NH_(2)-UiO-66/PyPD-COF异质结构筑及高效光催化产氢  

Constructing NH_(2)-UiO-66/PyPD-COF heterojunction topromote efficient photocatalytic hydrogen production

作　　者：吴海洋 张楠琦 牟迪 何漩[1] 杜星[1] 王大珩 方伟[1] 陈辉[1] 李薇馨 赵雷[1] WU Haiyang;ZHANG Nanqi;MOU Di;HE Xuan;DU Xing;WANG Daheng;FANG Wei;CHEN Hui;LI Weixin;ZHAO Lei(The State Key Laboratory of Refractories and Metallurgy,Wuhan University of Science and Technology,Wuhan 430081,China)

机构地区：[1]武汉科技大学省部共建耐火材料与冶金国家重点实验室,武汉430081

出　　处：《功能材料》2024年第1期1141-1150,共10页Journal of Functional Materials

基　　金：国家自然科学基金项目(22105151);湖北省自然科学基金(2021CFB469,2021CFB124,2022CFB626);湖北省重点研究项目(2022BAA094);武汉市知识创新工程(2022010801010306);湖北省教育厅科研计划(B2022017)。

摘　　要：有机框架化合物因分子水平结构可控、大的比表面积、高孔隙率、分散的化学活性位点以及良好稳定性等优点,在光催化解水制氢方面具有较大的应用潜力。采用溶剂热法,在共价有机框架PyPD-COF的合成过程中引入金属有机框架NH_(2)-UiO-66,原位形成NH_(2)-UiO-66/PyPD-COF异质结。通过TEM、EDS、XPS、FTIR、UV-Vis和光电流测试分析,光催化性能测试等手段对样品进行表征,构筑的NH_(2)-UiO-66/PyPD-COF异质结不仅可以保留原始MOF及COF组分的优良特性,还可在异质界面形成键连,利于促进界面间电荷迁移,降低电子-空穴复合率,提升光催化产氢效率至20.68 mmol·h^(-1)·g^(-1),分别为原始NH_(2)-UiO-66和PyPD-COF的86倍和3倍。同时,界面处的共价键键连使得复合样品具有良好的制氢稳定性,这为构筑高效光催化分解水产氢异质结光催化剂提供了一种新的策略。Organic framework compounds have great application potential in photocatalytic water hydrogen production due to the advantages of controllable molecular structure,large specific surface area,high porosity,dispersed chemical active sites and good stability.In this paper,the metal-organic framework NH_(2)-UiO-66 was introduced into the synthesis process of the covalent organic framework PyPD-COF by solvothermal method,and NH_(2)-UiO-66/PyPD-COF heterojunction was formed in situ.The samples were characterized by TEM,EDS,XPS,FTIR,UV-Vis and photocurrent analysis,as well as photocatalytic performance test.The constructed NH_(2)-UiO-66/PyPD-COF heterojunction could not only retain the excellent properties of the original MOF and COF components,but also form bonds at the heterogeneous interface.It is beneficial to promote interfacial charge transfer,reduce electron-hole recombination rate,and increase photocatalytic hydrogen production efficiency to 20.68 mmol/(h·g),which is 86 times and 3 times of the original NH_(2)-UiO-66 and PyPD-COF,respectively.At the same time,the covalent bond at the interface makes the composite sample have good hydrogen production stability,which provides a new strategy for the construction of efficient photocatalytic decomposition of aquatic hydrogen heterojunction photocatalysts.

关 键 词：NH_(2)-UiO-66 PyPD-COF 异质结 原位生长 光催化产氢 

分 类 号：TB332[一般工业技术—材料科学与工程]