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学者姓名：詹瑛瑛
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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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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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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 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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Carbonyl sulfide (COS) is commonly found in conventional fossil fuels, such as nature gas, oil-associated gas, and blast-furnace gas, and its untreated emission not only corrodes pipelines and poisons catalysts but will also inevitably pollute the environment and endanger human health. Catalytic hydrolysis is recognized as the most promising strategy to eliminate COS because it can be performed under mild reaction conditions with a high removal efficiency. Notably, alkali metals promote catalytic COS hydrolysis over Al2O3 owing to their electron donor properties, basicity, and electrostatic adsorption. However, despite the significant attraction of using potassium-promoted Al2O3 (K2CO3/Al2O3) as conventional catalysts for COS hydrolysis, the mechanism of COS hydrolysis over K2CO3/Al2O3 remains unclear and is controversial owing to the complex composition of the K species. In this study, commercial Al2O3 modified with potassium and sodium salts were synthesized using the wet impregnation method and characterized by various techniques. Based on the results of the activity measurements, the K2CO3-, K2C2O4-, NaHCO3-, Na2CO3-, and NaC2O4-modified catalysts had a positive effect on COS hydrolysis. Among them, the K2CO3/Al2O3 catalyst exhibited the highest COS conversion. Notably, the K2CO3/Al2O3 catalyst exhibited an excellent catalytic performance (-93%, 20 h), which is significantly better than that of pristine Al2O3 (-58%). Furthermore, this study provides strong evidence for the role of H2O during catalytic hydrolysis over K2CO3/Al2O3 using in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and X-ray photoelectron spectroscopy (XPS). The in situ DRIFTS analysis revealed that hydrogen thiocarbonate formed as an intermediate during COS hydrolysis over K2CO3/Al2O3. Meanwhile, the XPS findings suggested that sulfates and elemental sulfur accumulated on the catalyst surface, which may have contributed to catalyst poisoning. Additionally, the effect of water vapor content in the reaction pathway of COS hydrolysis over K2CO3/Al2O3 was investigated. The presence of excess water resulted in a reduction in catalytic activity owing to competitive adsorption between H2O and COS molecules on the catalyst surface. The enhancement in the catalytic activity over K2CO3/Al2O3 may be attributed to the formation of HO-Al-O-K interfacial sites. More importantly, all the catalysts were used under industrially relevant conditions, which provides valuable theoretical guidance for practical applications in the future. Thus, this detailed mechanistic study reveals new insights into the roles of the interfacial K co -catalyst, which provides a new opportunity for the rational design of stable and efficient catalysts for COS hydrolysis.
Keyword ：
Carbonyl sulfide Carbonyl sulfide Catalytic hydrolysis Catalytic hydrolysis Deactivation mechanism Deactivation mechanism HO-Al-O-K interface site HO-Al-O-K interface site Industrial-relevant condition Industrial-relevant condition
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| GB/T 7714 | Lei, Ganchang , Zheng, Yong , Cao, Yanning et al. Deactivation Mechanism of COS Hydrolysis over Potassium Modified Alumina [J]. | ACTA PHYSICO-CHIMICA SINICA , 2023 , 39 (9) . |
| MLA | Lei, Ganchang et al. "Deactivation Mechanism of COS Hydrolysis over Potassium Modified Alumina" . | ACTA PHYSICO-CHIMICA SINICA 39 . 9 (2023) . |
| APA | Lei, Ganchang , Zheng, Yong , Cao, Yanning , Shen, Lijuan , Wang, Shiping , Liang, Shijing et al. Deactivation Mechanism of COS Hydrolysis over Potassium Modified Alumina . | ACTA PHYSICO-CHIMICA SINICA , 2023 , 39 (9) . |
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Fe-doped LaCoO3 perovskite catalysts synthesized via a facile citric acid-assisted sol-gel route have been applied for the H2S selective oxidation. The as-synthesized LaFexCo1_xO3 perovskites exhibit a randomly macroporous structure formed by the accumulation of nanoparticles. Characterization studies reveal that appropriate Fe substitution effectively enhances the formation of oxygen vacancies, and thus improves the lattice oxygen mobility and H2S adsorbability, respectively. The obtained LaFe0.4Co0.6O3 exhibited remarkable catalytic activity, with the H2S conversion and sulfur yield of 100% at 190 degrees C. A combined approach of in-situ FT-IR and insitu Raman experiments disclosed that the plausible reaction pathway of H2S selective oxidation over LaFexCo1_ xO3 perovskites follows the Mars-van Krevelen mechanism. The density functional theory calculations revealed that Fe-doping improves the formation of oxygen vacancy and enhances the adsorption of H2S. This study offers new insights for the design of highly efficient perovskites for the selective oxidation of H2S.
