RSC Advances
·
2019
·Vol. 9
·期 20
·11046-11053
·
IF 3.049
Pengjian Wang,Junfeng Hui,Tingbiao Yuan,Peng Chen,Yue Su,Wenjie Liang,Fulin Chen,Xiaoyan Zheng,Yuxin Zhao,Shi Hu
Ultrafine nanoparticles of W-doped SnO2 with an average diameter of 6 nm were fabricated via a facile hydrothermal method. The material shows a reduced particle size and enhanced response to H2S gas as compared to the pristine SnO2 nanoparticles. The detection limit can be down to 100 ppb while the response time and recovery time of the 5%-doped one are reduced to 17 s and 7 s respectively. In addition, the material shows impressive long-term stability of the response through 40 cycles of injection with 10 ppm H2S, which is attractive for designing a durable hydrogen sulfide sensor. The doping of W results in the reduction of size and modification of the electronic band structure of SnO2, which reduces the response time and recovery time and further improves the sensing durability of the materials.
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INORGANICA CHIMICA ACTA
·
2023
·
IF 2.8
Zheng Li,Jing Wang,Xiaoxia Peng,Yu Chen,Mengyuan Geng
Hydrogen sulfide plays an essential roles in physiological and pathophysiological process. It is still a challenge to design a simple and reasonable H 2 S-specfic fluorescent probe. Herein, we develop a simple reaction-based fluorescent probe for detecting H 2 S in DMF/Tris-HCl buffer system. Fluorescence emission spectra were used to investigate the recognition performance of probe L towards hydrogen sulfide. The results shown that probe L has a specific recognition towards hydrogen sulfide over other tested metal cations and anions with a rapid response. The probe L combined with H 2 S in a 1: 1 manner with a detection limit of 0.372 μM. The appropriate pH range for detecting H 2 S was 4 ∼ 8. The proposed recognition mechanism was studied by fluorescence titration spectrum, Job’s plot, 1 H NMR titration experiment and mass spectrometry analysis. Moreover, probe L was applied in real water samples, test strips and fluorescent films to detect H 2 S successfully.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2022
·Vol. 24
·期 46
·28530-28539
·
IF 3.945
Yong-Hui Zhang,Ying-Ying Li,Xuan-Yu Yang,Fei-Long Gong,Jun-Li Chen,Ke-Feng Xie,Hao-Li Zhang,Shao-Ming Fang
Metal oxide sensors face the challenge of high response and fast recovery at low operating temperatures for the detection of toxic and flammable hydrogen sulfide (H2S) gases. Herein, novel In-doped ZnO with a sunflower-like structure and tunable surface properties was rationally synthesized. The substitutional In atom in the ZnO crystal can dramatically enhance the concentration of oxygen vacancies (Ov), the In–ZnO sites are responsible for fast recovery, and the formation of sub-stable sulfide intermediates gives rise to the high response towards H2S. As a result, the response of the optimized 4In–ZnO sensor is 3538.36 to 50 ppm H2S at a low operating temperature of 110 °C, which is 106 times higher than that of pristine ZnO. Moreover, the response time and recovery time to 50 ppm H2S are 100 s and 27 s, respectively, with high selectivity and stability. First-principles calculations revealed that 4In–ZnO with rich Ov exhibited higher adsorption energy for the H2S molecule than pristine ZnO, resulting in effortless H2S detection. Our work lays the foundation for the rational design of highly sensitive gas sensors through precise doping of atoms in oxygen-rich vacancies in semiconductor materials.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Xue-Yan Wu,Li-Yuan Zhu,Jie Sun,Kai-Yue Zhu,Xiao-Yong Miao,Meng-Yang Liu,Xue-Feng Zhao,Hong-Liang Lu
Pt nanoparticle (NP)-modified SnO2–ZnO (SnO2–ZnO–Pt) core–shell nanosheets (NSs) for hydrogen sulfide (H2S) gas sensing were successfully synthesized via atomic layer deposition, hydrothermal method, and magnetron sputtering. More importantly, the SnO2–ZnO–Pt NS sensing materials were synthesized in situ on microelectromechanical system (MEMS) devices, which are expected to be high-performance gas sensors with superior sensitivity, great selectivity, good reproducibility, and low power consumption. To be specific, the SnO2–ZnO–Pt NSs displayed a high sensitivity (Ra/Rg) of 30.43 and an excellent selectivity when detecting 5 ppm H2S at an operating temperature of 375 °C. Their rate of resistance change was 29.43, which was about 24 and 9 times those of the pristine SnO2 NS (∼1.25) and SnO2–ZnO core–shell NS (∼3.43) sensors, respectively. These substantially improved sensing properties could be mainly attributed to the formation of heterojunctions, catalytic sensitization effect, and increased specific surface area of Pt NP modification. Thus, the proposed SnO2–ZnO–Pt NS gas sensors demonstrate great potential as a high-performance sensing material for application in H2S gas sensors.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Li-Wen Mao,Li-Yuan Zhu,Tao Tao Wu,Lei Xu,Xuan-Hong Jin,Hong-Liang Lu
Heterostructured Nb 2 O 5 /SnO 2 core-shell nanorods are synthesized by a facile hydrothermal strategy and atomic layer deposition (ALD). The SnO 2 shell thicknesses varying from 7 to 34 nm exhibit a significant impact on sensing performance. The response enhancement mechanism of the Nb 2 O 5 /SnO 2 core-shell nanorods is illustrated based on the electron-depletion model. The Nb 2 O 5 /SnO 2 core-shell nanorods gas sensors were synthesized based on the micro-electromechanical systems (MEMS), which could provide variable operating temperatures for the gas sensors with highly integrated design and low power consumption. The response of the Nb 2 O 5 /SnO 2 core-shell nanorods gas sensor deposited with 20 nm SnO 2 shell towards 20 ppm H 2 S at 275 °C was 4.0, which showed a 3.8-fold of improvement compared with pristine Nb 2 O 5 nanorods. Furthermore, the well-structured core-shell nanorods gas sensors maintained stable performance after three months, presenting long-term stability and repeatability. The proposed Nb 2 O 5 /SnO 2 core-shell nanorods gas sensors demonstrate a potential strategy for the practical application in oil and gas drilling platforms and other industrial fields.
