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H2S
MICROCHEMICAL JOURNAL · 2023 · IF 4.8

Fluorine and oxygen-functionalized silicon nitride with abundant oxygen vacancies for cataluminescence sensing of H2S

Yu Zhou,Hui Gong,Hou-Jing Liu

Efficient, selective and highly sensitive detection of H 2 S is important for environmental protection and human security. Nanomaterials-based cataluminescence (CTL) sensors, especially metal-free catalysts, have been used for gas sensing. Herein, due to the efficient electron transfer and high specific area of silicon nitride (Si 3 N 4 ), combined with the strong electronegativity of fluorine and oxygen, we purposely synthesized F and O-modified Si 3 N 4 (F/O-Si 3 N 4 ) by engineering surface states and catalytic properties. We then used it to construct a H 2 S CTL gas sensor. Compared with other metal-based CTL sensors, the F/O-Si 3 N 4 -based CTL system exhibited high sensitivity and a longer lifetime stability. The detection limit was 0.027 μg mL −1 in the detection range of 0.49–8.17 μg mL −1 , and a relative standard deviation (RSD) of better than 3.3% were obtained. Further research demonstrated the luminescence mechanism, in which the rich oxygen vacancies of Si 3 N 4 promoted the adsorption of O 2 and the formation of F-Si sites due to the catalytic oxidation of H 2 S and the generation of SO 2 *. This served as the main emitter accounting for the strong CTL emission. This work is the first report of the application of Si 3 N 4 as a catalyst for CTL H 2 S sensing. This will expand the methods for enhancing the catalytic activity and practical applications of metal-free materials.

CAS / MDL: 64-17-5 60-29-7
研究领域: 材料科学 · 环境科学 · 传感器技术
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SENSORS AND ACTUATORS B-CHEMICAL · 2021 · IF 7.46

H2S sensor based on two-dimensional MoO3 nanoflakes: Transition between sulfidation and oxidation

Junqiang Bao,Ziyi Zhang,Yangong Zheng

H 2 S is a flammable, explosive, and highly toxic gas; consequently, a high-performance H 2 S sensor based on metal oxides is required. In this study, two-dimensional MoO 3 nanoflakes were synthesized through facile liquid-phase exfoliation. The thickness of the prepared MoO 3 is approximately 4.2 nm. High-performance was obtained using a gas sensor based on two-dimensional MoO 3 nanoflakes at a working temperature of 300 °C. In addition, the lowest detection limit can be in the range of parts per billion, and the sensor exhibits high resistance to humidity. The sensing mechanism is discussed based on the results of ex situ characterizations of the sensing process and computation of the electronic structure. The results indicate that the chemically reversible sensing process is based on the transition between sulfidation and oxidation, where sulfidation promotes the mobility of electrons and increases the conductivity of MoO 3 . This novel sensing mechanism provides a new perspective for the study of H 2 S sensors based on metal oxides.

研究领域: 材料科学 · 化学工程 · 电子工程
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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.

研究领域: 化学工程 · 能源科学 · 材料科学
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Advanced Science · 2015 ·Vol. 2 ·期 11 ·1500101 · IF 0

Experimental Sensing and Density Functional Theory Study of H2S and SOF2 Adsorption on Au-Modified Graphene

Xiaoxing Zhang,Lei Yu,Xiaoqing Wu,Weihua Hu

A gas sensor is used to detect SF 6 decomposed gases, which are related to insulation faults, to accurately assess the insulated status of electrical equipment. Graphene films (GrF) modified with Au nanoparticles are used as an adsorbent for the detection of H 2 S and SOF 2 , which are two characteristic products of SF 6 decomposed gases. Sensing experiments are conducted at room temperature. Results demonstrate that Au-modified GrF yields opposite responses to the tested gases and is thus considered a promising material for developing H 2 S- and SOF 2 -selective sensors. The first-principles approach is applied to simulate the interaction between the gases and Au-modified GrF systems and to interpret experimental data. The observed opposite resistance responses can be attributed to the charge-transfer differences related to the interfacial interaction between the gases and systems. The density of states and Mulliken population analysis results confirm the apparent charge transfer in Au-modified GrF chemisorption, whereas the van der Waals effect dominates the pristine graphene adsorption systems. Calculation results can also explicate the significant SOF 2 responses on Au-modified GrF. This work is important in graphene modulation and device design for selective detection.

