Annealing crystallization control mechanism of catalytic degradation properties of Fe-based amorphous ribbons

Yu Xiu-Dong; Liu Hai-Shun; Xue Lin; Zhang Xiang; Yang Wei-Ming

doi:10.7498/aps.73.20240249

Abstract

Amorphous alloys are meta-stable materials with long-range disordered atomic structure, which have excellent catalytic degradation performance and are also susceptible to crystallization, but the mechanism of the effect of crystallization on their catalytic properties has not been clarified. Therefore, the effect of the annealing crystallization process on the microstructure of Fe-Si-B-Cu-Nb industrial amorphous ribbons and their catalytic degradation properties for acid orange 7 are investigated in this work. It is found that the catalytic degradation performance of the ribbons decreases dramatically after having been annealed at 460–580 ℃ , and its reaction rate constant is less than 0.01 min^–1. The main reason is the formation of α-Fe precipitation phase in the ribbons after having been annealed at high temperatures and the destruction of the substable amorphous structure. These reduce the rate of hydroxyl radical formation. In contrast, the catalytic degradation performance of the 650–700 ℃ annealed ribbons increases significantly, which increases to 3.77 times the degradation rate of the as-cast ribbons. The decolorization rate of acid orange 7 by the annealed ribbons reaches 99.22% within 15 min, which is 1.12 times that of the as-cast ribbons. The improvement of the catalytic degradation performance is attributed to the primary cell effect between the crystalline phase and the metal compounds and the substitution reaction between the Cu-enriched clusters and zero-valent iron. In this study, the influence mechanism of annealing crystallization on the performance of Fe-Si-B-Cu-Nb industrial amorphous ribbons for degrading azo dyes is revealed, which provides theoretical and experimental support for using aged iron-based amorphous ribbons to purify printing and dyeing waste-water and achieve “purification of waste-water by using alloy waste”.

Keywords:

Authors and contacts

1.
School of Materials and Physics, China University of Mining and Technology, Xuzhou 221116, China
2.
School of Mechanics and Materials, Hohai University, Nanjing 210098, China
3.
School of Mechanics and Civil Engineering, China University of Mining and Technology, Xuzhou 221116, China

Corresponding author: Liu Hai-Shun, Liuhaishun@cumt.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 52371167), the Scientific Research and Innovation Program of Jiangsu Province, China (Grant No. KYCX23_2653), and the China University of Mining and Technology Master’s Degree “Distinguished Talent”Booster Program (Grant No. 2023WLJCRCZL272).

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References

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Cited By

图 1 Fe-Si-B-Cu-Nb工业条带的(a) XRD和(b) DSC图谱

Figure 1. (a) XRD spectrum and (b) DSC spectrum of Fe-Si-B-Cu-Nb industrial ribbon.

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图 2 Fe-Si-B-Cu-Nb工业条带不同温度退火后的XRD图谱

Figure 2. XRD patterns of Fe-Si-B-Cu-Nb industrial ribbons after annealing at different temperatures.

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图 3 工业非晶条带及其经不同温度退火20 min后降解酸性橙7的紫外光谱图　(a) 工业非晶条带; (b) 460℃; (c) 520 ℃; (d) 580 ℃; (e) 650 ℃; (f) 700 ℃

Figure 3. UV spectra of industrial amorphous ribbons and their degraded acid orange 7 after annealing at different temperatures for 20 min: (a) Industrial amorphous ribbon; (b) 460℃; (c) 520 ℃; (d) 580 ℃; (e) 650 ℃; (f) 700 ℃.

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图 4 Fe-Si-B-Cu-Nb工业非晶条带及其经不同温度退火后对酸性橙7的降解　(a) C_t/C₀归一曲线; (b)染料脱色率; (c) －ln函数; (d)反应速率常数柱状图

Figure 4. Degradation of acid orange II processed by Fe-Si-B-Cu-Nb industrial amorphous ribbons in the as-cast state and after different annealing temperatures: (a) C_t/C₀ normalized graph; (b) dye decolorization rate graph; (c) variation of the －ln function graph; (d) histogram of reaction rate constants.

