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DALTON TRANSACTIONS · 2024 · IF 3.5

Revealing the intrinsic nature of Cu- and Ce-doped Mn3O4 catalysts with positive and negative effects on CO oxidation using operando DRIFTS-MS

Zihao Hu,Xiaoying Zhou,Tiantian Zhang,Zuliang Wu,Jing Li,Wei Wang,Erhao Gao,Jiali Zhu,Shuiliang Yao

Aiming at the problem of the poor performance of an Mn-MOF-74-derived Mn3O4 catalyst in low-temperature carbon monoxide (CO) oxidation, copper (Cu) and cerium (Ce) elements were used to modify the Mn3O4 catalyst to improve its performance in low-temperature CO oxidation. According to the results of catalytic performance testing, the CO oxidation activity of the Cu0.3Mn2.7O4 catalyst was significantly improved compared with that of the pristine Mn3O4 catalyst, when a CO conversion rate of 90% was achieved at 118 °C. According to X-ray photoelectron spectroscopy and Brunauer–Emmett–Teller analyses, the (Mn2+ + Mn3+)/(Mn2+ + Mn3+ + Mn4+) ratio and the Oads/Ototal ratio increased after Cu doping, indicating promoted oxygen vacancy generation. In addition, the increased specific surface area was beneficial for the adsorption of reactant molecules and the exposure of active sites. According to H2-temperature-programmed reduction characterization, Cu doping significantly enhanced the performance of the Cu0.3Mn2.7O4 catalyst during low-temperature redox. Finally, these factors synergistically promoted the degradation of CO over the Cu0.3Mn2.7O4 catalyst. In addition, operando diffuse reflectance Fourier transform infrared spectroscopy results suggested the presence of more terminal-type oxygen, which is essential for the catalytic oxidation of CO on the surface of the Cu0.3Mn2.7O4 catalyst. Moreover, the Cu0.3Mn2.7O4 catalyst also showed excellent resistance to carbonate, and remarkable stability.

研究领域: 催化化学 · 材料科学
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Royal Society Open Science · 2018 ·Vol. 5 ·期 6 · IF 2.504

Cerium promoted V-g-C3N4 as highly efficient heterogeneous catalysts for the direct benzene hydroxylation

Cheng Wang,Liya Hu,Meiyin Wang,Bin Yue,Heyong He

A series of Cex-V-g-C3N4 catalysts with different cerium content were synthesized by a facile co-assembly method. Compared with pure V-g-C3N4 catalyst, the addition of cerium facilitated the high dispersion of vanadium species as well as the benzene adsorption ability of the corresponding catalysts. Also, the existence of cerium promoted the partial reduction of vanadium species, which improved the redox property of vanadium species as the active centres. The Cex-V-g-C3N4 catalysts showed considerably improved activity in the benzene hydroxylation reaction compared with V-g-C3N4 catalyst. Among the catalysts studied, Ce0.07-0.07 V-g-C3N4 exhibited the best catalytic activity with a benzene conversion of 33.7% and a phenol yield of 32.3% with good structural and catalytic stability, while only 24.7% of benzene conversion and phenol yield of 24.2% were obtained over 0.07 V-g-C3N4.

研究领域: 化学工程 · 催化材料科学
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INORGANIC CHEMISTRY · 2023 · IF 4.6

Strengthening the Stability of the Reconstructed NiOOH Phase for 5-Hydroxymethylfurfural Oxidation

Yifei Huang,Xuliang Pang,Jianguo Cui,Zhenzhen Huang,Guanhua Wang,Huaiquan Zhao,Hongye Bai,Weiqiang Fan

Electrochemical oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) is a promising approach to produce high-value chemicals such as 2,5-furandicarboxylic acid (FDCA). However, the undesirable stability of catalysts commonly limits its potential application value. In this work, NiOOH derived from Ni(OH)2 was determined as the main catalytic site for HMF oxidation, but the collapse of Ni(OH)2 caused severe instability during the electrocatalytic process because of the crystal structure mismatch between NiOOH and Ni(OH)2. The implantation of Ce in Ni(OH)2 (Ce-Ni(OH)2) was successfully realized to address the stability issue of bare Ni(OH)2, since the larger ion radius of Ce could increase the Ni–O bond length and d-spacing. As a result, the activity of 14%Ce-Ni(OH)2 has not obviously decayed after the 50 cyclic voltammetry (CV)-cycle test. HMF conversion is close to 100%, and the Faraday efficiency (FE) reaches 86.6% at the potential of 0.45 V vs Ag/AgCl. This study provides a new strategy to design stable catalysts for the conversion of biomass derivatives.