CAS / MDL: 16940-66-2 13453-07-1
研究领域: 材料科学 · 物理化学
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ANALYTICA CHIMICA ACTA · 2021 · IF 6.558

A bifunctional fluorescent probe based on “AND logic” for the simultaneous recognition of H2S/HNO and its bioimaging applications

Huawei Niu,Xintong Mi,Xinting Hua,Yuanyuan Zhang,Yaping Zhai,Fangyuan Qin,Yong Ye,Yufen Zhao

The reaction of NO and H 2 S to form HNO is a classical pathway in physiological conditions. The reported single recognition-type fluorescent probes are difficult to track precisely the relationships of H 2 S and HNO. It is necessary to develop a bifunctional fluorescence probe ( NJA ) for monitoring simultaneously the production of endogenous HNO and H 2 S. Using 7-Nitrobenzofurazan (NBD) and 2-(diphenylphosphine) benzoate as recognition sites, the obatined NJA can detect specifically HS − and HNO. The detection limit of HS − and HNO are 0.46 μM and 1.42 μM, respectively. Based on the dual recognition sites and input signals of the probe, a molecular “AND” logic gate was established to detect successfully H 2 S and HNO in MCF-7 cells. NJA based on “AND logic” provided a simple and robust tool for monitoring the production of endogenous HNO correlative with H 2 S and NO in living cells.

研究领域: 生物化学 · 细胞生物学
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JOURNAL OF NANOBIOTECHNOLOGY · 2021 ·Vol. 19 ·期 1 ·1-14 · IF 10.435

Sulourea-coordinated Pd nanocubes for NIR-responsive photothermal/H2S therapy of cancer

Guo Xiaoyang,Liu Jia,Jiang Lingdong,Gong Wanjun,Wu Huixia,He Qianjun

Background Photothermal therapy (PTT) frequently cause thermal resistance in tumor cells by inducing the heat shock response, limiting its therapeutic effect. Hydrogen sulfide (H2S) with appropriate concentration can reverse the Warburg effect in cancer cells. The combination of PTT with H2S gas therapy is expected to achieve synergistic tumor treatment.Methods Here, sulourea (Su) is developed as a thermosensitive/hydrolysable H2S donor to be loaded into Pd nanocubes through in-depth coordination for construction of the Pd-Su nanomedicine for the first time to achieve photo-controlled H2S release, realizing the effective combination of photothermal therapy and H2S gas therapy.Results The Pd-Su nanomedicine shows a high Su loading capacity (85 mg g−1), a high near-infrared (NIR) photothermal conversion efficiency (69.4%), and NIR-controlled H2S release by the photothermal-triggered hydrolysis of Su. The combination of photothermal heating and H2S produces a strong synergetic effect by H2S-induced inhibition of heat shock response, thereby effectively inhibiting tumor growth. Moreover, high intratumoral accumulation of the Pd-Su nanomedicine after intravenous injection also enables photothermal/photoacoustic dual-mode imaging-guided tumor treatment.Conclusion sThe proposed NIR-responsive heat/H2S release strategy provides a new approach for effective cancer therapy.Graphic abstract

研究领域: 纳米技术 · 癌症治疗 · 光热治疗 · 气体治疗 · 生物医学工程
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ANALYTICAL CHEMISTRY · 2024 · IF 6.7

Photoelectrochemical Sensor for H2S Based on a Lead-Free Perovskite/Metal–Organic Framework Composite

Mengfan Mao,Yexin Zu,Yating Zhang,Yongzhen Qiu,Yue Lin,Fang Luo,Zuquan Weng,Cuiying Lin,Bin Qiu,Zhenyu Lin

Halide perovskites have emerged as a highly promising class of photoelectric materials. However, the application of lead-based perovskites has been hindered by their toxicity and relatively weak stability. In this work, a composite material comprising a lead-free perovskite cesium copper iodide (CsCu2I3) nanocrystal and a metal–organic framework (MOF-801) has been synthesized through an in situ growth approach. The resulting composite material, denoted as CsCu2I3/MOF-801, demonstrates outstanding stability and exceptional optoelectronic characteristics. MOF-801 may serve a dual role by acting as a protective barrier between CsCu2I3 nanocrystals and the external environment, as well as promoting the efficient transfer of photogenerated charge carriers, thereby mitigating their recombination. Consequently, CsCu2I3/MOF-801 demonstrates its utility by providing both stability and a notably high initial photocurrent. Leveraging the inherent reactivity between H2S and the composite material, which results in the formation of Cu2S and structural alteration, an exceptionally sensitive photoelectrochemical sensor for H2S detection has been designed. This sensor exhibits a linear detection range spanning from 0.005 to 100 μM with a remarkable detection limit of 1.67 nM, rendering it highly suitable for precise quantification of H2S in rat brains. This eco-friendly sensor significantly broadens the application horizon of perovskite materials and lays a robust foundation for their future commercialization.

