期刊论文

Study on Mechanism for pH Affecting Hydrazine Bond Breaking with Platinum as Catalyst by ESR Method

Xia, L.

中文

原子能科学技术

1000-6931

2019

53

7

1238-1244

10.7538/yzk.2018.youxian.0637

国家自然科学基金资助项目（11575078）； 南华大学研究生科学基金资助项目（2018KYY025）；

本校为第一且通讯机构

为明确酸性条件下Pt催化N_2H_4还原U(Ⅵ)制备U(Ⅳ)的反应历程和反应机理,有针对性地提高其反应速率、优化工艺流程,本文采用电子自旋共振(ESR)法实验研究[DK]·NH_2转化为[DK]·OH的机理及0.25 mol/L和0.5 mol/L N_2H_4浓度条件下不同酸度的高氯酸体系中Pt催化N_2H_4分解过程中产生的自由基,确定反应过程中pH值对N_2H_4断键的影响机制。结果表明,在高氯酸介质中,Pt催化N_2H_4分解反应体系中检测到的[DK]·OH是由N_2H_4分解产生的[DK]·NH_2转化而来;该反应体系中酸度会对N_2H_4分解产生影响,在酸度逐渐降低的过程中Pt催化N_2H_4分解的反应速率表现为先增大后减小的趋势,其中在pH=1~2之间时Pt催化...

In order to determine the reaction process and reaction mechanism of U(Ⅳ) produced by hydrazine reducting U(Ⅵ) with platinum as catalyst in the nitric acid environment, improve the reaction rate, and optimize the process flow, the effect of pH value on hydrazine bond breaking with Pt as catalyst was studied. The electron-spin resonance (ESR) method was used to study the mechanism of conversion of •NH2 to •OH, and analyze the free radicals generated during the decomposition of hydrazine catalyzed by Pt in perchloric acid systems with differe...