Catalysts
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2022
·Vol. 12
·期 6
·606
·
IF 4.501
Yadong Wang,Qing Hu,Ximing Wang,Yanpeng Huang,Yuanhao Wang,Fenghuan Wang
Methane reforming with carbon dioxide (DRM) is one promising way to achieve carbon neutrality and convert methane to syngas for high-value chemical production. Catalyst development with better performance is the key to its potential large-scale industrial application due to its deactivation caused by carbon deposition and metal sintering. Hence, a Ni/CeO2catalyst (Ni/CeO2-M) with higher CO2conversion and better stability is prepared, supported on CeO2precipitated via a novel microimpinging stream reactor. A series of ex-situ or in-situ characterizations, such as CO titration measurements, two-step transient surface reaction (two-step TSR), CO2and CH4temperature-programmed surface reaction (CO2-TPSR and CH4-TPSR), X-ray absorption fine structure (XAFS), and in-situ Raman spectroscopy study, were used to investigate its structure and mechanism. In contrast to Ni supported on commercial CeO2(Ni/CeO2-C), the Ni/CeO2-M catalyst with stronger lattice oxygen mobility and higher oxygen storage capacity enhances its CO2activation ability and carbon deposition. The Ni particle size of the Ni/CeO2-M catalyst decreased, and a higher oxidation state was obtained due to the strong metal–support interaction. Besides the reaction performance improvement of the Ni/CeO2-M catalyst, the novel microimpinging stream reactor could achieve catalyst continuous production with a high preparation efficiency. This work provides a novel method for the high-performance catalyst preparation for DRM reaction and its mechanism study gives a deep insight into high-performance catalyst development via bottom-up study.Keywords:dry reforming of methane;oxygen vacancy;Ni/CeO2catalyst
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
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Shiyu Wu,Xincheng Cao,Peng Liu,Jiaping Zhao,Jianchun Jiang,Junming Xu
The selective hydrogenation of natural oils to produce fatty alcohols is a key process for synthesizing liquid alkanes and high-value chemicals. However, the development of catalysts capable of enhancing hydrodeoxygenation (HDO) selectivity while suppressing carbon–carbon (C–C) bond cleavage to minimize carbon loss remains a significant challenge. In this study, a FeReOx/CeO2 catalyst was developed, which was characterized by high selectivity to octadecanol (93.8%, 210 °C) and liquid alkanes from stearic acid under mild conditions. Notably, the FeReOx/CeO2 catalyst exhibited a higher hydrodeoxygenation selectivity in the production of liquid alkanes than decarboxylation (DCO) (C18: 84.2% vs C17: 15.8% at 240 °C). Detailed characterization of the FeReOx/CeO2 catalyst revealed that excellent catalytic activity originated from the synergistic interaction between Fe and ReOx. The introduction of ReOx not only enhanced the adsorption of stearic acid but also improved the dispersion of metallic Fe. The weak acidity of metallic Fe could inhibit the cleavage of the C–C bond to a certain extent to obtain alkane products with high hydrodeoxygenation selectivity. Furthermore, the catalyst exhibited strong stability without significant deactivation after five cycles.
研究领域:
催化化学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
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2022
·
IF 6.47
Longyi Xue,Ninghan Wei,Cheng Zhao,Xiaomei Hu,Junge Yun,Zimo Chen,Zhiyi Deng,Zhihang Chen
CeO 2 as selective catalytic reduction (SCR) catalyst has attracted wide attention due to its abundant surface acidity and excellent oxygen storage/release capacity. However, its further implication was hindered owing to insufficient catalytic activity and SO 2 resistance. Novel Cr doped CeO x catalysts were synthesized by solid phase method and used for NH 3 -SCR of NO x at middle-low temperature. The effect of Cr addition on the SCR performance and physicochemical properties of CeO 2 catalyst was investigated by activity test and characterizations. Among the tested catalysts, Cr(0.4)-CeO x catalyst exhibited excellent NO x removal efficiency, with >90% NO conversion within 180–300 °C, 100% NO conversion at 220 °C and outstanding SO 2 resistance at 240 °C under 100 or 600 ppm SO 2 . The characterizations results revealed that Cr modified CrCeO x catalyst could effectively increase BET surface area, pore volume, surface acidity and redox capacity. In situ DRIFTS indicated that SCR reactions over Cr(0.4)-CeO x catalyst followed Eley-Rideal mechanism and active –NH 2 was the major intermediate species. After sulfuration, Cr(0.4)-CeO x still exhibited excellent SCR activity due to the increase of Cr 6+ , Ce 3+ and O α concentration and the formation of Cr–O–Ce bond, new Brønsted acid site and more crystallized Cr 2 O 3 .
