Catalysis Science & Technology
·
2016
·Vol. 7
·期 1
·191-199
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IF 5.287
Zhanwei Ma,Shengli Zhao,Xiaoping Pei,Xumao Xiong,Bin Hu
Three ceria nanocrystals with different morphologies (nanocubes, nanorods, and nanoparticles) were synthesized and used as supports to evaluate the support morphology-dependent ammonia synthesis activity in the structure-sensitive ammonia synthesis reaction. The Ru/r-CeO2 catalyst shows a higher catalytic reaction rate (3830 μmol g−1 h) than that of Ru/c-CeO2 (1289 μmol g−1 h) and Ru/p-CeO2 (529 μmol g−1 h) under the reaction conditions of 400 °C, 1 MPa, and 60 mL min−1. In addition, promoters (Cs, K, and Ba) can effectively enhance the catalytic activity of the catalysts such as 2Cs–Ru/r-CeO2 (14 266 μmol g−1 h) and 2K–Ru/r-CeO2 (11 227 μmol g−1 h). The effect of the morphology of the CeO2 support on the metal–support interaction and catalytic performance of the Ru/CeO2 catalysts can be correlated to the exposed crystal planes and surface composition/electronic structure of the CeO2 support with diverse morphologies.
研究领域:
催化化学
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材料科学
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表面科学
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化学工程
·
无机化学
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DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2026
·
IF 17.2
Chengyang Sun,Haochen Zhang,Xiaohui Liu,Yanqin Wang
Catalytic hydrogenolysis offers a promising route for plastic waste upcycling. Herein, we demonstrate that oxygen vacancies (O V ) in CeO 2 supports dramatically enhanced this process. Reduction-engineered Ru/CeO 2 -NH 3 -800 exhibits 40% higher activity at 800 °C than untreated counterparts. Comprehensive characterization revealed unchanged Ru metal sites after treatment, but significantly increased oxygen vacancy content in the CeO 2 support. Isotopic C 6 –D 2 temperature-programmed surface reaction studies revealed that higher O V concentrations correlate with lower C–H bond activation temperatures, directly aligning with observed activity trends. We propose a novel Ru–Ce interfacial mechanism: O V -adjacent Ce 3+ –O sites activate C–H bonds to form *RCCR* intermediates, while dual Ru sites cleave C–C bonds via C–Ru coordination. This work establishes an O V -driven structure-activity relationship for the first time and reveals support-mediated C–H activation as crucial for advanced catalyst design.
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Catalysis Science & Technology
·
2020
·Vol. 11
·期 5
·1914-1921
·
IF 5.721
Xiaoxiao Qin,Xueyan Chen,Min Chen,Jianghao Zhang,Hong He,Changbin Zhang
Formaldehyde (HCHO) elimination at low temperature is of great interest for indoor air purification. In this work, 1 wt% Ru supported on CeO2 and Al2O3 catalysts were prepared by an impregnation method and subsequently tested for the catalytic oxidation of HCHO at low temperature. The activity of the Ru/CeO2 catalyst was significantly superior to the Ru/Al2O3 catalyst, achieving complete conversion of 130 ppm HCHO at 90 °C with a GHSV of 100 000 mL gcat−1 h−1. Brunauer–Emmett–Teller (BET) measurements, X-ray powder diffraction (XRD), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray photoelectron spectroscopy (XPS) and H2-temperature-programmed reduction (H2-TPR) were carried out to characterize the physical and chemical properties of the catalysts. The results revealed that RuOx species, rather than Ru0, were directly responsible for the HCHO oxidation over Ru/CeO2, and the excellent performance of Ru/CeO2 was mainly attributed to the strong interaction between Ru and CeO2, which induced a high dispersion and high redox capacity of RuOx species. The reaction mechanism of HCHO oxidation was also investigated using in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS). It was shown that the HCHO oxidation over the Ru/CeO2 and Ru/Al2O3 catalysts followed the same pathway of the direct formate oxidation (HCHO → HCOO + OH → H2O + CO2).
