Covalent triazine frameworks modified by ultrafine Pt nanoparticles for efficient photocatalytic hydrogen production  

作　　者：Xu Han Xueying Ge Wen-Wen He Wangwang Shen Tao Zhou Jian-Sen Wang Rong-Lin Zhong Abdullah MAl-Enizi Ayman Nafady Shengqian Ma 

机构地区：[1]School of Chemistry and Life Science,Advanced Institute of Materials Science,Changchun University of Technology,Changchun 130012,China [2]Laboratory of Theoretical and Computational Chemistry,Institute of Theoretical Chemistry,College of Chemistry,Jilin University,Changchun 130021,China [3]Department of Chemistry,University of North Texas,1508 W.Mulberry St.Denton,TX 76201,USA [4]Department of Chemistry,College of Science,King Saud University,Riyadh 11451,Saudi Arabia

出　　处：《Nano Research》2024年第6期4908-4915,共8页纳米研究（英文版）

基　　金：the National Natural Science Foundation of China(Nos.22271022 and 21701016);the Science and Technology Development Planning of Jilin Province(No.YDZJ202201ZYTS342);the China Scholarship Council(CSC No.201802335014);Partial support from the Robert A.Welch Foundation(B-0027)(S.M.)and Researchers Supporting Program(No.RSP-2024R55)at King Saud University,Riyadh,Saudi Arabia is also acknowledged.

摘　　要：Pt nanoparticles(PtNPs)as active species have always been considered as one of the best semiconductor materials for photocatalytic hydrogen production.In this study,a Schottky heterojunction has been successfully constructed by evenly loading ultrafine PtNPs onto a triazine-based covalent organic frameworks(COFs).This strategy maintained the high activity of these ultra-small PtNPs while maximizing the utilization of the Pt active sites.The fabricated PtNPs@covalent triazine-based framework-1(CTF-1)composite accomplished a significantly high rate of hydrogen evolution(20.0 mmol·g^(−1)·h^(−1),apparent quantum efficiency(AQE)=7.6%,atλ=450 nm)with 0.40 wt.%Pt loading,giving rise to a 44-fold-increase in the efficiency of the photocatalytic hydrogen production compared to the pristine CTF-1.Theoretical calculations revealed that the strong electron transfer(Q(Pt)=−0.726 qe,in the analysis of Bader charge,Q(Pt)is the charge quantity transferred from Pt cluster to CTF-1,and qe is the unit of charge transfer quantity)between PtNPs and CTF-1 triggers a strong interaction,which makes PtNPs being firmly attached to the structure of CTF-1,thereby enabling high stability and excellent hydrogen production efficiency.Importantly,the hydrogen binding free energy(ΔGH*)of PtNPs@CTF-1 is much lower than that of the unmodified CTF-1,leading to a much lower intermediate state and hence a significant improvement in photocatalytic performance.The overall findings of this work provide a new platform to incorporate metallic NPs into COFs for the design and fabrication of highly efficient photocatalysts.

关 键 词：Pt nanoparticles covalent triazine-based framework-1(CTF-1) PHOTOCATALYSTS hydrogen evolution reaction 

分 类 号：O643.3[理学—物理化学] O644.1[理学—化学]