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学者姓名：雷淦昌
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Abstract ：
The efficient utilization of hydrogen resources in H2S has aroused great attention in both resource utilization and environmental protection. Using H2S as a hydrogen resource donor for the reduction of nitrobenzene to aniline could be an effective method to replace H2. Herein, we fabricated the porous flower-like CoNi-LDO catalyst through facile morphology control engineering, which utilizes DMF as an intercalating agent to influence the structure and properties. Endowed with abundant electron-rich oxygen vacancies and enhanced basic sites capacity, the as-designed CoNi-D catalyst exhibits considerable aniline selectivity (96 %) and high catalytic stability over seven cycles at 110 degrees C. The potential single H-induced dissociation pathway for the reduction of nitrobenzene to aniline by H2S was explored using in situ FT-IR analysis. The present study could provide a feasible strategy for designing catalysts for the high-value utilization of H2S.
Keyword ：
CoNi-LDO CoNi-LDO H 2 S utilization H 2 S utilization Hydrogen resource Hydrogen resource Morphology engineering Morphology engineering Oxygen vacancies Oxygen vacancies
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| GB/T 7714 | Jiang, Weiping , Huang, Rui , Zheng, Xiaohai et al. Morphology-engineered porous flower-like CoNi-LDO with oxygen vacancies for the production of aromatic amines through waste H2S [J]. | JOURNAL OF HAZARDOUS MATERIALS , 2025 , 492 . |
| MLA | Jiang, Weiping et al. "Morphology-engineered porous flower-like CoNi-LDO with oxygen vacancies for the production of aromatic amines through waste H2S" . | JOURNAL OF HAZARDOUS MATERIALS 492 (2025) . |
| APA | Jiang, Weiping , Huang, Rui , Zheng, Xiaohai , Lei, Ganchang , Wang, Shiping , Shen, Lijuan et al. Morphology-engineered porous flower-like CoNi-LDO with oxygen vacancies for the production of aromatic amines through waste H2S . | JOURNAL OF HAZARDOUS MATERIALS , 2025 , 492 . |
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Developing efficient strategies for converting hazardous hydrogen sulfide (H2S) waste into valuable products is crucial for mitigating environmental pollution and maximizing resource utilization. Herein, we present a novel approach for the selective reduction of nitroarenes (PhNO2) to arylamines (PhNH2) utilizing H2S as the hydrogen source. This process is facilitated by isolated Fe-Nx sites embedded within graphitic carbon nitride (Fe-CN-x) obtained through a polymerization assembly method. The Fe-CN-3 catalyst, in particular, achieves PhNO2 conversion of 92.0 % with PhNH2 selectivity of 95.8 % at 110°C within 2 h reaction, outperforming the Bulk-CN, commercial active carbon, and commercial Fe2O3. Furthermore, the Fe-CN-3 catalyst can further trigger the reduction of other substituted PhNO2 with high activities. Importantly, the Fe-CN-3 catalyst is resistant to sulfur poisoning, exhibiting high durability, with no obvious decline of catalytic activity in five cycles. Systematic characterizations and density functional theory calculation (DFT) disclose that the isolated Fe atoms prefer to occupy four-coordinate doping configurations (Fe-N4) and the key to this mechanism is the hydrogen transfer process from PhNHOH* + HS* → PhNH* + S + H2O. © 2025 Elsevier B.V.
Keyword ：
Aniline Aniline High-value utilization High-value utilization Hydrogen sulfide Hydrogen sulfide Hydrogen utilization Hydrogen utilization Isolated Fe sites Isolated Fe sites Nitrobenzene hydrogenation Nitrobenzene hydrogenation
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| GB/T 7714 | Liu, X. , Xie, R. , Zheng, X. et al. Efficient isolated iron catalysts for selective arylamines synthesis using waste H2S as hydrogen source [J]. | Chemical Engineering Journal , 2025 , 512 . |
| MLA | Liu, X. et al. "Efficient isolated iron catalysts for selective arylamines synthesis using waste H2S as hydrogen source" . | Chemical Engineering Journal 512 (2025) . |
| APA | Liu, X. , Xie, R. , Zheng, X. , Shen, L. , Lei, G. , Jiang, L. . Efficient isolated iron catalysts for selective arylamines synthesis using waste H2S as hydrogen source . | Chemical Engineering Journal , 2025 , 512 . |
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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 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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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 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-delta 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-delta achieves an impressive 85.6% Ph-NO2 conversion and 81.9% Ph-NH2 selectivity at 1.5 MPa and 90 degrees 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.
Keyword ：
asymmetric oxygen vacancy asymmetric oxygen vacancy CeO2 CeO2 density functional theory density functional theory H2S utilization H2S utilization nitrobenzene hydrogenation nitrobenzene hydrogenation
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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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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 CuTiO2-8-F achieved nearly 100 % COS conversion at 70 degrees C and 93.5 % H2S yield at 130 degrees 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.
Keyword ：
Anatase TiO 2 Anatase TiO 2 COS hydrolysis COS hydrolysis Cu doping Cu doping DFT calculation DFT calculation Oxygen vacancy Oxygen vacancy
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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 CuTiO2-8 nanoflowers [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 492 . |
| MLA | Zheng, Xiaohai et al. "Oxygen vacancies-promoted removal of COS via catalytic hydrolysis over CuTiO2-8 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 CuTiO2-8 nanoflowers . | CHEMICAL ENGINEERING JOURNAL , 2024 , 492 . |
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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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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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