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学者姓名:王世萍
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Catalytic hydrolysis was considered as an efficient technology to remove carbonyl sulfide (COS). The introduction of oxygen vacancy (Ov) is a promising strategy to improve the catalytic performance of COS hydrolysis by promoting the adsorption and activation of reactants. Herein, we reported a Cu-doped TiO2 nanoflower with abundant oxygen vacancies for COS hydrolysis. The Cu species successfully entered the crystal lattice of TiO2 and induced more oxygen vacancies than pure TiO2. The Ov sites can effectively reduce the adsorption and activation energy of COS and H2O. Benefiting from the ample Ov sites, the resulting CuTiO2-δ-F achieved nearly 100 % COS conversion at 70 °C and 93.5 % H2S yield at 130 °C, which is better than that of pure TiO2. Furthermore, in situ FT-IR measurements and density functional theory (DFT) calculations were performed to reveal the reaction pathway in COS hydrolysis. © 2024 Elsevier B.V.
Keyword :
Activation energy Activation energy Copper Copper Copper compounds Copper compounds Density functional theory Density functional theory Hydrolysis Hydrolysis Infrared imaging Infrared imaging Nanoflowers Nanoflowers Oxygen vacancies Oxygen vacancies Sulfur compounds Sulfur compounds Titanium dioxide Titanium dioxide
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GB/T 7714 | Zheng, Xiaohai , Huang, Rui , Li, Bang et al. Oxygen vacancies-promoted removal of COS via catalytic hydrolysis over CuTiO2-δ nanoflowers [J]. | Chemical Engineering Journal , 2024 , 492 . |
MLA | Zheng, Xiaohai et al. "Oxygen vacancies-promoted removal of COS via catalytic hydrolysis over CuTiO2-δ nanoflowers" . | Chemical Engineering Journal 492 (2024) . |
APA | Zheng, Xiaohai , Huang, Rui , Li, Bang , Jiang, Weiping , Shen, Lijuan , Lei, Ganchang et al. Oxygen vacancies-promoted removal of COS via catalytic hydrolysis over CuTiO2-δ nanoflowers . | Chemical Engineering Journal , 2024 , 492 . |
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The conversion of H2S to high-value-added products is appealing for alleviating environmental pollution and realizing resource utilization. Herein, we report the reduction of nitrobenzene to aniline using waste H2S as a 'hydrogen donor' over the catalyst of FeCeO2−δ with abundant oxygen vacancies (Ov), especially an asymmetric oxygen vacancy (ASOv). The electron-rich nature of the ASOv sites facilitates electron transfer to the electron-deficient nitro group, promoting the adsorption and activation of Ph-NO2 through the elongation and cleavage of the N-O bond. Benefiting from the formation of abundant ASOv sites, the resulting FeCeO2−δ achieves an impressive 85.6% Ph-NO2 conversion and 81.9% Ph-NH2 selectivity at 1.5 MPa and 90 °C, which surpasses that of pure CeO2 with flower and rod morphologies. In situ FT-IR measurements combined with density functional theory calculations have elucidated a plausible reaction mechanism and a rate-limiting step in the hydrogenation of Ph-NO2 by H2S. © 2024 American Chemical Society.
Keyword :
Aniline Aniline Cerium oxide Cerium oxide Density functional theory Density functional theory Hydrogen Hydrogen Hydrogenation Hydrogenation Infrared imaging Infrared imaging Iron compounds Iron compounds Nitrobenzene Nitrobenzene Nitrogen oxides Nitrogen oxides Oxygen vacancies Oxygen vacancies
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GB/T 7714 | Zheng, Xiaohai , Li, Bang , Huang, Rui et al. Asymmetric Oxygen Vacancy-Promoted Synthesis of Aminoarenes from Nitroarenes Using Waste H2S as a 'Hydrogen Donor' [J]. | ACS Catalysis , 2024 , 14 (13) : 10245-10259 . |
MLA | Zheng, Xiaohai et al. "Asymmetric Oxygen Vacancy-Promoted Synthesis of Aminoarenes from Nitroarenes Using Waste H2S as a 'Hydrogen Donor'" . | ACS Catalysis 14 . 13 (2024) : 10245-10259 . |
APA | Zheng, Xiaohai , Li, Bang , Huang, Rui , Jiang, Weiping , Shen, Lijuan , Lei, Ganchang et al. Asymmetric Oxygen Vacancy-Promoted Synthesis of Aminoarenes from Nitroarenes Using Waste H2S as a 'Hydrogen Donor' . | ACS Catalysis , 2024 , 14 (13) , 10245-10259 . |
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Developing highly efficient catalysts for the transformation of hydrogen sulfide (H2S) pollutants into value-added products is crucial for both fundamental catalytic research and industrial chemistry. Herein, ferrititanate nanosheets (H0.8Ti1.2Fe0.8O4, denoted as NS-HTFO) exfoliated from lepidocrocite-type titanates are employed for the first time to catalyze the conversion of H2S to elemental sulfur. Collective experimental characterizations reveal that the as-designed NS-HTFO catalyst possesses ultrathin 2D structure and a large specific surface area, featuring abundant oxygen vacancies. Compared with its sandwich-like precursor of K0.8Ti1.2Fe0.8O4 (denoted as L-KTFO), the NS-HTFO catalyst displays notably enhanced desulfurization activity, achieving 100 % H2S conversion and over 93 % sulfur selectivity at temperatures ranging from 90 to 270 degrees C. Moreover, no significant decline in sulfur yield is observed over the course of a 100-hour evaluation, showing outstanding breakthrough sulfur capacity up to 4163 mg/gcat. This performance exceeds that of most recently reported catalysts. The possible catalytic mechanism for H2S-to-S selective oxidation over the NS-HTFO catalyst has also been investigated.
