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JOURNAL OF ALLOYS AND COMPOUNDS · 2020 · IF 4.65

Synthesis and room-temperature H2S sensing of Pt nanoparticle-functionalized SnO2 mesoporous nanoflowers

Yu-Ping Sun,Yan-Fei Zhao,Hao Sun,Fu-Chao Jia,Parveen Kumar,Bo Liu

Platinum nanoparticle (NP)-functionalized flower-like mesoporous SnO 2 with a high specific surface area (31.6 m 2 g –1 ) and large pore diameter (32.5 nm) was synthesized using a double-template technique. The presence of Pt NPs was confirmed by X-ray photoelectron spectroscopy. Pt NPs with a size distribution of 2–4 nm were anchored on mesopores of the pre-synthesized three-dimensional SnO 2 nanoflowers upon physical mixing. The resulting Pt NP-decorated three-dimensional SnO 2 mesoporous nanoflowers were incorporated into a gas sensor to detect H 2 S. The Pt–SnO 2 sensor exhibited enhanced gas sensing properties toward H 2 S, with a 100 ppb detection limit, fast response, low working temperature, excellent stability, and good selectivity. The 0.3 wt% Pt–SnO 2 sensor exhibited a high response and excellent selectivity to H 2 S at room temperature (response value to 5 ppm H 2 S at 30 °C was 160). The significant improvements in gas sensing properties were attributed to the synergistic effect of the mesoporous nanostructure induced by the double-template method and the catalytic sensitization of the Pt NPs. These findings offer guidance for designing mesoporous materials and low-temperature H 2 S sensors.

研究领域: 材料科学 · 纳米技术 · 气体传感 · 化学传感器 · 纳米材料
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JOURNAL OF MOLECULAR LIQUIDS · 2023 · IF 6

Density, viscosity, and H2S solubility of N-butylmorpholine bromide iron-based ionic liquids

Chao Li,Yun Teng,Huanong Cheng,Hongwei Jin,Kangkang Li,Zhou Feng,Zhonghao Li,Xinshun Tan,Shiqing Zheng

The density and viscosity of N-butylmorpholine bromide iron-based ionic liquids ( r FeCl 3 / [Nbmm]Br) with two iron-morpholine ratios ( r  = 0.8 and 1.0) mol·mol −1 were measured at 303.15–348.15 K and 101.3 kPa. Density and viscosity data were fitted by empirical correlations for temperature. The average relative errors were less than 0.02 % and 2 %, respectively. The density and viscosity decrease with increasing temperature. The density increases with the increase of r , while the viscosity shows the opposite trend. The gas-liquid equilibrium data of H 2 S in r FeCl 3 /[Nbmm]Br were measured by the isochoric pressure drop method at temperatures of 303.15–348.15 K, pressures of 0–200 kPa, and r of 0.8 and 1.0 mol·mol −1 . The total solubility of H 2 S increases with decreasing temperature, increasing pressure, and decreasing r . The measured solubility data were fitted by the reaction equilibrium thermodynamic model. Chemical reaction equilibrium constant and the Henry's constant at different temperatures and different r were obtained. The average relative error of model fitting is less than 3 %. The results show that the chemical reaction equilibrium constant and the Henry’s constant both decrease with the increase of r , and decrease of temperature. Effect of molecular structure on reaction equilibrium constants was explained by quantum chemistry calculation. The absorption of H 2 S in r FeCl 3 / [Nbmm]Br at low pressure is dominated by chemical absorption. With the increase of pressure, the proportion of physical absorption continues to increase, and gradually occupies the main part.

CAS / MDL: 7439-89-6
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AICHE JOURNAL · 2023 ·Vol. 69 ·期 7 ·e18087 · IF 3.7

H2S absorption with deep eutectic solvents: Low partial pressure capture and thermodynamic analysis

Bo Wang,Xuhao Xie,Lurui Wan,Wenbo Zhao,Yuan Chen

In the present work, a series of deep eutectic solvents (DESs) based on organic amine as hydrogen bond acceptors (HBAs), and ethylene glycol (EG) as hydrogen bond donor (HBD) were prepared for the H 2 S absorption. Thermal decomposition temperature, HBA mass ratios, alkalinity and structure effect on absorption behavior were systematically investigated. The reaction mechanism was demonstrated by FT-IR and 1 H NMR spectroscopy. The reaction equilibrium constants, Henry constant, enthalpy and entropy change were calculated based on the thermodynamic model to reveal the interactions between DESs and H 2 S. It was found that H 2 S absorption capacities of the most of DESs with HBA/HBD mass ratio of 1:4 was close to 1 mol/mol at 303.15 K and 0.2 bar. The absorption capacity of DESs depends on the alkalinity and structure of HBAs; Additionally, a good linear correlation between the alkalinity of HBA and the absorption equilibrium constant (ln K ) of DESs to H 2 S was found.