CAS / MDL: 10294-41-4
研究领域: 电化学 · 催化材料 · 生物质转化
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ACS Applied Nano Materials · 2024 · IF 5.3

Enhanced Phosphate Adsorption by Cerium-Doped Porous Boron Nitride Nanosheets

Yaxin Gu,Yi Fang,Huayi Cai,Shaobo Yang,Song Yan,Chaochao Cao,Chengchun Tang

Porous boron nitride material (p-BN), as a nanomaterial, is often used in pollutant removal (antibiotics and heavy metal ions in water, etc.), but its effectiveness for the removal of anionic pollutants has rarely been reported. Here, a cerium oxide modified p-BN (Ce/p-BN-X) was prepared and used for phosphate removal. It has a high specific surface area, a rich pore structure, abundant reactive groups such as amino groups, positively charged oxygen vacancies, and high stability, which enhanced the adsorption of phosphate. Moreover, the adsorption kinetics and isotherms analysis revealed that the adsorption capacity of Ce/p-BN-4 was 22.05 times higher than that of p-BN at an initial concentration of 20 mg L–1. The adsorption mechanism mainly includes ion exchange, inner-sphere complexation, and electrostatic attraction. In summary, this work provides a simple strategy to improve the adsorption of p-BN on phosphate, which greatly compensates for the deficiency of p-BN in anion adsorption and has great potential for application.

CAS / MDL: 7778-77-0
研究领域: 环境科学 · 材料科学
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Journal of Materials Chemistry A · 2022 ·Vol. 10 ·期 38 ·20350-20364 · IF 14.511

The facilitated cathodic elementary reactions of solid oxide electrolysis cells for CO2 conversion over a Ce decorated La0.43Ca0.37Ti0.94Ni0.06O3−δ electrocatalyst

Zhishan Li,Meilan Peng,Yinlong Zhu,Zhiwei Hu,Chih-Wen Pao,Yu-Chung Chang,Yifan Zhang,Yingru Zhao,Jianhui Li,Yifei Sun

A high temperature solid oxide electrolysis cell is recognized as a promising technology for CO2 conversion (CO2-SOEC). The development of alternative cathode materials substituting conventional Ni/YSZ is a great challenge for SOECs, on which multi-step elementary reactions (e.g., adsorption of CO2, conversion of reaction intermediates, and desorption of CO) occur in succession. Herein, the Ce decorated La0.43Ca0.37Ti0.94Ni0.06O3−δ perovskite (denoted as LCTNi-Ce) is synthesized and applied as a potential cathode electrocatalyst for a CO2-SOEC. The in situ exsolution strategy and A-site deficiency enable the surface decoration of plenty of Ni nanoparticles (NPs) serving as efficient reactive sites. Furthermore, the Ce decoration leads to increased oxygen vacancy concentration, accelerated oxygen exchange rate and improved CO desorption capacity. The symmetrical half-cell measurement confirmed the boosted electrolysis performance in both CO2/CO and CO2/H2 atmospheres. DRT analysis further evidences the facilitated oxygen ion transportation and gas adsorption/dissociation upon Ce decoration. Compared to a LCTNi cell, the LCTNi-Ce cell exhibits a significantly promoted current density of −0.557 A cm−2 in 50% CO2/50% H2 at 800 °C and 1.3 V, and a reduced Rp value of 0.514 Ω cm−2 under OCV condition.

研究领域: 材料科学 · 化学工程 · 能源技术
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Applied Sciences-Basel · 2021 ·Vol. 11 ·期 5 ·2018 · IF 2.679

Ultra-Deep Oxidative Desulfurization of Fuel with H2O2 Catalyzed by Mesoporous Silica-Supported Molybdenum Oxide Modified by Ce

Yang Chen,Qi Tian,Yongsheng Tian,Jiawei Cui,Guanghui Wang

A mesoporous silica-supported molybdenum oxide catalyst with a cerium(Ce) modifier was prepared by in situ synthesis and used in a hydrogen peroxide (H2O2) system for the desulfurization of dibenzothiophene (DBT), benzothiophene (BT), and 4,6-dimethyldibenzothiophene (4,6-DMDBT) fuel oils. The catalytic performance of the catalyst was studied. The catalyst was characterized by Fourier Transform Infra-Red (FT-IR), X-ray diffraction (XRD), Brunner−Emmet−Teller (BET), and X-ray Photoelectron Spectroscopy (XPS). The influences ofm(catalyst)/m(fuel oil),v(H2O2)/v(fuel oil), reaction temperature, and reaction time were investigated. The catalyst had excellent catalytic oxidation desulfurization performance under moderate operational conditions. The catalytic performance was in the order DBT > 4,6-DMDBT > BT. The kinetic analysis results showed that the reaction was a pseudo first-order kinetics process and the apparent activation energies of DBT, BT, and 4,6-DMDBT were 46.67 kJ/mol, 56.23 kJ/mol, and 55.54 kJ/mol, respectively. The reaction products of DBT, BT, and 4,6-DMDBT were DBTO2, BTO2, and 4,6-DMDBTO2, respectively. The recycling experiments indicated that DBT, BT, and 4,6-DMDBT removal could still reach levels of 94.0%, 63.0%, and 77.9% after five cycles.

