基于第一性原理的Pd/Al_(2)O_(3)单原子催化剂还原CO_(2)研究  

Study on CO_(2) reduction reaction of Pd/Al_(2)O_(3) single-atom catalysts based on first principle

作　　者：董世知[1] 刘伟[1] 李岩帅 尚文龙 叶昆 赵志龙 尹金鹏 DONG Shizhi;LIU Wei;LI Yanshuai;SHANG Wenlong;YE Kun;ZHAO Zhilong;YIN Jinpeng(College of Materials Science and Engineering,Liaoning Technical University,Fuxin 123000,China)

机构地区：[1]辽宁工程技术大学材料科学与工程学院,辽宁阜新123000

出　　处：《辽宁工程技术大学学报（自然科学版）》2022年第4期345-349,共5页Journal of Liaoning Technical University (Natural Science)

基　　金：国家自然科学基金(52102360)

摘　　要：为研究贵金属Pd单原子催化剂在CO_(2)合成气生成甲酸的催化机理,基于密度泛函理论研究了Pd在二维晶态/非晶态Al_(2)O_(3)上的最佳吸附位置并模拟计算.通过计算给出态密度、能带结构以及吸附能来验证催化剂的稳定性、高效性,并结合CO_(2)还原转化反应过程中表面能及迁移能垒的分析,定性阐述催化机制.研究结果表明:二维α-Al_(2)O_(3)负载Pd单原子具有良好的化学稳定性,较高的电子迁移能力.过渡态能垒均在可控范围,可以实现催化剂的绿色催化.其中非晶结构凭借表面更高的局域电子浓度,与单原子的协同作用更加显著.这为从原子层次认识催化机理提供了研究思路,促进具有工业催化潜力的新型功能化负载型催化剂的研究发展.In order to study the catalytic mechanism of the noble metal Pd single-atom catalyst for the formation of formic acid in CO_(2)syngas,the vintage adsorption location of Pd on two-dimensional crystalline/amorphous Al_(2)O_(3)was studied based on density functional theory.The stability and high efficiency of the catalyst were verified by calculating the density of states,band structure and adsorption energy,and combined with the analysis of surface energy and migration energy barrier in the process of CO_(2)reduction and conversion reaction,the catalytic mechanism is qualitatively explained.The consequence shows that two dimensionalα-Al_(2)O_(3)loaded Pd single-atom has good chemical stability and higher electron migration ability.The transition state energy barrier is controllable with range,which can realize the green catalysis of catalyst.The synergistic effect between the amorphous structure and the single-atom is more significant due to the higher local electron concentration on the surface.This is for understanding the catalytic mechanism at the atomic level,and promotes the research and development of new functional supported catalysts with industrial catalytic potential.

关 键 词：单原子催化剂 二维材料 迁移能垒 CO_(2)催化还原 非晶态材料 

分 类 号：X701[环境科学与工程—环境工程] O643.36[理学—物理化学]