研究领域: 材料科学 · 分析化学 · 环境科学 · 生物传感器
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SENSORS AND ACTUATORS B-CHEMICAL · 2023 · IF 8.4

2D/0D SnSe2/TiO2 nanocomposites for trace NO2 detection under H2S interference at room temperature

Chengjiu Zhao,Xuezheng Guo,Yanqiao Ding,Chengyao Liang,Bingsheng Du,Wen Niu,Weijie Qu,Yijie Shi,Shuren Cong,Gang Meng,Yong He

Complex gas environments and the demand for room temperature detection will provide challenges for chemo-resistive-type gas sensors in a variety of applications. In this work, 2D/0D SnSe 2 /TiO 2 composite is used as a sensing material, displaying good sensitivity and specificity to ppb-level NO 2 at ambient temperature (25 °C). The response value and time of the SnSe 2 /TiO 2 sensor are 207 % and 139s when exposed to 100 ppb NO 2 , as opposed to 62 % and 183s for the pristine SnSe 2 sensor. The composite sensor also offers great long-term stability for NO 2 and good gas selectivity. Notably, the SnSe 2 /TiO 2 sensor's mixed gases (NO 2 +H 2 S) measurement is done to examine its NO 2 detection capacity in the presence of interfering gas. The constructed composite sensor can accurately detect NO 2 even if the concentration of the reductive interfering H 2 S is 66.7 times higher than that of the oxidative target NO 2 . The effective usage of SnSe 2 modified by TiO 2 for low-concentration, room-temperature NO 2 detection in a complex gas environment is shown by the composite sensor's pleasing gas detection results.

CAS / MDL: 7446-08-4
研究领域: 材料科学 · 环境科学 · 传感器技术
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JOURNAL OF HAZARDOUS MATERIALS · 2020 · IF 9.038

Effects of Process Parameters on Sulfur Migration and H2S Generation during Supercritical Water Gasification of Sludge

Junhao Lin,Qinxiong Liao,Yaping Hu,Rui Ma,Chongwei Cui,Shichang Sun,Xiangli Liu

The generation of sulfur-containing pollution products affects the quality of biofuels obtained from the supercritical water gasification (SCWG) of sludge . This study investigates the effects of the gasification temperature, moisture content, and reaction atmosphere on the evolution of sulfur-containing compounds. The results showed that temperature was the key parameter causing the migration of sulfur from sludge to biogas and liquid products. The sludge decomposition reaction was dominated by ionic reactions at 360 °C, while the decomposition of organic matter was converted to free radical reactions as the temperature increased from 380 °C to 440 °C. The mercaptan and thioether contents of the bio-oil decreased to 0.3% at 440 °C. Correspondingly, the concentration of H 2 S increased from 6.7 ppm to 38.0 ppm. The decomposition of organic sulfur with an unstable structure (S-H bond and S-C bond) was the main cause of the increase in the content of H 2 S. Additionally, the solubility and oxidation properties of supercritical water were extremely strong. Some sulfur-containing organic compounds were converted into SO 4 2- via hydrolysis and oxidation reactions, forming sulfate crystals with heavy metals in the bio-char, which aided in achieving the synergistic immobilization of sulfur and heavy metals.

研究领域: 环境科学 · 能源工程
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CHEMICAL ENGINEERING SCIENCE · 2024 · IF 4.1

Insights into the coupling of H2S adsorption and subsequent C4H4S hydrogenation over Ni–Mo composite adsorbents

