RSC Advances
·
2016
·Vol. 6
·期 99
·96997-97003
·
IF 3.289
Xiang Ma,Haidi Liu,Weiman Li,Shengpan Peng,Yunfa Chen
A copper-based metal organic framework (MOF-199) with controllable size and shape was synthesized and used to remove gaseous methyl mercaptan (CH3SH). Characterizations of the synthesized MOF-199 samples before and after desulfurization were carried out by X-ray diffraction (XRD), Fourier transform infrared (FTIR), and X-ray photoelectron spectroscopy (XPS) to observe the adsorption mechanism of CH3SH on MOF-199. The adsorption performance of the synthesized MOF-199 materials and commercialized activated carbon (AC) and Cu loaded AC were evaluated by breakthrough experiments. All three synthesized MOF-199 materials show better performance than commercialized AC. The morphology and texture of MOF-199 materials have great influence on the performance of the adsorption process. The MOF-199 material synthesized by a hydrothermal method exhibited the highest sulfur compound capacity among the synthesized MOF-199 materials (74.7 mg of CH3SH/1 g MOF-199). The color change of MOF-199 during the CH3SH capturing process, indicated a strong interaction between the unsaturated copper sites and –SH group which finally formed CuS and gave rise to obvious damage to the MOF structure.
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
Processes
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2021
·Vol. 9
·期 2
·400
·
IF 2.847
Xiaohua Cao,Jichang Lu,Yutong Zhao,Rui Tian,Wenjun Zhang,Dedong He,Yongming Luo
Praseodymium (Pr)-promoted MCM-41 catalyst was investigated for the catalytic decomposition of methyl mercaptan (CH3SH). Various characterization techniques, such as X-ray diffraction (XRD), N2adsorption–desorption, temperature-programmed desorption of ammonia (NH3-TPD) and carbon dioxide (CO2-TPD), hydrogen temperature-programmed reduction (H2-TPR), and X-ray photoelectron spectrometer (XPS), were carried out to analyze the physicochemical properties of material. XPS characterization results showed that praseodymium was presented on the modified catalyst in the form of praseodymium oxide species, which can react with coke deposit to prolong the catalytic stability until 120 h. Meanwhile, the strong acid sites were proved to be the main active center over the 10% Pr/MCM-41 catalyst by NH3-TPD results during the catalytic elimination of methyl mercaptan. The possible reaction mechanism was proposed by analyzing the product distribution results. The final products were mainly small-molecule products, such as methane (CH4) and hydrogen sulfide (H2S). Dimethyl sulfide (CH3SCH3) was a reaction intermediate during the reaction. Therefore, this work contributes to the understanding of the reaction process of catalytic decomposition methyl mercaptan and the design of anti-carbon deposition catalysts.Keywords:rare earth;MCM-41;CH3SH decomposition;stability;reaction mechanism
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF RARE EARTHS
·
2025
·
IF 7.2
Zijun Huang,Xiaohua Cao,Huaiyu Xu,Miao Lin,Dedong He,Dingkai Chen,Jichang Lu,Yongming Luo
Methyl mercaptan (CH 3 SH) is notorious for global air pollution owing to its odorous characteristics and adverse health effects. Although CeO 2 is currently regarded as a promising catalyst for CH 3 SH decomposition, the high conversion temperature followed by high energy consumption is still a bottleneck. Herein, the cobalt-doped CeO 2 catalyst was synthesized by a facile one-pot preparation strategy and successfully reduces the decomposition temperature from 450 to 250 °C. Further studies demonstrate that the excellent low-temperature catalytic activity of Co 0.6 Ce 0.4 O 2– σ is attributed to its abundant oxygen vacancies and reactive oxygen species. Oxygen vacancies promote the adsorption and dissociation of CH 3 SH, while reactive oxygen species facilitate the decomposition of CH 3 SH. Moreover, Co acts as a sacrificial agent for the adsorption of sulfur species in CH 3 SH, while Ce is responsible for the adsorption and activation of CH 3 SH as the active metal phase. Furthermore, the migration and transformation mechanism of CH 3 SH on the surface of Co 0.6 Ce 0.4 O 2– σ was determined via in situ diffuse reflectance infrared Fourier transform spectra ( in situ -DRIFTS). This work provides a new strategy to synthesize high-performance catalysts for decomposing sulfur-containing volatile organic compounds (VOCs) at low temperatures, which is beneficial to decreasing the energy consumption.
