Ca/Fe添加劑對焦炭在H<sub>2</sub>O+CO<sub>2</sub>氣氛中溶損反應的影響

竇明輝; 韓嘉偉; 孫洋; 孫章; 梁英華

doi:10.13374/j.issn2095-9389.2022.09.05.001

Ca/Fe添加劑對焦炭在H₂O+CO₂氣氛中溶損反應的影響

doi: 10.13374/j.issn2095-9389.2022.09.05.001

華北理工大學化學工程學院，唐山 063210

基金項目: 國家自然科學基金面上資助項目（51874136）

詳細信息

通訊作者:
E-mail: sunz@ncst.edu.cn

中圖分類號: TF526+.1
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出版歷程
- 收稿日期: 2022-09-05
- 網絡出版日期: 2022-10-31

Effect of Ca/Fe additives on solution loss reactions of cokes in H₂O+CO₂ atmosphere

College of Chemical Engineering, North China University of Science and Technology, Tangshan 063210, China

More Information

Corresponding author: E-mail: sunz@ncst.edu.cn

摘要

摘要: 為了探究富氫高爐內Ca/Fe基高反應性焦炭的溶損反應特性，以CO₂（N₂）載帶不同摩爾比例H₂O蒸氣（0～30%）進行焦炭溶損實驗，通過分析尾氣中CO和H₂的含量，研究Ca/Fe添加劑對焦炭在H₂O+CO₂混合氣氛下碳溶反應和水煤氣反應的影響。研究表明，焦炭在H₂O+CO₂和H₂O+N₂兩種氣氛下的焦炭反應性隨H₂O蒸氣載帶率增加呈線性關系，焦炭在H₂O+CO₂氣氛中溶損反應的擬合斜率k值明顯小于在H₂O+N₂氣氛中的k值，H₂O+CO₂混合氣氛中H₂O和CO₂與焦炭反應存在競爭關系。而且基礎焦炭（BC）反應性的實驗與理論的差值明顯小于Ca/Fe基焦炭（BC+Ca、BC+Fe）的差值，表明Ca/Fe添加劑影響了CO₂和H₂O與焦炭共同反應時的競爭關系。基于兩種氣氛下速率常數的差異提煉了兩個抑制因子α_CO2/H2O和α_H2O/CO2，α_CO2/H2O定量表征CO₂對C+H₂O反應的抑制程度，α_CO2/H2O定量表征H₂O對C+CO₂反應的抑制程度，BC、BC+Fe、BC+Ca三種焦炭的α_CO2/H2O分別為0.260、0.251、0.170，而α_H2O/CO2分別為0.121、0.217、0.263，Ca/Fe添加劑降低了α_CO2/H2O而提高了α_H2O/CO2，說明Ca/Fe添加劑能夠減小CO₂對C+H₂O反應的抑制程度，顯著增強C+H₂O反應的活性。Ca/Fe基焦炭中催化活性物質為鐵酸鈣和硅鋁酸鈣，Ca/Fe元素在焦炭中賦存形式的不同導致了Ca/Fe添加劑對焦炭溶損反應催化效果的差異性。
- 焦炭 /
- Ca/Fe添加劑 /
- 溶損反應 /
- H₂O+CO₂混合氣氛 /
- 催化 /
- 抑制因子
Abstract: To examine the solution loss reaction properties of cokes with Ca/Fe additives in a hydrogen-rich blast furnace, the solution loss reactions of cokes were performed using a CO₂ (N₂) carrier gas with various percentages (0–30%) of H₂O vapor, and the effect of Ca/Fe additives on the Boudouard reaction (C + CO₂ = 2CO) and water–gas reaction (C + H₂O = CO + H₂) of cokes in a H₂O + CO₂ atmosphere was studied by examining the content of CO and H₂ in the off-gas. The results demonstrate that the coke reactivity has a positive linear relationship with the percentages of H₂O vapor in H₂O + CO₂ and H₂O + N₂ atmospheres, and the fitting slope k could be used to characterize the rate constant for the solution loss reaction of cokes in H₂O + CO₂ and H₂O + N₂ atmospheres. The k value for the solution loss reaction of the coke in the H₂O + CO₂ atmosphere is smaller than that of the coke in the H₂O + N₂ atmosphere, which shows that there is a competition between the reactions of H₂O and CO₂ with cokes in the H₂O + CO₂ atmosphere. Furthermore, the experimental reactivities of coke are smaller than their theoretical reactivities in the H₂O + CO₂ atmosphere, and the difference between the experimental and theoretical reactivities of the basic coke (BC) is less than those of the cokes with Ca/Fe additives (BC + Ca, BC + Fe), which shows that the Ca/Fe additives affect the competitive relationship of the reactions of CO₂ and H₂O with coke. Two inhibition factors, α_CO2/H2O and α_H2O/CO2, are proposed to measure the degree of inhibition based on the difference in the k value for the cokes in H₂O + CO₂ and H₂O + N₂ atmospheres. The inhibition factor α_CO2/H2O could quantitatively characterize the inhibition degree of CO₂ on C + H₂O reaction in the H₂O + CO₂ atmosphere, and the inhibition factor α_H2O/CO2 could quantitatively characterize the inhibition degree of H₂O on the C + CO₂ reaction in the H₂O + CO₂ atmosphere. The α_CO2/H2O factors of BC, BC + Fe, and BC + Ca cokes are 0.260, 0.251, and 0.170, respectively, and the α_H2O/CO2 factors of BC, BC + Fe, and BC + Ca are 0.121, 0.217, and 0.263, respectively. The Ca/Fe additives in cokes reduce the α_CO2/H2O factor and increase the α_H2O/CO2 factor, showing that Ca/Fe additives can attenuate the inhibition degree of CO₂ on the C + H₂O reaction and improve the activity of the C + H₂O reaction, and the Ca additive has a greater impact on the competitive relationship between the reactions of CO₂ and H₂O with coke than the Fe additive. The catalytically active substances in Ca/Fe additives in cokes could be CaFe₂O₄ and Ca₂Al₂SiO₇, and the difference in the existing states of Ca/Fe elements in cokes causes the difference in the catalytic effect of Ca/Fe additives on the solution loss reactions of cokes.
- coke /
- Ca/Fe additives /
- solution loss reaction /
- H₂O + CO₂ atmosphere /
- catalysis /
- inhibition factor