Keyword ：
Density functional theory Density functional theory Fe doped Fe doped H 2 S selective oxidation H 2 S selective oxidation LaCoO 3 perovskite LaCoO 3 perovskite Oxygen vacancy Oxygen vacancy
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| GB/T 7714 | Zheng, Xiaohai , Li, Bang , Shen, Lijuan et al. Oxygen vacancies engineering of Fe doped LaCoO3 perovskite catalysts for efficient H2S selective oxidation [J]. | APPLIED CATALYSIS B-ENVIRONMENTAL , 2023 , 329 . |
| MLA | Zheng, Xiaohai et al. "Oxygen vacancies engineering of Fe doped LaCoO3 perovskite catalysts for efficient H2S selective oxidation" . | APPLIED CATALYSIS B-ENVIRONMENTAL 329 (2023) . |
| APA | Zheng, Xiaohai , Li, Bang , Shen, Lijuan , Cao, Yanning , Zhan, Yingying , Zheng, Shoutian et al. Oxygen vacancies engineering of Fe doped LaCoO3 perovskite catalysts for efficient H2S selective oxidation . | APPLIED CATALYSIS B-ENVIRONMENTAL , 2023 , 329 . |
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Hydrogen sulfide (H2S) is a notorious andlethal gaswidely generated in human economic activities and natural occurrences.The growing demand for pollution control makes it vital for the developmentof efficient processes to remove and convert H2S into high-valuedproducts. As such, diversified technologies have been extensivelyexplored, including H2S splitting, selective oxidationof H2S, and simultaneous conversion of H2S andCO(2). In this review, the state-of-the-art processes forH(2)S conversion and utilization are reviewed. The potentialsof various value-added products from H2S utilization, suchas H-2, syngas, COS, CH3SH, and other sulfur-containingfine chemicals are elucidated in detail. Notably, the traditionaland emerging materials for H2S removal, mainly includingmetal oxide catalysts and carbon-based materials are also overviewedin this review. In addition, the catalytic mechanisms for these desulfurizationreactions are also briefly discussed. Lastly, perspectives are givenon the viability and technological gaps for each technology and correspondingcatalysts.