Keyword :
H2S-to-S selective oxidation H2S-to-S selective oxidation Oxygen vacancies Oxygen vacancies Surface basicity Surface basicity Ultrathin 2D structure Ultrathin 2D structure
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GB/T 7714 | Lei, Ganchang , Yao, Zheng , Qu, Jingqi et al. Modulating oxygen vacancies of Fe-doped Ti-based materials with ultrathin nanosheets for enhancing H2S-to-S selective oxidation [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 485 . |
MLA | Lei, Ganchang et al. "Modulating oxygen vacancies of Fe-doped Ti-based materials with ultrathin nanosheets for enhancing H2S-to-S selective oxidation" . | CHEMICAL ENGINEERING JOURNAL 485 (2024) . |
APA | Lei, Ganchang , Yao, Zheng , Qu, Jingqi , Chen, Jiaxin , Shen, Lijuan , Zheng, Xiaohai et al. Modulating oxygen vacancies of Fe-doped Ti-based materials with ultrathin nanosheets for enhancing H2S-to-S selective oxidation . | CHEMICAL ENGINEERING JOURNAL , 2024 , 485 . |
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Although controlled-release fertilizer (CRF) is a safer and more efficient strategy to administer nutrients for plant growth, it is still a daunting task to reduce the cost and improve the degradability of the synthetic resin coatings. In this paper, an inorganic/organic composite coating for urea fertilizer was prepared from a biodegradable castor oil-based polyurethane (PU) filled with the layered Na-bentonite (Na-BT), which was ultrasonically treated by a series of green PEG surfactants. Synergistically influenced by various intercalation ability, cation-hosting ability and hydrophilicity of the PEGs, the porous structures of the modified Na-BT (MBT) fillers were simply tuned by varying the Mn molecular weights of the PEGs, resulting in the adjustable water swelling and me-chanical properties of the MBT/PU composites. Moreover, it was confirmed that the water swelling property played a critical role in controlling the early stage of nutrient release, and the mechanical properties were important for the longevity of nutrient release from the CRFs. The best MBT/PU composite supported a CRF with a long-term release of 75 % in 38 days, which was much longer than the one based on pure PU (20 days).
