ACS Applied Nano Materials
·
2024
·
IF 5.3
Baoshan Teng,Chunhui Ma,Jiayu Chen,Yunlai Zhang,Baohuan Wei,Maohai Sang,Hui Wang,Yuhan Sun
Ammonia is recognized as the best carrier for hydrogen storage and transportation. Nanomaterial catalysts have eminent catalytic activity for ammonia decomposition. However, the preparation of low-loading, high-activity noble metal atomically dispersed nanometer ammonia decomposition catalysts and their reaction mechanisms remain obscure. In this work, we report the synthesis of a stable ruthenium (Ru) atomically dispersed catalyst with oxygen-rich defects achieved through hydrogen etching of the support CeO2NR nanorods. The oxygen defects result in the catalyst exhibiting a favorable low-temperature catalytic activity and an exceedingly high atom utilization rate for ammonia decomposition. The hydrogen production rate from ammonia decomposition per unit mass of Ru is as high as 2446 mmol H2 gRu–1 min–1 at 1 bar, 450 °C, and gas hour space velocity = 12,000 mL gcat–1 h–1. In this case, the highly dispersed Ru provided enough active sites, while the oxygen defects of the catalyst enhanced the electron transfer tunnel between Ru and the nanorod support under a Schottky contact model. The detailed mechanism of oxygen defects for improving the catalytic performance of ammonia decomposition was studied by DFT modeling. Thus, this work provides a promising strategy to improve the catalytic efficiency of an atomically dispersed Ru nanocatalyst.
研究领域:
材料科学
·
催化化学
·
理论化学
✓ 已验证
DOI
高影响因子
ChemCatChem
·
2022
·Vol. 14
·期 13
·e202200253
·
IF 5.497
Mingsheng Luo,Tong Qin,Qinglong Liu,Zhi Yang,Fengli Wang,Hong Li
Graphical Promoting : A series of Fe-modified CeO 2 catalysts with nanoparticle, nanorod, nanocube and nano-octahedron morphologies were synthesized by the hydrothermal method. The Fe-modified CeO 2 nanorod catalysts exhibit a remarkably promoting effect on the formation of DMC from CO 2 and methanol. A series of Fe-modified CeO 2 catalysts with nanoparticle, nanorod, nanocube and nano-octahedron morphologies were synthesized and applied for direct synthesis of dimethyl carbonate (DMC) from CO 2 and methanol. The Fe-modification shows a remarkably promoting effect on the formation of DMC over Fe-modified CeO 2 nanorod. The DMC yield was improved from 0.202 to 2.568 mmol DMC per g cat by 2 %Fe-modification of CeO 2 nanorod. A synergistic effect among the moderate acid-basic sites, specific surface area and surface composition resulted from Fe-modification was proposed to be crucial to obtaining the high reactivity of DMC formation.
研究领域:
催化化学
·
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Lingwei Yu,Leyi Zhou,Qi Guo,Hongchuan Zhang,Xi Xiao,Ruixue Zhao,Zifeng Yan,Ying Zhang
The challenge of converting carbon dioxide (CO 2 ) electroreduction into high value-added products is to obtain highly selective electrocatalysts. Research has shown that cuprous oxide (Cu 2 O) effectively facilitates the activation of CO 2 and suppress the competing hydrogen evolution reaction. However, during the process of electrochemical reduction, the valence state of Cu 2 O is prone to transformation. Herein, a series of Cu 2 O–CeO 2 -X catalysts (X represents different amounts of CeO 2 added) by applying Cu 2 O onto Cerium oxide (CeO 2 ) nanorods were synthesized via the impregnation method and used as electrocatalysts. We found that the Faradaic efficiency of methane (FE-CH 4 ) for Cu 2 O–CeO 2 -2 reached 65.1 % at −1.6 V vs. RHE, exceeding many catalysts previously reported. From the Cu LMM Auger spectra, it was found that the valence state of Cu species in Cu 2 O–CeO 2 -2 is mainly Cu 0 (accounting for 93.39 %), while in Cu 2 O–CeO 2 -3, the proportion of Cu 0 is 56.34 %. This indicates that CeO 2 has a regulatory effect on the valence state of Cu species. Additionally, we observed the valence state of Cu in Cu 2 O–CeO 2 -2 after