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Small · 2021 ·Vol. 17 ·期 52 ·2105643 · IF 13.281

The Dehydrogenation of H-S Bond into Sulfur Species on Supported Pd Single Atoms Allows Highly Selective and Sensitive Hydrogen Sulfide Detection

Bo Liu,Linjuan Zhang,Yuanyuan Luo,Lei Gao,Guotao Duan

The supported metal catalysts on scaffolds usually reveal multiple active sites, resulting in the occurrence of side reaction and being detrimental to the achievement of highly consistent catalysis. Single atom catalysts (SACs), possessed with highly consistent single active sites, have great potentials for overcoming such issues. Herein, the authors used SACs to modulate kinetic process of gas sensitive reaction. The supported Pd SACs, established by a metal organic frameworks-templated approach, promoted greatly the detection capacity to hydrogen sulfide (H 2 S) gas with a very high sensitivity and selectivity. Density functional theory calculations show that the supported Pd SACs not only increased the number of electrons transferring from H 2 S molecules to Pd SACs, but strengthened surface affinity to H 2 S. Moreover, the H  S bonds of H 2 S molecules absorbed on Pd atomic sites are more likely to be dehydrogenated directly into sulfur species. Significantly, quasi in situ XPS analysis confirmed the presence of sulfur species during H 2 S detection process, which may be a major cause for such detection signal. Based on these results, a suitable sensing principle for H 2 S gas driven by Pd SACs was put forward. This work will enrich catalytic electronics in chemiresistive gas sensing.

研究领域: 材料科学 · 催化化学 · 气体传感
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JOURNAL OF COORDINATION CHEMISTRY · 2018 · IF 1.703

Highly selective probe of a copper(II) complex based on a coumarin derivative for hydrogen sulfide detection

Yanmei Chen,Xuefang Shang,Weitong Pan,Congshu Li,Tianyun Wang

A fluorescent probe 1 containing copper(II) had been designed and synthesized based on a coumarin derivative. The molecular structure of probe 1 was characterized by 1H NMR, HRMS, IR, and elemental analysis. The interactions of 1 with biologically important anions and amino acid were determined by UV–Vis, fluorescence, and HRMS titration experiments. Results indicated that probe 1 showed the highest binding ability for HS− among studied anions (AcO−, H2PO4 −, F−, Cl−, Br−, and I−) and cysteine in pure dimethyl sulfoxide (DMSO) and HEPES buffer solution. As we expected, the response of UV–Vis spectra in aqueous solution was stronger than that of pure DMSO solvent. In addition, the binding ability for HS− was not hindered by the existence of other anions. HRMS titration experiment showed that the interacted mechanism was that the copper(II) ion in 1 was captured by HS− and then free ligand released. Furthermore, the detection limit of probe 1 with HS− was carried out through UV–Vis titration showing 1 to be highly sensitive for HS−.

研究领域: 分析化学 · 生物化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Aqueous-phase dual-functional chiral perovskites for hydrogen sulfide (H2S) detection and antibacterial applications in Escherichia coli

Jingran Zhang,Zihan Yuan,Chao Wang,Lele Liu,Yanan Wang,Yurong Guo,Guangjiu Zhao

Perovskite nanocrystals (PNCs) have attracted extensive attention for their potential applications in biology. However, only a handful of PNCs have been scrutinized in the biological domain due to issues such as instability, poor dispersion, and size inhomogeneity in polar solvents. The development of dual-functional perovskite nanomaterials with hydrogen sulfide (H 2 S) sensing and antibacterial capabilities is particularly intriguing. In this study, we prepared chiral quasi-two-dimensional (quasi-2D) perovskite nanomaterials, Bio(S-PEA) 2 CsPb 2 Br 7 and Bio(R-PEA) 2 CsPb 2 Br 7 , that were uniformly dispersed in aqueous media. The effective encapsulation of methoxypolyethylene glycol amine (mPEG-NH 2 ) improved water stability and uniformity of particle size. Circular dichroism (CD) signals were created by the successful insertion of chiral cations. These perovskites as probes showed a rapid and sensitive fluorescence quenching response to H 2 S, and the effect of imaging detection was observed at the Escherichia coli (E. coli) level. As antibacterial agents, their pronounced positive charge properties facilitated membrane lysis and subsequent E. coli death, indicating a significant antibacterial effect. This work has preliminary explored the application of chiral perovskites in biology and provides insight into the development of bifunctional perovskite nanomaterials for biological applications.

