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在加压富氧燃烧条件下再燃还原 NO 的动力学评价与优化研究。

A kinetic evaluation and optimization study on NO reduction by reburning under pressurized oxy-combustion.

机构信息

MOE Key Laboratory of Thermo-Fluid Science and Engineering, Xi'an Jiaotong University, Xi'an, China.

Henan Province Boiler Pressure Vessel Safety Inspection Institute, Zhengzhou, 450016, China.

出版信息

J Environ Manage. 2021 Jul 15;290:112690. doi: 10.1016/j.jenvman.2021.112690. Epub 2021 Apr 23.

Abstract

Pressurized oxy-combustion is an emerging and more efficient technology for carbon capture, utilization, and storage than the first generation (atmospheric) oxy-combustion. NO is a major conventional pollutant produced in pressurized oxy-combustion. In pressurized oxy-combustion, the utilization of latent heat from moisture and removal of acid gases (NOx and SOx) are mainly conducted in an integrated direct-contact wash column. Recent studies have shown that NOx particular inlet concentration should be maintained before direct contact wash column to remove NOx and SOx efficiently. As a result, minimizing NOx for environmental reasons, avoiding corrosion in carbon capture, utilization, and storage, and achieving effective NOx and SOx removal in direct contact wash columns are crucial. Reburning is a capable and affordable technology for NO reduction; however, this process is still less studied at elevated pressure, particularly in pressurized oxy-combustion. In this paper, the kinetic evaluation and optimization study on NO reduction by reburning under pressurized oxy-combustion was conducted. First, the most suitable mechanism was selected by comparing the results of different kinetic models with the experimental data in literature at atmospheric and elevated pressures. Based on the validated mechanism, a variety of parameters were studied at high pressure, i.e., comparing the effects of oxy and the air environment, different reburning fuels, residence time, HO concentration, CH/NO ratio, and equivalence ratio on the NO reduction. The results show that de-NOx efficiency in an oxy environment is significantly enhanced compared to the air environment. Improvement in the de-NOx efficiency is considerably higher with a pressure increase of up to 10 atm, but the effect is less prominent above 10 atm. The formation of HCN is significantly reduced while the N formation is enhanced as the pressure increases from 1 to 10 atm. The residence time required for the maximum NO reduction decreases as the pressure increases from 1 atm to 15 atm. At the higher pressure, the NO reduction rises prominently when the ratio of CH/NO increases from 1 to 2; however, the effect fades after that. At higher pressure, the NO reduction by CH reburning decreases as the HO concentration increases from 0 to 35%. The optimum equivalence ratio and high pressure for maximum NO reduction are 1.5 and 10 atm, respectively. This study could provide guidance for designing and optimizing a pressurized reburning process for NOx reduction in POC systems.

摘要

加压富氧燃烧是一种比第一代(大气)富氧燃烧更高效的碳捕集、利用和封存技术。NO 是加压富氧燃烧过程中产生的主要常规污染物。在加压富氧燃烧中,水分潜热的利用和酸气(NOx 和 SOx)的去除主要在集成的直接接触洗涤塔中进行。最近的研究表明,为了有效地去除 NOx 和 SOx,直接接触洗涤塔的入口处应保持特定的 NOx 浓度。因此,出于环境原因尽量减少 NOx、避免碳捕集、利用和封存中的腐蚀以及在直接接触洗涤塔中实现有效的 NOx 和 SOx 去除至关重要。再燃是一种可行且经济实惠的 NO 减排技术;然而,在高压下,特别是在加压富氧燃烧中,对该过程的研究仍然较少。本文对加压富氧燃烧条件下再燃还原 NO 的动力学评估和优化进行了研究。首先,通过将不同动力学模型的结果与文献中大气和高压下的实验数据进行比较,选择了最合适的机制。基于验证后的机制,在高压下研究了多种参数,即比较富氧和空气环境、不同再燃燃料、停留时间、HO 浓度、CH/NO 比和当量比对 NO 还原的影响。结果表明,与空气环境相比,在富氧环境中脱氮效率显著提高。随着压力从 1 增加到 10 大气压,脱氮效率的提高相当显著,但在 10 大气压以上,效果不明显。随着压力从 1 增加到 10 大气压,HCN 的形成显著减少,而 N 的形成增加。随着压力从 1 大气压增加到 15 大气压,最大 NO 还原所需的停留时间减少。在较高压力下,当 CH/NO 比从 1 增加到 2 时,NO 还原明显增加;然而,之后效果会减弱。在较高压力下,随着 HO 浓度从 0 增加到 35%,CH 再燃还原的 NO 减少。最大 NO 还原的最佳当量比和高压分别为 1.5 和 10 大气压。本研究可为设计和优化 POC 系统中 NOx 减排的加压再燃工艺提供指导。

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