the CO 2 reduction reaction and found that the proportion of Cu 0 changed little (94.97 %), which proves that CeO 2 plays a role in stabilizing the valence state of Cu. Research has demonstrated that Cu 0 can adsorb the ∗CO intermediate on its surface, followed by a hydrogenation reaction to generate CH 4 (∗CO + H + + e − → ∗CHO). Copper-based catalysts in which Cu 0 dominates among the Cu species are conducive to the conversion of CO 2 into CH 4 . In situ ATR-SEIRAS spectra confirmed the presence of key intermediates such as ∗CHO and explored the formation pathway of CH 4 (CO 2 → ∗COOH → ∗CO → ∗CHO → ∗OCH 2 → CH 4 ). This study provides a new way to design efficient copper oxide-based catalysts for CO 2 electroreduction by adjusting and stabilizing the ratio of copper valence state reasonably.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 7
·2577-2588
·
IF 6.119
Xian Wu,Weixin Qian,Haitao Zhang,Zhonghao Han,Hewei Zhang,Hongfang Ma,Dianhua Liu,Qiwen Sun,Weiyong Ying
CeO2 nanorods with a mean width of 11.9 nm were synthesized via a facile hydrothermal method. Subsequently, Fe/CeO2 and Fe/CeO2@xMnO2 catalysts were prepared from the CeO2 nanorods and applied in the high-temperature Fischer–Tropsch synthesis of light olefins. Results show that the CeO2 support donates electrons to Fe species, which promotes the dissociation of CO while suppressing the hydrogenation reaction, and then improves the selectivity to light olefins. The synergistic effect between Mn and Ce can improve the oxygen mobility on the catalyst surface and promote the electron-donating ability of Ce, thereby promoting the formation of χ-Fe5C2 and further improving the selectivity to light olefins. However, excess Mn hinders the contact between CeO2 and Fe species and the migration of O atoms, and electron transfer from Ce to Fe can be blocked. Additionally, the reduction of iron oxides was suppressed and subsequently the CO conversion was reduced. The best hydrocarbon distribution for light olefins was 40.4% at a CO conversion of 39.9% over the Fe/CeO2@0.2MnO2 catalyst.
研究领域:
化学工程
·
材料科学
·
催化反应
✓ 已验证
产品关联
DOI
高影响因子
ChemSusChem
·
2021
·Vol. 14
·期 16
·3382-3390
·
IF 8.928
Ting Feng,Jing Ding,Haiyan Li,Wei Wang,Bohua Dong,Lixin Cao
Graphical In hot water : CeO 2 /A−Fe(OH) 3 composites synthesized by a secondary water bath at 100 °C exhibit superior photocatalytic activity. A−Fe(OH) 3 increases specific surface area, passivates the surface of CeO 2 , and reduces the activation energy of water oxidation. This work provides a new insight into exploring amorphous cocatalysts to enhance photocatalytic O 2 evolution activity and augment the possibility of overall water splitting based on CeO 2 . Noble-metal-free composites with good photocatalytic property are of great interest. Here, CeO 2 nanorods composites loaded with amorphous Fe(OH) 3 cocatalyst were designed and prepared via a secondary water bath at 100 °C. The as-synthesized CeO 2 /amorphous Fe(OH) 3 composites exhibited superior light photocatalytic activities compared to pure CeO 2 , especially the sample with a loading time of 60 min. The photocatalytic oxygen generation rate could reach to 357.2 μmol h −1 g −1 , and the average apparent quantum yield (AQY) was 24.67 %, which was a 5.5-fold increase compared to the CeO 2 sample. The improvement of photocatalytic performance could be ascribed to three main reasons: First, loading the amorphous Fe(OH) 3 enlarged the specific surface area and passivated the surface of the pristine CeO 2 . Second, the amorphous Fe(OH) 3 ,which acted as a cocatalyst, provided many active sites, and reduced the reaction activation energy. Thirdly, the maximum interface with intimate contact between CeO 2 and amorphous Fe(OH) 3 cocatalyst accelerated the photogenerated charge separation efficiency and thus improved the photocatalytic performance of CeO 2 in photocatalytic water oxidation.
