Molecular Catalysis
·
2020
·
IF 3.687
Jiajun Dai,Yunlong Guo,Luhang Xu,Guilin Zhuang,Yi Zheng,Daohua Sun,Jiale Huang,Qingbiao Li
Bovine serum albumin (BSA)-templated CeO 2 was prepared by citrate sol-gel method and used as a support to synthesize Au catalyst for benzene oxidation. It was found that the Au/BSA-CeO 2 with 3.2 nm Au nanoparticles (NPs) gave rise to superior catalytic performance for benzene oxidation in which the temperature for 90 % benzene conversion was only 210 °C. In addition, the catalytic activity of Au/BSA-CeO 2 remained stable for 140 h of on-stream reaction. Besides, density functional theory calculation demonstrated how the porous structure of CeO 2 influenced the oxygen vacancy generation, and the synergetic effects of Au NPs and CeO 2 support facilitated the activation of benzene which was adsorbed on Au NPs prior to benzene oxidation. The catalysis of benzene oxidation over Au/CeO 2 catalyst follows the dual-site mechanism. BAS-templated CeO 2 support possessed hierarchical structure, abundant adsorbed oxygen species and synergic interaction with Au that determined the performance of Au/BSA-CeO 2 .
研究领域:
催化化学
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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
Green Energy & Environment
·
2020
·
IF 6.395
Zhaoning Song,Juncong Yuan,Zhenping Cai,Dong Lin,Xiang Feng,Nan Sheng,Yibin Liu,Xiaobo Chen,Xin Jin,De Chen,Chaohe Yang
The advocacy of green chemical industry has led to the development of highly efficient catalysts for direct gas-phase propene epoxidation with green, sustainable and simple essence. The S-1/TS-1@dendritic-SiO 2 material with three-layer core–shell structure was developed and used as the support for Au catalysts, which showed simultaneously fantastic PO formation rate, PO selectivity and stability (over 100 h) for propene epoxidation with H 2 and O 2 . It is found that silicalite-1 (S-1) core and the middle thin layer of TS-1 offer great mass transfer ability, which could be responsible for the excellent stability. The designed dendritic SiO 2 shell covers part of the acid sites on the external surface of TS-1, inhibiting the side reactions and improving the PO selectivity. Furthermore, three kinds of SiO 2 shell morphologies (i.e., dendritic, net, mesoporous shell) were designed, and relationship between shell morphology and catalytic performance was elucidated. The results in this paper harbour tremendous guiding significance for the design of highly efficient epoxidation catalysts.
研究领域:
化学工程
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催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 37
·15618-15629
·
IF 3.5
Wei Zhang,Jin Li,Cuilian Sun,Xiujing Xing,Yaokang Lv,Wei Xiong,Hao Li
Surface modification is one of the effective strategies to control the morphology and electrocatalytic performance of noble metal/transition metal oxide matrix composite catalysts. In this work, we successfully introduced modification groups such as –NH2, –COOH, and –SH on the surface of Fe3O4 using the hydrothermal method. It was found that when the modification group –COOH was introduced, the regular spherical morphology of Fe3O4 was still maintained in Fe3O4–COOH, while Fe3O4–COOH had a relatively smaller spherical particle size (≈155.9 nm). Due to its smaller particle size, Fe3O4–COOH has a larger active area than Fe3O4, exposing more active sites. The abundant active sites in Fe3O4–COOH provide more nucleation and growth sites for Au particles, which is beneficial for the recombination between Fe3O4–COOH and Au. In addition, the experimental results of exploring the effect of Au precursor dosage on the synthesis of the Fe3O4–COOH@Au structure and performance show that the synthesized Fe3O4–COOH@Au1.0 catalyst has higher electrocatalytic activity. Due to the larger electrochemically active surface area of the Fe3O4–COOH@Au1.0 catalyst compared to those of Fe3O4–COOH@Au0.5 and Fe3O4–COOH@Au1.5 catalysts, the adsorption and activation of NO2− reactants were accelerated, thereby improving the electrocatalytic performance. Therefore, owing to the morphological and structural characteristics of Fe3O4–COOH combined with the high activity of Au nanoparticles, the synthesized Fe3O4–COOH@Au exhibits effective electrocatalytic activity in the electrocatalytic NO2−RR synthesis of ammonia. At a voltage of −0.8 V (vs. RHE), the ammonia yield reached 2092.8 μg h−1 mgcat−1 and Faraday efficiency reached 81.2%. The findings of this work will enrich our understanding of the construction of efficient Fe3O4@Au catalysts based on surface functionalization and help to design efficient electrocatalytic NO2−RR catalysts for practical applications.