研究领域: 化学工程 · 环境科学
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Journal of Environmental Chemical Engineering · 2023 · IF 7.7

Study on CO-SCR performance of Ce modified OMS-2 catalysts

Chen Cai,Jiayin Chen,Wei Fu,Shuying Ning,Hao Zhou,Muhammad Kashif,Yaxin Su

The Ce-modified OMS-2 catalyst (Ce x -OMS-2) was synthesized by the hydrothermal synthesis method, after which its catalytic efficacy in the selective reduction of NO by CO was assessed. The experiments showed that Ce 0.08 -OMS-2 was capable of 100% NO conversion between 175 and 300 °C when 0.05%NO, 0.1%CO, 5%O 2 and N 2 were used as equilibrium gases, and the N 2 selectivity peaked at 93.2% at 175 °C. Additionally, Ce 0.08 -OMS-2 exhibits good sulfur resistance in the presence of 0.02% SO 2 and maintains more than 88% NO conversion at 175–275 °C. By using BET, XPS, H 2 -TPR, NH 3 -TPD, and In situ DRIFTS to characterize the catalysts, the effects of doping the active metal Ce on the physicochemical characteristics of OMS-2 catalysts were under investigation. In conclusion, the improvement of the low-temperature activity of the Ce x -OMS-2 catalyst is facilitated by lower agglomeration and crystallinity , larger specific surface area, smaller average pore size, enhanced surface oxygen vacancies, increased Mn 4+ concentration, and richer Brønsted acid. Reaction gas adsorbed species and intermediates on the catalyst surface were dynamically captured during In situ DRIFTS experiments. The CO-SCR reaction of the catalyst was found to follow the E-R mechanism below 200 ℃ and the L-H mechanism at 200–350 ℃.

研究领域: 环境科学 · 催化化学
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NEW JOURNAL OF CHEMISTRY · 2019 ·Vol. 43 ·期 35 ·13967-13978 · IF 3.069

Suppression of platinum sintering on Pt–M/ZSM-22 (M = Ce, La, and Re) catalyst for n-dodecane isomerization

Qiang Ning,Huaike Zhang,Yurong He,Zhiqiang Chen,Suyao Liu,Jie Ren

Small Pt particles (about 1.2 nm) were highly dispersed on ZSM-22 zeolites via a strong electrostatic adsorption (SEA) method and exhibited a promotion effect on the catalytic performance in n-dodecane isomerization in comparison with the conventional catalyst. Several promoters (Ce, La, and Re) were introduced to further improve the aggregation resistance of the small Pt particles. A series of characterization including H2-TPR, XPS and STEM as well as DFT calculations provided solid evidence that the strong interaction between Pt and promoter species not only effectively hinders the Pt aggregation but also alters the electronic state of the Pt sites. Moreover, Ce and La promoters also lead to a slightly improved amount of B acid sites determined by Py-FTIR. Thus, improved activity and selectivity were achieved on a Ce-modified catalyst due to the better balanced bifunctionality between the slightly increased acidity of zeolites and electron-deficiency of Pt. The electron-rich Pt sites are responsible for the significant increase of CH4 selectivity and the decrease of total isomer selectivity in n-dodecane isomerization. In addition, a high-temperature reduction test revealed the higher isomerization activity and selectivity (about 10% higher than the unmodified catalyst) of the Ce-modified catalyst owing to the strong bond of Pt–O–Ce, further confirming the positive effect of the Ce promoter on the sintering resistance of small Pt particles.