研究领域:
材料科学
·
环境科学
·
化学
✓ 已验证
DOI
PubMed
高影响因子
ChemPlusChem
·
2023
·Vol. 88
·期 3
·e202300023
·
IF 3.4
Cheng Nan,Huimin Yang,Fanfan Gao,Nan Gao,Wenjing Zhou,Haiyan Du,Zhenhai Liang
Graphical A series of molybdenum - doped CeO 2 nanorod catalysts were successfully fabricated via a hydrothermal reaction coupled with high temperature calcination. The obtained 5 %-Mo-CeO 2 nanorods provide as a superior electrocatalyst in neutral electrolytes of 0.1 M Na 2 SO 4 . Such electrocatalyst significantly enhances nitrogen reduction reaction performance with an NH 3 yield of 10.9 μg h −1 mg −1 cat at −0.45 V vs reversible hydrogen electrode (RHE) and a Faradaic efficiency of 26.5 % at −0.25 V vs RHE, much higher 4 times than of CeO 2 nanorods (2.6 μg h −1 mg −1 cat ; 4.9 %). As a green and sustainable strategy, the electrocatalytic N 2 reduction reaction (NRR) has been considered the best potential approach to replace the traditional Haber-Bosch process under ambient conditions. The key is to exploit efficient and low-cost electrocatalysts according to the current situation. Herein, a series of Molybdenum (Mo) doped CeO 2 nanorods (NR) catalysts were successfully fabricated via a hydrothermal reaction coupled with high temperature calcination. The nanorod structures were not altered after Mo atom doping. The obtained 5 %-Mo-CeO 2 nanorods act as a superior electrocatalyst in neutral electrolytes of 0.1 M Na 2 SO 4 . Such electrocatalyst significantly enhances NRR performance with an NH 3 yield of 10.9 μg h −1 mg −1 cat at −0.45 V vs reversible hydrogen electrode (RHE) and a Faradaic efficiency (FE) of 26.5 % at −0.25 V vs RHE. That outcome is 4 times higher than that of CeO 2 nanorods (2.6 μg h −1 mg −1 cat ; 4.9 %). Meanwhile, density functional theory (DFT) calculation shows the characteristics after Mo doping: the band gap value lowers, the density of states increases, electrons are more easily excited, and N 2 molecules are more easily adsorbed, thereby enhancing the activity of the electrocatalytic NRR.
研究领域:
材料科学
·
电化学
·
理论计算
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Jie Yao,Chengyi Li,Jianxin Feng,Bei Wei,Rongrong Xing,Shurong Ban,Li Tang,Bin Liu
Nanozymes with high peroxide (POD)-like activity have great practical potential in the colorimetric sensing of biomolecules in the medical and biological fields. However, their applications are limited by some disadvantages such as their low catalytic activity and poor biocompatibility. While designing and synthesizing nanozymes, elemental doping is used as an effective method to improve their enzymatic activity. Herein, CeO2 nanorods doped with different concentrations of Mn were synthesized via the hydrothermal method. Mn doping effectively improved the POD-like activity of the CeO2 nanorods. Notably, MnCe0.1 exhibited superior POD-like activity to that of CeO2. The improvement in the catalytic activity of MnCe0.1 was attributed to the presence of more exposed active sites and more oxygen vacancies compared with those of CeO2 nanorods. Using its excellent POD-like activity, the developed system exhibited linear detection ranges of 10–100 μM and 2.5–20 μM and detection limits of 1.94 μM and 0.37 μM for H2O2 and glutathione detection, respectively. Additionally, the developed MnCeX nanomaterials exhibit remarkable temporal stability and reusability. Finally, considering the excellent POD-like activity of MnCe0.1 nanozymes, they have good prospects for cancer treatment.
