生物质热解烟雾衍生DOM在水铁矿表面的分子分馏特性

姚舒馨; 钟寅华; 徐忆欣; 张慧颖; 陈卫锋; 倪进治; 魏然

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中国环境科学 ›› 2025, Vol. 45 ›› Issue (10) : 5422-5434.

大气污染与控制

生物质热解烟雾衍生DOM在水铁矿表面的分子分馏特性

姚舒馨¹, 钟寅华¹, 徐忆欣¹, 张慧颖¹, 陈卫锋², 倪进治^1,2, 魏然^1,3

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Molecular fractionation characteristics of biomass-pyrogenic smoke-derived dissolved organic matter on the surface of ferrihydrite

YAO Shu-xin¹, ZHONG Yin-hua¹, XU Yi-xin¹, ZHANG Hui-ying¹, CHEN Wei-feng², NI Jin-zhi^1,2, WEI Ran^1,3

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摘要

为探明生物质热解烟雾衍生的溶解性有机质(BSDOM)在水铁矿上的分馏特征及机制,本研究选取3种生物质来源(杉木、水稻秸秆和苜蓿)的BSDOM开展水铁矿吸附实验,通过紫外、红外和三维荧光光谱等技术分析了分馏前后溶液中BSDOM的有机组成和分子变化特征.研究发现BSDOM主要由类蛋白物质(57%~75%)构成,吸附机制以阳离子-π相互作用为主.分子量大、高芳香性物质更易吸附在水铁矿上,且多酚类物质优先被吸附.酸性条件可增强水铁矿与BSDOM之间的阳离子-π相互作用和配体交换,有利于吸附.而在高pH值(10.0~12.0)下,多酚类和短波类蛋白物质的吸附比增加,归因于氢键作用,长波类蛋白物质和类腐殖酸的吸附比降低是由于静电斥力的增强.本研究从分子角度揭示了BSDOM在水铁矿表面的分馏特征,有助于深入了解BSDOM在地表环境中的跨介质环境行为.

Abstract

In order to explore the fractionation characteristics and mechanisms of biomass-pyrogenic smoke-derived dissolved organic matter (BSDOM) on ferrihydrite, this study selected BSDOM derived from three biomass sources (fir-wood chips, rice straw, and alfalfa) to investigate its adsorption on ferrihydrite. The organic compositions and molecular variations of BSDOM in the solution before and after fractionation were characterized using ultraviolet-visible (UV-Vis) spectroscopy, Fourier transform infrared (FTIR) spectroscopy and three-dimensional excitation-emission matrix (3D-EEM) fluorescence spectroscopy. The results indicated that BSDOM primarily consisted of protein-like substances(57%~75%), with cation-π interactions identified as the dominant adsorption mechanism. High molecular weight and highly aromatic compounds exhibited stronger adsorption affinity to ferrihydrite, with polyphenols being preferentially adsorbed. The results demonstrated that acidic conditions enhanced cation-π interactions and ligand exchange between ferrihydrite and BSDOM, thereby promoting adsorption. At high pH(10.0~12.0), the adsorption of polyphenols and short-wave protein-like substances increased, likely due to hydrogen bonding. In contrast, the adsorption of long-wave protein-like substances and humic-like substances decreased, primarily because of increased electrostatic repulsion. This study elucidates the fractionation characteristics of BSDOM on ferrihydrite surfaces at a molecular level, providing insights into the cross-media environmental behavior of BSDOM in surface environments.

导出引用

姚舒馨, 钟寅华, 徐忆欣, 张慧颖, 陈卫锋, 倪进治, 魏然. 生物质热解烟雾衍生DOM在水铁矿表面的分子分馏特性[J]. 中国环境科学. 2025, 45(10): 5422-5434

YAO Shu-xin, ZHONG Yin-hua, XU Yi-xin, ZHANG Hui-ying, CHEN Wei-feng, NI Jin-zhi, WEI Ran. Molecular fractionation characteristics of biomass-pyrogenic smoke-derived dissolved organic matter on the surface of ferrihydrite[J]. China Environmental Science. 2025, 45(10): 5422-5434

中图分类号： X51

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