Keyword :
Composite coating Composite coating Intercalation Intercalation Mechanical property Mechanical property Surface charge Surface charge Water replacement Water replacement Water swelling Water swelling
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GB/T 7714 | Wang, Shiping , Huang, Rui , Ren, Kun et al. Structural control of PEG-intercalating Na-bentonite and its influence on the properties of castor oil-based polyurethane coating [J]. | PROGRESS IN ORGANIC COATINGS , 2023 , 178 . |
MLA | Wang, Shiping et al. "Structural control of PEG-intercalating Na-bentonite and its influence on the properties of castor oil-based polyurethane coating" . | PROGRESS IN ORGANIC COATINGS 178 (2023) . |
APA | Wang, Shiping , Huang, Rui , Ren, Kun , Shen, Lushen , Li, Xiang , Lei, Ganchang et al. Structural control of PEG-intercalating Na-bentonite and its influence on the properties of castor oil-based polyurethane coating . | PROGRESS IN ORGANIC COATINGS , 2023 , 178 . |
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天然气、油田伴生气、高炉煤气等化工生产过程中伴生COS气体,不仅会腐蚀管道和毒害催化剂,还会严重污染环境并危害人类健康。COS催化水解反应可在温和条件下高效的将COS脱除,是最具应用前景的COS脱除技术之一。碱金属元素因其具有独特的电子供体性质、表面碱性和静电吸附等特性,常被用作助催化剂以提高Al_2O_3的COS催化水解性能。近年来,以钾为助剂改性的Al_2O_3催化剂(K_2CO_3/Al_2O_3)在COS催化水解反应中得到广泛的应用,但由于负载在Al_2O_3上的K物种的组成复杂,目前研究者对K_2CO_3/Al_2O_3催化剂上COS水解机理的理解仍存在一定的困惑和争议。本论文通过湿法浸渍法合成出一系列钾盐和钠盐改性的Al_2O_3催化剂,并利用各类先进的表征技术对这些催化剂进行分析。活性测试表明,以K_2CO_3、K_2C_2O_4、NaHCO_3、Na_2CO_3和NaC_2O_4改性Al_2O_3催化剂均有助于COS的水解。其中K_2CO_3/Al_2O_3拥有最佳的COS水解性能,连续运行20 h后其COS转化率仍高于~93%,远远优于未改性的Al_2O_3 (~58%)。我们利用原位红外光谱和X射线光电子能谱探明了反应过程中催化剂的化学结构特征,阐明了H_2O分子在K_2CO_3/Al_2O_3上的水解作用机制。原位红外表明COS在K_2CO_3/Al_2O_3上的水解过程中形成了硫代碳酸氢盐中间产物。X射线光电子能谱表征证明催化剂的失活主要是因为催化剂表面积累了硫酸盐和单质硫。此外,我们还研究了水蒸气含量对COS水解性能的影响,研究发现,由于H_2O和COS分子在催化剂表面存在竞争吸附,过量的H_2O会引起催化活性的下降。上述研究表明,K_2CO_3/Al_2O_3催化剂上COS水解性能的提高主要是形成了HO-Al-O-K界面活性位。更为重要的是,所制备的催化剂都是在模拟工业工况条件下进行的,这为后续的工业应用提供了宝贵理论指导。本工作为理解助剂钾在Al_2O_3催化剂上COS水解活性的增强提供了新的见解,这为未来设计稳定高效的COS水解催化剂打开了新的发展方向。
Keyword :
HO-Al-O-K界面活性位点 HO-Al-O-K界面活性位点 催化水解 催化水解 失活机理 失活机理 工业工况条件 工业工况条件 羰基硫 羰基硫
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GB/T 7714 | 雷淦昌 , 郑勇 , 曹彦宁 et al. 钾改性氧化铝基羰基硫水解催化剂及其失活机理(英文) [J]. | 物理化学学报 , 2023 , 39 (09) : 115-124 . |
MLA | 雷淦昌 et al. "钾改性氧化铝基羰基硫水解催化剂及其失活机理(英文)" . | 物理化学学报 39 . 09 (2023) : 115-124 . |
APA | 雷淦昌 , 郑勇 , 曹彦宁 , 沈丽娟 , 王世萍 , 梁诗景 et al. 钾改性氧化铝基羰基硫水解催化剂及其失活机理(英文) . | 物理化学学报 , 2023 , 39 (09) , 115-124 . |
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Construction of efficient and stable catalytic combustion materials for the removal of unburnt methane (CH4) is very critical for both applied environmental catalysis and basic materials research. Herein, a facile hydrothermal approach is designed for the fabrication of Ir/UTZX (Ir/TiO2-ZrO2) catalysts. The as-synthesized Ir/UTZX catalysts possess unique sphere morphology as well as electronic structure, leading to enlarged exposure of catalytic sites and enhancement of redox properties. As a result, the representative Ir/UTZ5 catalyst achieves a CH4 conversion of nearly 100% at 425 & DEG;C. Significantly, Ir/UTZ5 displays high long-term stability, with no obvious decrease of catalytic activity in the run of 120 h, which is much higher than those of Ir/TiO2 and Ir/ZrO2 catalysts. Our findings offer insights for designing highly efficient and stable catalysts for CH4 catalytic combustion. & COPY; 2023 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
Keyword :
CH4 catalytic combustion CH4 catalytic combustion Ir-based catalysts Ir-based catalysts Synergy mechanism Synergy mechanism TiO2-ZrO2 composite oxides TiO2-ZrO2 composite oxides
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GB/T 7714 | Wang, Shiping , Zhang, Yaping , Lei, Ganchang et al. Rational design of three-dimensional porous Ir- supported TiO2-ZrO2 microspheres for low temperature methane combustion [J]. | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2023 , 48 (53) : 20279-20289 . |
MLA | Wang, Shiping et al. "Rational design of three-dimensional porous Ir- supported TiO2-ZrO2 microspheres for low temperature methane combustion" . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 48 . 53 (2023) : 20279-20289 . |
APA | Wang, Shiping , Zhang, Yaping , Lei, Ganchang , Bao, Jie , Zhan, Yingying . Rational design of three-dimensional porous Ir- supported TiO2-ZrO2 microspheres for low temperature methane combustion . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2023 , 48 (53) , 20279-20289 . |
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A highly efficient coupling of glycosyl stannanes and sulfonium salts enabled by synergistic Pd/Cu catalysis is disclosed, facilitating the construction of C -aryl/alkenyl glycals under mild conditions in high yields. The protocol tolerates a wide scope of functional groups including ketone, cyano, ester, amide, nitro, halide. The one-pot formal C -H glycosylation starting from arene is demonstrated with a reaction sequence of dibenzothiophenylation/Stille coupling. Besides, a gram-scale reaction is performed successfully, showing the high applicability of this protocol.(c) 2023 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.