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
CELLULOSE
·
2024
·Vol. 31
·期 13
·8279-8293
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IF 4.9
Hu Songnan,Li Peiyuan,Zhang Saisai,Huang Liulian,Chen Lihui,Hu Hui-Chao
The pulp industry, one of the oldest and largest chemical industries globally, plays a critical role in biomass utilization. Increasing kraft pulp yield has long perplexed researchers and engineers. Given that methyl mercaptan (MeSH) can be self-produced during the kraft pulping process, revisiting MeSH-assisted yield enhancement technology offers great attraction for pulp industry. MeSH’s strong nucleophilicity enables its consumption through both demethylation and non-demethylation reactions. Investigating the MeSH’s evolution at typical pulping conditions is crucial for achieving higher recovery rate of MeSH. This study found that higher pulping temperatures, increased alkali charge, and larger Na 2 S ratios improve the recyclable residual MeSH content in black liquors, increasing it from 17 to 36%. Under moderate pulping conditions, the residual MeSH content was approximately 30% of the original MeSH. Dimethyl sulfide (DMS), a valuable demethylation product of lignin or hemicellulose by MeSH, was found in black liquors at levels up to 15% of the original MeSH. Approximately half of MeSH participated in non-demethylation reactions and could not be recycled. X-ray photoelectron spectroscopy (XPS) analysis of separated kraft lignins suggested the generation pathway and chemical structure of new methylsulfur (MeS)-containing lignin. For economic balance and profitability, DMS recycling is proposed as cost compensation, or by adopting partial MeSH-assisted kraft pulping in batch digesting systems.
研究领域:
化学工程
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生物质利用
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制浆造纸工业
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Zichang Yang,Yuyao Xu,Li He,Xingkai Lu,Xiaolong Yao,Changming Li,Hainan Gao,Zhiliang Yao,Chao Wu
Photocatalytic oxidation technology holds considerable promise for effectively removing odor-causing compounds, yet conventional gas–solid photocatalytic systems suffer from critical limitations, including incomplete mineralization and persistent accumulation of toxic intermediates. To address this, a gas–liquid-solid photocatalytic oxidation system was developed utilizing a superhydrophilic/superhydrophobic photocatalyst. By synthesizing superhydrophobic Cu-doped UiO-66 and combining with TiO 2 , the resulting OCUN/T photocatalysts was thoroughly chatacterized and tested under various conditions. The optimized system achieved sustained methyl mercaptan removal rates exceeding 99 % over 10 h under low flow rates. Performance significantly improved under solar irradiation irradiance > 100 W/m 2 . This work elucidates the synergistic mechanism of interfacial mass transfer and photocatalytic degradation in the gas–liquid-solid system, providing a method for the purification of odor-causing compounds that minimizes secondary pollution.
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
JOURNAL OF CATALYSIS
·
2020
·
IF 7.888
Jichang Lu,Jian Fang,Zhizhi Xu,Dedong He,Siyou Feng,Yubei Li,Gengping Wan,Sufang He,Hua Wu,Yongming Luo
Supported MoS 2 based materials are widely used as heterogeneous catalysts. In this work, we propose a rapid and facile method (ultrasound-induced impregnation assisted by microwave thermal treatment) to synthesize mesoporous silica (SBA-15)-supported, few-layer, ordered and K-promoted MoS 2 nanosheets with different K/Mo ratios. The prepared catalysts are characterized by various physical and chemical techniques. Their catalytic performance is evaluated by methyl mercaptan (CH 3 SH) synthesis from CO/H 2 /H 2 S. The results show that our catalysts exhibit a much higher CO conversion and selectivity to CH 3 SH than the catalysts prepared using the conventional impregnation and reported in the literature. The good performance arises because of two main factors: MoS 2 nanosheets of only 2–4 layers and K promotion. Experimental characterizations and (density functional theory) calculations show that the former is the typical nano-size effect, and the latter stabilizes C S bonds when activating COS molecules.
