摘要
燃煤电厂作为CO_(2)主要排放源,其碳减排在“双碳”目标下备受关注。CO_(2)甲烷化被认为是实现碳循环利用最实用有效的途径,但当前CO_(2)甲烷化领域最广泛采用的镍基催化剂,易因烟气中的SO_(2)发生硫中毒而失活。本研究采用湿浸渍法制备了一系列Mn改性Ni/γ-Al_(2)O_(3)催化剂,该催化剂具有抗硫中毒性能。通过XRD、XPS、CO_(2)-TPD、SO_(2)-TPD和H_(2)-TPR等多种方法对催化剂结构和物理化学性质进行研究,阐明了其保持高反应活性的同时具备抗硫性质的机理。结果表明,4Mn-Ni/Al_(2)O_(3)具有最佳的催化性能和抗硫性能,CO_(2)转化率最高达到88.27%,SO_(2)通入3 h后,CO_(2)转化率仅下降11.32%。机理研究表明,Mn可作为牺牲位点保护Ni位点免受硫中毒,同时Ni-Mn之间相互作用抑制了SO_(2)在催化剂表面的吸附,进而提升抗硫性能。该研究为燃煤含SO_(2)烟气的CO_(2)直接甲烷化利用提供了一条可行性方案。
Coal-fired power plants,as the primary source of CO_(2)emissions,have garnered significant attention for carbon reduction under the“dual carbon”goals.CO_(2)methanation is considered to be the most practical and effective way to achieve carbon recycling,however,the most widely used nickel-based catalysts in CO_(2)methanation are prone to sulfur poisoning deactivation due to SO_(2)in the flue gas.In this paper,a series of Mn-modified Ni/γ-Al_(2)O_(3)were prepared by wet impregnation method,which had anti-sulfur poisoning properties.The structure and physicochemical properties of the catalysts were investigated using various methods such as XRD,XPS,CO_(2)-TPD,SO_(2)-TPD and H_(2)-TPR,and the mechanism by which the maintain high catalytic activity while possessing sulfur resistance was elucidated.The results show that 4Mn-Ni/Al_(2)O_(3)exhibits the best catalytic performance and sulfur resistance,with a maximum CO_(2)conversion rate of 88.27%.After 3 h of SO_(2)exposure,the CO_(2)conversion rate only decreased by 11.32%.Mechanistic studies indicate that Mn can serve as a sacrificial site to protect Ni sites from sulfur poisoning,while the interaction between Ni and Mn suppresses the adsorption of SO_(2)on the catalyst surface,thereby enhancing sulfur resistance.This research provides a feasible solution for the direct methanation of CO_(2)from coal-fired SO_(2)flue gas.
作者
申瑛
许紫阳
陈亮
王春波
SHEN Ying;XU Ziyang;CHEN Liang;WANG Chunbo(School of Energy Power and Mechanical Engineering,North China Electric Power University,Baoding 071003,China;Hebei Key Laboratory of Low Carbon and High Efficiency Power Generation Technology,North China Electric Power University,Baoding 071003,China)
出处
《燃料化学学报(中英文)》
北大核心
2026年第1期58-68,共11页
Journal of Fuel Chemistry and Technology
基金
国家自然科学基金(52306135)
河北省自然科学基金(E2024502035)资助。
关键词
催化活性
催化剂
抗硫性能
活性位点
甲烷
catalytic activity
catalyst
sulfur resistance
active site
methane
