Abstract Increased energy demand worldwide has caused faster depletion of sweet feedstock and increased exploitation of sourer hydrocarbon fuels. These fuels often contain acid gases (H 2 S and CO 2 ), mercaptans and trace amounts of benzene, toluene and xylene (BTX) that are harmful to human health, the environment and industrial equipment. The US EPA has proposed a reduction of sulfur in gasoline from 30 ppm to 10 ppm by 2017. To reach this goal, crude oil and gas must be subjected to more efficient desulfurization processes in which acid gases are major byproducts. The separated acid gases and associated impurities are further processed for material and energy recovery, as the fuels with high sulfur content are restricted due to their harmful effects. In this paper, a comprehensive review of the treatment of acid gases and associated impurities is given along with an advanced Claus process design that can capture much greater amounts of sulfur in the thermal stage to decrease the burden in catalytic stages and reduce operational costs. Claus process technology, although mature and commonly used for the recovery of sulfur and energy from acid gases, has low thermal stage efficiency that further deteriorates with change in acid gas composition. The non-uniformity of acid gas feed streams poses several technical and operational problems, resulting in higher operational costs and increased toxic gas emissions. Sulfur chemistry provides a path for improved understanding of the complex process in the thermal stage of the Claus reactor with a goal to recover both energy and improve the quality of sulfur produced, so that catalytic stages are minimal. The sulfur chemistry and kinetic models of H 2 S combustion are reviewed. Practical problems emanating from the presence of acid gas impurities (such as CO 2 , ammonia, light hydrocarbons, aromatics, COS and CS 2 ) during the acid gas conversion process are evaluated. Reactor conditions that mitigate the impact of impurities are also included. An urgent need exists for the development of comprehensive kinetic models that can capture the combustion chemistry of H 2 S along with the presence of trace quantities of aromatics, ammonia and other impurities during sulfur recovery in Claus reactors. Our current knowledge lacks a detailed chemistry, so that effective capture of acid gas conversion in the Claus thermal stage remains a challenge. Future studies must focus on a systematic coupling of the available kinetic models for neat H 2 S, hydrocarbon and ammonia fuels, and subsequent validation under partially oxidizing operating conditions in Claus reactors. Such a mechanism could help to improve the efficiency of sulfur recovery processes and sulfur quality for improved design of advanced Claus reactors with enhanced sulfur capture, energy recovery and mitigated environmental issues.

中文翻译：

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酸性气体处理硫化学研究进展

摘要 世界范围内能源需求的增加导致低硫原料的更快消耗和酸性碳氢燃料的开采增加。这些燃料通常含有对人体健康、环境和工业设备有害的酸性气体（H 2 S 和 CO 2 ）、硫醇和微量苯、甲苯和二甲苯 (BTX)。美国环保署已提议到 2017 年将汽油中的硫含量从 30 ppm 减少到 10 ppm。为实现这一目标，必须对原油和天然气进行更有效的脱硫工艺，其中酸性气体是主要副产品。分离出的酸性气体和相关杂质被进一步处理以进行材料和能量回收，因为硫含量高的燃料因其有害影响而受到限制。在本文中，对酸性气体和相关杂质的处理进行了全面审查，并提供了先进的克劳斯工艺设计，该设计可以在热阶段捕获更多的硫，以减少催化阶段的负担并降低运营成本。克劳斯工艺技术虽然成熟并普遍用于从酸性气体中回收硫和能量，但其热阶段效率低，随着酸性气体成分的变化而进一步恶化。酸性气体进料流的不均匀性带来了若干技术和操作问题，导致更高的操作成本和有毒气体排放量的增加。硫化学为更好地理解克劳斯反应器热阶段的复杂过程提供了一条途径，其目标是回收能量并提高所产生硫的质量，因此催化阶段最少。综述了 H 2 S 燃烧的硫化学和动力学模型。评估了酸性气体转化过程中酸性气体杂质（例如 CO 2 、氨、轻烃、芳烃、COS 和 CS 2 ）的存在所引起的实际问题。还包括减轻杂质影响的反应器条件。迫切需要开发综合动力学模型，该模型可以捕获 Claus 反应器中硫回收过程中 H 2 S 的燃烧化学以及痕量芳烃、氨和其他杂质的存在。我们目前的知识缺乏详细的化学反应，因此在克劳斯热阶段有效捕获酸性气体转化仍然是一个挑战。未来的研究必须集中在纯 H 2 S、碳氢化合物和氨燃料的可用动力学模型的系统耦合上，以及随后在克劳斯反应器中部分氧化操作条件下的验证。这种机制有助于提高硫回收过程的效率和硫质量，以改进具有增强硫捕获、能量回收和减轻环境问题的先进克劳斯反应器的设计。