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圖 1 實驗過程各參數實時曲線

Figure 1. Parameter curves in the experimental process

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圖 2 焦炭的反應性（PRI）與水蒸氣載帶率的關系. (a) BC (b) BC+Fe; (c) BC+Ca

Figure 2. Relationship of coke reactivity (PRI) with the percentages of steam in carrier gas: (a) BC; (b) BC + Fe; (c) BC + Ca

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圖 3 H₂O+CO₂混合氣氛下焦炭溶損反應尾氣中CO/H₂含量曲線. (a) BC; (b) BC+Fe; (c) BC+Ca

Figure 3. CO/H₂ content curves in the off-gas for coke solution loss reactions in the H₂O + CO₂ atmosphere: (a) BC; (b) BC + Fe; (c) BC + Ca

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圖 4 C+H₂O反應的焦炭反應性與水蒸氣載帶率的關系. (a) BC; (b) BC+Fe; (c) BC+Ca

Figure 4. Relationship of PRI in the C + H₂O reaction with the percentages of steam in carrier gas: (a) BC; (b) BC + Fe; (c) BC + Ca

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圖 5 C+ CO₂反應的焦炭反應性與水蒸氣載帶率的關系. (a) BC; (b) BC+Fe; (c) BC+Ca

Figure 5. Relationship of PRI in the C + CO₂ reaction with the percentages of steam in carrier gas: (a) BC; (b) BC + Fe; (c) BC + Ca

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圖 6 焦炭SEM-EDS能譜圖. (a) BC; (b)BC+Fe; (c)BC+Ca

Figure 6. SEM-EDS morphologies of cokes: (a) BC; (b) BC + Fe; (c) BC + Ca

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圖 7 焦炭溶盡碳素后灰渣的XRD圖譜. (a) BC; (b) BC+Fe; (c) BC+Ca

Figure 7. XRD patterns of ashes derived from cokes reacted with CO₂: (a) BC; (b) BC + Fe; (c) BC + Ca