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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Selective removal of H2S over CO2 in a membrane gas–liquid microdisperison microreactor

Yuchao Chen,Yubin Wang,Zifei Yan,Jian Deng,Guangsheng Luo

Efficient selective removal of H 2 S over CO 2 is the critical absorption process for the gas desulfurization in the petrochemical and refining industries. In this work, we tried to achieve high-selective removal of H 2 S from a mixed gas with CO 2 using a nonaqueous methyldiethanolamine solution in a membrane gas–liquid microdispersion microreactor. The influence of structural parameters and operation parameters on the removal efficiency of H 2 S and CO 2 were systematically investigated. In addition, the mechanism of selective absorption H 2 S over CO 2 was explained in detail. Furthermore, the selective absorption performance of the membrane microdispersion microreactor was compared with other devices. The results showed that the H 2 S removal efficiency and selective factor could be up to 99.4 % and 16.6, respectively. The selectivity factor of H 2 S to CO 2 in the membrane microdispersion microreactor is higher than that of most of reported devices. This work provides a promising selective absorption H 2 S device and technology for the process intensification of gas desulfurization.

CAS / MDL: 105-59-9
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CERAMICS INTERNATIONAL · 2023 · IF 5.2

Porous-Pt-CuO-driven electrochemical biosensor for tracking of endogenous H2S biomessenger molecules

Xiao Zhang,Qianhui Wei,Hongbin Zhao,Feng Wei,Tengfei Li

Hydrogen sulfide (H 2 S) is considered to be the third endogenous gas messenger after nitric oxide and carbon monoxide , and is closely related to physiological and pathological functions of human being. Rapid and real-time monitoring of endogenous H 2 S production in living cells is of great significance for clinical diagnoses of related disease and in-depth investigation of pathological processes. The application of electrochemical sensors has become a promising method to achieve real-time H 2 S monitoring comparing to other methods. Up to now, low-cost, and highly sensitive electrocatalysts for H 2 S detection are conspicuously scarce. Herein, we developed a high-efficient method to construct a H 2 S electrochemical sensor, which configure dissolved–H 2 S–sensitive electrochemical sensor using porous Pt-modified copper oxide (Pt–CuO) as electrocatalyst. The obtained sensor possessed remarkable H 2 S detection performance, achieving the detection limit of 0.5 ppm and apparent selectivity toward various gases (e.g., ammonia, nitrogen dioxide , and carbon dioxide). The electrochemical sensor was also applied for monitoring H 2 S released from mesenchymal stem cells. The enhanced sensing performance was attributed to: (1) electrocatalytic reaction between CuO and [H 2 S] (H 2 S and HS − ) was observed in the cyclic voltammetry curves with oxidation current peaks; (2) Pt catalytic activity promoted electron transfer during the detection process and further decreasing Pt–CuO resistance; and (3) enhanced diffusion of detection molecules/ions, which increased the reactivity sites through forming cross porous structures using sodium carbonate as sacrifice template. The proposed Pt–CuO-based electrochemical sensor shows great potential for applications in clinical diagnoses, and provides effective means to understand the role of H 2 S in biological processes.

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ANALYTICA CHIMICA ACTA · 2023 · IF 6.2

Two-dimensional black phosphorus/tin oxide heterojunctions for high-performance chemiresistive H2S sensing

Yong Zhou,Zhihao Hu,Hongchao Zhao,Yanjie Wang,Jing Li,Cheng Zou

Hydrogen sulfide (H 2 S) emission from industrial fields and bacteria decomposing of sulfur-containing organic matter poses a significant impact on human health and atmospheric environment, thus necessitating the development of a H 2 S sensor with high sensitivity and exclusive selectivity especially at a very low dose. Chemiresistive sensors based on traditional metal oxides were readily limited by the elevated operating temperature and severe cross-sensitivity. To overcome these obstacles, we prepared two dimensional (2D) tin oxide (SnO 2 ) nanosheets decorated with thin black phosphorus (BP) as the sensing layer of MEMS H 2 S sensors. Compared with pure SnO 2 counterparts, BP-SnO 2 sensors demonstrated lower optimal working temperature (130 °C vs. 160 °C), higher response (8.1 vs. 4.6) and faster response/recovery speeds (39.8 s/47.4 s vs. 79 s/140 s) toward 5 ppm H 2 S as well as larger sensitivity (1.3/ppm vs. 0.342/ppm). In addition, favorable repeatability, long-term stability, selectivity and humidity tolerance were exhibited. Thin BP not only served as an excellent conductivity platform within the composites, but enriched the adsorption sites by constructing p-n heterojunctions and introducing more oxygen vacancy , thus separately accelerating and strengthening the gas-solid interaction. This study showcased the application superiorities of BP nanosheets in the field of gas sensing, simultaneously providing a new strategy for trace H 2 S sensing via the 2D heterojunctions.