Keyword :
Carbohydrate Carbohydrate C-glycals C-glycals Glycosyl stannanes Glycosyl stannanes Stille coupling Stille coupling Sulfonium salts Sulfonium salts Synergistic catalysis Synergistic catalysis
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GB/T 7714 | Yan, Weitao , Zheng, Mingwen , Chuang, Peihsuan et al. Synergistic Pd/Cu catalysis enabled cross-coupling of glycosyl stannanes with sulfonium salts to access C -aryl/alkenyl glycals [J]. | CHINESE CHEMICAL LETTERS , 2023 , 34 (7) . |
MLA | Yan, Weitao et al. "Synergistic Pd/Cu catalysis enabled cross-coupling of glycosyl stannanes with sulfonium salts to access C -aryl/alkenyl glycals" . | CHINESE CHEMICAL LETTERS 34 . 7 (2023) . |
APA | Yan, Weitao , Zheng, Mingwen , Chuang, Peihsuan , Sun, Hao , Wang, Shiping , Xu, Chunfa et al. Synergistic Pd/Cu catalysis enabled cross-coupling of glycosyl stannanes with sulfonium salts to access C -aryl/alkenyl glycals . | CHINESE CHEMICAL LETTERS , 2023 , 34 (7) . |
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Developing economic controlled-release fertilizers (CRFs) with superior performance is an ongoing and important research area. This work investigated the co-modification of acid-activated attapulgite (ac-AT) to optimize its surface properties for polyurethane (PU) composite applications, specifically in the coatings of CRFs. The modified ac-AT (MAT) rods were obtained through treatment with 2.0 wt.% KH-560 coupling agent and in-situ grafting with stearic acid (SA). Varying the addition amount of SA resulted in the synthesis of different MAT fillers. Along with the adjustment of the filling amount, the properties of the MAT/PU composites were controlled. Notably, applying 1.5 wt.% SA onto the KH-560 treated ac-AT produced MAT with a contact angle of 100.8 & DEG;, enhancing hydrophobicity and dispersion within the PU matrix. Furthermore, at a filling amount of 9.0 wt.%, the MAT/PU composite exhibited the most favorable properties with a tensile strength of 2.37 MPa, making it the optimal coating for CRFs with 75% nutrient release within 46 days while the coating efficiency was 3.0 wt.%. This co-modification approach shows great potential in enhancing filler properties and promoting their application in organic coatings.