研究领域:
环境科学
·
催化化学
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Riyang Shu,Haozhe Huang,Bin Hu,Long Xie,Xintong Chen,Zhipeng Tian,Chao Wang,Jingtao Zhang,Sheng Yang,Xianglong Luo,Ying Chen
Methanol steam reforming is a popular technology for hydrogen production, but it usually suffers from the methanation side reaction and low hydrogen yield. Herein, a novel K-doped Ru/CeO2 catalyst was proposed to suppress methanation and enhance hydrogen production. The Ru-5K/CeO2 catalyst doped with 5 wt % K achieves 100% methanol conversion, a 0.578 mol·g–1·h–1 hydrogen production rate, and 66.4% hydrogen selectivity at 450 °C, with only 3.6% CH4, which is much better than other Ru–K/CeO2 catalysts. Under the same conditions, Ru/CeO2 and Ru-10K/CeO2 only achieve 0.268 mol·g–1·h–1 and 0.224 mol·g–1·h–1 hydrogen production rates, 64.1% and 64.5% hydrogen selectivity, respectively. The promotion effect and mechanism of K doping on the methanation suppression of Ru/CeO2 catalysts in the methanol steam reforming process were investigated in detail. Characterization and experimental results show that suitable K doping in the Ru/CeO2 catalyst enhances the metal–carrier interactions and induces the formation of abundant oxygen vacancies at the same time. And the hydrogen atom dissociation and water–gas shift reactions on the catalyst surface are promoted significantly. Additionally, in situ DRIFTS characterization presents that the Ru-5K/CeO2 catalyst dominates the formation of the bridged carbonyl (Ru-CO-K) intermediate. This inhibits methane formation due to the interaction between Ru and K, and strengthens the connection of CO generated by methanol decomposition. The increase in K leads to the formation of abundant oxygen vacancies in CeO2, which promotes the dissociation of water to form hydroxyl groups and hydrogen and facilitates the water–gas shift reaction. The conversion of bridged carbonyl groups to CO2 and H2 is also accelerated, and methane formation through this dual regulatory mechanism is thus inhibited. This work offers fresh perspectives and a useful reference for hydrogen production, contributing to the ongoing discussion on the role of alkali metals in promoting methanol steam reforming.
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Yin Liu,Liang Shuai,Lei Cao,Qian Zhu,Lanlan Fan,Liang Xu,Shixian Xiong
The widespread use of carbendazim (CBZ) fungicide calls for monitoring its toxic residues in food due to human health concerns. Herein, a Ru/CeO 2-x heterostructured composite was constructed by sodium borohydride reduction for the electrochemical sensing of CBZ. The rational design engineers abundant interfacial oxygen vacancies and Ru nanoclusters, which form interfacial Lewis acid-base pairs capable of dual-site recognition of CBZ molecules. Specifically, oxygen-vacancy Lewis acidic sites preferentially adsorb the electron-rich groups(such as lone pairs on amino groups), while Ru-based Lewis basic sites capture electron-deficient carbon atoms within the benzimidazole ring. Such synergistic adsorption and interfacial charge transfer markedly enhance the redox kinetics of CBZ. Consequently, the Ru/CeO 2-x /GCE sensor delivers an ultralow detection limit of 7.7 nM, along with excellent selectivity, reproducibility, and long-term stability. This work provides a new interfacial engineering strategy integrating oxygen-defect chemistry and electronic modulation for designing high-performance Lewis acid–base coupled sensing materials.
研究领域:
环境监测
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电分析化学
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纳米材料
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传感材料
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食品安全
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Yiwen Zou,Lin Dong,Siyang Yan,Jiaxu Liu,Lili Mu,Licheng Li,Yue Hu,Haifeng Qi,Shanjun Mao,Zupeng Chen
Efficient and selective N -alkylation of amines with alcohols via transfer hydrogenation is of great significance but extremely challenging. Here, we report the production of N –benzylaniline (BZA) from benzyl alcohol and aniline over various fine-shaped Ru/CeO 2 catalysts. The Ru/CeO 2 –R (rod) catalyst exhibits the highest catalytic activity among all catalysts, in which the yield of BZA reaches up to 88% with complete conversion, significantly higher than that of Ru/CeO 2 -C (cube, 52%) and Ru/CeO 2 -O (octahedron, 32%). Extensive experimental investigations disclose that Ru nanoparticles with a metallic state promote the dehydrogenation of the hydroxyl group and hydrogenation of imines, while the CeO 2 –R with rich oxygen vacancies facilitates the adsorption and activation of reactants. Furthermore, kinetic studies and time-resolved operando dual-beam Fourier transform infrared spectroscopy analysis confirms the transfer hydrogenation pathway, in which the benzyl alcohol is firstly dehydrogenated to benzaldehyde, followed by spontaneously reacting with aniline, and finally transforms into the N -benzylaniline rapidly.