研究领域: 生物化学 · 材料科学 · 微生物学
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DYES AND PIGMENTS · 2021 · IF 4.889

A multifunctional BODIPY based fluorescent probe for hydrogen sulfide detection and photodynamic anticancer therapy in HCT116 colon cancer cell

Yun-Yun Quan,Lanlan Fan,Hongyan Shen,Binbin Wu,Shanshan Kong,Yanshu Luo,Zu-Sheng Huang,Xiaoxia Ye

Development of multifunctional probes that can be simultaneously utilized for both efficient hydrogen sulfide detection and photodynamic therapy in cancer cells is in high demand but remains worldwide challenge. Herein, a fluorescent probe DB2T based on a BODIPY structure for H 2 S fluorescence “turn-on” detection together with light sensitive anticancer capacity has been designed and synthesized. The probe DB2T features high selectivity towards H 2 S, excellent low detection limit (6.39 nM), and good biocompatibility . Importantly, the probe DB2T has been satisfactorily applied in fluorescence imaging of exogenous H 2 S in zebrafish, and successfully employed in fluorescence imaging of endogenous H 2 S in HCT116 cell and tumor tissues. Moreover, evaluation of the phototherapy effect demonstrates that the probe DB2T performs well as a photosensitizer for photodynamic ablation of HCT116 cancer cells upon white light irradiation. This work should facilitate significant advances in rational design of fluorescence systems for H 2 S detection and even in the diagnosis and treatment of H 2 S related diseases.

研究领域: 生物化学 · 肿瘤学 · 药物开发
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Ultrathin Hexagonal PbO Nanosheets Induced by Laser Ablation in Water for Chemically Trapping Surface-Enhanced Raman Spectroscopy Chips and Detection of Trace Gaseous H2S

Hao Fu,Guangqiang Liu,Haoming Bao,Le Zhou,Hongwen Zhang,Qian Zhao,Yue Li,Weiping Cai

Lead oxide (PbO) nanosheets are of significance in the design of functional devices. However, facile, green, and fast fabrication of ultrathin and homogenous PbO nanosheets with a chemically clean surface is still desirable. Herein, a simple and chemically clean route is developed for fabricating such nanosheets via laser ablation of a lead target in water for a short time and then ambient aging. The obtained PbO nanosheets are (002)-oriented with microsize in planar dimension and ∼15 nm in thickness. They are mostly hexagonal in shape. Experimental observations of the morphological evolution have revealed that the formation of such PbO nanosheets can be attributed to two processes: (i) laser ablation-induced formation of ultrafine Pb and PbO nanoparticles (NPs) and (ii) PbO NP aggregation and their oriented connection growth. Importantly, a composite surface-enhanced Raman spectroscopy (SERS) chip is designed and fabricated by covering a PbO nanosheet monolayer on a Au NP film. Such a composite SERS chip can be used for the fast and trace detection of gaseous H2S in which the PbO nanosheets can effectively chemically trap H2S molecules, demonstrating a new application of these PbO nanosheets. The response of this chip to H2S can be detected within 10 s, and the detection limit is below 1 ppb. Also, this PbO nanosheet-based chip is reusable by heating after use. This study not only deepens the understanding of the NP-based formation mechanism of nanosheets but also provides the renewable SERS chips for the highly efficient detection of trace gaseous H2S.

