Department of Geography and Berkeley Atmospheric Science Center, 540 McCone Hall #4740, University of California at Berkeley, Berkeley, CA 94720, United States.
Talanta. 2012 Jan 15;88:581-6. doi: 10.1016/j.talanta.2011.11.038. Epub 2011 Nov 19.
Reduced sulfur compounds (RSCs) were measured at low concentrations in small volume air samples using a cryo-trapping inlet system and gas chromatograph outfitted with a sulfur chemiluminescence detector (GC-SCD). The relative sensitivity of the system to the RSCs follows the sequence H(2)S<CH(3)SH<OCS∼DMS<CS(2). The analytical system achieves a detection limit of 120ppt in a 100mL air sample, which is suitable for measuring reactive RSCs (e.g., H(2)S and CH(3)SH) at ambient or near ambient atmospheric concentrations. The inlet system allows for replicate sampling from a stored air sample (sub-sampling), thereby improving estimates of instrumental precision and demonstrating the reproducibility of the analytical method. Although the SCD theoretically provides linear responses equivalent to the sulfur mass injected, we found that the response properties for each RSC differed. At concentrations below 2ppb, the compounds H(2)S and CH(3)SH have diminished responses, leading to larger measurement uncertainties. Two generations of commercially available SilcoCan canisters were tested to evaluate the relative RSC loss due to storage in the canister and loss of inertness because of coating age. The older generation canister (>6 years from initial coating) saw significant loss of H(2)S and CH(3)SH within 2 days, while the more recent generation canister (<1 year from initial coating) yielded percent recoveries of RSCs in the range of 85% (H(2)S and CH(3)SH) to 95% (OCS, DMS and CS(2)) after 7 days of storage, suggesting that these canisters may be suitable for the short-term storage of low level RSCs. The development of this low concentration, low sample volume method is well suited for measuring RSC gas fluxes from natural soils in laboratory incubations and in field flux chamber studies.
采用低温捕集进样系统和配备硫化学发光检测器的气相色谱仪(GC-SCD),可在小体积空气样本中检测到低浓度的还原态硫化合物(RSCs)。该系统对 RSCs 的相对灵敏度依次为 H(2)S<CH(3)SH<OCS∼DMS<CS(2)。该分析系统在 100mL 空气样本中达到 120ppt 的检测限,适用于测量环境或近环境大气浓度下的反应性 RSCs(例如 H(2)S 和 CH(3)SH)。该进样系统允许从存储的空气样本中进行重复采样(亚采样),从而提高仪器精密度的估计值,并证明分析方法的重现性。尽管 SCD 从理论上提供与注入硫质量相当的线性响应,但我们发现每种 RSC 的响应特性都有所不同。在浓度低于 2ppb 时,H(2)S 和 CH(3)SH 等化合物的响应减弱,导致测量不确定度增大。我们测试了两代市售的 SilcoCan 罐,以评估由于储存在罐中以及由于涂层老化而导致的惰性丧失,RSC 的相对损失。较旧一代的罐(从初始涂层开始超过 6 年)在 2 天内会显著损失 H(2)S 和 CH(3)SH,而较新一代的罐(从初始涂层开始不到 1 年)在储存 7 天后,RSCs 的回收率在 85%(H(2)S 和 CH(3)SH)到 95%(OCS、DMS 和 CS(2))之间,表明这些罐可能适用于短期储存低浓度 RSCs。这种低浓度、小体积方法的开发非常适合测量实验室培养和野外通量箱研究中天然土壤的 RSC 气体通量。