Keyword :
attapulgite attapulgite composite coating composite coating fertilizer fertilizer polyurethane polyurethane surface modification surface modification
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GB/T 7714 | Wang, Shiping , Shen, Lushen , Yang, Honglin et al. Surface grafting stearic acid to the coupling agent on attapulgite: A reinforced filler in castor oil-based polyurethane coating [J]. | JOURNAL OF APPLIED POLYMER SCIENCE , 2023 , 140 (44) . |
MLA | Wang, Shiping et al. "Surface grafting stearic acid to the coupling agent on attapulgite: A reinforced filler in castor oil-based polyurethane coating" . | JOURNAL OF APPLIED POLYMER SCIENCE 140 . 44 (2023) . |
APA | Wang, Shiping , Shen, Lushen , Yang, Honglin , Cai, Guohui , Lei, Ganchang , Shen, Lijuan et al. Surface grafting stearic acid to the coupling agent on attapulgite: A reinforced filler in castor oil-based polyurethane coating . | JOURNAL OF APPLIED POLYMER SCIENCE , 2023 , 140 (44) . |
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天然气、油田伴生气、高炉煤气等化工生产过程中伴生COS气体,不仅会腐蚀管道和毒害催化剂,还会严重污染环境并危害人类健康.COS催化水解反应可在温和条件下高效的将COS脱除,是最具应用前景的COS脱除技术之一.碱金属元素因其具有独特的电子供体性质、表面碱性和静电吸附等特性,常被用作助催化剂以提高Al2O3的COS催化水解性能.近年来,以钾为助剂改性的Al2O3催化剂(K2CO3/Al2O3)在COS催化水解反应中得到广泛的应用,但由于负载在Al2O3上的K物种的组成复杂,目前研究者对K2CO3/Al2O3催化剂上COS水解机理的理解仍存在一定的困惑和争议.本论文通过湿法浸渍法合成出一系列钾盐和钠盐改性的Al2O3催化剂,并利用各类先进的表征技术对这些催化剂进行分析.活性测试表明,以K2CO3、K2C2O4、NaHCO3、Na2CO3和NaC2O4改性Al2O3催化剂均有助于COS的水解.其中K2CO3/Al2O3拥有最佳的COS水解性能,连续运行20 h后其COS转化率仍高于~93%,远远优于未改性的Al2O3(~58%).我们利用原位红外光谱和X射线光电子能谱探明了反应过程中催化剂的化学结构特征,阐明了H2O分子在K2CO3/Al2O3上的水解作用机制.原位红外表明COS在K2CO3/Al2O3上的水解过程中形成了硫代碳酸氢盐中间产物.X射线光电子能谱表征证明催化剂的失活主要是因为催化剂表面积累了硫酸盐和单质硫.此外,我们还研究了水蒸气含量对COS水解性能的影响,研究发现,由于H2O和COS分子在催化剂表面存在竞争吸附,过量的H2O会引起催化活性的下降.上述研究表明,K2CO3/Al2O3催化剂上COS水解性能的提高主要是形成了HO-Al-O-K界面活性位.更为重要的是,所制备的催化剂都是在模拟工业工况条件下进行的,这为后续的工业应用提供了宝贵理论指导.本工作为理解助剂钾在Al2O3催化剂上COS水解活性的增强提供了新的见解,这为未来设计稳定高效的COS水解催化剂打开了新的发展方向.
Keyword :
HO-Al-O-K界面活性位点 HO-Al-O-K界面活性位点 催化水解 催化水解 失活机理 失活机理 工业工况条件 工业工况条件 羰基硫 羰基硫
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GB/T 7714 | 雷淦昌 , 郑勇 , 曹彦宁 et al. 钾改性氧化铝基羰基硫水解催化剂及其失活机理 [J]. | 物理化学学报 , 2023 , 39 (9) : 109-118 . |
MLA | 雷淦昌 et al. "钾改性氧化铝基羰基硫水解催化剂及其失活机理" . | 物理化学学报 39 . 9 (2023) : 109-118 . |
APA | 雷淦昌 , 郑勇 , 曹彦宁 , 沈丽娟 , 王世萍 , 梁诗景 et al. 钾改性氧化铝基羰基硫水解催化剂及其失活机理 . | 物理化学学报 , 2023 , 39 (9) , 109-118 . |
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本发明公开了一种超小粒径二氧化铈的制备及其脱硫应用。该方法以铈盐为原料,氨水为pH调节剂,添加柠檬酸和硅烷偶联剂,合成具有超小粒径的二氧化铈。H2O2的添加可加速原料单元的快速消耗和CeO2的结晶过程,避免持续的晶粒长大。更重要的是,硅烷偶联剂与CeO2的配位作用可延缓催化剂颗粒尺寸的增大,降低CeO2纳米颗粒的团聚程度。所制备CeO2催化剂的粒径大小为4~9 nm,催化剂的超小粒径纳米颗粒可降低反应气和反应底物的传质阻力,促进H2S和硝基苯与催化剂活性位点的充分接触,有效地促进反应的进行,使催化剂在H2S选择性催化还原硝基苯制苯胺的反应中表现出良好的催化活性。
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GB/T 7714 | 江莉龙 , 郑小海 , 王世萍 et al. 一种超小粒径二氧化铈的制备及其脱硫应用 : CN202211075996.3[P]. | 2022-09-05 00:00:00 . |
MLA | 江莉龙 et al. "一种超小粒径二氧化铈的制备及其脱硫应用" : CN202211075996.3. | 2022-09-05 00:00:00 . |
APA | 江莉龙 , 郑小海 , 王世萍 , 詹瑛瑛 , 曹彦宁 . 一种超小粒径二氧化铈的制备及其脱硫应用 : CN202211075996.3. | 2022-09-05 00:00:00 . |
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