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DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2024
·
IF 7.2
Yucan He,Dongsen Mao,Qiangsheng Guo,Jun Yu
A series of highly ordered microporous Ce-based metal-organic frameworks (MOFs) were synthesized as the precursors for catalyst construction. The corresponding Ru catalysts were prepared by Ru impregnation on the derived CeO 2 by pyrolysis of Ce-MOF, and investigated for the CH 4 synthesis via CO 2 hydrogenation. Among the catalysts, Ru catalyst supported on the CeO 2 -B derived from Ce-BDC exhibited a highly competitive efficiency for CO 2 methanation, giving a CH 4 selectivity of 100% with a CO 2 conversion of 62% at 275 °C and 0.1 MPa, and the CH 4 productivity reached 0.49 mol/(mol Ru ·h). Characterization results revealed that more oxygen vacancies and corresponding surface oxygen species formed on the surface of CeO 2 -B derived from Ce-BDC caused to the stronger interaction between Ru and CeO 2 -B, which promoted the CO 2 adsorption and hydrogenation capacity of the catalyst, resulting in its better catalytic property. In situ diffuse reflectance infrared Fourier transform (DRIFT) studies further revealed that the route of HCOO* into CH 4 is a more competitive way of CO 2 hydrogenation to CH 4 .
研究领域:
化学工程
·
催化材料
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yu-Xuan Fu,Shu-Yi Huang,Ming-Shuai Sun,Yan Zhou,Dan-Dan Cai,Wen-Shuai Zhu,Wei Hui,Duan-Jian Tao
Current industrial catalysts for α-pinene hydrogenation suffer from harsh reaction conditions and poor selectivity to cis -pinane, primarily due to their inability to effectively adsorb α-pinene in a specific favorable configuration on the catalyst surface. In this study, a high-specific-surface-area, rod-shaped CeO 2 -supported ultra-fine Ru nanoparticle (average particle size of 4 nm) catalyst was synthesized via hydrothermal method for the highly stereoselective hydrogenation of α-pinene to cis -pinane. The resulting Ru/CeO 2 -H catalyst achieved an α-pinene conversion of 99.3 % and an impressive cis -pinane selectivity of up to 99.6 % under exceptionally low temperature (30°C), 0.6 MPa H 2 and 0.5 h with high TOF (1236 h −1 ). Density functional theory (DFT) calculations indicated that α-pinene preferentially adsorbs onto the Ru surface via the backside of its intramolecular dimethyl bridge. This particular adsorption mode lowers the energy barriers for further hydrogenation to generate cis -pinane. The oriented dimethyl-up configuration of α-pinene and ultra-low activation energy (12.04 kJ/mol obtained from kinetic tests) enable the highly selective production of cis -pinane at ambient temperature. Furthermore, the strong interaction between the CeO 2 -H support and highly dispersed Ru, combined with the ambient-temperature reaction conditions, effectively prevents metal nanoparticle agglomeration and coking, imparting the catalyst with exceptional stability. Notably, the catalyst was reused at least 15 times without observing any significant deactivation, demonstrating its significant potential for practical applications.
