摘要
A facile and effective impregnation combined with photo-deposition approach was adopted to deposit cadmium sulfide(CdS)nanoparticles on CTF-1,a covalent triazine-based frameworks(CTFs).In this system,CTF-1 not only acted as supporter but also served as photocatalyst and electron donor.The performance of the obtained CdS deposited CTF-1(CdS-CTF-1)nanocomposite was evaluated by H2 evolution reaction under visible light irradiation.As a result,CdS-CTF-1 exhibited high H2 production from water,far surpassing the Cd S/CTF-1 nanocomposite,in which Cd S was deposited via solvothermal method.The high activity of CdS-CTF-1 was attributed to the confined Cd S nanoparticles with small size,leading to expose more active sites.In addition,time-resolved spectroscopy indicated that the superior performance of Cd S-CTF-1 also can be ascribed to the fast electron transfer rate and injection efficiency(KET=0.18×10^9 s^-1,ηinj=39.38%)between Cd S and CTF-1 layers,which are 3.83 times faster and 4.84 times higher than that of Cd S/CTF-1 nanocomposite.This work represents the first example on using covalent organic frameworks(COFs)as a support and electron-donor for fabricating novel Cd S-COF nanocomposite system and its potential application in solar energy transformations.
本文采用一种简便有效的浸渍结合光沉积的方法实现了在共价有机框架(CTF-1)材料上沉积CdS纳米粒子.在该研究体系中,CTF-1材料不仅作为载体,还作为光催化剂和电子给体.在可见光照射下,作者考察了所制备的Cd S-CTF-1纳米复合材料的产氢性能.结果表明,CdS-CTF-1具有较高的光催化水制氢能力,其催化活性远远超过了用传统溶剂热法沉积Cd S的Cd S/CTF-1复合材料的光催化产氢活性.通过催化剂的形貌分析推测CdS-CTF-1的高活性可能源于其较小的Cd S纳米粒子尺寸(平均尺寸为16.52 nm),能够暴露出更多的活性位点,以致表现出较高的产氢性能.此外,通过时间分辨光谱研究发现CdS-CTF-1优异的催化性能还归因于Cd S纳米颗粒与CTF-1之间的快速电子转移速率和高效的注入效率(KET=0.18×10^9 s^–1,ηinj=39.38%),相比于CdS/CTF-1复合材料的电子转移速率和注入效率分别高出3.83和4.84倍.本研究利用共价有机框架(COFs)作为载体和电子供体制备了新型无机-有机纳米复合材料(CdS-CTF-1),并详细研究了其在太阳能转换中的潜在应用,讨论了其形貌结构对催化性能的影响,为后续开发高效的光催化材料实现可持续的能源转化提供借鉴.
基金
financially supported by the National Natural Science Foundation of China(51938007,51878325,51868050,51622806 and 51868052)
the Natural Science Foundation of Jiangxi Province(20162BCB22017,20165BCB18008,20171ACB20017,and 20171BAB206049)
the Ph.D.research startup foundation of Nanchang Hangkong University(EA201802367)
the foundation of Jiangxi Scientific Committee(DA201902167)for financial support.
