Journal of CO2 Utilization
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2021
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IF 7.132
Bowen Lu,Yongqing Xu,Zewu Zhang,Fan Wu,Xiaoshan Li,Cong Luo,Liqi Zhang
Cu-based catalysts had been widely used in CO 2 hydrogenation process for their excellent performance and high selectivity. Micron-sized Cu powder obtained by ball milling exhibited poor CO 2 activity for its large particle size and small specific surface area, limited its catalytic application. In this work, micron Cu powder was modified with CeO 2 species synthesized from different cerium precursor salts via a solution auto-combustion method to investigate CO 2 hydrogenation activity. This work revealed that CeO 2 species formed from cerium acetate precursor salt achieved excellent CO 2 performance (1.64 mol/g cat .h at 400 °C), which was 3.8 times and 6000 times higher than that from cerium nitrate salt or cerium chloride salt, respectively. Interestingly, a thick dense CeO 2 shell would be formed on micron Cu generated from cerium(III) chloride precursor salt, which inhibited CuO x reduction and had the opposite effect for RWGS reaction. In addition, the CuO x species in CeO 2 @Cu synthesized from cerium chloride salt resulted in the CH 4 selectivity. The enhancement performance of the CeO 2 @Cu prepared from cerium acetate salt and cerium nitrate salt could be attributed to the oxygen defects formed around the Cu-Ox-Ce interface area and metallic Cu in the RWGS reaction. Cerium precursor salts enhanced the structural integrity of CeO 2 @Cu and played a vital role in RWGS reaction. These results will support a new direction for exploring micron Cu powder in Cu-based catalysts for CO 2 utilization.
研究领域:
化学工程
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材料科学
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催化反应
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产品关联
DOI
高影响因子
DALTON TRANSACTIONS
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2022
·Vol. 51
·期 48
·18562-18571
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IF 4.569
Han Zhao,Longchun Bian,Junchen Du,Yunkun Zhao
The Pd distribution and the CeO2–Al2O3 combination are among the decisive factors for the performance of commercial three-way catalysts. Generally, the sufficient doping of Pd into ceria-based oxides and the intimate interaction between CeO2 and Al2O3 could both benefit the three-way catalytic reactions. However, in the present work, the moderate doping of Pd into CeO2 and less intimate CeO2–Al2O3 interaction were found to be responsible for the much higher catalytic activity (the decrease in T50 was 52, 119, or 55 °C for C3H6, CO, or NO) in PdCe/Al2O3-CP than PdCe/Al2O3-Imp, for which the Pd and Ce species were co-loaded onto Al2O3 through the co-precipitation or impregnation method, respectively. It was intriguing to find that the co-precipitated PdCeOx in PdCe/Al2O3-CP showed less sufficient doping of Pd into CeO2 than the co-impregnated PdCeOx in PdCe/Al2O3-Imp; as a result, both a higher fraction of highly active metallic Pd and a higher Pd dispersion were realized in PdCe/Al2O3-CP. Moreover, due to the less intimate CeO2–Al2O3 interaction, specifically the less severe penetration of the Pd and Ce species into Al2O3, PdCe/Al2O3-CP showed higher Pd dispersion, specific surface area, pore volume and size than PdCe/Al2O3-Imp. The presence of more abundant reactive Pd0, and the higher accessibility of the active Pd and CeO2 sites, together with improved redox properties and enriched oxygen vacancies contributed much to the enhanced three-way catalytic activity of PdCe/Al2O3-CP. Additionally, simultaneously optimizing the Pd distribution and the CeO2–Al2O3 combination in a single step, as reported in this work, is also highly desirable in industry.
研究领域:
化学工程
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催化材料科学
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DOI
PubMed
高影响因子
Catalysis Science & Technology
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2023
·Vol. 13
·期 6
·1855-1865
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IF 5
Shuyi Yang,Jiayi Deng,Jiaying Chen,Qingmei Tan,Tianren Liu,Ke Chen,Dongxue Han,Yingming Ma,Mengjiao Dai,Li Niu
The conversion of N2 and CO2 into urea through a photocatalytic C–N coupling reaction under ambient conditions serves as a novel green avenue for urea synthesis. However, the poor adsorption and C–N coupling capability of inert gas molecules hinder the efficient catalytic activity. Herein, palladium-decorated CeO2 (Pd–CeO2) was demonstrated as an efficient photocatalyst for C–N coupling reaction and delivered a remarkable urea yield rate of 9.2 μmol h−1 g−1, which was superior to that of pristine CeO2 (2.5 μmol h−1 g−1). Comprehensive investigations further endorsed that the emerged space-charge region in the CeO2(111)/Pd(111) interface not only effectively facilitates the targeted capture and activation of inert CO2 and N2 but also stabilizes the formation of key intermediates (*NCON). Besides, the effective inhibition of the endothermic *NNH intermediate is conducive to the subsequent C–N coupling process and the improvement of reaction selectivity. The reaction mechanism was studied in detail by density functional theory (DFT) with the formation of a C–N bond via a thermodynamically spontaneous reaction between *NN* and CO. This work provides novel insights into the conversion of CO2 and N2 into urea.
