INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Chunying Liu,Li Lv,Kun Liu,Junsu Jin,Jianguo Mi,Yongqiang Ren,Shisen Xu
By coupling CALF-20 on ZIF-7 via in situ crystallization in the confined micrometer-sized pores of poly(acrylates), a novel composite, namely, CALF-20-on-ZIF-7@poly(acrylates), has been synthesized for the simultaneous removal of CO2 and H2S from IGCC feed gas. Within this coupled crystal, CALF-20, known for its strong adsorption capacity and excellent stability toward CO2 and H2S, serves as the outer layer crystal to shift the adsorption/desorption hysteresis loop of inner ZIF-7 to beyond atmosphere pressure. Under high pressure, CO2 and H2S are automatically adsorbed. Upon reducing the pressure to the atmospheric level, CO2 is automatically released, while H2S remains temporarily due to its high adsorption energy. After about 150 cycles of CO2 adsorption/desorption of the kilogram-scale composite, H2S approaches saturation and is then removed by vacuuming. Since the content of H2S in IGCC feed gas is trivial, the total energy consumption for the composite regeneration is 0.16 MJ/kg (CO2). After 600 consecutive cycles, the CO2 adsorption capability of the composite decreases by 0.41%, demonstrating excellent cyclic stability.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
RSC Advances
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2018
·Vol. 8
·期 66
·38124-38130
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IF 2.936
Jiaojing Zhang,Hua Song,Yanguang Chen,Tianzhen Hao,Feng Li,Dandan Yuan,Xueqin Wang,Liang Zhao,Jinsen Gao
Amine-modified MCM-41 adsorbents (APTMS/MCM-41, PEI/MCM-41 and AAPTS/MCM-41) were prepared and characterized by XRD, N2 adsorption–desorption, FT-IR, TEM, SEM and TG-DTA. The performance of each adsorbent in a fixed adsorption bed for H2S removal was measured using a mixture of oxygen, nitrogen and hydrogen sulfide gases. It was found that the specific surface area decreased and the topography changed significantly after the use of each modified adsorbent. Nevertheless, all amine-modified MCM-41 adsorbents retained mesoporous silica of MCM-41. The H2S removal rate and saturated H2S capacity of APTMS/MCM-41 improved from 32.3% to 54.2% and 119.5 to 134.4 mg g−1, respectively, compared with that of MCM-41, and it showed the best performance among all adsorbents. APTMS/MCM-41, PEI/MCM-41 and AAPTS/MCM-41 were regenerated by maintaining at 423, 523 and 373 K in nitrogen for 3 h, respectively, and thus possessed high regenerability.
研究领域:
化学工程
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材料科学
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Juanjuan Feng,Yu Tian,Kunlin Li,Fei Wang,Kai Li,Ping Ning
Toxic H 2 S limits the high-value utilization of high-concentration CO in yellow phosphorus tail gas. High-performance adsorbents play a significant role in the purification of yellow phosphorus tail gas and the recovery of CO. In this study, manganese-based adsorbents doped with other metals (Cu, Co, Ni, Ce, and Fe) were synthesized and tested for H 2 S removal. The results demonstrate that doping α-MnO 2 with metals significantly enhances its desulfurization performance. Notably, the 20 % Ni/Mn adsorbent achieves the best performance, exhibiting an adsorption duration of approximately 50 h under test conditions and H 2 S capacity up to 854.35 mg/g. Mechanism studies show that the performance improvement is mainly attributed to the doping of Ni, which disrupts the growth of the α-MnO 2 rod-like structure, promoting the formation of fine particles and exposing more crystal interfaces. This is conducive to the migration and release of active lattice oxygen species on the adsorbent, thereby enhancing the adsorption-oxidation performance of the adsorbent for H 2 S. Moreover, Ni significantly promotes the formation of high-valent Mn, enhancing the adsorbent’s oxidation capability and facilitating the decomposition of H 2 S. This study proposes an innovative synthetic strategy for constructing adsorbents with high H 2 S adsorption performance under anaerobic and dry conditions.
