Experimental Studies and Computational Calculations to Advance our Understanding of Biochar Surface Chemical Functionalities Responsible for Pollutants Removal

提案：1703052PI: Manuel garcia - perez植物基（木质纤维素）原料的高温加工用于生产碳基材料（生物炭），用于去除农药和除草剂等环境污染物。已经发现影响生物炭质量的各种参数，包括原料组成、生产条件（例如温度和反应环境）和污染物。该项目的重点是增加我们对生物炭的基本认识，特别是与不同去除机制相关的活性位点的性质以及这些活性位点是如何形成的。在这个项目中，pi将整合实验和建模，以深入了解与几种污染物去除机制相关的生物炭化学结构（活性位点）。该项目的研究结果可用于指导生物炭去除环境污染物的优化生产。去除有机（农药和除草剂、医药和个人护理产品、增塑剂、染料和多芳香族化合物）、无机（磷酸盐、硝酸盐、铵和重金属）和气态（H2S、CH4和N2O）污染物的能力是生物炭的一个重要特性。PIs计划进行基础研究，以更好地了解生物炭的吸附速率和机理，以及这些因素与原料组成、碳化和后碳化条件的关系。他们将研究纤维素、半纤维素和木质素形成碳质固体的机理，以及不同表面功能作为吸附污染物的活性位点的作用。密度泛函理论（DFT）计算将用于为生物炭的拉曼、XPS和13C-NMR光谱分析提供新的反褶积策略。这些材料去除气态、有机、无机和重金属污染物的能力将被评估，结果将与生物炭的化学成分结果相关联。由此产生的相关性将允许识别生物炭中的相关活性位点。DFT计算将用于进一步探索与这些活性位点相关的吸附机制。这项研究将通过提供与污染物去除相关的碳质结构（多芳族缺陷，含氧和含氮官能团）形成机制的细节来影响该领域。本研究结果可作为一种强有力的环保工具，指导廉价碳质吸附剂的高效生产。

Proposal: 1703052PI: Manuel Garcia-PerezThe high-temperature processing of plant-based (lignocellulosic) feedstocks is used to produce carbon-based materials (biochars) that are used to remove environmental pollutants such as pesticides and herbicides. Various parameters have been found to affect biochar quality, including feedstock composition, production conditions (e. g., temperature and reaction environment), and contaminants. The focus of this project is to increase our fundamental understanding of biochars, especially the nature of the active sites associated with different removal mechanisms and how these active sites are formed. In this project the PIs will integrate experimentation and modeling to gain an insight into biochar chemical structures (active sites) associated with several pollutant removal mechanisms. Results of this project may be used to guide optimization of the production of biochars for removing environmental contaminants. The capacity to remove organic (pesticides and herbicides, pharmaceutical and personal care products, plasticizers, dyes and polyaromatic compounds) inorganic (phosphates, nitrates, ammonium and heavy metals) and gaseous (H2S, CH4, and N2O) pollutants is an important attribute of biochars. The PIs plan to perform fundamental research to better understand biochar adsorption rates and mechanisms and the relationships of these factors to feedstock composition, carbonization, and post-carbonization conditions. They will study the mechanism of carbonaceous solids formation from cellulose, hemicellulose, and lignin and the role of different surface functionalities as active sites for the adsorption of pollutants. Density Functional Theory (DFT) calculations will be used to inform new deconvolution strategies for the analysis of Raman, XPS, and 13C-NMR spectra of biochars. The capacity of these materials to remove gaseous, organic, inorganic, and heavy metal pollutants will be evaluated, and the results will be correlated with biochar chemical composition results. The resulting correlations will permit the identification of relevant active sites in biochars. DFT calculations will be used to further explore the adsorption mechanisms associated with these active sites. This research will impact the field by providing details of mechanisms responsible for the formation of carbonaceous structures (polyaromatic deficiencies, oxygen and nitrogen containing functional groups) that are relevant for pollutant removal. Results of this study may guide the efficient production of inexpensive carbonaceous adsorbents as a powerful environmental tool.