研究领域:
材料科学
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电化学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Reaction Kinetics Mechanisms and Catalysis
·
2020
·Vol. 132
·期 1
·417-429
·
IF 1.52
Xie Qi,Miao Changxi,Lei Tianqi,Hua Weiming,Yue Yinghong,Gao Zi
Dehydrogenation of ethane assisted by CO 2 has been investigated over Au catalyst supported on Y-doped CeO 2 nanorod. The catalysts were characterized by XRD, TEM, N 2 adsorption, XPS, TG, H 2 -TPR and Raman spectroscopy. Enhanced activity can be obtained after the proper Y doping. The optimal catalyst Au/Ce 0.9 Y 0.1 exhibits an ethane conversion of 20.9% and nearly 100% selectivity to ethylene without any evident tendency of deactivation in 50 h. The reducibility of surface oxygen species is found to play a key role in the dehydrogenation assisted by CO 2 , which can be improved by proper Y doping into CeO 2 nanorod. The promoting effect of CO 2 on activity is evident over Au/Ce 0.9 Y 0.1 catalyst, due to the quick transformation of H 2 product into H 2 O by the reverse water gas shift reaction. The catalyst stability is also improved by the addition of CO 2 , attributed to the elimination of coke by Bouduoard reaction.
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
JOURNAL OF POROUS MATERIALS
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2022
·Vol. 30
·期 3
·723-737
·
IF 2.523
Ke Yi-Hu,Qin Hong-Yu,Wang Xue,Li Hui,Liu Hai,Yuan Hong
Selective catalytic oxidation of polyols, e.g., the selective catalytic oxidation of the secondary –OH bond in glycerol, remains a considerable challenge. In this study, a series of mesoporous CuO–SnO 2 composite oxides were prepared by a hard-template method and used to support Au catalysts for the selective oxidation of glycerol to 1,3-dihydroxyacetone (DHA) under base-free conditions. Catalysts with different Cu:Sn molar ratios gave different catalytic performances. A high conversion of glycerol (100%) and selectivity for DHA (94.7%) were obtained in 2 h at 80 °C and P O2 = 1 MPa over the Au/CuO–SnO 2 -3:1 catalyst. Further investigation indicated that the high catalytic activity of Au/CuO–SnO 2 -3:1 is related to the small size and high dispersion of Au nanoparticles (NPs), the interactions between the Au NPs and the support, the synergistic effect between CuO and SnO 2 , and the amount of surface lattice oxygen species. Various reaction parameters, namely the glycerol:Au molar ratio, the reaction temperature, the initial O 2 pressure, the reaction time, and the support calcination temperature were studied. Although the conversion rate by the catalyst decreased after four cycles, the selectivity remained above 86%. Density functional theory calculations showed that the synergy between CuO and SnO 2 improves the catalytic activity in glycerol oxidation to DHA. The results show that mesoporous composite oxide supports have a wide range of potential applications in the selective oxidation of glycerol to other high-value-added products.