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表 1 配合煤樣性質指標

Table 1. Main characteristics of the blending coals

M_ad/% A_d/% V_ad/% S_t,d/% G Y/mm b/% R_max/% A/I

0.94 9.93 21.50 1.05 86.3 15.5 12 1.39 2.25

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表 2 焦炭的工業分析和熱性質

Table 2. Proximate analysis and thermal properties of cokes %

Coke M_ad A_ad V_ad S_t,ad CRI CSR

BC 0.07 12.3 0.9 1.0 22.24 63.39
BC + Fe 0.10 13.2 0.7 0.7 28.52 53.23
BC + Ca 0.09 13.4 1.2 0.8 39.26 36.94

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表 3 H₂O+CO₂混合氣氛中焦炭反應性的實驗值與理論值

Table 3. Experimental and theoretical values of coke reactivity in the H₂O + CO₂ atmosphere

Coke x_H2O /% PRI_exp /% PRI_cal /%

BC 0 17.24 17.24
10 18.90 24.19
20 20.80 28.44
30 22.44 32.34
BC + Fe 0 26.44 26.44
10 27.65 33.64
20 30.33 40.48
30 31.70 45.04
BC + Ca 0 34.85 34.85
10 37.40 43.45
20 38.50 47.40
30 41.07 53.61

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表 4 H₂O與CO₂與焦炭反應的相互抑制因子

Table 4. Inhibition factors of the reactions of H₂O and CO₂ with cokes

Coke k₁′ k₁ α_CO2/H2O k₂′ k₂ α_H2O/CO2

BC 0.548 0.288 0.260 0 ?0.121 0.121
BC + Fe 0.651 0.400 0.251 0 ?0.217 0.217
BC + Ca 0.636 0.466 0.170 0 ?0.263 0.263

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Ca/Fe添加劑對焦炭在H₂O+CO₂氣氛中溶損反應的影響

doi: 10.13374/j.issn2095-9389.2022.09.05.001

通訊作者:
E-mail: sunz@ncst.edu.cn

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Effect of Ca/Fe additives on solution loss reactions of cokes in H₂O+CO₂ atmosphere

Corresponding author: E-mail: sunz@ncst.edu.cn

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目錄

M_ad/%	A_d/%	V_ad/%	S_t,d/%	G	Y/mm	b/%	R_max/%	A/I
0.94	9.93	21.50	1.05	86.3	15.5	12	1.39	2.25

Coke	M_ad	A_ad	V_ad	S_t,ad	CRI	CSR
BC	0.07	12.3	0.9	1.0	22.24	63.39
BC + Fe	0.10	13.2	0.7	0.7	28.52	53.23
BC + Ca	0.09	13.4	1.2	0.8	39.26	36.94

Coke	x_H2O /%	PRI_exp /%	PRI_cal /%
BC	0	17.24	17.24
	10	18.90	24.19
	20	20.80	28.44
	30	22.44	32.34
BC + Fe	0	26.44	26.44
	10	27.65	33.64
	20	30.33	40.48
	30	31.70	45.04
BC + Ca	0	34.85	34.85
	10	37.40	43.45
	20	38.50	47.40
	30	41.07	53.61

Coke	k₁′	k₁	α_CO2/H2O	k₂′	k₂	α_H2O/CO2
BC	0.548	0.288	0.260	0	?0.121	0.121
BC + Fe	0.651	0.400	0.251	0	?0.217	0.217
BC + Ca	0.636	0.466	0.170	0	?0.263	0.263

留言板

Ca/Fe添加劑對焦炭在H2O+CO2氣氛中溶損反應的影響

doi: 10.13374/j.issn2095-9389.2022.09.05.001

通訊作者: E-mail: sunz@ncst.edu.cn

計量

出版歷程

Effect of Ca/Fe additives on solution loss reactions of cokes in H2O+CO2 atmosphere

Corresponding author: E-mail: sunz@ncst.edu.cn

參考文獻

計量

出版歷程

目錄

Ca/Fe添加劑對焦炭在H₂O+CO₂氣氛中溶損反應的影響

通訊作者:
E-mail: sunz@ncst.edu.cn

Effect of Ca/Fe additives on solution loss reactions of cokes in H₂O+CO₂ atmosphere