N2气氛下氨水溶液γ辐射分解行为

TL13; 某些压水堆中使用氨及其分解产生的H2抑制H2O2、O2和·OH等氧化性物种的浓度,在保持一回路的还原性化学环境的同时调节冷却剂pH,以减轻结构材料的腐蚀.本工作为了研究脱氧氨水溶液在辐射场中的分解行为,针对其在γ场中的辐解过程进行了实验研究,重点考察了N2压强、气相与液相体积之比和温度对氨水溶液辐解的影响,测定了剩余氨、H2和氮氧化物(NO2-和NO3-)的浓度及溶液的pH.结果表明:N2压强(0.5~5.0 MPa)及气液体积比的变化未对氨的分解和氮氧化物的生成造成影响,吸收剂量为28.8 kGy时,辐解产生的氮氧化物浓度约为1 mg/L,但N2压强和气液体积比的增加会显著降低H...

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Published in辐射研究与辐射工艺学报 Vol. 42; no. 1; pp. 28 - 37
Main Authors 郭子方, 张扬, 李一帆, 林子健, 刘春雨, 林鹏, 林铭章
Format Journal Article
LanguageChinese
Published 中国科学技术大学核科学技术学院 合肥 230026%中广核研究院有限公司 深圳 518028 01.02.2024
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ISSN1000-3436
DOI10.11889/j.1000-3436.2023-0088

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Abstract TL13; 某些压水堆中使用氨及其分解产生的H2抑制H2O2、O2和·OH等氧化性物种的浓度,在保持一回路的还原性化学环境的同时调节冷却剂pH,以减轻结构材料的腐蚀.本工作为了研究脱氧氨水溶液在辐射场中的分解行为,针对其在γ场中的辐解过程进行了实验研究,重点考察了N2压强、气相与液相体积之比和温度对氨水溶液辐解的影响,测定了剩余氨、H2和氮氧化物(NO2-和NO3-)的浓度及溶液的pH.结果表明:N2压强(0.5~5.0 MPa)及气液体积比的变化未对氨的分解和氮氧化物的生成造成影响,吸收剂量为28.8 kGy时,辐解产生的氮氧化物浓度约为1 mg/L,但N2压强和气液体积比的增加会显著降低H2的浓度.温度由25℃升至200℃时,氨的分解过程将大幅放缓,吸收剂量为14.4 kGy时,30 mg/L氨水中氨的分解比例由26.5%降至8.4%,高温有利于抑制氨的分解速率,但同时导致NO2-和NO3-的浓度分别升高34和3倍左右.此外,本工作中还建立了含氨冷却剂的辐解模型并对其可靠性进行了验证,不同温度下实验数据与模型预测结果的最大相对误差仅为4.1%.随后利用该模型计算了不同初始浓度的含氨冷却剂辐解过程中剩余氨的浓度变化,结果表明较高的初始浓度有利于体系中氨的保持,连续辐照的情况下单独使用氨抑制氧化性物种时需要及时对其进行补充.
AbstractList TL13; 某些压水堆中使用氨及其分解产生的H2抑制H2O2、O2和·OH等氧化性物种的浓度,在保持一回路的还原性化学环境的同时调节冷却剂pH,以减轻结构材料的腐蚀.本工作为了研究脱氧氨水溶液在辐射场中的分解行为,针对其在γ场中的辐解过程进行了实验研究,重点考察了N2压强、气相与液相体积之比和温度对氨水溶液辐解的影响,测定了剩余氨、H2和氮氧化物(NO2-和NO3-)的浓度及溶液的pH.结果表明:N2压强(0.5~5.0 MPa)及气液体积比的变化未对氨的分解和氮氧化物的生成造成影响,吸收剂量为28.8 kGy时,辐解产生的氮氧化物浓度约为1 mg/L,但N2压强和气液体积比的增加会显著降低H2的浓度.温度由25℃升至200℃时,氨的分解过程将大幅放缓,吸收剂量为14.4 kGy时,30 mg/L氨水中氨的分解比例由26.5%降至8.4%,高温有利于抑制氨的分解速率,但同时导致NO2-和NO3-的浓度分别升高34和3倍左右.此外,本工作中还建立了含氨冷却剂的辐解模型并对其可靠性进行了验证,不同温度下实验数据与模型预测结果的最大相对误差仅为4.1%.随后利用该模型计算了不同初始浓度的含氨冷却剂辐解过程中剩余氨的浓度变化,结果表明较高的初始浓度有利于体系中氨的保持,连续辐照的情况下单独使用氨抑制氧化性物种时需要及时对其进行补充.
Abstract_FL In some reactors,ammonia and its radiolytic product(H2)are used to scavenge the oxidizing species(H2O2,O2,and·OH).A reducing chemical environment is thus created and the pH of the coolant is regulated simultaneously.In the present study,the radiolytic behaviors of deoxygenated ammonia solution were studied in the γ-ray field.The impacts of N2 pressure,gas-liquid volume ratio,and temperature on deoxygenated ammonia solution radiolysis were investigated.The pH and the concentrations of residual ammonia,H2,and nitrogen oxides(NO2-and NO3-)were analyzed.The results revealed that the variation of N2 pressure(0.5~5.0 MPa)and gas-liquid volume ratio had no influence on the concentrations of residual ammonia and nitrogen oxides.NO2-and NO3-concentrations were approximately 1 mg/L at room temperature when the absorbed dose was 28.8 kGy.However,the apparent concentration of H2 significantly decreased with the N2 pressure and gas-liquid volume ratio.The loss fraction of ammonia considerably declined from 26.5%to 8.4%when the temperature increased from 25 to 200℃,demonstrating that the radiolysis of ammonia was suppressed at the elevated temperature.However,the concentrations of NO2-and NO3-increased to 34 and 3 times,respectively,at 200℃compared to those at 25℃.In addition,a radiolysis model of ammonia-containing coolant was established in the present study.The maximum relative error between experimental data and calculation results at any temperature was 4.1%.The model was thereafter used to calculate residual ammonia concentration with the absorbed dose under different initial ammonia concentrations.The results revealed that it was necessary to replenish ammonia regularly when using it alone to inhibit oxidizing species.
Author 林鹏
张扬
李一帆
刘春雨
林子健
郭子方
林铭章
AuthorAffiliation 中国科学技术大学核科学技术学院 合肥 230026%中广核研究院有限公司 深圳 518028
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Author_FL LI Yifan
LIU Chunyu
GUO Zifang
LIN Zijian
LIN Mingzhang
ZHANG Yang
LIN Peng
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DocumentTitle_FL γ-Radiolysis of the aqueous ammonia solution saturated by N2
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Keywords 氨水
Water chemistry
水化学
Coolant
Ammonia solution
辐射分解
冷却剂
反应堆
Radiolysis
Reactor
Language Chinese
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PublicationTitle 辐射研究与辐射工艺学报
PublicationTitle_FL Journal of Radiation Research and Radiation Processing
PublicationYear 2024
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Snippet TL13; 某些压水堆中使用氨及其分解产生的H2抑制H2O2、O2和·OH等氧化性物种的浓度,在保持一回路的还原性化学环境的同时调节冷却剂pH,以减轻结构材料的腐蚀.本工作为了研究脱...
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