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
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Xiang Li,Xueqian Wang,Langlang Wang,Li Yuan,Yixing Ma,Yibing Xie,Yiran Xiong,Ping Ning
The low S selectivity of catalysts for H 2 S removal significantly hinders its application in blast furnace gas desulfurization. In this study, Cu-based coconut shell biochar was modified with different types and contents of alkali species. The results showed that the S selectivity close to 100% was prolonged from 0 to 750 min. At the same time, the sulfur capacity was increased from 242.1 mg/g (before the modification) to 373.4 mg/g by using K 2 CO 3 -induced Cu-based biochar at 120 °C. In CO, H 2 O, and O 2 atmosphere, H 2 S was dissociated and oxidized to elemental S. Additionally, K 2 CO 3 exhibited an elemental S anchoring effect, making the S more stable at medium–high temperatures and weakening the reactivity of S with CO and ·O 2 – . Thus, less COS and SO 2 were generated. Moreover, the basic sites enhanced by K 2 CO 3 promoted the hydrolysis of COS to generate H 2 S, which entered the desulfurization cycle. K 2 CO 3 also showed a synergistic effect with the active components, generating more ·O 2 – to promote the oxygenation of H 2 S. The regeneration efficiency of the catalyst could be stabilized above 90%. These findings could provide guidance and reference for designing and applying desulfurization catalysts with high S selectivity and activity.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
Journal of Materials Chemistry A
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2025
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IF 9.5
Shuai Liu,Dicka Ar Rahim,Yan Zhang,Dan Wang,Ekkachai Kanchanatip,Yi He,Mi Yan
To advance the utilization of high-concentration CO2 produced in biogas upgrading, it is essential to remove associated hydrogen sulfide (H2S). This study presents a series of bimetallic Fe–Cu oxides supported on multi-walled carbon nanotubes (MWCNTs), which were synthesized to efficiently remove H2S from CO2-rich gas at low temperatures. The synergy of the bimetallic elements not only forms a multifaceted active phase but also causes new defects on the MWCNTs, creating more H2S/CO2 separation sites. The adsorption experiments demonstrate that the deep H2S removal performance of the adsorbent is unaffected by the CO2 concentration, achieving a maximum adsorption capacity of 30.11 mg g−1, which exceeds that of commercial desulfurizers and previously reported adsorbents. Additionally, density functional theory calculations were employed to elucidate that the introduction of Cu species increases the gap in the average adsorption energies between H2S and CO2. The adsorbent also exhibited stability after 4-cycle regeneration at room temperature, maintaining 62.6% of its initial H2S capacity. This work underscores the potential of Fe–Cu oxide/MWCNTs adsorbents as a viable, regenerable solution for H2S removal in CO2 purification, offering implications for carbon-negative construction.
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
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Yeshuang Wang,Mingxian Duan,Zhelin Su,Chao Yang,Yuxiao Wang,Tian Kou,Jiawei Kou,Huiling Fan
Cu–1,3,5-benzenetricarboxylate (Cu–BTC) exhibited potential for hydrogen sulfide (H 2 S) removal, however, its sulfur capacity is limited due to it relies only on the adsorption reaction path. Herein, a series of Fe-doped Cu–BTC materials (denoted as x Fe–Cu–BTC) were synthesized to enhance H 2 S removal capacity via a adsorption–oxidation bifunctional synergism mechanism. The prepared materials were characterized using various techniques, and their H 2 S removal performance was measured under dry and ambient conditions. The experimental results demonstrated that the 18%Fe–Cu–BTC shown the optimal breakthrough sulfur capacity of 122.8 mg S/g, marking a 2.1-fold and 10.3-fold improvement over pure Cu–BTC and Fe–BTC, respectively. The characterization analyses revealed that the Cu 2+ active sites initially react with H 2 S to form CuS, while the incorporated Fe 3+ sites trigger the oxidation of CuS, yielding elemental sulfur, Cu 2+ and Fe 2+ . The resultant Cu 2+ and Fe 2+ further engage in reactions with H 2 S to form CuS and FeS, thereby enhancing the H 2 S removal capacity via dual reaction pathways of adsorption and oxidation. Additionally, appropriate Fe doping increased the specific surface area and pore volume of Cu–BTC, which exposed more active sites and improved molecular diffusion. Based on the obtained findings, a plausible desulfurization mechanism involving adsorption and oxidation synergism for remove H 2 S was proposed.