Keyword ：
catalytic mechanism catalytic mechanism catalytic process catalytic process desulfurization desulfurization H2S H2S resourcesrecovery resourcesrecovery
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| GB/T 7714 | Zheng, Xiaohai , Lei, Ganchang , Wang, Shiping et al. Advances in Resources Recovery of H2S: A Review of Desulfurization Processes and Catalysts [J]. | ACS CATALYSIS , 2023 , 13 (17) : 11723-11752 . |
| MLA | Zheng, Xiaohai et al. "Advances in Resources Recovery of H2S: A Review of Desulfurization Processes and Catalysts" . | ACS CATALYSIS 13 . 17 (2023) : 11723-11752 . |
| APA | Zheng, Xiaohai , Lei, Ganchang , Wang, Shiping , Shen, Lijuan , Zhan, Yingying , Jiang, Lilong . Advances in Resources Recovery of H2S: A Review of Desulfurization Processes and Catalysts . | ACS CATALYSIS , 2023 , 13 (17) , 11723-11752 . |
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The high cost and difficulty in sustainability have hindered the wide application of the general synthetic resins in the controlled-release fertilizers (CRF). Here, the degradable castor oil-based polyurethane (PU) was filled by the natural pyrophyllite (PY) powders, which were pre-modified with few amount (<0.5 %) of NDZ-201 coupling agent though a simple and economic mechanochemical method. Furthermore, the composite materials of PU and the modified PY (MPY/PU) with enhanced comprehensive properties were prepared and applied in CRF. Moreover, the release behaviors of the coated fertilizers were investigated while tuning the addition amount of modifier or the filling amount of MPY, and it was confirmed that the release performance was highly depended on the hydrophobic and mechanical properties of the composite coating. As a result, the best optimized MPY/PU coating exhibited significantly superior performance to the pure PU materials, and the duration of 80 % nitrogen release was more than 40 days. This confirms that the MPY/PU composite is a promising coating material for the CRF granules.(c) 2022 The Author(s). Published by Elsevier B.V. on behalf of King Saud University. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
Keyword ：
Composite material Composite material Controlled-release fertilizer Controlled-release fertilizer Hydrolytic stability Hydrolytic stability Mechanochemical modifica-tion Mechanochemical modifica-tion Pyrophyllite Pyrophyllite
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| GB/T 7714 | Wang, Shiping , Li, Xiang , Ren, Kun et al. Surface modification of pyrophyllite for optimizing properties of castor oil-based polyurethane composite and its application in controlled-release fertilizer [J]. | ARABIAN JOURNAL OF CHEMISTRY , 2023 , 16 (2) . |
| MLA | Wang, Shiping et al. "Surface modification of pyrophyllite for optimizing properties of castor oil-based polyurethane composite and its application in controlled-release fertilizer" . | ARABIAN JOURNAL OF CHEMISTRY 16 . 2 (2023) . |
| APA | Wang, Shiping , Li, Xiang , Ren, Kun , Huang, Rui , Lei, Ganchang , Shen, Lijuan et al. Surface modification of pyrophyllite for optimizing properties of castor oil-based polyurethane composite and its application in controlled-release fertilizer . | ARABIAN JOURNAL OF CHEMISTRY , 2023 , 16 (2) . |
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The activation of H2O is a key step of the COS hydrolysis,which may be tuned by oxygen vacancy defects in the catalysts.Herein,we have introduced Cu into Co3O4 to regulate the oxygen vacancy defect content of the catalysts.In situ DRIFTS and XPS spectra reveal that COS and H2O are adsorbed and activated by oxygen vacancy.The 10 at％Cu doped Co3O4 sample(10Cu-Co3O4)exhibits the optimal activity,100％of COS conversion at 70 ℃.The improved oxygen vacancies of Cu-Co3O4 accelerate the activation of H2O to form active-OH.COS binds with hydroxyl to form the intermediate HSCO2,and then the activated-OH on the oxygen vacancy reacts with HSCO2 to form HCO3.Meanwhile,the catalyst exhibits high catalytic stability because copper species(Cu+/Cu2+)redox cycle mitigate the sulfation of Co3O4(Co2+/Co3+).Our work offers a promising approach for the rational design of cobalt-related catalysts in the highly efficient hydrolysis COS process.
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| GB/T 7714 | Guanyu Mu , Yan Zeng , Yong Zheng et al. Oxygen vacancy defects engineering on Cu-doped Co3O4 for promoting effective COS hydrolysis [J]. | 绿色能源与环境（英文版） , 2023 , 8 (3) : 831-841 . |
| MLA | Guanyu Mu et al. "Oxygen vacancy defects engineering on Cu-doped Co3O4 for promoting effective COS hydrolysis" . | 绿色能源与环境（英文版） 8 . 3 (2023) : 831-841 . |
| APA | Guanyu Mu , Yan Zeng , Yong Zheng , Yanning Cao , Fujian Liu , Shijing Liang et al. Oxygen vacancy defects engineering on Cu-doped Co3O4 for promoting effective COS hydrolysis . | 绿色能源与环境（英文版） , 2023 , 8 (3) , 831-841 . |
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