Effect of ZnO in borosilicate solidification glass on Mo leaching rate in simulated high-level radioactive waste and its model prediction

Hailong DONG; Chen DAI; Zhongdi LI; Shubin CHEN; Sijun FAN; Liyan ZHANG

doi:10.11889/j.0253-3219.2024.hjs.47.060502

NUCLEAR TECHNIQUES, Volume. 47, Issue 6, 060502(2024)

Effect of ZnO in borosilicate solidification glass on Mo leaching rate in simulated high-level radioactive waste and its model prediction

Hailong DONG¹, Chen DAI^2,3, Zhongdi LI¹, Shubin CHEN², Sijun FAN², and Liyan ZHANG^2、*

Author Affiliations

¹China Nuclear Power Engineering Co., Ltd., Beijing 100840, China

²Special Glass and Optical Fiber Research Center, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Shanghai 201800, China

³College of Materials Science and Engineering, Hunan University, Changsha 410082, China

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Figures & Tables(14)

Fig. 1. Photograph of glass samples

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Fig. 2. IR absorption spectra of glasses

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Fig. 3. Measured (black) and curve- fitting (red) derived IR spectra of Zn-1 and Zn-5 glass with peaks (P1~P10) (color online)

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Fig. 4. Diagram of initial structure-r_Mo model

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Fig. 5. Test results of XRD and DSC of sample Zn-1.5

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Fig. 6. Results diagram of step-by-step model iteration by validation glasses V₁ (a), V₂ (b), V₃ (c)

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Table 1. Compositions of glass (mass %, RE₂O₃=Rare Earth)

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Table 1. Compositions of glass (mass %, RE₂O₃=Rare Earth)

样品Sample	SiO₂	B₂O₃	Al₂O₃	Na₂O	ZnO	CaO	Li₂O	BaO	Cs₂O	RE₂O₃	ZrO₂	MoO₃
Zn-1	40.71	15.31	6.12	5.67	1.0	9.57	2.42	1.65	1.61	7.77	5.10	3.06
Zn-1.5	40.50	15.23	6.09	5.64	1.5	9.52	2.40	1.65	1.60	7.73	5.08	3.05
Zn-3.5	39.68	14.92	5.97	5.52	3.5	9.33	2.36	1.61	1.57	7.57	4.97	2.98
Zn-4	39.47	14.85	5.94	5.49	4.0	9.28	2.34	1.60	1.56	7.53	4.95	2.97
Zn-4.5	39.27	14.77	5.91	5.47	4.5	9.23	2.33	1.60	1.56	7.50	4.92	2.95
Zn-5	39.06	14.69	5.88	5.44	5.0	9.19	2.32	1.59	1.55	7.46	4.90	2.94

Table 2. Density, Mo leaching rate r_Mo, T_g and ZnO

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Table 2. Density, Mo leaching rate r_Mo, T_g and ZnO

样品 Sample	密度 Density/ g∙cm^-3	T_g-DSC / ℃	T_g-CTE / ℃	CTE / 10^-6 K^-1	r_Mo/ g∙m^-2∙d^-1	ZnO / mol%
Zn-1	2.82	532.1	542.5	8.26	0.020 7	0.87
Zn-1.5	2.82	532.6	541.0	8.50	0.435 7	1.31
Zn-3.5	2.86	522.5	534.0	8.27	0.026 1	3.05
Zn-4	2.86	528.8	536.3	8.18	0.088 7	3.49
Zn-4.5	2.87	527.0	535.6	8.31	0.054 5	3.93
Zn-5	2.84	520.8	533.0	8.34	0.046 0	4.37

Table 3. IR peak fitting band assignments from references^[32-33]

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Table 3. IR peak fitting band assignments from references^[32-33]