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
RSC Advances
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2018
·Vol. 8
·期 25
·13798-13805
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IF 2.936
Lianghu Su,Chenwei Liu,Kangkang Liang,Yudong Chen,Longjiang Zhang,Xiaolin Li,Zhihua Han,Guangyin Zhen,Xiaoli Chai,Xu Sun
The removal performance of high-concentration H2S (ca. 10 000 ppm) from simulated biogas by zero-valent iron nanoparticles (NZVI), with the majority of the particles in the size range of 60–150 nm, at different reaction temperatures (room temperature, 100 °C, 200 °C and 250 °C) were evaluated using a custom-designed quartz fixed-bed reactor. The results showed that the H2S removal capacities of NZVI were quite limited at room temperature and 100 °C, being 12.56 and 14.77 mg H2S gNZVI−1, respectively. However, these values increased significantly to 391.02 (200 °C) and 488.95 (250 °C) mg H2S gNZVI−1. Scanning electron microscopy analysis showed that the products of the NZVI–H2S reaction aggregated to form irregular polygonal-shaped structures. The main X-ray diffraction pattern peaks of the product matched well with troilite, and no pyrite was observed. The deconvolution of the X-ray photoelectron spectrometry peaks showed the presence of monosulphide (S2−) and disulphide (S22−) in the product, in which 36% of the sulphur existed as monosulphide and 64% as disulphide. It is proposed that the effective removal of hydrogen sulphide by NZVI at elevated temperatures can be attributed to the combination of nano-constituents, oxide shell and underlying Fe core to produce FeS similar to troilite and amorphous FeS2.
研究领域:
环境科学
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化学工程
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材料科学
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2019
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IF 3.375
Haifeng Li,Sheng Su,Yan Peng,Linkang Wu,Kai Xu,Lijun Liu,Mengxia Qing,Song Hu,Yi Wang,Jun Xiang
High temperature sorbents for removing H2S comprising manganese oxide and Al2O3 support modified with La loadings were prepared with wet impregnation. The removal of H2S and the regeneration of sorbents were conducted at 850 °C to investigate the effect of the support modified with La on the desulfurization ability and durability of the Mn/La/Al2O3 sorbents. The fresh sorbent, first sulfide sorbent, and fourth regenerated sorbent were characterized by nitrogen isothermal adsorption, X-ray power diffraction, scanning electron microscopy, and H2 temperature-programmed reduction. The results showed that the highest initial breakthrough sulfur capacity (BSC) was obtained with Mn/0.78%La/Al2O3(M/0.78L), and the initial BSC decreased with increased La loadings due to the inhibiting of excessive La on the reaction between MnO and H2S. The BSC of sorbents with lower La loadings suffered more serious deactivation than MnxOy/Al2O3 during successive desulfurization–regeneration cycles, and the BSC durability of sorbents increased with an increase in La loadings and calcination temperature of La/Al2O3. Mn/4.83%La/Al2O3 with La/Al2O3 calcined at 900 °C (M/4.83H) had the best BSC durability, which was better than the BSC durability of MnxOy/Al2O3 (M) during several desulfurization–regeneration cycles. The characterization results showed that the structure of the M/4.83H sorbent was more stable than other sorbents. The M/4.83H sorbent derived the La(AlO3) phase, which could maintain the structural stability of the sorbent during several desulfurization–regeneration cycles. The formation of the LaAlO3 phase may inhibit MnxOy from dissolving into Al2O3, which was beneficial for the durability of sorbents during several successive desulfurization–regeneration cycles.
研究领域:
化学工程
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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
FUEL
·
2021
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IF 6.609
Haifeng Li,Tao Liu,Sheng Su,Mei Jin,Wen Fang,Lijun Liu,Yi Wang,Song Hu,Jun Xiang
Ce modified Mn x O y /Al 2 O 3 -La have been prepared to investigate the effect of Ce loadings on pre-breakthrough H 2 S removal efficiency, breakthrough sulfur capacity (BSC) and BSC durability of the sorbents during desulfurization-regeneration cycles. The results showed Ce modification could improve the pre-breakthrough H 2 S removal efficiency of regenerated sorbents during desulfurization-regeneration cycles. The XPS characterization showed that the Ce can promote the binding energy of Mn ion to shift to lower energy, which enhanced H 2 S adsorption on the regenerated sorbent. However, the Ce loading sequence had effect on BSC durability of sorbent during desulfurization-regeneration cycles. The Ce-Mn x O y /Al 2 O 3 -La with co-impregnation of Mn and Ce oxides had higher BSC than Mn x O y /Al 2 O 3 -La, while the Ce/Mn x O y /Al 2 O 3 -La with Ce loading on the surface of Mn x O y /Al 2 O 3 -La had lower BSC and worse BSC durability than Mn x O y /Al 2 O 3 -La. The characterization results showed Ce-Mn x O y /Al 2 O 3 -La obtained better surface area and pore structure than Mn x O y /Al 2 O 3 -La, and Ce ion can promote the increasing of the around electron density of Mn ion, which was beneficial for H 2 S adsorption of Ce-Mn x O y /Al 2 O 3 -La. The poor surface area and pore structure would cause the low BSC of Ce/Mn x O y /Al 2 O 3 -La, and less stability of pore structure might lead to poorer BSC durability of Ce/Mn x O y /Al 2 O 3 -La than Mn x O y /Al 2 O 3 -La during desulfurization-regeneration cycles.
