Journal of Cleaner Production
·
2025
·
IF 10
Jian Gao,Yu Zhou,Bingran Wang,Wenxuan Luo,Peng Wu,Kai Shen,Yaping Zhang
Catalytic hydrolysis technology is a promising solution for carbonyl sulfide (COS) treatment, but it is still difficult to scale up due to the poor selectivity of H 2 S and low stability of the catalyst. Developing an efficient catalyst, therefore, remains a significant challenge. Although perovskite-based catalysts are widely utilized in various applications, they are less commonly applied to carbonyl sulfide hydrolysis. Moreover, the effects of doping modification and the hydrolysis reaction mechanism remain to be fully elucidated. Through extensive testing and evaluation of various lanthanide perovskite materials, LaAlO 3 has demonstrated excellent catalytic hydrolysis performance. At 100 °C, LaAlO 3 exhibits a COS removal efficiency of 37 % and an H 2 S selectivity of 52 %. After modification via potassium doping at the A-site, the catalyst achieves near-complete conversion of COS to H 2 S and maintains stable operation for extended periods under high space velocity. The adsorption energies of various adsorption sites were calculated using DFT, confirming the optimal adsorption sites for reactants COS and H 2 O. Water undergoes dissociative adsorption on the catalyst to form -OH groups, which then adsorb COS through the Eley-Rideal (E-R) mechanism, leading to the formation of the hydrolysis intermediate HSCO 2 − . Reactive oxygen species, on the other hand, facilitate the dissociative adsorption of H 2 O, leading to the formation of more surface hydroxyl groups. Meanwhile, calculations indicate that K doping significantly enhances the adsorption energy of the reactants. The structure and properties of the catalysts have been characterized using a variety of techniques. The results have shown that K doping increases the content of weak basic sites and O 2 − in LaAlO 3 . Consequently, the catalytic activity of La 0.8 K 0.2 AlO 3 prepared by the sol-gel method is enhanced, showing higher selectivity and stability. This work provides new solutions and insights for the application of perovskites in the field of environmental catalysis. Owing to its simple preparation method, low cost, and high efficiency, the modified LaAlO 3 catalyst exhibits excellent environmental and economic benefits.
研究领域:
环境催化
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2024
·
IF 7.7
Yubiao Li,Yu Liu,Xueqian Wang,Yixing Ma,Ping Ning,Langlang Wang,Xiang Li,Rui Cao
Activated alumina-based composite oxide support is a commonly used support in hydrodesulfurization (HDS) catalysts, which not only retains the performance advantages of each component in the composite oxide support, but also significantly improves the defects of a single activated alumina support, such as the strong metal-support force of interaction. In this study, NiO-Al 2 O 3 composite support was prepared by introducing NiO-modified Al 2 O 3 , and MoS 2 /NiO-Al 2 O 3 catalysts were prepared for the hydrodesulfurization of COS by liquid phase reduction method. In the COS hydrogenation reaction, the MoS 2 /NiO-Al 2 O 3 catalyst achieved complete conversion of COS at 220 °C and showed more than 99.9% H 2 S selectivity. In stability tests, the catalyst maintained a COS conversion of over 99% throughout the 23-h hydrogenation reaction. Various characterization results show that the NiO-Al 2 O 3 composite support prepared by introducing NiO-modified Al 2 O 3 weakens the metal-support interaction force between MoS 2 and NiO-Al 2 O 3 composite support, which is conducive to the synthesis of MoS 2 with multilayer and long wafer structures. And it can significantly increase the formation rate of MoS 2 to 87.9%, which greatly improves the active site content of the catalyst. Furthermore, the dual modulation of MoS 2 and Al 2 O 3 by NiO modulated the surface alkalinity of the catalysts and promoted the formation of a large number of active edge sites in the MoS 2 /NiO-Al 2 O 3 catalysts, which in turn significantly improved the HDS performance of the catalysts. In addition, EPR characterization combined with experiments showed that the sulfur vacancies are the active sites for catalytic COS hydrodesulfurization over MoS 2 -based catalysts.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2018
·Vol. 9
·期 2
·336-346
·
IF 5.365
Jinjin Lin,Jiangshan Hu,Chengwei Qiu,Huijuan Huang,Lu Chen,Yanyu Xie,Zizhong Zhang,Huaxiang Lin,Xuxu Wang
Solar-driven carbon dioxide (CO2) reduction with water is an important and attractive approach for converting CO2 to fuel and chemicals. Developing intimate heterostructure photocatalysts is essential for efficient solar energy conversion. Here, we fabricated an efficient CaTiO3/TiO2 heterostructure composite by simple in situ hydrothermal etching of {001} facet-exposed TiO2 nanosheets with saturated calcium hydroxide solution. CaTiO3/TiO2 not only possesses an intimate contact heterostructure due to its matching band structures and similar crystal structures but also has enhanced-surface basicity to facilitate CO2 adsorption and activation for the CO2 conversion. Under irradiation, the CaTiO3/TiO2 sample greatly enhances photocatalytic CO2 reduction and shows CO production (11.72 μmol g−1 h−1) 5.6 times higher than that of bare TiO2 nanosheets. The excellent photocatalytic performance of the CaTiO3/TiO2 heterostructures is attributed to the intimate construction of CaTiO3 on TiO2 nanosheets to facilitate the separation of photogenerated charges and the basicity of CaTiO3 to provide more abundant active sites for CO2 adsorption. This study provides fundamental guidance for the rational design of efficient heterostructure photocatalysts for an outstanding photocatalytic CO2 reduction performance.