研究领域:
催化化学
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材料科学
·
绿色化学
✓ 已验证
DOI
高影响因子
Journal of Materiomics
·
2024
·
IF 8.4
Di Wu,Yingxin He,Chi Lin,Bing Li,Jiangping Ma,Lujie Ruan,Yajie Feng,Chaogang Ban,Junjie Ding,Xiaoxing Wang,Danmei Yu,Li-Yong Gan,Xiaoyuan Zhou
Piezo-catalysis, which leverages mechanical energy to drive chemical reactions, is emerging as a promising method for sustainable energy production. While the enhancement of piezo-catalytic performance through metal-support interactions is well-documented, the critical influence of the synthesis atmosphere during metal-loaded piezo-catalyst preparation has been a notable gap in the field. To this end, we systematically investigate how different atmospheric conditions during the synthesis of catalysts—without gas flow or with Ar, N 2 and O 2 —affect metal dispersion, oxidation states, piezo-carrier dynamics, and electronic structure, and subsequently shape the metal-support interactions and piezo-catalytic activity. ZnO/Au, with Au deposited on ZnO, is selected as the model system, and hydrogen evolution reaction is used as the probe reaction. Our results demonstrate that an oxygen-enriched atmosphere significantly enhances the metal-support interactions, achieving an ultrahigh net hydrogen yield of 16.5 mmol·g –1 ·h –1 on ZnO/Au, a 3.58-fold increase over pristine ZnO. Specifically, the performance improvements substantially surpass those synthesized under other atmospheric conditions. Conversely, exposure to CO 2 transforms the ZnO support into ZnCO 3 , adversely affecting its catalytic activity. These findings reveal the crucial impact of synthesis conditions on piezo-catalyst performance and thereby open new avenues for optimizing catalyst systems for enhanced sustainability.
研究领域:
材料科学
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能源科学
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 42
·18173-18184
·
IF 3.288
Yi-Hu Ke,Xue Wang,Hong-Yu Qin,Hai Liu,Hong Yuan,Chun-Ling Liu,Wen-Sheng Dong
A series of Au catalysts supported on Cu–Al composite oxides were prepared and applied for the selective catalytic oxidation of glycerol to 1,3-dihydroxyacetone (DHA) in base-free conditions. The optimal Au/CuAlO-3 catalyst (the molar ratio of Cu/Al was 5 : 1) exhibited the best performance, and reached the glycerol conditions of 76.7% and DHA selectivity of 97.3% under the optimized reaction conditions. The high catalytic activity of the Au/CuAlO-3 catalyst correlated to the large concentration of surface-active oxygen species, the low reduction temperature of the support, the small size of Au nanoparticles (NPs) and the interactions between Au NPs and the support. This work demonstrates that Cu–Al composite oxides are promising supports for selective catalytic oxidation of glycerol to DHA, and may offer guidelines for designing efficient support for the selective conversion of glycerol to other high value-added products.
研究领域:
化学工程
·
催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
AICHE JOURNAL
·
2024
·
IF 3.5
Yifan Yan,Pengjie Hao,Yu Fu,Wangsong Chen,Qiwei Shi,Hua Zhou,Xianggui Kong,Zhenhua Li,Mingfei Shao,Xue Duan
Utilizing sustainable electrocatalysis to upcycle glycerol (GLY; the by-product of biodiesel) to lactic acid (LA; the key monomers for biodegradable polymer) is an efficient way to reduce the cost of biodiesel, which is also consistent with the waste-to-wealth principle. However, current research still suffers from issues of low LA selectivity (<80%), especially at high current density. Herein, we designed a cooperative catalyst by modifying BiO x nanolayers on gold nanoparticles (BiO x /Au), achieving high LA selectivity (82%) at high current density (226 mA cm −2 at 1.05 V vs. RHE), outperforming most of the reported works in the literature. We reveal that BiO x could promote the adsorption of the middle hydroxyl of GLY, which facilitates the formation of DHA and thus enables high LA selectivity. Moreover, the electron-deficient Au in BiO x /Au is responsible for the enhanced current density, which is more beneficial to generate reactive oxygen species (OH*). To further reveal the application potential of this electrocatalytic strategy, we realized that the conversion of crude GLY extracted from cooking oil to LA coupled with H 2 production using a membrane-free flow electrolyzer, demonstrating a sustainable fashion to convert biodiesel waste into high value-added product and H 2 fuel.
研究领域:
电化学
·
催化
·
可持续化学
·
可再生能源
✓ 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）