Nanomaterials
·
2023
·Vol. 13
·期 4
·775
·
IF 5.3
Hong Su,Jiangping Liu,Yanan Hu,Tianhao Ai,Chenhao Gong,Jichang Lu,Yongming Luo
As a representative sulfur-containing volatile organic compounds (S-VOCs), CH3SH has attracted widespread attention due to its adverse environmental and health risks. The performance of Mn-based catalysts and the effect of their crystal structure on the CH3SH catalytic reaction have yet to be systematically investigated. In this paper, two different crystalline phases of tunneled MnO2(α-MnO2and β-MnO2) with the similar nanorod morphology were used to remove CH3SH, and their physicochemical properties were comprehensively studied using high-resolution transmission electron microscope (HRTEM) and electron paramagnetic resonance (EPR), H2-TPR, O2-TPD, Raman, and X-ray photoelectron spectroscopy (XPS) analysis. For the first time, we report that the specific reaction rate for α-MnO2(0.029 mol g−1h−1) was approximately 4.1 times higher than that of β-MnO2(0.007 mol g−1h−1). The as-synthesized α-MnO2exhibited higher CH3SH catalytic activity towards CH3SH than that of β-MnO2, which can be ascribed to the additional oxygen vacancies, stronger surface oxygen migration ability, and better redox properties from α-MnO2. The oxygen vacancies on the catalyst surface provided the main active sites for the chemisorption of CH3SH, and the subsequent electron transfer led to the decomposition of CH3SH. The lattice oxygen on catalysts could be released during the reaction and thus participated in the further oxidation of sulfur-containing species. CH3SSCH3, S0, SO32−, and SO42−were identified as the main products of CH3SH conversion. This work offers a new understanding of the interface interaction mechanism between Mn-based catalysts and S-VOCs.Keywords:CH3SH decomposition;MnO2;oxygen vacancies;oxygen migration
研究领域:
催化化学
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环境科学
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DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 28
·15499-15508
·
IF 11.9
Junqing Chang,Chaohao Hu,Zanhong Deng,Meng Li,Chengyin Shen,Shimao Wang,Longqing Mi,Ruofan Zhang,Qingli Zhang,Gang Meng
Methyl mercaptan (MM) is one kind of volatile sulfur compound (VSC) with odor and properties (inflammable, highly toxic, and corrosive) similar to H2S; therefore, the highly sensitive and selective monitoring of ambient MM by chemiresistors is strongly essential, but it remains a challenge owing to its relatively weak reducibility/response in comparison with H2S. In this study, a novel chemiresistor composed of hexahedral particles SBO-loaded CdS nanoparticles has been prepared via a facile chemical precipitation method for the super-sensitive and highly-selective recognition of MM. The heterostructural CdS/SBO (0.05%) chemiresistor exhibited an extremely high response (114.7) to 100 ppm MM at a relatively low operating temperature (100 °C) and was about 36- and 9-fold higher than pure SBO and CdS chemiresistor, respectively. Various characterizations suggested that the sulfurization–desulfurization reaction, the abundant oxygen vacancies, and the generation of n–n heterojunctions at the interface promote the redox reaction of surface-active substances, thereby, boosting the outstanding MM response characteristics. In addition, the heterostructural chemiresistor possesses good selectivity, weak humidity interference, a lower limit of detection (LoD) of 82 ppb, and long-term stability (∼6% decline of response after 120 days), which promises practical applications in air quality (odor) monitoring.
研究领域:
材料科学
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环境科学
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传感器技术
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DOI
高影响因子
Small
·
2025
·
IF 12.1
Su Tang,Tao Zhong,Zhangnan Yao,Wei Qu,Ting Li,Huinan Zhao,Shuanghong Tian,Chun He
Frustrated Lewis pairs (FLPs) present new opportunities for the development of highly active spinel materials for the activation of stable molecules. Herein, a Ni and Co-based spinel with abundant FLPs sites (NiCo 2 O 4 -F) is synthesized through morphologic defect engineering and used for efficient catalytic ozonation CH 3 SH elimination. Characterization results reveal that the NiCo 2 O 4 -F with nanoflower structure exposes more surface oxygen vacancies (Ov), inducing local charge redistribution and forming active regions. Ov acts as Lewis basic sites, while the unsaturated coordinated Ni atoms (Ni uc ) act as Lewis acidic sites, and spatially ≈4.08 Å. The Ov···Ni uc FLPs function as “electron shuttles” in the reaction, facilitating specific adsorption of reactants via the dual acidic–basic reaction sites, thereby activating O 3 to generate ·O 2 − and 1 O 2 species to achieve deep oxidation of CH 3 SH. The resulting NiCo 2 O 4 -F catalyst exhibits an outstanding CH 3 SH removal efficiency of 94.4%, achieving a high mass activity (5.6 ppm mg −1 ), which is 70 times greater than that of commercial MnO 2 (0.08 ppm mg −1 ). This work presents a promising approach to developing sophisticated ozone catalysts by controllable construction of acid–base sites on spinel surface, enhancing the understanding of the role of FLPs structure in molecular activation.