CAS / MDL: 57-09-0
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AICHE JOURNAL · 2014 ·Vol. 60 ·期 12 ·4232-4240 · IF 2.581

Protic ionic liquids for the selective absorption of H2S from CO2: Thermodynamic analysis

Kuan Huang,Xiao-Min Zhang,Yun Xu,You-Ting Wu,Xing-Bang Hu,Yun Xu

The solubilities of H 2 S and CO 2 in four protic ionic liquids (PILs)—methyldiethanolammonium acetate, methyldiethanolammonium formate, dimethylethanolammonium acetate, and dimethylethanolammonium formate were determined at 303.2–333.2 K and 0–1.2 bar. It is shown PILs have higher absorption capacity for H 2 S than normal ionic liquids (ILs) and the Henry's law constants of H 2 S in PILs (3.5–11.5 bar at 303.2 K) are much lower than those in normal ILs. In contrast, the solubility of CO 2 in PILs is found to be a magnitude lower than that of H 2 S, implying these PILs have both higher absorption capacity for H 2 S and higher ideal selectivity of H 2 S/CO 2 (8.9–19.5 at 303.2 K) in comparison with normal ILs. The behavior of H 2 S and CO 2 absorption in PILs is further demonstrated based on thermodynamic analysis. The results illustrate that PILs are a kind of promising absorbents for the selective separation of H 2 S/CO 2 and believed to have potential use in gas sweetening. © 2014 American Institute of Chemical Engineers AIChE J 60: 4232–4240, 2014

研究领域: 化学工程 · 环境科学
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NEUROGASTROENTEROLOGY AND MOTILITY · 2016 ·Vol. 28 ·期 5 ·687-692 · IF 3.31

A novel pathway for the production of H2S by DAO in rat jejunum

S. Tang,D. Huang,N. An,D. Chen,D. Zhao

Background Hydrogen sulfide (H 2 S) is endogenously generated from L-cysteine (L-Cys) by the enzymes cystathionine- β -synthase (CBS) and cystathionine- γ -Lyase (CSE). Hydrogen sulfide is also produced from D-cysteine (D-Cys) by D-Amino acid oxidase (DAO). Methods The H 2 S production was measured by the methylene blue assay. The expression of DAO was investigated by Western blotting and immunohistochemistry. The short-circuit current ( I sc) was recorded using the Ussing chamber technique. Key Results The epithelium in rat jejunum possesses DAO, and generates H 2 S. D-cysteine, originally used as a negative control for L-Cys, significantly increases the H 2 S release, which is inhibited by I2CA, an inhibitor of DAO. In vitro study by Ussing chamber technique reveals that D-Cys decreases the I sc across the epithelium of the rat jejunum and enhances the Na + -coupled L-alanine transport. Conclusions & Inferences A novel pathway for the production of H 2 S by DAO exists in rat jejunum.

CAS / MDL: 54-47-7 853645-22-4
研究领域: 生理学 · 生物化学 · 胃肠生理学
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

H2S cracking to produce H2 through microwave discharge catalysis of graphitized petroleum coke

Zhiyang Zhao,Dongqiang Cai,Juan Liu,Guifu Zou,Qiang Zhang,Zhanlong Song,Cuiping Wang,Longzhi Li

Direct cracking of hydrogen sulfide (H 2 S) can be used to obtain high purity hydrogen (H 2 ), thus avoiding the waste of hydrogen resources by the traditional Krauss process. Microwave-induced discharge of spherical graphitization petroleum coke (PC) was proposed to solve the problem of low efficiency and high energy consumption of H 2 S cracking. The PC was prepared by microwave-assisted desulfurization and metal (Fe, Co) catalytic graphitization to obtain better discharge effect. Subsequently, the graphitized PC was applied to induce microwave discharge, and the effects of graphitization parameters on the discharge performance were discussed. Lastly, the attention was concentrated on multi-effects catalytic decoupling and cracking kinetic properties of microwave-induced discharge for H 2 S cracking. PC with Fe 1 /Co 2 loading exhibited greater graphitization degree ( I D / I G  = 1.027) (30.7 % than petroleum coke), brought stronger discharge intensity (initial and ending intensity at 4.08 V and 2.73 V in one-hour), and better discharge stability (67 % after one-hour) compared to PC raw coke. H 2 S cracking through microwave discharge catalysis exhibited a favorable catalytic effect, obtained a complete conversion at the initial stage and remained 95.58 % after one-hour, with H 2 yield of 98.1 %. With Fe 1 /Co 2 loading, H 2 S cracking had the least activated energy, 14.96 kJ/mol, which was the multi-effects of microwave discharge catalysis, thermal-catalysis and Co-catalysis. It was further calculated that discharge-catalysis dominated in H 2 S cracking, with the highest contribution, followed by Co-catalysis, and thermal-catalysis had the lowest contribution.