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FUEL
·
2020
·
IF 5.578
Long Ma,Shuzhen Chen,Changlei Qin,Susu Chen,Weiyang Yuan,Xu Zhou,Jingyu Ran
Li 4 SiO 4 is a well-acknowledged CO 2 sorbent in the sorption-enhanced reforming system for low-cost H 2 production with a high purity. However, the inevitable presence of H 2 S in the biomass-derived syngas etc. could possibly affect the in-situ CO 2 adsorption significantly, which is important but has never been reported. In this work, the adsorption of CO 2 using Li 4 SiO 4 was investigated under varying H 2 S concentrations and reaction temperatures, and a series of characterization techniques were utilized to understand the effect of H 2 S and its action mechanism. The results show that the presence of H 2 S causes a rapid loss-in-capacity of Li 4 SiO 4 in capturing CO 2 during the cyclic reactions, and a higher concentration greatly exacerbates the problem. Moreover, the negative impact of H 2 S is found to have a strong relationship to the reaction temperature. It is proposed that at 325~475 °C, Li 4 SiO 4 and H 2 S react to form bits of Li 2 S and some kinds of sulfates, and at 625~775 °C, a large amount of dense KLiSO 4 is generated covering the surface of the sorbent. In contrast, at a high temperature above 925 °C, sintering of Li 4 SiO 4 plays a critical role, leading to a significant change on its microstructure.
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CATALYSIS LETTERS
·
2020
·Vol. 151
·期 6
·1728-1737
·
IF 2.482
Huang Huiting,Shen Lijuan,Yang Shuai,Hu Wenjian,Zhang Lili,Feng Jianyong,Jiang Lilong,Yu Tao,Li Zhaosheng,Zou Zhigang
Abstract In addition to traditional metal oxides, N-containing compound would become efficient catalyst for H 2 S selective oxidation. TaON and Ta 3 N 5 , taking as examples, with porous structure are able to selectively oxidize H 2 S into sulfur. TaON exhibits ca. 99% H 2 S conversion and ca. 89% sulfur selectivity at 250 ℃, while Ta 3 N 5 exhibits near complete H 2 S conversion (~ 100%) and 86% sulfur selectivity at 250 ℃. TaON of lower N content shows higher sulfur selectivity (~ 90–100%) above 130 ℃, compared with that (~ 86–95%) over Ta 3 N 5 . Whereas, Ta 3 N 5 of higher N content demonstrates higher H 2 S conversion (~ 30–40%) below 160 ℃, compared with that (~ 6–30%) over TaON. Temperature programmed desorption results show that Ta 3 N 5 owns larger amount of acid sites and weaker basic sites than TaON. Over Ta 3 N 5 , the reactant molecules could dissociatively adsorb on acid sites more frequently and could be easier to move across the weaker basic sites, thus increasing probability for reaction at low temperature. Manipulating both cations and anions in N-containing compound can alter surface property for optimization of selective H 2 S oxidation. Graphic Abstract
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ENERGY & FUELS
·
2017
·
IF 3.091
Kuan Huang,Jia-Yin Zhang,Xing-Bang Hu,You-Ting Wu
The development of ionic liquid-based absorbents for selective separation of H2S from CO2 is of interest to the natural gas industry. In this work, a series of tertiary-amine functionalized protic ionic liquids (TA-PILs) were synthesized by neutralizing one of the tertiary amine groups in diamine compounds with acetic acid, leaving the other tertiary amine group as the functional site for selective absorption of H2S. To overcome the high viscosity of pure ionic liquids, TA-PILs were dissolved in water to give mixed absorbents. The effects of TA-PIL species, TA-PIL concentration, and experimental temperature on the solubilities of H2S and CO2, and absorption kinetics of H2S and CO2 in aqueous TA-PILs were investigated systematically. The reaction equilibrium constants and absorption enthalpy of H2S and CO2 in aqueous TA-PILs were also calculated by correlating the solubility data with a reaction equilibrium thermodynamic model. Results demonstrated that aqueous TA-PILs have high absorption capacities for H2S. Although the equilibrium selectivities of H2S/CO2 in aqueous TA-PILs are minimized, they still display significant kinetic selectivities for the two gases. More importantly, the TA-PILs designed are featured with low cost and facile synthesis, making them more attractive than other functionalized ionic liquids reported in the literature for application in selective separation of H2S from CO2.
