废钒钛系脱硝催化剂碱法回收研究进展

doi:10.16085/j.issn.1000-6613.2022-1116

摘要/Abstract

摘要：

废钒钛系脱硝催化剂属于HW50危险废物，富含V、W/Mo和Ti战略金属资源，具有污染性和资源性的双重特性，对其进行回收具有重要的经济价值和环境效益。碱法回收是当前的主流回收工艺。本文主要总结了废钒钛系脱硝催化剂碱浸法和碱焙烧法回收的研究进展，重点分析了采用NaOH、NH₄OH、(NH₄)₂CO₃等碱性溶液浸出以及采用NaOH、Na₂CO₃、CaO等碱性化合物焙烧提取工艺参数及对其中有价金属元素的回收效果。针对当前碱法工艺存在的碱耗量大、能耗高、废液产生量大、污染严重等相应问题，提出了进一步关注点应集中于阐明多种碱性物质之间的协同作用，通过混合碱的耦合反应提升回收效果。本文对降低废钒钛系脱硝催化剂回收能耗，提升碱性化合物利用率和回收产品质量具有良好的指导意义。

关键词: 废钒钛系脱硝催化剂, 回收, 碱浸法, 碱焙烧法

Abstract:

Waste vanadium-titanium-based deNO _x catalysts belong to HW50 hazardous wastes. They are rich in V, W/Mo and Ti strategic metal resources, and have dual characteristics of pollution and resources, and thus their recycling has important economic value and environmental benefits. Alkali recovery is the current mainstream recovery process. This paper mainly summarized the research progress of alkali leaching and alkali calcination recovery of waste vanadium-titanium-based deNO _x catalysts. The process parameters of leaching with alkaline solutions such as NaOH, NH₄OH and (NH₄)₂CO₃, calcination and extraction with alkaline compounds such as NaOH, Na₂CO₃ and CaO, and the recovery effect of valuable metal elements are analyzed. In view of the corresponding problems such as large alkali consumption, high energy consumption, large amount of waste liquid and serious pollution in the current alkali process, it is proposed that further attention should be focused on the clarification of the synergistic effect between various alkaline substances that is through the coupling reaction of mixed alkalis to improv the recovery effect. This paper have good guiding significance for reducing the energy consumption of waste vanadium-titanium-based deNO _x catalyst recovery and improving the utilization rate of basic compounds and the quality of recovered products.

Key words: spent vanadium-titanium-based deNO _x catalyst, recovery, alkali leaching, alkali calcination

中图分类号:

X773

张新远, 张柏林, 张深根. 废钒钛系脱硝催化剂碱法回收研究进展[J]. 化工进展, 2022, 41(S1): 580-594.

ZHANG Xinyuan, ZHANG Bolin, ZHANG Shengen. Research progress on recovery of spent vanadium-titanium based deNO _x catalyst with alkaline process[J]. Chemical Industry and Engineering Progress, 2022, 41(S1): 580-594.

图/表 18

图1 2014—2026年废脱硝催化剂预测产生量[13]

表1 几组不同工作环境废钒钛系脱硝催化剂成分（质量分数）

样品	TiO₂/%	V₂O₅/%	WO₃/%	SO₃/%	As₂O₃/%	Al₂O₃/%	CaO/%	P₂O₅/%	其他/%
样品A	84.33	0.77	4.56	3.20	0.08	1.96	1.08	0.14	3.88
样品B	86.98	1.37	2.21	3.11	0.08	1.32	0.90	2.73	1.30
样品C	84.83	0.84	2.7	4.3	0..30	1.25	1.70	0.12	3.96
样品D	74.93	2.16	4.01	10.57	0.19	1.05	1.92	0.10	5.07

图2 碱浸法总体工艺路线

图3 NaOH体系反应热力学计算结果[30]

图4 核收缩模型浸出示意图[31]

图5 NH4OH体系反应热力学计算[26, 39]

图6 废脱硝催化剂浸出渣的SEM和XRD图[37]

图7 (NH4)2CO3浸出体系热力学和动力学计算、浸出渣表征[41]

表2 不同成分的混合碱液对W、V浸出率对比

基础碱液	添加物	W浸出率（最高）/%	V浸出率（最高）/%	参考文献
20%Na₂CO₃	无	74.17	60.00	［45］
	5%~8% NaOH	74.75	99.9	［36，45］
	0~10% Na₃PO₄	72.67	87.77	［45］
	0~7% NaNO₃	74.95	88.84	［45］

图8 钠化焙烧工艺流程

图9 钙化焙烧工艺流程

图10 550℃焙烧样品的SEM和XRD图像[50]

图11 NaOH焙烧过程HSC软件热力学计算结果[50]

图12 焙烧后样品的XRD和SEM图[62, 65]

图13 不同温度钙化焙烧各反应的吉布斯自由能[66]

图14 连续焙烧CaO-H2C2O4浸出法

图15 CaO-H2C2O4浸出法物相变化[67]

图16 混合碱焙烧工艺流程[71]

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