通过实验表征、计算机辅助结构解析和原子模拟对切尔西土壤腐植酸进行三维结构模拟  

3-D Structural Modeling of Humic Acids through Experimental Characterization,Computer Assisted Structure Elucidation and Atomistic Simulations.1.Chelsea Soil Humic Acid

作　　者：Mamadou S.Diallo Andre Simpson Paul Gassman Jean Loup Faulon James H.Johnson William A.Goddard Patrick G.Hatcher 袁飞 巩冠群(译)[7] Mamadou S.Diallo;Andre Simpson;Paul Gassman;Jean Loup Faulon;James H.Johnson;William A.Goddard;Patrick G.Hatcherwrite;Yuanfei;Gong Guanqun(translate)(Materials and Process Simulation Center,Beckman Institute 139-74,California Institute of Technology,Pasadena,California,91125;Department ol Civil Engineering,Howard University,Washington,D.C.,20059;Department of Physical Sciences,University of Toronto,Scarborough College,Toronto,MIC 1A4;4 Environmental Molecular Sciences Laboratory,Pacific Northwest National Laboratory,Richland,Washington,99352;Computational Biology&Evolutionary Computing Department,Sandia National Laboratories,Livermore,California,94551-0969;Department of Chemistry,The Ohio State University,Columbus,Ohio,43210;School of Chemical Engineering,China University of Mining and Technology,Xuzhou,221116)

机构地区：[1]加州理工学院贝克曼研究所139-74材料和工艺模拟中心,加利福尼亚州帕萨迪纳91125 [2]霍华德大学土木工程系,华盛顿特区20059 [3]多伦多大学斯卡伯勒学院物理科学系,加拿大多伦多MIC 1A4 [4]太平洋西北国家实验室环境分子科学实验室,华盛顿州里奇兰99352 [5]桑迪亚国家实验室计算生物学和进化计算部,加利福尼亚州利弗莫尔94551-0969 [6]俄亥俄州立大学化学系,俄亥俄州哥伦布43210 [7]中国矿业大学化工学院,徐州221116

出　　处：《腐植酸》2022年第5期60-75,共16页Humic Acid

摘　　要：本文描述了一个用于开发腐植酸(HAs)三维结构模型的完整的实验和计算框架。这种方法结合了实验表征、计算机辅助结构解析(CASE)和原子模拟,生成与HAs的分析数据和热力学/结构特性相一致的所有三维结构模型或这些模型的代表性样本。从元素分析、漫反射傅里叶变换红外光谱、一维/二维~1H和C溶液核磁共振光谱和电喷雾电离四极杆飞行时间质谱(ESI QqTOF MS)中获得的结构数据,结合CASE程序SIGNATURE,生成了切尔西土壤腐植酸(HA)所有的三维结构模型。这些模型随后被用作初始三维结构,进行恒温恒压分子动力学模拟,以估算其体密度和Hildebrand溶解度参数。只有少数模型异构体显示出的分子组成和体热力学性质与实验数据一致。这些模型异构体的等摩尔混合物的模拟C核磁共振光谱与切尔西土壤HA的实测光谱相比有较好的一致性。This paper describes an integrated experimental and computational framework for developing 3-D structural models for humic acids(HAs).This approach combines experimental characterization,computer assisted structure elucidation(CASE),and atomistic simulations to generate all 3-D structural models or a representative sample of these models consistent with the analytical data and bulk thermodynamic/structural properties of HAs.To illustrate this methodology,structural data derived from elemental analysis,diffuse reflectance FT-IR spectroscopy,1-D/2-D~1H andC solution NMR spectroscopy,and electrospray ionization quadrupole time-of-flight mass spectrometry(ESI QqTOF MS)are employed as input to the CASE program SIGNATURE to generate all 3-D structural models for Chelsea soil humic acid(HA).These models are subsequently used as starting 3-D structures to carry out constant temperature-constant pressure molecular dynamics simulations to estimate their bulk densities and Hildebrand solubility parameters.Surprisingly,only a few model isomers are found to exhibit molecular compositions and bulk thermodynamic properties consistent with the experimental data.The simulatedC NMR spectrum of an equimolar mixture of these model isomers compares favorably with the measured spectrum of Chelsea soil HA.

关 键 词：土壤 多肽和蛋白质 分子模拟 碳水化合物 核磁共振光谱 

分 类 号：TQ314.1[化学工程—高聚物工业]