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学者姓名：王世萍
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Abstract ：
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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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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Previous N-glycosylation approaches have predominately involved acidic conditions, facing challenges of low stereoselectivity and limited scope. Herein, we introduce a radical activation strategy that enables versatile and stereoselective N-glycosylation using readily accessible glycosyl sulfinate donors under basic conditions and exhibits exceptional tolerance towards various N-aglycones containing alkyl, aryl, heteroaryl and nucleobase functionalities. Preliminary mechanistic studies indicate a pivotal role of iodide, which orchestrates the formation of a glycosyl radical from the glycosyl sulfinate and subsequent generation of the key intermediate, a configurationally well-defined glycosyl iodide, which is subsequently attacked by an N-aglycone in a stereospecific SN2 manner to give the desired N-glycosides. An alternative route involving the coupling of a glycosyl radical and a nitrogen-centered radical is also proposed, affording the exclusive 1,2-trans product. This novel approach promises to broaden the synthetic landscape of N-glycosides, offering a powerful tool for the construction of complex glycosidic structures under mild conditions. © 2024 Wiley-VCH GmbH.
Keyword ：
glycosyl iodides glycosyl iodides glycosyl sulfinates glycosyl sulfinates N-glycosides N-glycosides N-glycosylation N-glycosylation radical reactions radical reactions
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| GB/T 7714 | Ding, W. , Chen, X. , Sun, Z. et al. A Radical Activation Strategy for Versatile and Stereoselective N-Glycosylation [J]. | Angewandte Chemie - International Edition , 2024 , 63 (36) . |
| MLA | Ding, W. et al. "A Radical Activation Strategy for Versatile and Stereoselective N-Glycosylation" . | Angewandte Chemie - International Edition 63 . 36 (2024) . |
| APA | Ding, W. , Chen, X. , Sun, Z. , Luo, J. , Wang, S. , Lu, Q. et al. A Radical Activation Strategy for Versatile and Stereoselective N-Glycosylation . | Angewandte Chemie - International Edition , 2024 , 63 (36) . |
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The limited degradability and high production costs associated with traditional epoxy resin pose obstacles to its sustainable development. In this study, hybrid material of epoxidized soybean oil-derived epoxy resin (ESOR) and hydrothermal carbon microspheres (HTCs) was designed. Investigations confirmed the presence of diverse oxygen-containing groups on the HTCs, with the carboxyl content specially increased through air activation, which also increased the specific surface area. These alterations enhanced the interfacial interactions between HTCs and ESOR. As a result, the optimized composite exhibited the most notable tensile strength of 3.91 MPa, approximately 22.6 % higher than that of the pure ESOR. Importantly, the incorporation of the air-activated HTCs, which had the water holding and cation exchange capabilities, significantly enhanced the degradability of the ESOR matrix, about 68.3 wt% and 100.0 wt% of the ESOR decomposed respectively from 5HTC300/ESOR and 7 HTC300/ESOR immersed in 0.5 wt% NaOH for 15 day, without the use of organic solvents. While applying the composite materials in coated fertilizers with a 0.5 wt% paraffin outer layer, the best one can slowly release 47.7 % P in 20 days. © 2024 The Korean Society of Industrial and Engineering Chemistry
Keyword ：
Air-activation Air-activation Bio-based epoxy resin Bio-based epoxy resin Coated fertilizers Coated fertilizers Degradability Degradability Hydrothermal carbon microspheres Hydrothermal carbon microspheres
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| GB/T 7714 | Zhan, Y. , Yang, H. , Guo, C. et al. Improving the degradability of epoxy resin with enhanced mechanical properties via hydrothermal carbon microspheres [J]. | Journal of Industrial and Engineering Chemistry , 2024 , 142 : 177-186 . |
| MLA | Zhan, Y. et al. "Improving the degradability of epoxy resin with enhanced mechanical properties via hydrothermal carbon microspheres" . | Journal of Industrial and Engineering Chemistry 142 (2024) : 177-186 . |
| APA | Zhan, Y. , Yang, H. , Guo, C. , Li, X. , Wang, S. , Zheng, X. et al. Improving the degradability of epoxy resin with enhanced mechanical properties via hydrothermal carbon microspheres . | Journal of Industrial and Engineering Chemistry , 2024 , 142 , 177-186 . |
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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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The catalytic cleavage of carbon-sulfur (C & boxH;S) double bonds on the metal sites without deactivation has aroused great interest in both fundamental catalytic research and industrial chemistry. Herein, activity descriptors are developed via machine learning and density functional theory (DFT) calculations to screen transition-metal single-site catalysts, which quantify the effect of both atomic electronic properties and coordination configuration on the hydrolysis of C & boxH;S double bonds. The valence electron number and electronegativity of active sites are found to be well related to C & boxH;S activation and sulfur poisoning, where Fe demonstrates high catalytic potential among a series of metal centers. On the other hand, the isolated Fe-1 and Fe-2 sites favor carbonyl sulfide (COS) adsorption and activation, while the COS easily dissociates into *S and *CO on Fe-3 hollow site, thus resulting in the formation of robust Fe-S bonds and catalyst deactivation. As anticipated, the as-designed Fe-1-N-4 site achieves a COS conversion of ca. 96% at 100 degrees C, slightly better than the Fe-2-N-4 site, approximately 8 times higher than that of the Fe/C, which is also better than those of other monatomic catalysts (such as Co-NC, Ni-NC, Sn-NC, and Bi-NC). The combination of in situ characterizations and theoretical calculations suggests that *COS and *H2O/*OH have a competitive adsorption relationship on Fe-N-4 sites, and two Fe-N-4 sites can synergistically catalyze the COS hydrolysis through the spilled H and OH.