研究领域:
化学工程
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
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2025
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IF 5.4
Yanjie Hou,Jialing Liu,Guannan Zhang,Zhenyu Xiang,Xinpeng Wu,Jianbo Song,Sijin Li
Reactive oxygen species (ROS) play a crucial role in both physiological and pathological processes within the cardiovascular system. However, an excess of ROS can result in oxidative stress, which may lead to cellular damage, dysfunction, and the promotion of various cardiovascular diseases. How to remove the excess ROS is especially important. Cerium oxide (CeO 2 ), a well-known antioxidant, has the ability to scavenge ROS. However, it is important to improve the antioxidant activity of CeO 2 while avoiding cytotoxicity. In this paper, different nanocomposites have been obtained by compositing different masses of transition metal carbide/carbon-nitride (Ti 3 C 2 T x ) with CeO 2 . In the POD activity assay, COMX-50 shows the best ability to decompose hydrogen peroxide. In subsequent free radical scavenging experiments, COMX-50 scavenges free radicals better than CeO 2 and Ti 3 C 2 T x , which may be attributed to the excellent electron transport ability of Ti 3 C 2 T x to facilitate free radical scavenging. Meanwhile, the POD activity and ROS scavenging ability of COMX-50 exhibit concentration and time dependence. More importantly, COMX-50 can promote the spreading and proliferation of endothelial cells. This provides a new strategy to combat cardiovascular diseases caused by oxidative stress.
研究领域:
生物医学工程
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心血管医学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2020
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IF 5.774
Ruyi Qian,Tongdong Shen,Qiangqiang Yang,Kun-Yi Andrew Lin,Shaoping Tong
Graphite felt (GF) supported cerium oxide (CeO 2 ) composite was prepared by the impregnation method and used to active persulfate (PS) for degradation of isoniazid (INH). The structure and morphology of the catalyst were characterized by X-ray diffraction, X-ray photoelectron spectrum and scanning electron microscope. The effects of some key parameters including initial PS concentration, initial pH value, catalyst dosage, reaction temperature and inorganic ions on INH degradation were investigated in CeO 2 /GF/PS system. It was found that 94.39% of INH and 89.9% of TOC could be removed within 10 min under the controlled conditions (1.2 g/L CeO 2 /GF, 0.25 g/L PS, initial pH at 6.8 and temperature at 25 ℃). The degradation intermediates of INH were identified by liquid chromatography-mass spectrometry and ion chromatography, and the possible degradation pathway was also proposed. The radical competition tests indicated that hydroxyl radical ( OH), sulfate radical (SO 4 − ), superoxide ( O 2 − ) and singlet oxygen ( 1 O 2 ) coexisted in CeO 2 /GF/PS system, in which OH was the predominated one. The recycling experiment showed the CeO 2 /GF was an excellently stable catalyst for activation of PS.
研究领域:
环境科学
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药学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Zhuo Ma,Yihui Li,Zheng Li,Ziyin Liu,Xuepeng Wang,Yuan Tan,Xingkun Chen,Wei Lu,Yunjie Ding
Increasing dimethyl oxalate (DMO) hydrogenation activity remains a challenge. A Cu catalyst was designed by creating Cu nanoparticles (NPs) over SiO 2 layer formed on the CeO 2 particles (SiO 2 @CeO 2 ) using the ammonia evaporation method followed by the calcination and reduction step. The optimized 30Cu/SiO 2 @5CeO 2 catalyst shows good performance in the micro-packed bed reactor (100 % DMO conversion, 95.9 % ethylene glycol (EG) selectivity, 200 h stability) under the condition of the ratio of H 2 to DMO (H 2 /DMO) = 30, 190 °C and 2 MPa in the run, and CeO 2 was proved to be effective in the DMO hydrogenation process. The exposed CeO 2 on the surface of catalyst was found to facilitate the formation of Cu + by its interaction between adjacent Cu nanoparticles, resulting in the faster adsorption and dissociation of C=O bond on the catalyst surface, according to the characterization results obtained by the XRD, XPS and in situ FT-IR, etc.