峰值位置Peak position P1~P10 / cm^-1	峰面积Band area	振动峰归属Band assignments
450~462	A₁	δ (O-B-O) and δ (Si-O-Si)
518~528	A₂	Si-O-Si rocking
690~707	A₃	δ (B-O-B) in pentaborate, δ (B-O-Si), δ (B-O-B) in [BO₃]
747~780	A₄	Si-O-Si and ν_as (B-O) in [BO₄]
836~883	A₅	ν_s(Si-O-Si)
945~973	A₆	ν(Si-O-Si), ν(B-O) in BO₄ from di-, penta-borate
995~1 078	A₇	ν_as(Si-O-Si) in [SiO₄], ν_as(Si-O) in Q³, ν(B-O) in BO₄ from tri-, tetra-, penta-borate
1 120~1 209	A₈	ν(Si-O-Si) in [SiO₄] (Q⁴)
1 276~1 398	A₉	ν_as [BO₃] and ν_as BO₂O^-
1 400~1 440	A₁₀	偏硼三角单元的振动Vibration of metaborate triangle

Table 4. Deconvolution peak areas of the IR spectra of the glasses

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Table 4. Deconvolution peak areas of the IR spectra of the glasses

样品Sample	A₁	A₂	A₃	A₄	A₅	A₆	A₇	A₈	A₉	A₁₀	A₆+A₇
Zn-1	7.5	0.9	1.8	0.6	0.0	18.9	47.1	1.4	6.8	15.0	66.0
Zn-1.5	6.4	1.4	1.7	0.5	3.8	0.0	45.5	21.3	0.5	19.0	45.4
Zn-3.5	7.7	0.9	2.2	1.0	7.9	22.6	38.1	0.0	1.3	18.4	60.7
Zn-4	8.7	0.7	1.5	0.0	1.6	5.0	57.1	10.4	1.5	13.4	62.1
Zn-4.5	6.4	1.3	2.4	0.4	11.5	0.4	51.8	0.0	14.5	11.4	52.1
Zn-5	8.3	0.7	1.7	0.8	7.1	0.0	46.2	14.3	1.0	19.9	46.2

Table 5. Designed glass compositions of validation samples V₁, V₂, V₃ (mass, %)

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Table 5. Designed glass compositions of validation samples V₁, V₂, V₃ (mass, %)

样品Sample	SiO₂	B₂O₃	Al₂O₃	Na₂O	ZnO	CaO	Li₂O	BaO	Cs₂O	RE₂O₃	ZrO₂	MoO₃
V₁	42.23	10.00	6.35	5.88	3.18	9.93	2.51	1.72	1.67	8.06	5.29	3.18
V₂	35.47	13.34	5.34	16.00	2.67	8.34	2.11	1.44	1.41	6.77	4.45	2.67
V₃	40.73	15.32	6.13	5.67	3.06	9.58	2.42	1.66	1.61	7.77	3.00	3.06

Table 6. Deconvolution peak areas of the IR spectra of the validation glasses
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Table 6. Deconvolution peak areas of the IR spectra of the validation glasses
样品Sample A₁ A₂ A₃ A₄ A₅ A₆ A₇ A₈ A₉ A₁₀ A₆+A₇
V₁ 9.4 0.7 2.3 1.39 7.69 0 48.4 7.98 2.8 19.3 48.4
V₂ 8.8 1.0 2.5 0.42 0 16.93 51.06 0.12 3.6 15.4 68.0
V₃ 8.5 1.6 1.8 0.6 3.32 0 66.51 0.90 3.3 13.5 66.5

Table 7. Model predicted and measured r_Mo of the validation glasses
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Table 7. Model predicted and measured r_Mo of the validation glasses
样品Sample V₁ V₂ V₃
Pred.r_Mo 0.028 0.017 0.206
Mea.r_Mo 0.012 0.032 0.195

Table 8. Closely related glass components to A₂ and A₈with the correlation coefficients (R₂O=alikali)
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Table 8. Closely related glass components to A₂ and A₈with the correlation coefficients (R₂O=alikali)
截距Intercept B₂O₃ ZnO R₂O R₂O×B₂O₃ ZrO₂
A₂ -36.2 1.73 — 1.46 1.81 -0.14
A₈ -14.5 — 3.31 -0.44 — 3.23

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Hailong DONG, Chen DAI, Zhongdi LI, Shubin CHEN, Sijun FAN, Liyan ZHANG. Effect of ZnO in borosilicate solidification glass on Mo leaching rate in simulated high-level radioactive waste and its model prediction[J]. NUCLEAR TECHNIQUES, 2024, 47(6): 060502

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