研究领域:
材料科学
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环境科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2015
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IF 3.942
Jun Chen,Shuanghong Tian,Jiang Lu,Ya Xiong
This study aims to provide a direction to tailor catalytic activity of catalyst by selectively exposing a crystal facet. Herein three sheet-like MgO materials with the primarily exposed crystal facet of (1 1 1), (1 1 0), (2 0 0) were prepared, respectively. Results show that the catalytic ozonation on each MgO substantially enhanced the removal of 4-chlorophenol and total organic carbon when compared with ozonation alone or that on traditional MgO. The pseudo first-order reaction constant of 4-chlorophenol removal in ozonation catalyzed by MgO(1 1 1), MgO(1 1 0), MgO(2 0 0) is 4.8, 2.5, 3.1 times higher than that in the single ozonation, respectively. When different dosage but the same surface area of MgO was applied, their catalytic activities changed as MgO(1 1 1) > MgO(1 1 0) > MgO(2 0 0). It indicates that the catalytic activity significantly depends on the crystal facet besides the surface area. That is because the drawbacks, such as edges, steps, and kinks, on each facet decreased in the order of (1 1 1) > (1 1 0) > (2 0 0). CO 2 -TPD and zeta potential measurement show that the drawbacks caused more and stronger surface basic groups in the form of hydroxyl and isolated oxygen due to the availability of more unsaturated coordination sites. These active basic centers make the easy formation of basic microenvironment near MgO particles and thus favor the ozonation. Finally, the catalytic mechanism was explored and compared by evaluating the ozone decomposition, qualitatively and quantitatively identifying hydroxyl radicals, and determining the ozone utilization efficiency. It reveals that MgO with more surface basic groups can enhance the transformation rate of ozone to hydroxyl radicals more efficiently. All these results show that MgO is a very potential ozonation catalyst and the catalytic activity can be tailored by exposing crystal facet with more drawbacks.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2019
·Vol. 6
·期 7
·1767-1774
·
IF 5.934
Yanfang Zhao,Xiaoxin Zou,Hui Chen,Xuefeng Chu,Guo-Dong Li
Formaldehyde is one of the most harmful environmental toxins, which should be less than 60 ppb indoors. Although some sensors, based on metal oxide semiconductors, are fabricated for the detection of formaldehyde, the sensing performance is not satisfactory yet. In this work, some rare earth metals are successfully introduced into In2O3 by a simple electrospinning method. The structure, composition and chemical state of the products are investigated by XRD, TEM, EDS, XPS, TPD and a Kelvin probe. And the sensor based on 5Y-doped In2O3 exhibits the highest response to formaldehyde. Moreover, this sensor also shows an ultra-low detection limit (50 ppb), a short response time (1 s) and good selectivity. It is believed that the improved sensing response and selectivity may originate from the elevated Fermi level and the increased surface basicity of In2O3, leading to the increase of chemisorbed oxygen on the surface and adsorption of formaldehyde.