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
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Yi-Ran Du,Rui Wang,Qing-Shan Niu,Yi-Yu Tao,Bao-Hua Xu
In this study, the bimetallic RuM-CeO 2 (M = Ni, Fe, Cu, K and Cs) catalysts were facilely fabricated by taking the commercially available CeO 2 (99.95 % metals basis, Aladdin, < 50 nm of diameter) as the support. They displayed distinct catalytic performance, especially the chemo-selectivity, on the methoxycarbonylation of styrene with CO and CH 3 OH. Impressively, Ru 2 Ni 0.6 -CeO 2 provided an up to 90.1 % yield of methyl phenylpropionate with satisfied linear selectivity (L/B = 91/9). The characterization and mechanistic results demonstrated that the doping of proper amount of Ni species enriches the local oxygen vacancy (Vö) at the surface but slightly reduces the charge at Ru sites, thereby modulating the interfacial Lewis acid − base pair (Ru-O-Ce-Vö) for catalysis. It thus enhances the CH 3 OH dissociation, leading to high coverage of OCH 3 species with low adsorption energy and relatively weak acidity. Further, the insertion of CO becomes readily due to the weak Ru-CO affinity at electron-deficient Ru center therein. As such, the apparent activation energies ( E a ) of styrene methoxycarbonylation over Ru 2 -CeO 2 (71.2 kJ mol −1 ) is nearly half-reduced by doping Ni element (Ru 2 Ni 0.6 -CeO 2 : 37.5 kJ mol −1 ). Meanwhile, the competitive side reactions at the surface of Ru 2 Ni 0.6 -CeO 2 is inhibited without sufficient acid strength and acid sites. Both aromatic olefins and cyclic olefins were well tolerated under such a system.
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
ACS Applied Nano Materials
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2021
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IF 5.097
Zhi Liu,Jia Zheng,Lianfeng Duan,Zhi Zhu
CO2 photoreduction into high-valued fuels is considered as a promising route to alleviate the clash between the environment and energy. Morphology-dependent CeO2 nanocrystallines with special crystal planes and increased amounts of specific surface areas, structural defects, and active sites have recently demonstrated excellent performance in catalysis. In this article, a biomass-assisted synthesis of CeO2 (BC) photocatalyst is successfully synthesized via a simple yet effective hydrothermal-calcining method by using commercial Ce(NO3)3 as a precursor and leaves of Alternanthera philoxeroides (LAP) as a crystal growth modifier. The amount of LAP introduced into the precursor has a significant effect on regulating the growth of the formed CeO2 from nanocubes to nanorods for the resulting BCs. Owing to the emergence of the just right microenvironment for regulating the growth of the CeO2 nanocrystalline, the optimal sample of BC-15 with a morphology of nanorods is found to be the most efficient one as a photocatalyst for CO2 reduction under visible light. As the major product, the CO yield (126.8 μmol g–1 at a reaction time of 6 h) of BC-15 is ∼7.4-fold of the reference CeO2 nanocubes synthesized without LAP in the precursor. In addition, the underlying evolution process of the nanorods and detailed mechanism insight into the boosted CO2 photoreduction performance are investigated by means of a series of experimental characterizations and results. The present work provides a meaningful protocol to utilize the crystal phase engineering strategy to design morphology dependence of photocatalysts and assisted synthesis with renewable biomass materials for solar-to-fuel conversion.
