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Physical and electrochemical study of halide-modified activated carbons.

机译：卤化物改性活性炭的物理和电化学研究。

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摘要

The current thesis aims to improve the electrochemical capacity of activated carbon electrodes, which enjoy prominent position in commercial electrochemical capacitors. Our approach was to develop electrochemical capacity by developing faradaic pseudocapacitance in carbon through a novel mechanochemical modification using iodine and bromine.;Various commercial carbons were mechanochemically modified via solid-state iodation and vapour phase iodine-incorporation. The halidation-induced changes in the structure, composition, morphology, electrical and electrochemical properties of carbon materials were studied using different characterization techniques encompassing XRD, XRF, XPS, Raman spectroscopy, BET study, TEM, SAXS and electrochemical testing followed by an intensive battery of physical and electrochemical characterization. The introduction of iodine into carbon system led to the formation of polyiodide species that were preferentially reacted within the micropore voids within the carbon leading to the development of a faradaic reaction at 3.1V. In spite of the lower surface area of modified carbon, we observed manyfold increase in its electrochemical capacity. Parallel inception of non-faradaic development and faradaic pseudocapacitive reaction led to promising gravimetric, surface area normalized and volumetric capacity in iodated carbons. With promising electrochemical improvement post halidation process, the chemical halidation method was extended to different class of carbons and halides. Carbons ranging from amorphous (activated) carbons to crystalline carbons (graphites, fluorographites) were iodine-modified to gain further insight on the local graphite-iodine chemical interaction. In addition, the effect of pore size distribution on chemical iodation process was studied by using in-house fabricated microporous carbon. A comparative study of commercial mesoporous carbons and in-house fabricated microporous carbons showed higher iodine-uptake ability and larger volumetric capacity development in case of microporous carbons. For halides, bromine was also tested in activated carbons, which showed similar set of physical and electrochemical modification, but to a smaller degree.;Carbon-polyhalide nanocomposites form a very interesting system both for fundamental research and as new electrode systems for asymmetric hybrid capacitor and low-voltage high power battery type applications.
机译：本论文旨在提高活性炭电极的电化学容量，活性炭电极在商用电化学电容器中占有重要地位。我们的方法是通过使用碘和溴进行新颖的机械化学修饰来开发碳中的法拉第伪电容，从而提高电化学容量。各种商品碳通过固态碘化和气相碘掺入进行机械化学修饰。使用XRD，XRF，XPS，拉曼光谱，BET研究，TEM，SAXS和电化学测试等不同的表征技术，研究了卤化物诱导的碳材料的结构，组成，形态，电学和电化学特性的变化，随后使用了密集电池物理和电化学表征。将碘引入碳系统导致形成多碘物质，这些物质优先在碳中的微孔空隙内反应，从而导致在3.1V时发生法拉第反应。尽管改性碳的表面积较低，但我们观察到其电化学容量却增加了许多倍。非法拉第发展和法拉第拟电容反应的平行开始导致了碘碳中有希望的重量，表面积归一化和体积容量。随着卤化后电化学性能的改善，化学卤化方法扩展到了不同种类的碳和卤化物。对碳进行了改性，从非晶态（活性碳）到结晶碳（石墨，氟石墨），以进一步了解局部石墨-碘的化学相互作用。此外，通过使用内部制造的微孔碳研究了孔径分布对化学碘化过程的影响。商业中孔碳和内部制造的微孔碳的比较研究显示，在微孔碳的情况下，碘的吸收能力更高，容量发展更大。对于卤化物，还对活性炭中的溴进行了测试，其表现出相似的一组物理和电化学改性，但程度较小；碳-多卤化物纳米复合材料形成了非常有趣的系统，无论是用于基础研究还是作为用于非对称混合电容器的新电极系统和低压大功率电池类型的应用。

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  • 作者

    Barpanda, Prabeer.;

  • 作者单位

    Rutgers The State University of New Jersey - New Brunswick.;

  • 授予单位 Rutgers The State University of New Jersey - New Brunswick.;
  • 学科 Chemistry Inorganic.;Engineering Materials Science.
  • 学位 Ph.D.
  • 年度 2009
  • 页码 246 p.
  • 总页数 246
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 无机化学;工程材料学;
  • 关键词

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