研究领域:
催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Fuyuan Qi,Weiping Yang,Lan-Lan Lou,Shuangxi Liu,Kai Yu
Oxygen vacancies play an important role in the oxidation of biomass-derived alcohols and aldehydes using ceria-based catalysts. In this study, a highly oxygen vacancy-defective Pt/H-CeO 2 catalyst was synthesized by a straightforward strategy that involved the control of the addition of ascorbic acid and nitric acid. The addition of ascorbic acid, which acted as a pore-forming agent, promoted the hydrolysis, crystallization, and subsequent growth of Ce precursor salt, resulting in the synthesis of H-CeO 2 with abundant oxygen vacancy defects and a porous thin sheet-like morphology. However, the addition of nitric acid significantly inhibited the generation of oxygen vacancy defects. The obtained H-CeO 2 exhibited significantly increased oxygen vacancy content, active oxygen species, and specific surface area compared with CeO 2 with lower oxygen vacancy defects (L-CeO 2 ). These remarkable features led to enhanced catalytic activity of Pt/H-CeO 2 for the oxidation of 5-hydroxymethylfurfural (HMF) compared with Pt/L-CeO 2 . This can be mainly attributed to the enhanced adsorption and activation of O 2 molecules by abundant oxygen vacancies, allowing more active oxygen species to participate in the dehydrogenation of HMF. This work provides an example of oxygen defect engineering for ceria-based catalysts to boost the catalytic selective oxidation performance.
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
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2018
·
IF 4.229
Bin Li,Baohua Zhang,Qingqing Guan,Shanshuai Chen,Ping Ning
An effective Ni/CeO 2 catalyst prepared by the polyol reduction method for degrading phenol into CH 4 , H 2 and CO 2 in supercritical water (SCW) was developed. About 80% carbon gasification efficiency can be achieved at 525 °C and 60 min with 5 wt% phenol, 0.098 kg/m 3 water density and 0.5 g Ni/CeO 2 /g phenol catalyst, forming CH 4 and H 2 as the main gaseous products. Comparison study indicated that the efficiency of present Ni/CeO 2 catalyst was about 20% higher than that of a commercial catalyst, i.e., Ni/SiO 2 Al 2 O 3 from Sigma-Aldrich with 65 wt%Ni, at a reaction conditions of 500 °C and 30 min. The characterization analyses of BET, TPR, XRD , XPS and TEM indicated that there was a NiCe alloy formed in Ni/CeO 2 , which could be important to enhance the activities of the carbon gasification efficiencies and gas yields. A kinetic modelings were conducted and the results showed that the lnA and the activation energy (Ea) of gasification were 7.1 ± 0.5 and 58.1 ± 3.2 kJ/mol for the gaseous product, and were 2.6 ± 0.9 and Ea is 36.6 ± 5.6 kJ/mol for the char formation , respectively. The present Ni-based-metal Ni/CeO 2 catalyst is cheaper and has a potential application for the gasification to convert phenol into gases fuels in SCW process.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Xuqian Wang,Wendan Zheng,Wenhua Tong,Aimin Zhang,Yongkui Zhang,Yabo Wang
Organophosphorus esters (OPEs) are important chemicals functioning as extractants, plasticizers, flame retardants, solvents, additives, etc., and are also recognized as hazardous organic liquids generated from industrial processes. Herein, we developed a CeO2-catalyzed degradation with simultaneous phosphorus immobilization technology to treat typical OPE solvents. Under the investigated reaction conditions of a temperature of 180 °C, a reaction time of 3 h, and a dosage of ball-milled CeO2 of 19.8 g mL–1 of the OPE, the model pollutant of tributyl phosphate (TBP) was efficiently degraded with phosphorus immobilization efficiency near 100%. Meanwhile, the mineralization efficiency of TBP was also as high as 98%, which was reflected by the chemical oxygen demand change of liquid products. Gaseous products generated from CeO2-catalyzed TBP degradation could also fulfill the requirements of an environmental standard. Further mechanism studies indicated that the surface oxygen vacancy in CeO2 induced the in situ formation of superoxide radicals, which dominated TBP degradation. During catalytic degradation, the P-containing species were mainly immobilized as cerium phosphate, while the hydrocarbon chains of TBP were degraded into small molecules and finally mineralized into inorganic species. The developed CeO2-catalyzed OPE degradation approach was also applicable to aromatic and halogenated OPEs, i.e., tricresyl phosphate and tris(2-chloroethyl) phosphate. This study provided a possible alternative for waste treatment of the waste of OPEs with low environmental risks.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2019
·
IF 4.63
Yihu Dai,Xiaofang Chu,Jingjing Gu,Xing Gao,Min Xu,Di Lu,Xiaoyue Wan,Wei Qi,Bingsen Zhang,Yanhui Yang
The CeO 2 -supported ternary RuSnB catalysts were synthesized by incipient wetness impregnation procedures and applied in hydrogenation of cinnamaldehyde in pure water as the solvent. A synergy effect between Ru-based catalysts and water molecules has afforded the efficiently selective transformation of cinnamaldehyde to cinnamyl alcohol with the satisfactory conversion and selectivity. Structural characterization results suggested the incorporation of Ru sites into the SnO x matrix and the electronic interaction between Ru and B additives in RuSnB/CeO 2 catalyst. The isotopic exchange studies have demonstrated that both dissociative activation of H 2 and H 2 O (deuterated D 2 and D 2 O) were apparently affected by the status of Ru sites. Furthermore, the kinetics tests in D 2 O solvent have also revealed the co-existence of water-involved hydrogen-exchange route with the direct hydrogenation route using dissociative H 2 during the hydrogenation reaction. The optimal Ru 2 Sn 1 B 1 /CeO 2 catalyst could afford the best H 2 O-activation capability and thus accelerate the reaction rate in the H 2 O-involved hydrogenation.
