强氧还原性氮化硼的制备及其催化甲烷部分氧化反应性能
Preparation of strongly oxygen reduction boron nitride and its catalytic performance for partial oxidation of methane
闫妍琼 1王晓斌 2陈海洁 1吕岩 1原沁波 3丁传敏 1王俊文1
作者信息
- 1. 太原理工大学 化学工程与技术学院,山西 太原 030024
- 2. 上海电气国控环球工程有限公司,山西 太原 030024
- 3. 清创人和生态工程技术有限公司,山西 太原 030031
- 折叠
摘要
氮化硼(BN)作为一种新兴的二维无机材料,近年来在烷烃氧化脱氢方面得到了广泛的应用,目前有研究表明氧物种的引入可以使BN具有更好的催化性能.采用以硼酸为硼源、尿素为氮源直接共融的合成方法制备了含氧BN催化剂(n(硼酸):n(尿素)=1:1、1:2、1:3和1:4),探究了在温度400～700℃、空速14400 mL/(g·h)和V(CH4):V(O2)=2:1的反应条件下,催化剂在甲烷部分氧化(POM)反应中的催化性能.采用FT-IR、ICP-OES、XRD和循环伏安(CV)等测试方法对催化剂的含氧官能团、元素含量(质量分数)、晶相结构和氧还原性能等进行了表征.结果表明,在POM反应中,n(硼酸):n(尿素)=1:2条件下制得的催化剂(BN-1:2)表现出最佳的催化性能(CH4转化率43%,CO选择性72%,H2选择性17%).与其他3种催化剂相比,BN-1:2具有最高的结晶度,使其与O2的相互作用更强,促进O2活化,而且BN-1:2在CV测试中具有最大的电流密度(3.4889×10-4 A/cm2),说明其具有最强的氧还原性能,可促进活性位点形成,从而表现出更好的催化性能.
Abstract
As an emerging two-dimensional inorganic material,boron nitride(BN)has been widely used in the oxidative dehydrogenation of alkanes in recent years,and it is now shown that the introduction of oxygen species makes the BN have a better catalytic performance.The oxygenated BN catalysts(n(boric acid):n(urea)=1:1,1:2,1:3 and 1:4)were prepared by direct co-fusion synthesis using boric acid as the boron source and urea as the nitrogen source.Under the conditions of temperature from 400 to 700℃,space velocity 14400 mL/(g·h)and V(CH4):V(O2)=2:1,the catalytic performances of the catalysts for partial oxidation of methane(POM)reaction were investigated.The oxygen-containing functional groups,elemental contents(mass fraction),crystalline structures and oxygen reduction abilities of the catalysts were characterized by FT-IR,ICP-OES,XRD and cyclic voltammetry(CV).The results show that in POM reaction,the catalyst(BN-1:2)under the condition of n(boric acid):n(urea)=1:2 exhibites the best catalytic performance(CH4 conversion rate of 43%,CO selectivity of 72%and H2 selectivity of 17%).Compared with the other three catalysts,BN-1:2 has the highest crystallinity,which makes the interaction between BN-1:2 and O2 stronger and promotes O2 activation.BN-1:2 has the highest current density in CV tests,indicating that it has the strongest oxygen reduction capability(3.4889×10-4 A/cm2),which promotes active site formation and thus exhibits better catalytic performance.
关键词
氮化硼/甲烷部分氧化/氧还原性能/催化剂Key words
boron nitride/partial oxidation of methane/oxygen reduction capability/catalysts引用本文复制引用
出版年
2024
国家科技期刊平台
NSTL
万方数据