Keyword ：
carbon-sulfurbonds cleavage carbon-sulfurbonds cleavage hydrolysis mechanism exploration hydrolysis mechanism exploration isolated Fe-N-4 site isolated Fe-N-4 site metal activesite design metal activesite design valence electron descriptor valence electron descriptor
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| GB/T 7714 | Lei, Ganchang , Lin, Xiaoyun , Yan, Hongping et al. Valence Electron and Coordination Structure Guided Metal Active Site Design for Hydrolytic Cleavage of Carbon-Sulfide Double Bonds [J]. | ACS CATALYSIS , 2024 , 14 (22) : 17103-17112 . |
| MLA | Lei, Ganchang et al. "Valence Electron and Coordination Structure Guided Metal Active Site Design for Hydrolytic Cleavage of Carbon-Sulfide Double Bonds" . | ACS CATALYSIS 14 . 22 (2024) : 17103-17112 . |
| APA | Lei, Ganchang , Lin, Xiaoyun , Yan, Hongping , Shen, Lijuan , Wang, Shiping , Liang, Shijing et al. Valence Electron and Coordination Structure Guided Metal Active Site Design for Hydrolytic Cleavage of Carbon-Sulfide Double Bonds . | ACS CATALYSIS , 2024 , 14 (22) , 17103-17112 . |
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The use of bio-oil-based polymers in fertilizer coatings has drawn significant academic interest. However, the challenge remains to eliminate toxic chemicals while enhancing comprehensive properties. This study focused on synthesizing a degradable polymer from epoxidized soybean oil (ESO) without organic solvent at low temperature (120°C), accomplished through a modified curing agent (MCA). This MCA was made of an acidic eutectic mixture of phthalic anhydride (PA) and its glycerides, produced from inexpensive, low-toxic phthalic anhydride and glycerol. The process utilized a small quantity of zinc acetate (0.5 wt%) to facilitate the formation of phthalic triglyceride in the MCA and mitigate PA sublimation, resulting in the enhanced cross-link degree, superior mechanical properties and hydrophobicity of the ESO-based resin (ESOR). Under optimal preparation conditions, the solvent-free ESOR-coated fertilizer exhibited an extended longevity of 53 days, with an 80 % phosphorus release. This coating material can undergo hydrolytic degradation in soil and in-situ conversion into carboxylates. These findings hold significant potential for advancing the applications of ESOR in green and sustainable agriculture. © 2024 Elsevier B.V.
Keyword ：
Carboxylation Carboxylation Curing Curing Fertilizers Fertilizers Plastic coatings Plastic coatings Soybean oil Soybean oil Temperature Temperature Zinc compounds Zinc compounds
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| GB/T 7714 | Zhan, Yingying , Guo, Caiyan , Yang, Honglin et al. Moderate-temperature curing of epoxidized soybean oil for highly efficient coated fertilizer [J]. | Industrial Crops and Products , 2024 , 220 . |
| MLA | Zhan, Yingying et al. "Moderate-temperature curing of epoxidized soybean oil for highly efficient coated fertilizer" . | Industrial Crops and Products 220 (2024) . |
| APA | Zhan, Yingying , Guo, Caiyan , Yang, Honglin , Li, Xiang , Wang, Shiping , Zheng, Xiaohai et al. Moderate-temperature curing of epoxidized soybean oil for highly efficient coated fertilizer . | Industrial Crops and Products , 2024 , 220 . |
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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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We report the first use of carbon-doped boron nitride (BCN) for H2S-selective catalytic oxidation. The obtained carbon-doped BN with an ultrathin layer structure exhibits outstanding H2S elimination and high S yield. In particular, BN doped carbon nanosheets display better catalytic performance than traditional catalysts, such as iron- and carbon-based catalysts. The findings of the present work shed a new light on metal-free catalysts for efficient catalytic removal of toxic H2S.
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| GB/T 7714 | Lei, Ganchang , Qi, Sihui , Li, Haiyan et al. Carbon-doped boron nitride nanosheets as an efficient metal-free catalyst for the selective oxidation of H2S [J]. | PHYSICAL CHEMISTRY CHEMICAL PHYSICS , 2023 , 25 (47) : 32317-32322 . |
| MLA | Lei, Ganchang et al. "Carbon-doped boron nitride nanosheets as an efficient metal-free catalyst for the selective oxidation of H2S" . | PHYSICAL CHEMISTRY CHEMICAL PHYSICS 25 . 47 (2023) : 32317-32322 . |
| APA | Lei, Ganchang , Qi, Sihui , Li, Haiyan , Xue, Yinjiang , Shen, Lijuan , Zheng, Xiaohai et al. Carbon-doped boron nitride nanosheets as an efficient metal-free catalyst for the selective oxidation of H2S . | PHYSICAL CHEMISTRY CHEMICAL PHYSICS , 2023 , 25 (47) , 32317-32322 . |
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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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