限域型催化剂Ni@S_(2)对甲烷干重整反应性能影响  

Effect of confined catalyst Ni@S_(2) on performance of methane dry reforming reaction

作　　者：朱继成 杨期鑫 梁浩权 王增坤 欧阳富贵 邸婧 盖希坤 ZHU Jicheng;YANG Qixin;LIANG Haoquan;WANG Zengkun;OUYANG Fugui;DI Jing;GAI Xikun(College of Biological and Chemical Engineering,Zhejiang University of Science and Technology,Hangzhou 310023,China)

机构地区：[1]浙江科技大学生物与化学工程学院,浙江杭州310023

出　　处：《无机盐工业》2025年第2期138-146,共9页Inorganic Chemicals Industry

基　　金：重质油国家重点实验室开放课题项目(SKLHOP202202002);浙江省“尖兵”“领雁”研发攻关计划项目(2023C04021);浙江科技大学科研成果奖培育项目(2023JLZD008)。

摘　　要：甲烷干重整反应(DRM)能够合理利用CO_(2)和CH_(4)两种温室气体,生产出环保清洁的燃料CO和H_(2),然而该工艺所使用的镍基催化剂在高温下易发生积炭和烧结,难以满足工业化生产的需求。基于此,采用研磨晶化法制备了限域型Ni@S_(2)(Silicalite-2)催化剂。结果表明,限域型Ni@S_(2)催化剂呈现出橄榄状晶体结构,比表面积大,孔径分布窄,且NiO纳米颗粒均匀地分散在Silicalite-2骨架中,NiO平均晶粒尺寸约为4.63nm。在700℃下进行6h的甲烷干重整反应[进料流速Fin=40mL/min,V(CH_(4))∶V(CO_(2))∶V(Ar)=44∶44∶12],相较于负载型催化剂10Ni/SiO_(2),限域型10Ni@S_(2)催化剂的CH_(4)瞬时转化率从65.51%提高至91.91%,CO_(2)的瞬时转化率从71.89%提高至91.14%,积炭率从16.30%降低至1.20%。催化剂优异的催化性能和稳定性得益于其限域结构,不仅避免了活性组分烧结,降低了NiO的颗粒尺寸,还提高了金属与载体间的相互作用力。该研究为低成本、高稳定性的镍基催化剂的开发开辟了新的方向。The dry reforming reaction(DRM)of methane can rationally utilize two greenhouse gases of CO_(2) and CH_(4) to pro-duce environmentally friendly and clean fuels of CO and H_(2).However,the nickel-based catalysts used in this process are susceptible to carbon accumulation and sintering at high temperatures,which makes it difficult to satisfy the demands of in-dustrial production.Based on this,domain-limited Ni@S_(2)(Silicalite-2)catalysts were prepared by the grinding crystalliza-tion method.The results showed that the domain-limited Ni@S_(2) catalyst exhibited an olivine-like crystal structure with a large specific surface area and a narrow pore size distribution,and the NiO nanoparticles were uniformly dispersed in the Silicalite-2 skeleton,with an average NiO grain size of about 4.63 nm.After the dry reforming reaction at 700℃for 6 h[Fin=40 mL/min,V(CH_(4))∶V(CO_(2))∶V(Ar)=44∶44∶12],compared with the loaded catalyst 10Ni/SiO_(2),the confined 10Ni@S_(2) catalysts exhibited excellent catalytic activity and carbon deposition resistance,the instantaneous conversion of CH_(4) was in-creased from 65.51%to 91.91%,the instantaneous conversion of CO_(2) was increased from 71.89%to 91.14%,and the car-bon deposition rate was decreased from 16.30%to 1.20%.The excellent catalytic performance and stability of the catalyst were due to the limited domain structure,which avoided the sintering of the active component,reduced the particle size of NiO,and improved the interaction between the metal and the support.This study opened up a new direction for the prepara-tion of low cost and high stability nickel-based catalysts.

关 键 词：研磨晶化法 甲烷干重整反应 Silicate-2沸石 限域型催化剂 积炭 

分 类 号：O643.3[理学—物理化学]