CAS / MDL: 151-21-3
研究领域: 材料科学 · 化学 · 环境科学
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Analytical Methods · 2022 ·Vol. 14 ·期 12 ·1239-1245 · IF 3.532

A sensitive colorimetric hydrogen sulfide detection approach based on copper-metal–organic frameworks and a smartphone

Chengyi Hong,Dandan Li,Ziyue Wang,Boyuan Liu,Wenmin Zhang,Kailong Zhang,Zhiyong Huang

In this study, we demonstrate a colorimetric approach for the detection of hydrogen sulfide (H2S) in water samples with high sensitivity. Firstly, copper-metal–organic frameworks (Cu-MOFs) were synthesized by ultrasonic-assisted hydrothermal method, presenting a maximum absorption peak at 700 nm. It was found that Cu-MOFs could react with H2S to form a copper–sulfur complex along with a decrease of the absorption peak at 700 nm and a visible color change from blue to tan. Under the optimal reaction conditions, the absorption intensity at 700 nm was linear with H2S concentration in a range of 0.05–2 mM (R2 = 0.9928), providing a detection limit of 22 μM. Furthermore, the method was successfully applied to the detection of H2S in lake water samples with a recovery rate between 94.4% and 112.6%. In addition, a practical and portable device for on-site H2S detection was designed by using agarose hydrogels, and a simple colorimetric detection method based on a smartphone was developed. This analytical method showed good selectivity for H2S compared to other interfering substances, and the feasibility of the agarose hydrogel-based device was proved by the determination of H2S in real lake water samples.

CAS / MDL: 68-12-2
研究领域: 分析化学 · 环境科学
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ACS Sensors · 2024 · IF 8.2

Cu–Pt/CrN Fuel Cell Gas Sensor Achieves ppb-Level H2S Detection at Room Temperature

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.

研究领域: 材料科学 · 传感器技术 · 环境监测
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-8 · IF 14.7

Femtomolar hydrogen sulfide detection via hybrid small-molecule nano-arrays

Xing Xing,Wu Luyan,Zhang Yuchen,Pan Jiahao,Ishigaki Yusuke,Xie Huaqing,Suzuki Takanori,Ye Deju,Zhang Jianhua,Zhang Weihua,Lu Zhenda

Early disease diagnosis hinges on the sensitive detection of signaling molecules. Among these, hydrogen sulfide (H 2 S) has emerged as a critical player in cardiovascular and nervous system signaling. On-chip immunoassays, particularly nanoarray-based interfacial detection, offer promising avenues for ultra-sensitive analysis due to their confined reaction volumes and precise signal localization. Beyond the DNA or protein biomolecules array, this work presents a promising hybrid small molecule nano-array for H 2 S detection, using the power of dual molecules: a dye for fluorescence emission and a quencher with specific H 2 S reactivity. Upon H 2 S interaction, the quenched fluorescence reignites, creating an easily detectable array of bright spots. The molecule nano-array sensor shows exceptional responses to H 2 S over 8 magnitudes of dynamic range from 1 fM to 0.1 μM, with a remarkable detection limit of 1 fM, just using a 10 μL solution. This H 2 S detection method has the potential to significantly improve bioassay platforms, and the hybrid small-molecule nano-arrays we developed could be a valuable tool for advancing signaling molecule detection.

