CHEMICAL ENGINEERING SCIENCE
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2024
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IF 4.1
Yeshuang Wang,Zhelin Su,Mingxian Duan,Huiling Fan,Ju Shangguan,Chao Yang
Metal oxides-based adsorbents used for desulfurization encounter significant challenges during practical application owing to their inferior reusability and the nature of solid waste of their desulfurization products. This situation might be alleviated to some extent through a rational design of Ni–Mo composite, enabling them firstly to be used as adsorbents for H 2 S removal, and then being utilized as catalysts after desulfurization for C 4 H 4 S hydrogenation. The Ni–Mo composites before and after desulfurization were characterized using XRD, FT-IR, SEM, N 2 adsorption–desorption, XPS, CO 2 -TPD and H 2 -TPR techniques. The experimental findings suggested that Ni and Mo species function as primary active sites for H 2 S adsorption and C 4 H 4 S hydrogenation reactions, respectively. The Ni and Mo composite greatly facilitated the coupling of these two reactions due to the formation of NiMoO 4 phase. This novel active phase not only boosted the interaction between metal and H 2 S but also promoted the formation of weak and moderate alkaline sites, thereby significantly enhancing desulfurization performance. Importantly, this active phase fostered the sulfurization of Mo species and transforming into a Ni–Mo–S component, further favoring the subsequent catalytic reaction in C 4 H 4 S hydrogenation. Consequently, the prepared Ni–Mo composite oxides exhibited excellent properties in H 2 S adsorption and C 4 H 4 S hydrogenation activity, surpassing the capabilities of single metal adsorbents and commercial hydrogenation catalysts.
研究领域:
化学工程
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催化材料科学
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产品关联
DOI
高影响因子
Journal of Environmental Sciences
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2024
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IF 5.9
Kaini Ma,Kai Li,Ping Ning,Jiayu Feng,Jiacheng Bao,Lei Shi,Xiangyu Wang,Xin Sun
This study employed a wet impregnation method to synthesize five types of Cu/HZSM-5 adsorbents with Si/Al ratios of 25, 50, 85, 200, and 300, used for the removal of H 2 S in low-temperature, low-oxygen environments. The impact of different Si/Al ratios on the adsorption oxidative performance of Cu 30 /HZSM-5–85 adsorbents was investigated. According to the performance test results, Cu 30 /HZSM-5–85 exhibited the highest breakthrough capacity, reaching 231.75 mg H 2 S/g sorbent . Cu/HZSM-5 sorbent maintains a strong ability to remove H 2 S even under humid conditions and shows excellent water resistance. XRD , BET, and XPS results revealed that CuO is the primary active species, with Cu 30 /HZSM-5–85 having the largest surface area and highest CuO content, providing more active sites for H 2 S adsorption. H 2 -TPR and O 2 -TPD results confirmed that Cu 30 /HZSM-5–85 sorbent exhibits outstanding redox properties and oxygen storage capacity, contributing to excellent oxygen transferability in the molecular sieve adsorption-oxidation process. With notable characteristics such as a large surface area, high desulfurization efficiency, and water resistance, Cu 30 /HZSM-5–85 sorbents hold significant importance for industrial applications.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Shuwen Peng,Yuran Li,Bin Wang,Yanbin Cui,Jinglei Tian,Hongqiang Liu,Tingyu Zhu
Removal of sulfur species from blast furnace gas is urgently needed due to the strict emission limits imposed on iron-steel industrial flue gas. Improving the sulfur capacity of H 2 S is a crucial challenge to reduce the operation cost. NiFe layered double hydroxide (LDH) adsorbents were synthesized using the hydrothermal method to strengthen the adsorption of H 2 S, achieving a high sulfur capacity of 133.6 mg/g at 50 °C. Characterization studies have revealed that the reaction pathway of H 2 S on the NiFe LDH surface involves adsorption, dissociation and oxidation. It has been clarified that the high sulfur capacity can be attributed to the abundant H 2 S dissociation sites and the excellent O 2 activation sites. The dissociation sites of H 2 S encompass metal sites, -OH and CO 3 2- . The interaction between O 2 and the bridge site of asymmetric metal atoms significantly enhances the dissociation of O 2 . Strengthening the dissociation of H 2 S and O 2 improves the sulfur capacity. The deactivation of adsorbents comes from the continuous consumption of oxygen species mainly composed of -OH and the deposition of sulfur species in the smaller mesopores ranging from 2 to 10 nm. This work provides useful insights into designing highly efficient iron-based adsorbents for the desulfurization of blast furnace gas.
研究领域:
材料科学
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环境工程
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Jiayu Feng,Lijuan Jia,Fei Wang,Xin Sun,Ping Ning,Chi Wang,Yuan Li,Kai Li
In this work, we report a novel urea-modified copper-based material (XUrea@Cu) obtained by directly calcinating a mixture of urea and copper nitrate. This material enables the efficient purification of H 2 S under dry and anaerobic conditions. The performance test results showed that the H 2 S capacity of the optimal adsorbent (2Urea@Cu) could reach 364.2 mg(H 2 S)∙g sorbent -1 , which is much superior to those of other adsorbents in the literature. Further study demonstrates that the ultra-desulfurization performance of 2Urea@Cu is mainly attributed to the extensive alkaline site, the high concentrations of active oxygen, and the abundance of oxygen vacancy; which are quite effective for capturing H 2 S (acidic and strong reducibility). Interestingly, the deactivation adsorbent (De-2Urea@Cu) is mainly composed of high-purity CuS, which means that the Urea@Cu adsorbent can simultaneously achieve efficient purification of H 2 S and recovery of sulfur resources since CuS is a valuable product. In addition, in-situ FT-IR and theoretical calculation results indicate that H 2 S molecules dissociate on the CuO(1 1 1) surface by stepwise dehydrogenation, while S combines with adjacent Cu to form CuS. The consumption of active components (CuO) and the accumulation of reaction products (CuS) are the primary reasons for the deactivation of adsorbents. Considering the simple preparation process, low cost, and excellent H 2 S adsorption activity, these urea-modified copper-based materials are very promising H 2 S adsorbents.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
Journal of Environmental Sciences
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2023
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IF 6.9
Yongqi Yan,Xinyu Yang,Ping Ning,Chi Wang,Xin Sun,Fei Wang,Peng Gao,Kai Li
In this study, non-thermal plasma (NTP) was employed to modify the Cu/TiO 2 adsorbent to efficiently purify H 2 S in low-temperature and micro-oxygen environments. The effects of Cu loading amounts and atmospheres of NTP treatment on the adsorption-oxidation performance of the adsorbents were investigated. The NTP modification successfully boosted the H 2 S removal capacity to varying degrees, and the optimized adsorbent treated by air plasma (Cu/TiO 2 -Air) attained the best H 2 S breakthrough capacity of 113.29 mg H 2 S/g adsorbent , which was almost 5 times higher than that of the adsorbent without NTP modification. Further studies demonstrated that the superior performance of Cu/TiO 2 -Air was attributed to increased mesoporous volume, more exposure of active sites (CuO) and functional groups (amino groups and hydroxyl groups), enhanced Ti-O-Cu interaction, and the favorable ratio of active oxygen species. Additionally, the X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) results indicated the main reason for the deactivation was the consumption of the active components (CuO) and the agglomeration of reaction products (CuS and SO 4 2− ) occupying the active sites on the surface and the inner pores of the adsorbents.
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
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