Yeshuang Wang,Zhelin Su,Mingxian Duan,Huiling Fan,Ju Shangguan,Chao Yang

Metal oxides-based adsorbents used for desulfurization encounter significant challenges during practical application owing to their inferior reusability and the nature of solid waste of their desulfurization products. This situation might be alleviated to some extent through a rational design of Ni–Mo composite, enabling them firstly to be used as adsorbents for H 2 S removal, and then being utilized as catalysts after desulfurization for C 4 H 4 S hydrogenation. The Ni–Mo composites before and after desulfurization were characterized using XRD, FT-IR, SEM, N 2 adsorption–desorption, XPS, CO 2 -TPD and H 2 -TPR techniques. The experimental findings suggested that Ni and Mo species function as primary active sites for H 2 S adsorption and C 4 H 4 S hydrogenation reactions, respectively. The Ni and Mo composite greatly facilitated the coupling of these two reactions due to the formation of NiMoO 4 phase. This novel active phase not only boosted the interaction between metal and H 2 S but also promoted the formation of weak and moderate alkaline sites, thereby significantly enhancing desulfurization performance. Importantly, this active phase fostered the sulfurization of Mo species and transforming into a Ni–Mo–S component, further favoring the subsequent catalytic reaction in C 4 H 4 S hydrogenation. Consequently, the prepared Ni–Mo composite oxides exhibited excellent properties in H 2 S adsorption and C 4 H 4 S hydrogenation activity, surpassing the capabilities of single metal adsorbents and commercial hydrogenation catalysts.

CAS / MDL: 12054-85-2
研究领域: 化学工程 · 催化材料科学
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APPLIED SURFACE SCIENCE · 2024 · IF 6.3

2D electrodeposition assembly of Cu/Cu2O nanoarrays for low temperature H2S sensing

Huijuan Chen,Fangrui Gao,Wenbin Ren,Lulu Du,Kaifeng Xue,Pinhua Zhang,Changmin Shi,Li Lv,Guangliang Cui

Ultra-sensitive hydrogen sulfide (H 2 S) detection technology at low temperatures provides critical support for the application of one-time alert systems under extreme conditions, ensuring reliable monitoring of H 2 S in low-temperature environments and enhancing safety and practicability. In this study, we developed a novel low-temperature H 2 S sensor based on Cu/Cu 2 O nanoarrays, prepared through a combination of 2D electrodeposition in situ assembly and the hydrothermal method. The heterointerface between Cu nanowires and Cu 2 O nanocubes presents a high barrier, which can be modulated to zero through the formation of continuous Cu x S conductive channels via the vulcanization reaction, thereby achieving excellent sensitivity and selectivity towards H 2 S at low temperatures. At freezing temperatures and low H 2 S concentrations (≤20 ppm), the sensors show ideal recovery and reasonable sensitivity (R=150 to 10 ppm H 2 S at 0 °C). However, the response significantly increases (R=5624 at 10 ppm H 2 S at 50 °C) and recovery is lost under reversed conditions. First-principles calculations have confirmed that the enhanced H 2 S adsorption at the heterointerface is the primary reason for the robust response observed at 0 °C. Experimental results demonstrate that the Cu/Cu 2 O nanoarrays were capable of rapid detection of H 2 S at low temperatures through modulation of heterointerface barriers.

研究领域: 材料科学 · 化学传感器 · 表面科学
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MICROCHEMICAL JOURNAL · 2025 · IF 5.1

Preparation and sensing performance investigation of ZIF-8-derived ZnO-supported Ag nanoparticle assemblies for trace H2S gas detection

Lei Zhang,Zhen Zhao,Hongming Zhang,Wanli Jiao

To detect trace hydrogen sulfide (H 2 S) safely, more sensitively and less expensively, a new synthesized ZIF-8-derived ZnO-supported Ag nanoparticle assemblies have been investigated. In the successful formation, ZIF-8 was synthesized in room temperature aqueous solution, followed by ultrasonication to produce Ag + /ZIF-8 compounds, and yielded Ag/ZnO assemblies after sintering. Various characterizations have been done to confirm the morphology, surface chemical state and electron distribution by XRD, SEM, XPS, BET and DRIFT. The sensing test results indicate that at an exciting operating temperature of 100 °C, the A-2 labeled sensor exhibits excellent H 2 S detection capabilities, including a response value of 104 for 2.5 ppm H 2 S, the minimum detection limit of 1.1 ppb, satisfied selectivity, significant resilience against humidity and long time stability. More significantly, a valuable test of 140 h real time detection of the H 2 S emission from fresh fish meat has been performed successfully, providing effective data for protein spoilage assessment. Rhombic dodecahedron structure, catalysis of Ag nanoparticles and overflow effect of H 2 S result in the distinct sensing mechanism, providing novel insights and theoretical foundations for developing highly efficient trace H 2 S gas sensors.

研究领域: 材料科学 · 传感器技术 · 环境监测
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