Planar fluorescence sensors for two-dimensional measurements of H2S distributions and dynamics in sedimentary deposits

Planar fluorescence sensors for two-dimensional measurements of H2S distributions and dynamics in sedimentary deposits
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DOI:
10.1016/j.marchem.2013.08.001
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发表时间:
2013-12-20
期刊:
影响因子:
3
通讯作者:
Aller, Robert C.
Aller, Robert C.
中科院分区:
地球科学2区
文献类型:
--
作者:
Zhu, Qingzhi;Aller, Robert C.

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平面荧光传感器已被开发用于通过使用派洛宁 Y (PY) 作为新型 H2S 指示剂来测量海洋沉积物中的二维硫化氢 (H2S) 分布。传感箔是通过将 PY 非共价固定在透明聚酯片上的乙基纤维素聚合物膜中,并用透气有机硅涂覆它们来制备的。传感器发出的 567 nm 荧光(554 nm 激发)与溶液中的 H2S 浓度成反比。使用了两种主要传感器改进型:M1 和 M2。 M1 传感器在不可检测 (nd) 至 3150 μ mol/l 范围内对 H2S 显示出优异的线性响应,检测限为 40 μ mol/l H2S (3 sigma),可用于高浓度 H2S 测量。 M2传感器的动态工作动态范围为nd-125 μmol/l H2S,检测限为4 μmol/l(3 sigma),可用于检测样品中的低含量H2S。 M1 传感器的响应时间 (t(90)) 和恢复时间 (R-90) 分别类似于 60 秒和 30 秒,M2 传感器的响应时间 (t(90)) 和恢复时间 (R-90) 类似于 15 秒。这些荧光传感器仅对 H2S 敏感,对离子硫化物和二硫化物不敏感,并且其性能与温度和其他溶解气体(如氧气、CO2、NH3 和 N-2)无关。由于有机硅膜对荧光团的保护,没有观察到沉积物孔隙水中主要离子和微量元素的干扰。该传感器简单、稳定、可长时间半可逆(M2 可逆),已成功用于测量硫化盐沼沉积物中的二维 H2S 分布和动态,理论像素分辨率接近 50 x 50 μm。海洋沉积物中复杂的异质 H2S 分布以及先前未记录的与有人居住和废弃的生物结构相关的时间依赖性生物地球化学反应动力学很容易被揭示。 (C) 2013 Elsevier B.V. 保留所有权利。
Planar fluorescence sensors have been developed for measuring two-dimensional hydrogen sulfide (H2S) distributions in marine sediments by using pyronin Y (PY) as a novel H2S indicator. Sensing foils were prepared by non-covalently immobilizing PY in ethyl cellulose polymer membranes on transparent polyester sheets, and coating them with gas permeable silicone. Fluorescence from the sensors emitted at 567 nm (excitation at 554 nm) is inversely correlated to H2S concentration in solution. Two primary sensor modifications, M1 and M2, were used. The M1 sensor shows an excellent linear response versus H2S in the range of non-detectable (nd) to 3150 mu mol/l with a detection limit of 40 mu mol/l H2S (3 sigma), and it can be utilized for high concentration H2S measurement. The M2 sensor has a dynamic working dynamic range of nd-125 mu mol/l H2S with a detection limit of 4 mu mol/l (3 sigma) and can be used to detect low level H2S in samples. The response time (t(90)) and recovery time (R-90) of the M1 sensor are similar to 60 and 30 s, respectively, and for the M2, similar to 15 s. These fluorosensors are only sensitive to H2S rather than ionic sulfide and bisulfide species, and their performance is independent of temperature and other dissolved gases such as oxygen, CO2, NH3 and N-2. No interferences from major ions and trace elements in sediment porewater were observed due to the protection of the fluorophore by the silicone membrane. The sensors are simple, stable, and semi-reversible (reversible for M2) for extended periods, and have been successfully used to measure 2-dimensional H2S distributions and dynamics in sulfidic salt marsh sediments with a theoretical pixel resolution of similar to 50 x 50 mu m. Complex heterogeneous H2S distributions in marine sediments and previously undocumented time-dependent biogeochemical reaction dynamics associated with both inhabited and abandoned biogenic structures were readily revealed. (C) 2013 Elsevier B.V. All rights reserved.