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图 5 不同温度退火条带降解酸性橙7后的表面SEM图　(a)—(d)未退火; (e)—(h) 580 ℃退火; (i)—(l) 700 ℃退火

Figure 5. SEM images of the alloy surface after degrading the acid orange II: (a)–(d) As-cast alloys without annealing; (e)–(h) after annealing at 580 ℃; (i)–(l) after annealing at 700 ℃.

DownLoad: Full-Size Img PowerPoint

图 6 700 ℃退火20 min后条带表面(a) SEM图像及对应的(b) Cu, (c) O, (d) C, (e) Fe和(f) Si元素分布图像

Figure 6. SEM images of Fe-Si-B-Cu-Nb alloy after annealing at 700 ℃ for 20 min (a); the corresponding elemental distribution maps of (b) Cu, (c) O, (d) C, (e) Fe, and (f) Si.

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表 1 用于偶氮染料催化降解的典型非晶合金比较

Table 1. Comparison of typical amorphous alloys for catalytic degradation of azo dyes.

合金成分	样品状态	染料种类	反应速率常数(k_obs)	循环次数	参考文献
Fe₈₃Si₅B₈P₄	条带	亚甲基蓝	0.514	—	[13]
(Fe₇₈Si₉B₁₃)₉₉Zr₁	条带	亚甲基蓝	0.24	—	[14]
Fe₈₄B₁₆	条带	直接蓝6	0.110	—	[16]
Fe₇₈Si₉B₁₃	条带	甲基蓝	0.085	—	[17]
Fe₇₈Si₁₁B₉P₂	条带	酸性橙7	0.082	17	[20]
Fe₈₀P₁₃C₇	条带	亚甲基蓝	0.56	23	[21]
Cu₄₆Zr_44.5Al_7.5Gd₂	条带	酸性橙7	0.48	80	[28]
Mg₆₅Cu₂₅Y₁₀	粉末	直接蓝6	0.585	—	[29]
Co₆₅Mo₁₅B₂₀	非晶丝	直接蓝6	2.31	20	[30]
Cu_47.5Zr₄₆Al_6.5	条带	酸性橙7	0.165	10	[31]
Co₇₈Si₈B₁₄	粉末	酸性橙7	—	8	[32]
FeSiBCuNb	条带	酸性橙7	0.094	50	本工作
FeSiBCuNb (700℃退火后)	条带	酸性橙7	0.36	—	本工作

DownLoad: CSV

表 2 α-Fe晶粒尺寸计算结果

Table 2. Calculation results of α-Fe grain size.

	温度/℃
	460	520	580	650	700
β_hkl/(°)	0.80	0.71	0.66	0.27	0.21
D_hkl/nm	11.54	12.68	13.72	33.74	42.52
(hkl)	(220)	(220)	(220)	(220)	(220)