研究领域:
材料科学
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环境科学
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催化化学
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DOI
PubMed
高影响因子
CHEMOSPHERE
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2022
·
IF 8.943
Juping You,Jie Shao,Jianmeng Chen,Dongzhi Chen
A new strain, Pseudomonas sp. SJ-1, which was able to remove model odorous organics methanethiol (MT) has been isolated from the wastewater treatment plant and identified via 16S rRNA analysis . Initial MT concentration, temperature and pH played an important role in MT removal, and up to 100% of 260 mg L −1 of MT could be removed within 11 h under the optimum conditions (30 °C, pH 7.0) with an average degradation rate of 23.6 mg L −1 h −1 , which was the highest one in literature so far. The silicone particles were added as the non-aqueous phases (NAP) to enhance the performance of MT degradation. The results indicated that the maximum degradation rate and specific cell growth of strain SJ-1 were 2.36 times and 1.31 times by Haldane kinetic model analysis in the NAP added test. The SO 4 2− was identified as the major intermediate and CO 2 as a final product in MT biodegradation. Overall, this is the first report that a newly isolated Pseudomonas sp. could use high concentration MT as sole energy source and carbon source and its activity could be enhanced by adding NAP. The results provide a suggestion for the development of more effective and reliable biological treatment processes.
研究领域:
环境科学
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微生物学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Qian Li,Jiahui Zhang,Wang Xu,Haiqiang Wang,Jiayu Zhou,Qingguo Chen,Jianmeng Chen,Dongzhi Chen
Odor pollution, represented by low-concentration volatile organic sulfur compounds (VOSCs), has become a difficult issue in the field of air pollution control. Photocatalytic oxidation technology is applicable for the treatment of low-concentration VOSCs. However, currently available photocatalysts often suffer from limited efficiency and severe deactivation. Herein, flower-like BiOX (X = Cl, Br, I) microspheres abundant with oxygen vacancies (OVs) were developed for the removal of the model pollutant CH 3 SH. BiOI exhibited the optimal CH 3 SH oxidation performance, with the removal efficiency stabilizing at 75% within 180-min simulated solar-light irradiation, while BiOCl and BiOBr deactivated from 38% and 55% to 20% and 22%, respectively. Mechanism analysis found, OVs and I - synergistically endowed BiOI with better CH 3 SH adsorption and activation, enhanced light harvesting, quicker charge transfer, and more affluent •OH and •O 2 - productions. Photogenerated e - and •OH took a predominantly irreplaceable part in CH 3 SH oxidation, followed by •O 2 - and h + . New pathways of CH 3 SH photocatalytic oxidation was proposed, and dimethyl trisulfide was firstly found as its oxidation product. Besides, the oxidation products SO 4 2- was proved to be converted to •SO 4 - radicals to further promote CH 3 SH oxidation, and the largest production of •SO 4 - over BiOI might be responsible for its excellent performance. Furthermore, the strong adsorption and substantial accumulation of CH 3 SO 3 H on BiOCl and BiOBr might be the key cause of their rapid deactivation. This work would inspire the construction of more effective photocatalysts for the purification of VOSCs odor.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
FOOD CHEMISTRY
·
2024
·
IF 8.5
Xin Yao,Yangyang Li,Jun Tang,Jieyao Yu,Yanyan Zhang,Xiaochun Wan,Guoyu Zhang,Xiaoting Zhai
Cooked note is an undesired flavor in green tea, while the key odorants and inhibition mechanisms were unknown. Here, volatiles of four green tea samples and two thermal reaction models of methionine-glucose and methional were assessed using gas chromatography‑sulfur chemiluminescence detector and two dimensional gas chromatography-time-of-flight mass spectrometry. Nonvolatiles of reaction models were determined using ultra performance liquid chromatography-Q-Exactive orbitrap mass spectrometry. Four cooked smelling sulfur-containing odorants including dimethyl trisulfide, dimethyl sulfide, diethyl disulfide, and methanethiol having odor activity values > 1 were characterized in tea samples. Aroma addition tests confirmed dimethyl trisulfide (> 0.4 μg/L) as a reliable predictor of the cooked note. Seven sulfur-containing odorants were detected in reaction models. The addition of (−)-epigallocatechin gallate depleted glucose and interrupted the reaction, thus reduced sulfur-containing odorants' amounts. The study provides a novel insight on targeted strategic guidance for mitigating cooked off-flavor during the thermal processing of green tea production.