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Materials Research Express
·
2017
·Vol. 4
·期 9
·095022
·
IF 1.068
Haojie Duan,Lei Yan,Yue He,Haiying Li,Li Liu,Yali Cheng,Liting Du
In2O3 nanofibers (NFs) and toruloid nanotubes (TNTs) were fabricated by conventional electrospinning process and their sensing properties toward H2S gas were researched. Thermogravimetric analysis, x-ray diffractometry, energy dispersive spectroscopy and scanning electron microscopy were carefully used to investigate the structures, chemical compositions and morphologies of these samples. The novel structure (TNTs) first used nonpolar mineral oil as the control agent of morphology, and the principle of forming toruloid nanotubes was studied. Phase separation plays a critical role in the process of forming toruloid nanotubes structure automatically. The new application of phase separation provided a simple and effective approach for controlling structure. The research indicated that thin-walled toruloid nanotubes showed higher responses toward H2S compared to nanofibers or thick-walled toruloid nanotubes. Additionally, their excellent selectivity can be attributed to the special gas-sensing mechanism of In2O3 for H2S.
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ACS Sensors
·
2024
·
IF 8.2
Huan Wang,Chonghui Zhu,Xiaohui Yan,Zhaorui Zhang,Huashuai Hu,Mengmeng Xu,Yu Liang,Minghui Yang
Fuel cell gas sensors have emerged as promising advanced sensing devices owing to their advantageous features of low power consumption and cost-effectiveness. However, commercially available Pt/C electrodes pose significant challenges in terms of stability and accurate detection of low concentrations of target gases. Here, we introduce an efficient Cu–Pt/CrN-based fuel cell gas sensor, designed specifically for the ultrasensitive detection of hydrogen sulfide (H2S) at room temperature. Compared to the commercial Pt/C sensor, the Cu–Pt/CrN sensor exhibits excellent sensitivity (0.26 μA/ppm), with an increase in the selectivity by a factor of 2.5, and demonstrates good stability over a 2 month period. The enhanced sensing performance can be attributed to the modulation of the electronic arrangement of Pt by Cu, resulting in an augmentation of H2S adsorption. The Cu–Pt/CrN fuel cell gas sensor provides an opportunity for detecting parts per billion-level H2S in various applications.
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JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
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.
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Molecular Catalysis
·
2024
·
IF 3.9
Lina Sun,Ping Ning,Jie Yang,Xin Song,Kai Li
This study used metal oxide-modified metal-organic frameworks to examine H 2 S catalytic oxidation selectivity. The findings revealed that the oxidation mechanisms and products differed between Fe 2 O 3 /UiO-66 and Al 2 O 3 /UiO-66. The dithionates were intermediate products of H 2 S oxidation on Al 2 O 3 /UiO-66, whereas the bisulfates were intermediate products on Fe 2 O 3 /UiO-66. Fe 2 O 3 /UiO-66 showed stronger surface oxidation activity than Al 2 O 3 /UiO-66. The formation of sulfate/SO 2 was primarily attributable to surface oxygen, whereas elemental sulfur was primarily related to lattice oxygen. The product generation processes of H 2 S on Fe 2 O 3 /UiO-66 and Al 2 O 3 /UiO-66 surfaces were as follows: H 2 S → HSO 4 2− → SO 2 → S for Fe 2 O 3 /UiO-66, while H 2 S → S 2 O 4 2− → SO 2 for Al 2 O 3 /UiO-66. H 2 O and surface oxygen have the potential to alter H 2 S adsorption on the catalyst surface. For Fe 2 O 3 , the conversion of H 2 S to SO 2 involves both an oxidation process and a reduction process. For Al 2 O 3 , the conversion of H 2 S to SO 2 includes two oxidation processes. Due to the oxidation step of S 2 O 4 2− limiting the generation of SO 2 , the reduction process of SO 2 was also hindered, which in turn restricted the production of S over Al 2 O 3 . Fe 2 O 3 can achieve the oxidation and removal of H 2 S at lower reaction temperatures, while also creating elemental S.
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