DownLoad: CSV

[1]	杨卫明, 刘海顺, 敦超超, 赵玉成, 窦林名 2012 物理学报 61 106802 Google Scholar Yang W M, Liu H S, Dun C C, Zhao Y C, Dou L M 2012 Acta Phys. Sin. 61 106802 Google Scholar
[2]	柳延辉 2017 物理学报 66 176106 Google Scholar Liu Y H 2017 Acta Phys. Sin. 66 176106 Google Scholar
[3]	柯海波, 蒲朕, 张培, 张鹏国, 徐宏扬, 黄火根, 刘天伟, 王英敏 2017 物理学报 66 176104 Google Scholar Ke H B, Pu Z, Zhang P, Zhang P G, Xu H Y, Huang H G, Liu T W, Wang Y M, 2017 Acta Phys. Sin. 66 176104 Google Scholar
[4]	Lai L M, Liu T H, Cai X H, Wang M, Zhang S B, Chen W, Guo S F 2021 Scripta Mater 203 114095 Google Scholar
[5]	孙奕韬, 王超, 吕玉苗, 胡远超, 罗鹏, 刘明, 咸海杰, 赵德乾, 丁大伟, 孙保安, 潘明祥, 闻平, 白海洋, 柳延辉, 汪卫华 2018 物理学报 67 126101 Google Scholar Sun Y T, Wang C, Lu Y M, Hu Y C, Luo P, Liu M, Xian H J, Zhao D Q, Ding D W, Sun B A, Pan M X, Wen P, Bai H Y, Liu Y H, Wang W H 2018 Acta Phys. Sin. 67 126101 Google Scholar
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[7]	Ge Y, Cheng J, Mo J, Xue L, Zhang B, Hong S, Wu Y, Liang X, Zhang X 2024 J. Alloy Compd. 976 173173 Google Scholar
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[11]	Qiao J C, Wang Q, Pelletier J M, Kato H, Casalini R, Crespo D, Pineda E, Yao Y, Yang Y 2019 Prog. Mater. Sci. 104 250 Google Scholar
[12]	Liang S X, Jia Z, Zhang W C, Li X F, Wang W M, Lin H C, Zhang L C 2018 Appl. Catal. B-Environ. 221 108 Google Scholar
[13]	Zuo M Q, Yi S H, Choi J 2021 J. Environ. Sci. 105 116 Google Scholar
[14]	Miao F, Wang Q Q, Di S Y, Yun L, Zhou J, Shen B L 2020 J. Mater. Sci. Technol. 53 163 Google Scholar
[15]	Chen Q, Yan Z C, Zhang H, Zhang L C, Ma H J, Wang W L, Wang W M 2020 Materials 13 3694 Google Scholar
[16]	Tang Y, Shao Y, Chen N, Yao K F 2015 Rsc Adv. 5 6215 Google Scholar
[17]	Jia Z, Duan X G, Qin P, Zhang W C, Wang W M, Yang C, Sun H Q, Wang S B, Zhang L C 2017 Adv. Funct. Mat. 27 1702258 Google Scholar
[18]	Liang S X, Wang X Q, Zhang W C, Liu Y J, Wang W M, Zhang L C 2020 Appl. Mat. Today 19 100543 Google Scholar
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[20]	Ji L, Chen J W, Zheng Z G, Qiu Z G, Peng S Y, Zhou S H, Zeng D C 2020 J. Phys. Chem. Solids 145 109546 Google Scholar
[21]	Wang Q Q, Chen M X, Lin P H, Cui Z Q, Chu C L, Shen B L 2018 J. Mat. Chem. A 6 10686 Google Scholar
[22]	Hou L, Wang Q Q, Fan X D, Miao F, Yang W M, Shen B L 2019 New J. Chem. 43 6126 Google Scholar
[23]	Chen S Q, Li M, Ji Q M, Chen X, Lan S, Feng T, Yao K F 2021 J. Non-Cryst. Solids 571 121070 Google Scholar
[24]	Tan L, Wang X Y, Wang S K, Qin X R, Xiao L F, Li C L, Sun S Q, Hu S Q 2023 New J. Chem. 47 11723 Google Scholar
[25]	Wei J, Zheng Z G, Zhao L, Qiu Z G, Zeng D C 2023 Colloid Surface A 666 131227 Google Scholar
[26]	Lassoued A, Li J F 2023 J. Phys. Chem. Solids 180 111475 Google Scholar
[27]	Yang W M, Wang Q Q, Li W Y, Xue L, Liu H S, Zhou J, Mo J Y, Shen B L 2019 Mat. Design 161 136 Google Scholar
[28]	Zheng K L, Qin X D, Zhu Z W, Zheng S J, Li H L, Fu H M, Zhang H F 2020 J. Mat. Chem. A 8 10855 Google Scholar
[29]	Luo X K, Li R, Zong J Y, Zhang Y, Li H F, Zhang T 2014 Appl. Surf. Sci. 305 314 Google Scholar
[30]	Tang M F, Lai L M, Ding D Y, Liu T H, Kang W Z, Guo N, Song B, Guo S F 2022 J. Non-Cryst. Solids 576 121282 Google Scholar
[31]	Zhao B W, Zhu Z W, Qin X D, Li Z K, Zhang H F 2020 J. Mat. Sci. Technol. 46 88 Google Scholar
[32]	Qin X D, Zhu Z W, Liu G, Fu H M, Zhang H W, Wang A M, Li H, Zhang H F, 2015 Sci. Rep. 5 18226 Google Scholar
[33]	Xie S H, Huang P, Kruzic J J, Zeng X, Qian H 2016 Sci. Rep. 6 21947 Google Scholar
[34]	陈双琴 2018 博士学位论文 (北京: 清华大学) Chen S Q 2018 Ph. D Dissertation (Beijing: Tsinghua University
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