yield and an average conversion rate of 1.24 × 10 −5 mol/(g cat .s) within short time of 10 min. The interfacial charge transfer in the surface structure of the catalyst along with the Ni metal content was revealed by various characterizations. This research provides a preliminary method for electron transfer regulation of Ni/CeO 2 catalysts in acetol production from fructose hydrogenolysis, showing practical application potentials due to the simple preparation of the catalyst that possibly contribute to the reactions on a large scale.
研究领域:
催化化学
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可再生化学
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生物质转化
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多相催化
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绿色化学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·Vol. 47
·期 83
·35352-35364
·
IF 7.139
Zhichao Yu,Wei Zhang,Yongxi Zhang,Yaokun Fu,Ying Cheng,Sanyang Guo,Yuan Li,Shumin Han
Magnesium hydroxide (MgH 2 ) has excellent reversibility and high capacity, and is one of the most promising materials for hydrogen storage in practical applications. However, it suffers from high dehydrogenation temperature and slow sorption kinetics. Rare earth hydrides and transition metals can both significantly improve the de/hydrogenation kinetics of MgH 2 . In this work, MgH 2 –Mg 2 NiH 4 –CeH 2.73 is in-situ synthesized by introducing Ni@CeO 2 into MgH 2 . The unique coating structure of Ni@CeO 2 facilitates homogeneous distribution of synergetic CeH 2.73 and Mg 2 NiH 4 catalytic sites in subsequent ball milling process. The as-fabricated composite MgH 2 -10 wt% Ni@CeO 2 powders possess superior hydrogenation/dehydrogenation characteristics, absorbing 4.1 wt% hydrogen within 60 min at 100 °C and releasing 5.44 wt% H 2 within 10 min at 350 °C. The apparent activation energy of MgH 2 -10 wt% Ni@CeO 2 is determined to be 84.8 kJ/mol and it has favorable hydrogen cycling stability with almost no decay in capacity after 10 cycles.
研究领域:
材料科学
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无机化学
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能源化学
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纳米催化
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氢能源存储
✓ 已验证
DOI
高影响因子
Engineering
·
2021
·
IF 7.553
Xinyu Cao,Tiancheng Pu,Bar Mosevitzky Lis,Israel E. Wachs,Chong Peng,Minghui Zhu,Yongkang Hu
Reductive pretreatment is an important step for activating supported metal catalysts but has received little attention. In this study, reconstruction of the supported nickel catalyst was found to be sensitive to pretreatment conditions. In contrast to the traditional activation procedure in hydrogen, activating the catalyst in syngas created supported Ni nanoparticles with a polycrystalline structure containing an abundance of grain boundaries. The unique post-activation catalyst structure offered enhanced CO adsorption and an improved CO methanation rate. The current strategy to tune the catalyst structure via manipulating the activation conditions can potentially guide the rational design of other supported metal catalysts.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
ChemCatChem
·
2026
·Vol. 18
·期 6
·e01859
·
IF 4.1
Jiahao Qi,Shangmeng Ning,Yuan Liu,Yongdan Li,Cuijuan Zhang
Developing high-performance Ni-based catalysts is critical for the practical application of dry reforming of methane (DRM). Herein, the 10wt%Ni/CeO 2 catalyst was mediated by CeAlO 3 formed by interfacial reaction between impregnated Al species and the CeO 2 support. The resultant CeAlO 3 has a significant influence on the structural properties and the catalytic performance. CeAlO 3 can enhance the dispersion of Ni, introduce more oxygen ion vacancies and medium basic sites, which contribute to the high activity and high coking resistance. Furthermore, the enhanced interaction between Ni and the support impedes the sintering of Ni nanoparticles, leading to improved stability. The sample with Al:Ce molar ratio of 0.1 demonstrates impressive performance, at 800°C and 120,000 mL/(h·g cat ), the CH 4 , CO 2 conversion and H 2 /CO ratio are 94.3%, 90.7%, and 0.92, respectively. The activity decreases by <5% over 200 h test at 750°C with a carbon accumulation rate of only 0.54 mg C/(g cat ·h).
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产品关联
DOI
高影响因子
ADVANCED ENGINEERING MATERIALS
·
2020
·Vol. 22
·期 11
·2000402
·
IF 3.217
Yanpeng Xue,Shuqiang Wang,Yanyan Xue,Lili Cao,Mengyan Nie,Ying Jin
Until now, superhydrophobic materials that are scale-up fabrication and application to harsh environments remain challenging because of their fragile mechanical durability. Because of their unique electronic structure, rare-earth oxides (REOs) have been proven to be intrinsically hydrophobic. Herein, cerium oxide particles (CeO 2 ) are added to the coating by coelectrodeposition. The Co–Ni/CeO 2 composite coating from the electrolyte containing 3.44 g L −1 possesses a flower-like hierarchical structure, displaying a superhydrophobic behavior after the modification by 1H,1H,2H,2H-perfluorooctyltrichlorosilane (PFTEOS). More importantly, excellent mechanical durability with critical abrasion distance of 22.5 m is achieved under a 5 kPa fixed normal pressure in the liner abrasion test before the loss of superhydrophobicity. Also, electrochemical measurements demonstrate that the superhydrophobic composite coatings display high corrosion resistance.
