高分散Ag/C_(3)N_(4)的制备及对硝基苯酚催化还原性能的研究  

Preparation of Highly Dispersed Ag/C_(3)N_(4)for Catalytic Reduction of p-nitrophenol

作　　者：陈兵兵[1,2] 解鹤 康建 马钰 薛亮 付昱 CHEN Bing-bing;JIE He;KANG Jian;MA Yu;XUE Liang;FU Yu(School of Science and Chemical Engineering,Ningxia Institute of Science and Technology,Shizuishan 753000,China;Department of Chemistry,College of Science,Northeastern University,Shengyang 110000,China)

机构地区：[1]宁夏理工学院理学与化学工程学院,宁夏石嘴山753000 [2]东北大学理学院化学系,辽宁沈阳110000

出　　处：《化学试剂》2024年第2期55-60,共6页Chemical Reagents

基　　金：国家自然科学基金项目(22175030);宁夏自然科学基金项目(2022AAC03342,2022AAC03343,2022AAC03350)。

摘　　要：金属纳米颗粒的聚集现象严重影响了催化效率,利用简单的方法制备高分散的金属基催化剂具有一定的挑战性;首先利用柔喷雾技术在液液界面上制备了3种银配位的超分子前驱体膜,即三聚氰胺/三聚氰酸/硝酸银超分子(MC-Ag)、三聚氰胺/巴比妥酸/硝酸银超分子(MB-Ag)和三聚氰胺/三聚氰酸/巴比妥酸/硝酸银超分子(MCB-Ag);再热缩聚得到高分散的MC-Ag/C_(3)N_(4)、MB-Ag/NC和MCB-Ag/NC这3种银负载材料。在对硝基苯酚的催化还原实验中,MC-Ag/C_(3)N_(4)、MB-Ag/NC和MCB-Ag/NC表观速率常数(k_(app))分别为192.5×10^(-3)、126.8×10^(-3)和128.8×10^(-3)min^(-1);MC-Ag/C_(3)N_(4)展现出了优良的催化性能,在20 min内催化效率高达99.8%,经过5次循环后催化效果仍保持在97%以上,催化性能主要是MC-Ag/C_(3)N_(4)具有g-C_(3)N_(4)二维结构使银纳米粒子更加分散,更有利于接触更多的活性位点;同时柔喷雾技术为纳米颗粒的制备和形貌的调控提供了新的思路。The aggregation of metal nanoparticles can significantly impact catalytic efficiency,posing a challenge in the preparation of highly dispersed metal-based catalysts through simple methods.To address this issue,we initially prepared three types of silver-coordinated supramolecular precursor films at the liquid-liquid interface using the soft spray technique.These films were identified as melamine/cyanuric acid/silver nitrate supramolecular(MC-Ag),melamine/barbituric acid/silver nitrate supramolecular(MB-Ag),and melamine/cyanuric acid/barbituric acid/silver nitrate supramolecular(MCB-Ag).Subsequently,we obtained highly dispersed MC-Ag/C_(3)N_(4),MB-Ag/NC,and MCB-Ag/NC through thermal polycondensation.In the catalytic reduction of p-nitrophenol,the apparent rate constants(k_(app))of MC-Ag/C_(3)N_(4),MB-Ag/NC and MCB-Ag/NC were determined as 192.5×10^(-3),126.8×10^(-3)and 128.8×10^(-3)min^(-1),respectively.Notably,MC-Ag/C_(3)N_(4)exhibited outstanding catalytic performance with an efficiency as high as 99.8%within 20 min.The catalytic effect remains above 97%after 5 cycles,mainly due to the g-C_(3)N_(4)two-dimensional structure of MC-Ag/C_(3)N_(4),which makes silver nanoparticles more dispersed and more conducive to contact with more active sites.It is noteworthy that soft spray technology provides a novel approach for the preparation and morphology control of nanoparticles.

关 键 词：柔喷雾技术 热缩聚 对硝基苯酚 催化还原 

分 类 号：O643.3[理学—物理化学]