研究领域:
催化化学
·
绿色化学
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Shanshan Shao,Xianliang Xiang,Xiaohua Li,Huiyan Zhang,Rui Xiao,Yixi Cai
Acetic acid, n-butyraldehyde, furfural, n-butanol, and ethyl acetate as model compounds of biomass pyrolysis vapors were selected as reactants for ketonization over CeO2. Catalytic conversion of single components was conducted to understand their ketonization characteristics and also to obtain the overlapped temperature range. The results showed that the yield of acetone from directional ketonization of acetic acid reached a maximum of 97.4% at 360 °C over CeO2 with numerous oxygen vacancies, while n-butyraldehyde, n-butanol, and ethyl acetate performed the best at 420 °C with limited yield of ketones of 47.2, 35.1, and 85.4%, respectively. At the overlapped 420 °C, owing to the dehydration of acetic acid molecules, the ketonization of n-butyraldehyde was promoted with the largest overall yield of ketones of 96.5%. A mixture of furfural/acetic acid (1:4) brought about a lower yield of ketones of 78.8%, indicating a negative synergism due to active sites occupation by furfural adsorption.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Jiaxing Hou,Guohao Zou,Xinrui Liu,Mingge Li,Pengyu Yang,Xiaobin Zhang,Yan Chen,Qian Zhang,Xiaoping Wu,Tiejun Wang
The one-step hydrothermal reconstruction of bioethanol into higher alcohols represents a pivotal advancement in green chemistry, addressing both environmental sustainability and energy regeneration. Herein, a rational design of Ni@C-CeO2 catalysts via a sol–gel method for efficient aqueous-phase ethanol C–C coupling was reported. Systematic investigation of Ni loading and precursor carbonization temperature revealed their critical roles in modulating catalyst microstructure and performance. The optimized Ni-2@C-CeO2-500 catalyst demonstrated exceptional activity under 190 °C and 12 h, achieving ethanol conversion of 72.0% and C4+ alcohol yield of 55.6%. Advanced characterization techniques unveiled structure-performance relationships: (1) controlled Ni loading ensured optimal nanoparticle dispersion, while excessive loading induced aggregation; (2) carbonization at 500 °C balanced carbon matrix architecture and CeO2 reducibility. XPS analysis revealed that oxygen vacancy concentration critically modulates strong metal–support interactions through Ce3+-induced charge redistribution, facilitating interfacial electron transfer during reaction. Furthermore, the Ni-2@C-CeO2-500 catalyst demonstrated excellent stability with sustained activity retention over five consecutive cycles. This work establishes a renewable and technologically viable alternative to conventional petroleum-derived chemicals widely utilized in the chemical industry, demonstrating significant potential for applications in green and sustainable chemistry.