研究领域: 催化化学 · 材料科学 · 计算化学
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Journal of Physical Chemistry C · 2022 · IF 4.177

Pseudocapacitive Behavior of Ce Modified CoO through a Galvanostatic Charge–Discharge Test: Distinguishing between Surface-Control and Diffusion-Control Current

Lin Zhu,Zhen Ai,Baoli Wang,Siyue Zhang,Ruyi Zou,Yuhao Huang,Wei Sun

This paper presents an attempt on deconvoluting diffusion-control current (id) and surface-control current (is) from total current in a galvanostatic charge–discharge (GCD) test. Using this strategy, the pseudocapacitive behavior of nanosized Ce-CoO dispersed on graphene support was studied in detail. The results show that id is greatly affected by operating potential and occupies some proportion of the total pseudocapacitive current. The main functions of Ce in the composite material include promoting the proportion of is or inhibiting id and finally stimulating a specific capacitance (Cs) value increased from 192 to 726 F g–1. The Bode curve in the low-frequency region also proves that Ce can promote the performance of pseudocapacitance.

研究领域: 材料科学 · 电化学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2023 · IF 7.2

Rare-earth modified platinum-based electrocatalysts incorporating anodic glycerol oxidation reactions while promoting cathodic hydrogen evolution reactions

Yannan Hai,Ying Chang,Jingchun Jia,Aiju Xu,Meilin Jia

Glycerol electrooxidation (GOR) is a safe and clean method for conversion of glycerol. In the course of this work, a series of Pt x Ce/C catalysts have been synthesized by successive polyol reduction methods as well as etching and calcination . Various physicochemical characterrisation and electrochemical measurements have demonstrated the excellent performance of Pt 3 Ce/C composites in glycerol oxidation (GOR) and hydrogen evolution reactions (HER). The Pt 3 Ce/C catalyst showed better performance in GOR and HER compared to commercially available Pt/C electrocatalysts . This paper demonstrates an energy efficient electrocatalyst for the simultaneous precipitation of hydrogen from glycerol oxidation.

研究领域: 电化学 · 催化材料
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Journal of Environmental Chemical Engineering · 2023 · IF 7.7

Selective catalytic reduction of NOX with CH4 over In/SSZ-13 zeolites: The enhancement of high-temperature catalytic activity by Ce modification

Chenxi Wang,Gang Lv,Yunqiang Li,Ye Liu,Chonglin Song

The selective catalytic reduction of nitrogen oxides by methane (CH 4 /NO X -SCR) is a potential technique for the abatement of the NO X emissions from lean-burn GDI engines, due to the excellent thermal stability of CH 4 . This work focuses on the promotion of In/SSZ-13 catalysts by Ce modification for the CH 4 /NO X -SCR performance at high temperatures. A series of In/SSZ-13 and Ce-In/SSZ-13 catalysts were prepared using the wetness impregnation method. The effects of Ce modification on the catalytic performance were analysed in detail using the scanning electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, ultraviolet-visible diffuse reflectance spectrum and temperature-programmed desorption/reduction techniques. The results show that the Ce modification significantly enhances the high-temperature activity of the In/SSZ-13 catalysts for the NO X -SCR reaction, especially for the 5 wt% Ce-15 wt% In/SSZ-13 sample which has more than 75% NO X conversion at 390–700 °C. In addition, the Ce modification enhances the water vapor tolerance of the catalyst sample. The Ce modification increases not only the concentration of surface chemisorption oxygen species, but also the relative amount of InO + species which serve as the main active sites for CH 4 activation. Furthermore, the incorporation of Ce into In/SSZ-13 greatly promotes NO X adsorption on the catalyst surface. Most importantly, the Ce modification makes In species well-dispersed on the catalyst surface and thus suppresses the formation of bulk In 2 O 3 species which are more active for the CH 4 non-selective oxidation. The combination of all these effects results in the Ce-In/SSZ-13 samples with the superior catalytic activity .

研究领域: 环境科学 · 催化化学
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Surfaces and Interfaces · 2021 · IF 4.837

Enhanced antioxidant capability and osteogenic property of medical titanium by cerium plasma immersion ion implantation

Haifeng Zhang,Jiajun Qiu,Xuanyong Liu

Titanium and its alloys have been widely used as orthopedic and dental implants. However, during practical use, wear debris and surface corrosion will cause the overproduction of reactive oxygen species leading to an inflammatory reaction, which has detrimental effects on osteogenesis around the titanium implants. To solve this problem, in this work, cerium modified titanium surface was constructed by plasma immersion ion implantation (PIII) technology. The mechanical property, corrosion resistance, antioxidant capability, and osteogenic properties of modified titanium were systematically studied. The results indicate that surface hardness and corrosion resistance of modified titanium are markedly improved and the reactive oxygen species level is reduced. Moreover, cell spreading, proliferation, alkaline phosphatase, and collagen secretion of rBMSCs on modified titanium surfaces are improved.

研究领域: 生物材料学 · 医学工程
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