研究领域:
食品科学
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农业化学
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分析化学
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DOI
PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2021
·
IF 7.46
Jiayu Jian,Xiao Xiao,Jinxuan Cao,Yizhong Shen
Owing to lack of the effective chromogenic groups, a convenient, precise, and real-time assay for the detection of methyl mercaptan (CH 3 SH) still remains many huge challenges, but it is of great importance to the food and agribusiness related industries. In this work, we proposed an interesting and efficient fluorescence sensing strategy-based alcohol oxidase (AOX)-triggered in situ synthesis of bovine serum albumin-stabilized copper nanoclusters (BSA-CuNCs) for sensitive and selective detection of CH 3 SH. In the presence of CH 3 SH, AOX-assisted O 2 could catalyze it to be H 2 O 2 , which could further trigger BSA-Cu 2+ system to in situ synthesize of BSA-CuNCs, emitting fluorescence signals. On this basis, CH 3 SH concentration-dependent fluorescence emission of BSA-CuNCs was observed, thus allowing for developing a novel fluorescence sensing platform for reporting the levels of CH 3 SH with a broad linear range from 1.0 to 300.0 μM and a low detection limit of 0.19 μM. More significantly, we exploited this sensing strategy to monitor CH 3 SH in real ham samples with acceptable results. This work gives a new insight into applying in situ synthesis strategy to develop a new category of fluorescence sensing platform, achieving convenient, low-cost, reliable, and precise measurements in real food and agriculture-related systems, thereby manifesting a promising potential in food safety monitoring.
研究领域:
分析化学
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食品科学
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纳米技术
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DOI
高影响因子
mBio
·
2024
·Vol. 15
·期 3
·
IF 5.1
Qun Cao,Xuanyu Liu,Qingda Wang,Zongzheng Liu,Yongzhen Xia,Luying Xun,Huaiwei Liu
Methanethiol (MT) is a sulfur-containing compound produced during dimethylsulfoniopropionate (DMSP) degradation by marine bacteria. The C–S bond of MT can be cleaved by methanethiol oxidases (MTOs) to release a sulfur atom. However, the cleaving process remains unclear, and the species of sulfur product is uncertain. It has long been assumed that MTOs produce hydrogen sulfide (H2S) from MT. Herein, we studied the MTOs in the Rhodobacteraceae family—whose members are important DMSP degraders ubiquitous in marine environments. We identified 57 MTOs from 1,904 Rhodobacteraceae genomes. These MTOs were grouped into two major clusters. Cluster 1 members share three conserved cysteine residues, while cluster 2 members contain one conserved cysteine residue. We examined the products of three representative MTOs both in vitro and in vivo. All of them produced sulfane sulfur other than H2S from MT. Their conserved cysteines are substrate-binding sites in which the MTO–S–S–CH3 complex is formed. This finding clarified the sulfur product of MTOs and enlightened the MTO-catalyzing process. Moreover, this study connected DMSP degradation with sulfane sulfur metabolism, filling a critical gap in the DMSP degradation pathway and representing new knowledge in the marine sulfur cycle field.
