Enhancing photo-generated carriers transfer of K-C_(3)N_(4)/UiO-66-NH_(2) with Er doping for efficient photocatalytic oxidation of furfural to furoic acid  

Er掺杂增强K-C_(3)N_(4)/UiO-66-NH_(2)的光生载流子转移用于糠醛高效光催化氧化制糠酸

作　　者：WANG Haocun LIU Lingtao BIAN Junjie LI Chunhu 王浩存;刘令涛;卞俊杰;李春虎(中国海洋大学化学化工学院海洋化学理论与工程技术教育部重点实验室,山东青岛266100)

机构地区：[1]Key Laboratory of Marine Chemistry Theory and Technology of Ministry of Education,Ocean University of China,Qingdao 266100,China

出　　处：《燃料化学学报（中英文）》2024年第11期1617-1628,共12页Journal of Fuel Chemistry and Technology

基　　金：supported by Natural Science Foundation of Shandong Province(ZR2022MB049);National Natural Science Foundation of China(22078174)。

摘　　要：Biomass-derived platform molecules,such as furfural,are abundant and renewable feedstock for valuable chemical production.It is critical to synthesize highly efficient photocatalysts for selective oxidation under visible light.The Er@K-C_(3)N_(4)/UiO-66-NH_(2) catalyst was synthesized using a straight-forward hydrothermal technique,and exhibited exceptional efficiency in the photocatalytic oxidation of furfural to furoic acid.The catalyst was thoroughly characterized,confirming the effective adjustment of the band gap energy of Er@K-C_(3)N_(4)/UiO-66-NH_(2).Upon the optimized reaction conditions,the conversion rate of furfural reached 89.3%,with a corresponding yield of furoic acid at 79.8%.The primary reactive oxygen species was identified as·O_(2)^(-) from ESR spectra and scavenger tests.The incorporation of Er and K into the catalyst enhanced the photogenerated carriers transfer rate,hence increasing the separating efficiency of photogenerated electron-hole pairs.This study expands the potential applications of rare earth element doped g-C_(3)N_(4) in the photocatalytic selective oxidation of furfurans.生物质衍生的平台分子如糠醛是一种丰富、可再生的化工原料,可被转化为高值化学品。在糠醛转化为高值化学品的过程中,制备可见光响应的高效选择氧化光催化剂至关重要。本研究采用直接水热法合成了Er@K-C_(3)N_(4)/UiO-66-NH_(2)催化剂,在糠醛光催化氧化制备糠酸的反应中表现出优异的催化活性。对催化剂进行了充分的表征,证实Er@KC_(3)N_(4)/UiO-66-NH_(2)催化剂的带隙被有效调控。反应条件优化后,糠醛的转化率达到89.3%,相应的糠酸产率为79.8%。ESR测试和活性氧物种捕获实验的结果表明,反应过程中的主要活性氧物种为·O_(2)^(-)。Er和K的掺杂提高了催化剂的光生载流子转移速率,从而提高了光生电子-空穴对的分离效率。本研究拓展了稀土元素掺杂g-C_(3)N_(4)在糠醛光催化选择性氧化中的潜在应用。

关 键 词：FURFURAL furoic acid selective catalytic oxidation MOFS carbon nitride 

分 类 号：TK6[动力工程及工程热物理—生物能]