研究领域:
化学工程
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材料科学
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产品关联
DOI
高影响因子
ACS Omega
·
2025
·
IF 4.3
Liang Ma,Yuting Zhang,Anlin Liu,Zhisheng Zhao,Liwang Wang,Yulong Chang,Xiaoxu Duan,Peng Gao
Hydrogen sulfide (H2S) is an extremely noxious impurity generated from industrial processes, but conventional absorption devices applied to remove H2S are often constrained by low mass transfer coefficients and large equipment volume. To overcome these limitations, we propose a novel high-jet oscillating purifier (HOP) and systematically investigate the key operational parameters that influence desulfurization performance when HOP is combined with a methyl diethanolamine (MDEA) solution. Experimental results demonstrated that H2S removal efficiency and mass transfer coefficients increased with absorption flow rate (0.06–0.12 m3/h), methyl diethanolamine concentration (0.8–3.2 wt %), and inlet H2S concentration (20–160 mg/m3), but decreased with methyl diethanolamine solution temperature (25–85 °C). Intriguingly, inlet gas flow rates (5 and 17 m3/h) improved removal efficiency but reduced mass transfer coefficients. Radial injection (α = 0°) of absorption liquid achieved optimal performance, yielding peak efficiency at 98.7%, surpassing nonradial injection (α = ±45°) by 12.3–15.8%. The mass transfer coefficients (KGa) at 0.0715 kmol·m–3·kPa–1·s–1, are about ten times higher than conventional devices. Semiempiric equation (R2 = 0.99, p < 0.001) was derived to predict KGa across operational conditions. The industrial application indicated that HOP achieved an average removal efficiency higher than 95.1% with only 1/8 of the device volume compared to conventional scrubbers. The study indicates that HOP combined with MDEA solution has great potential for application in removing H2S for industrial plants.
研究领域:
化学工程
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环境工程
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气体净化
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工业污染控制
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Xinpeng Liu,Baohua Wang,Xiaole Dong,Yahui Qiu,Qingmei Meng
The desulfurization and regeneration performance of nanofluids composed of oxidizing ionic liquids and four inert nanoparticles are investigated. The addition of different nanoparticles has been proved to have enhancement effect on the H 2 S removal performance of oxidizing ionic liquids. The nanofluids with SiO 2 nanoparticles showed the most significant strengthening desulfurization performance as well as regeneration performance. The optimal weight ratio of SiO 2 nanoparticles in nanofluids was confirmed as 0.5%. The regeneration efficiency of the optimal nanofluid system can exceed 88%, which is far higher than that before the addition of SiO 2 nanoparticles. The mass transfer coefficient increased significantly after the addition of nanoparticles. The nanoparticles and nanofluids before and after absorption were characterized by Fourier transform infrared spectra , nuclear magnetic resonance, scanning electron microscope , transmission electron microscope, energy dispersive spectrum and X-ray photoelectron spectroscopy. It was found that the structure and morphology of SiO 2 nanoparticles remained basically unchanged in the absorption-regeneration process. The main final desulfurization product was identified as sulfate.
研究领域:
化学工程
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENERGY & FUELS
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2019
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IF 3.021
XiangFeng Tian,LeMeng Wang,Dong Fu
The absorption performance including absorption capacity and loading values of low-partial-pressure H2S in tetramethylammonium glycinate ([N1111][Gly]) promoted N-methyldiethanolamine (MDEA) aqueous solution was measured. The apparent absorption rate was calculated from the time-dependent absorption capacity. The effects of absorbent composition, temperature, and H2S partial pressure on absorption capacity and apparent absorption rate were demonstrated. The H2S removal efficiency was verified in a tray tower using the [N1111][Gly]–MDEA aqueous solution as an absorbent, and the results show that the removal efficiency can reach 100%, which met the requirement of the first degree of Chinese cleaner production standard (coking industry, HJ/T 126-2003, I, H2S ≤ 0.2 g/m3). Compared with the traditional amine-based absorbents like MDEA–monoethanolamine aqueous solution, the [N1111][Gly]-promoted MDEA aqueous solution has a higher absorption capacity and a higher absorption rate for H2S. Moreover, when the mass fraction of MDEA reaches up to 50%, the removal efficiency in the tray tower can still reach 100%. The decrease of the water content in the absorbent can greatly reduce the energy cost of the regeneration of rich solution and the cooling of poor solution. Therefore, the new absorbent proposed in this work has good commercial application potential in the field of desulfurization of the coke oven gas.
研究领域:
化学工程
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环境工程
✓ 已验证
产品关联
DOI
高影响因子