研究领域:
材料科学
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环境科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2018
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IF 0
Xiaoqing Gao,Shanhui Zhu,Yongwang Li
The mild depolymerization of lignin into aromatic monomer is a grand challenge owing to the various aryl ether C–O bonds, particularly for the most abundant β-O-4, α-O-4 and 4-O-5 linkages. Rod-shaped CeO 2 supported AuPd bimetallic catalysts fabricated by sol-immobilization method presented robust alloy structure, as evidenced by TEM, XPS, UV–vis, and CO-DRIFTS. For the hydrogenolysis of C O bond model compound with formic acid, Au 1 Pd 1 /CeO 2 showed about 23.5 and 6 folds increase in activity compared with its monometallic counterparts Au/CeO 2 and Pd/CeO 2 , respectively. The outstanding performance was mainly ascribed to the increased adsorption ability of electron-deficient Pd for aromatic C–O bond. Additionally, formic acid-mediated Au 1 Pd 1 /CeO 2 has efficiently performed hydrogenolysis of real lignin into a variety of valuable monophenols, achieving 44.1% yield at low temperature.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
JOURNAL OF CATALYSIS
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2021
·
IF 7.92
Zhenhua Zhang,Liping Fan,Weiqi Liao,Feiyue Zhao,Cen Tang,Jing Zhang,Ming Feng,Ji-Qing Lu
Several CeO 2 -CuO/Cu 2 O nanocomposites with different CuO structures were used to identify the structure sensitivity of CuO in the CeO 2 -CuO/Cu 2 O catalyzed CO oxidation. The CO oxidation catalyzed by various CuO-CeO 2 interfacial sites involves a typical Mars-van Krevelen mechanism, in which the CuO-CeO 2 interfaces in the CeO 2 -CuO/c-Cu 2 O (cubes) nanocomposites are more intrinsically active, exhibiting ca. 15 kJ mol −1 lower activation energy than those in the CeO 2 -CuO/o-Cu 2 O (octahedra) and CeO 2 -CuO/d-Cu 2 O (rhombic dodecahedra) nanocomposites at CeO 2 loadings no less than 0.75 wt%. The higher activity is relevant to lower coordinated oxygen ions on CuO/c-Cu 2 O surface and thus better CO reactivity for the CeO 2 -CuO/c-Cu 2 O nanocomposites, which therefore indicates that the active oxygen species on CuO-CeO 2 interface should come from CuO rather than CeO 2 . Moreover, a highly active 13.2 %CeO 2 -CuO/c-Cu 2 O(s) catalyst for CO oxidation is realized on fine Cu 2 O cubes, which thus has high density of active sites.
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
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2023
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IF 4.5
Hao Sun,Boxuan Jin,Shuyi Cao,Jinghan Zhang,Tianhang Li,Xiaojing Liu,Guihua Liu,Jingde Li
Developing low-cost and high-performance electrocatalysts for water splitting is crucial for hydrogen production. In this study, a high-performance hydrogen and oxygen evolution reaction (HER/OER) bifunctional electrocatalyst is developed by introducing oxygen-deficient CeO 2 nanoparticles on (Ni, Co) 2 P nanosheets. The introduction of defective CeO 2 modulates the electronic structure of the CeO 2 @(Ni, Co) 2 P/NF interface, which offers a synergistic effect promoting the HER/OER reaction in the alkaline water splitting process. Specifically, the CeO 2 @(Ni, Co) 2 P/NF electrode exhibits an overpotential of 151 mV for HER and 257 mV for OER at current density of 100 mA·cm −2 . In the overall water electrolysis test, it exhibits excellent stability performance at a cell voltage of 1.70 V around 100 mA·cm −2 . This work shows an alternative strategy for the development of active bifunctional water splitting electrocatalysts.
研究领域:
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
CHEMICAL ENGINEERING JOURNAL
·
2023
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IF 15.1
Yuchuan Ye,Jing Xu,Liangjun Gao,Shaohong Zang,Liqiao Chen,Luhui Wang,Liuye Mo
The impregnation method is one of the most popular methods for preparing various types of supported catalysts. However, the preparation of highly active catalysts by the conventional impregnation method is still a great challenge. In this paper, a modified impregnation method (MI) was developed to prepare CuO/CeO 2 catalysts for the catalytic oxidation of ethyl acetate (EA). It was found that the 5 %CuO/CeO 2 catalyst (5-MI-500) prepared by MI method achieves 100% EA conversion at a low temperature of 200 °C. However, the temperature for 100% EA conversion over the 5 %CuO/CeO 2 catalyst prepared by the conventional method is as high as 300 °C. Notably, the 5-MI-500 catalyst exhibits the highest proportion of well-dispersed CuO and Cu-O-Ce structures, which synergistically enhance catalyst activity. The well-dispersed CuO particles enhance the redox ability of the catalyst, while the Cu-O-Ce structure provides high activated oxygen via oxygen vacancy and better thermal stability during catalytic reaction. Accordingly, the possible reaction mechanism over the 5-MI-500 catalyst for EA oxidation was proposed. This study demonstrates that the MI method reported in this paper can provide a feasible methodology to prepare highly active catalysts with unique structures.
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
DOI
高影响因子
危险品化学品经营许可证（带存储）