新型外循环式高放废液蒸发浓缩脱硝釜

Novel External Circulation High-level Waste Liquid Evaporation and Concentration Denitration Kettle

  • 摘要: TRPO工艺是我国自主开发的高放废液处理流程,处理对象是Purex主工艺产生的高放废液。为满足TRPO工艺进料条件和降低流程负荷,高放废液需经蒸发浓缩脱硝操作进行体积、酸度、金属离子浓度等调整,但存在3个操作难点——爆沸、尾气净化、沉淀累积。为此,本文提出一种新型外循环式高放废液蒸发浓缩脱硝釜,通过加热区、蒸发区和脱硝反应区分离设计,辅以主动消除反应诱导期、内置旋风分离器、沉淀主动控制结构等改进措施,较好地解决了上述操作难点。台架试验表明:在反应釜内径为70 cm时,其处理通量可达56 L/h,酸度波动幅度小于0.1 mol/L,以Cs为示踪元素的二次蒸汽净化系数达8.6×106,浓缩液中锆离子以沉淀形式去除后,浓度可降低至11.8 ppm。验证试验表明,所提出的新型外循环式高放废液蒸发浓缩脱硝釜能够较好地满足TRPO工艺和主工艺的衔接需求,并可用于其他有类似需求的环节。

     

    Abstract: The TRPO process, an independently developed high-level liquid waste (HLLW) treatment process in China, is primarily designed to address the treatment of the HLLW generated from the Purex process. Solvent extraction is used in the TRPO process to remove long-lived alpha nuclides from HLLW, thereby significantly reducing the technical difficulty of long-term deep geological disposal of HLLW vitrified waste forms. To align with the feed conditions of the TRPO process and reduce the process load, the HLLW requires adjustment in terms of volume, acidity, and metal ion concentration through evaporation concentration and denitration operations. However, this process is accompanied by three significant operational challenges: boilover, droplet entrainment, and precipitate accumulation. Boilover can cause equipment vibration, and in severe cases, it may lead to equipment damage and the risk of radioactive leakage. Droplet entrainment can result in excessive radioactive emissions in the exhaust gas, endangering environmental safety. Excessive accumulation of precipitates can cause equipment clogging and scarring on the reactor wall. This paper proposes a novel external circulation kettle for the evaporation and denitration of HLLW. The design of the kettle strategically separates the heating zone, evaporation zone, and denitration reaction zone through lengthening the external circulation pipe and optimizing the feeding position of the denitration agent (formic acid). Here the heater is arranged at the lower part of the external circulation pipe, and heat is transferred into the reactor through convection. Additionally, improvements such as the elimination of the reaction induction period, the incorporation of a built-in cyclone separator, and the implementation of a precipitate control structure effectively address the aforementioned operational challenges. Demonstration tests indicate that the kettle, with an inner diameter of 70 cm, achieves a processing capacity of 56 L/h, maintains an acidity fluctuation range of less than 0.1 mol/L, and demonstrates a decontamination factor of 8.6×106 when cesium (Cs) is utilized as a tracer element. By promoting the precipitation of molybdenum ions with zirconium (Zr) ions, the Zr concentration can be reduced from 435.8 ppm in the feed solution to 85.5 ppm in the concentrated solution, with a Zr removal efficiency of 84.9%. Furthermore, when the concentrated solution is continuously subjected to heat preservation operation under total reflux mode (80-90 ℃ for 8 h; 96-98 ℃ for 7 h), the Zr concentration can ultimately be decreased to 11.8 ppm, achieving an overall Zr removal efficiency of 97.3%. These further confirm that the proposed novel external circulation kettle can satisfactorily meet the interfacing requirements with both the TRPO process and the Purex process, and it is also applicable to other similar operational units.

     

/

返回文章
返回