研究领域: 生物化学 · 医学检测 · 纳米技术
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RSC Advances · 2017 ·Vol. 7 ·期 45 ·28542-28547 · IF 3.108

Synthesis and gas sensing properties of molybdenum oxide modified tungsten oxide microstructures for ppb-level hydrogen sulphide detection

Jie Hu,Yongjiao Sun,Xiu Wang,Lin Chen,Wengdong Zhang,Yong Chen

Flower-like molybdenum oxide@tungsten oxide (MoO3@WO3) composite microstructures were successfully synthesized by hydrothermal and impregnation methods. The fabricated samples were characterized by XRD, EDS, SEM and TEM, and the results show that the MoO3@WO3 composite is composed of crystallized nanosheets with a thickness of about 40 nm. The gas sensing properties of the MoO3@WO3 composite microstructures towards hydrogen sulfide (H2S) were investigated as a function of operating temperature and gas concentration. The gas sensors based on MoO3@WO3 composites show better sensing performances than that of a pure one. Moreover, the Mo6W-based gas sensor exhibits the highest response (28.5 towards 10 ppm H2S), fast response/recovery time (2 s/5 s), low detection limit (20 ppb) and good selectivity at optimum operating temperature (250 °C). Such an excellent performance can be attributed to the heterojunction between MoO3 and WO3.

CAS / MDL: 12054-85-2 13283-01-7
研究领域: 材料科学 · 传感器技术
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MICROCHIMICA ACTA · 2023 ·Vol. 190 ·期 8 ·1-8 · IF 5.7

BSA-assisted ultrasound synthesis of water stable CsPbBr3 nanocrystals for sensitive fluorescent detection of hydrogen sulfide in human serum

Huang Feng,Deng Lei,Wang Tingting,Zhang Aomei,Yang Minghui,Hou Yi

A bovine serum albumin (BSA)-assisted ultrasonication strategy was developed for the synthesis of CsPbBr 3 nanocrystals (NCs) with stable fluorescence properties in aqueous solution. Such a preparation method is simple, fast and does not require complex equipment. The results show that the synthesized CsPbBr 3 NCs are homogeneous in particle size and have good solubility and stability in water. The CsPbBr 3 NCs have been utilized as fluorescence probe for rapid detection of hydrogen sulfide (H 2 S) in human serum. The reaction of H 2 S with the lead sites on the surface of CsPbBr 3 NCs produces lead sulfide (PbS), resulting in the decrease of fluorometric intensity of CsPbBr 3 NCs. Our designed fluorescent assay has a linear S 2− detecting range of 10 ~ 800 nM with a detection limit of 7.05 nM. The assay was used to determine H 2 S in human serum with spiked recoveries ranging from 94.98% to 102.69%. This work opens new avenues for the application of halide lead perovskite in different biosensing areas. Graphical abstract

研究领域: 纳米技术 · 分析化学 · 生物传感
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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
研究领域: 生物医学工程 · 分析化学
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NEW JOURNAL OF CHEMISTRY · 2019 ·Vol. 43 ·期 18 ·6848-6855 · IF 3.069

A novel near-infrared fluorescent hydrogen sulfide probe for live cell and tissue imaging

Xiaoting Huang,Haiyang Liu,Jiewen Zhang,Boren Xiao,Fengxu Wu,Yueying Zhang,Ying Tan,Yuyang Jiang

A dicyanoisophorone-based near-infrared fluorescent probe (NIR-NP) was successfully designed for hydrogen sulfide (H2S) detection. 7-Nitro-1,2,3-benzoxadiazole (NBD) amine, an electron-withdrawing group, was applied to quench the fluorescence of dicyanoisophorone-based fluorescent dyes and could be removed by H2S-specific thiolysis of an NBD amine bond, leading to a significant fluorescence turn-on response. The probe could quantitatively detect H2S with a lower detection limit (0.03 μM) in vitro and in living cells. The probe with a large Stokes shift (186 nm) showed a high selectivity to H2S in the presence of other biothiols, including glutathione, homocysteine, and cysteine. Moreover, the probe was successfully applied to image endogenous H2S in different tumor cells and in liver tissues. The excellent properties of the probe and its applications in cell and tissue imaging indicated its potential for further exploration and application of H2S in the pathophysiology of cancers and even in the diagnosis of H2S-related diseases.

研究领域: 分子影像学 · 肿瘤学 · 化学生物学 · 分子生物学 · 生物分析化学 · 转化医学
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