研究领域:
微生物学
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环境科学
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海洋生物学
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DOI
PubMed
高影响因子
Foods
·
2023
·Vol. 12
·期 13
·2464
·
IF 5.2
Guihu Zhang,Peng Xiao,Youqiang Xu,Honghua Li,Hehe Li,Jinyuan Sun,Baoguo Sun
Baijiu, a prevalent alcoholic beverage, boasts over 2000 aroma compounds, with sulfur-containing compounds being the most influential in shaping its flavor. Benzenemethanethiol, a distinctive odorant in baijiu, is known to enhance the holistic flavor profile of baijiu. Despite its importance, there is very little literature on the biotransformation mechanism of benzenemethanethiol. Thus, extensive research efforts have been made to elucidate the formation mechanism of this compound in order to improve baijiu production. In this study, 12 yeast strains capable of generating benzenemethanethiol were isolated from baijiu daqu, and theSaccharomyces cerevisiaestrain J14 was selected for further investigation. The fermentation conditions were optimized, and it was found that the optimal conditions for producing benzenemethanethiol were at 28 °C for 24 h with a 4% (v/v) inoculum of 3.025 g/L L-cysteine. This is the first time that yeast has been shown to produce benzenemethanethiol isolated from the baijiu fermentation system. These findings also suggest that benzenemethanethiol can be metabolized by yeast using L-cysteine and benzaldehyde as precursor substrates.Keywords:Saccharomyces cerevisiae;baijiu;daqu;benzenemethanethiol;formation mechanism
研究领域:
发酵科学
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食品科学
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微生物学
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生物化学
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DOI
PubMed
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2018
·Vol. 165
·期 7
·B335
·
IF 3.662
Ahmat Ali,Tursun Abdiryim,Xueli Huang,Ruxangul Jamal,Rena Simayi
Conducting polymers decorated with noble metals are good electrochemical sensors for biological species. In this work, we developed a polymer of methanethiol-grafted poly(3,4-ethylenedioxythiophene) hollow spheres (Poly(EDOT-MeSH)) using SiO2 nanospheres as a hard template. The Poly(EDOT-MeSH) spheres were used as both a reductant and stabilizer to decorate gold nanoparticles (Au NPs). FTIR, XRD, EDX, SEM and TEM analyses were used to characterize the Poly(EDOT-MeSH)/Au hollow spheres. The chemical bond between S and Au was confirmed by XPS. The electrochemical performance of the Poly(EDOT-MeSH)/Au hollow spheres was determined by cyclic voltammetry (CV) and differential pulse voltammetry (DPV). The results revealed that the Poly(EDOT-MeSH)/Au hollow sphere-based electrochemical sensor possesses an excellent conductivity and high redox reversibility with detection limits (S/N = 3) of 5.3, 0.04 and 0.12 μM in the linear ranges of 50–320 μM, 0.05 μM − 780 μM and 0.8 μM − 250 μM for the determination of AA, DA and UA, respectively. These results will further the development of this type of electrochemical sensor for biological species.
研究领域:
材料科学
·
分析化学
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生物医学工程
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DOI
高影响因子
HIGH PERFORMANCE POLYMERS
·
2013
·
IF 0.85
Chaoyun Luo,Jiandong Zuo,Jianqing Zhao
An epoxy prepolymer with high refractive index, diglycidyl ether of thiodiphenol (DGETP), was synthesized by 4,4′-thiodiphenol and epichlorohydrin via a two-step method. The curing agent o-benzenedimethanethiol (OBDMT) was synthesized by thiourea method. Fourier transform infrared spectroscopy and proton nuclear magnetic resonance were employed to characterize the structures of these resins. The cured product of DGETP and OBDMT was analyzed by differential scanning calorimetry, ultraviolet–visible spectrometer, and Abbe refractometer and compared with the property of traditional curing agent of methyl hexahydrophthalic anhydride (MHHPA) and ordinary bisphenol A diglycidyl ether epoxy prepolymer cured products. The lower curing temperature and glass transition temperature of DGETP than those of MHHPA can be mainly attributed to the strong rotation capability of thioether bond. The zero light transmittance region of DGETP/OBDMT curing adhesive (200–380 nm) was broader than that of the other three. The refractive index of DGETP/OBDMT was up to 1.654.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
ADVANCED SYNTHESIS & CATALYSIS
·
2023
·Vol. 365
·期 7
·1048-1057
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IF 5.4
Xiao-Ling Tang,Ning Li,Yan-Lai Liu,Jing-Peng Li,Kai-Xuan Zhao,Zhi-Qiang Liu,Yu-Guo Zheng
L-Methionine is the unique sulfur-containing amino acid essential for humans and animals, which is widely used in pharmaceutical, food and feed industries. Its green and efficient production has attracted a great deal of attention. Fermentation-enzymatic coupling route is regarded to be promising for L-methionine biosynthesis, while O- succinyl-L-homoserine mercaptotransferase (MetZ) is the key biocatalyst. Exploring and engineering of MetZ with ideal catalytic properties is highly desired. Herein, the MetZ from Chromobacterium violaceum ( Cv MetZ) was screened and through in silico analyses, potential beneficial amino acid residues both at the access channel and around the oxygen anion holes were anchored for site-saturation mutagenesis. The positive mutants were obtained with improved activity for L-methionine biosynthesis using O -succinyl-L-homoserine (OSH) and methyl mercaptan as substrate. The best mutant was further applied for L-methionine production and supply of methyl mercaptan was optimized in a fed-batch approach. The conversion of 100 g/L OSH reached 92% with L-methionine yield of 62.6 g/L, which was well coupled with the OSH fermentation level.
研究领域:
生物化学
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合成生物学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）