研究领域:
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
JOURNAL OF CATALYSIS
·
2016
·
IF 7.354
Wei-You Zhou,Peng Tian,Fu’an Sun,Ming-Yang He,Qun Chen
The development of a highly active and selective catalytic system that is economical, environmentally benign, and easily recoverable is highly desirable. Bifunctional hybrid catalysts originated from metalloporphyrins (MTSPP; M = Co, Fe, and Mn), and hydrotalcite have been synthesized, characterized, and investigated in the aerobic oxidation of alcohols in the presence of isobutyraldehyde. The designed catalysts exhibited excellent activity, broad applicable scope, and good stability in the oxidation. The effect of surface basicity on the catalytic performance has been studied in detail. The research results showed that as well as protecting the metalloporphyrin molecule, the surface basicity of hydrotalcite also contributed to improving the catalytic activity and the selectivity of aldehyde, and a synergistic effect was observed in the catalytic system. A proposed mechanism for the reaction involving the formation of high-valence cobalt–oxo porphyrin intermediate was postulated based on catalytic results and Hammett and H 2 18 O experiments.
研究领域:
催化化学
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材料科学
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有机化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY
·
2017
·Vol. 17
·期 12
·8818-8826
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IF 1.483
Liu Jingwei,Huo Minfeng,Zhu Yan
Mn–Na2WO4/SiO2 synthesized by Urea-assisted hydrothermal-Impregnation route has more and stronger surface basic sites, and more surface lattice oxygen, leading to higher methane conversion with higher selectivity toward ethane and ethylene in oxidative
coupling of methane reaction, compared to Mn–Na2WO4/SiO2 produced by Co-precipitation-Impregnation (CPI) and Sequential Impregnation (SI) methods.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Yafei Guo,Chang Tan,Jian Sun,Weiling Li,Jubing Zhang,Chuanwen Zhao
Business cost concern of solid CO 2 adsorbents has motivated the production of porous activated carbons from waste biomass materials. In this work, porous activated carbons were prepared from sugarcane bagasse using different activating agents (air, CO 2 , H 3 PO 4 and NaOH). Chemically activated porous carbons exhibited better physicochemical properties as compared to the physically activated carbons. Particularly, NaOH-activated carbon (CAC-S) featured a high specific surface area (1149 m 2 /g) and a large pore volume (1.73 cm 3 /g). X-ray photoelectron spectroscopy (XPS) analysis confirmed that the CAC-S adsorbent exhibited enhanced total basicity. The desired CAC-S adsorbent showed superior isothermal CO 2 uptakes of 5.50 and 4.28 mmol CO 2 /g at 0 °C and 25 °C and 1 bar. The isosteric heat of adsorption was predicted as 43.96 kJ/mol from the Clausius-Clapeyron equation and Toth model, which indicated intensified interaction between CO 2 molecules and the basic carbon surface. The excellent CO 2 adsorption performance should be associated with the improved textural properties and enriched surface basicity benefited from NaOH activation. Overall, CAC-S is considered as a promising adsorbent for CO 2 adsorption. The recycling of sugarcane bagasse as solid CO 2 adsorbents presents environmental implications with respect to waste management and pollutants mitigation.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2014
·Vol. 21
·期 21
·12563-12568
·
IF 2.757
Shen Shuguang,Li Meina,Li Binbin,Zhao Zhijun
In order to find an effective method for treating urea wastewater, the experiments on the hydrolysis of urea in wastewater were conducted in a fixed bed reactor with different aluminas (α-Al 2 O 3 , γ-Al 2 O 3 , and η-Al 2 O 3 ) as catalysts respectively in contrast with inert ceramic particle. The results indicate that the three alumina catalysts show obvious catalytic activity for urea hydrolysis at 125 °C. The order of activity is η-Al 2 O 3 > γ-Al 2 O 3 > α-Al 2 O 3 , and the activity difference increases with increasing temperature. According to the characterization results, surface acidity has little impact on the activity of catalyst. However, it was found that surface basicity of alumina catalyst plays an important role in catalytic hydrolysis of urea, and the activity of catalyst may be also influenced by the basic strength. With η-Al 2 O 3 as catalyst, the urea concentration in wastewater is reduced to 4.96 mg/L at a temperature of 165 °C. Moreover, the η-Al 2 O 3 shows a good stability for urea hydrolysis. The hydrolysis of urea over η-Al 2 O 3 catalyst can evidently reduce the reaction temperature and is promising to replace industrial thermal hydrolysis process.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Chemistry-An Asian Journal