研究领域:
催化化学
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材料科学
·
理论化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Wanchao Gong,Jinhao Li,Qing Yi,Gongde Wu,Gongjin Yang,Changlong Zheng,Xiaodong Wu,Jie Wan,Shuang Liu
Ru/CeO 2 recipes have gained increasing attention as cost-effective catalysts for soot combustion under the NO x -free and oxygen-lean conditions characteristic of gasoline particulate filters (GPFs). Nevertheless, the intrinsic heterogeneity of Ru-based species in these catalytic systems has not been adequately addressed, resulting in ambiguous structure-activity correlations and an incomplete mechanistic picture. In this study, we aim to bridge this gap by systematically investigating a model Ru/CeO 2 catalyst (∼1 wt% Ru) supported on nanocube-shaped CeO 2 . Combining kinetic analysis, transient oxygen cutoff experiments, and spectroscopic characterization, we identified two distinct types of Ru-based active entities: sub-nanometer RuO x clusters strongly interacting with the support and larger RuO 2 nanoparticles. Although both species contributed to soot combustion, the nanoparticles underwent irreversible reduction under oxygen-lean atmospheres, whereas the RuO x clusters maintained redox stability via dynamic oxygen exchange with the CeO 2 support. These findings underscore the essential role of recognizing and regulating metal species heterogeneity in catalyst design, laying a foundation for the development of more efficient and durable Ru/CeO 2 catalysts for automotive emission control.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2026
·
IF 9.2
Wujian Zhang,Jinghua Liu,Haodong Zhao,Jian Guan,Zhenxiang Li,Keyi Mou,Yuchen Chen,Zongjian Liu,Ying Li,Aimin Chen,Haodong Tang
Synergistic air-calcination and CO-reduction tailor the interfacial structure of Ru/CeO 2 catalysts. • Abundant Ru n+ –O V –Ce 3+ interfaces enhance low-temperature WGS performance. • Ru n + sites moderate CO adsorption and oxygen vacancies facilitate water dissociation. The catalytic efficiency of Ru/CeO 2 in the water–gas shift (WGS) reaction is frequently limited by its insufficient capacity to activate water molecules, which substantially impairs low-temperature performance. In this study, an interfacial engineering strategy combining air calcination with CO reduction is developed to construct a Ru/CeO 2 -R catalyst enriched with Ru n+ –O V –Ce 3+ interfacial structures. This specially designed interface significantly enhances the activity of low-temperature WGS. Advanced characterization techniques, including XPS, TEM, Raman spectroscopy, and in situ DRIFTS, demonstrate that Ru n + species reduce excessive CO adsorption, thereby enhancing reaction selectivity. Meanwhile, oxygen vacancies facilitate water dissociation and increase the reaction rate. Consequently, the Ru/CeO 2 -R catalyst achieves an impressive CO conversion rate of 9.56 mol CO ·g Ru −1 h −1 at 200 °C. This research introduces a straightforward and controllable method for tailoring interfacial electronic structures, offering valuable insights for the rational design of highly efficient catalysts for low-temperature WGS. Download: Download high-res image (237KB) Download: Download full-size image
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高影响因子
ACS Catalysis
·
2024
·
IF 11.3
Pengfei Liu,Changlong Zheng,Wei Liu,Xiaodong Wu,Shuang Liu
Controlling the oxidative redispersion behavior of supported metal nanoparticles is of central importance in producing high-performance catalysts applied under industry-related oxidation conditions. So far, considerable efforts have been paid to understanding reactant (including O2)-induced disintegration, while much less is known about the influences of support defects like hydroxyl (OH) and oxygen vacancy (VO) on the stabilization of metal–reactant complexes. In this article, by using H2 as a reducing agent, the roles of OH groups and VO in oxidative redispersion of Ru over CeO2 nanorods were distinguished and further disentangled by comparison with the cases of CO-pretreated Ru/CeO2. Supported by electron microscopy, in situ diffuse reflectance infrared Fourier transform spectroscopy, in situ X-ray photoelectron spectroscopy, Raman, and other characterizations, we showed that the doubly bridging OH (II) groups on CeO2(111) steps (type II or III) played major roles in stabilizing Ru–Ox complexes and producing atomically dispersed Ru species, while the surface VO sites assisted dehydrogenation and prevented OH overcapping on the reactive Ru sites. The propylene combustion activity of the thus-obtained single-site Ru/CeO2 was far superior to that of a benchmark Pt/Al2O3 catalyst. The results suggested that well-designed H2 treatments could be used to maximize the effectiveness of (reactant-induced) metal redispersion over CeO2, and attention should be paid on possible metal redispersion when dealing with catalysis over systems accessible to reactants (e.g., hydrogen, water, and/or hydrocarbons) that give rise to CeO2 surface hydroxyls in working conditions.
研究领域:
催化化学
·
材料化学
·
表面科学
·
纳米材料
·
环境催化
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DOI
高影响因子
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