研究领域:
绿色化学
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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
CATALYSIS LETTERS
·
2019
·Vol. 149
·期 4
·1007-1016
·
IF 2.372
Liu Pengcheng,Niu Ruyue,Li Wei,Wang Shuang,Li Jinping
Three Ru/CeO 2 catalysts with different morphologies of CeO 2 (cube spheres, microspheres and nano rods) were used to evaluate the support-morphology-dependent ammonia synthesis activity. Catalytic experiments show that the Ru/CeO 2 –CS catalyst has higher catalytic activity (27,000 µmol g −1 h −1 ) than Ru/CeO 2 –MS (21,000 µmol g −1 h −1 ) and Ru/CeO 2 –NR (15,000 µmol g −1 h −1 ) under the reaction conditions of 450 °C, 3 MPa, H 2 /N 2 = 3:1 (60 mL min −1 ). The transmission electron microscopy analysis showed that the dispersion of active metal Ru is affected by the morphology of CeO 2 . Brunauer–Emmett–Teller indicates that the 3–5 nm the pore size of CeO 2 supports contributes to the active metal Ru enters the pores of the CeO 2 support, which improves the dispersion of Ru and prevents the sintering and agglomeration of Ru in some extent. TPR studies shown that the reduction of ruthenium oxide is influenced by the morphology of CeO 2 . XPS and CO 2 -TPD demonstrated that the Ru/CeO 2 –CS catalyst exhibited higher surface oxygen vacancies, higher basic site density and lower Ru binding energy, indicating that Ru nanoparticles in Ru/CeO 2 –CS is more electron-rich and are more capable of back-donating electrons to adsorbed N 2 and subsequently activate N 2 . Our results indicate that the morphology effect of the CeO 2 supports on the Ru/CeO 2 catalyst is related to the pore size distribution and the surface oxygen vacancies of the CeO 2 supports, ratio of Ru n+ , basic site density. Graphical Abstract
The CeO 2 –CS (cube spheres) morphology facilitated the dispersion of the active metal Ru and the 3 nm the pore size of CeO 2 –CS contributed to the Ru enters the pores of the support. And the Ru/CeO 2 –CS catalyst exhibited higher surface oxygen vacancies and lower Ru binding energy, which enhanced the adsorption of hydrogen and nitrogen species and thus weakened the N≡N bond.
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
Scientific Reports
·
2019
·Vol. 9
·期 1
·1-14
·
IF 4.011
Dong Fang,Meng Yu,Han Weiliang,Zhao Haijun,Tang Zhicheng
Here, we synthesized a series of Cu/CeO 2 catalysts with different morphology and size, including Cu/CeO 2 nanospheres (Cu/CeO 2 -S), Cu/CeO 2 nanoparticles (Cu/CeO 2 -P), Cu/CeO 2 nanorods (Cu/CeO 2 -R) and flower-like Cu/CeO 2 microspheres (Cu/CeO 2 -F) to systematically explore the structure-activity relationship in CO oxidation. Crucially, the effect of morphology, crystal size, Ce 4+ /Ce 3+ species, oxygen vacancies derived from the removal of lattice oxygen (O latt ) species in CeO 2 and lattice defect sites on CO activity was revealed through various characterizations. It was clearly discovered that the activity of these catalysts was as follows: Cu/CeO 2 -R > Cu/CeO 2 -P > Cu/CeO 2 -S > Cu/CeO 2 -F, and the Cu/CeO 2 -R catalyst preferentially showed the best catalytic performance with a 90% conversion of CO even at 58 °C, owned the smaller particles size of CeO 2 and CuO, and exhibited the higher concentration of O latt species and oxygen vacancies. Besides, it is also verified that the Cu/CeO 2 -F sample exhibited the larger CeO 2 crystal size (17.14 nm), which led to the lower Cu dispersion and CO conversion, even at 121 °C (T 90 ). Most importantly, we discovered that the amount of surface lattice defect sites was positively related to the reaction rate of CO. Simultaneously, DFT calculation also demonstrated that the introduced oxygen vacancies in CeO 2 could accelerate the oxidation of CO by the alteration of CO adsorption energy. Therefore, the morphology, the crystal size, the content of oxygen vacancies, as well as lattice defects of Cu/CeO 2 catalyst might work together for CO oxidation reaction.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Long Xie,Bin Hu,Riyang Shu,Zhipeng Tian,Ying Chen,Chao Wang
Methanol reforming has been a popular pathway to produce hydrogen due to the high hydrogen storage density of methanol. CeO 2 as the support is widely used for catalytic methanol reforming, but the effect of CeO 2 morphology on the reaction mechanism has not been revealed out. In this study, the catalytic performances of Ru/CeO 2 with different CeO 2 morphology, including rod , cubic and their mixed, were investigated in methanol reforming for the production of hydrogen. By regulating the temperature during hydrothermal preparation, different CeO 2 supports can be achieved. Results showed that Ru/CeO 2 catalyst with rod CeO 2 (Ru/r-CeO 2 ) exhibited a much better catalytic performance than the cubic catalyst (Ru/c-CeO 2 ) and the mixed catalyst (Ru/m-CeO 2 ), with a higher yield of hydrogen and a lower selectivity of CO product. This was mainly due to the large surface area that favored the dispersion of Ru metal site and the interaction between Ru and CeO 2 support that improved the electron transfer to benefit the formation of oxygen vacancy . Therefore, the Ru/r-CeO 2 catalyst possessed abundant oxygen vacancy , which enabled to adsorb the methanol efficiently and trigger the methanol reforming reaction . It also can enhance the adsorption of CO and water and promote the water-gas-shift reaction to increase the yield of hydrogen production .
研究领域:
催化化学
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能源科学
✓ 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）