基于密度泛函理论镍配合物光催化产氢性能研究  

Research on the Photocatalytic Hydrogen Production Performance of Nickel Complexes Based on Density Functional Theory

作　　者：尹巧巧 黄颍 连婉琪 李双[1] 苗体方[1] YIN Qiaoqiao;HUANG Ying;LIAN Wanqi;LI Shuang;MIAO Tifang(School of Chemistry and Materials Science,Huaibei Normal University,235000,Huaibei,Anhui,China)

机构地区：[1]淮北师范大学化学与材料科学学院,安徽淮北235000

出　　处：《淮北师范大学学报（自然科学版）》2024年第4期24-28,共5页Journal of Huaibei Normal University：Natural Sciences

基　　金：安徽省高校科学研究项目(KJ2021B03)。

摘　　要：为开发新型高效光解水产氢催化剂,以金属镍(II)配合物为研究对象合成配合物[Ni(hql)_(2)(L_(1))](hql=8-羟基喹啉,L_(1)=5-氯-1,10-菲咯啉)(配合物1)和[Ni(hql)_(2)(L_(2))](L_(2)=1,10-菲咯啉-5-氨基)(配合物2)。产氢测试结果显示,2个配合物活性存在差异,配合物2表现相对较好的性能,催化活性为1401.83μmol·g^(-1)·h^(-1)。利用密度泛函理论(DFT)在B3LYP/6-31G(d)水平上计算前线分子轨道、静电势及电子吸收光谱,成功地验证催化剂的构效关系。针对结构相似但取代基不同的配合物,实验与理论相结合方法更为经济和高效,能够更深入地探究配合物结构和产氢性能关系。To develop novel and efficient photocatalysts for hydrogen production via water splitting,nickel(II)complexes[Ni(hql)_(2)(L_(1))](hql=8-hydroxyquinoline,L_(1)=5-chloro-1,10-phenanthroline)(complex 1)and[Ni(hql)_(2)(L_(2))](L_(2)=1,10-phenanthroline-5-amine)(complex 2)were synthesized.Hydrogen production tests revealed differences in activity between the two complexes,with complex 2 exhibiting superior performance,achieving a catalytic activity of 1401.83μmol·g^(-1)·h^(-1).Density Functional Theory(DFT)calculations at the B3LYP/6-31G(d)level were employed to compute the frontier molecular orbitals,electrostatic potential,and electronic absorption spectra,successfully validating the structure-activity relationship of the catalysts.For structurally similar complexes with different substituents,a combined experimental and theoretical approach is proved more economical and efficient,providing deeper insights into the relationship between complex structure and hydrogen production performance.

关 键 词：镍配合物 光催化 产氢 密度泛函理论 

分 类 号：O641[理学—物理化学]