研究领域:
生物医学工程
·
材料科学与工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2021
·
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
·
环境科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Zhihua Zhao,Xianghao Meng,Ayesha Yousaf,Zhigang Shao,Lan Wu
MoO 3 nanorods, successfully modified with CeO 2 , were synthesized using the hydrothermal technique and subsequently utilized for gas detection. Various techniques were employed to test and analyze the MoO 3 /CeO 2 materials. Numerous characterizations have confirmed that the synthesized MoO 3 /CeO 2 possesses excellent properties. The synthesized MoO 3 nanorods demonstrated uniformity in size, with an approximate diameter of 146 nm. CeO 2 nanoparticles were distinctly visible on the surface of the MoO 3 nanorods. The MoO 3 /CeO 2 sensor demonstrated significantly enhanced sensing performance for triethylamine at 240 °C. Specifically, the MoO 3 /CeO 2 sensor exhibited a reactivity of 73.1 to 20 ppm of triethylamine, signifying an improvement of 3.5 times compared to the reactivity of the MoO 3 nanorods. The sensor based on MoO 3 /CeO 2 exhibited high selectivity, good repeatability, and a lower detection limit for TEA. The enhancement of the gas-sensing performance of the MoO 3 /CeO 2 sensor may have been attributed to the accelerated electron transfer facilitated by the heterojunction formed between MoO 3 and CeO 2 . Additionally, underlying sensing mechanism was investigated using Density Functional Theory (DFT) methodologies.
研究领域:
材料科学
·
传感器技术
·
食品检测
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2019
·
IF 2.938
Qi Song,Rui Ran,Jiancai Ding,Xiaodong Wu,Zichun Si,Duan Weng
Porous ceria nanorods modified with Fe or Co were prepared via a hydrothermal method. The structural properties, catalytic activities for the total oxidation of propane, and catalytic mechanisms of these materials were systematically investigated by X-ray diffraction, Raman spectroscopy, N 2 adsorption–desorption, scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, catalytic activity measurements and in situ Fourier transform infrared spectroscopy. Co-modified ceria exhibited the best catalytic activity during propane oxidation as well as enhanced reducibility due to the synergistic interactions between the Co and the CeO 2 support. Variations in the activating ability and reducibility of the catalysts resulted in the formation of distinctive intermediates during the catalytic process, and this explained the observed differences in catalytic performance.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Lulu Guo,Mengmeng Liu,Xuguang Zhang,Taotao Sui
The development of feasible and facile method to construct oxygen vacancies on metal oxides is crucial for improving their gas sensing properties. In this work, we developed a highly sensitive and stable CO gas sensor based on metal-organic frameworks (MOFs) template-derived Pt nanoparticles (NPs)-functionalized CeO 2 nanorods (Pt-CeO 2 ) with abundant oxygen vacancies through facile solvothermal method. The obtained Pt-CeO 2 -based sensors exhibit good thermal stability and superior CO sensing performance with high response value of 47.7% towards 500 ppm CO at 300 °C, which is higher than that of the pristine CeO 2 sensor (17.8%). Moreover, Pt-CeO 2 -based sensor exhibits excellent selectivity, rapid response/recovery speed (9/11 s) and remarkable long-term stability toward CO. Finally, the enhanced CO sensing mechanism is proposed through a combination of experiments and characterizations, which is attributed to porous structure, abundant oxygen vacancies and electron sensitization effect of Pt NPs. This work not only provides unique insights into the facile design of metal oxide-based nanomaterials with abundant oxygen vacancies, but also has great application potential in building sensing systems for fast CO detection.
研究领域:
材料科学
·
传感器技术
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2018
·Vol. 8
·期 67
·38641-38647
·
IF 2.936
Tianyu Guo,Xiaorong Nie,Jianping Du,Jinping Li
A series of Pd/CeO2-nanorods catalysts modified with alkaline-earth metals were prepared by the incipient impregnation method. Their catalytic properties in low-concentration methane oxidation were also investigated. The catalysts were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy and H2-temperature-programmed reduction techniques. The catalytic results show that the Ca element doped in Pd/CeO2, with optimum molar ratio of Pd to Ca of 2 and calcination temperature of 450 °C, improved the properties of the Pd-based catalyst remarkably, which is attributed to strong Pd–support interaction and high oxygen mobility. Therefore, calcium is more suitable as a promoter for enhancing the activities of the Pd/CeO2 catalyst in methane oxidation.
研究领域:
化学工程
·
催化材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）