【摘要】 目的 基于直接进样-高分辨质谱法，高通量筛查污水样品中新污染物并优选关键新污染物。方法 污水样品经滤膜过滤后，直接采用本课题组先前建立的液相色谱-飞行时间质谱仪（LC-TOF-MS）方法进行分析，采用C18色谱柱梯度洗脱分离，经一级质谱全扫描模式和二级非信息依赖数据采集模式获取精确分子质量数及特征离子碎片信息。对获得的原始数据经开源质谱数据分析平台MZmine 3进行特征峰识别、峰对齐后，随后通过MassBank、PubChem等数据库进行高通量筛查策略检索，最终与标准品色谱峰保留时间和质谱特征碎片离子比对并确认。结果 本研究共检出13种新污染物，其中包括7种工业化学品、4种药物、1种农药和1种代谢产物。检出率较高的污染物为二甲双胍（86.2%）、2-羟基苯并噻唑（79.3%）、1,2-苯并异噻唑-3-酮（72.4%）和1,2-苯并异噻唑-3-酮（72.4%）。污染物定量浓度范围为1.37～19.05 ng/mL,其中三聚氰胺（19.05 ng/mL）和呋塞米（18.49ng/mL）浓度最高。生态风险评估表明，1,2-苯并异噻唑-3-酮、4-氨基乙酰苯胺、肌酸酐、2-羟基苯并噻唑和呋塞米的风险熵较高，需被列为优先关注的污染物。结论 本研究利用直接进样结合高分辨质谱的非靶向筛查技术，高效识别污水样品中新污染物，优选出5种生态风险较高的关键污染物。研究成果不仅提升了新污染物环境监测的广度和深度，还为环境法医学及健康风险评估等跨学科研究提供了重要技术支持。更多还原

【Abstract】 Objective To establish a high-throughput non-targeted screening and prioritization method for emerging pollutants(EPs) in sewage using direct injection high-resolution mass spectrometry(HRMS). Methods The sewage samples were filtered by membrane filter and directly subjected to the liquid chromatography-time-of-flight mass spectrometer based on a method modified from our previous study. A C18 chromatographic column was applied for a gradient elution separation, and accurate mass and mass spectral fragment information were obtained through the MS full scan mode and MS/MS DIA data collection mode. After peak detection and alignment, the features from the raw data through open source software MZmine 3, and then high-throughput screening strategies such as MassBank and PubChem databases were used for compound annotation. Finally, the candidate features were confirmed with chemical standards by compared their retention time and mass spectrum fragmentation ion peaks. Results 13 EPs were identified, including 7 industrial chemicals, 4 pharmaceuticals, 1 pesticide and 1 metabolite. High detection rates were observed for metformin(86.2 %), 2-hydroxybenzothiazole(79.3 %), 1,2-benzisothiazole-3-one(72.4 %), and 1,2-benzisothiazole-3-one(72.4 %). The quantitative concentration range of EPs was 1.37 ～ 19.05 ng/mL, with the high concentrations observed for melamine(19.05 ng/mL) and furosemide(18.49 ng/mL). Ecological risk assessment identified 1,2-benzisothiazol-3-one, 4-aminoacetophenone, creatinine, 2-hydroxybenzothiazole, and furosemide as key pollutants. Conclusion This direct injection coupled with HRMS workflow enables efficient non-targeted screening and prioritization of emerging EPs in sewage samples, highlighting five ecotoxicologically critical EPs. The methodology enhances environmental monitoring capabilities and provide critical technical support for interdisciplinary research such as environmental forensics and health risk assessment.更多还原