研究领域:
材料科学
·
表面工程
✓ 已验证
DOI
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Zhen Zhang,Minghui Yu,Meiqing Shen,Wei Li,Gurong Shen
Ni-based catalysts, as non-noble metal alternatives, are widely regarded for their potential in ammonia decomposition for hydrogen production. However, their performance at low temperatures is suboptimal, necessitating the addition of promoters and a clear understanding of their mechanisms to enhance catalytic activity. In this study, we have successfully improved the low-temperature ammonia decomposition performance of Ni/CeO 2 by incorporating alkaline earth metals and conducted a comprehensive analysis of the underlying structural and electronic effects. The findings reveal that alkaline earth metals can enhance the basicity of the catalyst and increase electron density around the active metal sites, thereby facilitating the rate-determining step of recombination and desorption of N atom. Moreover, the presence of alkaline earth metals disrupts hydrogen adsorption stability on the catalysts, effectively mitigating the impact of hydrogen inhibition. Based on systematic kinetic experiments, a kinetic model was developed that accurately captures the hydrogen inhibition effect for Ni/CeO 2 catalysts. The insights into the promotional mechanisms of alkaline earth metals offer theoretical guidance for the development of highly active and cost-effective catalysts for ammonia decomposition.
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
ACS Catalysis
·
2026
·
IF 13.6
Wenmin Liao,Siyu Liu,Hui Xie,Jingdong Lin,Shaolong Wan,Shuai Wang
Ethanol steam reforming (ESR) enables renewable biomass-derived H2 production but suffers from selectivity and deactivation challenges. While CeO2-supported metal catalysts are widely explored for ESR owing to strong metal–support interactions and inherent oxygen storage capacity, persistent ambiguities in facet-dependent performance arise from methodological constraints in decoupling intrinsic facet effects from metal particle size variations. By synthesizing morphology-controlled CeO2 supports exposing distinct facets ({100}, {110}, {111}) and anchoring size-uniform Ni nanoparticles (∼2 nm), we decoupled facet contributions to reveal how facet-specific Lewis acidity governs OH* reactivity at Ni–CeO2 interfaces. Combined kinetic assessments, in situ spectroscopy, and density functional theory identify α-C–H abstraction from CH3CH2O* by interfacial OH* as the kinetically relevant step, with acetate intermediates directly formed from CH3CH2O* (not acetaldehyde) facilitating C–C bond scission under steam-rich conditions. Ni supported on {100}-rich CeO2 nanocubes enhances OH* reactivity via weakened Lewis acidity, lowering acetate formation barriers. This facet-modulated interfacial chemistry achieves 426 mmol gcat–1 h–1 H2 formation rate and 72.1% CO2 selectivity at 400 °C, surpassing literature benchmarks under comparable conditions. These findings elucidate how facet-dependent interfacial chemistry dictates ESR performance on Ni/CeO2 catalysts, providing mechanistic insights beyond conventional oxygen storage capacity correlations.
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DOI
高影响因子
Catalysts
·
2018
·Vol. 8
·期 7
·257
·
IF 3.465
Lin Li,Bo Jiang,Dawei Tang,Zhouwei Zheng,Cong Zhao
Chemical looping reforming (CLR) technique is a prospective option for hydrogen production. Improving oxygen mobility and sintering resistance are still the main challenges of the development of high-performance oxygen carriers (OCs) in the CLR process. This paper explores the performance of Ni/CeO2nanorod (NR) as an OC in CLR of ethanol. Various characterization methods such as N2adsorption-desorption, X-ray diffraction (XRD), Raman spectra, transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), H2temperature-programmed reduction (TPR), and H2chemisorption were utilized to study the properties of fresh OCs. The characterization results show the Ni/CeO2-NR possesses high Ni dispersion, abundant oxygen vacancies, and strong metal-support interaction. The performance of prepared OCs was tested in a packed-bed reactor. H2selectivity of 80% was achieved by Ni/CeO2-NR in 10-cycle stability test. The small particle size and abundant oxygen vacancies contributed to the water gas shift reaction, improving the catalytic activity. The covered interfacial Ni atoms closely anchored on the underlying surface oxygen vacancies on the (111) facets of CeO2-NR, enhancing the anti-sintering capability. Moreover, the strong oxygen mobility of CeO2-NR also effectively eliminated surface coke on the Ni particle surface.Keywords:chemical looping reforming;hydrogen;oxygen carrier;CeO2;nanorod
研究领域:
能源科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
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