研究领域:
催化材料
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物理化学
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产品关联
DOI
高影响因子
ACS Omega
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2023
·
IF 4.1
Pengju Liang,Sihui Duan,Qiang Ma,Liangliang Zhang,Guangwen Chu,Bao-Chang Sun
This work presents a screening method of physical solvents for methyl mercaptan (MeSH) absorption using quantum chemical calculations. The absorption solubility and thermodynamic behaviors of dimethyl sulfoxide (DMSO), sulfolane (SUL), propylene carbonate (PC), N,N-dimethylformamide (DMF), and 1-methyl-2-pyrrolidinone (NMP) for MeSH were calculated and analyzed using the COSMO-RS model, and the absorption mechanism was probed combining the quantum theory of atoms in molecules (QTAIM) and reduced density gradient (RDG). Results show that the absorption solubility of the five solvents for MeSH by COSMO-RS model calculations follow the order of NMP > PC > DMSO > SUL > DMF, and the van der Waals forces and hydrogen bond forces determine the absorption solubility of physical solvents for MeSH. In addition, the experimental results of MeSH Henry coefficients in the above five solvents follow the same order as the calculated results. However, the calculated Henry coefficients’ value largely deviates from the experimental value; therefore, we believe that this calculation method is only available for qualitative screening. This work provided a feasible approach to screening high-performance physical solvents for MeSH removal.
研究领域:
化学工程
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环境科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
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2025
·
IF 6.5
Yuxuan Xie,Zhao Li,Ziruo Zeng,Lina Sun,Shuangyou Bao,Xin Sun,Kunlin Li,Chi Wang,Fei Wang,Ping Ning,Kai Li
To investigate the mechanism of the role of active center size on the selectivity of methyl mercaptan (CH 3 SH) and methane (CH 4 ) in the deep hydrogenation reaction of carbon disulfide (CS 2 ), it was first derived from DFT calculations that the Pt cluster geometries showed a decreasing and increasing pattern on the energy barriers of the two key hydrogenation steps: (I) HCSS* to HCSSH* and (II) deep hydrogenation of CH 2 S* to CH 3 SH. For further validation, we synthesized Pt NPs with varied average sizes (1.7–4.0 nm) using a reduction-agglomeration strategy to probe the source of size sensitivity at low Pt loading. It was found that the active centers of Pt NPs located in the 2.0–3.0 nm region have the highest proportion of medium-coordinated Pt sites, which can effectively promote hydrogen spillover and enhance the HCSS* pathway. Finally, with this modulation strategy, the catalytic activity and selectivity were significantly improved at 1 wt% Pt loading, which exceeded that of the fresh 4 wt% Pt/Al 2 O 3 catalyst, and the long-term stable production of CH 3 SH (selectivity was maintained at 80 %) was achieved at 250 ℃ in the high-concentration CS 2 environment.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
Journal of Cleaner Production
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2024
·
IF 9.7
Li He,Zichang Yang,Yuyao Xu,Xingkai Lu,Sory Kaba,Changming Li,Xiaolong Yao,Dong Xu,Zhiliang Yao
Odor pollutants produced by broiler houses can significantly impact the quality of the life of residents and the ecological environment, so it is crucial to explore odor purification technologies. In this study, a defect-rich CuUiO-66@TiO 2 photocatalyst was successfully synthesized for the photocatalytic degradation of five typical odors in broiler houses. CuUiO-66 and TiO 2 in a 1:3 ratio was the most effective in removing odors, capable of removing 99% of methyl mercaptan, 99% of dimethyl sulfide, 99% of dimethyl disulphide, 86.47% of toluene and 63.09% of ethyl acetate in 60 min. After five cycles degradation, the photocatalyst can remain the crystal structure and keep the photocatalytic degradation rate at 95.2% of methyl mercaptan. Furthermore, the proposed mechanisms for the removal of five odors by CU1T3 have been discussed. Therefore, this study has developed a highly efficient photocatalyst that can effectively eliminate odors emitted from broiler houses. This is a promising solution to address the challenges of odor treatment in the near future.