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SENSORS AND ACTUATORS B-CHEMICAL · 2019 · IF 6.393

PdCu alloy nanosheets-constructed 3D flowers: New highly sensitive materials for H2S detection

Hongyuan Shang,Hui Xu,Qingyun Liu,Yukou Du

Hydrogen sulfide (H 2 S) could be directly produced in mammals and recognized as a third gasotransmitter, which are closely associated with physiological and pathological processes. However, the detailed mechanism remains unclear, mainly due to a lack of robust sensors to accurately and quantitatively detect its concentrations in biological samples. Herein, for the first time, we develop a new electrochemical sensor for the detection of H 2 S based on the chemical reaction between copper oxide (CuO and Cu 2 O) and hydrogen sulfide (including H 2 S and HS − ) at a neutral solution (pH 7.4). Interestingly, when Na 2 S exists, copper and its oxide can be converted into Cu 2 S and CuS, resulting in an increase in the oxidation peak current of Cu 2 S-CuS with the increase of Na 2 S concentration, which is a direct evidence confirming the excellent sensor for the H 2 S detection. More importantly, the linear relationship between the oxidation peak currents of Cu 2 S-CuS and Na 2 S concentration is observed from 0.4 μM to 400 μM with a low detection limit of 0.2 μM, and satisfying selectivity. The developed strategy may have a great potential for further understanding the roles that biological H 2 S plays in biological systems.

CAS / MDL: 64-19-7
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2024 · IF 7.7

AChE activity self-breathing control mechanisms regulated by H2Sn and GSH: Persulfidation and glutathionylation on sulfhydryl after disulfide bonds cleavage

Yanwen Zhu,Zhaoliang Hu,Yunen Liu,Tingcai Yan,Ling Liu,Yanqun Wang,Bing Bai

Hydrogen sulfide (H 2 S), or dihydrogen sulfane (H 2 S n ), acts as a signal molecule through the beneficial mechanism of persulfidation, known as the post-translational transformation of cysteine residues to persulfides. We previously reported that Glutathione (GSH) could regulate enzyme activity through S-desulfurization or glutathionylation of residues to generate protein-SG or protein-SSG, releasing H 2 S. However, little is known about the mechanisms by which H 2 S n and GSH affect the disulfide bonds . In this study, we provide direct evidences that H 2 S n and GSH modify the sulfhydryl group on Cys272, which forms disulfide bonds in acetylcholinesterase (AChE), to generate Cys-SSH and Cys-SSG, respectively. Glutathionylation of disulfide is a two-step reaction based on nucleophilic substitution, in which the first C S bond is broken, then the S S bond is broken to release H 2 S. H 2 S n and GSH controlled self-breathing motion in enzyme catalysis by disconnecting specific disulfide bonds and modifying cysteine residues, thereby regulating AChE activity. Here, we elucidated H 2 S n and GSH mechanisms on disulfide in the AChE system and proposed a self-breathing control theory induced by H 2 S n and GSH. These theoretical findings shed light on the biological functions of H 2 S n and GSH on sulfhydryl and disulfide bonds and enrich the theory of enzyme activity regulation.

研究领域: 生物化学 · 分子生物学 · 酶学
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RSC Advances · 2014 ·Vol. 5 ·期 9 ·6879-6885 · IF 3.708

A heating-up method for the synthesis of pure phase kesterite Cu2ZnSnS4 nanocrystals using a simple coordinating sulphur precursor

Ping An,Zhurong Liang,Xueqing Xu,Xin Wang,Hu Jin,Nan Wang,Junxia Wang,Furong Zhu

Pure phase kesterite Cu2ZnSnS4 (CZTS) nanocrystals (NCs) have been successfully synthesized via a heating-up method utilizing metal salts as cation sources and thioacetamide (TAA) as a coordinating sulphur precursor in combination with oleylamine (OAm) as a coordinating ligand and solvent. The slower release of H2S from the metal–TAA complexes, as compared with the commonly used sulphur powder, is crucial for control of the grain size and size distribution of the NCs. As dominating coordinating ligands, OAm led to Sn-rich nuclei and kesterite CZTS NCs. The formation of pure phase kesterite CZTS NCs depends significantly on the temperature and Zn2+/Sn4+ molar ratio of the reaction system. The formation mechanism of the pure phase kesterite CZTS NCs has been clarified taking into account the chemical potentials of the elements involved.

研究领域: 材料科学 · 纳米技术 · 化学工程
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