机构地区:[1]苏州科技大学土木工程学院,苏州215011 [2]硅基材料安徽省实验室,蚌埠233000
出 处:《科学通报》2025年第2期288-300,共13页Chinese Science Bulletin
基 金:国家自然科学基金(51902219);江苏省自然科学基金(BK20190949);硅基材料安徽省实验室开放课题基金(2022KF15);江苏高校“青蓝工程”(2023年)资助。
摘 要:挥发性有机物(volatile organic compounds,VOCs)的排放对环境和人类健康造成极大危害.四氧化三钴(Co_(3)O_(4))对VOCs有着极高的催化降解能力,被认为是最有潜力取代贵金属催化剂的金属氧化物之一.本文分别讨论了前驱体、沉淀剂、反应温度及后续热处理温度对制备的Co_(3)O_(4)催化剂催化降解苯活性的影响,通过对不同制备条件下的Co_(3)O_(4)催化剂光热催化苯活性的对比分析,获取了具有高效催化活性的Co_(3)O_(4)催化剂优化制备方案.研究发现,以醋酸钴作为前驱体、尿素作为沉淀剂、90℃反应、后续300℃煅烧制得的Co_(3)O_(4)催化剂表现出光热催化降解VOCs的最佳活性,最优的Co_(3)O_(4)催化剂在仅5 min内对15μL苯的催化降解率高达95.3%,并具有出色的催化稳定性.结合X射线衍射(X-ray diffraction,XRD)、扫描电子显微镜(scanning electron microscopy,SEM)、光吸收能力、比表面积测量(Brunauer-Emmett-Teller,BET)等表征结果,探究了Co_(3)O_(4)催化剂催化降解效率差异的原因.对最优Co_(3)O_(4)催化剂进行了进一步的室温下光催化、不同温度下热催化、光热催化活性以及活化能分析,发现其在200、240、290℃下光热协同催化效率始终大于光催化与热催化的简单加和,因此Co_(3)O_(4)催化剂在催化降解VOCs中存在光热协同效应.Volatile organic compounds(VOCs)are a class of organic compounds that are easily volatilized at room temperature,causing serious damage to the human body,soil,and water bodies,and affecting the balance of the ecosystem.Cobalt tetraoxide(Co_(3)O_(4))has a very high catalytic degradation ability for VOCs and is considered to be one of the metal oxides with the greatest potential to replace precious metal catalysts.Relevant studies have shown that Co_(3)O_(4)catalysts prepared under different conditions have excellent photocatalytic and thermocatalytic activities.This paper discusses the effects of precursors,precipitants,reaction temperatures,and subsequent heat treatment temperatures on the catalytic degradation activity of benzene by the prepared Co_(3)O_(4)catalysts.The activity differences of the samples were determined by the degradation rate of 15μL benzene and the CO2 generation rate of the Co_(3)O_(4)catalysts prepared under different conditions at 290℃,and the optimized preparation scheme of the Co_(3)O_(4)catalyst with high catalytic activity was obtained.The study found that the Co_(3)O_(4)catalyst prepared with cobalt acetate as a precursor,urea as a precipitant,90℃reaction,and subsequent 300℃calcination showed the best activity in photothermocatalytic degradation of VOCs.The optimal Co_(3)O_(4)catalyst had a catalytic degradation rate of 95.3%for 15μL benzene in only 5 min,and maintained a catalytic degradation rate of more than 95%for 15μL benzene after 10 photothermocatalytic degradation stability tests,proving its good catalytic stability.Combined with the test characterization results of XRD,SEM,UV-Vis-IR,TG,etc.,the reasons for the difference in catalytic degradation efficiency of Co_(3)O_(4)catalysts were explored:Co_(3)O_(4)catalysts prepared under different conditions have different absorption capacities for ultraviolet-visible-infrared light,and calcination at a too high temperature will increase the surface area of the Co_(3)O_(4)catalyst,resulting in a reduction in its active attach
关 键 词:Co_(3)O_(4) 光催化 光热催化 热催化 挥发性有机物
分 类 号:X701[环境科学与工程—环境工程] O643.36[理学—物理化学]
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