·
2024
·Vol. 19
·期 21
·e202400235
·
IF 3.5
Shuangyan Zi,Kai Li,Xueqi Wang,Lina Sun,Yu Tian,Bei Huang,Heping Zeng,Yixing Ma
This study utilized a hydrothermal method to synthesize various metal-modified rod-like ceria catalysts (Fe, Co, Cu, Ni, La), achieving efficient COS removal at low temperatures. The research identified surface oxygen vacancies and basic sites as critical factors that influence the catalytic performance of COS hydrolysis. The addition of different metals to pristine ceria rods increased the specific surface area, oxygen vacancy content (Ov), and basicity, which enhanced the catalysts′ sulfur resistance and stability. Among all the catalysts tested, 10La-CeO 2 demonstrated the highest COS removal rate. This is because La doping significantly augmented Ov, providing more H 2 O adsorption and activation sites. Furthermore, 10La-CeO 2 showed enhanced Lewis basicity, making it easier for COS to adsorb and promote hydrolysis. The in situ DRIFTS results confirmed that appropriate oxygen vacancies and basic sites favored the formation of intermediates such as HCO 3 − and HSCO 2 − , promoting the decomposition of COS into H 2 S and CO 2 .
研究领域:
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2023
·
IF 5.5
Fengqin Guo,Liguo Wang,Yan Cao,Peng He,Huiquan Li
A series of Mg 3 Al 1−x Ce x O composite oxide catalysts were prepared by co-precipitation for the transesterification of ethylene glycol to ethylene carbonate. The characterization results revealed that the addition of cerium changed the acid-base properties of the catalyst and that the strong basic sites on the catalyst surface played an important role in the reaction. The Mg 3 Al 0.9 Ce 0.1 O catalyst showed the highest catalytic activity (ethylene carbonate yield 98.1%). Compared with pure Mg-Al oxide, the appropriate addition of Ce was conducive to improving the surface basicity and adsorbed oxygen content of the catalyst. Additionally, the reaction process of the formation of ethylene glycol hydroxyl group with the alkoxy anion formed by the catalyst attacking the carbonyl carbon of nucleophilic dimethyl carbonate to form an adsorption intermediate (HEMC) on the catalyst surface for further intramolecular rearrangement to form ethylene carbonate was confirmed by operando infrared spectroscopy. The reaction kinetics shows that the reaction conforms to the second-order kinetic equation, and the activation energy is 53.71 kJ·mol −1 . Catalytic stability in a fixed-bed reactor was studied. After a long cycle of use (150 h), the yield of ethylene carbonate was stabilized at about 89.0%.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
BIOMASS & BIOENERGY
·
2025
·
IF 5.8
Yunfei Liu,Hewei Yu,Xiuxiu Chen,Zekai Sun,Lizeng Peng,Hongyu Si
This study focused on the optimized preparation of biodiesel over a ZrO 2 -modified CaO catalyst. CaO/ZrO 2 catalysts were synthesized by impregnation, co-precipitation, and sol-gel methods, and analyzed by various characterization methods, including N 2 adsorption-desorption, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), thermally programmed desorption of CO 2 (CO 2 -TPD), and scanning electron microscopy (SEM). The CaO/ZrO 2 catalyst synthesized by the impregnation method had a uniform microstructure, good crystallinity, a uniform spherical particle structure with large pores and slits, and a density of surface alkali sites of 1.898 mmol g - 1 . Using the impregnation method, the best synthesis conditions were determined as a calcination temperature of 700 °C and a Ca/Zr molar ratio of 3:2. Furthermore, the optimal reaction conditions were determined by single-factor experiments as a catalyst dosage of 8 wt%, a molar ratio of methanol to oil of 12, a reaction temperature of 64 °C, and a reaction time of 2 h. Under these reaction conditions, the yield of fatty acid methyl esters (FAME) reached 95.9 %, decreasing only marginally to 77.6 % after four reuses of the catalyst. It is hoped that this study may provide important research guidance for developing solid basic catalysts for preparing FAME by transesterification under mild conditions.
研究领域:
催化化学
·
可再生能源
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材料科学
✓ 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）