研究领域:
环境科学
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材料科学
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化学工程
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农业工程
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产品关联
DOI
高影响因子
CELLULOSE
·
2025
·
IF 4.8
Li Peiyuan,Hu Songnan,Huang Suyue,Zhang Saisai,Hu Hui-Chao
Increasing kraft pulp yield has long been a critical objective in the pulp and paper industry. In recent years, methyl mercaptan (MeSH) has been recognized as an effective additive for enhancing kraft pulping yields in both softwood and hardwood. To elucidate the underlying mechanisms, this study investigates the impact of MeSH introduction on bamboo kraft pulping, with a focus on understanding its role in enhancing delignification efficiency and protecting carbohydrates. A comparative analysis on kraft lignin reveals that MeSH introduction significantly reduces lignin’s molecular weight by approximately 30%, and the phenolic hydroxyl group content drastically increases by 21.7%. That promotes the dissolution of kraft lignin in pulping liquors, thus accelerating delignification and shortening H-factor by 29.5% and lowering alkali charge by 2%. Analysis of polymerization degree (with a 56% reduction in its decrease) and reducing end group content (decreasing by 12%) in cooked dissolving pulps verifies that MeSH inhibits both carbohydrate peeling reactions and alkaline hydrolysis, and the primarily contribution is on the protective effect on cellulose (82.1%). Therefore, we believe that the main mechanism using MeSH as additives includes two aspects, i.e., accelerating delignification and preventing carbohydrate degradation, which collectively promotes the yield increase of bamboo kraft pulp by 2.8%.
研究领域:
制浆化学
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生物质转化
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林产化工
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高分子降解
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纤维素科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2024
·
IF 12.2
Xiang Gao,Huanhuan Chen,Huimin Qiu,Yang Zhang,Jie Cheng,Yizhong Shen
Due to the typical volatility of gaseous pollutant methyl mercaptan (CH 3 SH), the development of a facile, reliable, and accurate onsite environmental surveillance of highly toxic CH 3 SH faces many challenges, but it is critical to environmental atmosphere assessment and safeguarding public health. Here, we prepared a novel bimetallic carbon dots (Fe&Cu@CDs) nanozyme with high peroxidase-mimicking activity to design a portable hydrogel kit for onsite visual H 2 O 2 -self-supplying enzymatic cascade catalytic colorimetric and photothermal signal synergistic amplification dual-modal monitoring of CH 3 SH in atmospheric environment. Assisted by alcohol oxidase (AOX), CH 3 SH could be specifically converted into H 2 O 2 for oxidizing chromogenic substrate 3,3′,5,5′-tetramethylbenzidine (TMB) catalyzed by Fe&Cu@CDs to produce dark blue ox-TMB with absorption at 652 nm and photothermal characters. Consequently, a CH 3 SH concentration-dependent change both in naked-eye color and photothermal effect-triggered temperature were observed. By hybridizing AOX-assisted Fe&Cu@CDs + TMB with agarose, a H 2 O 2 -self-supplying colorimetric and photothermal signal synergistic amplification sensory hydrogel kit integrated with Color Picker APP-installed smartphone and 660 nm laser-equipped handheld thermal imager for CH 3 SH was proposed with acceptable results in atmospheric environment around wastepile ( e.g. , solid waste and food waste piles), which exhibited great potentials to further develop commercial onsite monitoring platforms in warning-early abnormal atmospheric CH 3 SH for safeguarding environmental health.
研究领域:
环境科学
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分析化学
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纳米技术
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）