摘要
将稻壳与烷基化废硫酸经原位磺化可制得磺化炭材料,该材料可应用于环境修复领域。对磺化炭衍生溶解性有机质(SBC-DOM)组成的深入分析有助于评估其在环境中的作用与影响。为全面研究SBC-DOM的分子组成,利用4种不同极性溶剂(二氯甲烷、丙酮、甲醇和水)对SBC-DOM进行提取,采用傅里叶变换离子回旋共振质谱(FT-ICR MS)结合正/负离子模式电喷雾电离源(ESI±)对其分子组成进行表征。结果表明:ESI不同电离模式测得SBC-DOM的分子组成具有高度互补性,不同溶剂提取的SBC-DOM组成差异较大。含硫化合物(26.75%~71.05%)和不饱和脂肪族化合物(22.75%~45.00%)是SBC-DOM的主要组成部分。甲醇提取SBC-DOM中可检测分子式高达7765个,其化学多样性最高,且化合物分子量更大;水提取SBC-DOM中不饱和脂肪族化合物的相对含量(35.95%~45.00%)最高,具有更高的生物可利用性;而丙酮和二氯甲烷提取SBC-DOM的不饱和度(DBE_(wa))与芳香度(AI_(wa))更高,芳香类化合物的相对含量更高。研究显示,SBC-DOM中酸性化合物与强极性含硫化合物占绝对优势,应优先采用ESI(-)电离模式检测分析,在环境修复应用中选择水对SBC-DOM进行提取更为合适。SBC-DOM的详细分子组成可为评估烷基化废酸制得磺化炭在不同实际应用中的环境影响提供基础数据支撑。
Sulfonated biochar materials are synthesized through an in-situ sulfonation process utilizing rice husk and spent sulfuric acid from alkylation processes.These materials have promising applications in environmental remediation.A thorough examination of the molecular composition of dissolved organic matter derived from sulfonated biochar(SBC-DOM)is essential for understanding its environmental role and impacts.To delve into the molecular composition of SBC-DOM,a comprehensive study was conducted using four distinct polar solvents:dichloromethane(CH_(2)Cl2),acetone(CH3COCH3),methanol(CH3OH),and distilled water(H_(2)O).DOM was extracted from sulfonated biochar using these solvents and then analyzed by Fourier transform ion cyclotron resonance mass spectrometry(FT-ICR MS).The analysis was performed using both positive and negative ion electrospray ionization(ESI±).The results showed that the molecular composition of SBC-DOM determined by the different ESI ionization modes was highly complementary.Moreover,the solvents significantly influenced the composition of the extracted SBC-DOM.Sulfur-containing compounds and unsaturated aliphatic compounds were identified as the predominant components,accounting for 26.75%-71.05%and 22.75%-45.00%of the SBC-DOM,respectively.Notably,methanol-extracted SBC-DOM exhibited the greatest chemodiversity and molecular weight,with up to 7765 detectable molecular formulas.In contrast,water-extracted SBC-DOM had the highest relative content of unsaturated aliphatic compounds(from 35.95%to 45%),indicating higher bioavailability.Acetone and dichloromethane extractions produced SBC-DOM with higher degrees of unsaturation(DBE_(wa))and aromaticity(AI_(wa)),along with a greater relative content of highly aromatic compounds(10.78%and 12.15%).The study underscored that acidic and strongly polar sulfur-containing compounds are predominant in SBC-DOM,suggesting that ESI(-)ionization mode is suitable for their analysis.Furthermore,water is recommended as the solvent of choice for extracting SBCDOM in environmental remediation applications.The detailed molecular compositions of SBC-DOM can provide basic data to support the assessment of the environmental impacts of sulfonated biochar made from alkylated waste acids in different practical applications.
作者
蒋郑峰
何晨
史权
高飞
周志茂
于海濛
王若欣
JIANG Zhengfeng;HE Chen;SHI Quan;GAO Fei;ZHOU Zhimao;YU Haimeng;WANG Ruoxin(Petrochemical Research Institute,PetroChina Company Limited,Beijing 100195,China;State Key Laboratory of Heavy Oil Processing,China University of Petroleum,Beijing 102249,China;CAS Key Laboratory of Green Process and Engineering,Institute of Process Engineering,Chinese Academy of Sciences,Beijing 100190,China;National Elite Institute of Engineering,CNPC,Beijing 100096,China)
出处
《环境科学研究》
北大核心
2025年第2期376-385,共10页
Research of Environmental Sciences
基金
中国石油大学(北京)科研基金项目(No.2462023YJRC003)。
关键词
烷基化废硫酸
磺化炭
溶解性有机质
正/负离子模式电喷雾电离源
傅里叶变换离子回旋共振质谱
waste sulfuric acid of alkylated
sulfonated biochar
dissolved organic matters(DOM)
positive-/negative-ion electrospray ionization(ESI)
Fourier transform ion cyclotron resonance mass spectrometry(FT-ICR MS)
