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

作　　者：闫妍琼 王晓斌 陈海洁 吕岩 原沁波 丁传敏[1] 王俊文[1] YAN Yanqiong;WANG Xiaobin;CHEN Haijie;LV Yan;YUAN Qinbo;DING Chuanmin;WANG Junwen(College of Chemical Engineering and Technology,Taiyuan University of Technology,Taiyuan 030024,Shanxi,China;Shanghai Electric Group State Owned Huanqiu Engineering Co.,Ltd.,Taiyuan 030024,Shanxi,China;Qing Chuang Ren He Ecological Engineering Technology Co.,Ltd.,Taiyuan 030031,Shanxi,China)

机构地区：[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

出　　处：《低碳化学与化工》2024年第12期27-32,46,共7页Low-Carbon Chemistry and Chemical Engineering

基　　金：山西自然科学基金面上项目(202203021221091)。

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(CH_(4)):V(O_(2))=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(CH_(4)转化率43%,CO选择性72%,H_(2)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O_(2)的相互作用更强,促进O_(2)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/cm^(2)),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。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(CH_(4)):V(O_(2))=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(CH_(4)conversion rate of 43%,CO selectivity of 72%and H_(2)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 O_(2)stronger and promotes O_(2)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/cm^(2)),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 

分 类 号：TQ426[化学工程] O643.36[理学—物理化学]